Articles | Volume 23, issue 2
https://doi.org/10.5194/acp-23-1227-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-23-1227-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
24 Jan 2023
Research article |
| 24 Jan 2023
| 24 Jan 2023
Nitrogen oxides in the free troposphere: implications for tropospheric oxidants and the interpretation of satellite NO2 measurements
Harvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 01238, USA
now at: Global Modeling and Assimilation Office, NASA Goddard
Space Flight Center, Greenbelt, MD 20771, USA
now at: Science Systems and Applications, Inc., Lanham, MD 20706, USA
Daniel J. Jacob
Harvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 01238, USA
Department of Earth and Planetary Sciences, Harvard University,
Cambridge, MA 02138, USA
Ruijun Dang
Harvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 01238, USA
Lok N. Lamsal
Atmospheric Chemistry and Dynamics Laboratory, NASA Goddard Space
Flight Center, Greenbelt, MD 20771, USA
GESTAR II, University of Maryland Baltimore County, Baltimore, MD 21250, USA
Sarah A. Strode
Atmospheric Chemistry and Dynamics Laboratory, NASA Goddard Space
Flight Center, Greenbelt, MD 20771, USA
GESTAR II, Morgan State University, Baltimore, MD 21251, USA
Stephen D. Steenrod
Atmospheric Chemistry and Dynamics Laboratory, NASA Goddard Space
Flight Center, Greenbelt, MD 20771, USA
GESTAR II, University of Maryland Baltimore County, Baltimore, MD 21250, USA
K. Folkert Boersma
Satellite Observations Department, Royal Netherlands Meteorological Institute (KNMI), De Bilt, the Netherlands
Meteorology and Air Quality Group, Wageningen University, Wageningen, the Netherlands
Sebastian D. Eastham
Laboratory for Aviation and the Environment, Department of
Aeronautics and Astronautics, Massachusetts Institute of Technology, Cambridge, MA 02139, USA
Joint Program on the Science and Policy of Global Change,
Massachusetts Institute of Technology, Cambridge, MA 02139, USA
Thibaud M. Fritz
Laboratory for Aviation and the Environment, Department of
Aeronautics and Astronautics, Massachusetts Institute of Technology, Cambridge, MA 02139, USA
Chelsea Thompson
NOAA Chemical Sciences Laboratory, Boulder, CO 80305, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO 80309, USA
Jeff Peischl
NOAA Chemical Sciences Laboratory, Boulder, CO 80305, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO 80309, USA
Ilann Bourgeois
NOAA Chemical Sciences Laboratory, Boulder, CO 80305, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO 80309, USA
now at: Extreme Environments Research Laboratory, École
Polytechnique Fédérale de Lausanne Valais Wallis, Sion, Switzerland
now at: Plant Ecology Research Laboratory, École Polytechnique
Fédérale de Lausanne, Lausanne, Switzerland
Ilana B. Pollack
Department of Atmospheric Sciences, Colorado State University, Fort Collins, CO 80523, USA
Benjamin A. Nault
Center for Aerosols and Cloud Chemistry, Aerodyne Research, Inc.,
Billerica, MA 01821, USA
Ronald C. Cohen
Department of Earth and Planetary Science, University of California Berkeley, Berkeley, CA 94720, USA
Department of Chemistry, University of California Berkeley,
Berkeley, CA 94720, USA
Pedro Campuzano-Jost
Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO 80309, USA
Department of Chemistry, University of Colorado Boulder, Boulder, CO 80309, USA
Jose L. Jimenez
Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO 80309, USA
Department of Chemistry, University of Colorado Boulder, Boulder, CO 80309, USA
Simone T. Andersen
Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, YO10 5DD, UK
Lucy J. Carpenter
Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, YO10 5DD, UK
Tomás Sherwen
Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, YO10 5DD, UK
National Centre for Atmospheric Science, University of York, York
YO10 5DD, UK
Mat J. Evans
Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, YO10 5DD, UK
National Centre for Atmospheric Science, University of York, York
YO10 5DD, UK
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We examined aerosol particles from wildfires and identified tarballs (TBs) from the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) campaign. This study reveals the compositions, abundance, sizes, and mixing states of TBs and shows that TBs formed as the smoke aged for up to 5 h. This study provides measurements of TBs from various biomass-burning events and ages, enhancing our knowledge of TB emissions and our understanding of their climate impact.
Fernando Chouza, Thierry Leblanc, Patrick Wang, Steven S. Brown, Kristen Zuraski, Wyndom Chace, Caroline C. Womack, Jeff Peischl, John Hair, Taylor Shingler, and John Sullivan
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2024-154, https://doi.org/10.5194/amt-2024-154, 2024
Revised manuscript accepted for AMT
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The JPL lidar group developed the SMOL (Small Mobile Ozone Lidar), an affordable ozone differential absorption lidar (DIAL) system covering all altitudes from 200 m to 10 km. a.g.l. The comparison with airborne in-situ and lidar measurements shows very good agreement. An additional comparison with nearby surface ozone measuring instruments indicates unbiased measurements by the SMOL lidars down to 200 m above ground level.
Carley D. Fredrickson, Scott J. Janz, Lok N. Lamsal, Ursula A. Jongebloed, Joshua L. Laughner, and Joel A. Thornton
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2024-158, https://doi.org/10.5194/amt-2024-158, 2024
Preprint under review for AMT
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We present an analysis of high-resolution remote sensing measurements of nitrogen-containing trace gases emitted by wildfires. The measurements were made using an instrument on the NASA ER-2 aircraft in the summer of 2019. We find that time-resolved fire intensity is critical to quantify trace gas emissions over a fire’s entire lifespan. These findings have implications for improving air pollution forecasts downwind of wildfires using computer models of atmospheric chemistry and meteorology.
Qianqian Zhang, K. Folkert Boersma, Chiel van der Laan, Alba Mols, Bin Zhao, Shengyue Li, and Yuepeng Pan
EGUsphere, https://doi.org/10.5194/egusphere-2024-2641, https://doi.org/10.5194/egusphere-2024-2641, 2024
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Accurate NOx emission estimates are required to better understand air pollution. This study investigates and demonstrates the ability of the superposition column model in combination with TROPOMI tropospheric NO2 column data to estimate city-scale NOx emissions and lifetimes and their variabilities. The results of this work nevertheless confirm the strength of the superposition column model in estimating urban NOx emissions with reasonable accuracy.
Hendrik Fuchs, Aaron Stainsby, Florian Berg, René Dubus, Michelle Färber, Andreas Hofzumahaus, Frank Holland, Kelvin H. Bates, Steven S. Brown, Matthew M. Coggon, Glenn S. Diskin, Georgios I. Gkatzelis, Christopher M. Jernigan, Jeff Peischl, Michael A. Robinson, Andrew W. Rollins, Nell B. Schafer, Rebecca H. Schwantes, Chelsea E. Stockwell, Patrick R. Veres, Carsten Warneke, Eleanor M. Waxman, Lu Xu, Kristen Zuraski, Andreas Wahner, and Anna Novelli
EGUsphere, https://doi.org/10.5194/egusphere-2024-2752, https://doi.org/10.5194/egusphere-2024-2752, 2024
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Significant improvements have been made to the instruments used to measure OH reactivity, which is equivalent to the sum of air pollutant concentrations. Accurate and precise measurements with a high time resolution have been achieved, allowing use on aircraft, as demonstrated during flights in the USA.
Pinchas Nürnberg, Sarah A. Strode, and Ralf Sussmann
Atmos. Chem. Phys., 24, 10001–10012, https://doi.org/10.5194/acp-24-10001-2024, https://doi.org/10.5194/acp-24-10001-2024, 2024
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We created a set of scaling factors describing the diurnal increase in stratospheric nitrogen oxides above Zugspitze, Germany. We used these factors to validate recently published model simulation data. On the one hand, this validation enables the use of the validated data to better understand the stratospheric photochemistry. On the other hand, it can improve satellite validation, which has implications for the understanding of urban smog events and other pollution events in the troposphere.
Ryan J. Pound, Lucy V. Brown, Mat J. Evans, and Lucy J. Carpenter
Atmos. Chem. Phys., 24, 9899–9921, https://doi.org/10.5194/acp-24-9899-2024, https://doi.org/10.5194/acp-24-9899-2024, 2024
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Iodine-mediated loss of ozone to the ocean surface and the subsequent emission of iodine species has a large effect on the troposphere. Here we combine recent experimental insights to develop a box model of the process, which we then parameterize and incorporate into the GEOS-Chem transport model. We find that these new insights have a small impact on the total emission of iodine but significantly change its distribution.
Audrey Gaudel, Ilann Bourgeois, Meng Li, Kai-Lan Chang, Jerald Ziemke, Bastien Sauvage, Ryan M. Stauffer, Anne M. Thompson, Debra E. Kollonige, Nadia Smith, Daan Hubert, Arno Keppens, Juan Cuesta, Klaus-Peter Heue, Pepijn Veefkind, Kenneth Aikin, Jeff Peischl, Chelsea R. Thompson, Thomas B. Ryerson, Gregory J. Frost, Brian C. McDonald, and Owen R. Cooper
Atmos. Chem. Phys., 24, 9975–10000, https://doi.org/10.5194/acp-24-9975-2024, https://doi.org/10.5194/acp-24-9975-2024, 2024
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The study examines tropical tropospheric ozone changes. In situ data from 1994–2019 display increased ozone, notably over India, Southeast Asia, and Malaysia and Indonesia. Sparse in situ data limit trend detection for the 15-year period. In situ and satellite data, with limited sampling, struggle to consistently detect trends. Continuous observations are vital over the tropical Pacific Ocean, Indian Ocean, western Africa, and South Asia for accurate ozone trend estimation in these regions.
Andrew O. Langford, Raul J. Alvarez II, Kenneth C. Aikin, Sunil Baidar, W. Alan Brewer, Steven S. Brown, Matthew M. Coggan, Patrick D. Cullis, Jessica Gilman, Georgios I. Gkatzelis, Detlev Helmig, Bryan J. Johnson, K. Emma Knowland, Rajesh Kumar, Aaron D. Lamplugh, Audra McClure-Begley, Brandi J. McCarty, Ann M. Middlebrook, Gabriele Pfister, Jeff Peischl, Irina Petropavlovskikh, Pamela S. Rickley, Andrew W. Rollins, Scott P. Sandberg, Christoph J. Senff, and Carsten Warneke
EGUsphere, https://doi.org/10.5194/egusphere-2024-1938, https://doi.org/10.5194/egusphere-2024-1938, 2024
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High ozone (O3) formed by reactions of nitrogen oxides (NOx) and volatile organic compounds (VOCs) can harm human health and welfare. High O3 is usually associated with hot summer days, but under certain conditions, high O3 can also form under winter conditions. In this study, we describe a high O3 event that occurred in Colorado during the COVID-19 quarantine that was caused in part by the decrease in traffic, and in part by a shallow inversion created by descent of stratospheric air.
Yujin J. Oak, Daniel J. Jacob, Nicholas Balasus, Laura H. Yang, Heesung Chong, Junsung Park, Hanlim Lee, Gitaek T. Lee, Eunjo S. Ha, Rokjin J. Park, Hyeong-Ahn Kwon, and Jhoon Kim
Atmos. Meas. Tech., 17, 5147–5159, https://doi.org/10.5194/amt-17-5147-2024, https://doi.org/10.5194/amt-17-5147-2024, 2024
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We present an improved NO2 product from GEMS by calibrating it to TROPOMI using machine learning and by reprocessing both satellite products to adopt common NO2 profiles. Our corrected GEMS product combines the high data density of GEMS with the accuracy of TROPOMI, supporting the combined use for analyses of East Asia air quality including emissions and chemistry. This method can be extended to other species and geostationary satellites including TEMPO and Sentinel-4.
Benjamin A. Nault, Katherine R. Travis, James H. Crawford, Donald R. Blake, Pedro Campuzano-Jost, Ronald C. Cohen, Joshua P. DiGangi, Glenn S. Diskin, Samuel R. Hall, L. Gregory Huey, Jose L. Jimenez, Kyung-Eun Min, Young Ro Lee, Isobel J. Simpson, Kirk Ullmann, and Armin Wisthaler
Atmos. Chem. Phys., 24, 9573–9595, https://doi.org/10.5194/acp-24-9573-2024, https://doi.org/10.5194/acp-24-9573-2024, 2024
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Ozone (O3) is a pollutant formed from the reactions of gases emitted from various sources. In urban areas, the density of human activities can increase the O3 formation rate (P(O3)), thus impacting air quality and health. Observations collected over Seoul, South Korea, are used to constrain P(O3). A high local P(O3) was found; however, local P(O3) was partly reduced due to compounds typically ignored. These observations also provide constraints for unmeasured compounds that will impact P(O3).
Katherine R. Travis, Benjamin A. Nault, James H. Crawford, Kelvin H. Bates, Donald R. Blake, Ronald C. Cohen, Alan Fried, Samuel R. Hall, L. Gregory Huey, Young Ro Lee, Simone Meinardi, Kyung-Eun Min, Isobel J. Simpson, and Kirk Ullman
Atmos. Chem. Phys., 24, 9555–9572, https://doi.org/10.5194/acp-24-9555-2024, https://doi.org/10.5194/acp-24-9555-2024, 2024
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Human activities result in the emission of volatile organic compounds (VOCs) that contribute to air pollution. Detailed VOC measurements were taken during a field study in South Korea. When compared to VOC inventories, large discrepancies showed underestimates from chemical products, liquefied petroleum gas, and long-range transport. Improved emissions and chemistry of these VOCs better described urban pollution. The new chemical scheme is relevant to urban areas and other VOC sources.
Tianle Pan, Andrew T. Lambe, Weiwei Hu, Yicong He, Minghao Hu, Huaishan Zhou, Xinming Wang, Qingqing Hu, Hui Chen, Yue Zhao, Yuanlong Huang, Doug R. Worsnop, Zhe Peng, Melissa A. Morris, Douglas A. Day, Pedro Campuzano-Jost, Jose-Luis Jimenez, and Shantanu H. Jathar
Atmos. Meas. Tech., 17, 4915–4939, https://doi.org/10.5194/amt-17-4915-2024, https://doi.org/10.5194/amt-17-4915-2024, 2024
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This study systematically characterizes the temperature enhancement in the lamp-enclosed oxidation flow reactor (OFR). The enhancement varied multiple dimensional factors, emphasizing the complexity of temperature inside of OFR. The effects of temperature on the flow field and gas- or particle-phase reaction inside OFR were also evaluated with experiments and model simulations. Finally, multiple mitigation strategies were demonstrated to minimize this temperature increase.
Edward J. Strobach, Sunil Baidar, Brian J. Carroll, Steven S. Brown, Kristen Zuraski, Matthew Coggon, Chelsea E. Stockwell, Lu Xu, Yelena L. Pichugina, W. Alan Brewer, Carsten Warneke, Jeff Peischl, Jessica Gilman, Brandi McCarty, Maxwell Holloway, and Richard Marchbanks
Atmos. Chem. Phys., 24, 9277–9307, https://doi.org/10.5194/acp-24-9277-2024, https://doi.org/10.5194/acp-24-9277-2024, 2024
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Large-scale weather patterns are isolated from local patterns to study the impact that different weather scales have on air quality measurements. While impacts from large-scale meteorology were evaluated by separating ozone (O3) exceedance (>70 ppb) and non-exceedance (<70 ppb) days, we developed a technique that allows direct comparisons of small temporal variations between chemical and dynamics measurements under rapid dynamical transitions.
Felipe Cifuentes, Henk Eskes, Folkert Boersma, Enrico Dammers, and Charlotte Bryan
EGUsphere, https://doi.org/10.5194/egusphere-2024-2225, https://doi.org/10.5194/egusphere-2024-2225, 2024
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We tested the capability of the flux divergence approach (FDA) to reproduce known NOX emissions using synthetic NO2 satellite column retrievals derived from high-resolution model simulations. The FDA accurately reproduced NOX emissions when column observations were limited to the boundary layer and when the variability of NO2 lifetime, NOX:NO2 ratio, and NO2 profile shapes were correctly modeled. This introduces a strong model dependency, reducing the simplicity of the original FDA formulation.
Patrick Dewald, Tobias Seubert, Simone T. Andersen, Gunther N. T. E. Türk, Jan Schuladen, Max R. McGillen, Cyrielle Denjean, Jean-Claude Etienne, Olivier Garrouste, Marina Jamar, Sergio Harb, Manuela Cirtog, Vincent Michoud, Mathieu Cazaunau, Antonin Bergé, Christopher Cantrell, Sebastien Dusanter, Bénédicte Picquet-Varrault, Alexandre Kukui, Chaoyang Xue, Abdelwahid Mellouki, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 24, 8983–8997, https://doi.org/10.5194/acp-24-8983-2024, https://doi.org/10.5194/acp-24-8983-2024, 2024
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In the scope of a field campaign in a suburban forest near Paris in the summer of 2022, we measured the reactivity of the nitrate radical NO3 towards biogenic volatile organic compounds (BVOCs; e.g. monoterpenes) mainly below but also above the canopy. NO3 reactivity was the highest during nights with strong temperature inversions and decreased strongly with height. Reactions with BVOCs were the main removal process of NO3 throughout the diel cycle below the canopy.
Olivia G. Norman, Colette L. Heald, Pedro Campuzano-Jost, Hugh Coe, Marc N. Fiddler, Jaime R. Green, Jose L. Jimenez, Katharina Kaiser, Jin Liao, Ann M. Middlebrook, Benjamin A. Nault, John B. Nowak, Johannes Schneider, and André Welti
EGUsphere, https://doi.org/10.5194/egusphere-2024-2296, https://doi.org/10.5194/egusphere-2024-2296, 2024
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This study finds that one component of secondary inorganic aerosols, nitrate, is greatly overestimated by a global atmospheric chemistry model compared to observations from 11 flight campaigns. None of the loss and production pathways explored can explain the nitrate bias alone. The model’s inability to capture the variability in the observations remains and requires future investigation to avoid biases in policy-related studies (i.e., air quality, health, climate impacts of these aerosols).
Amir H. Souri, Bryan N. Duncan, Sarah A. Strode, Daniel C. Anderson, Michael E. Manyin, Junhua Liu, Luke D. Oman, Zhen Zhang, and Brad Weir
Atmos. Chem. Phys., 24, 8677–8701, https://doi.org/10.5194/acp-24-8677-2024, https://doi.org/10.5194/acp-24-8677-2024, 2024
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We explore a new method of using the wealth of information obtained from satellite observations of Aura OMI NO2, HCHO, and MERRA-2 reanalysis in NASA’s GEOS model equipped with an efficient tropospheric OH (TOH) estimator to enhance the representation of TOH spatial distribution and its long-term trends. This new framework helps us pinpoint regional inaccuracies in TOH and differentiate between established prior knowledge and newly acquired information from satellites on TOH trends.
Haipeng Lin, Louisa K. Emmons, Elizabeth W. Lundgren, Laura Hyesung Yang, Xu Feng, Ruijun Dang, Shixian Zhai, Yunxiao Tang, Makoto M. Kelp, Nadia K. Colombi, Sebastian D. Eastham, Thibaud M. Fritz, and Daniel J. Jacob
Atmos. Chem. Phys., 24, 8607–8624, https://doi.org/10.5194/acp-24-8607-2024, https://doi.org/10.5194/acp-24-8607-2024, 2024
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Tropospheric ozone is a major air pollutant, a greenhouse gas, and a major indicator of model skill. Global atmospheric chemistry models show large differences in simulations of tropospheric ozone, but isolating sources of differences is complicated by different model environments. By implementing the GEOS-Chem model side by side to CAM-chem within a common Earth system model, we identify and evaluate specific differences between the two models and their impacts on key chemical species.
Irene C. Dedoussi, Daven K. Henze, Sebastian D. Eastham, Raymond L. Speth, and Steven R. H. Barrett
Geosci. Model Dev., 17, 5689–5703, https://doi.org/10.5194/gmd-17-5689-2024, https://doi.org/10.5194/gmd-17-5689-2024, 2024
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Atmospheric model gradients provide a meaningful tool for better understanding the underlying atmospheric processes. Adjoint modeling enables computationally efficient gradient calculations. We present the adjoint of the GEOS-Chem unified chemistry extension (UCX). With this development, the GEOS-Chem adjoint model can capture stratospheric ozone and other processes jointly with tropospheric processes. We apply it to characterize the Antarctic ozone depletion potential of active halogen species.
Elise Penn, Daniel J. Jacob, Zichong Chen, James D. East, Melissa P. Sulprizio, Lori Bruhwiler, Joannes D. Maasakkers, Hannah Nesser, Zhen Qu, Yuzhong Zhang, and John Worden
EGUsphere, https://doi.org/10.5194/egusphere-2024-2260, https://doi.org/10.5194/egusphere-2024-2260, 2024
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The hydroxyl radical (OH), destroys many air pollutants, including methane. Global mean OH cannot be directly measured, so it is inferred with the methyl chloroform (MCF) proxy. MCF is decreasing, and a replacement is needed. We use satellite observations of methane in two spectral ranges as a proxy for OH instead. We find shortwave infrared observations can characterize yearly OH and its seasonality, but not the latitudinal distribution. Thermal infrared observations add little information.
Tong Sha, Siyu Yang, Qingcai Chen, Liangqing Li, Xiaoyan Ma, Yan-Lin Zhang, Zhaozhong Feng, K. Folkert Boersma, and Jun Wang
Atmos. Chem. Phys., 24, 8441–8455, https://doi.org/10.5194/acp-24-8441-2024, https://doi.org/10.5194/acp-24-8441-2024, 2024
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Using an updated soil reactive nitrogen emission scheme in the Unified Inputs for Weather Research and Forecasting coupled with Chemistry (UI-WRF-Chem) model, we investigate the role of soil NO and HONO (Nr) emissions in air quality and temperature in North China. Contributions of soil Nr emissions to O3 and secondary pollutants are revealed, exceeding effects of soil NOx or HONO emission. Soil Nr emissions play an important role in mitigating O3 pollution and addressing climate change.
Matthew J. Rowlinson, Mat J. Evans, Lucy J. Carpenter, Katie A. Read, Shalini Punjabi, Adedayo Adedeji, Luke Fakes, Ally Lewis, Ben Richmond, Neil Passant, Tim Murrells, Barron Henderson, Kelvin H. Bates, and Detlev Helmig
Atmos. Chem. Phys., 24, 8317–8342, https://doi.org/10.5194/acp-24-8317-2024, https://doi.org/10.5194/acp-24-8317-2024, 2024
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Ethane and propane are volatile organic compounds emitted from human activities which help to form ozone, a pollutant and greenhouse gas, and also affect the chemistry of the lower atmosphere. Atmospheric models tend to do a poor job of reproducing the abundance of these compounds in the atmosphere. By using regional estimates of their emissions, rather than globally consistent estimates, we can significantly improve the simulation of ethane in the model and make some improvement for propane.
Maarten Krol, Bart van Stratum, Isidora Anglou, and Klaas Folkert Boersma
Atmos. Chem. Phys., 24, 8243–8262, https://doi.org/10.5194/acp-24-8243-2024, https://doi.org/10.5194/acp-24-8243-2024, 2024
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This paper presents detailed plume simulations of nitrogen oxides and carbon dioxide that are emitted from four large industrial facilities world-wide. Results from the high-resolution simulations that include atmospheric chemistry are compared to nitrogen dioxide observations from satellites. We find good performance of the model and show that common assumptions that are used in simplified models need revision. This work is important for the monitoring of emissions using satellite data.
Chelsea E. Stockwell, Matthew M. Coggon, Rebecca H. Schwantes, Colin Harkins, Bert Verreyken, Congmeng Lyu, Qindan Zhu, Lu Xu, Jessica B. Gilman, Aaron Lamplugh, Jeff Peischl, Michael A. Robinson, Patrick R. Veres, Meng Li, Andrew W. Rollins, Kristen Zuraski, Sunil Baidar, Shang Liu, Toshihiro Kuwayama, Steven S. Brown, Brian C. McDonald, and Carsten Warneke
EGUsphere, https://doi.org/10.5194/egusphere-2024-1899, https://doi.org/10.5194/egusphere-2024-1899, 2024
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In urban areas, emissions from everyday products like paints, cleaners, and personal care products, along with non-traditional sources such as cooking are important sources that impact air quality. This study used a model to evaluate how these emissions impact ozone in the Los Angeles Basin, and quantifies the impact of gaseous cooking emissions for the first time. Accurate representation of these and other man-made sources in inventories is crucial to inform effective air quality policies.
Sarah E. Hancock, Daniel Jacob, Zichong Chen, Hannah Nesser, Aaron Davitt, Daniel J. Varon, Melissa P. Sulprizio, Nicholas Balasus, Lucas A. Estrada, James D. East, Elise Penn, Cynthia A. Randles, John Worden, Ilse Aben, Robert J. Parker, and Joannes D. Maasakkers
EGUsphere, https://doi.org/10.5194/egusphere-2024-1763, https://doi.org/10.5194/egusphere-2024-1763, 2024
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We quantify 2021 methane emissions in South America at up to 25 km × 25 km resolution using satellite methane observations. We find a 55 % upward correction to the national anthropogenic inventories reported to the United Nations Framework Convention on Climate Change (UNFCCC) under the Paris Agreement. Our estimates match inventories for Brazil, Bolivia, and Paraguay but are much higher for other countries. Livestock emissions (65 % of anthropogenic emissions) show the largest discrepancies.
Laura Hyesung Yang, Daniel J. Jacob, Ruijun Dang, Yujin J. Oak, Haipeng Lin, Jhoon Kim, Shixian Zhai, Nadia K. Colombi, Drew C. Pendergrass, Ellie Beaudry, Viral Shah, Xu Feng, Robert M. Yantosca, Heesung Chong, Junsung Park, Hanlim Lee, Won-Jin Lee, Soontae Kim, Eunhye Kim, Katherine R. Travis, James H. Crawford, and Hong Liao
Atmos. Chem. Phys., 24, 7027–7039, https://doi.org/10.5194/acp-24-7027-2024, https://doi.org/10.5194/acp-24-7027-2024, 2024
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The Geostationary Environment Monitoring Spectrometer (GEMS) provides hourly measurements of NO2. We use the chemical transport model to find how emissions, chemistry, and transport drive the changes in NO2 observed by GEMS at different times of the day. In winter, the chemistry plays a minor role, and high daytime emissions dominate the diurnal variation in NO2, balanced by transport. In summer, emissions, chemistry, and transport play an important role in shaping the diurnal variation in NO2.
Gregory P. Schill, Karl D. Froyd, Daniel M. Murphy, Christina J. Williamson, Charles Brock, Tomás Sherwen, Mat J. Evans, Eric A. Ray, Eric C. Apel, Rebecca S. Hornbrook, Alan J. Hills, Jeff Peischl, Tomas B. Ryerson, Chelsea R. Thompson, Ilann Bourgeois, Donald R. Blake, Joshua P. DiGangi, and Glenn S. Diskin
EGUsphere, https://doi.org/10.5194/egusphere-2024-1399, https://doi.org/10.5194/egusphere-2024-1399, 2024
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Using single-particle mass spectrometry, we show that trace concentrations of bromine and iodine are ubiquitous in remote tropospheric aerosol, and suggest that aerosols are an important part of the global reactive iodine budget. Comparisons to a global climate model with detailed iodine chemistry are favorable in the background atmosphere; however, the model cannot replicate our measurements near the ocean surface, in biomass burning plumes, and in the stratosphere.
Drew C. Pendergrass, Daniel J. Jacob, Yujin J. Oak, Jeewoo Lee, Minseok Kim, Jhoon Kim, Seoyoung Lee, Shixian Zhai, Hitoshi Irie, and Hong Liao
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2024-172, https://doi.org/10.5194/essd-2024-172, 2024
Preprint withdrawn
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Fine particles suspended in the atmosphere are a major form of air pollution and an important public health burden. However, measurements of particulate matter are sparse in space and in places like East Asia monitors are established after regulatory policies to improve pollution have changed. In this paper, we use machine learning to fill in the gaps. We train an algorithm to predict pollution at the surface from the atmosphere’s opacity, then produce high resolution maps of data without gaps.
Juliëtte C. S. Anema, Klaas Folkert Boersma, Piet Stammes, Gerbrand Koren, William Woodgate, Philipp Köhler, Christian Frankenberg, and Jacqui Stol
Biogeosciences, 21, 2297–2311, https://doi.org/10.5194/bg-21-2297-2024, https://doi.org/10.5194/bg-21-2297-2024, 2024
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To keep the Paris agreement goals within reach, negative emissions are necessary. They can be achieved with mitigation techniques, such as reforestation, which remove CO2 from the atmosphere. While governments have pinned their hopes on them, there is not yet a good set of tools to objectively determine whether negative emissions do what they promise. Here we show how satellite measurements of plant fluorescence are useful in detecting carbon uptake due to reforestation and vegetation regrowth.
Melinda K. Schueneman, Douglas A. Day, Dongwook Kim, Pedro Campuzano-Jost, Seonsik Yun, Marla P. DeVault, Anna C. Ziola, Paul J. Ziemann, and Jose L. Jimenez
Aerosol Research, 2, 59–76, https://doi.org/10.5194/ar-2-59-2024, https://doi.org/10.5194/ar-2-59-2024, 2024
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Our study presents a novel method for quantifying mass spectrometer responses to molecular species in organic aerosols. Traditional calibrations often fail for complex mixtures like secondary organic aerosol. We combined chromatography with statistical component analysis to improve separation and quantification, achieving promising agreement with direct calibration. Our findings offer a new approach to assess aerosol composition, especially beneficial for complex mixtures.
Qindan Zhu, Rebecca H. Schwantes, Matthew Coggon, Colin Harkins, Jordan Schnell, Jian He, Havala O. T. Pye, Meng Li, Barry Baker, Zachary Moon, Ravan Ahmadov, Eva Y. Pfannerstill, Bryan Place, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Anthony Bucholtz, John H. Seinfeld, Carsten Warneke, Chelsea E. Stockwell, Lu Xu, Kristen Zuraski, Michael A. Robinson, J. Andrew Neuman, Patrick R. Veres, Jeff Peischl, Steven S. Brown, Allen H. Goldstein, Ronald C. Cohen, and Brian C. McDonald
Atmos. Chem. Phys., 24, 5265–5286, https://doi.org/10.5194/acp-24-5265-2024, https://doi.org/10.5194/acp-24-5265-2024, 2024
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Volatile organic compounds (VOCs) fuel the production of air pollutants like ozone and particulate matter. The representation of VOC chemistry remains challenging due to its complexity in speciation and reactions. Here, we develop a chemical mechanism, RACM2B-VCP, that better represents VOC chemistry in urban areas such as Los Angeles. We also discuss the contribution of VOCs emitted from volatile chemical products and other anthropogenic sources to total VOC reactivity and O3.
Jack H. Bruno, Dylan Jervis, Daniel J. Varon, and Daniel J. Jacob
Atmos. Meas. Tech., 17, 2625–2636, https://doi.org/10.5194/amt-17-2625-2024, https://doi.org/10.5194/amt-17-2625-2024, 2024
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Methane is a potent greenhouse gas and a current high-priority target for short- to mid-term climate change mitigation. Detection of individual methane emitters from space has become possible in recent years, and the volume of data for this task has been rapidly growing, outpacing processing capabilities. We introduce an automated approach, U-Plume, which can detect and quantify emissions from individual methane sources in high-spatial-resolution satellite data.
Hannah Nesser, Daniel J. Jacob, Joannes D. Maasakkers, Alba Lorente, Zichong Chen, Xiao Lu, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Margaux Winter, Shuang Ma, A. Anthony Bloom, John R. Worden, Robert N. Stavins, and Cynthia A. Randles
Atmos. Chem. Phys., 24, 5069–5091, https://doi.org/10.5194/acp-24-5069-2024, https://doi.org/10.5194/acp-24-5069-2024, 2024
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We quantify 2019 methane emissions in the contiguous US (CONUS) at a ≈ 25 km × 25 km resolution using satellite methane observations. We find a 13 % upward correction to the 2023 US Environmental Protection Agency (EPA) Greenhouse Gas Emissions Inventory (GHGI) for 2019, with large corrections to individual states, urban areas, and landfills. This may present a challenge for US climate policies and goals, many of which target significant reductions in methane emissions.
Matthew M. Coggon, Chelsea E. Stockwell, Lu Xu, Jeff Peischl, Jessica B. Gilman, Aaron Lamplugh, Henry J. Bowman, Kenneth Aikin, Colin Harkins, Qindan Zhu, Rebecca H. Schwantes, Jian He, Meng Li, Karl Seltzer, Brian McDonald, and Carsten Warneke
Atmos. Chem. Phys., 24, 4289–4304, https://doi.org/10.5194/acp-24-4289-2024, https://doi.org/10.5194/acp-24-4289-2024, 2024
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Residential and commercial cooking emits pollutants that degrade air quality. Here, ambient observations show that cooking is an important contributor to anthropogenic volatile organic compounds (VOCs) emitted in Las Vegas, NV. These emissions are not fully presented in air quality models, and more work may be needed to quantify emissions from important sources, such as commercial restaurants.
Lucy V. Brown, Ryan J. Pound, Lyndsay S. Ives, Matthew R. Jones, Stephen J. Andrews, and Lucy J. Carpenter
Atmos. Chem. Phys., 24, 3905–3923, https://doi.org/10.5194/acp-24-3905-2024, https://doi.org/10.5194/acp-24-3905-2024, 2024
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Ozone is deposited from the lower atmosphere to the surface of the ocean; however, the chemical reactions which drive this deposition are currently not well understood. Of particular importance is the reaction between ozone and iodide, and this work measures the kinetics of this reaction and its temperature dependence, which we find to be negligible. We then investigate the subsequent emissions of iodine-containing species from the surface ocean, which can further impact ozone.
Pieter Rijsdijk, Henk Eskes, Arlene Dingemans, Folkert Boersma, Takashi Sekiya, Kazuyuki Miyazaki, and Sander Houweling
EGUsphere, https://doi.org/10.5194/egusphere-2024-632, https://doi.org/10.5194/egusphere-2024-632, 2024
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Clustering high-resolution satellite observations into superobservations improves model validation and data assimilation applications. In our paper, we derive quantitative uncertainties for satellite NO2 column observations based on knowledge of the retrievals, including a detailed analysis of spatial error correlations and representativity errors. The superobservations and uncertainty estimates are tested in a global chemical data assimilation system and are found to improve the forecasts.
James M. Roberts, Siyuan Wang, Patrick R. Veres, J. Andrew Neuman, Michael A. Robinson, Ilann Bourgeois, Jeff Peischl, Thomas B. Ryerson, Chelsea R. Thompson, Hannah M. Allen, John D. Crounse, Paul O. Wennberg, Samuel R. Hall, Kirk Ullmann, Simone Meinardi, Isobel J. Simpson, and Donald Blake
Atmos. Chem. Phys., 24, 3421–3443, https://doi.org/10.5194/acp-24-3421-2024, https://doi.org/10.5194/acp-24-3421-2024, 2024
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We measured cyanogen bromide (BrCN) in the troposphere for the first time. BrCN is a product of the same active bromine chemistry that destroys ozone and removes mercury in polar surface environments and is a previously unrecognized sink for active Br compounds. BrCN has an apparent lifetime against heterogeneous loss in the range 1–10 d, so it serves as a cumulative marker of Br-radical chemistry. Accounting for BrCN chemistry is an important part of understanding polar Br cycling.
Melissa A. Morris, Demetrios Pagonis, Douglas A. Day, Joost A. de Gouw, Paul J. Ziemann, and Jose L. Jimenez
Atmos. Meas. Tech., 17, 1545–1559, https://doi.org/10.5194/amt-17-1545-2024, https://doi.org/10.5194/amt-17-1545-2024, 2024
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Polymer absorption of volatile organic compounds (VOCs) is important to characterize for atmospheric sampling setups (as interactions cause sampling delays) and indoor air quality. Here we test different polymer materials and quantify their absorptive capacities through modeling. We found the main polymers in carpets to be highly absorptive, acting as large reservoirs for indoor pollution. We also demonstrated how polymer tubes can be used as a low-cost gas separation technique.
Sebastian D. Eastham, Guillaume P. Chossière, Raymond L. Speth, Daniel J. Jacob, and Steven R. H. Barrett
Atmos. Chem. Phys., 24, 2687–2703, https://doi.org/10.5194/acp-24-2687-2024, https://doi.org/10.5194/acp-24-2687-2024, 2024
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Emissions from aircraft are known to cause air quality impacts worldwide, but the scale and mechanisms of this impact are not well understood. This work uses high-resolution computational modeling of the atmosphere to show that air pollution changes from aviation are mostly the result of emissions during cruise (high-altitude) operations, that these impacts are related to how much non-aviation pollution is present, and that prior regional assessments have underestimated these impacts.
Kelvin H. Bates, Mathew J. Evans, Barron H. Henderson, and Daniel J. Jacob
Geosci. Model Dev., 17, 1511–1524, https://doi.org/10.5194/gmd-17-1511-2024, https://doi.org/10.5194/gmd-17-1511-2024, 2024
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Accurate representation of rates and products of chemical reactions in atmospheric models is crucial for simulating concentrations of pollutants and climate forcers. We update the widely used GEOS-Chem atmospheric chemistry model with reaction parameters from recent compilations of experimental data and demonstrate the implications for key atmospheric chemical species. The updates decrease tropospheric CO mixing ratios and increase stratospheric nitrogen oxide mixing ratios, among other changes.
Alexander T. Archibald, Bablu Sinha, Maria Russo, Emily Matthews, Freya Squires, N. Luke Abraham, Stephane Bauguitte, Thomas Bannan, Thomas Bell, David Berry, Lucy Carpenter, Hugh Coe, Andrew Coward, Peter Edwards, Daniel Feltham, Dwayne Heard, Jim Hopkins, James Keeble, Elizabeth C. Kent, Brian King, Isobel R. Lawrence, James Lee, Claire R. Macintosh, Alex Megann, Ben I. Moat, Katie Read, Chris Reed, Malcolm Roberts, Reinhard Schiemann, David Schroeder, Tim Smyth, Loren Temple, Navaneeth Thamban, Lisa Whalley, Simon Williams, Huihui Wu, and Ming-Xi Yang
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2023-405, https://doi.org/10.5194/essd-2023-405, 2024
Revised manuscript accepted for ESSD
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Here we present an overview of the data generated as part of the North Atlantic Climate System Integrated Studies (ACSIS) programme which are available through dedicated repositories at the Centre for Environmental Data Analysis (CEDA, www.ceda.ac.uk) and the British Oceanographic Data Centre (BODC, bodc.ac.uk). ACSIS data cover the full North Atlantic System comprising: the North Atlantic Ocean, the atmosphere above it including its composition, Arctic Sea Ice and the Greenland Ice Sheet.
Milan Y. Patel, Pietro F. Vannucci, Jinsol Kim, William M. Berelson, and Ronald C. Cohen
Atmos. Meas. Tech., 17, 1051–1060, https://doi.org/10.5194/amt-17-1051-2024, https://doi.org/10.5194/amt-17-1051-2024, 2024
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Low-cost particulate matter (PM) sensors are becoming increasingly common in community monitoring and atmospheric research, but these sensors require proper calibration to provide accurate reporting. Here, we propose a hygroscopic growth calibration scheme that evolves in time to account for seasonal changes in hygroscopic growth. In San Francisco and Los Angeles, CA, applying a seasonal hygroscopic growth calibration can account for sensor biases driven by the seasonal cycles in PM composition.
Huisheng Bian, Mian Chin, Peter R. Colarco, Eric C. Apel, Donald R. Blake, Karl Froyd, Rebecca S. Hornbrook, Jose Jimenez, Pedro Campuzano Jost, Michael Lawler, Mingxu Liu, Marianne Tronstad Lund, Hitoshi Matsui, Benjamin A. Nault, Joyce E. Penner, Andrew W. Rollins, Gregory Schill, Ragnhild B. Skeie, Hailong Wang, Lu Xu, Kai Zhang, and Jialei Zhu
Atmos. Chem. Phys., 24, 1717–1741, https://doi.org/10.5194/acp-24-1717-2024, https://doi.org/10.5194/acp-24-1717-2024, 2024
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This work studies sulfur in the remote troposphere at global and seasonal scales using aircraft measurements and multi-model simulations. The goal is to understand the sulfur cycle over remote oceans, spread of model simulations, and observation–model discrepancies. Such an understanding and comparison with real observations are crucial to narrow down the uncertainties in model sulfur simulations and improve understanding of the sulfur cycle in atmospheric air quality, climate, and ecosystems.
Georgios I. Gkatzelis, Matthew M. Coggon, Chelsea E. Stockwell, Rebecca S. Hornbrook, Hannah Allen, Eric C. Apel, Megan M. Bela, Donald R. Blake, Ilann Bourgeois, Steven S. Brown, Pedro Campuzano-Jost, Jason M. St. Clair, James H. Crawford, John D. Crounse, Douglas A. Day, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, Jessica B. Gilman, Hongyu Guo, Johnathan W. Hair, Hannah S. Halliday, Thomas F. Hanisco, Reem Hannun, Alan Hills, L. Gregory Huey, Jose L. Jimenez, Joseph M. Katich, Aaron Lamplugh, Young Ro Lee, Jin Liao, Jakob Lindaas, Stuart A. McKeen, Tomas Mikoviny, Benjamin A. Nault, J. Andrew Neuman, John B. Nowak, Demetrios Pagonis, Jeff Peischl, Anne E. Perring, Felix Piel, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Thomas B. Ryerson, Melinda K. Schueneman, Rebecca H. Schwantes, Joshua P. Schwarz, Kanako Sekimoto, Vanessa Selimovic, Taylor Shingler, David J. Tanner, Laura Tomsche, Krystal T. Vasquez, Patrick R. Veres, Rebecca Washenfelder, Petter Weibring, Paul O. Wennberg, Armin Wisthaler, Glenn M. Wolfe, Caroline C. Womack, Lu Xu, Katherine Ball, Robert J. Yokelson, and Carsten Warneke
Atmos. Chem. Phys., 24, 929–956, https://doi.org/10.5194/acp-24-929-2024, https://doi.org/10.5194/acp-24-929-2024, 2024
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This study reports emissions of gases and particles from wildfires. These emissions are related to chemical proxies that can be measured by satellite and incorporated into models to improve predictions of wildfire impacts on air quality and climate.
Sohyeon Jeon, Michael J. Walker, Donna T. Sueper, Douglas A. Day, Anne V. Handschy, Jose L. Jimenez, and Brent J. Williams
Atmos. Meas. Tech., 16, 6075–6095, https://doi.org/10.5194/amt-16-6075-2023, https://doi.org/10.5194/amt-16-6075-2023, 2023
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A searchable database tool for the Aerosol Mass Spectrometer (AMS) and Aerosol Chemical Speciation Monitor (ACSM) mass spectral datasets was built to improve the efficiency of data analysis using Igor Pro. The tool incorporates the published mass spectra (MS) and sample information uploaded on the website. The tool allows users to compare their own mass spectrum with the reference MS in the database.
Tianle Yuan, Fei Liu, Lok N. Lamsal, and Hua Song
EGUsphere, https://doi.org/10.22541/essoar.168771101.14987378/v1, https://doi.org/10.22541/essoar.168771101.14987378/v1, 2023
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We train and apply a state-of-the-art deep learning model to detect NO2 plumes emitted by ships using NO2 retrievals from TROPOMI. By applying the model, we can detect individual plumes with excellent fidelity. The aggregated data show major shipping routes, but miss other routes. The missing routes are due to high cloudiness. Our method can be potentially useful for monitoring ship emissions of NOx and verifying compliance of emission standards.
Tobias Christoph Valentin Werner Riess, Klaas Folkert Boersma, Ward Van Roy, Jos de Laat, Enrico Dammers, and Jasper van Vliet
Atmos. Meas. Tech., 16, 5287–5304, https://doi.org/10.5194/amt-16-5287-2023, https://doi.org/10.5194/amt-16-5287-2023, 2023
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Satellite retrievals of trace gases require prior knowledge of the vertical distribution of the pollutant, which is usually obtained from models. Using aircraft-measured vertical NO2 profiles over the North Sea in summer 2021, we evaluate the Transport Model 5 profiles used in the TROPOMI NO2 retrieval. We conclude that driven by the low horizontal resolution and the overestimated vertical mixing, resulting NO2 columns are 20 % too low. This has important implications for emission estimates.
Wenfu Tang, Louisa K. Emmons, Helen M. Worden, Rajesh Kumar, Cenlin He, Benjamin Gaubert, Zhonghua Zheng, Simone Tilmes, Rebecca R. Buchholz, Sara-Eva Martinez-Alonso, Claire Granier, Antonin Soulie, Kathryn McKain, Bruce C. Daube, Jeff Peischl, Chelsea Thompson, and Pieternel Levelt
Geosci. Model Dev., 16, 6001–6028, https://doi.org/10.5194/gmd-16-6001-2023, https://doi.org/10.5194/gmd-16-6001-2023, 2023
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The new MUSICAv0 model enables the study of atmospheric chemistry across all relevant scales. We develop a MUSICAv0 grid for Africa. We evaluate MUSICAv0 with observations and compare it with a previously used model – WRF-Chem. Overall, the performance of MUSICAv0 is comparable to WRF-Chem. Based on model–satellite discrepancies, we find that future field campaigns in an eastern African region (30°E–45°E, 5°S–5°N) could substantially improve the predictive skill of air quality models.
Clara M. Nussbaumer, Bryan K. Place, Qindan Zhu, Eva Y. Pfannerstill, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Ryan Ward, Anthony Bucholtz, John H. Seinfeld, Allen H. Goldstein, and Ronald C. Cohen
Atmos. Chem. Phys., 23, 13015–13028, https://doi.org/10.5194/acp-23-13015-2023, https://doi.org/10.5194/acp-23-13015-2023, 2023
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NOx is a precursor to hazardous tropospheric ozone and can be emitted from various anthropogenic sources. It is important to quantify NOx emissions in urban environments to improve the local air quality, which still remains a challenge, as sources are heterogeneous in space and time. In this study, we calculate NOx emissions over Los Angeles, based on aircraft measurements in June 2021, and compare them to a local emission inventory, which we find mostly overpredicts the measured values.
Eva Y. Pfannerstill, Caleb Arata, Qindan Zhu, Benjamin C. Schulze, Roy Woods, John H. Seinfeld, Anthony Bucholtz, Ronald C. Cohen, and Allen H. Goldstein
Atmos. Chem. Phys., 23, 12753–12780, https://doi.org/10.5194/acp-23-12753-2023, https://doi.org/10.5194/acp-23-12753-2023, 2023
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The San Joaquin Valley is an agricultural area with poor air quality. Organic gases drive the formation of hazardous air pollutants. Agricultural emissions of these gases are not well understood and have rarely been quantified at landscape scale. By combining aircraft-based emission measurements with land cover information, we found mis- or unrepresented emission sources. Our results help in understanding of pollution sources and in improving predictions of air quality in agricultural regions.
Qindan Zhu, Bryan Place, Eva Y. Pfannerstill, Sha Tong, Huanxin Zhang, Jun Wang, Clara M. Nussbaumer, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Anthony Bucholtz, John H. Seinfeld, Allen H. Goldstein, and Ronald C. Cohen
Atmos. Chem. Phys., 23, 9669–9683, https://doi.org/10.5194/acp-23-9669-2023, https://doi.org/10.5194/acp-23-9669-2023, 2023
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Nitrogen oxide (NOx) is a hazardous air pollutant, and it is the precursor of short-lived climate forcers like tropospheric ozone and aerosol particles. While NOx emissions from transportation has been strictly regulated, soil NOx emissions are overlooked. We use the airborne flux measurements to observe NOx emissions from highways and urban and cultivated soil land cover types. We show non-negligible soil NOx emissions, which are significantly underestimated in current model simulations.
Drew C. Pendergrass, Daniel J. Jacob, Hannah Nesser, Daniel J. Varon, Melissa Sulprizio, Kazuyuki Miyazaki, and Kevin W. Bowman
Geosci. Model Dev., 16, 4793–4810, https://doi.org/10.5194/gmd-16-4793-2023, https://doi.org/10.5194/gmd-16-4793-2023, 2023
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We have built a tool called CHEEREIO that allows scientists to use observations of pollutants or gases in the atmosphere, such as from satellites or surface stations, to update supercomputer models that simulate the Earth. CHEEREIO uses the difference between the model simulations of the atmosphere and real-world observations to come up with a good guess for the actual composition of our atmosphere, the true emissions of various pollutants, and whatever else they may want to study.
Adedayo R. Adedeji, Stephen J. Andrews, Matthew J. Rowlinson, Mathew J. Evans, Alastair C. Lewis, Shigeru Hashimoto, Hitoshi Mukai, Hiroshi Tanimoto, Yasunori Tohjima, and Takuya Saito
Atmos. Chem. Phys., 23, 9229–9244, https://doi.org/10.5194/acp-23-9229-2023, https://doi.org/10.5194/acp-23-9229-2023, 2023
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We use the GEOS-Chem model to interpret observations of CO, C2H6, C3H8, NOx, NOy and O3 made from Hateruma Island in 2018. The model captures many synoptic-scale events and the seasonality of most pollutants at the site but underestimates C2H6 and C3H8 during the winter. These underestimates are unlikely to be reconciled by increases in biomass burning emissions but could be reconciled by increasing the Asian anthropogenic source of C2H6 and C3H8 by factors of around 2 and 3, respectively.
Nicholas Balasus, Daniel J. Jacob, Alba Lorente, Joannes D. Maasakkers, Robert J. Parker, Hartmut Boesch, Zichong Chen, Makoto M. Kelp, Hannah Nesser, and Daniel J. Varon
Atmos. Meas. Tech., 16, 3787–3807, https://doi.org/10.5194/amt-16-3787-2023, https://doi.org/10.5194/amt-16-3787-2023, 2023
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We use machine learning to remove biases in TROPOMI satellite observations of atmospheric methane, with GOSAT observations serving as a reference. We find that the TROPOMI biases relative to GOSAT are related to the presence of aerosols and clouds, the surface brightness, and the specific detector that makes the observation aboard TROPOMI. The resulting blended TROPOMI+GOSAT product is more reliable for quantifying methane emissions.
Kevin J. Nihill, Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Bin Yuan, Jordan E. Krechmer, Kanako Sekimoto, Jose L. Jimenez, Joost de Gouw, Christopher D. Cappa, Colette L. Heald, Carsten Warneke, and Jesse H. Kroll
Atmos. Chem. Phys., 23, 7887–7899, https://doi.org/10.5194/acp-23-7887-2023, https://doi.org/10.5194/acp-23-7887-2023, 2023
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In this work, we collect emissions from controlled burns of biomass fuels that can be found in the western United States into an environmental chamber in order to simulate their oxidation as they pass through the atmosphere. These findings provide a detailed characterization of the composition of the atmosphere downwind of wildfires. In turn, this will help to explore the effects of these changing emissions on downwind populations and will also directly inform atmospheric and climate models.
Daniel J. Varon, Daniel J. Jacob, Benjamin Hmiel, Ritesh Gautam, David R. Lyon, Mark Omara, Melissa Sulprizio, Lu Shen, Drew Pendergrass, Hannah Nesser, Zhen Qu, Zachary R. Barkley, Natasha L. Miles, Scott J. Richardson, Kenneth J. Davis, Sudhanshu Pandey, Xiao Lu, Alba Lorente, Tobias Borsdorff, Joannes D. Maasakkers, and Ilse Aben
Atmos. Chem. Phys., 23, 7503–7520, https://doi.org/10.5194/acp-23-7503-2023, https://doi.org/10.5194/acp-23-7503-2023, 2023
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We use TROPOMI satellite observations to quantify weekly methane emissions from the US Permian oil and gas basin from May 2018 to October 2020. We find that Permian emissions are highly variable, with diverse economic and activity drivers. The most important drivers during our study period were new well development and natural gas price. Permian methane intensity averaged 4.6 % and decreased by 1 % per year.
Daniel C. Anderson, Bryan N. Duncan, Julie M. Nicely, Junhua Liu, Sarah A. Strode, and Melanie B. Follette-Cook
Atmos. Chem. Phys., 23, 6319–6338, https://doi.org/10.5194/acp-23-6319-2023, https://doi.org/10.5194/acp-23-6319-2023, 2023
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We describe a methodology that combines machine learning, satellite observations, and 3D chemical model output to infer the abundance of the hydroxyl radical (OH), a chemical that removes many trace gases from the atmosphere. The methodology successfully captures the variability of observed OH, although further observations are needed to evaluate absolute accuracy. Current satellite observations are of sufficient quality to infer OH, but retrieval validation in the remote tropics is needed.
Ruijun Dang, Daniel J. Jacob, Viral Shah, Sebastian D. Eastham, Thibaud M. Fritz, Loretta J. Mickley, Tianjia Liu, Yi Wang, and Jun Wang
Atmos. Chem. Phys., 23, 6271–6284, https://doi.org/10.5194/acp-23-6271-2023, https://doi.org/10.5194/acp-23-6271-2023, 2023
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We use the GEOS-Chem model to better understand the magnitude and trend in free tropospheric NO2 over the contiguous US. Model underestimate of background NO2 is largely corrected by considering aerosol nitrate photolysis. Increase in aircraft emissions affects satellite retrievals by altering the NO2 shape factor, and this effect is expected to increase in future. We show the importance of properly accounting for the free tropospheric background in interpreting NO2 observations from space.
Zichong Chen, Daniel J. Jacob, Ritesh Gautam, Mark Omara, Robert N. Stavins, Robert C. Stowe, Hannah Nesser, Melissa P. Sulprizio, Alba Lorente, Daniel J. Varon, Xiao Lu, Lu Shen, Zhen Qu, Drew C. Pendergrass, and Sarah Hancock
Atmos. Chem. Phys., 23, 5945–5967, https://doi.org/10.5194/acp-23-5945-2023, https://doi.org/10.5194/acp-23-5945-2023, 2023
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We quantify methane emissions from individual countries in the Middle East and North Africa by inverse analysis of 2019 TROPOMI satellite observations of atmospheric methane. We show that the ability to simply relate oil/gas emissions to activity metrics is compromised by stochastic nature of local infrastructure and management practices. We find that the industry target for oil/gas methane intensity is achievable through associated gas capture, modern infrastructure, and centralized operations.
Haihui Zhu, Randall V. Martin, Betty Croft, Shixian Zhai, Chi Li, Liam Bindle, Jeffrey R. Pierce, Rachel Y.-W. Chang, Bruce E. Anderson, Luke D. Ziemba, Johnathan W. Hair, Richard A. Ferrare, Chris A. Hostetler, Inderjeet Singh, Deepangsu Chatterjee, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jack E. Dibb, Joshua S. Schwarz, and Andrew Weinheimer
Atmos. Chem. Phys., 23, 5023–5042, https://doi.org/10.5194/acp-23-5023-2023, https://doi.org/10.5194/acp-23-5023-2023, 2023
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Particle size of atmospheric aerosol is important for estimating its climate and health effects, but simulating atmospheric aerosol size is computationally demanding. This study derives a simple parameterization of the size of organic and secondary inorganic ambient aerosol that can be applied to atmospheric models. Applying this parameterization allows a better representation of the global spatial pattern of aerosol size, as verified by ground and airborne measurements.
Shixian Zhai, Daniel J. Jacob, Drew C. Pendergrass, Nadia K. Colombi, Viral Shah, Laura Hyesung Yang, Qiang Zhang, Shuxiao Wang, Hwajin Kim, Yele Sun, Jin-Soo Choi, Jin-Soo Park, Gan Luo, Fangqun Yu, Jung-Hun Woo, Younha Kim, Jack E. Dibb, Taehyoung Lee, Jin-Seok Han, Bruce E. Anderson, Ke Li, and Hong Liao
Atmos. Chem. Phys., 23, 4271–4281, https://doi.org/10.5194/acp-23-4271-2023, https://doi.org/10.5194/acp-23-4271-2023, 2023
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Anthropogenic fugitive dust in East Asia not only causes severe coarse particulate matter air pollution problems, but also affects fine particulate nitrate. Due to emission control efforts, coarse PM decreased steadily. We find that the decrease of coarse PM is a major driver for a lack of decrease of fine particulate nitrate, as it allows more nitric acid to form fine particulate nitrate. The continuing decrease of coarse PM requires more stringent ammonia and nitrogen oxides emission controls.
Nadia K. Colombi, Daniel J. Jacob, Laura Hyesung Yang, Shixian Zhai, Viral Shah, Stuart K. Grange, Robert M. Yantosca, Soontae Kim, and Hong Liao
Atmos. Chem. Phys., 23, 4031–4044, https://doi.org/10.5194/acp-23-4031-2023, https://doi.org/10.5194/acp-23-4031-2023, 2023
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Surface ozone, detrimental to human and ecosystem health, is very high and increasing in South Korea. Using a global model of the atmosphere, we found that emissions from South Korea and China contribute equally to the high ozone observed. We found that in the absence of all anthropogenic emissions over East Asia, ozone is still very high, implying that the air quality standard in South Korea is not practically achievable unless this background external to East Asia can be decreased.
Chi Li, Randall V. Martin, Ronald C. Cohen, Liam Bindle, Dandan Zhang, Deepangsu Chatterjee, Hongjian Weng, and Jintai Lin
Atmos. Chem. Phys., 23, 3031–3049, https://doi.org/10.5194/acp-23-3031-2023, https://doi.org/10.5194/acp-23-3031-2023, 2023
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Models are essential to diagnose the significant effects of nitrogen oxides (NOx) on air pollution. We use an air quality model to illustrate the variability of NOx resolution-dependent simulation biases; how these biases depend on specific chemical environments, driving mechanisms, and vertical variabilities; and how these biases affect the interpretation of satellite observations. High-resolution simulations are thus critical to accurately interpret NOx and its relevance to air quality.
Laura Hyesung Yang, Daniel J. Jacob, Nadia K. Colombi, Shixian Zhai, Kelvin H. Bates, Viral Shah, Ellie Beaudry, Robert M. Yantosca, Haipeng Lin, Jared F. Brewer, Heesung Chong, Katherine R. Travis, James H. Crawford, Lok N. Lamsal, Ja-Ho Koo, and Jhoon Kim
Atmos. Chem. Phys., 23, 2465–2481, https://doi.org/10.5194/acp-23-2465-2023, https://doi.org/10.5194/acp-23-2465-2023, 2023
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A geostationary satellite can now provide hourly NO2 vertical columns, and obtaining the NO2 vertical columns from space relies on NO2 vertical distribution from the chemical transport model (CTM). In this work, we update the CTM to better represent the chemistry environment so that the CTM can accurately provide NO2 vertical distribution. We also find that the changes in NO2 vertical distribution driven by a change in mixing depth play an important role in the NO2 column's diurnal variation.
Laura Tomsche, Felix Piel, Tomas Mikoviny, Claus J. Nielsen, Hongyu Guo, Pedro Campuzano-Jost, Benjamin A. Nault, Melinda K. Schueneman, Jose L. Jimenez, Hannah Halliday, Glenn Diskin, Joshua P. DiGangi, John B. Nowak, Elizabeth B. Wiggins, Emily Gargulinski, Amber J. Soja, and Armin Wisthaler
Atmos. Chem. Phys., 23, 2331–2343, https://doi.org/10.5194/acp-23-2331-2023, https://doi.org/10.5194/acp-23-2331-2023, 2023
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Ammonia (NH3) is an important trace gas in the atmosphere and fires are among the poorly investigated sources. During the 2019 Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) aircraft campaign, we measured gaseous NH3 and particulate ammonium (NH4+) in smoke plumes emitted from 6 wildfires in the Western US and 66 small agricultural fires in the Southeastern US. We herein present a comprehensive set of emission factors of NH3 and NHx, where NHx = NH3 + NH4+.
Amir H. Souri, Matthew S. Johnson, Glenn M. Wolfe, James H. Crawford, Alan Fried, Armin Wisthaler, William H. Brune, Donald R. Blake, Andrew J. Weinheimer, Tijl Verhoelst, Steven Compernolle, Gaia Pinardi, Corinne Vigouroux, Bavo Langerock, Sungyeon Choi, Lok Lamsal, Lei Zhu, Shuai Sun, Ronald C. Cohen, Kyung-Eun Min, Changmin Cho, Sajeev Philip, Xiong Liu, and Kelly Chance
Atmos. Chem. Phys., 23, 1963–1986, https://doi.org/10.5194/acp-23-1963-2023, https://doi.org/10.5194/acp-23-1963-2023, 2023
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We have rigorously characterized different sources of error in satellite-based HCHO / NO2 tropospheric columns, a widely used metric for diagnosing near-surface ozone sensitivity. Specifically, the errors were categorized/quantified into (i) an inherent chemistry error, (ii) the decoupled relationship between columns and the near-surface concentration, (iii) the spatial representativeness error of ground satellite pixels, and (iv) the satellite retrieval errors.
Fangqun Yu, Gan Luo, Arshad Arjunan Nair, Sebastian Eastham, Christina J. Williamson, Agnieszka Kupc, and Charles A. Brock
Atmos. Chem. Phys., 23, 1863–1877, https://doi.org/10.5194/acp-23-1863-2023, https://doi.org/10.5194/acp-23-1863-2023, 2023
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Particle number concentrations and size distributions in the stratosphere are studied through model simulations and comparisons with measurements. The nucleation scheme used in most of the solar geoengineering modeling studies overpredicts the nucleation rates and particle number concentrations in the stratosphere. The model based on updated nucleation schemes captures reasonably well some aspects of particle size distributions but misses some features. The possible reasons are discussed.
Joanna Joiner, Sergey Marchenko, Zachary Fasnacht, Lok Lamsal, Can Li, Alexander Vasilkov, and Nickolay Krotkov
Atmos. Meas. Tech., 16, 481–500, https://doi.org/10.5194/amt-16-481-2023, https://doi.org/10.5194/amt-16-481-2023, 2023
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Nitrogen dioxide (NO2) is an important trace gas for both air quality and climate. NO2 affects satellite ocean color products. A new ocean color instrument – OCI (Ocean Color Instrument) – will be launched in 2024 on a NASA satellite. We show that it will be possible to measure NO2 from OCI even though it was not designed for this. The techniques developed here, based on machine learning, can also be applied to instruments already in space to speed up algorithms and reduce the effects of noise.
John Douros, Henk Eskes, Jos van Geffen, K. Folkert Boersma, Steven Compernolle, Gaia Pinardi, Anne-Marlene Blechschmidt, Vincent-Henri Peuch, Augustin Colette, and Pepijn Veefkind
Geosci. Model Dev., 16, 509–534, https://doi.org/10.5194/gmd-16-509-2023, https://doi.org/10.5194/gmd-16-509-2023, 2023
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We focus on the challenges associated with comparing atmospheric composition models with satellite products such as tropospheric NO2 columns. The aim is to highlight the methodological difficulties and propose sound ways of doing such comparisons. Building on the comparisons, a new satellite product is proposed and made available, which takes advantage of higher-resolution, regional atmospheric modelling to improve estimates of troposheric NO2 columns over Europe.
Cynthia H. Whaley, Kathy S. Law, Jens Liengaard Hjorth, Henrik Skov, Stephen R. Arnold, Joakim Langner, Jakob Boyd Pernov, Garance Bergeron, Ilann Bourgeois, Jesper H. Christensen, Rong-You Chien, Makoto Deushi, Xinyi Dong, Peter Effertz, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Greg Huey, Ulas Im, Rigel Kivi, Louis Marelle, Tatsuo Onishi, Naga Oshima, Irina Petropavlovskikh, Jeff Peischl, David A. Plummer, Luca Pozzoli, Jean-Christophe Raut, Tom Ryerson, Ragnhild Skeie, Sverre Solberg, Manu A. Thomas, Chelsea Thompson, Kostas Tsigaridis, Svetlana Tsyro, Steven T. Turnock, Knut von Salzen, and David W. Tarasick
Atmos. Chem. Phys., 23, 637–661, https://doi.org/10.5194/acp-23-637-2023, https://doi.org/10.5194/acp-23-637-2023, 2023
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This study summarizes recent research on ozone in the Arctic, a sensitive and rapidly warming region. We find that the seasonal cycles of near-surface atmospheric ozone are variable depending on whether they are near the coast, inland, or at high altitude. Several global model simulations were evaluated, and we found that because models lack some of the ozone chemistry that is important for the coastal Arctic locations, they do not accurately simulate ozone there.
Qianqian Zhang, K. Folkert Boersma, Bin Zhao, Henk Eskes, Cuihong Chen, Haotian Zheng, and Xingying Zhang
Atmos. Chem. Phys., 23, 551–563, https://doi.org/10.5194/acp-23-551-2023, https://doi.org/10.5194/acp-23-551-2023, 2023
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We developed an improved superposition column model and used the latest released (v2.3.1) TROPOMI satellite NO2 observations to estimate daily city-scale NOx and CO2 emissions. The results are verified against bottom-up emissions and OCO-2 XCO2 observations. We obtained the day-to-day variation of city NOx and CO2 emissions, allowing policymakers to gain real-time information on spatial–temporal emission patterns and the effectiveness of carbon and nitrogen regulation in urban environments.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven C. Wofsy
Atmos. Chem. Phys., 23, 99–117, https://doi.org/10.5194/acp-23-99-2023, https://doi.org/10.5194/acp-23-99-2023, 2023
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We have prepared a unique and unusual result from the recent ATom aircraft mission: a measurement-based derivation of the production and loss rates of ozone and methane over the ocean basins. These are the key products of chemistry models used in assessments but have thus far lacked observational metrics. It also shows the scales of variability of atmospheric chemical rates and provides a major challenge to the atmospheric models.
Srijana Lama, Sander Houweling, K. Folkert Boersma, Ilse Aben, Hugo A. C. Denier van der Gon, and Maarten C. Krol
Atmos. Chem. Phys., 22, 16053–16071, https://doi.org/10.5194/acp-22-16053-2022, https://doi.org/10.5194/acp-22-16053-2022, 2022
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Hydroxyl radical (OH) is the important chemical species that determines the lifetime of some greenhouse gases and trace gases. OH plays a vital role in air pollution chemistry. OH has a short lifetime and is extremely difficult to measure directly. OH concentrations derived from the chemistry transport model (CTM) have uncertainties of >50 %. Therefore, in this study, OH is derived indirectly using satellite date in urban plumes.
Simone T. Andersen, Beth S. Nelson, Katie A. Read, Shalini Punjabi, Luis Neves, Matthew J. Rowlinson, James Hopkins, Tomás Sherwen, Lisa K. Whalley, James D. Lee, and Lucy J. Carpenter
Atmos. Chem. Phys., 22, 15747–15765, https://doi.org/10.5194/acp-22-15747-2022, https://doi.org/10.5194/acp-22-15747-2022, 2022
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The cycling of NO and NO2 is important to understand to be able to predict O3 concentrations in the atmosphere. We have used long-term measurements from the Cape Verde Atmospheric Observatory together with model outputs to investigate the cycling of nitrogen oxide (NO) and nitrogen dioxide (NO2) in very clean marine air. This study shows that we understand the processes occurring in very clean air, but with small amounts of pollution in the air, known chemistry cannot explain what is observed.
Pamela S. Rickly, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Glenn M. Wolfe, Ryan Bennett, Ilann Bourgeois, John D. Crounse, Jack E. Dibb, Joshua P. DiGangi, Glenn S. Diskin, Maximilian Dollner, Emily M. Gargulinski, Samuel R. Hall, Hannah S. Halliday, Thomas F. Hanisco, Reem A. Hannun, Jin Liao, Richard Moore, Benjamin A. Nault, John B. Nowak, Jeff Peischl, Claire E. Robinson, Thomas Ryerson, Kevin J. Sanchez, Manuel Schöberl, Amber J. Soja, Jason M. St. Clair, Kenneth L. Thornhill, Kirk Ullmann, Paul O. Wennberg, Bernadett Weinzierl, Elizabeth B. Wiggins, Edward L. Winstead, and Andrew W. Rollins
Atmos. Chem. Phys., 22, 15603–15620, https://doi.org/10.5194/acp-22-15603-2022, https://doi.org/10.5194/acp-22-15603-2022, 2022
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Biomass burning sulfur dioxide (SO2) emission factors range from 0.27–1.1 g kg-1 C. Biomass burning SO2 can quickly form sulfate and organosulfur, but these pathways are dependent on liquid water content and pH. Hydroxymethanesulfonate (HMS) appears to be directly emitted from some fire sources but is not the sole contributor to the organosulfur signal. It is shown that HMS and organosulfur chemistry may be an important S(IV) reservoir with the fate dependent on the surrounding conditions.
Helen L. Fitzmaurice and Ronald C. Cohen
Atmos. Chem. Phys., 22, 15403–15411, https://doi.org/10.5194/acp-22-15403-2022, https://doi.org/10.5194/acp-22-15403-2022, 2022
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We develop a novel method for finding heavy-duty vehicle (HDV) emission factors (g PM kg fuel) using regulatory sensor networks and publicly available traffic data. We find that particulate matter emission factors have decreased by a factor of ~ 9 in the past decade in the San Francisco Bay area. Because of the wide availability of similar data sets across the USA and globally, this method could be applied to other settings to understand long-term trends and regional differences in HDV emissions.
Randall V. Martin, Sebastian D. Eastham, Liam Bindle, Elizabeth W. Lundgren, Thomas L. Clune, Christoph A. Keller, William Downs, Dandan Zhang, Robert A. Lucchesi, Melissa P. Sulprizio, Robert M. Yantosca, Yanshun Li, Lucas Estrada, William M. Putman, Benjamin M. Auer, Atanas L. Trayanov, Steven Pawson, and Daniel J. Jacob
Geosci. Model Dev., 15, 8731–8748, https://doi.org/10.5194/gmd-15-8731-2022, https://doi.org/10.5194/gmd-15-8731-2022, 2022
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Atmospheric chemistry models must be able to operate both online as components of Earth system models and offline as standalone models. The widely used GEOS-Chem model operates both online and offline, but the classic offline version is not suitable for massively parallel simulations. We describe a new generation of the offline high-performance GEOS-Chem (GCHP) that enables high-resolution simulations on thousands of cores, including on the cloud, with improved access, performance, and accuracy.
Thibaud M. Fritz, Sebastian D. Eastham, Louisa K. Emmons, Haipeng Lin, Elizabeth W. Lundgren, Steve Goldhaber, Steven R. H. Barrett, and Daniel J. Jacob
Geosci. Model Dev., 15, 8669–8704, https://doi.org/10.5194/gmd-15-8669-2022, https://doi.org/10.5194/gmd-15-8669-2022, 2022
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We bring the state-of-the-science chemistry module GEOS-Chem into the Community Earth System Model (CESM). We show that some known differences between results from GEOS-Chem and CESM's CAM-chem chemistry module may be due to the configuration of model meteorology rather than inherent differences in the model chemistry. This is a significant step towards a truly modular Earth system model and allows two strong but currently separate research communities to benefit from each other's advances.
William F. Swanson, Chris D. Holmes, William R. Simpson, Kaitlyn Confer, Louis Marelle, Jennie L. Thomas, Lyatt Jaeglé, Becky Alexander, Shuting Zhai, Qianjie Chen, Xuan Wang, and Tomás Sherwen
Atmos. Chem. Phys., 22, 14467–14488, https://doi.org/10.5194/acp-22-14467-2022, https://doi.org/10.5194/acp-22-14467-2022, 2022
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Radical bromine molecules are seen at higher concentrations during the Arctic spring. We use the global model GEOS-Chem to test whether snowpack and wind-blown snow sources can explain high bromine concentrations. We run this model for the entire year of 2015 and compare results to observations of bromine from floating platforms on the Arctic Ocean and at Utqiaġvik. We find that the model performs best when both sources are enabled but may overestimate bromine production in summer and fall.
Youhua Tang, Patrick C. Campbell, Pius Lee, Rick Saylor, Fanglin Yang, Barry Baker, Daniel Tong, Ariel Stein, Jianping Huang, Ho-Chun Huang, Li Pan, Jeff McQueen, Ivanka Stajner, Jose Tirado-Delgado, Youngsun Jung, Melissa Yang, Ilann Bourgeois, Jeff Peischl, Tom Ryerson, Donald Blake, Joshua Schwarz, Jose-Luis Jimenez, James Crawford, Glenn Diskin, Richard Moore, Johnathan Hair, Greg Huey, Andrew Rollins, Jack Dibb, and Xiaoyang Zhang
Geosci. Model Dev., 15, 7977–7999, https://doi.org/10.5194/gmd-15-7977-2022, https://doi.org/10.5194/gmd-15-7977-2022, 2022
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This paper compares two meteorological datasets for driving a regional air quality model: a regional meteorological model using WRF (WRF-CMAQ) and direct interpolation from an operational global model (GFS-CMAQ). In the comparison with surface measurements and aircraft data in summer 2019, these two methods show mixed performance depending on the corresponding meteorological settings. Direct interpolation is found to be a viable method to drive air quality models.
Sarah A. Strode, Ghassan Taha, Luke D. Oman, Robert Damadeo, David Flittner, Mark Schoeberl, Christopher E. Sioris, and Ryan Stauffer
Atmos. Meas. Tech., 15, 6145–6161, https://doi.org/10.5194/amt-15-6145-2022, https://doi.org/10.5194/amt-15-6145-2022, 2022
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We use a global atmospheric chemistry model simulation to generate scaling factors that account for the daily cycle of NO2 and ozone. These factors facilitate comparisons between sunrise and sunset observations from SAGE III/ISS and observations from other instruments. We provide the scaling factors as monthly zonal means for different latitudes and altitudes. We find that applying these factors yields more consistent comparisons between observations from SAGE III/ISS and other instruments.
Haolin Wang, Xiao Lu, Daniel J. Jacob, Owen R. Cooper, Kai-Lan Chang, Ke Li, Meng Gao, Yiming Liu, Bosi Sheng, Kai Wu, Tongwen Wu, Jie Zhang, Bastien Sauvage, Philippe Nédélec, Romain Blot, and Shaojia Fan
Atmos. Chem. Phys., 22, 13753–13782, https://doi.org/10.5194/acp-22-13753-2022, https://doi.org/10.5194/acp-22-13753-2022, 2022
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We report significant global tropospheric ozone increases in 1995–2017 based on extensive aircraft and ozonesonde observations. Using GEOS-Chem (Goddard Earth Observing System chemistry model) multi-decadal global simulations, we find that changes in global anthropogenic emissions, in particular the rapid increases in aircraft emissions, contribute significantly to the increases in tropospheric ozone and resulting radiative impact.
William Atkinson, Sebastian D. Eastham, Y.-H. Henry Chen, Jennifer Morris, Sergey Paltsev, C. Adam Schlosser, and Noelle E. Selin
Geosci. Model Dev., 15, 7767–7789, https://doi.org/10.5194/gmd-15-7767-2022, https://doi.org/10.5194/gmd-15-7767-2022, 2022
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Understanding policy effects on human-caused air pollutant emissions is key for assessing related health impacts. We develop a flexible scenario tool that combines updated emissions data sets, long-term economic modeling, and comprehensive technology pathways to clarify the impacts of climate and air quality policies. Results show the importance of both policy levers in the future to prevent long-term emission increases from offsetting near-term air quality improvements from existing policies.
Nicole A. June, Anna L. Hodshire, Elizabeth B. Wiggins, Edward L. Winstead, Claire E. Robinson, K. Lee Thornhill, Kevin J. Sanchez, Richard H. Moore, Demetrios Pagonis, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Matthew M. Coggon, Jonathan M. Dean-Day, T. Paul Bui, Jeff Peischl, Robert J. Yokelson, Matthew J. Alvarado, Sonia M. Kreidenweis, Shantanu H. Jathar, and Jeffrey R. Pierce
Atmos. Chem. Phys., 22, 12803–12825, https://doi.org/10.5194/acp-22-12803-2022, https://doi.org/10.5194/acp-22-12803-2022, 2022
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The evolution of organic aerosol composition and size is uncertain due to variability within and between smoke plumes. We examine the impact of plume concentration on smoke evolution from smoke plumes sampled by the NASA DC-8 during FIREX-AQ. We find that observed organic aerosol and size distribution changes are correlated to plume aerosol mass concentrations. Additionally, coagulation explains the majority of the observed growth.
Therese S. Carter, Colette L. Heald, Jesse H. Kroll, Eric C. Apel, Donald Blake, Matthew Coggon, Achim Edtbauer, Georgios Gkatzelis, Rebecca S. Hornbrook, Jeff Peischl, Eva Y. Pfannerstill, Felix Piel, Nina G. Reijrink, Akima Ringsdorf, Carsten Warneke, Jonathan Williams, Armin Wisthaler, and Lu Xu
Atmos. Chem. Phys., 22, 12093–12111, https://doi.org/10.5194/acp-22-12093-2022, https://doi.org/10.5194/acp-22-12093-2022, 2022
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Fires emit many gases which can contribute to smog and air pollution. However, the amount and properties of these chemicals are not well understood, so this work updates and expands their representation in a global atmospheric model, including by adding new chemicals. We confirm that this updated representation generally matches measurements taken in several fire regions. We then show that fires provide ~15 % of atmospheric reactivity globally and more than 75 % over fire source regions.
Lu Shen, Ritesh Gautam, Mark Omara, Daniel Zavala-Araiza, Joannes D. Maasakkers, Tia R. Scarpelli, Alba Lorente, David Lyon, Jianxiong Sheng, Daniel J. Varon, Hannah Nesser, Zhen Qu, Xiao Lu, Melissa P. Sulprizio, Steven P. Hamburg, and Daniel J. Jacob
Atmos. Chem. Phys., 22, 11203–11215, https://doi.org/10.5194/acp-22-11203-2022, https://doi.org/10.5194/acp-22-11203-2022, 2022
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We use 22 months of TROPOMI satellite observations to quantity methane emissions from the oil (O) and natural gas (G) sector in the US and Canada at the scale of both individual basins as well as country-wide aggregates. We find that O/G-related methane emissions are underestimated in these inventories by 80 % for the US and 40 % for Canada, and 70 % of the underestimate in the US is from five O/G basins, including Permian, Haynesville, Anadarko, Eagle Ford, and Barnett.
Ilann Bourgeois, Jeff Peischl, J. Andrew Neuman, Steven S. Brown, Hannah M. Allen, Pedro Campuzano-Jost, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Jessica B. Gilman, Georgios I. Gkatzelis, Hongyu Guo, Hannah A. Halliday, Thomas F. Hanisco, Christopher D. Holmes, L. Gregory Huey, Jose L. Jimenez, Aaron D. Lamplugh, Young Ro Lee, Jakob Lindaas, Richard H. Moore, Benjamin A. Nault, John B. Nowak, Demetrios Pagonis, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Vanessa Selimovic, Jason M. St. Clair, David Tanner, Krystal T. Vasquez, Patrick R. Veres, Carsten Warneke, Paul O. Wennberg, Rebecca A. Washenfelder, Elizabeth B. Wiggins, Caroline C. Womack, Lu Xu, Kyle J. Zarzana, and Thomas B. Ryerson
Atmos. Meas. Tech., 15, 4901–4930, https://doi.org/10.5194/amt-15-4901-2022, https://doi.org/10.5194/amt-15-4901-2022, 2022
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Understanding fire emission impacts on the atmosphere is key to effective air quality management and requires accurate measurements. We present a comparison of airborne measurements of key atmospheric species in ambient air and in fire smoke. We show that most instruments performed within instrument uncertainties. In some cases, further work is needed to fully characterize instrument performance. Comparing independent measurements using different techniques is important to assess their accuracy.
Shang Liu, Barbara Barletta, Rebecca S. Hornbrook, Alan Fried, Jeff Peischl, Simone Meinardi, Matthew Coggon, Aaron Lamplugh, Jessica B. Gilman, Georgios I. Gkatzelis, Carsten Warneke, Eric C. Apel, Alan J. Hills, Ilann Bourgeois, James Walega, Petter Weibring, Dirk Richter, Toshihiro Kuwayama, Michael FitzGibbon, and Donald Blake
Atmos. Chem. Phys., 22, 10937–10954, https://doi.org/10.5194/acp-22-10937-2022, https://doi.org/10.5194/acp-22-10937-2022, 2022
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California’s ozone persistently exceeds the air quality standards. We studied the spatial distribution of volatile organic compounds (VOCs) that produce ozone over the most polluted regions in California using aircraft measurements. We find that the oxygenated VOCs have the highest ozone formation potential. Spatially, biogenic VOCs are important during high ozone episodes in the South Coast Air Basin, while dairy emissions may be critical for ozone production in San Joaquin Valley.
Zichong Chen, Daniel J. Jacob, Hannah Nesser, Melissa P. Sulprizio, Alba Lorente, Daniel J. Varon, Xiao Lu, Lu Shen, Zhen Qu, Elise Penn, and Xueying Yu
Atmos. Chem. Phys., 22, 10809–10826, https://doi.org/10.5194/acp-22-10809-2022, https://doi.org/10.5194/acp-22-10809-2022, 2022
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We quantify methane emissions in China and contributions from different sectors by inverse analysis of 2019 TROPOMI satellite observations of atmospheric methane. We find that anthropogenic methane emissions for China are underestimated in the national inventory. Our estimate of emissions indicates a small life-cycle loss rate, implying net climate benefits from the current
coal-to-gasenergy transition in China. However, this small loss rate can be misleading given China's high gas imports.
Daniel C. Anderson, Melanie B. Follette-Cook, Sarah A. Strode, Julie M. Nicely, Junhua Liu, Peter D. Ivatt, and Bryan N. Duncan
Geosci. Model Dev., 15, 6341–6358, https://doi.org/10.5194/gmd-15-6341-2022, https://doi.org/10.5194/gmd-15-6341-2022, 2022
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The hydroxyl radical (OH) is the most important chemical in the atmosphere for removing certain pollutants, including methane, the second-most-important greenhouse gas. We present a methodology to create an easily modifiable parameterization that can calculate OH concentrations in a computationally efficient way. The parameterization, which predicts OH within 5 %, can be integrated into larger climate models to allow for calculation of the interactions between OH, methane, and other chemicals.
Aditya Kumar, R. Bradley Pierce, Ravan Ahmadov, Gabriel Pereira, Saulo Freitas, Georg Grell, Chris Schmidt, Allen Lenzen, Joshua P. Schwarz, Anne E. Perring, Joseph M. Katich, John Hair, Jose L. Jimenez, Pedro Campuzano-Jost, and Hongyu Guo
Atmos. Chem. Phys., 22, 10195–10219, https://doi.org/10.5194/acp-22-10195-2022, https://doi.org/10.5194/acp-22-10195-2022, 2022
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We use the WRF-Chem model with new implementations of GOES-16 wildfire emissions and plume rise based on fire radiative power (FRP) to interpret aerosol observations during the 2019 NASA–NOAA FIREX-AQ field campaign and perform model evaluations. The model shows significant improvements in simulating the variety of aerosol loading environments sampled during FIREX-AQ. Our results also highlight the importance of accurate wildfire diurnal cycle and aerosol chemical mechanisms in models.
Aaron Pearlman, Monica Cook, Boryana Efremova, Francis Padula, Lok Lamsal, Joel McCorkel, and Joanna Joiner
Atmos. Meas. Tech., 15, 4489–4501, https://doi.org/10.5194/amt-15-4489-2022, https://doi.org/10.5194/amt-15-4489-2022, 2022
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NOAA’s Geostationary Extended Observations (GeoXO) constellation is planned to consist of an atmospheric composition instrument (ACX) to support air quality forecasting and monitoring. As design trade-offs are being studied, we investigated one parameter, the polarization sensitivity, which has yet to be fully documented for NO2 retrievals. Our simulation study explores these impacts to inform the ACX’s development and better understand polarization’s role in trace gas retrievals.
Daniel J. Jacob, Daniel J. Varon, Daniel H. Cusworth, Philip E. Dennison, Christian Frankenberg, Ritesh Gautam, Luis Guanter, John Kelley, Jason McKeever, Lesley E. Ott, Benjamin Poulter, Zhen Qu, Andrew K. Thorpe, John R. Worden, and Riley M. Duren
Atmos. Chem. Phys., 22, 9617–9646, https://doi.org/10.5194/acp-22-9617-2022, https://doi.org/10.5194/acp-22-9617-2022, 2022
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We review the capability of satellite observations of atmospheric methane to quantify methane emissions on all scales. We cover retrieval methods, precision requirements, inverse methods for inferring emissions, source detection thresholds, and observations of system completeness. We show that current instruments already enable quantification of regional and national emissions including contributions from large point sources. Coverage and resolution will increase significantly in coming years.
Daniel J. Varon, Daniel J. Jacob, Melissa Sulprizio, Lucas A. Estrada, William B. Downs, Lu Shen, Sarah E. Hancock, Hannah Nesser, Zhen Qu, Elise Penn, Zichong Chen, Xiao Lu, Alba Lorente, Ashutosh Tewari, and Cynthia A. Randles
Geosci. Model Dev., 15, 5787–5805, https://doi.org/10.5194/gmd-15-5787-2022, https://doi.org/10.5194/gmd-15-5787-2022, 2022
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Reducing atmospheric methane emissions is critical to slow near-term climate change. Globally surveying satellite instruments like the TROPOspheric Monitoring Instrument (TROPOMI) have unique capabilities for monitoring atmospheric methane around the world. Here we present a user-friendly cloud-computing tool that enables researchers and stakeholders to quantify methane emissions across user-selected regions of interest using TROPOMI satellite observations.
Linghan Zeng, Jack Dibb, Eric Scheuer, Joseph M. Katich, Joshua P. Schwarz, Ilann Bourgeois, Jeff Peischl, Tom Ryerson, Carsten Warneke, Anne E. Perring, Glenn S. Diskin, Joshua P. DiGangi, John B. Nowak, Richard H. Moore, Elizabeth B. Wiggins, Demetrios Pagonis, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Lu Xu, and Rodney J. Weber
Atmos. Chem. Phys., 22, 8009–8036, https://doi.org/10.5194/acp-22-8009-2022, https://doi.org/10.5194/acp-22-8009-2022, 2022
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Wildfires emit aerosol particles containing brown carbon material that affects visibility and global climate and is toxic. Brown carbon is poorly characterized due to measurement limitations, and its evolution in the atmosphere is not well known. We report on aircraft measurements of brown carbon from large wildfires in the western United States. We compare two methods for measuring brown carbon and study the evolution of brown carbon in the smoke as it moved away from the burning regions.
Katherine R. Travis, James H. Crawford, Gao Chen, Carolyn E. Jordan, Benjamin A. Nault, Hwajin Kim, Jose L. Jimenez, Pedro Campuzano-Jost, Jack E. Dibb, Jung-Hun Woo, Younha Kim, Shixian Zhai, Xuan Wang, Erin E. McDuffie, Gan Luo, Fangqun Yu, Saewung Kim, Isobel J. Simpson, Donald R. Blake, Limseok Chang, and Michelle J. Kim
Atmos. Chem. Phys., 22, 7933–7958, https://doi.org/10.5194/acp-22-7933-2022, https://doi.org/10.5194/acp-22-7933-2022, 2022
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The 2016 Korea–United States Air Quality (KORUS-AQ) field campaign provided a unique set of observations to improve our understanding of PM2.5 pollution in South Korea. Models typically have errors in simulating PM2.5 in this region, which is of concern for the development of control measures. We use KORUS-AQ observations to improve our understanding of the mechanisms driving PM2.5 and the implications of model errors for determining PM2.5 that is attributable to local or foreign sources.
John R. Worden, Daniel H. Cusworth, Zhen Qu, Yi Yin, Yuzhong Zhang, A. Anthony Bloom, Shuang Ma, Brendan K. Byrne, Tia Scarpelli, Joannes D. Maasakkers, David Crisp, Riley Duren, and Daniel J. Jacob
Atmos. Chem. Phys., 22, 6811–6841, https://doi.org/10.5194/acp-22-6811-2022, https://doi.org/10.5194/acp-22-6811-2022, 2022
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This paper is intended to accomplish two goals: 1) describe a new algorithm by which remotely sensed measurements of methane or other tracers can be used to not just quantify methane fluxes, but also attribute these fluxes to specific sources and regions and characterize their uncertainties, and 2) use this new algorithm to provide methane emissions by sector and country in support of the global stock take.
Hannah Walker, Daniel Stone, Trevor Ingham, Sina Hackenberg, Danny Cryer, Shalini Punjabi, Katie Read, James Lee, Lisa Whalley, Dominick V. Spracklen, Lucy J. Carpenter, Steve R. Arnold, and Dwayne E. Heard
Atmos. Chem. Phys., 22, 5535–5557, https://doi.org/10.5194/acp-22-5535-2022, https://doi.org/10.5194/acp-22-5535-2022, 2022
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Glyoxal is a ubiquitous reactive organic compound in the atmosphere, which may form organic aerosol and impact the atmosphere's oxidising capacity. There are limited measurements of glyoxal's abundance in the remote marine atmosphere. We made new measurements of glyoxal using a highly sensitive technique over two 4-week periods in the tropical Atlantic atmosphere. We show that daytime measurements are mostly consistent with our chemical understanding but a potential missing source at night.
Pinya Wang, Yang Yang, Huimin Li, Lei Chen, Ruijun Dang, Daokai Xue, Baojie Li, Jianping Tang, L. Ruby Leung, and Hong Liao
Atmos. Chem. Phys., 22, 4705–4719, https://doi.org/10.5194/acp-22-4705-2022, https://doi.org/10.5194/acp-22-4705-2022, 2022
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China is now suffering from both severe ozone (O3) pollution and heat events. We highlight that North China Plain is the hot spot of the co-occurrences of extremes in O3 and high temperatures in China. Such coupled extremes exhibit an increasing trend during 2014–2019 and will continue to increase until the middle of this century. And the coupled extremes impose more severe health impacts to human than O3 pollution occurring alone because of elevated O3 levels and temperatures.
Jos van Geffen, Henk Eskes, Steven Compernolle, Gaia Pinardi, Tijl Verhoelst, Jean-Christopher Lambert, Maarten Sneep, Mark ter Linden, Antje Ludewig, K. Folkert Boersma, and J. Pepijn Veefkind
Atmos. Meas. Tech., 15, 2037–2060, https://doi.org/10.5194/amt-15-2037-2022, https://doi.org/10.5194/amt-15-2037-2022, 2022
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Nitrogen dioxide (NO2) is one of the main data products measured by the Tropospheric Monitoring Instrument (TROPOMI) on the Sentinel-5 Precursor (S5P) satellite. This study describes improvements in the TROPOMI NO2 retrieval leading to version v2.2, operational since 1 July 2021. It compares results with previous versions v1.2–v1.4 and with Ozone Monitoring Instrument (OMI) and ground-based measurements.
Glenn M. Wolfe, Thomas F. Hanisco, Heather L. Arkinson, Donald R. Blake, Armin Wisthaler, Tomas Mikoviny, Thomas B. Ryerson, Ilana Pollack, Jeff Peischl, Paul O. Wennberg, John D. Crounse, Jason M. St. Clair, Alex Teng, L. Gregory Huey, Xiaoxi Liu, Alan Fried, Petter Weibring, Dirk Richter, James Walega, Samuel R. Hall, Kirk Ullmann, Jose L. Jimenez, Pedro Campuzano-Jost, T. Paul Bui, Glenn Diskin, James R. Podolske, Glen Sachse, and Ronald C. Cohen
Atmos. Chem. Phys., 22, 4253–4275, https://doi.org/10.5194/acp-22-4253-2022, https://doi.org/10.5194/acp-22-4253-2022, 2022
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Smoke plumes are chemically complex. This work combines airborne observations of smoke plume composition with a photochemical model to probe the production of ozone and the fate of reactive gases in the outflow of a large wildfire. Model–measurement comparisons illustrate how uncertain emissions and chemical processes propagate into simulated chemical evolution. Results provide insight into how this system responds to perturbations, which can help guide future observation and modeling efforts.
Helen L. Fitzmaurice, Alexander J. Turner, Jinsol Kim, Katherine Chan, Erin R. Delaria, Catherine Newman, Paul Wooldridge, and Ronald C. Cohen
Atmos. Chem. Phys., 22, 3891–3900, https://doi.org/10.5194/acp-22-3891-2022, https://doi.org/10.5194/acp-22-3891-2022, 2022
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On-road emissions are thought to vary widely from existing predictions, as the effects of the age of the vehicle fleet, the performance of emission control systems, and variations in speed are difficult to assess under ambient driving conditions. We present an observational approach to characterize on-road emissions and show that the method is consistent with other approaches to within ~ 3 %.
Meloë S. F. Kacenelenbogen, Qian Tan, Sharon P. Burton, Otto P. Hasekamp, Karl D. Froyd, Yohei Shinozuka, Andreas J. Beyersdorf, Luke Ziemba, Kenneth L. Thornhill, Jack E. Dibb, Taylor Shingler, Armin Sorooshian, Reed W. Espinosa, Vanderlei Martins, Jose L. Jimenez, Pedro Campuzano-Jost, Joshua P. Schwarz, Matthew S. Johnson, Jens Redemann, and Gregory L. Schuster
Atmos. Chem. Phys., 22, 3713–3742, https://doi.org/10.5194/acp-22-3713-2022, https://doi.org/10.5194/acp-22-3713-2022, 2022
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The impact of aerosols on Earth's radiation budget and human health is important and strongly depends on their composition. One desire of our scientific community is to derive the composition of the aerosol from satellite sensors. However, satellites observe aerosol optical properties (and not aerosol composition) based on remote sensing instrumentation. This study assesses how much aerosol optical properties can tell us about aerosol composition.
Tobias Christoph Valentin Werner Riess, Klaas Folkert Boersma, Jasper van Vliet, Wouter Peters, Maarten Sneep, Henk Eskes, and Jos van Geffen
Atmos. Meas. Tech., 15, 1415–1438, https://doi.org/10.5194/amt-15-1415-2022, https://doi.org/10.5194/amt-15-1415-2022, 2022
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This paper reports on improved monitoring of ship nitrogen oxide emissions by TROPOMI. With its fantastic resolution we can identify lanes of ship nitrogen dioxide (NO2) pollution not detected from space before. The quality of TROPOMI NO2 data over sea is improved further by recent upgrades in cloud retrievals and the use of sun glint scenes. Lastly, we study the impact of COVID-19 on ship NO2 in European seas and compare the found reductions to emission estimates gained from ship-specific data.
Tia R. Scarpelli, Daniel J. Jacob, Shayna Grossman, Xiao Lu, Zhen Qu, Melissa P. Sulprizio, Yuzhong Zhang, Frances Reuland, Deborah Gordon, and John R. Worden
Atmos. Chem. Phys., 22, 3235–3249, https://doi.org/10.5194/acp-22-3235-2022, https://doi.org/10.5194/acp-22-3235-2022, 2022
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We present a spatially explicit version of the national inventories of oil, gas, and coal methane emissions as submitted by individual countries to the United Nations Framework Convention on Climate Change (UNFCCC) in 2021. We then use atmospheric modeling to compare our inventory emissions to atmospheric methane observations with the goal of identifying potential under- and overestimates of oil–gas methane emissions in the national inventories.
Drew C. Pendergrass, Shixian Zhai, Jhoon Kim, Ja-Ho Koo, Seoyoung Lee, Minah Bae, Soontae Kim, Hong Liao, and Daniel J. Jacob
Atmos. Meas. Tech., 15, 1075–1091, https://doi.org/10.5194/amt-15-1075-2022, https://doi.org/10.5194/amt-15-1075-2022, 2022
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This paper uses a machine learning algorithm to infer high-resolution maps of particulate air quality in eastern China, Japan, and the Korean peninsula, using data from a geostationary satellite along with meteorology. We then perform an extensive evaluation of this inferred air quality and use it to diagnose trends in the region. We hope this paper and the associated data will be valuable to other scientists interested in epidemiology, air quality, remote sensing, and machine learning.
Lu Shen, Daniel J. Jacob, Mauricio Santillana, Kelvin Bates, Jiawei Zhuang, and Wei Chen
Geosci. Model Dev., 15, 1677–1687, https://doi.org/10.5194/gmd-15-1677-2022, https://doi.org/10.5194/gmd-15-1677-2022, 2022
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The high computational cost of chemical integration is a long-standing limitation in global atmospheric chemistry models. Here we present an adaptive and efficient algorithm that can reduce the computational time of atmospheric chemistry by 50 % and maintain the error below 2 % for important species, inspired by machine learning clustering techniques and traditional asymptotic analysis ideas.
Andrew O. Langford, Christoph J. Senff, Raul J. Alvarez II, Ken C. Aikin, Sunil Baidar, Timothy A. Bonin, W. Alan Brewer, Jerome Brioude, Steven S. Brown, Joel D. Burley, Dani J. Caputi, Stephen A. Conley, Patrick D. Cullis, Zachary C. J. Decker, Stéphanie Evan, Guillaume Kirgis, Meiyun Lin, Mariusz Pagowski, Jeff Peischl, Irina Petropavlovskikh, R. Bradley Pierce, Thomas B. Ryerson, Scott P. Sandberg, Chance W. Sterling, Ann M. Weickmann, and Li Zhang
Atmos. Chem. Phys., 22, 1707–1737, https://doi.org/10.5194/acp-22-1707-2022, https://doi.org/10.5194/acp-22-1707-2022, 2022
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The Fires, Asian, and Stratospheric Transport–Las Vegas Ozone Study (FAST-LVOS) combined lidar, aircraft, and in situ measurements with global models to investigate the contributions of stratospheric intrusions, regional and Asian pollution, and wildfires to background ozone in the southwestern US during May and June 2017 and demonstrated that these processes contributed to background ozone levels that exceeded 70 % of the US National Ambient Air Quality Standard during the 6-week campaign.
Ka Ming Fung, Colette L. Heald, Jesse H. Kroll, Siyuan Wang, Duseong S. Jo, Andrew Gettelman, Zheng Lu, Xiaohong Liu, Rahul A. Zaveri, Eric C. Apel, Donald R. Blake, Jose-Luis Jimenez, Pedro Campuzano-Jost, Patrick R. Veres, Timothy S. Bates, John E. Shilling, and Maria Zawadowicz
Atmos. Chem. Phys., 22, 1549–1573, https://doi.org/10.5194/acp-22-1549-2022, https://doi.org/10.5194/acp-22-1549-2022, 2022
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Understanding the natural aerosol burden in the preindustrial era is crucial for us to assess how atmospheric aerosols affect the Earth's radiative budgets. Our study explores how a detailed description of dimethyl sulfide (DMS) oxidation (implemented in the Community Atmospheric Model version 6 with chemistry, CAM6-chem) could help us better estimate the present-day and preindustrial concentrations of sulfate and other relevant chemicals, as well as the resulting aerosol radiative impacts.
Douglas A. Day, Pedro Campuzano-Jost, Benjamin A. Nault, Brett B. Palm, Weiwei Hu, Hongyu Guo, Paul J. Wooldridge, Ronald C. Cohen, Kenneth S. Docherty, J. Alex Huffman, Suzane S. de Sá, Scot T. Martin, and Jose L. Jimenez
Atmos. Meas. Tech., 15, 459–483, https://doi.org/10.5194/amt-15-459-2022, https://doi.org/10.5194/amt-15-459-2022, 2022
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Particle-phase nitrates are an important component of atmospheric aerosols and chemistry. In this paper, we systematically explore the application of aerosol mass spectrometry (AMS) to quantify the organic and inorganic nitrate fractions of aerosols in the atmosphere. While AMS has been used for a decade to quantify nitrates, methods are not standardized. We make recommendations for a more universal approach based on this analysis of a large range of field and laboratory observations.
Dongwook Kim, Changmin Cho, Seokhan Jeong, Soojin Lee, Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Jason C. Schroder, Jose L. Jimenez, Rainer Volkamer, Donald R. Blake, Armin Wisthaler, Alan Fried, Joshua P. DiGangi, Glenn S. Diskin, Sally E. Pusede, Samuel R. Hall, Kirk Ullmann, L. Gregory Huey, David J. Tanner, Jack Dibb, Christoph J. Knote, and Kyung-Eun Min
Atmos. Chem. Phys., 22, 805–821, https://doi.org/10.5194/acp-22-805-2022, https://doi.org/10.5194/acp-22-805-2022, 2022
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CHOCHO was simulated using a 0-D box model constrained by measurements during the KORUS-AQ mission. CHOCHO concentration was high in large cities, aromatics being the most important precursors. Loss path to aerosol was the highest sink, contributing to ~ 20 % of secondary organic aerosol formation. Our work highlights that simple CHOCHO surface uptake approach is valid only for low aerosol conditions and more work is required to understand CHOCHO solubility in high-aerosol conditions.
Xiao Lu, Daniel J. Jacob, Haolin Wang, Joannes D. Maasakkers, Yuzhong Zhang, Tia R. Scarpelli, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Hannah Nesser, A. Anthony Bloom, Shuang Ma, John R. Worden, Shaojia Fan, Robert J. Parker, Hartmut Boesch, Ritesh Gautam, Deborah Gordon, Michael D. Moran, Frances Reuland, Claudia A. Octaviano Villasana, and Arlyn Andrews
Atmos. Chem. Phys., 22, 395–418, https://doi.org/10.5194/acp-22-395-2022, https://doi.org/10.5194/acp-22-395-2022, 2022
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We evaluate methane emissions and trends for 2010–2017 in the gridded national emission inventories for the United States, Canada, and Mexico by inversion of in situ and satellite methane observations. We find that anthropogenic methane emissions for all three countries are underestimated in the national inventories, largely driven by oil emissions. Anthropogenic methane emissions in the US peak in 2014, in contrast to the report of a steadily decreasing trend over 2010–2017 from the US EPA.
Alexander J. Turner, Philipp Köhler, Troy S. Magney, Christian Frankenberg, Inez Fung, and Ronald C. Cohen
Biogeosciences, 18, 6579–6588, https://doi.org/10.5194/bg-18-6579-2021, https://doi.org/10.5194/bg-18-6579-2021, 2021
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This work builds a high-resolution estimate (500 m) of gross primary productivity (GPP) over the US using satellite measurements of solar-induced chlorophyll fluorescence (SIF) from the TROPOspheric Monitoring Instrument (TROPOMI) between 2018 and 2020. We identify ecosystem-specific scaling factors for estimating gross primary productivity (GPP) from TROPOMI SIF. Extreme precipitation events drive four regional GPP anomalies that account for 28 % of year-to-year GPP differences across the US.
Debora Griffin, Chris A. McLinden, Enrico Dammers, Cristen Adams, Chelsea E. Stockwell, Carsten Warneke, Ilann Bourgeois, Jeff Peischl, Thomas B. Ryerson, Kyle J. Zarzana, Jake P. Rowe, Rainer Volkamer, Christoph Knote, Natalie Kille, Theodore K. Koenig, Christopher F. Lee, Drew Rollins, Pamela S. Rickly, Jack Chen, Lukas Fehr, Adam Bourassa, Doug Degenstein, Katherine Hayden, Cristian Mihele, Sumi N. Wren, John Liggio, Ayodeji Akingunola, and Paul Makar
Atmos. Meas. Tech., 14, 7929–7957, https://doi.org/10.5194/amt-14-7929-2021, https://doi.org/10.5194/amt-14-7929-2021, 2021
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Satellite-derived NOx emissions from biomass burning are estimated with TROPOMI observations. Two common emission estimation methods are applied, and sensitivity tests with model output were performed to determine the accuracy of these methods. The effect of smoke aerosols on TROPOMI NO2 columns is estimated and compared to aircraft observations from four different aircraft campaigns measuring biomass burning plumes in 2018 and 2019 in North America.
Jin Liao, Glenn M. Wolfe, Reem A. Hannun, Jason M. St. Clair, Thomas F. Hanisco, Jessica B. Gilman, Aaron Lamplugh, Vanessa Selimovic, Glenn S. Diskin, John B. Nowak, Hannah S. Halliday, Joshua P. DiGangi, Samuel R. Hall, Kirk Ullmann, Christopher D. Holmes, Charles H. Fite, Anxhelo Agastra, Thomas B. Ryerson, Jeff Peischl, Ilann Bourgeois, Carsten Warneke, Matthew M. Coggon, Georgios I. Gkatzelis, Kanako Sekimoto, Alan Fried, Dirk Richter, Petter Weibring, Eric C. Apel, Rebecca S. Hornbrook, Steven S. Brown, Caroline C. Womack, Michael A. Robinson, Rebecca A. Washenfelder, Patrick R. Veres, and J. Andrew Neuman
Atmos. Chem. Phys., 21, 18319–18331, https://doi.org/10.5194/acp-21-18319-2021, https://doi.org/10.5194/acp-21-18319-2021, 2021
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Formaldehyde (HCHO) is an important oxidant precursor and affects the formation of O3 and other secondary pollutants in wildfire plumes. We disentangle the processes controlling HCHO evolution from wildfire plumes sampled by NASA DC-8 during FIREX-AQ. We find that OH abundance rather than normalized OH reactivity is the main driver of fire-to-fire variability in HCHO secondary production and estimate an effective HCHO yield per volatile organic compound molecule oxidized in wildfire plumes.
Kelvin H. Bates, Daniel J. Jacob, Ke Li, Peter D. Ivatt, Mat J. Evans, Yingying Yan, and Jintai Lin
Atmos. Chem. Phys., 21, 18351–18374, https://doi.org/10.5194/acp-21-18351-2021, https://doi.org/10.5194/acp-21-18351-2021, 2021
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Simple aromatic compounds (benzene, toluene, xylene) have complex gas-phase chemistry that is inconsistently represented in atmospheric models. We compile recent experimental and theoretical insights to develop a new mechanism for gas-phase aromatic oxidation that is sufficiently compact for use in multiscale models. We compare our new mechanism to chamber experiments and other mechanisms, and implement it in a global model to quantify the impacts of aromatic oxidation on tropospheric chemistry.
Auke J. Visser, Laurens N. Ganzeveld, Ignacio Goded, Maarten C. Krol, Ivan Mammarella, Giovanni Manca, and K. Folkert Boersma
Atmos. Chem. Phys., 21, 18393–18411, https://doi.org/10.5194/acp-21-18393-2021, https://doi.org/10.5194/acp-21-18393-2021, 2021
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Dry deposition is an important sink for tropospheric ozone that affects ecosystem carbon uptake, but process understanding remains incomplete. We apply a common deposition representation in atmospheric chemistry models and a multi-layer canopy model to multi-year ozone deposition observations. The multi-layer canopy model performs better on diurnal timescales compared to the common approach, leading to a substantially improved simulation of ozone deposition and vegetation ozone impact metrics.
Leigh R. Crilley, Louisa J. Kramer, Francis D. Pope, Chris Reed, James D. Lee, Lucy J. Carpenter, Lloyd D. J. Hollis, Stephen M. Ball, and William J. Bloss
Atmos. Chem. Phys., 21, 18213–18225, https://doi.org/10.5194/acp-21-18213-2021, https://doi.org/10.5194/acp-21-18213-2021, 2021
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Nitrous acid (HONO) is a key source of atmospheric oxidants. We evaluate if the ocean surface is a source of HONO for the marine boundary layer, using measurements from two contrasting coastal locations. We observed no evidence for a night-time ocean surface source, in contrast to previous work. This points to significant geographical variation in the predominant HONO formation mechanisms in marine environments, reflecting possible variability in the sea-surface microlayer composition.
Sabour Baray, Daniel J. Jacob, Joannes D. Maasakkers, Jian-Xiong Sheng, Melissa P. Sulprizio, Dylan B. A. Jones, A. Anthony Bloom, and Robert McLaren
Atmos. Chem. Phys., 21, 18101–18121, https://doi.org/10.5194/acp-21-18101-2021, https://doi.org/10.5194/acp-21-18101-2021, 2021
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We use 2010–2015 surface and satellite observations to disentangle methane from anthropogenic and natural sources in Canada. Using a chemical transport model (GEOS-Chem), the mismatch between modelled and observed methane concentrations can be used to infer emissions according to Bayesian statistics. Compared to prior knowledge, we show higher anthropogenic emissions attributed to energy and/or agriculture in Western Canada and lower natural emissions from Boreal wetlands.
Shixian Zhai, Daniel J. Jacob, Jared F. Brewer, Ke Li, Jonathan M. Moch, Jhoon Kim, Seoyoung Lee, Hyunkwang Lim, Hyun Chul Lee, Su Keun Kuk, Rokjin J. Park, Jaein I. Jeong, Xuan Wang, Pengfei Liu, Gan Luo, Fangqun Yu, Jun Meng, Randall V. Martin, Katherine R. Travis, Johnathan W. Hair, Bruce E. Anderson, Jack E. Dibb, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jung-Hun Woo, Younha Kim, Qiang Zhang, and Hong Liao
Atmos. Chem. Phys., 21, 16775–16791, https://doi.org/10.5194/acp-21-16775-2021, https://doi.org/10.5194/acp-21-16775-2021, 2021
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Geostationary satellite aerosol optical depth (AOD) has tremendous potential for monitoring surface fine particulate matter (PM2.5). Our study explored the physical relationship between AOD and PM2.5 by integrating data from surface networks, aircraft, and satellites with the GEOS-Chem chemical transport model. We quantitatively showed that accurate simulation of aerosol size distributions, boundary layer depths, relative humidity, coarse particles, and diurnal variations in PM2.5 are essential.
Siqi Ma, Daniel Tong, Lok Lamsal, Julian Wang, Xuelei Zhang, Youhua Tang, Rick Saylor, Tianfeng Chai, Pius Lee, Patrick Campbell, Barry Baker, Shobha Kondragunta, Laura Judd, Timothy A. Berkoff, Scott J. Janz, and Ivanka Stajner
Atmos. Chem. Phys., 21, 16531–16553, https://doi.org/10.5194/acp-21-16531-2021, https://doi.org/10.5194/acp-21-16531-2021, 2021
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Predicting high ozone gets more challenging as urban emissions decrease. How can different techniques be used to foretell the quality of air to better protect human health? We tested four techniques with the CMAQ model against observations during a field campaign over New York City. The new system proves to better predict the magnitude and timing of high ozone. These approaches can be extended to other regions to improve the predictability of high-O3 episodes in contemporary urban environments.
Zachary C. J. Decker, Michael A. Robinson, Kelley C. Barsanti, Ilann Bourgeois, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Frank M. Flocke, Alessandro Franchin, Carley D. Fredrickson, Georgios I. Gkatzelis, Samuel R. Hall, Hannah Halliday, Christopher D. Holmes, L. Gregory Huey, Young Ro Lee, Jakob Lindaas, Ann M. Middlebrook, Denise D. Montzka, Richard Moore, J. Andrew Neuman, John B. Nowak, Brett B. Palm, Jeff Peischl, Felix Piel, Pamela S. Rickly, Andrew W. Rollins, Thomas B. Ryerson, Rebecca H. Schwantes, Kanako Sekimoto, Lee Thornhill, Joel A. Thornton, Geoffrey S. Tyndall, Kirk Ullmann, Paul Van Rooy, Patrick R. Veres, Carsten Warneke, Rebecca A. Washenfelder, Andrew J. Weinheimer, Elizabeth Wiggins, Edward Winstead, Armin Wisthaler, Caroline Womack, and Steven S. Brown
Atmos. Chem. Phys., 21, 16293–16317, https://doi.org/10.5194/acp-21-16293-2021, https://doi.org/10.5194/acp-21-16293-2021, 2021
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To understand air quality impacts from wildfires, we need an accurate picture of how wildfire smoke changes chemically both day and night as sunlight changes the chemistry of smoke. We present a chemical analysis of wildfire smoke as it changes from midday through the night. We use aircraft observations from the FIREX-AQ field campaign with a chemical box model. We find that even under sunlight typical
nighttimechemistry thrives and controls the fate of key smoke plume chemical processes.
Arseniy Karagodin-Doyennel, Eugene Rozanov, Timofei Sukhodolov, Tatiana Egorova, Alfonso Saiz-Lopez, Carlos A. Cuevas, Rafael P. Fernandez, Tomás Sherwen, Rainer Volkamer, Theodore K. Koenig, Tanguy Giroud, and Thomas Peter
Geosci. Model Dev., 14, 6623–6645, https://doi.org/10.5194/gmd-14-6623-2021, https://doi.org/10.5194/gmd-14-6623-2021, 2021
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Here, we present the iodine chemistry module in the SOCOL-AERv2 model. The obtained iodine distribution demonstrated a good agreement when validated against other simulations and available observations. We also estimated the iodine influence on ozone in the case of present-day iodine emissions, the sensitivity of ozone to doubled iodine emissions, and when considering only organic or inorganic iodine sources. The new model can be used as a tool for further studies of iodine effects on ozone.
Eric J. Hintsa, Fred L. Moore, Dale F. Hurst, Geoff S. Dutton, Bradley D. Hall, J. David Nance, Ben R. Miller, Stephen A. Montzka, Laura P. Wolton, Audra McClure-Begley, James W. Elkins, Emrys G. Hall, Allen F. Jordan, Andrew W. Rollins, Troy D. Thornberry, Laurel A. Watts, Chelsea R. Thompson, Jeff Peischl, Ilann Bourgeois, Thomas B. Ryerson, Bruce C. Daube, Yenny Gonzalez Ramos, Roisin Commane, Gregory W. Santoni, Jasna V. Pittman, Steven C. Wofsy, Eric Kort, Glenn S. Diskin, and T. Paul Bui
Atmos. Meas. Tech., 14, 6795–6819, https://doi.org/10.5194/amt-14-6795-2021, https://doi.org/10.5194/amt-14-6795-2021, 2021
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We built UCATS to study atmospheric chemistry and transport. It has measured trace gases including CFCs, N2O, SF6, CH4, CO, and H2 with gas chromatography, as well as ozone and water vapor. UCATS has been part of missions to study the tropical tropopause; transport of air into the stratosphere; greenhouse gases, transport, and chemistry in the troposphere; and ozone chemistry, on both piloted and unmanned aircraft. Its design, capabilities, and some results are shown and described here.
Xiaomeng Jin, Qindan Zhu, and Ronald C. Cohen
Atmos. Chem. Phys., 21, 15569–15587, https://doi.org/10.5194/acp-21-15569-2021, https://doi.org/10.5194/acp-21-15569-2021, 2021
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We describe direct estimates of NOx emissions and lifetimes for biomass burning plumes using daily TROPOMI retrievals of NO2. Satellite-derived NOx emission factors are consistent with those from in situ measurements. We observe decreasing NOx lifetime with fire intensity, which is due to the increase in NOx abundance and radical production. Our findings suggest promise for applying space-based observations to track the emissions and chemical evolution of reactive nitrogen from wildfires.
Hélène Angot, Connor Davel, Christine Wiedinmyer, Gabrielle Pétron, Jashan Chopra, Jacques Hueber, Brendan Blanchard, Ilann Bourgeois, Isaac Vimont, Stephen A. Montzka, Ben R. Miller, James W. Elkins, and Detlev Helmig
Atmos. Chem. Phys., 21, 15153–15170, https://doi.org/10.5194/acp-21-15153-2021, https://doi.org/10.5194/acp-21-15153-2021, 2021
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After a multidecadal global decline in atmospheric abundance of ethane and propane (precursors of tropospheric ozone and aerosols), previous work showed a reversal of this trend in 2009–2015 in the Northern Hemisphere due to the growth in oil and natural gas production in North America. Here we show a temporary pause in the growth of atmospheric ethane and propane in 2015–2018 and highlight the critical need for additional top-down studies to further constrain ethane and propane emissions.
Charles A. Brock, Karl D. Froyd, Maximilian Dollner, Christina J. Williamson, Gregory Schill, Daniel M. Murphy, Nicholas J. Wagner, Agnieszka Kupc, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jason C. Schroder, Douglas A. Day, Derek J. Price, Bernadett Weinzierl, Joshua P. Schwarz, Joseph M. Katich, Siyuan Wang, Linghan Zeng, Rodney Weber, Jack Dibb, Eric Scheuer, Glenn S. Diskin, Joshua P. DiGangi, ThaoPaul Bui, Jonathan M. Dean-Day, Chelsea R. Thompson, Jeff Peischl, Thomas B. Ryerson, Ilann Bourgeois, Bruce C. Daube, Róisín Commane, and Steven C. Wofsy
Atmos. Chem. Phys., 21, 15023–15063, https://doi.org/10.5194/acp-21-15023-2021, https://doi.org/10.5194/acp-21-15023-2021, 2021
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The Atmospheric Tomography Mission was an airborne study that mapped the chemical composition of the remote atmosphere. From this, we developed a comprehensive description of aerosol properties that provides a unique, global-scale dataset against which models can be compared. The data show the polluted nature of the remote atmosphere in the Northern Hemisphere and quantify the contributions of sea salt, dust, soot, biomass burning particles, and pollution particles to the haziness of the sky.
Liam Bindle, Randall V. Martin, Matthew J. Cooper, Elizabeth W. Lundgren, Sebastian D. Eastham, Benjamin M. Auer, Thomas L. Clune, Hongjian Weng, Jintai Lin, Lee T. Murray, Jun Meng, Christoph A. Keller, William M. Putman, Steven Pawson, and Daniel J. Jacob
Geosci. Model Dev., 14, 5977–5997, https://doi.org/10.5194/gmd-14-5977-2021, https://doi.org/10.5194/gmd-14-5977-2021, 2021
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Atmospheric chemistry models like GEOS-Chem are versatile tools widely used in air pollution and climate studies. The simulations used in such studies can be very computationally demanding, and thus it is useful if the model can simulate a specific geographic region at a higher resolution than the rest of the globe. Here, we implement, test, and demonstrate a new variable-resolution capability in GEOS-Chem that is suitable for simulations conducted on supercomputers.
Zhe Peng, Julia Lee-Taylor, Harald Stark, John J. Orlando, Bernard Aumont, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 14649–14669, https://doi.org/10.5194/acp-21-14649-2021, https://doi.org/10.5194/acp-21-14649-2021, 2021
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We use the fully explicit GECKO-A model to study the OH reactivity (OHR) evolution in the NO-free photooxidation of several volatile organic compounds. Oxidation progressively produces more saturated and functionalized species, then breaks them into small species. OHR per C atom evolution is similar for different precursors once saturated multifunctional species are formed. We also find that partitioning of these species to chamber walls leads to large deviations in chambers from the atmosphere.
Zhen Qu, Daniel J. Jacob, Lu Shen, Xiao Lu, Yuzhong Zhang, Tia R. Scarpelli, Hannah Nesser, Melissa P. Sulprizio, Joannes D. Maasakkers, A. Anthony Bloom, John R. Worden, Robert J. Parker, and Alba L. Delgado
Atmos. Chem. Phys., 21, 14159–14175, https://doi.org/10.5194/acp-21-14159-2021, https://doi.org/10.5194/acp-21-14159-2021, 2021
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The recent launch of TROPOMI offers an unprecedented opportunity to quantify the methane budget from a top-down perspective. We use TROPOMI and the more mature GOSAT methane observations to estimate methane emissions and get consistent global budgets. However, TROPOMI shows biases over regions where surface albedo is small and provides less information for the coarse-resolution inversion due to the larger error correlations and spatial variations in the number of observations.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven Wofsy
Atmos. Chem. Phys., 21, 13729–13746, https://doi.org/10.5194/acp-21-13729-2021, https://doi.org/10.5194/acp-21-13729-2021, 2021
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The NASA Atmospheric Tomography (ATom) mission built a climatology of the chemical composition of tropospheric air parcels throughout the middle of the Pacific and Atlantic oceans. The level of detail allows us to reconstruct the photochemical budgets of O3 and CH4 over these vast, remote regions. We find that most of the chemical heterogeneity is captured at the resolution used in current global chemistry models and that the majority of reactivity occurs in the
hottest20 % of parcels.
Haipeng Lin, Daniel J. Jacob, Elizabeth W. Lundgren, Melissa P. Sulprizio, Christoph A. Keller, Thibaud M. Fritz, Sebastian D. Eastham, Louisa K. Emmons, Patrick C. Campbell, Barry Baker, Rick D. Saylor, and Raffaele Montuoro
Geosci. Model Dev., 14, 5487–5506, https://doi.org/10.5194/gmd-14-5487-2021, https://doi.org/10.5194/gmd-14-5487-2021, 2021
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Emissions are a central component of atmospheric chemistry models. The Harmonized Emissions Component (HEMCO) is a software component for computing emissions from a user-selected ensemble of emission inventories and algorithms. It allows users to select, add, and scale emissions from different sources through a configuration file with no change to the model source code. We demonstrate the implementation of HEMCO in several models, all sharing the same HEMCO core code and database library.
Yi Yin, Frederic Chevallier, Philippe Ciais, Philippe Bousquet, Marielle Saunois, Bo Zheng, John Worden, A. Anthony Bloom, Robert J. Parker, Daniel J. Jacob, Edward J. Dlugokencky, and Christian Frankenberg
Atmos. Chem. Phys., 21, 12631–12647, https://doi.org/10.5194/acp-21-12631-2021, https://doi.org/10.5194/acp-21-12631-2021, 2021
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The growth of methane, the second-most important anthropogenic greenhouse gas after carbon dioxide, has been accelerating in recent years. Using an ensemble of multi-tracer atmospheric inversions constrained by surface or satellite observations, we show that global methane emissions increased by nearly 1 % per year from 2010–2017, with leading contributions from the tropics and East Asia.
Isabelle De Smedt, Gaia Pinardi, Corinne Vigouroux, Steven Compernolle, Alkis Bais, Nuria Benavent, Folkert Boersma, Ka-Lok Chan, Sebastian Donner, Kai-Uwe Eichmann, Pascal Hedelt, François Hendrick, Hitoshi Irie, Vinod Kumar, Jean-Christopher Lambert, Bavo Langerock, Christophe Lerot, Cheng Liu, Diego Loyola, Ankie Piters, Andreas Richter, Claudia Rivera Cárdenas, Fabian Romahn, Robert George Ryan, Vinayak Sinha, Nicolas Theys, Jonas Vlietinck, Thomas Wagner, Ting Wang, Huan Yu, and Michel Van Roozendael
Atmos. Chem. Phys., 21, 12561–12593, https://doi.org/10.5194/acp-21-12561-2021, https://doi.org/10.5194/acp-21-12561-2021, 2021
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This paper assess the performances of the TROPOMI formaldehyde observations compared to its predecessor OMI at different spatial and temporal scales. We also use a global network of MAX-DOAS instruments to validate both satellite datasets for a large range of HCHO columns. The precision obtained with daily TROPOMI observations is comparable to monthly OMI observations. We present clear detection of weak HCHO column enhancements related to shipping emissions in the Indian Ocean.
Hannah Nesser, Daniel J. Jacob, Joannes D. Maasakkers, Tia R. Scarpelli, Melissa P. Sulprizio, Yuzhong Zhang, and Chris H. Rycroft
Atmos. Meas. Tech., 14, 5521–5534, https://doi.org/10.5194/amt-14-5521-2021, https://doi.org/10.5194/amt-14-5521-2021, 2021
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Analytical inversions of satellite observations of atmospheric composition can improve emissions estimates and quantify errors but are computationally expensive at high resolutions. We propose two methods to decrease this cost. The methods reproduce a high-resolution inversion at a quarter of the cost. The reduced-dimension method creates a multiscale grid. The reduced-rank method solves the inversion where information content is highest.
Erin R. Delaria, Jinsol Kim, Helen L. Fitzmaurice, Catherine Newman, Paul J. Wooldridge, Kevin Worthington, and Ronald C. Cohen
Atmos. Meas. Tech., 14, 5487–5500, https://doi.org/10.5194/amt-14-5487-2021, https://doi.org/10.5194/amt-14-5487-2021, 2021
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The use of a dense network of low-cost CO2 sensors is an attractive option for measuring CO2 emissions in cities. However, these low-cost sensors are also subject to uncertainties. Here, we describe a novel method of field calibration for correcting temperature-related errors in the CO2 sensors deployed in the BEACO2N network. We show that with this temperature correction, we can achieve a sufficiently low network error to allow for the evaluation of CO2 emissions at a neighborhood scale.
Benjamin A. Nault, Duseong S. Jo, Brian C. McDonald, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Jason C. Schroder, James Allan, Donald R. Blake, Manjula R. Canagaratna, Hugh Coe, Matthew M. Coggon, Peter F. DeCarlo, Glenn S. Diskin, Rachel Dunmore, Frank Flocke, Alan Fried, Jessica B. Gilman, Georgios Gkatzelis, Jacqui F. Hamilton, Thomas F. Hanisco, Patrick L. Hayes, Daven K. Henze, Alma Hodzic, James Hopkins, Min Hu, L. Greggory Huey, B. Thomas Jobson, William C. Kuster, Alastair Lewis, Meng Li, Jin Liao, M. Omar Nawaz, Ilana B. Pollack, Jeffrey Peischl, Bernhard Rappenglück, Claire E. Reeves, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Min Shao, Jacob M. Sommers, James Walega, Carsten Warneke, Petter Weibring, Glenn M. Wolfe, Dominique E. Young, Bin Yuan, Qiang Zhang, Joost A. de Gouw, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 11201–11224, https://doi.org/10.5194/acp-21-11201-2021, https://doi.org/10.5194/acp-21-11201-2021, 2021
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Secondary organic aerosol (SOA) is an important aspect of poor air quality for urban regions around the world, where a large fraction of the population lives. However, there is still large uncertainty in predicting SOA in urban regions. Here, we used data from 11 urban campaigns and show that the variability in SOA production in these regions is predictable and is explained by key emissions. These results are used to estimate the premature mortality associated with SOA in urban regions.
Jianfeng Li, Yuhang Wang, Ruixiong Zhang, Charles Smeltzer, Andrew Weinheimer, Jay Herman, K. Folkert Boersma, Edward A. Celarier, Russell W. Long, James J. Szykman, Ruben Delgado, Anne M. Thompson, Travis N. Knepp, Lok N. Lamsal, Scott J. Janz, Matthew G. Kowalewski, Xiong Liu, and Caroline R. Nowlan
Atmos. Chem. Phys., 21, 11133–11160, https://doi.org/10.5194/acp-21-11133-2021, https://doi.org/10.5194/acp-21-11133-2021, 2021
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Comprehensive evaluations of simulated diurnal cycles of NO2 and NOy concentrations, vertical profiles, and tropospheric vertical column densities at two different resolutions with various measurements during the DISCOVER-AQ 2011 campaign show potential distribution biases of NOx emissions in the National Emissions Inventory 2011 at both 36 and 4 km resolutions, providing another possible explanation for the overestimation of model results.
Yenny Gonzalez, Róisín Commane, Ethan Manninen, Bruce C. Daube, Luke D. Schiferl, J. Barry McManus, Kathryn McKain, Eric J. Hintsa, James W. Elkins, Stephen A. Montzka, Colm Sweeney, Fred Moore, Jose L. Jimenez, Pedro Campuzano Jost, Thomas B. Ryerson, Ilann Bourgeois, Jeff Peischl, Chelsea R. Thompson, Eric Ray, Paul O. Wennberg, John Crounse, Michelle Kim, Hannah M. Allen, Paul A. Newman, Britton B. Stephens, Eric C. Apel, Rebecca S. Hornbrook, Benjamin A. Nault, Eric Morgan, and Steven C. Wofsy
Atmos. Chem. Phys., 21, 11113–11132, https://doi.org/10.5194/acp-21-11113-2021, https://doi.org/10.5194/acp-21-11113-2021, 2021
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Vertical profiles of N2O and a variety of chemical species and aerosols were collected nearly from pole to pole over the oceans during the NASA Atmospheric Tomography mission. We observed that tropospheric N2O variability is strongly driven by the influence of stratospheric air depleted in N2O, especially at middle and high latitudes. We also traced the origins of biomass burning and industrial emissions and investigated their impact on the variability of tropospheric N2O.
Xueling Liu, Arthur P. Mizzi, Jeffrey L. Anderson, Inez Fung, and Ronald C. Cohen
Atmos. Chem. Phys., 21, 9573–9583, https://doi.org/10.5194/acp-21-9573-2021, https://doi.org/10.5194/acp-21-9573-2021, 2021
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Observations of winds in the planetary boundary layer remain sparse, making it challenging to simulate and predict the atmospheric conditions that are most important for describing and predicting urban air quality. Here we investigate the application of data assimilation of NO2 columns as will be observed from geostationary orbit to improve predictions and retrospective analysis of wind fields in the boundary layer.
Wenfu Tang, David P. Edwards, Louisa K. Emmons, Helen M. Worden, Laura M. Judd, Lok N. Lamsal, Jassim A. Al-Saadi, Scott J. Janz, James H. Crawford, Merritt N. Deeter, Gabriele Pfister, Rebecca R. Buchholz, Benjamin Gaubert, and Caroline R. Nowlan
Atmos. Meas. Tech., 14, 4639–4655, https://doi.org/10.5194/amt-14-4639-2021, https://doi.org/10.5194/amt-14-4639-2021, 2021
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We use high-resolution airborne mapping spectrometer measurements to assess sub-grid variability within satellite pixels over urban regions. The sub-grid variability within satellite pixels increases with increasing satellite pixel sizes. Temporal variability within satellite pixels decreases with increasing satellite pixel sizes. This work is particularly relevant and useful for future satellite design, satellite data interpretation, and point-grid data comparisons.
Xu Feng, Haipeng Lin, Tzung-May Fu, Melissa P. Sulprizio, Jiawei Zhuang, Daniel J. Jacob, Heng Tian, Yaping Ma, Lijuan Zhang, Xiaolin Wang, Qi Chen, and Zhiwei Han
Geosci. Model Dev., 14, 3741–3768, https://doi.org/10.5194/gmd-14-3741-2021, https://doi.org/10.5194/gmd-14-3741-2021, 2021
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WRF-GC is an online coupling of the WRF meteorological model and GEOS-Chem chemical transport model for regional atmospheric chemistry and air quality modeling. In WRF-GC v2.0, we implemented the aerosol–radiation interactions and aerosol–cloud interactions, as well as the capability to nest multiple domains for high-resolution simulations based on the modular framework of WRF-GC v1.0. This allows the GEOS-Chem users to investigate the meteorology–atmospheric chemistry interactions.
Richard H. Moore, Elizabeth B. Wiggins, Adam T. Ahern, Stephen Zimmerman, Lauren Montgomery, Pedro Campuzano Jost, Claire E. Robinson, Luke D. Ziemba, Edward L. Winstead, Bruce E. Anderson, Charles A. Brock, Matthew D. Brown, Gao Chen, Ewan C. Crosbie, Hongyu Guo, Jose L. Jimenez, Carolyn E. Jordan, Ming Lyu, Benjamin A. Nault, Nicholas E. Rothfuss, Kevin J. Sanchez, Melinda Schueneman, Taylor J. Shingler, Michael A. Shook, Kenneth L. Thornhill, Nicholas L. Wagner, and Jian Wang
Atmos. Meas. Tech., 14, 4517–4542, https://doi.org/10.5194/amt-14-4517-2021, https://doi.org/10.5194/amt-14-4517-2021, 2021
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Atmospheric particles are everywhere and exist in a range of sizes, from a few nanometers to hundreds of microns. Because particle size determines the behavior of chemical and physical processes, accurately measuring particle sizes is an important and integral part of atmospheric field measurements! Here, we discuss the performance of two commonly used particle sizers and how changes in particle composition and optical properties may result in sizing uncertainties, which we quantify.
Christina J. Williamson, Agnieszka Kupc, Andrew Rollins, Jan Kazil, Karl D. Froyd, Eric A. Ray, Daniel M. Murphy, Gregory P. Schill, Jeff Peischl, Chelsea Thompson, Ilann Bourgeois, Thomas B. Ryerson, Glenn S. Diskin, Joshua P. DiGangi, Donald R. Blake, Thao Paul V. Bui, Maximilian Dollner, Bernadett Weinzierl, and Charles A. Brock
Atmos. Chem. Phys., 21, 9065–9088, https://doi.org/10.5194/acp-21-9065-2021, https://doi.org/10.5194/acp-21-9065-2021, 2021
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Aerosols in the stratosphere influence climate by scattering and absorbing sunlight and through chemical reactions occurring on the particles’ surfaces. We observed more nucleation mode aerosols (small aerosols, with diameters below 12 nm) in the mid- and high-latitude lowermost stratosphere (8–13 km) in the Northern Hemisphere (NH) than in the Southern Hemisphere. The most likely cause of this is aircraft emissions, which are concentrated in the NH at similar altitudes to our observations.
Daniel M. Murphy, Karl D. Froyd, Ilann Bourgeois, Charles A. Brock, Agnieszka Kupc, Jeff Peischl, Gregory P. Schill, Chelsea R. Thompson, Christina J. Williamson, and Pengfei Yu
Atmos. Chem. Phys., 21, 8915–8932, https://doi.org/10.5194/acp-21-8915-2021, https://doi.org/10.5194/acp-21-8915-2021, 2021
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New measurements in the lower stratosphere highlight differences between particles that originated in the troposphere or the stratosphere. The stratospheric-origin particles have relatively large radiative effects because they are at nearly the optimum diameter for light scattering. The tropospheric particles contribute significantly to surface area. These and other chemical and physical properties are then extended to study the implications if material were to be added to the stratosphere.
Hongyu Guo, Pedro Campuzano-Jost, Benjamin A. Nault, Douglas A. Day, Jason C. Schroder, Dongwook Kim, Jack E. Dibb, Maximilian Dollner, Bernadett Weinzierl, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 3631–3655, https://doi.org/10.5194/amt-14-3631-2021, https://doi.org/10.5194/amt-14-3631-2021, 2021
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We utilize a set of high-quality datasets collected during the NASA Atmospheric Tomography Mission to investigate the impact of differences in observable particle sizes across aerosol instruments in aerosol measurement comparisons. Very good agreement was found between chemically and physically derived submicron aerosol volume. Results support a lack of significant unknown biases in the response of an Aerodyne aerosol mass spectrometer (AMS) when sampling remote aerosols across the globe.
Anteneh Getachew Mengistu, Gizaw Mengistu Tsidu, Gerbrand Koren, Maurits L. Kooreman, K. Folkert Boersma, Torbern Tagesson, Jonas Ardö, Yann Nouvellon, and Wouter Peters
Biogeosciences, 18, 2843–2857, https://doi.org/10.5194/bg-18-2843-2021, https://doi.org/10.5194/bg-18-2843-2021, 2021
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In this study, we assess the usefulness of Sun-Induced Fluorescence of Terrestrial Ecosystems Retrieval (SIFTER) data from the GOME-2A instrument and near-infrared reflectance of vegetation (NIRv) from MODIS to capture the seasonality and magnitudes of gross primary production (GPP) derived from six eddy-covariance flux towers in Africa in the overlap years between 2007–2014. We also test the robustness of sun-induced fluoresence and NIRv to compare the seasonality of GPP for the major biomes.
David R. Lyon, Benjamin Hmiel, Ritesh Gautam, Mark Omara, Katherine A. Roberts, Zachary R. Barkley, Kenneth J. Davis, Natasha L. Miles, Vanessa C. Monteiro, Scott J. Richardson, Stephen Conley, Mackenzie L. Smith, Daniel J. Jacob, Lu Shen, Daniel J. Varon, Aijun Deng, Xander Rudelis, Nikhil Sharma, Kyle T. Story, Adam R. Brandt, Mary Kang, Eric A. Kort, Anthony J. Marchese, and Steven P. Hamburg
Atmos. Chem. Phys., 21, 6605–6626, https://doi.org/10.5194/acp-21-6605-2021, https://doi.org/10.5194/acp-21-6605-2021, 2021
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The Permian Basin (USA) is the world’s largest oil field. We use tower- and aircraft-based approaches to measure how methane emissions in the Permian Basin changed throughout 2020. In early 2020, 3.3 % of the region’s gas was emitted; then in spring 2020, the loss rate temporarily dropped to 1.9 % as oil price crashed. We find this short-term reduction to be a result of reduced well development, less gas flaring, and fewer abnormal events despite minimal reductions in oil and gas production.
Simone T. Andersen, Lucy J. Carpenter, Beth S. Nelson, Luis Neves, Katie A. Read, Chris Reed, Martyn Ward, Matthew J. Rowlinson, and James D. Lee
Atmos. Meas. Tech., 14, 3071–3085, https://doi.org/10.5194/amt-14-3071-2021, https://doi.org/10.5194/amt-14-3071-2021, 2021
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NOx has been measured in remote marine air via chemiluminescence detection using two different methods for NO2 to NO photolytic conversion: (a) internal diodes and a reaction chamber made of Teflon-like barium-doped material, which causes a NO2 artefact, and (b) external diodes and a quartz photolysis cell. Once corrections are made for the artefact of (a), the two converters are shown to give comparable NO2 mixing ratios, giving confidence in the quantitative measurement of NOx at low levels.
Chelsea E. Stockwell, Matthew M. Coggon, Georgios I. Gkatzelis, John Ortega, Brian C. McDonald, Jeff Peischl, Kenneth Aikin, Jessica B. Gilman, Michael Trainer, and Carsten Warneke
Atmos. Chem. Phys., 21, 6005–6022, https://doi.org/10.5194/acp-21-6005-2021, https://doi.org/10.5194/acp-21-6005-2021, 2021
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Volatile chemical products are emerging as a large source of petrochemical organics in urban environments. We identify markers for the coatings category by linking ambient observations to laboratory measurements, investigating volatile organic compound (VOC) composition, and quantifying key VOC emissions via controlled evaporation experiments. Ingredients and sales surveys are used to confirm the prevalence and usage trends to support the assignment of water and solvent-borne coating tracers.
Alexander Vasilkov, Nickolay Krotkov, Eun-Su Yang, Lok Lamsal, Joanna Joiner, Patricia Castellanos, Zachary Fasnacht, and Robert Spurr
Atmos. Meas. Tech., 14, 2857–2871, https://doi.org/10.5194/amt-14-2857-2021, https://doi.org/10.5194/amt-14-2857-2021, 2021
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To explicitly account for aerosol effects in the OMI cloud and nitrogen dioxide algorithms, we use a model of aerosol optical properties from a global aerosol assimilation system and radiative transfer computations. Accounting for anisotropic reflection of Earth's surface is an important feature of the approach. Comparisons of the cloud and tropospheric nitrogen dioxide retrievals with implicit and explicit aerosol corrections are carried out for a selected area with high pollution.
Daniel J. Varon, Dylan Jervis, Jason McKeever, Ian Spence, David Gains, and Daniel J. Jacob
Atmos. Meas. Tech., 14, 2771–2785, https://doi.org/10.5194/amt-14-2771-2021, https://doi.org/10.5194/amt-14-2771-2021, 2021
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Satellites can detect methane emissions by measuring sunlight reflected from the Earth's surface and atmosphere. Here we show that the European Space Agency's Sentinel-2 twin satellites can be used to monitor anomalously large methane point sources around the world, with global coverage every 2–5 days and 20 m spatial resolution. We demonstrate this previously unreported capability through high-frequency Sentinel-2 monitoring of two strong methane point sources in Algeria and Turkmenistan.
Eloise A. Marais, John F. Roberts, Robert G. Ryan, Henk Eskes, K. Folkert Boersma, Sungyeon Choi, Joanna Joiner, Nader Abuhassan, Alberto Redondas, Michel Grutter, Alexander Cede, Laura Gomez, and Monica Navarro-Comas
Atmos. Meas. Tech., 14, 2389–2408, https://doi.org/10.5194/amt-14-2389-2021, https://doi.org/10.5194/amt-14-2389-2021, 2021
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Nitrogen oxides in the upper troposphere have a profound influence on the global troposphere, but routine reliable observations there are exceedingly rare. We apply cloud-slicing to TROPOMI total columns of nitrogen dioxide (NO2) at high spatial resolution to derive near-global observations of NO2 in the upper troposphere and show consistency with existing datasets. These data offer tremendous potential to address knowledge gaps in this oft underappreciated portion of the atmosphere.
Xiao Lu, Daniel J. Jacob, Yuzhong Zhang, Joannes D. Maasakkers, Melissa P. Sulprizio, Lu Shen, Zhen Qu, Tia R. Scarpelli, Hannah Nesser, Robert M. Yantosca, Jianxiong Sheng, Arlyn Andrews, Robert J. Parker, Hartmut Boesch, A. Anthony Bloom, and Shuang Ma
Atmos. Chem. Phys., 21, 4637–4657, https://doi.org/10.5194/acp-21-4637-2021, https://doi.org/10.5194/acp-21-4637-2021, 2021
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We use an analytical solution to the Bayesian inverse problem to quantitatively compare and combine the information from satellite and in situ observations, and to estimate global methane budget and their trends over the 2010–2017 period. We find that satellite and in situ observations are to a large extent complementary in the inversion for estimating global methane budget, and reveal consistent corrections of regional anthropogenic and wetland methane emissions relative to the prior inventory.
Melinda K. Schueneman, Benjamin A. Nault, Pedro Campuzano-Jost, Duseong S. Jo, Douglas A. Day, Jason C. Schroder, Brett B. Palm, Alma Hodzic, Jack E. Dibb, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 2237–2260, https://doi.org/10.5194/amt-14-2237-2021, https://doi.org/10.5194/amt-14-2237-2021, 2021
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This work focuses on two important properties of the aerosol, acidity, and sulfate composition, which is important for our understanding of aerosol health and environmental impacts. We explore different methods to understand the composition of the aerosol with measurements from a specific instrument and apply those methods to a large dataset. These measurements are confounded by other factors, making it challenging to predict aerosol sulfate composition; pH estimations, however, show promise.
Joannes D. Maasakkers, Daniel J. Jacob, Melissa P. Sulprizio, Tia R. Scarpelli, Hannah Nesser, Jianxiong Sheng, Yuzhong Zhang, Xiao Lu, A. Anthony Bloom, Kevin W. Bowman, John R. Worden, and Robert J. Parker
Atmos. Chem. Phys., 21, 4339–4356, https://doi.org/10.5194/acp-21-4339-2021, https://doi.org/10.5194/acp-21-4339-2021, 2021
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We use 2010–2015 GOSAT satellite observations of atmospheric methane over North America in a high-resolution inversion to estimate methane emissions. We find general consistency with the gridded EPA inventory but higher oil and gas production emissions, with oil production emissions twice as large as in the latest EPA Greenhouse Gas Inventory. We find lower wetland emissions than predicted by WetCHARTs and a small increasing trend in the eastern US, apparently related to unconventional oil/gas.
Yuzhong Zhang, Daniel J. Jacob, Xiao Lu, Joannes D. Maasakkers, Tia R. Scarpelli, Jian-Xiong Sheng, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Jinfeng Chang, A. Anthony Bloom, Shuang Ma, John Worden, Robert J. Parker, and Hartmut Boesch
Atmos. Chem. Phys., 21, 3643–3666, https://doi.org/10.5194/acp-21-3643-2021, https://doi.org/10.5194/acp-21-3643-2021, 2021
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We use 2010–2018 satellite observations of atmospheric methane to interpret the factors controlling atmospheric methane and its accelerating increase during the period. The 2010–2018 increase in global methane emissions is driven by tropical and boreal wetlands and tropical livestock (South Asia, Africa, Brazil), with an insignificant positive trend in emissions from the fossil fuel sector. The peak methane growth rates in 2014–2015 are also contributed by low OH and high fire emissions.
Christoph A. Keller, Mathew J. Evans, K. Emma Knowland, Christa A. Hasenkopf, Sruti Modekurty, Robert A. Lucchesi, Tomohiro Oda, Bruno B. Franca, Felipe C. Mandarino, M. Valeria Díaz Suárez, Robert G. Ryan, Luke H. Fakes, and Steven Pawson
Atmos. Chem. Phys., 21, 3555–3592, https://doi.org/10.5194/acp-21-3555-2021, https://doi.org/10.5194/acp-21-3555-2021, 2021
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This study combines surface observations and model simulations to quantify the impact of COVID-19 restrictions on air quality across the world. The presented methodology removes the confounding impacts of meteorology on air pollution. Our results indicate that surface concentrations of nitrogen dioxide, an important air pollutant emitted during the combustion of fossil fuels, declined by up to 60 % following the implementation of COVID-19 containment measures.
Duseong S. Jo, Alma Hodzic, Louisa K. Emmons, Simone Tilmes, Rebecca H. Schwantes, Michael J. Mills, Pedro Campuzano-Jost, Weiwei Hu, Rahul A. Zaveri, Richard C. Easter, Balwinder Singh, Zheng Lu, Christiane Schulz, Johannes Schneider, John E. Shilling, Armin Wisthaler, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 3395–3425, https://doi.org/10.5194/acp-21-3395-2021, https://doi.org/10.5194/acp-21-3395-2021, 2021
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Secondary organic aerosol (SOA) is a major component of submicron particulate matter, but there are a lot of uncertainties in the future prediction of SOA. We used CESM 2.1 to investigate future IEPOX SOA concentration changes. The explicit chemistry predicted substantial changes in IEPOX SOA depending on the future scenario, but the parameterization predicted weak changes due to simplified chemistry, which shows the importance of correct physicochemical dependencies in future SOA prediction.
Demetrios Pagonis, Pedro Campuzano-Jost, Hongyu Guo, Douglas A. Day, Melinda K. Schueneman, Wyatt L. Brown, Benjamin A. Nault, Harald Stark, Kyla Siemens, Alex Laskin, Felix Piel, Laura Tomsche, Armin Wisthaler, Matthew M. Coggon, Georgios I. Gkatzelis, Hannah S. Halliday, Jordan E. Krechmer, Richard H. Moore, David S. Thomson, Carsten Warneke, Elizabeth B. Wiggins, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 1545–1559, https://doi.org/10.5194/amt-14-1545-2021, https://doi.org/10.5194/amt-14-1545-2021, 2021
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We describe the airborne deployment of an extractive electrospray time-of-flight mass spectrometer (EESI-MS). The instrument provides a quantitative 1 Hz measurement of the chemical composition of organic aerosol up to altitudes of
7 km, with single-compound detection limits as low as 50 ng per standard cubic meter.
Inés Sanz-Morère, Sebastian D. Eastham, Florian Allroggen, Raymond L. Speth, and Steven R. H. Barrett
Atmos. Chem. Phys., 21, 1649–1681, https://doi.org/10.5194/acp-21-1649-2021, https://doi.org/10.5194/acp-21-1649-2021, 2021
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Contrails cause ~50 % of aviation climate impacts, but this is highly uncertain. This is partly due to the effect of overlap between contrails and other cloud layers. We developed a model to quantify this effect, finding that overlap with natural clouds increased contrails' radiative forcing in 2015. This suggests that cloud avoidance may help in reducing aviation's climate impacts. We also find that contrail–contrail overlap reduces impacts by ~3 %, increasing non-linearly with optical depth.
Angharad C. Stell, Luke M. Western, Tomás Sherwen, and Matthew Rigby
Atmos. Chem. Phys., 21, 1717–1736, https://doi.org/10.5194/acp-21-1717-2021, https://doi.org/10.5194/acp-21-1717-2021, 2021
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Although it is the second-most important greenhouse gas, our understanding of the atmospheric-methane budget is limited. The uncertainty highlights the need for new tools to investigate sources and sinks. Here, we use a Gaussian process emulator to efficiently approximate the response of atmospheric-methane observations to changes in the most uncertain emission or loss processes. With this new method, we rigorously quantify the sensitivity of atmospheric observations to budget uncertainties.
Mike J. Newland, Daniel J. Bryant, Rachel E. Dunmore, Thomas J. Bannan, W. Joe F. Acton, Ben Langford, James R. Hopkins, Freya A. Squires, William Dixon, William S. Drysdale, Peter D. Ivatt, Mathew J. Evans, Peter M. Edwards, Lisa K. Whalley, Dwayne E. Heard, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, Archit Mehra, Stephen D. Worrall, Asan Bacak, Hugh Coe, Carl J. Percival, C. Nicholas Hewitt, James D. Lee, Tianqu Cui, Jason D. Surratt, Xinming Wang, Alastair C. Lewis, Andrew R. Rickard, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 21, 1613–1625, https://doi.org/10.5194/acp-21-1613-2021, https://doi.org/10.5194/acp-21-1613-2021, 2021
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We report the formation of secondary pollutants in the urban megacity of Beijing that are typically associated with remote regions such as rainforests. This is caused by extremely low levels of nitric oxide (NO), typically expected to be high in urban areas, observed in the afternoon. This work has significant implications for how we understand atmospheric chemistry in the urban environment and thus for how to implement effective policies to improve urban air quality.
Tijl Verhoelst, Steven Compernolle, Gaia Pinardi, Jean-Christopher Lambert, Henk J. Eskes, Kai-Uwe Eichmann, Ann Mari Fjæraa, José Granville, Sander Niemeijer, Alexander Cede, Martin Tiefengraber, François Hendrick, Andrea Pazmiño, Alkiviadis Bais, Ariane Bazureau, K. Folkert Boersma, Kristof Bognar, Angelika Dehn, Sebastian Donner, Aleksandr Elokhov, Manuel Gebetsberger, Florence Goutail, Michel Grutter de la Mora, Aleksandr Gruzdev, Myrto Gratsea, Georg H. Hansen, Hitoshi Irie, Nis Jepsen, Yugo Kanaya, Dimitris Karagkiozidis, Rigel Kivi, Karin Kreher, Pieternel F. Levelt, Cheng Liu, Moritz Müller, Monica Navarro Comas, Ankie J. M. Piters, Jean-Pierre Pommereau, Thierry Portafaix, Cristina Prados-Roman, Olga Puentedura, Richard Querel, Julia Remmers, Andreas Richter, John Rimmer, Claudia Rivera Cárdenas, Lidia Saavedra de Miguel, Valery P. Sinyakov, Wolfgang Stremme, Kimberly Strong, Michel Van Roozendael, J. Pepijn Veefkind, Thomas Wagner, Folkard Wittrock, Margarita Yela González, and Claus Zehner
Atmos. Meas. Tech., 14, 481–510, https://doi.org/10.5194/amt-14-481-2021, https://doi.org/10.5194/amt-14-481-2021, 2021
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This paper reports on the ground-based validation of the NO2 data produced operationally by the TROPOMI instrument on board the Sentinel-5 Precursor satellite. Tropospheric, stratospheric, and total NO2 columns are compared to measurements collected from MAX-DOAS, ZSL-DOAS, and PGN/Pandora instruments respectively. The products are found to satisfy mission requirements in general, though negative mean differences are found at sites with high pollution levels. Potential causes are discussed.
Lok N. Lamsal, Nickolay A. Krotkov, Alexander Vasilkov, Sergey Marchenko, Wenhan Qin, Eun-Su Yang, Zachary Fasnacht, Joanna Joiner, Sungyeon Choi, David Haffner, William H. Swartz, Bradford Fisher, and Eric Bucsela
Atmos. Meas. Tech., 14, 455–479, https://doi.org/10.5194/amt-14-455-2021, https://doi.org/10.5194/amt-14-455-2021, 2021
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The NASA standard nitrogen dioxide (NO2) version 4.0 product for OMI Aura incorporates the most salient improvements. It represents the first global satellite trace gas retrieval with OMI–MODIS synergy accounting for surface reflectance anisotropy in cloud and NO2 retrievals. Improved spectral fitting procedures for NO2 and oxygen dimer (for cloud) retrievals and reliance on high-resolution field-of-view-specific input information for NO2 and cloud retrievals help enhance the NO2 data quality.
Susan S. Kulawik, John R. Worden, Vivienne H. Payne, Dejian Fu, Steven C. Wofsy, Kathryn McKain, Colm Sweeney, Bruce C. Daube Jr., Alan Lipton, Igor Polonsky, Yuguang He, Karen E. Cady-Pereira, Edward J. Dlugokencky, Daniel J. Jacob, and Yi Yin
Atmos. Meas. Tech., 14, 335–354, https://doi.org/10.5194/amt-14-335-2021, https://doi.org/10.5194/amt-14-335-2021, 2021
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This paper shows comparisons of a new single-footprint methane product from the AIRS satellite to aircraft-based observations. We show that this AIRS methane product provides useful information to study seasonal and global methane trends of this important greenhouse gas.
Megan S. Claflin, Demetrios Pagonis, Zachary Finewax, Anne V. Handschy, Douglas A. Day, Wyatt L. Brown, John T. Jayne, Douglas R. Worsnop, Jose L. Jimenez, Paul J. Ziemann, Joost de Gouw, and Brian M. Lerner
Atmos. Meas. Tech., 14, 133–152, https://doi.org/10.5194/amt-14-133-2021, https://doi.org/10.5194/amt-14-133-2021, 2021
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We have developed a field-deployable gas chromatograph with thermal desorption preconcentration and detector switching between two high-resolution mass spectrometers for in situ measurements of volatile organic compounds (VOCs). This system combines chromatography with both proton transfer and electron ionization to offer fast time response and continuous molecular speciation. This technique was applied during the 2018 ATHLETIC campaign to characterize VOC emissions in an indoor environment.
David C. Loades, Mingxi Yang, Thomas G. Bell, Adam R. Vaughan, Ryan J. Pound, Stefan Metzger, James D. Lee, and Lucy J. Carpenter
Atmos. Meas. Tech., 13, 6915–6931, https://doi.org/10.5194/amt-13-6915-2020, https://doi.org/10.5194/amt-13-6915-2020, 2020
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The loss of ozone to the sea surface was measured from the south coast of the UK and was found to be more rapid than previous observations over the open ocean. This is likely a consequence of different chemistry and biology in coastal environments. Strong winds appeared to speed up the loss of ozone. A better understanding of what influences ozone loss over the sea will lead to better model estimates of total ozone in the troposphere.
Reem A. Hannun, Andrew K. Swanson, Steven A. Bailey, Thomas F. Hanisco, T. Paul Bui, Ilann Bourgeois, Jeff Peischl, and Thomas B. Ryerson
Atmos. Meas. Tech., 13, 6877–6887, https://doi.org/10.5194/amt-13-6877-2020, https://doi.org/10.5194/amt-13-6877-2020, 2020
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We have developed a cavity-enhanced absorption instrument to measure ozone in the atmosphere. The detection technique enables highly sensitive measurements in fast averaging times. The compact, robust instrument is suitable for operation in varied field environments, including aboard research aircraft. We have successfully flown the instrument and demonstrated its performance capabilities with measurements of ozone deposition rates over the coastal Pacific Ocean.
Junfeng Wang, Jianhuai Ye, Dantong Liu, Yangzhou Wu, Jian Zhao, Weiqi Xu, Conghui Xie, Fuzhen Shen, Jie Zhang, Paul E. Ohno, Yiming Qin, Xiuyong Zhao, Scot T. Martin, Alex K. Y. Lee, Pingqing Fu, Daniel J. Jacob, Qi Zhang, Yele Sun, Mindong Chen, and Xinlei Ge
Atmos. Chem. Phys., 20, 14091–14102, https://doi.org/10.5194/acp-20-14091-2020, https://doi.org/10.5194/acp-20-14091-2020, 2020
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We compared the organics in total submicron matter and those coated on BC cores during summertime in Beijing and found large differences between them. Traffic-related OA was associated significantly with BC, while cooking-related OA did not coat BC. In addition, a factor likely originated from primary biomass burning OA was only identified in BC-containing particles. Such a unique BBOA requires further field and laboratory studies to verify its presence and elucidate its properties and impacts.
Erin R. Delaria, Bryan K. Place, Amy X. Liu, and Ronald C. Cohen
Atmos. Chem. Phys., 20, 14023–14041, https://doi.org/10.5194/acp-20-14023-2020, https://doi.org/10.5194/acp-20-14023-2020, 2020
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Observations of NO2 deposition to vegetation have been widely reported, but the magnitude and mechanism remain uncertain. We use laboratory measurements to study NO2 deposition to leaves of 10 native California tree species. We report important differences in the uptake rates between species and find that this process is primarily diffusion-regulated. We suggest that processes within leaves at a cellular level represent a negligible limitation to NO2 deposition at the canopy level.
Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Hongyu Guo, Duseong S. Jo, Anne V. Handschy, Demetrios Pagonis, Jason C. Schroder, Melinda K. Schueneman, Michael J. Cubison, Jack E. Dibb, Alma Hodzic, Weiwei Hu, Brett B. Palm, and Jose L. Jimenez
Atmos. Meas. Tech., 13, 6193–6213, https://doi.org/10.5194/amt-13-6193-2020, https://doi.org/10.5194/amt-13-6193-2020, 2020
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Collecting particulate matter, or aerosols, onto filters to be analyzed offline is a widely used method to investigate the mass concentration and chemical composition of the aerosol, especially the inorganic portion. Here, we show that acidic aerosol (sulfuric acid) collected onto filters and then exposed to high ammonia mixing ratios (from human emissions) will lead to biases in the ammonium collected onto filters, and the uptake of ammonia is rapid (< 10 s), which impacts the filter data.
Gaia Pinardi, Michel Van Roozendael, François Hendrick, Nicolas Theys, Nader Abuhassan, Alkiviadis Bais, Folkert Boersma, Alexander Cede, Jihyo Chong, Sebastian Donner, Theano Drosoglou, Anatoly Dzhola, Henk Eskes, Udo Frieß, José Granville, Jay R. Herman, Robert Holla, Jari Hovila, Hitoshi Irie, Yugo Kanaya, Dimitris Karagkiozidis, Natalia Kouremeti, Jean-Christopher Lambert, Jianzhong Ma, Enno Peters, Ankie Piters, Oleg Postylyakov, Andreas Richter, Julia Remmers, Hisahiro Takashima, Martin Tiefengraber, Pieter Valks, Tim Vlemmix, Thomas Wagner, and Folkard Wittrock
Atmos. Meas. Tech., 13, 6141–6174, https://doi.org/10.5194/amt-13-6141-2020, https://doi.org/10.5194/amt-13-6141-2020, 2020
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We validate several GOME-2 and OMI tropospheric NO2 products with 23 MAX-DOAS and 16 direct sun instruments distributed worldwide, highlighting large horizontal inhomogeneities at several sites affecting the validation results. We propose a method for quantification and correction. We show the application of such correction reduces the satellite underestimation in almost all heterogeneous cases, but a negative bias remains over the MAX-DOAS and direct sun network ensemble for both satellites.
Yiqi Zheng, Joel A. Thornton, Nga Lee Ng, Hansen Cao, Daven K. Henze, Erin E. McDuffie, Weiwei Hu, Jose L. Jimenez, Eloise A. Marais, Eric Edgerton, and Jingqiu Mao
Atmos. Chem. Phys., 20, 13091–13107, https://doi.org/10.5194/acp-20-13091-2020, https://doi.org/10.5194/acp-20-13091-2020, 2020
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This study aims to address a challenge in biosphere–atmosphere interactions: to what extent can biogenic organic aerosol (OA) be modified through human activities? From three surface network observations, we show OA is weakly dependent on sulfate and aerosol acidity in the summer southeast US, on both long-term trends and monthly variability. The results are in strong contrast to a global model, GEOS-Chem, suggesting the need to revisit the representation of aqueous-phase secondary OA formation.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Ole Kirner, Sarah Strode, Simone Tilmes, Edward J. Dlugokencky, and Bo Zheng
Atmos. Chem. Phys., 20, 13011–13022, https://doi.org/10.5194/acp-20-13011-2020, https://doi.org/10.5194/acp-20-13011-2020, 2020
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Decadal trends and variations in OH are critical for understanding atmospheric CH4 evolution. We quantify the impacts of OH trends and variations on the CH4 budget by conducting CH4 inversions on a decadal scale with an ensemble of OH fields. We find the negative OH anomalies due to enhanced fires can reduce the optimized CH4 emissions by up to 10 Tg yr−1 during El Niño years and the positive OH trend from 1986 to 2010 results in a ∼ 23 Tg yr−1 additional increase in optimized CH4 emissions.
Melodie Lao, Leigh R. Crilley, Leyla Salehpoor, Teles C. Furlani, Ilann Bourgeois, J. Andrew Neuman, Andrew W. Rollins, Patrick R. Veres, Rebecca A. Washenfelder, Caroline C. Womack, Cora J. Young, and Trevor C. VandenBoer
Atmos. Meas. Tech., 13, 5873–5890, https://doi.org/10.5194/amt-13-5873-2020, https://doi.org/10.5194/amt-13-5873-2020, 2020
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Nitrous acid (HONO) is a key intermediate in the generation of oxidants and fate of nitrogen oxides in the atmosphere. High-purity calibration sources that produce stable atmospherically relevant levels under field conditions have not been made to date, reducing measurement accuracy. In this study a simple salt-coated tube humidified with water vapor is demonstrated to produce pure stable low levels of HONO, with modifications allowing the generation of higher amounts.
Viral Shah, Daniel J. Jacob, Jonathan M. Moch, Xuan Wang, and Shixian Zhai
Atmos. Chem. Phys., 20, 12223–12245, https://doi.org/10.5194/acp-20-12223-2020, https://doi.org/10.5194/acp-20-12223-2020, 2020
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Cloud water pH affects atmospheric chemistry, and acid rain damages ecosystems. We use model simulations along with observations to present a global view of cloud water and precipitation pH. Sulfuric acid, nitric acid, and ammonia control the pH in the northern midlatitudes, but carboxylic acids and dust cations are important in the tropics and subtropics. The acid inputs to many nitrogen-saturated ecosystems are high enough to cause acidification, with ammonium as the main acidifying species.
Swaleha Inamdar, Liselotte Tinel, Rosie Chance, Lucy J. Carpenter, Prabhakaran Sabu, Racheal Chacko, Sarat C. Tripathy, Anvita U. Kerkar, Alok K. Sinha, Parli Venkateswaran Bhaskar, Amit Sarkar, Rajdeep Roy, Tomás Sherwen, Carlos Cuevas, Alfonso Saiz-Lopez, Kirpa Ram, and Anoop S. Mahajan
Atmos. Chem. Phys., 20, 12093–12114, https://doi.org/10.5194/acp-20-12093-2020, https://doi.org/10.5194/acp-20-12093-2020, 2020
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Iodine chemistry is generating a lot of interest because of its impacts on the oxidising capacity of the marine boundary and depletion of ozone. However, one of the challenges has been predicting the right levels of iodine in the models, which depend on parameterisations for emissions from the sea surface. This paper discusses the different parameterisations available and compares them with observations, showing that our current knowledge is still insufficient, especially on a regional scale.
Wayne M. Angevine, Jeff Peischl, Alice Crawford, Christopher P. Loughner, Ilana B. Pollack, and Chelsea R. Thompson
Atmos. Chem. Phys., 20, 11855–11868, https://doi.org/10.5194/acp-20-11855-2020, https://doi.org/10.5194/acp-20-11855-2020, 2020
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Emissions of air pollutants must be known for a wide variety of applications. Different methods of estimating emissions often disagree substantially. In this study, we apply standard methods to a well-known source, a power plant. We explore the uncertainty implied by the different answers that come from the different methods, different samples taken over several years, and different pollutants. We find that the overall uncertainty of emissions estimates is about 30 %.
Ke Li, Daniel J. Jacob, Lu Shen, Xiao Lu, Isabelle De Smedt, and Hong Liao
Atmos. Chem. Phys., 20, 11423–11433, https://doi.org/10.5194/acp-20-11423-2020, https://doi.org/10.5194/acp-20-11423-2020, 2020
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Surface summer ozone increased in China from 2013 to 2019 despite new governmental efforts targeting ozone pollution. We find that the ozone increase is mostly due to anthropogenic drivers, although meteorology also plays a role. Further analysis for the North China Plain shows that PM2.5 continued to decrease through 2019, while emissions of volatile organic compounds (VOCs) stayed flat. This could explain the anthropogenic increase in ozone, as PM2.5 scavenges the radical precursors of ozone.
Kazuyuki Miyazaki, Kevin Bowman, Takashi Sekiya, Henk Eskes, Folkert Boersma, Helen Worden, Nathaniel Livesey, Vivienne H. Payne, Kengo Sudo, Yugo Kanaya, Masayuki Takigawa, and Koji Ogochi
Earth Syst. Sci. Data, 12, 2223–2259, https://doi.org/10.5194/essd-12-2223-2020, https://doi.org/10.5194/essd-12-2223-2020, 2020
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This study presents the results from the Tropospheric Chemistry Reanalysis version 2 (TCR-2) for 2005–2018 obtained from the assimilation of multiple satellite measurements of ozone, CO, NO2, HNO3, and SO2 from the OMI, SCIAMACHY, GOME-2, TES, MLS, and MOPITT instruments. The evaluation results demonstrate the capability of the reanalysis products to improve understanding of the processes controlling variations in atmospheric composition, including long-term changes in air quality and emissions.
Ilann Bourgeois, Jeff Peischl, Chelsea R. Thompson, Kenneth C. Aikin, Teresa Campos, Hannah Clark, Róisín Commane, Bruce Daube, Glenn W. Diskin, James W. Elkins, Ru-Shan Gao, Audrey Gaudel, Eric J. Hintsa, Bryan J. Johnson, Rigel Kivi, Kathryn McKain, Fred L. Moore, David D. Parrish, Richard Querel, Eric Ray, Ricardo Sánchez, Colm Sweeney, David W. Tarasick, Anne M. Thompson, Valérie Thouret, Jacquelyn C. Witte, Steve C. Wofsy, and Thomas B. Ryerson
Atmos. Chem. Phys., 20, 10611–10635, https://doi.org/10.5194/acp-20-10611-2020, https://doi.org/10.5194/acp-20-10611-2020, 2020
Li Zhang, Meiyun Lin, Andrew O. Langford, Larry W. Horowitz, Christoph J. Senff, Elizabeth Klovenski, Yuxuan Wang, Raul J. Alvarez II, Irina Petropavlovskikh, Patrick Cullis, Chance W. Sterling, Jeff Peischl, Thomas B. Ryerson, Steven S. Brown, Zachary C. J. Decker, Guillaume Kirgis, and Stephen Conley
Atmos. Chem. Phys., 20, 10379–10400, https://doi.org/10.5194/acp-20-10379-2020, https://doi.org/10.5194/acp-20-10379-2020, 2020
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Measuring and quantifying the sources of elevated springtime ozone in the southwestern US is challenging but relevant to the implications for control policy. Here we use intensive field measurements and two global models to study ozone sources in the region. We find that ozone from the stratosphere, wildfires, and Asia is an important source of high-ozone events in the region. Our analysis also helps understand the uncertainties in ozone simulations with individual models.
Srijana Lama, Sander Houweling, K. Folkert Boersma, Henk Eskes, Ilse Aben, Hugo A. C. Denier van der Gon, Maarten C. Krol, Han Dolman, Tobias Borsdorff, and Alba Lorente
Atmos. Chem. Phys., 20, 10295–10310, https://doi.org/10.5194/acp-20-10295-2020, https://doi.org/10.5194/acp-20-10295-2020, 2020
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Rapid urbanization has increased the consumption of fossil fuel, contributing the degradation of urban air quality. Burning efficiency is a major factor determining the impact of fuel burning on the environment. We quantify the burning efficiency of fossil fuel use over six megacities using satellite remote sensing data. City governance can use these results to understand air pollution scenarios and to formulate effective air pollution control strategies.
Xiao Lu, Lin Zhang, Tongwen Wu, Michael S. Long, Jun Wang, Daniel J. Jacob, Fang Zhang, Jie Zhang, Sebastian D. Eastham, Lu Hu, Lei Zhu, Xiong Liu, and Min Wei
Geosci. Model Dev., 13, 3817–3838, https://doi.org/10.5194/gmd-13-3817-2020, https://doi.org/10.5194/gmd-13-3817-2020, 2020
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This study presents the development and evaluation of a new climate chemistry model, BCC-GEOS-Chem v1.0, which couples the GEOS-Chem chemical transport model as an atmospheric chemistry component in the Beijing Climate Center atmospheric general circulation model. A 3-year (2012–2014) simulation of BCC-GEOS-Chem v1.0 shows that the model captures well the spatiotemporal distributions of tropospheric ozone, other gaseous pollutants, and aerosols.
Erik van Schaik, Maurits L. Kooreman, Piet Stammes, L. Gijsbert Tilstra, Olaf N. E. Tuinder, Abram F. J. Sanders, Willem W. Verstraeten, Rüdiger Lang, Alessandra Cacciari, Joanna Joiner, Wouter Peters, and K. Folkert Boersma
Atmos. Meas. Tech., 13, 4295–4315, https://doi.org/10.5194/amt-13-4295-2020, https://doi.org/10.5194/amt-13-4295-2020, 2020
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With our improved algorithm we have generated a stable, long-term dataset of fluorescence measurements from the GOME-2A satellite instrument. In this study we determined a correction for the degradation of GOME-2A in orbit and applied this correction along with other improvements to our SIFTER v2 retrieval algorithm. The result is a coherent dataset of daily and monthly averaged fluorescence values for the period 2007–2018 to track worldwide changes in photosynthetic activity by vegetation.
Mengyao Liu, Jintai Lin, Hao Kong, K. Folkert Boersma, Henk Eskes, Yugo Kanaya, Qin He, Xin Tian, Kai Qin, Pinhua Xie, Robert Spurr, Ruijing Ni, Yingying Yan, Hongjian Weng, and Jingxu Wang
Atmos. Meas. Tech., 13, 4247–4259, https://doi.org/10.5194/amt-13-4247-2020, https://doi.org/10.5194/amt-13-4247-2020, 2020
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Nitrogen oxides (NOx = NO + NO2) are important air pollutants in the troposphere and play crucial roles in the formation of ozone and particulate matter. The recently launched TROPOspheric Monitoring Instrument (TROPOMI) provides an opportunity to retrieve tropospheric concentrations of nitrogen dioxide (NO2) at an unprecedented high horizontal resolution. This work presents a new NO2 retrieval product over East Asia and further quantifies key factors affecting the retrieval, including aerosol.
Ifayoyinsola Ibikunle, Andreas Beyersdorf, Pedro Campuzano-Jost, Chelsea Corr, John D. Crounse, Jack Dibb, Glenn Diskin, Greg Huey, Jose-Luis Jimenez, Michelle J. Kim, Benjamin A. Nault, Eric Scheuer, Alex Teng, Paul O. Wennberg, Bruce Anderson, James Crawford, Rodney Weber, and Athanasios Nenes
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-501, https://doi.org/10.5194/acp-2020-501, 2020
Publication in ACP not foreseen
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Analysis of observations over South Korea during the NASA/NIER
KORUS-AQ field campaign show that aerosol is fairly acidic (mean pH 2.43 ± 0.68). Aerosol formation is always sensitive to HNO3 levels, especially in highly polluted regions, while it is only exclusively sensitive to NH3 in some rural/remote regions. Nitrate levels accumulate because dry deposition velocity is low. HNO3 reductions achieved by NOx controls can be the most effective PM reduction strategy for all conditions observed.
Sarah A. Strode, James S. Wang, Michael Manyin, Bryan Duncan, Ryan Hossaini, Christoph A. Keller, Sylvia E. Michel, and James W. C. White
Atmos. Chem. Phys., 20, 8405–8419, https://doi.org/10.5194/acp-20-8405-2020, https://doi.org/10.5194/acp-20-8405-2020, 2020
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The 13C : 12C isotopic ratio in methane (CH4) provides information about CH4 sources, but loss of CH4 by reaction with OH and chlorine (Cl) also affects this ratio. Tropospheric Cl provides a small and uncertain sink for CH4 but has a large effect on its isotopic ratio. We use the GEOS model with several different Cl fields to test the sensitivity of methane's isotopic composition to tropospheric Cl. Cl affects the global mean, hemispheric gradient, and seasonal cycle of the isotopic ratio.
Haipeng Lin, Xu Feng, Tzung-May Fu, Heng Tian, Yaping Ma, Lijuan Zhang, Daniel J. Jacob, Robert M. Yantosca, Melissa P. Sulprizio, Elizabeth W. Lundgren, Jiawei Zhuang, Qiang Zhang, Xiao Lu, Lin Zhang, Lu Shen, Jianping Guo, Sebastian D. Eastham, and Christoph A. Keller
Geosci. Model Dev., 13, 3241–3265, https://doi.org/10.5194/gmd-13-3241-2020, https://doi.org/10.5194/gmd-13-3241-2020, 2020
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Online coupling of meteorology and chemistry models often presents maintenance issues with hard-wired coding. We present WRF-GC, an one-way online coupling of the WRF meteorological model and GEOS-Chem atmospheric chemistry model for regional atmospheric chemistry and air quality modeling. Our coupling structure allows future versions of either parent model to be immediately integrated into WRF-GC. The WRF-GC model was able to well reproduce regional PM2.5 with greater computational efficiency.
Peter D. Ivatt and Mathew J. Evans
Atmos. Chem. Phys., 20, 8063–8082, https://doi.org/10.5194/acp-20-8063-2020, https://doi.org/10.5194/acp-20-8063-2020, 2020
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We investigate the potential of using a decision tree algorithm to identify and correct the tropospheric ozone bias in a chemical transport model. We train the algorithm on 2010–2015 ground and column observation data and test the algorithm on the 2016–2017 data using the ground data as well as independent flight data. We find the algorithm is successfully able to identify and correct the bias, improving the model performance.
Ying Li, Douglas A. Day, Harald Stark, Jose L. Jimenez, and Manabu Shiraiwa
Atmos. Chem. Phys., 20, 8103–8122, https://doi.org/10.5194/acp-20-8103-2020, https://doi.org/10.5194/acp-20-8103-2020, 2020
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Viscosity is an important property of organic aerosols, but viscosity measurements of ambient organic aerosols are scarce. We developed a method to predict glass transition temperatures using volatility and the atomic oxygen-to-carbon ratio. The method was applied to field observations of volatility distributions to predict viscosity of ambient organic aerosols, yielding consistent results with ambient particle phase-state measurements and global simulations.
Steven Compernolle, Tijl Verhoelst, Gaia Pinardi, José Granville, Daan Hubert, Arno Keppens, Sander Niemeijer, Bruno Rino, Alkis Bais, Steffen Beirle, Folkert Boersma, John P. Burrows, Isabelle De Smedt, Henk Eskes, Florence Goutail, François Hendrick, Alba Lorente, Andrea Pazmino, Ankie Piters, Enno Peters, Jean-Pierre Pommereau, Julia Remmers, Andreas Richter, Jos van Geffen, Michel Van Roozendael, Thomas Wagner, and Jean-Christopher Lambert
Atmos. Chem. Phys., 20, 8017–8045, https://doi.org/10.5194/acp-20-8017-2020, https://doi.org/10.5194/acp-20-8017-2020, 2020
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Tropospheric and stratospheric NO2 columns from the OMI QA4ECV NO2 satellite product are validated by comparison with ground-based measurements at 11 sites. The OMI stratospheric column has a small negative bias, and the OMI tropospheric column has a stronger negative bias relative to the ground-based data. Discrepancies are attributed to comparison errors (e.g. difference in horizontal smoothing) and measurement errors (e.g. clouds, aerosols, vertical smoothing and a priori profile assumptions).
Katherine R. Travis, Colette L. Heald, Hannah M. Allen, Eric C. Apel, Stephen R. Arnold, Donald R. Blake, William H. Brune, Xin Chen, Róisín Commane, John D. Crounse, Bruce C. Daube, Glenn S. Diskin, James W. Elkins, Mathew J. Evans, Samuel R. Hall, Eric J. Hintsa, Rebecca S. Hornbrook, Prasad S. Kasibhatla, Michelle J. Kim, Gan Luo, Kathryn McKain, Dylan B. Millet, Fred L. Moore, Jeffrey Peischl, Thomas B. Ryerson, Tomás Sherwen, Alexander B. Thames, Kirk Ullmann, Xuan Wang, Paul O. Wennberg, Glenn M. Wolfe, and Fangqun Yu
Atmos. Chem. Phys., 20, 7753–7781, https://doi.org/10.5194/acp-20-7753-2020, https://doi.org/10.5194/acp-20-7753-2020, 2020
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Atmospheric models overestimate the rate of removal of trace gases by the hydroxyl radical (OH). This is a concern for studies of the climate and air quality impacts of human activities. Here, we evaluate the performance of a commonly used model of atmospheric chemistry against data from the NASA Atmospheric Tomography Mission (ATom) over the remote oceans where models have received little validation. The model is generally successful, suggesting that biases in OH may be a concern over land.
Jiayue Huang, Lyatt Jaeglé, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mat J. Evans, Nicolas Theys, and Sungyeon Choi
Atmos. Chem. Phys., 20, 7335–7358, https://doi.org/10.5194/acp-20-7335-2020, https://doi.org/10.5194/acp-20-7335-2020, 2020
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Large-scale enhancements of tropospheric BrO and the depletion of surface ozone are often observed in the springtime Arctic. Here, we use a chemical transport model to examine the role of sea salt aerosol from blowing snow in explaining these phenomena. We find that our simulation can account for the spatiotemporal variability of satellite observations of BrO. However, the model has difficulty in producing the magnitude of observed ozone depletion events.
Manuela van Pinxteren, Khanneh Wadinga Fomba, Nadja Triesch, Christian Stolle, Oliver Wurl, Enno Bahlmann, Xianda Gong, Jens Voigtländer, Heike Wex, Tiera-Brandy Robinson, Stefan Barthel, Sebastian Zeppenfeld, Erik Hans Hoffmann, Marie Roveretto, Chunlin Li, Benoit Grosselin, Veronique Daële, Fabian Senf, Dominik van Pinxteren, Malena Manzi, Nicolás Zabalegui, Sanja Frka, Blaženka Gašparović, Ryan Pereira, Tao Li, Liang Wen, Jiarong Li, Chao Zhu, Hui Chen, Jianmin Chen, Björn Fiedler, Wolf von Tümpling, Katie Alana Read, Shalini Punjabi, Alastair Charles Lewis, James Roland Hopkins, Lucy Jane Carpenter, Ilka Peeken, Tim Rixen, Detlef Schulz-Bull, María Eugenia Monge, Abdelwahid Mellouki, Christian George, Frank Stratmann, and Hartmut Herrmann
Atmos. Chem. Phys., 20, 6921–6951, https://doi.org/10.5194/acp-20-6921-2020, https://doi.org/10.5194/acp-20-6921-2020, 2020
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An introduction to a comprehensive field campaign performed at the Cape Verde Atmospheric Observatory regarding ocean–atmosphere interactions is given. Chemical, physical, biological and meteorological techniques were applied, and measurements of bulk water, the sea surface microlayer, cloud water and ambient aerosol particles took place. Oceanic compounds were found to be transferred to atmospheric aerosol and to the cloud level; however, sea spray contributions to CCN and INPs were limited.
Pablo E. Saide, Meng Gao, Zifeng Lu, Daniel L. Goldberg, David G. Streets, Jung-Hun Woo, Andreas Beyersdorf, Chelsea A. Corr, Kenneth L. Thornhill, Bruce Anderson, Johnathan W. Hair, Amin R. Nehrir, Glenn S. Diskin, Jose L. Jimenez, Benjamin A. Nault, Pedro Campuzano-Jost, Jack Dibb, Eric Heim, Kara D. Lamb, Joshua P. Schwarz, Anne E. Perring, Jhoon Kim, Myungje Choi, Brent Holben, Gabriele Pfister, Alma Hodzic, Gregory R. Carmichael, Louisa Emmons, and James H. Crawford
Atmos. Chem. Phys., 20, 6455–6478, https://doi.org/10.5194/acp-20-6455-2020, https://doi.org/10.5194/acp-20-6455-2020, 2020
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Air quality forecasts over the Korean Peninsula captured aerosol optical depth but largely overpredicted surface PM during a Chinese haze transport event. Model deficiency was related to the calculation of optical properties. In order to improve it, aerosol size representation needs to be refined in the calculations, and the representation of aerosol properties, such as size distribution, chemical composition, refractive index, hygroscopicity parameter, and density, needs to be improved.
Lu Shen, Daniel J. Jacob, Mauricio Santillana, Xuan Wang, and Wei Chen
Geosci. Model Dev., 13, 2475–2486, https://doi.org/10.5194/gmd-13-2475-2020, https://doi.org/10.5194/gmd-13-2475-2020, 2020
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Chemical mechanisms in air quality models tend to get more complicated with time, reflecting both increasing knowledge and the need for greater scope. This objectively improves the models but increases the computational burden. In this work, we present an approach that can reduce the computational cost of chemical integration by 30–40 % while maintaining an accuracy better than 1 %. It retains the complexity of the full mechanism where it is needed and preserves full diagnostic information.
Camille Mouchel-Vallon, Julia Lee-Taylor, Alma Hodzic, Paulo Artaxo, Bernard Aumont, Marie Camredon, David Gurarie, Jose-Luis Jimenez, Donald H. Lenschow, Scot T. Martin, Janaina Nascimento, John J. Orlando, Brett B. Palm, John E. Shilling, Manish Shrivastava, and Sasha Madronich
Atmos. Chem. Phys., 20, 5995–6014, https://doi.org/10.5194/acp-20-5995-2020, https://doi.org/10.5194/acp-20-5995-2020, 2020
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The GoAmazon 2014/5 field campaign took place near the city of Manaus, Brazil, isolated in the Amazon rainforest, to study the impacts of urban pollution on natural air masses. We simulated this campaign with an extremely detailed organic chemistry model to understand how the city would affect the growth and composition of natural aerosol particles. Discrepancies between the model and the measurements indicate that the chemistry of naturally emitted organic compounds is still poorly understood.
Sungyeon Choi, Lok N. Lamsal, Melanie Follette-Cook, Joanna Joiner, Nickolay A. Krotkov, William H. Swartz, Kenneth E. Pickering, Christopher P. Loughner, Wyat Appel, Gabriele Pfister, Pablo E. Saide, Ronald C. Cohen, Andrew J. Weinheimer, and Jay R. Herman
Atmos. Meas. Tech., 13, 2523–2546, https://doi.org/10.5194/amt-13-2523-2020, https://doi.org/10.5194/amt-13-2523-2020, 2020
Andrew T. Lambe, Ezra C. Wood, Jordan E. Krechmer, Francesca Majluf, Leah R. Williams, Philip L. Croteau, Manuela Cirtog, Anaïs Féron, Jean-Eudes Petit, Alexandre Albinet, Jose L. Jimenez, and Zhe Peng
Atmos. Meas. Tech., 13, 2397–2411, https://doi.org/10.5194/amt-13-2397-2020, https://doi.org/10.5194/amt-13-2397-2020, 2020
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We present a new method to continuously generate N2O5 in the gas phase that is injected into a reactor where it decomposes to generate nitrate radicals (NO3). To assess the applicability of the method towards different chemical systems, we present experimental and model characterization of the integrated NO3 exposure and other metrics as a function of operating conditions. We demonstrate the method by characterizing secondary organic aerosol particles generated from the β-pinene + NO3 reaction.
Andrew W. Rollins, Pamela S. Rickly, Ru-Shan Gao, Thomas B. Ryerson, Steven S. Brown, Jeff Peischl, and Ilann Bourgeois
Atmos. Meas. Tech., 13, 2425–2439, https://doi.org/10.5194/amt-13-2425-2020, https://doi.org/10.5194/amt-13-2425-2020, 2020
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Nitric oxide (NO) is a key atmospheric constituent controlling atmospheric oxidation chemistry and tropospheric ozone formation. Existing instrumentation capable of quantifying NO at very low mixing ratios is uncommon and typically relies on chemiluminescence. We describe and demonstrate a new laser-based technique (LIF) with significant practical and technical advantages to CL. This technique is expected to allow for advances in understanding of atmospheric radical chemistry.
Thibaud M. Fritz, Sebastian D. Eastham, Raymond L. Speth, and Steven R. H. Barrett
Atmos. Chem. Phys., 20, 5697–5727, https://doi.org/10.5194/acp-20-5697-2020, https://doi.org/10.5194/acp-20-5697-2020, 2020
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Aircraft exhaust drives formation of ozone and is a dominant anthropogenic influence in the upper troposphere. These impacts are mitigated by non-linear chemistry inside the aircraft plume, which cuts off part of the ozone production pathway and reduces the long-term impact of aircraft in a way which is not captured by current models. The ice clouds which form in aircraft exhaust ("contrails") also play a role, converting emitted nitrogen oxides into more stable forms such as nitric acid.
Sophia Brilke, Nikolaus Fölker, Thomas Müller, Konrad Kandler, Xianda Gong, Jeff Peischl, Bernadett Weinzierl, and Paul M. Winkler
Atmos. Chem. Phys., 20, 5645–5656, https://doi.org/10.5194/acp-20-5645-2020, https://doi.org/10.5194/acp-20-5645-2020, 2020
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Atmospheric particle size distributions with the focus on freshly nucleated particles were measured during the A-LIFE field experiment in Cyprus. A DMA-train was set up for the first time in an atmospheric environment and captures the sub-10 nm particle dynamics. Several new particle formation (NPF) events are studied in detail, of which some did not show particle growth beyond 10 nm indicating that NPF may occur more frequently than estimated when the sub-10 nm size range is not covered.
Xiaoyi Zhao, Debora Griffin, Vitali Fioletov, Chris McLinden, Alexander Cede, Martin Tiefengraber, Moritz Müller, Kristof Bognar, Kimberly Strong, Folkert Boersma, Henk Eskes, Jonathan Davies, Akira Ogyu, and Sum Chi Lee
Atmos. Meas. Tech., 13, 2131–2159, https://doi.org/10.5194/amt-13-2131-2020, https://doi.org/10.5194/amt-13-2131-2020, 2020
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Pandora NO2 measurements made at three sites located in the Toronto area are used to evaluate the TROPOspheric Monitoring Instrument (TROPOMI) NO2 data products, including standard NO2 and research data developed using a high-resolution regional air quality forecast model. TROPOMI pixels located upwind and downwind from the Pandora sites were analyzed by a new wind-based validation method, which revealed the spatial patterns of local and transported emissions and regional air quality changes.
Alma Hodzic, Pedro Campuzano-Jost, Huisheng Bian, Mian Chin, Peter R. Colarco, Douglas A. Day, Karl D. Froyd, Bernd Heinold, Duseong S. Jo, Joseph M. Katich, John K. Kodros, Benjamin A. Nault, Jeffrey R. Pierce, Eric Ray, Jacob Schacht, Gregory P. Schill, Jason C. Schroder, Joshua P. Schwarz, Donna T. Sueper, Ina Tegen, Simone Tilmes, Kostas Tsigaridis, Pengfei Yu, and Jose L. Jimenez
Atmos. Chem. Phys., 20, 4607–4635, https://doi.org/10.5194/acp-20-4607-2020, https://doi.org/10.5194/acp-20-4607-2020, 2020
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Organic aerosol (OA) is a key source of uncertainty in aerosol climate effects. We present the first pole-to-pole OA characterization during the NASA Atmospheric Tomography aircraft mission. OA has a strong seasonal and zonal variability, with the highest levels in summer and over fire-influenced regions and the lowest ones in the southern high latitudes. We show that global models predict the OA distribution well but not the relative contribution of OA emissions vs. chemical production.
Ryan J. Pound, Tomás Sherwen, Detlev Helmig, Lucy J. Carpenter, and Mat J. Evans
Atmos. Chem. Phys., 20, 4227–4239, https://doi.org/10.5194/acp-20-4227-2020, https://doi.org/10.5194/acp-20-4227-2020, 2020
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Ozone is an important pollutant with impacts on health and the environment. Ozone is lost to plants, land and the oceans. Loss to the ocean is slow compared to all other types of land cover and has not received as much attention. We build on previous work to more accurately model ozone loss to the ocean. We find changes in the concentration of ozone over the oceans, notably the Southern Ocean, which improves model performance.
Alexander B. Thames, William H. Brune, David O. Miller, Hannah M. Allen, Eric C. Apel, Donald R. Blake, T. Paul Bui, Roisin Commane, John D. Crounse, Bruce C. Daube, Glenn S. Diskin, Joshua P. DiGangi, James W. Elkins, Samuel R. Hall, Thomas F. Hanisco, Reem A. Hannun, Eric Hintsa, Rebecca S. Hornbrook, Michelle J. Kim, Kathryn McKain, Fred L. Moore, Julie M. Nicely, Jeffrey Peischl, Thomas B. Ryerson, Jason M. St. Clair, Colm Sweeney, Alex Teng, Chelsea R. Thompson, Kirk Ullmann, Paul O. Wennberg, and Glenn M. Wolfe
Atmos. Chem. Phys., 20, 4013–4029, https://doi.org/10.5194/acp-20-4013-2020, https://doi.org/10.5194/acp-20-4013-2020, 2020
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Oceans and the atmosphere exchange volatile gases that react with the hydroxyl radical (OH). During a NASA airborne study, measurements of the total frequency of OH reactions, called the OH reactivity, were made in the marine boundary layer of the Atlantic and Pacific oceans. The measured OH reactivity often exceeded the OH reactivity calculated from measured chemical species. This missing OH reactivity appears to be from unmeasured volatile organic compounds coming out of the ocean.
Becky Alexander, Tomás Sherwen, Christopher D. Holmes, Jenny A. Fisher, Qianjie Chen, Mat J. Evans, and Prasad Kasibhatla
Atmos. Chem. Phys., 20, 3859–3877, https://doi.org/10.5194/acp-20-3859-2020, https://doi.org/10.5194/acp-20-3859-2020, 2020
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Nitrogen oxides are important for the formation of tropospheric oxidants and are removed from the atmosphere mainly through the formation of nitrate. We compare observations of the oxygen isotopes of nitrate with a global model to test our understanding of the chemistry nitrate formation. We use the model to quantify nitrate formation pathways in the atmosphere and identify key uncertainties and their relevance for the oxidation capacity of the atmosphere.
Jos van Geffen, K. Folkert Boersma, Henk Eskes, Maarten Sneep, Mark ter Linden, Marina Zara, and J. Pepijn Veefkind
Atmos. Meas. Tech., 13, 1315–1335, https://doi.org/10.5194/amt-13-1315-2020, https://doi.org/10.5194/amt-13-1315-2020, 2020
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The Tropospheric Monitoring Instrument (TROPOMI) provides atmospheric trace gase and cloud and aerosol property measurements at unprecedented spatial resolution. This study focusses on the TROPOMI NO2 slant column density (SCD) retrieval: the retrieval method used, the stability of and uncertainties in the SCDs, and a comparison with Ozone Monitoring Instrument (OMI) NO2 SCDs. TROPOMI shows a superior performance compared to OMI/QA4ECV and operates as anticipated from instrument specifications.
Tia R. Scarpelli, Daniel J. Jacob, Joannes D. Maasakkers, Melissa P. Sulprizio, Jian-Xiong Sheng, Kelly Rose, Lucy Romeo, John R. Worden, and Greet Janssens-Maenhout
Earth Syst. Sci. Data, 12, 563–575, https://doi.org/10.5194/essd-12-563-2020, https://doi.org/10.5194/essd-12-563-2020, 2020
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Methane, a potent greenhouse gas, is emitted through the exploitation of oil, gas, and coal resources, and many efforts to reduce emissions have targeted these sources. We have created a global inventory of oil, gas, and coal methane emissions based on country reporting to the United Nations. The inventory can be used along with satellite observations of methane to better understand the contribution of these sources to global emissions and to identify potential biases in emissions reporting.
Sidhant J. Pai, Colette L. Heald, Jeffrey R. Pierce, Salvatore C. Farina, Eloise A. Marais, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Ann M. Middlebrook, Hugh Coe, John E. Shilling, Roya Bahreini, Justin H. Dingle, and Kennedy Vu
Atmos. Chem. Phys., 20, 2637–2665, https://doi.org/10.5194/acp-20-2637-2020, https://doi.org/10.5194/acp-20-2637-2020, 2020
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Aerosols in the atmosphere have significant health and climate impacts. Organic aerosol (OA) accounts for a large fraction of the total aerosol burden, but models have historically struggled to accurately simulate it. This study compares two very different OA model schemes and evaluates them against a suite of globally distributed airborne measurements with the goal of providing insight into the strengths and weaknesses of each approach across different environments.
Erin R. Delaria and Ronald C. Cohen
Atmos. Chem. Phys., 20, 2123–2141, https://doi.org/10.5194/acp-20-2123-2020, https://doi.org/10.5194/acp-20-2123-2020, 2020
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Uptake of nitrogen dioxide (NO2) through pores in the surfaces of leaves has been identified as a significant, but inadequately understood, loss process of atmospheric nitrogen oxides. We have constructed a simple model for examining the impact of NO2 foliar uptake on the atmospheric chemistry of nitrogen oxides. We show that an accurate representation in atmospheric models of the effects of weather and soil conditions on leaf NO2 uptake may be important for accurately predicting NO2 deposition.
Therese S. Carter, Colette L. Heald, Jose L. Jimenez, Pedro Campuzano-Jost, Yutaka Kondo, Nobuhiro Moteki, Joshua P. Schwarz, Christine Wiedinmyer, Anton S. Darmenov, Arlindo M. da Silva, and Johannes W. Kaiser
Atmos. Chem. Phys., 20, 2073–2097, https://doi.org/10.5194/acp-20-2073-2020, https://doi.org/10.5194/acp-20-2073-2020, 2020
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Fires and the smoke they emit impact air quality, health, and climate, but the abundance and properties of smoke remain uncertain and poorly constrained. To explore this, we compare model simulations driven by four commonly-used fire emission inventories with surface, aloft, and satellite observations. We show that across inventories smoke emissions differ by factors of 4 to 7 over North America, challenging our ability to accurately characterize the impact of smoke on air quality and climate.
Viral Shah, Daniel J. Jacob, Ke Li, Rachel F. Silvern, Shixian Zhai, Mengyao Liu, Jintai Lin, and Qiang Zhang
Atmos. Chem. Phys., 20, 1483–1495, https://doi.org/10.5194/acp-20-1483-2020, https://doi.org/10.5194/acp-20-1483-2020, 2020
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We analyze 15 years of satellite observations of nitrogen dioxide (NO2) and use an atmospheric chemistry model to understand the seasonal changes and trends in nitrogen oxides (NOx) over China. We show that the seasonal changes in NO2 occur due to changes in the NOx oxidation lifetime. We find that Chinese NOx emissions peaked in 2011 and had decreased by about 25 % by 2018. But the decrease in NO2 in winter was larger, likely because of a simultaneous decrease in the NOx oxidation lifetime.
Michal T. Filus, Elliot L. Atlas, Maria A. Navarro, Elena Meneguz, David Thomson, Matthew J. Ashfold, Lucy J. Carpenter, Stephen J. Andrews, and Neil R. P. Harris
Atmos. Chem. Phys., 20, 1163–1181, https://doi.org/10.5194/acp-20-1163-2020, https://doi.org/10.5194/acp-20-1163-2020, 2020
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The effectiveness of transport of short-lived halocarbons to the upper troposphere and lower stratosphere remains an important unknown in quantifying the supply of ozone-depleting substances to the stratosphere. In early 2014, a major field campaign in Guam in the western Pacific, involving UK and US research aircraft, sampled the tropical troposphere and lower stratosphere. The resulting measurements of CH3I, CHBr3 and CH2Br2 are compared here with calculations from a Lagrangian model.
Alexander J. Turner, Philipp Köhler, Troy S. Magney, Christian Frankenberg, Inez Fung, and Ronald C. Cohen
Biogeosciences, 17, 405–422, https://doi.org/10.5194/bg-17-405-2020, https://doi.org/10.5194/bg-17-405-2020, 2020
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We present the highest resolution solar-induced chlorophyll fluorescence (SIF) dataset from satellite measurements, providing previously unobservable phenomena related to plant photosynthesis. We find a strong correspondence between TROPOMI SIF and AmeriFlux GPP. We then observe a double peak in the seasonality of California's photosynthesis, not seen by traditional vegetation indices (e.g., MODIS). This is further corroborated by EOF/PC analysis.
Le Kuai, Kevin W. Bowman, Kazuyuki Miyazaki, Makoto Deushi, Laura Revell, Eugene Rozanov, Fabien Paulot, Sarah Strode, Andrew Conley, Jean-François Lamarque, Patrick Jöckel, David A. Plummer, Luke D. Oman, Helen Worden, Susan Kulawik, David Paynter, Andrea Stenke, and Markus Kunze
Atmos. Chem. Phys., 20, 281–301, https://doi.org/10.5194/acp-20-281-2020, https://doi.org/10.5194/acp-20-281-2020, 2020
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The tropospheric ozone increase from pre-industrial to the present day leads to a radiative forcing. The top-of-atmosphere outgoing fluxes at the ozone band are controlled by ozone, water vapor, and temperature. We demonstrate a method to attribute the models’ flux biases to these key players using satellite-constrained instantaneous radiative kernels. The largest spread between models is found in the tropics, mainly driven by ozone and then water vapor.
Paul S. Romer Present, Azimeh Zare, and Ronald C. Cohen
Atmos. Chem. Phys., 20, 267–279, https://doi.org/10.5194/acp-20-267-2020, https://doi.org/10.5194/acp-20-267-2020, 2020
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The chemistry of nitrogen oxides (NOx) affects both air quality and climate through its role in the production of ozone and secondary aerosols. We find that recent changes in emissions have caused a significant shift in the chemical loss of NOx away from direct production of HNO3 and towards production of organic nitrates. This shift is leading to a flatter distribution of NOx across the United States and helping transform air pollution from a local issue into a broader regional concern.
Fei Liu, Bryan N. Duncan, Nickolay A. Krotkov, Lok N. Lamsal, Steffen Beirle, Debora Griffin, Chris A. McLinden, Daniel L. Goldberg, and Zifeng Lu
Atmos. Chem. Phys., 20, 99–116, https://doi.org/10.5194/acp-20-99-2020, https://doi.org/10.5194/acp-20-99-2020, 2020
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We present a novel method to infer CO2 emissions from individual power plants, based on satellite observations of co-emitted NO2. We find that the CO2 emissions estimated by our satellite-based method during 2005–2017 are in reasonable agreement with the CEMS measurements for US power plants. The broader implication of our methodology is that it has the potential to provide an additional constraint on CO2 emissions from power plants in regions of the world without reliable emissions accounting.
Sophie L. Haslett, Jonathan W. Taylor, Mathew Evans, Eleanor Morris, Bernhard Vogel, Alima Dajuma, Joel Brito, Anneke M. Batenburg, Stephan Borrmann, Johannes Schneider, Christiane Schulz, Cyrielle Denjean, Thierry Bourrianne, Peter Knippertz, Régis Dupuy, Alfons Schwarzenböck, Daniel Sauer, Cyrille Flamant, James Dorsey, Ian Crawford, and Hugh Coe
Atmos. Chem. Phys., 19, 15217–15234, https://doi.org/10.5194/acp-19-15217-2019, https://doi.org/10.5194/acp-19-15217-2019, 2019
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Three aircraft datasets from the DACCIWA campaign in summer 2016 are used here to show there is a background mass of pollution present in the lower atmosphere in southern West Africa. We suggest that this likely comes from biomass burning in central and southern Africa, which has been carried into the region over the Atlantic Ocean. This would have a negative health impact on populations living near the coast and may alter the impact of growing city emissions on cloud formation and the monsoon.
Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Kanako Sekimoto, Bin Yuan, Jessica B. Gilman, David H. Hagan, Vanessa Selimovic, Kyle J. Zarzana, Steven S. Brown, James M. Roberts, Markus Müller, Robert Yokelson, Armin Wisthaler, Jordan E. Krechmer, Jose L. Jimenez, Christopher Cappa, Jesse H. Kroll, Joost de Gouw, and Carsten Warneke
Atmos. Chem. Phys., 19, 14875–14899, https://doi.org/10.5194/acp-19-14875-2019, https://doi.org/10.5194/acp-19-14875-2019, 2019
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Wildfire emissions significantly contribute to adverse air quality; however, the chemical processes that lead to hazardous pollutants, such as ozone, are not fully understood. In this study, we describe laboratory experiments where we simulate the atmospheric chemistry of smoke emitted from a range of biomass fuels. We show that certain understudied compounds, such as furans and phenolic compounds, are significant contributors to pollutants formed as a result of typical atmospheric oxidation.
Karl D. Froyd, Daniel M. Murphy, Charles A. Brock, Pedro Campuzano-Jost, Jack E. Dibb, Jose-Luis Jimenez, Agnieszka Kupc, Ann M. Middlebrook, Gregory P. Schill, Kenneth L. Thornhill, Christina J. Williamson, James C. Wilson, and Luke D. Ziemba
Atmos. Meas. Tech., 12, 6209–6239, https://doi.org/10.5194/amt-12-6209-2019, https://doi.org/10.5194/amt-12-6209-2019, 2019
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Single-particle mass spectrometer (SPMS) instruments characterize the composition of individual aerosol particles in real time. We present a new method that combines SPMS composition with independently measured particle size distributions to determine absolute number, surface area, volume, and mass concentrations of mineral dust, biomass burning, sea salt, and other climate-relevant atmospheric particle types, with a fast time response applicable to aircraft sampling.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Didier A. Hauglustaine, Sophie Szopa, Ann R. Stavert, Nathan Luke Abraham, Alex T. Archibald, Slimane Bekki, Makoto Deushi, Patrick Jöckel, Béatrice Josse, Douglas Kinnison, Ole Kirner, Virginie Marécal, Fiona M. O'Connor, David A. Plummer, Laura E. Revell, Eugene Rozanov, Andrea Stenke, Sarah Strode, Simone Tilmes, Edward J. Dlugokencky, and Bo Zheng
Atmos. Chem. Phys., 19, 13701–13723, https://doi.org/10.5194/acp-19-13701-2019, https://doi.org/10.5194/acp-19-13701-2019, 2019
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The role of hydroxyl radical changes in methane trends is debated, hindering our understanding of the methane cycle. This study quantifies how uncertainties in the hydroxyl radical may influence methane abundance in the atmosphere based on the inter-model comparison of hydroxyl radical fields and model simulations of CH4 abundance with different hydroxyl radical scenarios during 2000–2016. We show that hydroxyl radical changes could contribute up to 54 % of model-simulated methane biases.
Brett B. Palm, Xiaoxi Liu, Jose L. Jimenez, and Joel A. Thornton
Atmos. Meas. Tech., 12, 5829–5844, https://doi.org/10.5194/amt-12-5829-2019, https://doi.org/10.5194/amt-12-5829-2019, 2019
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We introduce a coaxial, low-pressure ion–molecule reaction (IMR) region for iodide-adduct chemical ionization mass spectrometry, designed to decrease the effects of IMR wall interactions with organic/inorganic gases. This IMR has 3–10 times shorter delay times than previous IMRs. We introduce a conceptual framework for understanding and subtracting the background signal due to analyte molecules interacting with IMR walls. This framework can be applied to other tubing and instrument systems.
Daniel H. Cusworth, Daniel J. Jacob, Daniel J. Varon, Christopher Chan Miller, Xiong Liu, Kelly Chance, Andrew K. Thorpe, Riley M. Duren, Charles E. Miller, David R. Thompson, Christian Frankenberg, Luis Guanter, and Cynthia A. Randles
Atmos. Meas. Tech., 12, 5655–5668, https://doi.org/10.5194/amt-12-5655-2019, https://doi.org/10.5194/amt-12-5655-2019, 2019
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We examine the potential for global detection of methane plumes from individual point sources with the new generation of spaceborne imaging spectrometers scheduled for launch in 2019–2025. We perform methane retrievals on simulated scenes with varying surfaces and atmospheric methane concentrations. Our results suggest that imaging spectrometers in space could play a transformative role in the future for quantifying methane emissions from point sources on a global scale.
Qindan Zhu, Joshua L. Laughner, and Ronald C. Cohen
Atmos. Chem. Phys., 19, 13067–13078, https://doi.org/10.5194/acp-19-13067-2019, https://doi.org/10.5194/acp-19-13067-2019, 2019
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Lightning NOx represents > 80 % of the NOx source in the upper troposphere. Despite its importance, lightning NOx is poorly understood. This work improves model performance in representing lighting NOx and reduces the uncertainty in satellite NO2 retrievals caused by poor representation of lightning NOx emissions in a priori assumptions.
Daun Jeong, Roger Seco, Dasa Gu, Youngro Lee, Benjamin A. Nault, Christoph J. Knote, Tom Mcgee, John T. Sullivan, Jose L. Jimenez, Pedro Campuzano-Jost, Donald R. Blake, Dianne Sanchez, Alex B. Guenther, David Tanner, L. Gregory Huey, Russell Long, Bruce E. Anderson, Samuel R. Hall, Kirk Ullmann, Hye-jung Shin, Scott C. Herndon, Youngjae Lee, Danbi Kim, Joonyoung Ahn, and Saewung Kim
Atmos. Chem. Phys., 19, 12779–12795, https://doi.org/10.5194/acp-19-12779-2019, https://doi.org/10.5194/acp-19-12779-2019, 2019
Auke J. Visser, K. Folkert Boersma, Laurens N. Ganzeveld, and Maarten C. Krol
Atmos. Chem. Phys., 19, 11821–11841, https://doi.org/10.5194/acp-19-11821-2019, https://doi.org/10.5194/acp-19-11821-2019, 2019
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Health and ecosystem impacts of O3 generally occur when O3 concentrations are highest, but most air quality models underestimate peak O3. We derived European NOx emissions based on satellite NO2 column data and evaluated the impact on model-simulated NO2 and ozone. We show that a simulation with satellite-derived NOx emissions leads to better agreement with independent in situ observations of surface NO2 and O3, which helps to reduce the model underestimations of peak ozone concentrations.
Shixian Zhai, Daniel J. Jacob, Xuan Wang, Lu Shen, Ke Li, Yuzhong Zhang, Ke Gui, Tianliang Zhao, and Hong Liao
Atmos. Chem. Phys., 19, 11031–11041, https://doi.org/10.5194/acp-19-11031-2019, https://doi.org/10.5194/acp-19-11031-2019, 2019
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Observed annual mean PM2.5 decreased by 30–50 % in China from 2013–2018. However, meteorologically PM2.5 variability complicates trend attribution. We used a stepwise multiple linear regression model to quantitatively separate contributions from anthropogenic emissions and meteorology. Results show that 88 % of the PM2.5 decrease across China is attributable to anthropogenic emission changes, and 12 % is attributable to meteorology.
Katherine R. Travis and Daniel J. Jacob
Geosci. Model Dev., 12, 3641–3648, https://doi.org/10.5194/gmd-12-3641-2019, https://doi.org/10.5194/gmd-12-3641-2019, 2019
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Models of ozone air pollution are often evaluated with the policy metric set by the EPA of the maximum daily 8 h average ozone concentration. These models may be used in policy settings to evaluate air quality regulations. However, most models have difficulty simulating how ozone varies over the course of the day, and thus the use of this metric in model evaluation is problematic. Improved representation of mixed layer dynamics and ozone loss to the surface is needed to resolve this issue.
Tomás Sherwen, Rosie J. Chance, Liselotte Tinel, Daniel Ellis, Mat J. Evans, and Lucy J. Carpenter
Earth Syst. Sci. Data, 11, 1239–1262, https://doi.org/10.5194/essd-11-1239-2019, https://doi.org/10.5194/essd-11-1239-2019, 2019
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Iodine plays an important role in the Earth system, as a nutrient to the biosphere and by changing the concentrations of climate and air-quality species. However, there are uncertainties on the magnitude of iodine’s role, and a key uncertainty is our understanding of iodide in the global sea-surface. Here we take a data-driven approach using a machine learning algorithm to convert a sparse set of sea-surface iodide observations into a spatially and temporally resolved dataset for use in models.
Leon King, Ieuan J. Roberts, Liselotte Tinel, and Lucy J. Carpenter
Ocean Sci. Discuss., https://doi.org/10.5194/os-2019-87, https://doi.org/10.5194/os-2019-87, 2019
Preprint withdrawn
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Recent studies suggest that the sea surface microlayer is ubiquitously enriched in surfactants, even at high wind speeds, which exert a control on air-sea gas exchange. These conclusions are partly based on voltammetry measurements of
surfactant activity(SA). Here, we show that the response of SA-voltammetry varies widely for different surfactants, becomes saturated above total surfactant concentrations of 1–2 mg L-1, and shows a poor correlation in natural waters with surface film pressure.
Kelvin H. Bates and Daniel J. Jacob
Atmos. Chem. Phys., 19, 9613–9640, https://doi.org/10.5194/acp-19-9613-2019, https://doi.org/10.5194/acp-19-9613-2019, 2019
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Isoprene is a highly reactive chemical released to the atmosphere by plants. Its gas-phase reactions and interactions with chemicals released by human activity have far-reaching atmospheric consequences, contributing to ozone and particulate pollution and prolonging the lifetime of methane, a potent greenhouse gas. We use global simulations with a new isoprene reaction scheme to quantify those effects and to show how recently discovered aspects of isoprene chemistry play out on a global scale.
Xin Chen, Dylan B. Millet, Hanwant B. Singh, Armin Wisthaler, Eric C. Apel, Elliot L. Atlas, Donald R. Blake, Ilann Bourgeois, Steven S. Brown, John D. Crounse, Joost A. de Gouw, Frank M. Flocke, Alan Fried, Brian G. Heikes, Rebecca S. Hornbrook, Tomas Mikoviny, Kyung-Eun Min, Markus Müller, J. Andrew Neuman, Daniel W. O'Sullivan, Jeff Peischl, Gabriele G. Pfister, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Stephen R. Shertz, Chelsea R. Thompson, Victoria Treadaway, Patrick R. Veres, James Walega, Carsten Warneke, Rebecca A. Washenfelder, Petter Weibring, and Bin Yuan
Atmos. Chem. Phys., 19, 9097–9123, https://doi.org/10.5194/acp-19-9097-2019, https://doi.org/10.5194/acp-19-9097-2019, 2019
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Volatile organic compounds (VOCs) affect air quality and modify the lifetimes of other pollutants. We combine a high-resolution 3-D atmospheric model with an ensemble of aircraft observations to perform an integrated analysis of the VOC budget over North America. We find that biogenic emissions provide the main source of VOC reactivity even in most major cities. Our findings point to key gaps in current models related to oxygenated VOCs and to the distribution of VOCs in the free troposphere.
Duseong S. Jo, Alma Hodzic, Louisa K. Emmons, Eloise A. Marais, Zhe Peng, Benjamin A. Nault, Weiwei Hu, Pedro Campuzano-Jost, and Jose L. Jimenez
Geosci. Model Dev., 12, 2983–3000, https://doi.org/10.5194/gmd-12-2983-2019, https://doi.org/10.5194/gmd-12-2983-2019, 2019
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We developed a parameterization method for IEPOX-SOA based on the detailed chemical mechanism. Our parameterizations were tested using a box model and 3-D chemical transport model, which accurately captured the spatiotemporal distribution and response to changes in emissions compared to the explicit full chemistry, while being more computationally efficient. The method developed in this study can be applied to global climate models for long-term studies with a lower computational cost.
Rachel F. Silvern, Daniel J. Jacob, Loretta J. Mickley, Melissa P. Sulprizio, Katherine R. Travis, Eloise A. Marais, Ronald C. Cohen, Joshua L. Laughner, Sungyeon Choi, Joanna Joiner, and Lok N. Lamsal
Atmos. Chem. Phys., 19, 8863–8878, https://doi.org/10.5194/acp-19-8863-2019, https://doi.org/10.5194/acp-19-8863-2019, 2019
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The US EPA reports a steady decrease in nitrogen oxide (NOx) emissions from fuel combustion over the 2005–2017 period, while satellite observations show a leveling off after 2009, suggesting emission reductions and related air quality gains have halted. We show the sustained decrease in NOx emissions is in fact consistent with observed trends in surface NO2 and ozone concentrations and that the flattening of the satellite trend reflects a growing influence from the non-anthropogenic background.
Ilana B. Pollack, Jakob Lindaas, J. Robert Roscioli, Michael Agnese, Wade Permar, Lu Hu, and Emily V. Fischer
Atmos. Meas. Tech., 12, 3717–3742, https://doi.org/10.5194/amt-12-3717-2019, https://doi.org/10.5194/amt-12-3717-2019, 2019
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A closed-path infrared absorption spectrometer was outfitted with the option for active continuous passivation for measuring large, rapid gradients in atmospheric NH3 from a research aircraft. In-flight and ground observations show utility in passivant addition for recovering instrument time response when sampling surfaces are contaminated and cannot be cleaned in a timely manner and for maintaining rapid time response in an NH3-rich and humid environment over a several-week-long field campaign.
Benjamin L. Deming, Demetrios Pagonis, Xiaoxi Liu, Douglas A. Day, Ranajit Talukdar, Jordan E. Krechmer, Joost A. de Gouw, Jose L. Jimenez, and Paul J. Ziemann
Atmos. Meas. Tech., 12, 3453–3461, https://doi.org/10.5194/amt-12-3453-2019, https://doi.org/10.5194/amt-12-3453-2019, 2019
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Losses or measurement delays of gas-phase compounds sampled through tubing are important to atmospheric science. Here we characterize 14 tubing materials by measuring the effects on step changes in organic compound concentration. We find that polymeric tubings exhibit absorptive partitioning behaviour while glass and metal tubings show adsorptive partitioning. Adsorptive materials impart complex humidity, concentration, and VOC–VOC interaction dependencies that absorptive tubings do not.
Suzane S. de Sá, Luciana V. Rizzo, Brett B. Palm, Pedro Campuzano-Jost, Douglas A. Day, Lindsay D. Yee, Rebecca Wernis, Gabriel Isaacman-VanWertz, Joel Brito, Samara Carbone, Yingjun J. Liu, Arthur Sedlacek, Stephen Springston, Allen H. Goldstein, Henrique M. J. Barbosa, M. Lizabeth Alexander, Paulo Artaxo, Jose L. Jimenez, and Scot T. Martin
Atmos. Chem. Phys., 19, 7973–8001, https://doi.org/10.5194/acp-19-7973-2019, https://doi.org/10.5194/acp-19-7973-2019, 2019
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This study investigates the impacts of urban and fire emissions on the concentration, composition, and optical properties of submicron particulate matter (PM1) in central Amazonia during the dry season. Biomass-burning and urban emissions appeared to contribute at least 80 % of brown carbon absorption while accounting for 30 % to 40 % of the organic PM1 mass concentration. Only a fraction of the 9-fold increase in mass concentration relative to the wet season was due to biomass burning.
Xiaoxi Liu, Benjamin Deming, Demetrios Pagonis, Douglas A. Day, Brett B. Palm, Ranajit Talukdar, James M. Roberts, Patrick R. Veres, Jordan E. Krechmer, Joel A. Thornton, Joost A. de Gouw, Paul J. Ziemann, and Jose L. Jimenez
Atmos. Meas. Tech., 12, 3137–3149, https://doi.org/10.5194/amt-12-3137-2019, https://doi.org/10.5194/amt-12-3137-2019, 2019
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Delays or losses of gases in sampling tubing and instrumental surfaces due to surface interactions can lead to inaccurate quantification. By sampling with several chemical ionization mass spectrometers and six tubing materials, we quantify delays of semivolatile organic compounds and small polar gases. Delay times generally increase with decreasing volatility or increasing polarity and also depend on materials. The method and results will inform inlet material selection and instrumental design.
Joannes D. Maasakkers, Daniel J. Jacob, Melissa P. Sulprizio, Tia R. Scarpelli, Hannah Nesser, Jian-Xiong Sheng, Yuzhong Zhang, Monica Hersher, A. Anthony Bloom, Kevin W. Bowman, John R. Worden, Greet Janssens-Maenhout, and Robert J. Parker
Atmos. Chem. Phys., 19, 7859–7881, https://doi.org/10.5194/acp-19-7859-2019, https://doi.org/10.5194/acp-19-7859-2019, 2019
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We use 2010–2015 satellite observations of atmospheric methane to improve estimates of methane emissions and their trends, as well as the concentration and trend of tropospheric OH (hydroxyl radical, methane's main sink). We find overestimates of Chinese coal and Middle East oil/gas emissions in the prior estimate. The 2010–2015 growth in methane is attributed to an increase in emissions from India, China, and areas with large tropical wetlands. The contribution from OH is small in comparison.
Charles A. Brock, Christina Williamson, Agnieszka Kupc, Karl D. Froyd, Frank Erdesz, Nicholas Wagner, Matthews Richardson, Joshua P. Schwarz, Ru-Shan Gao, Joseph M. Katich, Pedro Campuzano-Jost, Benjamin A. Nault, Jason C. Schroder, Jose L. Jimenez, Bernadett Weinzierl, Maximilian Dollner, ThaoPaul Bui, and Daniel M. Murphy
Atmos. Meas. Tech., 12, 3081–3099, https://doi.org/10.5194/amt-12-3081-2019, https://doi.org/10.5194/amt-12-3081-2019, 2019
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From 2016 to 2018 a NASA aircraft profiled the atmosphere from 180 m to ~12 km from the Arctic to the Antarctic over both the Pacific and Atlantic oceans. This program, ATom, sought to sample atmospheric chemical composition to compare with global climate models. We describe the how measurements of particulate matter were made during ATom, and show that the instrument performance was excellent. Data from this project can be used with confidence to evaluate models and compare with satellites.
Lu Shen, Daniel J. Jacob, Xiong Liu, Guanyu Huang, Ke Li, Hong Liao, and Tao Wang
Atmos. Chem. Phys., 19, 6551–6560, https://doi.org/10.5194/acp-19-6551-2019, https://doi.org/10.5194/acp-19-6551-2019, 2019
Lei Zhu, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Xuan Wang, Tomás Sherwen, Mat J. Evans, Qianjie Chen, Becky Alexander, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Michael Le Breton, Thomas J. Bannan, and Carl J. Percival
Atmos. Chem. Phys., 19, 6497–6507, https://doi.org/10.5194/acp-19-6497-2019, https://doi.org/10.5194/acp-19-6497-2019, 2019
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We quantify the effect of sea salt aerosol on tropospheric bromine chemistry with a new mechanistic description of the halogen chemistry in a global atmospheric chemistry model. For the first time, we are able to reproduce the observed levels of bromide activation from the sea salt aerosol in a manner consistent with bromine oxide radical measured from various platforms. Sea salt aerosol plays a far more complex role in global tropospheric chemistry than previously recognized.
Aristeidis K. Georgoulias, Ronald J. van der A, Piet Stammes, K. Folkert Boersma, and Henk J. Eskes
Atmos. Chem. Phys., 19, 6269–6294, https://doi.org/10.5194/acp-19-6269-2019, https://doi.org/10.5194/acp-19-6269-2019, 2019
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In this paper, a ∼21-year self-consistent global dataset from four different satellite sensors is compiled for the first time to study the long-term tropospheric NO2 patterns and trends. A novel method capable of detecting the year when a reversal of trends happened shows that tropospheric NO2 concentrations switched from positive to negative trends and vice versa over several regions around the globe during the last 2 decades.
Jingyuan Shao, Qianjie Chen, Yuxuan Wang, Xiao Lu, Pengzhen He, Yele Sun, Viral Shah, Randall V. Martin, Sajeev Philip, Shaojie Song, Yue Zhao, Zhouqing Xie, Lin Zhang, and Becky Alexander
Atmos. Chem. Phys., 19, 6107–6123, https://doi.org/10.5194/acp-19-6107-2019, https://doi.org/10.5194/acp-19-6107-2019, 2019
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Sulfate is a key species contributing to particle formation and growth during wintertime Chinese haze events. This study combines observations and modeling of oxygen isotope signatures in sulfate aerosol to investigate its formation mechanisms, with a focus on heterogeneous production on aerosol surface via H2O2, O3, and NO2 and trace metal catalyzed oxidation. Contributions from different formation pathways are presented.
Ali Akherati, Christopher D. Cappa, Michael J. Kleeman, Kenneth S. Docherty, Jose L. Jimenez, Stephen M. Griffith, Sebastien Dusanter, Philip S. Stevens, and Shantanu H. Jathar
Atmos. Chem. Phys., 19, 4561–4594, https://doi.org/10.5194/acp-19-4561-2019, https://doi.org/10.5194/acp-19-4561-2019, 2019
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Unburned and partially burned organic compounds emitted from fossil fuel and biomass combustion can react in the atmosphere in the presence of sunlight to form particles. In this work, we use an air pollution model to examine the influence of these organic compounds released by motor vehicles and fires on fine particle pollution in southern California.
Christoph A. Keller and Mat J. Evans
Geosci. Model Dev., 12, 1209–1225, https://doi.org/10.5194/gmd-12-1209-2019, https://doi.org/10.5194/gmd-12-1209-2019, 2019
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Computer simulations of atmospheric chemistry are a central tool to study the impact of air pollutants on the environment. These models are highly complex and require a lot of computing resources. In this study we show that machine learning can be used to predict air pollution with an accuracy that is comparable to the traditional, computationally expensive method. Such a machine-learning-based model has the potential to be orders of magnitude faster.
Xuan Wang, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Lei Zhu, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mathew J. Evans, Ben H. Lee, Jessica D. Haskins, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Gregory L. Huey, and Hong Liao
Atmos. Chem. Phys., 19, 3981–4003, https://doi.org/10.5194/acp-19-3981-2019, https://doi.org/10.5194/acp-19-3981-2019, 2019
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Chlorine radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a comprehensive simulation of tropospheric chlorine in a global 3-D model, which includes explicit accounting of chloride mobilization from sea salt aerosol. We find the chlorine chemistry contributes 1.0 % of the global oxidation of methane and decreases global burdens of tropospheric ozone by 7 % and OH by 3 % through the associated bromine radical chemistry.
Jerry R. Ziemke, Luke D. Oman, Sarah A. Strode, Anne R. Douglass, Mark A. Olsen, Richard D. McPeters, Pawan K. Bhartia, Lucien Froidevaux, Gordon J. Labow, Jacquie C. Witte, Anne M. Thompson, David P. Haffner, Natalya A. Kramarova, Stacey M. Frith, Liang-Kang Huang, Glen R. Jaross, Colin J. Seftor, Mathew T. Deland, and Steven L. Taylor
Atmos. Chem. Phys., 19, 3257–3269, https://doi.org/10.5194/acp-19-3257-2019, https://doi.org/10.5194/acp-19-3257-2019, 2019
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Both a 38-year merged satellite record of tropospheric ozone from TOMS/OMI/MLS/OMPS and a MERRA-2 GMI model simulation show large increases of 6–7 Dobson units from the Near East to India–East Asia and eastward over the Pacific. These increases in tropospheric ozone are attributed to increases in pollution over the region over the last several decades. Secondary 38-year increases of 4–5 Dobson units with both GMI model and satellite measurements occur over central African–tropical Atlantic.
Alba Badia, Claire E. Reeves, Alex R. Baker, Alfonso Saiz-Lopez, Rainer Volkamer, Theodore K. Koenig, Eric C. Apel, Rebecca S. Hornbrook, Lucy J. Carpenter, Stephen J. Andrews, Tomás Sherwen, and Roland von Glasow
Atmos. Chem. Phys., 19, 3161–3189, https://doi.org/10.5194/acp-19-3161-2019, https://doi.org/10.5194/acp-19-3161-2019, 2019
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The oceans have an impact on the composition and reactivity of the troposphere through the emission of gases and particles. Thus, a quantitative understanding of the marine atmosphere is crucial to examine the oxidative capacity and climate forcing. This study investigates the impact of halogens in the tropical troposphere and explores the sensitivity of this to uncertainties in the fluxes and their chemical processing. Our modelled tropospheric Ox loss due to halogens ranges from 20 % to 60 %.
Anna L. Hodshire, Pedro Campuzano-Jost, John K. Kodros, Betty Croft, Benjamin A. Nault, Jason C. Schroder, Jose L. Jimenez, and Jeffrey R. Pierce
Atmos. Chem. Phys., 19, 3137–3160, https://doi.org/10.5194/acp-19-3137-2019, https://doi.org/10.5194/acp-19-3137-2019, 2019
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A global chemical-transport model is used to determine the impact of methanesulfonic acid (MSA) on the aerosol size distribution and associated radiative effects, testing varying assumptions of MSA’s effective volatility and nucleating ability. We find that MSA mass best matches the ATom airborne measurements when volatility varies as a function of temperature, relative humidity, and available gas-phase bases, and the MSA radiative forcing is on the order of -50 mW m-2 over the Southern Ocean.
Jin Liao, Thomas F. Hanisco, Glenn M. Wolfe, Jason St. Clair, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Alan Fried, Eloise A. Marais, Gonzalo Gonzalez Abad, Kelly Chance, Hiren T. Jethva, Thomas B. Ryerson, Carsten Warneke, and Armin Wisthaler
Atmos. Chem. Phys., 19, 2765–2785, https://doi.org/10.5194/acp-19-2765-2019, https://doi.org/10.5194/acp-19-2765-2019, 2019
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Organic aerosol (OA) intimately links natural and anthropogenic emissions with air quality and climate. Direct OA measurements from space are currently not possible. This paper describes a new method to estimate OA by combining satellite HCHO and in situ OA and HCHO. The OA estimate is validated with the ground network. This new method has a potential for mapping observation-based global OA estimate.
Kate R. Smith, Peter M. Edwards, Peter D. Ivatt, James D. Lee, Freya Squires, Chengliang Dai, Richard E. Peltier, Mat J. Evans, Yele Sun, and Alastair C. Lewis
Atmos. Meas. Tech., 12, 1325–1336, https://doi.org/10.5194/amt-12-1325-2019, https://doi.org/10.5194/amt-12-1325-2019, 2019
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Clusters of low-cost, low-power atmospheric gas sensors were built into a sensor instrument to monitor NO2 and O3 in Beijing, alongside reference instruments, aiming to improve the reliability of sensor measurements. Clustering identical sensors and using the median sensor signal was used to minimize drift over short and medium timescales. Three different machine learning techniques were used for all the sensor data in an attempt to correct for cross-interferences, which worked to some degree.
Cristen Adams, Chris A. McLinden, Mark W. Shephard, Nolan Dickson, Enrico Dammers, Jack Chen, Paul Makar, Karen E. Cady-Pereira, Naomi Tam, Shailesh K. Kharol, Lok N. Lamsal, and Nickolay A. Krotkov
Atmos. Chem. Phys., 19, 2577–2599, https://doi.org/10.5194/acp-19-2577-2019, https://doi.org/10.5194/acp-19-2577-2019, 2019
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We estimated how much carbon monoxide, ammonia, and nitrogen oxides were emitted in the smoke from the Fort McMurray Horse River wildfire using satellite data and air quality models. The fire emitted amounts of carbon monoxide that were similar to anthropogenic (human-caused) emissions for all of Alberta over a full year. We also estimated large amounts of ammonia and nitrogen oxides emitted from the fire. These results can be used to evaluate the performance of air quality forecasting models.
Federica Pacifico, Claire Delon, Corinne Jambert, Pierre Durand, Eleanor Morris, Mat J. Evans, Fabienne Lohou, Solène Derrien, Venance H. E. Donnou, Arnaud V. Houeto, Irene Reinares Martínez, and Pierre-Etienne Brilouet
Atmos. Chem. Phys., 19, 2299–2325, https://doi.org/10.5194/acp-19-2299-2019, https://doi.org/10.5194/acp-19-2299-2019, 2019
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Biogenic fluxes from soil at a local and regional scale are crucial to study air pollution and climate. Here we present field measurements of soil fluxes of nitric oxide (NO) and ammonia (NH3) observed over four different land cover types, i.e. bare soil, grassland, maize field, and forest, at an inland rural site in Benin, West Africa, during the DACCIWA field campaign in
June and July 2016.
Shino Toma, Steve Bertman, Christopher Groff, Fulizi Xiong, Paul B. Shepson, Paul Romer, Kaitlin Duffey, Paul Wooldridge, Ronald Cohen, Karsten Baumann, Eric Edgerton, Abigail R. Koss, Joost de Gouw, Allen Goldstein, Weiwei Hu, and Jose L. Jimenez
Atmos. Chem. Phys., 19, 1867–1880, https://doi.org/10.5194/acp-19-1867-2019, https://doi.org/10.5194/acp-19-1867-2019, 2019
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Acyl peroxy nitrates (APN) were measured near the ground in Alabama using GC in summer 2013 to study biosphere–atmosphere interactions. APN were lower than measured in the SE USA over the past 2 decades. Historical data showed APN in 2013 was limited by NOx and production was dominated by biogenic precursors more than in the past. Isoprene-derived MPAN correlated with isoprene hydroxynitrates as NOx-dependent products. MPAN varied with aerosol growth, but not with N-containing particles.
Daniel L. Goldberg, Pablo E. Saide, Lok N. Lamsal, Benjamin de Foy, Zifeng Lu, Jung-Hun Woo, Younha Kim, Jinseok Kim, Meng Gao, Gregory Carmichael, and David G. Streets
Atmos. Chem. Phys., 19, 1801–1818, https://doi.org/10.5194/acp-19-1801-2019, https://doi.org/10.5194/acp-19-1801-2019, 2019
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Using satellite data, we are able to estimate the emissions of NOx (NOx=NO+NO2), a toxic group of air pollutants, in the Seoul metropolitan area. We first develop an enhanced satellite product that better observes NO2 in urban regions. Using this new product, we derive NOx emissions to be twice as large as the emissions reported by the South Korean government. The implication is that the measures taken to reduce NOx emissions in South Korea have not been as effective as regulators have thought.
Dagny A. Ullmann, Mallory L. Hinks, Adrian M. Maclean, Christopher L. Butenhoff, James W. Grayson, Kelley Barsanti, Jose L. Jimenez, Sergey A. Nizkorodov, Saeid Kamal, and Allan K. Bertram
Atmos. Chem. Phys., 19, 1491–1503, https://doi.org/10.5194/acp-19-1491-2019, https://doi.org/10.5194/acp-19-1491-2019, 2019
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We measured the viscosity and diffusion of organic molecules in secondary organic aerosol (SOA) generated from the ozonolysis of limonene. The results suggest that the mixing times of large organics in the SOA studied are short (< 1 h) for conditions found in the planetary boundary layer. The results also show that the Stokes–Einstein equation gives accurate predictions of diffusion coefficients of large organics within the studied SOA up to a viscosity of 102 to 104 Pa s.
Shaojie Song, Meng Gao, Weiqi Xu, Yele Sun, Douglas R. Worsnop, John T. Jayne, Yuzhong Zhang, Lei Zhu, Mei Li, Zhen Zhou, Chunlei Cheng, Yibing Lv, Ying Wang, Wei Peng, Xiaobin Xu, Nan Lin, Yuxuan Wang, Shuxiao Wang, J. William Munger, Daniel J. Jacob, and Michael B. McElroy
Atmos. Chem. Phys., 19, 1357–1371, https://doi.org/10.5194/acp-19-1357-2019, https://doi.org/10.5194/acp-19-1357-2019, 2019
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Chemistry responsible for sulfate production in northern China winter haze remains mysterious. We propose a potentially key pathway through the reaction of formaldehyde and sulfur dioxide that has not been accounted for in previous studies. The special atmospheric conditions favor the formation and existence of their complex, hydroxymethanesulfonate (HMS).
Zhe Peng, Julia Lee-Taylor, John J. Orlando, Geoffrey S. Tyndall, and Jose L. Jimenez
Atmos. Chem. Phys., 19, 813–834, https://doi.org/10.5194/acp-19-813-2019, https://doi.org/10.5194/acp-19-813-2019, 2019
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The use of oxidation flow reactors (OFRs) has been rapidly increasing. We investigate organic peroxy radical (RO2) chemistry in OFRs by kinetic modeling. It is found that, at low NO, UV intensity should be limited to avoid high radical levels leading to significant reaction of RO2 with OH and negligible RO2 isomerization, both of which are atmospherically irrelevant. We also develop two RO2 fate estimators (for general use and for OFRs) to aid experiment design and interpretation.
Juhi Nagori, Ruud H. H. Janssen, Juliane L. Fry, Maarten Krol, Jose L. Jimenez, Weiwei Hu, and Jordi Vilà-Guerau de Arellano
Atmos. Chem. Phys., 19, 701–729, https://doi.org/10.5194/acp-19-701-2019, https://doi.org/10.5194/acp-19-701-2019, 2019
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Secondary organic aerosol (SOA) is produced through a complex interaction of sunlight, volatile organic compounds emitted from trees, anthropogenic emissions, and atmospheric chemistry. We are able to successfully model the formation and diurnal evolution of SOA using a model that takes into consideration the surface and boundary layer dynamics (1–2 km from the surface) and photochemistry above the southeastern US with data collected during the SOAS campaign to constrain the model.
Andrew T. Lambe, Jordan E. Krechmer, Zhe Peng, Jason R. Casar, Anthony J. Carrasquillo, Jonathan D. Raff, Jose L. Jimenez, and Douglas R. Worsnop
Atmos. Meas. Tech., 12, 299–311, https://doi.org/10.5194/amt-12-299-2019, https://doi.org/10.5194/amt-12-299-2019, 2019
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This paper is an evaluation of methods used to generate OH radicals under conditions with high concentrations of NO and NO2 to simulate oxidation chemistry in polluted urban atmospheres over equivalent atmospheric timescales of ~ 1 day.
Joshua L. Laughner, Qindan Zhu, and Ronald C. Cohen
Atmos. Meas. Tech., 12, 129–146, https://doi.org/10.5194/amt-12-129-2019, https://doi.org/10.5194/amt-12-129-2019, 2019
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We compared v3.0B of the BEHR satellite NO2 product against independent measurements to verify its accuracy. We found that the BEHR product generally performs better than standard NO2 products and the previous version of BEHR. Outside of the SE US, using daily NO2 profiles results in similar or better agreement with independent measurements than using monthly profiles, and direct evaluation of those profiles shows they better describe NO2 distribution in urban areas than monthly profiles.
Mengyao Liu, Jintai Lin, K. Folkert Boersma, Gaia Pinardi, Yang Wang, Julien Chimot, Thomas Wagner, Pinhua Xie, Henk Eskes, Michel Van Roozendael, François Hendrick, Pucai Wang, Ting Wang, Yingying Yan, Lulu Chen, and Ruijing Ni
Atmos. Meas. Tech., 12, 1–21, https://doi.org/10.5194/amt-12-1-2019, https://doi.org/10.5194/amt-12-1-2019, 2019
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China has become the world’s largest emitter of NOx, which mainly comes from vehicle exhaust, power plants, etc. However, there are no official ground-based measurements before 2013, so satellites have been widely used to monitor and analyze NOx pollution here. Aerosol is the key factor influencing the accuracy of the satellite NOx product. Our study provides a more accurate way to account for aerosol's influence compared to current widely used products.
K. Folkert Boersma, Henk J. Eskes, Andreas Richter, Isabelle De Smedt, Alba Lorente, Steffen Beirle, Jos H. G. M. van Geffen, Marina Zara, Enno Peters, Michel Van Roozendael, Thomas Wagner, Joannes D. Maasakkers, Ronald J. van der A, Joanne Nightingale, Anne De Rudder, Hitoshi Irie, Gaia Pinardi, Jean-Christopher Lambert, and Steven C. Compernolle
Atmos. Meas. Tech., 11, 6651–6678, https://doi.org/10.5194/amt-11-6651-2018, https://doi.org/10.5194/amt-11-6651-2018, 2018
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This paper describes a new, improved data record of 22+ years of coherent nitrogen dioxide (NO2) pollution measurements from different satellite instruments. Our work helps to ensure that climate data are of sufficient quality to draw reliable conclusions and shape decisions. It shows how dedicated intercomparisons of retrieval sub-steps have led to improved NO2 measurements from the GOME, SCIAMACHY, GOME-2(A), and OMI sensors, and how quality assurance of the new data product is achieved.
Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Jason C. Schroder, Bruce Anderson, Andreas J. Beyersdorf, Donald R. Blake, William H. Brune, Yonghoon Choi, Chelsea A. Corr, Joost A. de Gouw, Jack Dibb, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, L. Gregory Huey, Michelle J. Kim, Christoph J. Knote, Kara D. Lamb, Taehyoung Lee, Taehyun Park, Sally E. Pusede, Eric Scheuer, Kenneth L. Thornhill, Jung-Hun Woo, and Jose L. Jimenez
Atmos. Chem. Phys., 18, 17769–17800, https://doi.org/10.5194/acp-18-17769-2018, https://doi.org/10.5194/acp-18-17769-2018, 2018
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Aerosol impacts visibility and human health in large cities. Sources of aerosols are still highly uncertain, especially for cities surrounded by numerous other cities. We use observations collected during the Korea–United States Air Quality study to determine sources of organic aerosol (OA). We find that secondary OA (SOA) is rapidly produced over Seoul, South Korea, and that the sources of the SOA originate from short-lived hydrocarbons, which originate from local emissions.
Lu Shen, Daniel J. Jacob, Loretta J. Mickley, Yuxuan Wang, and Qiang Zhang
Atmos. Chem. Phys., 18, 17489–17496, https://doi.org/10.5194/acp-18-17489-2018, https://doi.org/10.5194/acp-18-17489-2018, 2018
Eloise A. Marais, Daniel J. Jacob, Sungyeon Choi, Joanna Joiner, Maria Belmonte-Rivas, Ronald C. Cohen, Steffen Beirle, Lee T. Murray, Luke D. Schiferl, Viral Shah, and Lyatt Jaeglé
Atmos. Chem. Phys., 18, 17017–17027, https://doi.org/10.5194/acp-18-17017-2018, https://doi.org/10.5194/acp-18-17017-2018, 2018
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We intercompare two new products of global upper tropospheric nitrogen dioxide (NO2) retrieved from the Ozone Monitoring Instrument (OMI). We evaluate these products with aircraft observations from NASA DC8 aircraft campaigns and interpret the useful information these products can provide about nitrogen oxides (NOx) in the global upper troposphere using the GEOS-Chem chemical transport model.
Jian-Xiong Sheng, Daniel J. Jacob, Joannes D. Maasakkers, Yuzhong Zhang, and Melissa P. Sulprizio
Atmos. Meas. Tech., 11, 6379–6388, https://doi.org/10.5194/amt-11-6379-2018, https://doi.org/10.5194/amt-11-6379-2018, 2018
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We conduct Observing System Simulation Experiments to compare the ability of future satellite measurements of atmospheric methane columns for constraining methane emissions at the 25 km scale. We find that the geostationary instruments can do much better than TROPOMI and are less sensitive to cloud cover. GeoCARB observing twice a day would provide 70 % of the information from the nominal GEO-CAPE mission considered by NASA in response to the Decadal Survey of the US National Research Council.
Daniel H. Cusworth, Daniel J. Jacob, Jian-Xiong Sheng, Joshua Benmergui, Alexander J. Turner, Jeremy Brandman, Laurent White, and Cynthia A. Randles
Atmos. Chem. Phys., 18, 16885–16896, https://doi.org/10.5194/acp-18-16885-2018, https://doi.org/10.5194/acp-18-16885-2018, 2018
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Methane emissions from oil/gas fields originate from a large number of small and densely clustered point sources. We examine the potential of recently launched or planned satellites to locate these high-mode emitters through measurements of atmospheric methane. We find that the recently launched TROPOMI and the planned GeoCARB instruments are successful at locating high-emitting sources for fields of 20-50 emitters within the 50 × 50 km2 geographic domain but are unsuccessful for denser fields.
Samuel R. Hall, Kirk Ullmann, Michael J. Prather, Clare M. Flynn, Lee T. Murray, Arlene M. Fiore, Gustavo Correa, Sarah A. Strode, Stephen D. Steenrod, Jean-Francois Lamarque, Jonathan Guth, Béatrice Josse, Johannes Flemming, Vincent Huijnen, N. Luke Abraham, and Alex T. Archibald
Atmos. Chem. Phys., 18, 16809–16828, https://doi.org/10.5194/acp-18-16809-2018, https://doi.org/10.5194/acp-18-16809-2018, 2018
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Photolysis (J rates) initiates and drives atmospheric chemistry, and Js are perturbed by factors of 2 by clouds. The NASA Atmospheric Tomography (ATom) Mission provides the first comprehensive observations on how clouds perturb Js through the remote Pacific and Atlantic basins. We compare these cloud-perturbation J statistics with those from nine global chemistry models. While basic patterns agree, there is a large spread across models, and all lack some basic features of the observations.
Joshua L. Laughner, Qindan Zhu, and Ronald C. Cohen
Earth Syst. Sci. Data, 10, 2069–2095, https://doi.org/10.5194/essd-10-2069-2018, https://doi.org/10.5194/essd-10-2069-2018, 2018
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This paper describes the upgrade of the BErkeley High Resolution (BEHR) NO2 retrieval from versions 2.1C to 3.0B. This retrieval measures NO2 over the continental US using input data at higher spatial and temporal resolution than global retrievals. We analyze how each part of the upgrade affected the measured NO2. Most interestingly, we find that using NO2 profiles at daily (rather than monthly) time resolution does lead to differences in multi-month averages for regions affected by lightning.
Jiayue Huang, Lyatt Jaeglé, and Viral Shah
Atmos. Chem. Phys., 18, 16253–16269, https://doi.org/10.5194/acp-18-16253-2018, https://doi.org/10.5194/acp-18-16253-2018, 2018
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The contribution of blowing snow and frost flower as sources of sea salt aerosols (SSA) over polar regions remains uncertain, despite its potentially important role in polar climate and chemistry. Using chemical transport models and satellite observations, we find that blowing snow emissions are the dominant source of SSA over sea ice during the cold season. We infer a monthly snow salinity on first-year sea ice that decreases from fall–spring, minimizing the model discrepancy to within 10 %.
Lu Hu, Christoph A. Keller, Michael S. Long, Tomás Sherwen, Benjamin Auer, Arlindo Da Silva, Jon E. Nielsen, Steven Pawson, Matthew A. Thompson, Atanas L. Trayanov, Katherine R. Travis, Stuart K. Grange, Mat J. Evans, and Daniel J. Jacob
Geosci. Model Dev., 11, 4603–4620, https://doi.org/10.5194/gmd-11-4603-2018, https://doi.org/10.5194/gmd-11-4603-2018, 2018
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We present a full-year online global simulation of tropospheric chemistry at 12.5 km resolution. To the best of our knowledge, such a resolution in a state-of-the-science global simulation of tropospheric chemistry is unprecedented. This simulation will serve as the Nature Run for observing system simulation experiments to support the future geostationary satellite constellation for tropospheric chemistry, and can also be used for various air quality applications.
Barbara Ervens, Armin Sorooshian, Abdulmonam M. Aldhaif, Taylor Shingler, Ewan Crosbie, Luke Ziemba, Pedro Campuzano-Jost, Jose L. Jimenez, and Armin Wisthaler
Atmos. Chem. Phys., 18, 16099–16119, https://doi.org/10.5194/acp-18-16099-2018, https://doi.org/10.5194/acp-18-16099-2018, 2018
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The paper presents a new framework that can be used to identify emission scenarios in which aerosol populations are most likely modified by chemical processes in clouds. We show that in neither very polluted nor in very clean air masses is this the case. Only if the ratio of possible aerosol mass precursors (sulfur dioxide, some organics) and preexisting aerosol mass is sufficiently high will aerosol particles show substantially modified physicochemical properties upon cloud processing.
Yuzhong Zhang, Daniel J. Jacob, Joannes D. Maasakkers, Melissa P. Sulprizio, Jian-Xiong Sheng, Ritesh Gautam, and John Worden
Atmos. Chem. Phys., 18, 15959–15973, https://doi.org/10.5194/acp-18-15959-2018, https://doi.org/10.5194/acp-18-15959-2018, 2018
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We assess the potential of using satellite observations of atmospheric methane to monitor global mean tropospheric OH concentration, a key parameter for the oxidizing power of the atmosphere.
Azimeh Zare, Paul S. Romer, Tran Nguyen, Frank N. Keutsch, Kate Skog, and Ronald C. Cohen
Atmos. Chem. Phys., 18, 15419–15436, https://doi.org/10.5194/acp-18-15419-2018, https://doi.org/10.5194/acp-18-15419-2018, 2018
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Organic nitrates play an important role in concentrations and distribution of NOx, ozone and aerosol as the most important air pollutants. We develop a state-of-the-science detailed chemical mechanism representing individual organic nitrates, which is appropriate to use in air quality models and results in a more accurate simulation of atmospheric chemistry. Using this mechanism we explore production and removal processes of organic nitrates in a rural environment that are poorly constrained.
Daniel J. Varon, Daniel J. Jacob, Jason McKeever, Dylan Jervis, Berke O. A. Durak, Yan Xia, and Yi Huang
Atmos. Meas. Tech., 11, 5673–5686, https://doi.org/10.5194/amt-11-5673-2018, https://doi.org/10.5194/amt-11-5673-2018, 2018
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Methane is a powerful greenhouse gas emitted from numerous human activities. Space-based observation of point sources would be a cost-effective monitoring solution, but the resolution of most current and planned methane-observing satellites is too coarse to resolve individual emitters. We simulate fine-resolution (50 m) satellite observations of methane plumes as would be measured by GHGSat (to be launched in 2019) and show that such data can usefully quantify large methane point sources.
Liang Feng, Paul I. Palmer, Robyn Butler, Stephen J. Andrews, Elliot L. Atlas, Lucy J. Carpenter, Valeria Donets, Neil R. P. Harris, Ross J. Salawitch, Laura L. Pan, and Sue M. Schauffler
Atmos. Chem. Phys., 18, 14787–14798, https://doi.org/10.5194/acp-18-14787-2018, https://doi.org/10.5194/acp-18-14787-2018, 2018
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We infer surface fluxes of bromoform (CHBr3) and dibromoform (CH2Br2) from CAST and CONTRAST aircraft observations over the western Pacific, using a tagged version of the GEOS-Chem global 3-D atmospheric chemistry model and a Maximum A Posteriori inverse model. Using the aircraft data, we estimate the regional fluxes about 20–40 % smaller than the prior inventories by Ordóñez et al. (2012). We find no evidence to support a robust linear relationship between CHBr3 and CH2Br2 oceanic emissions.
William H. Brune, Xinrong Ren, Li Zhang, Jingqiu Mao, David O. Miller, Bruce E. Anderson, Donald R. Blake, Ronald C. Cohen, Glenn S. Diskin, Samuel R. Hall, Thomas F. Hanisco, L. Gregory Huey, Benjamin A. Nault, Jeff Peischl, Ilana Pollack, Thomas B. Ryerson, Taylor Shingler, Armin Sorooshian, Kirk Ullmann, Armin Wisthaler, and Paul J. Wooldridge
Atmos. Chem. Phys., 18, 14493–14510, https://doi.org/10.5194/acp-18-14493-2018, https://doi.org/10.5194/acp-18-14493-2018, 2018
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Thunderstorms pull in polluted air from near the ground, transport it up through clouds containing lightning, and deposit it at altitudes where airplanes fly. The resulting chemical mixture in this air reacts to form ozone and particles, which affect climate. In this study, aircraft observations of the reactive gases responsible for this chemistry generally agree with modeled values, even in ice clouds. Thus, atmospheric oxidation chemistry appears to be mostly understood for this environment.
Erin R. Delaria, Megan Vieira, Julie Cremieux, and Ronald C. Cohen
Atmos. Chem. Phys., 18, 14161–14173, https://doi.org/10.5194/acp-18-14161-2018, https://doi.org/10.5194/acp-18-14161-2018, 2018
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Observations of NOx exchange between the atmosphere and vegetation have been widely reported. However, the magnitude, direction, and mechanism of this atmosphere–biosphere exchange remain uncertain across different ecosystems. We use laboratory measurements to study the rates of NOx deposition to the leaves of a California oak tree species. We detect no evidence of NOx emission and find that NOx loss to oak leaves is substantial even at low NOx concentrations relevant to forested environments.
Alexis A. Shusterman, Jinsol Kim, Kaitlyn J. Lieschke, Catherine Newman, Paul J. Wooldridge, and Ronald C. Cohen
Atmos. Chem. Phys., 18, 13773–13785, https://doi.org/10.5194/acp-18-13773-2018, https://doi.org/10.5194/acp-18-13773-2018, 2018
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We describe the diversity and heterogeneity of urban CO2 levels observed using the BErkeley Atmospheric CO2 Observation Network, a distributed instrument of > 50 CO2 sensors stationed every ~ 2 km across the San Francisco Bay Area. We demonstrate that relatively simple mathematical techniques, applied to these observations, can be used to detect the small changes in highway CO2 emissions expected to result from upcoming fuel economy regulations, affirming the policy relevance of low-cost sensors.
Qianjie Chen, Tomás Sherwen, Mathew Evans, and Becky Alexander
Atmos. Chem. Phys., 18, 13617–13637, https://doi.org/10.5194/acp-18-13617-2018, https://doi.org/10.5194/acp-18-13617-2018, 2018
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Uncertainty in the natural tropospheric sulfur cycle represents the largest source of uncertainty in radiative forcing estimates of sulfate aerosol. This study investigates the natural sulfur cycle in the marine troposphere using the GEOS-Chem model. We found that BrO is important for DMS oxidation and multiphase chemistry is important for MSA production and loss, which have implications for the yield of SO2 and MSA from DMS oxidation and the radiative effect of DMS-derived sulfate aerosol.
Robyn Butler, Paul I. Palmer, Liang Feng, Stephen J. Andrews, Elliot L. Atlas, Lucy J. Carpenter, Valeria Donets, Neil R. P. Harris, Stephen A. Montzka, Laura L. Pan, Ross J. Salawitch, and Sue M. Schauffler
Atmos. Chem. Phys., 18, 13135–13153, https://doi.org/10.5194/acp-18-13135-2018, https://doi.org/10.5194/acp-18-13135-2018, 2018
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Natural sources of short-lived bromoform and dibromomethane are important for determining the inorganic bromine budget in the stratosphere that drives ozone loss. Two new modelling techniques describe how different geographical source regions influence their atmospheric variability over the western Pacific. We find that it is driven primarily by open ocean sources, and we use atmospheric observations to help estimate their contributions to the upper tropospheric inorganic bromine budget.
Anna L. Hodshire, Brett B. Palm, M. Lizabeth Alexander, Qijing Bian, Pedro Campuzano-Jost, Eben S. Cross, Douglas A. Day, Suzane S. de Sá, Alex B. Guenther, Armin Hansel, James F. Hunter, Werner Jud, Thomas Karl, Saewung Kim, Jesse H. Kroll, Jeong-Hoo Park, Zhe Peng, Roger Seco, James N. Smith, Jose L. Jimenez, and Jeffrey R. Pierce
Atmos. Chem. Phys., 18, 12433–12460, https://doi.org/10.5194/acp-18-12433-2018, https://doi.org/10.5194/acp-18-12433-2018, 2018
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We investigate the nucleation and growth processes that shape the aerosol size distribution inside oxidation flow reactors (OFRs) that sampled ambient air from Colorado and the Amazon rainforest. Results indicate that organics are important for both nucleation and growth, vapor uptake was limited to accumulation-mode particles, fragmentation reactions were important to limit particle growth at higher OH exposures, and an H2SO4-organics nucleation mechanism captured new particle formation well.
Jian-Xiong Sheng, Daniel J. Jacob, Alexander J. Turner, Joannes D. Maasakkers, Joshua Benmergui, A. Anthony Bloom, Claudia Arndt, Ritesh Gautam, Daniel Zavala-Araiza, Hartmut Boesch, and Robert J. Parker
Atmos. Chem. Phys., 18, 12257–12267, https://doi.org/10.5194/acp-18-12257-2018, https://doi.org/10.5194/acp-18-12257-2018, 2018
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Analysis of 7 years (2010–2016) of GOSAT methane trends over Canada, the contiguous US, and Mexico suggests that US methane emissions increased by 2.5 ± 1.4 % a−1 over the 7-year period, with contributions from both oil–gas systems and livestock in the Midwest. Mexican emissions show a decrease that can be attributed to a decreasing cattle population. Canadian emissions show year-to-year variability driven by wetland emissions and correlated with wetland areal extent.
Suzane S. de Sá, Brett B. Palm, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Gabriel Isaacman-VanWertz, Lindsay D. Yee, Joel Brito, Samara Carbone, Igor O. Ribeiro, Glauber G. Cirino, Yingjun Liu, Ryan Thalman, Arthur Sedlacek, Aaron Funk, Courtney Schumacher, John E. Shilling, Johannes Schneider, Paulo Artaxo, Allen H. Goldstein, Rodrigo A. F. Souza, Jian Wang, Karena A. McKinney, Henrique Barbosa, M. Lizabeth Alexander, Jose L. Jimenez, and Scot T. Martin
Atmos. Chem. Phys., 18, 12185–12206, https://doi.org/10.5194/acp-18-12185-2018, https://doi.org/10.5194/acp-18-12185-2018, 2018
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This study aimed at understanding and quantifying the changes in mass concentration and composition of submicron airborne particulate matter (PM) in Amazonia due to urban pollution. Downwind of Manaus, PM concentrations increased by up to 200 % under polluted compared with background conditions. The observed changes included contributions from both primary and secondary processes. The differences in organic PM composition suggested a shift in the pathways of secondary production with pollution.
Juliane L. Fry, Steven S. Brown, Ann M. Middlebrook, Peter M. Edwards, Pedro Campuzano-Jost, Douglas A. Day, José L. Jimenez, Hannah M. Allen, Thomas B. Ryerson, Ilana Pollack, Martin Graus, Carsten Warneke, Joost A. de Gouw, Charles A. Brock, Jessica Gilman, Brian M. Lerner, William P. Dubé, Jin Liao, and André Welti
Atmos. Chem. Phys., 18, 11663–11682, https://doi.org/10.5194/acp-18-11663-2018, https://doi.org/10.5194/acp-18-11663-2018, 2018
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This paper uses measurements made during research aircraft flights through power plant smokestack emissions plumes as a natural laboratory in the field experiment. We investigated a specific source of airborne particulate matter from the combination of human-produced NOx pollutant emissions (the smokestack plumes) with isoprene emitted by naturally by trees in the southeastern United States. These field-based yields appear to be higher than those typically measured in chamber studies.
Prasad Kasibhatla, Tomás Sherwen, Mathew J. Evans, Lucy J. Carpenter, Chris Reed, Becky Alexander, Qianjie Chen, Melissa P. Sulprizio, James D. Lee, Katie A. Read, William Bloss, Leigh R. Crilley, William C. Keene, Alexander A. P. Pszenny, and Alma Hodzic
Atmos. Chem. Phys., 18, 11185–11203, https://doi.org/10.5194/acp-18-11185-2018, https://doi.org/10.5194/acp-18-11185-2018, 2018
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Recent measurements of NOx and HONO suggest that photolysis of particulate nitrate in sea-salt aerosols is important in terms of marine boundary layer oxidant chemistry. We present the first global-scale assessment of the significance of this new chemical pathway for NOx, O3, and OH in the marine boundary layer. We also present a preliminary assessment of the potential impact of photolysis of particulate nitrate associated with other aerosol types on continental boundary layer chemistry.
Sarah A. Strode, Junhua Liu, Leslie Lait, Róisín Commane, Bruce Daube, Steven Wofsy, Austin Conaty, Paul Newman, and Michael Prather
Atmos. Chem. Phys., 18, 10955–10971, https://doi.org/10.5194/acp-18-10955-2018, https://doi.org/10.5194/acp-18-10955-2018, 2018
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The GEOS-5 atmospheric model provided forecasts for the Atmospheric Tomography Mission (ATom). GEOS-5 shows skill in simulating the carbon monoxide (CO) measured in ATom-1. African fires contribute to high CO over the tropical Atlantic, but non-fire sources are the main contributors elsewhere. ATom aims to provide a chemical climatology, so we consider whether ATom-1 occurred during a typical summer month. Satellite observations suggest ATom-1 occurred in a clean but not exceptional month.
Alba Lorente, K. Folkert Boersma, Piet Stammes, L. Gijsbert Tilstra, Andreas Richter, Huan Yu, Said Kharbouche, and Jan-Peter Muller
Atmos. Meas. Tech., 11, 4509–4529, https://doi.org/10.5194/amt-11-4509-2018, https://doi.org/10.5194/amt-11-4509-2018, 2018
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Light reflected by Earth’s surface is different in each direction: it appears brighter or darker in certain viewing directions. Currently this effect is not accounted for in satellite retrievals; thus surface reflectance climatologies and cloud fractions show an east-west bias across orbits (GOME2,OMI). The effect for NO2 measurements in partly cloudy scenes is substantial. We recommend that this effect in UV/Vis sensors coherently accounted for, and will be especially beneficial for TROPOMI.
Sebastian D. Eastham, Michael S. Long, Christoph A. Keller, Elizabeth Lundgren, Robert M. Yantosca, Jiawei Zhuang, Chi Li, Colin J. Lee, Matthew Yannetti, Benjamin M. Auer, Thomas L. Clune, Jules Kouatchou, William M. Putman, Matthew A. Thompson, Atanas L. Trayanov, Andrea M. Molod, Randall V. Martin, and Daniel J. Jacob
Geosci. Model Dev., 11, 2941–2953, https://doi.org/10.5194/gmd-11-2941-2018, https://doi.org/10.5194/gmd-11-2941-2018, 2018
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Global atmospheric chemical transport models are crucial tools in atmospheric science, used to address problems ranging from climate change to acid rain. GEOS-Chem High Performance (GCHP) is a new implementation of the widely used GEOS-Chem model, designed for massively parallel architectures. GCHP v11-02c is shown to be highly scalable from 6 to over 500 cores, enabling the routine simulation of global atmospheric chemistry from the surface to the stratopause at resolutions of ~50 km or finer.
Lindsay D. Yee, Gabriel Isaacman-VanWertz, Rebecca A. Wernis, Meng Meng, Ventura Rivera, Nathan M. Kreisberg, Susanne V. Hering, Mads S. Bering, Marianne Glasius, Mary Alice Upshur, Ariana Gray Bé, Regan J. Thomson, Franz M. Geiger, John H. Offenberg, Michael Lewandowski, Ivan Kourtchev, Markus Kalberer, Suzane de Sá, Scot T. Martin, M. Lizabeth Alexander, Brett B. Palm, Weiwei Hu, Pedro Campuzano-Jost, Douglas A. Day, Jose L. Jimenez, Yingjun Liu, Karena A. McKinney, Paulo Artaxo, Juarez Viegas, Antonio Manzi, Maria B. Oliveira, Rodrigo de Souza, Luiz A. T. Machado, Karla Longo, and Allen H. Goldstein
Atmos. Chem. Phys., 18, 10433–10457, https://doi.org/10.5194/acp-18-10433-2018, https://doi.org/10.5194/acp-18-10433-2018, 2018
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Biogenic volatile organic compounds react in the atmosphere to form secondary organic aerosol, yet the chemical pathways remain unclear. We collected filter samples and deployed a semi-volatile thermal desorption aerosol gas chromatograph in the central Amazon. We measured 30 sesquiterpenes and 4 diterpenes and find them to be important for reactive ozone loss. We estimate that sesquiterpene oxidation contributes at least 0.4–5 % (median 1 %) of observed submicron organic aerosol mass.
Marina Zara, K. Folkert Boersma, Isabelle De Smedt, Andreas Richter, Enno Peters, Jos H. G. M. van Geffen, Steffen Beirle, Thomas Wagner, Michel Van Roozendael, Sergey Marchenko, Lok N. Lamsal, and Henk J. Eskes
Atmos. Meas. Tech., 11, 4033–4058, https://doi.org/10.5194/amt-11-4033-2018, https://doi.org/10.5194/amt-11-4033-2018, 2018
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Nitrogen dioxide and formaldehyde satellite data are used for air quality and climate studies. We quantify and characterise slant column uncertainties from different research groups. Our evaluation is motivated by recently improved techniques and by a desire to provide fully traceable uncertainty budget for climate records generated within the QA4ECV project. The improved slant columns are in agreement but with substantial differences in the reported uncertainties between groups and instruments.
Ruixiong Zhang, Yuhang Wang, Charles Smeltzer, Hang Qu, William Koshak, and K. Folkert Boersma
Atmos. Meas. Tech., 11, 3955–3967, https://doi.org/10.5194/amt-11-3955-2018, https://doi.org/10.5194/amt-11-3955-2018, 2018
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This study focuses on how to improve OMI NO2 retrievals for trend analysis. We retrieve OMI tropospheric NO2 vertical column densities (VCDs) and obtain the NO2 seasonal trends over the United States, which are compared with coincident in situ surface NO2 measurements from the Air Quality System network. We find that three procedures are essential in comparing both datasets, including the ocean trend removal, the albedo update, and the lightning filter.
Alexander J. Turner, Daniel J. Jacob, Joshua Benmergui, Jeremy Brandman, Laurent White, and Cynthia A. Randles
Atmos. Chem. Phys., 18, 8265–8278, https://doi.org/10.5194/acp-18-8265-2018, https://doi.org/10.5194/acp-18-8265-2018, 2018
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We conduct a 1-week WRF-STILT simulation to generate methane column footprints at 1.3 km spatial resolution and hourly temporal resolution over the Barnett Shale. We find that a week of TROPOMI observations should provide regional (~30 km) information on temporally invariant sources and GeoCARB should provide information on temporally invariant sources at 2–7 km spatial resolution. An instrument precision better than 6 ppb is an important threshold for achieving fine resolution of emissions.
Jian-Xiong Sheng, Daniel J. Jacob, Alexander J. Turner, Joannes D. Maasakkers, Melissa P. Sulprizio, A. Anthony Bloom, Arlyn E. Andrews, and Debra Wunch
Atmos. Chem. Phys., 18, 6483–6491, https://doi.org/10.5194/acp-18-6483-2018, https://doi.org/10.5194/acp-18-6483-2018, 2018
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We use observations of boundary layer methane from the SEAC4RS aircraft campaign over the Southeast US to estimate methane emissions in that region. Our results suggest that the EPA inventory is regionally unbiased but there are large local biases, suggesting variable emission factors. Our results also suggest that the choice of landcover map is the dominant source of error for wetland emission estimates.
Michael J. Prather, Clare M. Flynn, Xin Zhu, Stephen D. Steenrod, Sarah A. Strode, Arlene M. Fiore, Gustavo Correa, Lee T. Murray, and Jean-Francois Lamarque
Atmos. Meas. Tech., 11, 2653–2668, https://doi.org/10.5194/amt-11-2653-2018, https://doi.org/10.5194/amt-11-2653-2018, 2018
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A new protocol for merging in situ atmospheric chemistry measurements with 3-D models is developed. This technique can identify the most reactive air parcels in terms of tropospheric production/loss of O3 & CH4. This approach highlights differences in 6 global chemistry models even with composition specified. Thus in situ measurements from, e.g., NASA's ATom mission can be used to develop a chemical climatology of, not only the key species, but also the rates of key reactions in each air parcel.
Mike J. Newland, Andrew R. Rickard, Tomás Sherwen, Mathew J. Evans, Luc Vereecken, Amalia Muñoz, Milagros Ródenas, and William J. Bloss
Atmos. Chem. Phys., 18, 6095–6120, https://doi.org/10.5194/acp-18-6095-2018, https://doi.org/10.5194/acp-18-6095-2018, 2018
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Stabilised Criegee intermediates (SCIs) are formed in the reaction of alkenes with ozone, both of which are ubiquitous throughout the troposphere. We determine the fate and global distribution of SCI from monoterpene ozonolysis. One major fate of SCI is reaction with H2O, but for a fraction of SCIs, unimolecular reactions dominate. Concentrations of SCIs are high enough regionally to play a key role in the conversion of sulfur dioxide to aerosol, affecting air quality and climate.
Jiawei Zhuang, Daniel J. Jacob, and Sebastian D. Eastham
Atmos. Chem. Phys., 18, 6039–6055, https://doi.org/10.5194/acp-18-6039-2018, https://doi.org/10.5194/acp-18-6039-2018, 2018
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Our work explains why current model simulations are unable to capture the intercontinental influences of pollution plumes that are often observed over some regions like California. Due to inadequate vertical grid resolution in these models, the plumes get diffused too rapidly during intercontinental transport. Increasing the vertical grid resolution greatly improves the simulation of plumes and considerably increases the estimate of local surface pollution influence.
Isabelle De Smedt, Nicolas Theys, Huan Yu, Thomas Danckaert, Christophe Lerot, Steven Compernolle, Michel Van Roozendael, Andreas Richter, Andreas Hilboll, Enno Peters, Mattia Pedergnana, Diego Loyola, Steffen Beirle, Thomas Wagner, Henk Eskes, Jos van Geffen, Klaas Folkert Boersma, and Pepijn Veefkind
Atmos. Meas. Tech., 11, 2395–2426, https://doi.org/10.5194/amt-11-2395-2018, https://doi.org/10.5194/amt-11-2395-2018, 2018
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This paper introduces the formaldehyde (HCHO) tropospheric vertical column retrieval algorithm implemented in the TROPOMI/Sentinel-5 Precursor operational processor, and comprehensively describes its various retrieval steps. Furthermore, algorithmic improvements developed in the framework of the EU FP7-project QA4ECV are described for future updates of the processor. Detailed error estimates are discussed in the light of Copernicus user requirements and needs for validation are highlighted.
Pieternel F. Levelt, Joanna Joiner, Johanna Tamminen, J. Pepijn Veefkind, Pawan K. Bhartia, Deborah C. Stein Zweers, Bryan N. Duncan, David G. Streets, Henk Eskes, Ronald van der A, Chris McLinden, Vitali Fioletov, Simon Carn, Jos de Laat, Matthew DeLand, Sergey Marchenko, Richard McPeters, Jerald Ziemke, Dejian Fu, Xiong Liu, Kenneth Pickering, Arnoud Apituley, Gonzalo González Abad, Antti Arola, Folkert Boersma, Christopher Chan Miller, Kelly Chance, Martin de Graaf, Janne Hakkarainen, Seppo Hassinen, Iolanda Ialongo, Quintus Kleipool, Nickolay Krotkov, Can Li, Lok Lamsal, Paul Newman, Caroline Nowlan, Raid Suleiman, Lieuwe Gijsbert Tilstra, Omar Torres, Huiqun Wang, and Krzysztof Wargan
Atmos. Chem. Phys., 18, 5699–5745, https://doi.org/10.5194/acp-18-5699-2018, https://doi.org/10.5194/acp-18-5699-2018, 2018
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The aim of this paper is to highlight the many successes of the Ozone Monitoring Instrument (OMI) spanning more than 13 years. Data from OMI have been used in a wide range of applications. Due to its unprecedented spatial resolution, in combination with daily global coverage, OMI plays a unique role in measuring trace gases important for the ozone layer, air quality, and climate change. OMI data continue to be used for new research and applications.
Jennifer Kaiser, Daniel J. Jacob, Lei Zhu, Katherine R. Travis, Jenny A. Fisher, Gonzalo González Abad, Lin Zhang, Xuesong Zhang, Alan Fried, John D. Crounse, Jason M. St. Clair, and Armin Wisthaler
Atmos. Chem. Phys., 18, 5483–5497, https://doi.org/10.5194/acp-18-5483-2018, https://doi.org/10.5194/acp-18-5483-2018, 2018
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Isoprene emissions from vegetation have a large effect on atmospheric chemistry and air quality. Here we use the adjoint of GEOS-Chem in an inversion of OMI formaldehyde observations to produce top-down estimates of isoprene emissions in the southeast US during the summer of 2013. We find that MEGAN v2.1 is biased high on average by 40 %. Our downward correction of isoprene emissions leads to a small reduction in modeled surface O3 and decreases the contribution of isoprene to organic aerosol.
Richard Newton, Geraint Vaughan, Eric Hintsa, Michal T. Filus, Laura L. Pan, Shawn Honomichl, Elliot Atlas, Stephen J. Andrews, and Lucy J. Carpenter
Atmos. Chem. Phys., 18, 5157–5171, https://doi.org/10.5194/acp-18-5157-2018, https://doi.org/10.5194/acp-18-5157-2018, 2018
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We consider the ozone measurements from aircraft during the CAST/CONTRAST/ATTREX campaigns of 2014. Low concentrations of ozone were found in the layer of 10–15 km altitude, which is indicative of uplift of ozone-poor air from near the sea surface to 10–15 km altitude. Chemicals that have origins in the sea were found in greater abundance when ozone concentrations were low compared to when ozone concentrations were high. The lowest ozone concentrations were found in the Southern Hemisphere.
Jinsol Kim, Alexis A. Shusterman, Kaitlyn J. Lieschke, Catherine Newman, and Ronald C. Cohen
Atmos. Meas. Tech., 11, 1937–1946, https://doi.org/10.5194/amt-11-1937-2018, https://doi.org/10.5194/amt-11-1937-2018, 2018
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The newest generation of air quality sensors is small, low cost, and easy to deploy. These sensors are an attractive option for developing dense observation networks in support of regulatory activities and scientific research. However, these sensors are difficult to interpret. Here we describe a novel calibration strategy for a set of low cost sensors and demonstrate this calibration on a subset of the sensors comprising BEACO2N, a distributed network at the San Francisco Bay Area.
Jacob T. Shaw, Richard T. Lidster, Danny R. Cryer, Noelia Ramirez, Fiona C. Whiting, Graham A. Boustead, Lisa K. Whalley, Trevor Ingham, Andrew R. Rickard, Rachel E. Dunmore, Dwayne E. Heard, Ally C. Lewis, Lucy J. Carpenter, Jacqui F. Hamilton, and Terry J. Dillon
Atmos. Chem. Phys., 18, 4039–4054, https://doi.org/10.5194/acp-18-4039-2018, https://doi.org/10.5194/acp-18-4039-2018, 2018
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The lifetime of a chemical in the atmosphere is largely governed by the rate of its reaction with the hydroxyl radical (OH). Measurements of rates for many of the thousands of identified volatile organic compounds (VOCs) have yet to be determined experimentally. We have developed a new technique for the rapid determination of gas-phase rate coefficients for the simultaneous reactions between multiple VOCs and OH. The method is tasted across a range of scenarios and is used to derive new values.
Daniel Stone, Tomás Sherwen, Mathew J. Evans, Stewart Vaughan, Trevor Ingham, Lisa K. Whalley, Peter M. Edwards, Katie A. Read, James D. Lee, Sarah J. Moller, Lucy J. Carpenter, Alastair C. Lewis, and Dwayne E. Heard
Atmos. Chem. Phys., 18, 3541–3561, https://doi.org/10.5194/acp-18-3541-2018, https://doi.org/10.5194/acp-18-3541-2018, 2018
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Halogen chemistry in the troposphere impacts oxidising capacity, but model studies assessing the nature of these impacts can vary according to the model framework used. In this work we present simulations of OH and HO2 radicals using both box and global model frameworks, and compare to observations made at the Cape Verde Atmospheric Observatory. We highlight, and rationalise, differences between the model frameworks.
Abigail R. Koss, Kanako Sekimoto, Jessica B. Gilman, Vanessa Selimovic, Matthew M. Coggon, Kyle J. Zarzana, Bin Yuan, Brian M. Lerner, Steven S. Brown, Jose L. Jimenez, Jordan Krechmer, James M. Roberts, Carsten Warneke, Robert J. Yokelson, and Joost de Gouw
Atmos. Chem. Phys., 18, 3299–3319, https://doi.org/10.5194/acp-18-3299-2018, https://doi.org/10.5194/acp-18-3299-2018, 2018
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Non-methane organic gases (NMOGs) were detected by proton-transfer-reaction mass spectrometry (PTR-ToF) during an extensive laboratory characterization of wildfire emissions. Identifications for PTR-ToF ion masses are proposed and supported by a combination of techniques. Overall excellent agreement with other instrumentation is shown. Scalable emission factors and ratios are reported for many newly reported reactive species. An analysis of chemical characteristics is presented.
Jingqiu Mao, Annmarie Carlton, Ronald C. Cohen, William H. Brune, Steven S. Brown, Glenn M. Wolfe, Jose L. Jimenez, Havala O. T. Pye, Nga Lee Ng, Lu Xu, V. Faye McNeill, Kostas Tsigaridis, Brian C. McDonald, Carsten Warneke, Alex Guenther, Matthew J. Alvarado, Joost de Gouw, Loretta J. Mickley, Eric M. Leibensperger, Rohit Mathur, Christopher G. Nolte, Robert W. Portmann, Nadine Unger, Mika Tosca, and Larry W. Horowitz
Atmos. Chem. Phys., 18, 2615–2651, https://doi.org/10.5194/acp-18-2615-2018, https://doi.org/10.5194/acp-18-2615-2018, 2018
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This paper is aimed at discussing progress in evaluating, diagnosing, and improving air quality and climate modeling using comparisons to SAS observations as a guide to thinking about improvements to mechanisms and parameterizations in models.
Paul S. Romer, Kaitlin C. Duffey, Paul J. Wooldridge, Eric Edgerton, Karsten Baumann, Philip A. Feiner, David O. Miller, William H. Brune, Abigail R. Koss, Joost A. de Gouw, Pawel K. Misztal, Allen H. Goldstein, and Ronald C. Cohen
Atmos. Chem. Phys., 18, 2601–2614, https://doi.org/10.5194/acp-18-2601-2018, https://doi.org/10.5194/acp-18-2601-2018, 2018
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Observations of increased ozone on hotter days are widely reported, but the mechanisms driving this relationship remain uncertain. We use measurements from the rural southeastern United States to study how temperature affects ozone production. We find that changing NOx emissions, most likely from soil microbes, can be a major driver of increased ozone with temperature in the continental background. These findings suggest that ozone will increase with temperature under a wide range of conditions.
Jingyi Li, Jingqiu Mao, Arlene M. Fiore, Ronald C. Cohen, John D. Crounse, Alex P. Teng, Paul O. Wennberg, Ben H. Lee, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Jeff Peischl, Ilana B. Pollack, Thomas B. Ryerson, Patrick Veres, James M. Roberts, J. Andrew Neuman, John B. Nowak, Glenn M. Wolfe, Thomas F. Hanisco, Alan Fried, Hanwant B. Singh, Jack Dibb, Fabien Paulot, and Larry W. Horowitz
Atmos. Chem. Phys., 18, 2341–2361, https://doi.org/10.5194/acp-18-2341-2018, https://doi.org/10.5194/acp-18-2341-2018, 2018
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We present the first comprehensive model evaluation of summertime reactive oxidized nitrogen using a high-resolution chemistry–climate model with up-to-date isoprene oxidation chemistry, along with a series of observations from aircraft campaigns and ground measurement networks from 2004 to 2013 over the Southeast US. We investigate the impact of NOx emission reductions on changes in reactive nitrogen speciation and export efficiency as well as ozone in the past and future decade.
Karen Yu, Christoph A. Keller, Daniel J. Jacob, Andrea M. Molod, Sebastian D. Eastham, and Michael S. Long
Geosci. Model Dev., 11, 305–319, https://doi.org/10.5194/gmd-11-305-2018, https://doi.org/10.5194/gmd-11-305-2018, 2018
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Global simulations of atmospheric chemistry are generally conducted with off-line chemical transport models (CTMs) driven by archived meteorological data from general circulation models (GCMs). The off-line approach has the advantages of simplicity and expediency, but it is unable to reproduce the GCM transport exactly. We investigate the cascade of errors associated with the off-line approach using the GEOS-5 GCM and GEOS-Chem CTM and discuss improvements in the use of archived meteorology.
Xuan Wang, Colette L. Heald, Jiumeng Liu, Rodney J. Weber, Pedro Campuzano-Jost, Jose L. Jimenez, Joshua P. Schwarz, and Anne E. Perring
Atmos. Chem. Phys., 18, 635–653, https://doi.org/10.5194/acp-18-635-2018, https://doi.org/10.5194/acp-18-635-2018, 2018
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Brown carbon (BrC) contributes significantly to uncertainty in estimating the global direct radiative effect (DRE) of aerosols. We develop a global model simulation of BrC and test it against BrC absorption measurements from two aircraft campaigns in the continental United States. We suggest that BrC DRE has been overestimated previously due to the lack of observational constraints from direct measurements and omission of the effects of photochemical whitening.
Brett B. Palm, Suzane S. de Sá, Douglas A. Day, Pedro Campuzano-Jost, Weiwei Hu, Roger Seco, Steven J. Sjostedt, Jeong-Hoo Park, Alex B. Guenther, Saewung Kim, Joel Brito, Florian Wurm, Paulo Artaxo, Ryan Thalman, Jian Wang, Lindsay D. Yee, Rebecca Wernis, Gabriel Isaacman-VanWertz, Allen H. Goldstein, Yingjun Liu, Stephen R. Springston, Rodrigo Souza, Matt K. Newburn, M. Lizabeth Alexander, Scot T. Martin, and Jose L. Jimenez
Atmos. Chem. Phys., 18, 467–493, https://doi.org/10.5194/acp-18-467-2018, https://doi.org/10.5194/acp-18-467-2018, 2018
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Ambient air was oxidized by OH or O3 in an oxidation flow reactor during both wet and dry seasons in the GoAmazon2014/5 campaign to study secondary organic aerosol (SOA) formation. We investigated how much biogenic, urban, and biomass burning sources contributed to the ambient concentrations of SOA precursor gases and how their contributions changed diurnally and seasonally. SOA yields and hygroscopicity of organic aerosol in the oxidation flow reactor were also studied.
Theodore K. Koenig, Rainer Volkamer, Sunil Baidar, Barbara Dix, Siyuan Wang, Daniel C. Anderson, Ross J. Salawitch, Pamela A. Wales, Carlos A. Cuevas, Rafael P. Fernandez, Alfonso Saiz-Lopez, Mathew J. Evans, Tomás Sherwen, Daniel J. Jacob, Johan Schmidt, Douglas Kinnison, Jean-François Lamarque, Eric C. Apel, James C. Bresch, Teresa Campos, Frank M. Flocke, Samuel R. Hall, Shawn B. Honomichl, Rebecca Hornbrook, Jørgen B. Jensen, Richard Lueb, Denise D. Montzka, Laura L. Pan, J. Michael Reeves, Sue M. Schauffler, Kirk Ullmann, Andrew J. Weinheimer, Elliot L. Atlas, Valeria Donets, Maria A. Navarro, Daniel Riemer, Nicola J. Blake, Dexian Chen, L. Gregory Huey, David J. Tanner, Thomas F. Hanisco, and Glenn M. Wolfe
Atmos. Chem. Phys., 17, 15245–15270, https://doi.org/10.5194/acp-17-15245-2017, https://doi.org/10.5194/acp-17-15245-2017, 2017
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Tropospheric inorganic bromine (BrO and Bry) shows a C-shaped profile over the tropical western Pacific Ocean, and supports previous speculation that marine convection is a source for inorganic bromine from sea salt to the upper troposphere. The Bry profile in the tropical tropopause layer (TTL) is complex, suggesting that the total Bry budget in the TTL is not closed without considering aerosol bromide. The implications for atmospheric composition and bromine sources are discussed.
Ben Newsome and Mat Evans
Atmos. Chem. Phys., 17, 14333–14352, https://doi.org/10.5194/acp-17-14333-2017, https://doi.org/10.5194/acp-17-14333-2017, 2017
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We explore the uncertainty in the predictions of a chemical transport model (GEOS-Chem) from uncertainty in 60 inorganic rate constants and photolysis rates. We find uncertainty in the global mean ozone burden of 10 %, in global mean OH of 16 %, methane lifetimes of 16 %, and tropospheric ozone radiative forcings of 13 %. Reductions in the uncertainty of rate constants of these simple reactions would reduce uncertainty in our understanding of atmospheric composition.
Demetrios Pagonis, Jordan E. Krechmer, Joost de Gouw, Jose L. Jimenez, and Paul J. Ziemann
Atmos. Meas. Tech., 10, 4687–4696, https://doi.org/10.5194/amt-10-4687-2017, https://doi.org/10.5194/amt-10-4687-2017, 2017
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Laboratory studies were conducted to investigate gas-wall partitioning of atmospheric organic compounds in Teflon tubing and inside an instrument used to monitor concentrations. Rapid partitioning caused time delays in instrument response that vary with tubing length and diameter, flow rate, and compound volatility. Tubing delay times of seconds to hours were described using a model that also included effects of instrument surfaces. The results can enable better design of air sampling systems.
Peter M. Edwards and Mathew J. Evans
Atmos. Chem. Phys., 17, 13669–13680, https://doi.org/10.5194/acp-17-13669-2017, https://doi.org/10.5194/acp-17-13669-2017, 2017
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Understanding tropospheric ozone chemistry has been at the centre of the field of atmospheric chemistry for the last 30 years. However, our conceptual approach to diagnosing ozone production in global models has not advanced in this time. Our work presents a new and powerful approach for diagnosing tropospheric ozone production, providing a significant enhancement in our ability to understand the processes controlling ozone and how we can validate our assessment of these processes.
Joshua L. Laughner and Ronald C. Cohen
Atmos. Meas. Tech., 10, 4403–4419, https://doi.org/10.5194/amt-10-4403-2017, https://doi.org/10.5194/amt-10-4403-2017, 2017
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NO2 (a gas that plays an important role in air quality) can be measured by satellite-based instruments. These measurements require a best guess of the vertical distribution of NO2 and are very sensitive to the changes in that distribution near the top of the troposphere (~ 12 km). NO2 concentrations at this altitude are strongly influenced by lightning; therefore, we study how different representations of lightning in models that provide that best guess affect the NO2 measured by satellites.
Adrian M. Maclean, Christopher L. Butenhoff, James W. Grayson, Kelley Barsanti, Jose L. Jimenez, and Allan K. Bertram
Atmos. Chem. Phys., 17, 13037–13048, https://doi.org/10.5194/acp-17-13037-2017, https://doi.org/10.5194/acp-17-13037-2017, 2017
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Using laboratory data, meteorological fields and a chemical transport model, we investigated how often mixing times are < 1 h within SOA in the planetary boundary layer (PBL). Based on viscosity data for alpha-pinene SOA generated using mass concentrations of ~1000 µg m −3, mixing times in biogenic SOA are < 1h most of the time.
Jerald R. Ziemke, Sarah A. Strode, Anne R. Douglass, Joanna Joiner, Alexander Vasilkov, Luke D. Oman, Junhua Liu, Susan E. Strahan, Pawan K. Bhartia, and David P. Haffner
Atmos. Meas. Tech., 10, 4067–4078, https://doi.org/10.5194/amt-10-4067-2017, https://doi.org/10.5194/amt-10-4067-2017, 2017
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We combine satellite measurements of ozone and cloud properties from the Aura OMI and MLS instruments for 2004–2016 to measure ozone in the mid–upper levels of deep convective clouds. Our results ascribe upward injection of low boundary layer ozone (varying from low to high amounts) as a major driver of the measured concentrations of ozone in thick clouds. Our OMI/MLS generated ozone product is made available to the public for use in science applications.
Zhe Peng and Jose L. Jimenez
Atmos. Chem. Phys., 17, 11991–12010, https://doi.org/10.5194/acp-17-11991-2017, https://doi.org/10.5194/acp-17-11991-2017, 2017
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Oxidation flow reactors (OFRs) have been increasingly used to study atmospheric chemistry at high NO. We show that it is very difficult to obtain high-NO chemistry (in terms of RO2 fate) in OFRs by initial NO injection. Past OFR studies with combustion sources generally had too-high precursor and NOx concentrations that caused several types of experimental artifacts. A strong dilution (× 100 or larger) may be needed for such experiments to avoid undesired chemistry.
Ryan Thalman, Suzane S. de Sá, Brett B. Palm, Henrique M. J. Barbosa, Mira L. Pöhlker, M. Lizabeth Alexander, Joel Brito, Samara Carbone, Paulo Castillo, Douglas A. Day, Chongai Kuang, Antonio Manzi, Nga Lee Ng, Arthur J. Sedlacek III, Rodrigo Souza, Stephen Springston, Thomas Watson, Christopher Pöhlker, Ulrich Pöschl, Meinrat O. Andreae, Paulo Artaxo, Jose L. Jimenez, Scot T. Martin, and Jian Wang
Atmos. Chem. Phys., 17, 11779–11801, https://doi.org/10.5194/acp-17-11779-2017, https://doi.org/10.5194/acp-17-11779-2017, 2017
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Particle hygroscopicity, mixing state, and the hygroscopicity of organic components were characterized in central Amazonia for 1 year; their seasonal and diel variations were driven by a combination of primary emissions, photochemical oxidation, and boundary layer development. The relationship between the hygroscopicity of organic components and their oxidation level was examined, and the results help to reconcile the differences among the relationships observed in previous studies.
Daniel L. Goldberg, Lok N. Lamsal, Christopher P. Loughner, William H. Swartz, Zifeng Lu, and David G. Streets
Atmos. Chem. Phys., 17, 11403–11421, https://doi.org/10.5194/acp-17-11403-2017, https://doi.org/10.5194/acp-17-11403-2017, 2017
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We developed a new satellite NO2 product using a high spatial resolution (1.33 × 1.33 km) model simulation constrained by aircraft observations. The high-resolution satellite product is now able to observe the spatial heterogeneities of NO2 pollution over a large area with more clarity. The satellite is now in better agreement with monitors at ground level observing the same pollution.
Benjamin N. Murphy, Matthew C. Woody, Jose L. Jimenez, Ann Marie G. Carlton, Patrick L. Hayes, Shang Liu, Nga L. Ng, Lynn M. Russell, Ari Setyan, Lu Xu, Jeff Young, Rahul A. Zaveri, Qi Zhang, and Havala O. T. Pye
Atmos. Chem. Phys., 17, 11107–11133, https://doi.org/10.5194/acp-17-11107-2017, https://doi.org/10.5194/acp-17-11107-2017, 2017
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We incorporate recent findings about the behavior of organic pollutants in urban airsheds into the Community Multiscale Air Quality (CMAQ) model to refine predictions of organic particulate pollution in the United States. The new techniques, which account for the volatility and ongoing chemistry of airborne organic compounds, substantially reduce biases, particularly in the winter time and near emission sources.
Peter Knippertz, Andreas H. Fink, Adrien Deroubaix, Eleanor Morris, Flore Tocquer, Mat J. Evans, Cyrille Flamant, Marco Gaetani, Christophe Lavaysse, Celine Mari, John H. Marsham, Rémi Meynadier, Abalo Affo-Dogo, Titike Bahaga, Fabien Brosse, Konrad Deetz, Ridha Guebsi, Issaou Latifou, Marlon Maranan, Philip D. Rosenberg, and Andreas Schlueter
Atmos. Chem. Phys., 17, 10893–10918, https://doi.org/10.5194/acp-17-10893-2017, https://doi.org/10.5194/acp-17-10893-2017, 2017
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In June–July 2016 DACCIWA (Dynamics–Aerosol–Chemistry–Cloud Interactions in West Africa), a large, EU-funded European–African project, organised an international field campaign in densely populated southern West Africa, including measurements from ground sites, research aircraft, weather balloons and urban sites. This paper gives an overview of the atmospheric evolution during this period focusing on meteorological (precipitation, cloudiness, winds) and composition (gases, particles) aspects.
Jakob Lindaas, Delphine K. Farmer, Ilana B. Pollack, Andrew Abeleira, Frank Flocke, Rob Roscioli, Scott Herndon, and Emily V. Fischer
Atmos. Chem. Phys., 17, 10691–10707, https://doi.org/10.5194/acp-17-10691-2017, https://doi.org/10.5194/acp-17-10691-2017, 2017
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Wildfire smoke is becoming increasingly important for air quality in the US. We used measurements taken during the summer 2015 near Denver, CO, to provide a case study of how wildfire smoke can impact air quality, specifically ozone, which is harmful to humans. Wildfire smoke during this time period was associated with about 15 % more ozone than we would expect under normal conditions. This smoke came from fires in the Pacific Northwest and likely impacted much of the central and western US.
Nickolay A. Krotkov, Lok N. Lamsal, Edward A. Celarier, William H. Swartz, Sergey V. Marchenko, Eric J. Bucsela, Ka Lok Chan, Mark Wenig, and Marina Zara
Atmos. Meas. Tech., 10, 3133–3149, https://doi.org/10.5194/amt-10-3133-2017, https://doi.org/10.5194/amt-10-3133-2017, 2017
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We describe the new version 3 OMI NO2 standard product (SPv3) based on significant improvements in both the estimation of the SCDs and the AMFs. The new SCDs and stratospheric VCDs are systematically lower (by ~ 10–40 %) than previous estimates. Tropospheric VCDs are also reduced over polluted areas. Initial evaluation over unpolluted areas has shown that the new SPv3 products agree better with independent satellite- and ground-based FTIR measurements.
Carlena J. Ebben, Tamara L. Sparks, Paul J. Wooldridge, Teresa L. Campos, Christopher A. Cantrell, Roy L. Mauldin, Andrew J. Weinheimer, and Ronald C. Cohen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-671, https://doi.org/10.5194/acp-2017-671, 2017
Revised manuscript has not been submitted
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We use observations from the FRAPPÉ campaign to examine the evolution of reactive nitrogen as it is transported from Denver. We provide estimates for dilution rates, chemical lifetimes, and deposition rates. While dilution is the primary loss process in the immediate outflow from Denver, chemically, a majority of NOx is converted to HNO3 and is subsequently deposited. Understanding the evolution of reactive nitrogen informs how urban emissions affect air quality in the surrounding regions.
Abigail Koss, Bin Yuan, Carsten Warneke, Jessica B. Gilman, Brian M. Lerner, Patrick R. Veres, Jeff Peischl, Scott Eilerman, Rob Wild, Steven S. Brown, Chelsea R. Thompson, Thomas Ryerson, Thomas Hanisco, Glenn M. Wolfe, Jason M. St. Clair, Mitchell Thayer, Frank N. Keutsch, Shane Murphy, and Joost de Gouw
Atmos. Meas. Tech., 10, 2941–2968, https://doi.org/10.5194/amt-10-2941-2017, https://doi.org/10.5194/amt-10-2941-2017, 2017
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Oil and gas extraction activity can cause air quality issues through emission of reactive chemicals. VOCs related to extraction operations in the United States were measured by PTR-ToF-MS from aircraft during the SONGNEX campaign in March–April 2015. The detailed analysis in this work provides a guide to interpreting PTR-ToF measurements in oil- and gas-producing regions, and it includes fundamental observations of VOC speciation and mixing ratios.
Weiwei Hu, Pedro Campuzano-Jost, Douglas A. Day, Philip Croteau, Manjula R. Canagaratna, John T. Jayne, Douglas R. Worsnop, and Jose L. Jimenez
Atmos. Meas. Tech., 10, 2897–2921, https://doi.org/10.5194/amt-10-2897-2017, https://doi.org/10.5194/amt-10-2897-2017, 2017
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Aerosol mass spectrometers (AMS) from ARI are used widely to measure the non-refractory species in PM1. Recently, a new capture vapourizer (CV) has been designed to reduce the need for a bounce-related CE correction in the commonly used standard vapourizer (SV) installed in AMS. To test the CV, the fragments, CE and size distributions of four pure inorganic species in the CV-AMS are investigated in various laboratory experiments. Results from the co-located SV-AMS are also shown as a comparison.
Prettiny K. Ma, Yunliang Zhao, Allen L. Robinson, David R. Worton, Allen H. Goldstein, Amber M. Ortega, Jose L. Jimenez, Peter Zotter, André S. H. Prévôt, Sönke Szidat, and Patrick L. Hayes
Atmos. Chem. Phys., 17, 9237–9259, https://doi.org/10.5194/acp-17-9237-2017, https://doi.org/10.5194/acp-17-9237-2017, 2017
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Airborne particulate matter (PM) negatively impacts air quality in cities throughout the world. An important fraction of PM is organic aerosol. We have evaluated and developed several new models for secondary organic aerosol (SOA), which is formed from the chemical processing of gaseous precursors. Using our model results, we have quantified important SOA sources and precursors and also identified possible model parameterizations that could be used for air quality predictions.
Katherine R. Travis, Daniel J. Jacob, Christoph A. Keller, Shi Kuang, Jintai Lin, Michael J. Newchurch, and Anne M. Thompson
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-596, https://doi.org/10.5194/acp-2017-596, 2017
Preprint retracted
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Models severely overestimate surface ozone in the Southeast US during summertime which has implications for the design of air quality regulations. We use a model (GEOS-Chem) to interpret ozone observations from a suite of observations taken during August–September 2013. The model is unbiased relative to observations below 1 km but is biased high at the surface. We attribute this bias to model representation error, an underestimate in low-cloud, and insufficient treatment of vertical mixing.
Michael J. Prather, Xin Zhu, Clare M. Flynn, Sarah A. Strode, Jose M. Rodriguez, Stephen D. Steenrod, Junhua Liu, Jean-Francois Lamarque, Arlene M. Fiore, Larry W. Horowitz, Jingqiu Mao, Lee T. Murray, Drew T. Shindell, and Steven C. Wofsy
Atmos. Chem. Phys., 17, 9081–9102, https://doi.org/10.5194/acp-17-9081-2017, https://doi.org/10.5194/acp-17-9081-2017, 2017
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We present a new approach for comparing atmospheric chemistry models with measurements based on what these models are used to do, i.e., calculate changes in ozone and methane, prime greenhouse gases. This method anticipates a new type of measurements from the NASA Atmospheric Tomography (ATom) mission. In comparing the mixture of species within air parcels, we focus on those responsible for key chemical changes and weight these parcels by their chemical reactivity.
Viral Shah and Lyatt Jaeglé
Atmos. Chem. Phys., 17, 8999–9017, https://doi.org/10.5194/acp-17-8999-2017, https://doi.org/10.5194/acp-17-8999-2017, 2017
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We use a model of mercury chemistry and transport in the atmosphere, along with ground- and aircraft-based mercury observations, to learn that oxidized mercury chemically produced in the free troposphere descends in the subtropical anticyclones and makes up much of the mercury depositing to the Earth's surface. Our findings imply that mercury chemistry in the free troposphere and transport in the subtropics are important links between global emissions and surface deposition of mercury.
Christopher Chan Miller, Daniel J. Jacob, Eloise A. Marais, Karen Yu, Katherine R. Travis, Patrick S. Kim, Jenny A. Fisher, Lei Zhu, Glenn M. Wolfe, Thomas F. Hanisco, Frank N. Keutsch, Jennifer Kaiser, Kyung-Eun Min, Steven S. Brown, Rebecca A. Washenfelder, Gonzalo González Abad, and Kelly Chance
Atmos. Chem. Phys., 17, 8725–8738, https://doi.org/10.5194/acp-17-8725-2017, https://doi.org/10.5194/acp-17-8725-2017, 2017
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The use of satellite glyoxal observations for estimating isoprene emissions has been limited by knowledge of the glyoxal yield from isoprene. We use SENEX aircraft observations over the southeast US to evaluate glyoxal yields from isoprene in a 3-D atmospheric model. The SENEX observations support a pathway for glyoxal formation in pristine regions that we propose here, which may have implications for improving isoprene emissions estimates from upcoming high-resolution geostationary satellites.
Hyun-Deok Choi, Hongyu Liu, James H. Crawford, David B. Considine, Dale J. Allen, Bryan N. Duncan, Larry W. Horowitz, Jose M. Rodriguez, Susan E. Strahan, Lin Zhang, Xiong Liu, Megan R. Damon, and Stephen D. Steenrod
Atmos. Chem. Phys., 17, 8429–8452, https://doi.org/10.5194/acp-17-8429-2017, https://doi.org/10.5194/acp-17-8429-2017, 2017
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We evaluate global ozone–carbon monoxide (O3–CO) correlations in a chemistry and transport model during July–August with TES-Aura satellite observations and examine the sensitivity of model simulations to input meteorological data and emissions. Results show that O3–CO correlations may be used effectively to constrain the sources of regional tropospheric O3 in global 3-D models, especially for those regions where convective transport of pollution plays an important role.
Xueling Liu, Arthur P. Mizzi, Jeffrey L. Anderson, Inez Y. Fung, and Ronald C. Cohen
Atmos. Chem. Phys., 17, 7067–7081, https://doi.org/10.5194/acp-17-7067-2017, https://doi.org/10.5194/acp-17-7067-2017, 2017
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We describe a chemical ensemble data assimilation system with high spatial and temporal resolution that simultaneously adjusts meteorological and chemical variables and NOx emissions. We investigate the sensitivity of emission inversions to the accuracy and uncertainty of the wind analyses and the emission update scheme. The results provide insight into optimal uses of the observations from future geostationary satellite missions that will observe atmospheric composition.
A. Anthony Bloom, Kevin W. Bowman, Meemong Lee, Alexander J. Turner, Ronny Schroeder, John R. Worden, Richard Weidner, Kyle C. McDonald, and Daniel J. Jacob
Geosci. Model Dev., 10, 2141–2156, https://doi.org/10.5194/gmd-10-2141-2017, https://doi.org/10.5194/gmd-10-2141-2017, 2017
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Wetland emissions are a principal source of uncertainty in the global atmospheric methane budget due to poor knowledge of wetland processes. We construct a wetland methane emission and uncertainty dataset for use in global atmospheric methane models. Our wetland model ensemble is based on static wetland maps, satellite-derived inundation and carbon cycle models. The ensemble performs favourably against regional flux estimates and atmospheric methane measurements relative to previous studies.
Suzane S. de Sá, Brett B. Palm, Pedro Campuzano-Jost, Douglas A. Day, Matthew K. Newburn, Weiwei Hu, Gabriel Isaacman-VanWertz, Lindsay D. Yee, Ryan Thalman, Joel Brito, Samara Carbone, Paulo Artaxo, Allen H. Goldstein, Antonio O. Manzi, Rodrigo A. F. Souza, Fan Mei, John E. Shilling, Stephen R. Springston, Jian Wang, Jason D. Surratt, M. Lizabeth Alexander, Jose L. Jimenez, and Scot T. Martin
Atmos. Chem. Phys., 17, 6611–6629, https://doi.org/10.5194/acp-17-6611-2017, https://doi.org/10.5194/acp-17-6611-2017, 2017
Zhe Jiang, Helen Worden, John R. Worden, Daven K. Henze, Dylan B. A. Jones, Avelino F. Arellano, Emily V. Fischer, Liye Zhu, Kazuyuki Miyazaki, K. Folkert Boersma, and Vivienne H. Payne
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-382, https://doi.org/10.5194/acp-2017-382, 2017
Preprint withdrawn
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We investigated the variation of US tropospheric NO2 in the past decade. We demonstrated significant divergence between the time variation in tropospheric NO2 columns from OMI retrievals and surface measurements. Our analysis suggests limited contributions from local effects such as fossil fuel emissions, lightning, or instrument artifacts, and indicates possible important contributions from long-range transport of Asian emissions that are modulated by ENSO.
Caroline C. Womack, J. Andrew Neuman, Patrick R. Veres, Scott J. Eilerman, Charles A. Brock, Zachary C. J. Decker, Kyle J. Zarzana, William P. Dube, Robert J. Wild, Paul J. Wooldridge, Ronald C. Cohen, and Steven S. Brown
Atmos. Meas. Tech., 10, 1911–1926, https://doi.org/10.5194/amt-10-1911-2017, https://doi.org/10.5194/amt-10-1911-2017, 2017
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The accurate detection of reactive nitrogen species (NOy) is key to understanding tropospheric ozone production. Typically, NOy is detected by thermal conversion to NO2, followed by NO2 detection. Here, we assess the conversion efficiency of several NOy species to NO2 in a thermal dissociation cavity ring-down spectrometer and discuss how this conversion efficiency is affected by certain experimental conditions, such as oven residence time, and interferences from non-NOy species.
Hannah M. Horowitz, Daniel J. Jacob, Yanxu Zhang, Theodore S. Dibble, Franz Slemr, Helen M. Amos, Johan A. Schmidt, Elizabeth S. Corbitt, Eloïse A. Marais, and Elsie M. Sunderland
Atmos. Chem. Phys., 17, 6353–6371, https://doi.org/10.5194/acp-17-6353-2017, https://doi.org/10.5194/acp-17-6353-2017, 2017
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Mercury is a toxic, global pollutant released to the air from human activities like coal burning. Chemical reactions in air determine how far mercury is transported before it is deposited to the environment, where it may be converted to a form that accumulates in fish. We use a 3-D atmospheric model to evaluate a new set of chemical reactions and its effects on mercury deposition. We find it is consistent with observations and leads to increased deposition to oceans, especially in the tropics.
Hongyu Guo, Jiumeng Liu, Karl D. Froyd, James M. Roberts, Patrick R. Veres, Patrick L. Hayes, Jose L. Jimenez, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 17, 5703–5719, https://doi.org/10.5194/acp-17-5703-2017, https://doi.org/10.5194/acp-17-5703-2017, 2017
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Fine particle pH is linked to many environmental impacts by affecting particle concentration and composition. Predicted Pasadena, CA (CalNex campaign), PM1 pH is 1.9 and PM2.5 pH 2.7, the latter higher due to sea salts. The model predicted gas–particle partitionings of HNO3–NO3−, NH3–NH4+, and HCl–Cl− are in good agreement, verifying the model predictions. A summary of contrasting locations in the US and eastern Mediterranean shows fine particles are generally highly acidic, with pH below 3.
Katie A. Read, Luis M. Neves, Lucy J. Carpenter, Alastair C. Lewis, Zoe L. Fleming, and John Kentisbeer
Atmos. Chem. Phys., 17, 5393–5406, https://doi.org/10.5194/acp-17-5393-2017, https://doi.org/10.5194/acp-17-5393-2017, 2017
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This paper presents 4 years of total gaseous mercury data obtained from measurements made at the Cape Verde Atmospheric Observatory, a subtropical site in the Atlantic Ocean. The data show a clear decreasing trend in the overall concentrations but in air from sub-Saharan Africa the trend is less significant and the data more variable. We attribute this result to an influence from artisanal small-scale gold mining in this region, a source for which there is uncertain information.
Brett B. Palm, Pedro Campuzano-Jost, Douglas A. Day, Amber M. Ortega, Juliane L. Fry, Steven S. Brown, Kyle J. Zarzana, William Dube, Nicholas L. Wagner, Danielle C. Draper, Lisa Kaser, Werner Jud, Thomas Karl, Armin Hansel, Cándido Gutiérrez-Montes, and Jose L. Jimenez
Atmos. Chem. Phys., 17, 5331–5354, https://doi.org/10.5194/acp-17-5331-2017, https://doi.org/10.5194/acp-17-5331-2017, 2017
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Ambient forest air was oxidized by OH, O3, or NO3 inside an oxidation flow reactor, leading to formation of particulate matter from any gaseous precursors found in the air. Closure was achieved between the amount of particulate mass formed from O3 and NO3 oxidation and the amount predicted from speciated gaseous precursors, which was in contrast to previous results for OH oxidation (Palm et al., 2016). Elemental analysis of the particulate mass formed in the reactor is presented.
Rachel F. Silvern, Daniel J. Jacob, Patrick S. Kim, Eloise A. Marais, Jay R. Turner, Pedro Campuzano-Jost, and Jose L. Jimenez
Atmos. Chem. Phys., 17, 5107–5118, https://doi.org/10.5194/acp-17-5107-2017, https://doi.org/10.5194/acp-17-5107-2017, 2017
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We identify a fundamental discrepancy between thermodynamic equilibrium theory and observations of inorganic aerosol composition in the eastern US in summer that shows low ammonium sulfate aerosol ratios. In addition, from 2003 to 2013, while SO2 emissions have declined due to US emission controls, aerosols have become more acidic in the southeastern US. To explain these observations, we suggest that the large and increasing source of organic aerosol may be affecting thermodynamic equilibrium.
Bin Yuan, Matthew M. Coggon, Abigail R. Koss, Carsten Warneke, Scott Eilerman, Jeff Peischl, Kenneth C. Aikin, Thomas B. Ryerson, and Joost A. de Gouw
Atmos. Chem. Phys., 17, 4945–4956, https://doi.org/10.5194/acp-17-4945-2017, https://doi.org/10.5194/acp-17-4945-2017, 2017
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In this study, we measured emissions of volatile organic compounds (VOCs) from concentrated animal feeding operations (CAFOs) using both mobile laboratory and aircraft measurements. We will use this data set to investigate chemical compositions of VOC emissions and sources apportionment for these VOC emissions in different facilities.
Chris Reed, Mathew J. Evans, Leigh R. Crilley, William J. Bloss, Tomás Sherwen, Katie A. Read, James D. Lee, and Lucy J. Carpenter
Atmos. Chem. Phys., 17, 4081–4092, https://doi.org/10.5194/acp-17-4081-2017, https://doi.org/10.5194/acp-17-4081-2017, 2017
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The source of ozone-depleting compounds in the remote troposphere has been thought to be long-range transport of secondary pollutants such as organic nitrates. Processing of organic nitrates to nitric acid and subsequent deposition on surfaces in the atmosphere was thought to remove these nitrates from the ozone–NOx–HOx cycle. We found through observation of NOx in the remote tropical troposphere at the Cape Verde Observatory that surface nitrates can be released back into the atmosphere.
Chelsea R. Thompson, Paul B. Shepson, Jin Liao, L. Greg Huey, Chris Cantrell, Frank Flocke, and John Orlando
Atmos. Chem. Phys., 17, 3401–3421, https://doi.org/10.5194/acp-17-3401-2017, https://doi.org/10.5194/acp-17-3401-2017, 2017
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The generally accepted mechanism leading to ozone depletion events in the Arctic assumes efficient gas-phase recycling of bromine atoms, such that the rate of ozone depletion has often been estimated as the rate that Br atoms regenerate through gas-phase BrO + BrO and BrO + ClO reactions. Using a large suite of data from the OASIS2009 campaign, our modeling results show that the gas-phase regeneration of Br is less efficient than expected and that heterogeneous recycling on surfaces is critical.
Alba Lorente, K. Folkert Boersma, Huan Yu, Steffen Dörner, Andreas Hilboll, Andreas Richter, Mengyao Liu, Lok N. Lamsal, Michael Barkley, Isabelle De Smedt, Michel Van Roozendael, Yang Wang, Thomas Wagner, Steffen Beirle, Jin-Tai Lin, Nickolay Krotkov, Piet Stammes, Ping Wang, Henk J. Eskes, and Maarten Krol
Atmos. Meas. Tech., 10, 759–782, https://doi.org/10.5194/amt-10-759-2017, https://doi.org/10.5194/amt-10-759-2017, 2017
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Choices and assumptions made to represent the state of the atmosphere introduce an uncertainty of 42 % in the air mass factor calculation in trace gas satellite retrievals in polluted regions. The AMF strongly depends on the choice of a priori trace gas profile, surface albedo data set and the correction method to account for clouds and aerosols. We call for well-designed validation exercises focusing on situations when AMF structural uncertainty has the highest impact on satellite retrievals.
Sebastian D. Eastham and Daniel J. Jacob
Atmos. Chem. Phys., 17, 2543–2553, https://doi.org/10.5194/acp-17-2543-2017, https://doi.org/10.5194/acp-17-2543-2017, 2017
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Intercontinental atmospheric transport can disrupt local chemistry and cause air quality issues thousands of kilometers from the source, complicating correct attribution of air quality exceedances. This transport occurs in long, thin plumes which current-generation models consistently fail to reproduce. Our study investigates the cause of this failure, finding that greater vertical resolution than is currently available is required to reliably resolve the plumes and their effects.
Jason E. Williams, K. Folkert Boersma, Phillipe Le Sager, and Willem W. Verstraeten
Geosci. Model Dev., 10, 721–750, https://doi.org/10.5194/gmd-10-721-2017, https://doi.org/10.5194/gmd-10-721-2017, 2017
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The launch of Earth-orbiting satellites with small footprints necessitates the development of global chemistry transport models which are able to differentiate between high- and low-emission regimes and provide dedicated a priori tropospheric columns of trace gas species for the purpose of deriving accurate retrievals of integrated columns. We focus on the effects introduced with respect to global trace gas distributions in TM5-MP when increasing horizontal resolution from 3 × 2 to 1 × 1 degrees.
Nga Lee Ng, Steven S. Brown, Alexander T. Archibald, Elliot Atlas, Ronald C. Cohen, John N. Crowley, Douglas A. Day, Neil M. Donahue, Juliane L. Fry, Hendrik Fuchs, Robert J. Griffin, Marcelo I. Guzman, Hartmut Herrmann, Alma Hodzic, Yoshiteru Iinuma, José L. Jimenez, Astrid Kiendler-Scharr, Ben H. Lee, Deborah J. Luecken, Jingqiu Mao, Robert McLaren, Anke Mutzel, Hans D. Osthoff, Bin Ouyang, Benedicte Picquet-Varrault, Ulrich Platt, Havala O. T. Pye, Yinon Rudich, Rebecca H. Schwantes, Manabu Shiraiwa, Jochen Stutz, Joel A. Thornton, Andreas Tilgner, Brent J. Williams, and Rahul A. Zaveri
Atmos. Chem. Phys., 17, 2103–2162, https://doi.org/10.5194/acp-17-2103-2017, https://doi.org/10.5194/acp-17-2103-2017, 2017
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Oxidation of biogenic volatile organic compounds by NO3 is an important interaction between anthropogenic
and natural emissions. This review results from a June 2015 workshop and includes the recent literature
on kinetics, mechanisms, organic aerosol yields, and heterogeneous chemistry; advances in analytical
instrumentation; the current state NO3-BVOC chemistry in atmospheric models; and critical needs for
future research in modeling, field observations, and laboratory studies.
Adam P. Bateman, Zhaoheng Gong, Tristan H. Harder, Suzane S. de Sá, Bingbing Wang, Paulo Castillo, Swarup China, Yingjun Liu, Rachel E. O'Brien, Brett B. Palm, Hung-Wei Shiu, Glauber G. Cirino, Ryan Thalman, Kouji Adachi, M. Lizabeth Alexander, Paulo Artaxo, Allan K. Bertram, Peter R. Buseck, Mary K. Gilles, Jose L. Jimenez, Alexander Laskin, Antonio O. Manzi, Arthur Sedlacek, Rodrigo A. F. Souza, Jian Wang, Rahul Zaveri, and Scot T. Martin
Atmos. Chem. Phys., 17, 1759–1773, https://doi.org/10.5194/acp-17-1759-2017, https://doi.org/10.5194/acp-17-1759-2017, 2017
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The occurrence of nonliquid and liquid physical states of submicron atmospheric particulate matter (PM) downwind of an urban region in central Amazonia was investigated. Air masses representing background conditions, urban pollution, and regional- and continental-scale biomass were measured. Anthropogenic influences contributed to the presence of nonliquid PM in the atmospheric particle population, while liquid PM dominated during periods of biogenic influence.
Tomás Sherwen, Mat J. Evans, Lucy J. Carpenter, Johan A. Schmidt, and Loretta J. Mickley
Atmos. Chem. Phys., 17, 1557–1569, https://doi.org/10.5194/acp-17-1557-2017, https://doi.org/10.5194/acp-17-1557-2017, 2017
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We model pre-industrial to present day changes using the GEOS-Chem global chemical transport model with halogens (Cl, Br, I). The model better captures pre-industrial O3 observations with halogens included. Halogens buffer the tropospheric forcing of O3 (RFTO3) from pre-industrial to present day, reducing RFTO3 by 0.087 Wm−2. This reduction is greater than that from halogens on stratospheric O3 (−0.05 Wm−2). This suggests that models that do not include halogens will overestimate RFTO3by ~ 25%.
Alexander Vasilkov, Wenhan Qin, Nickolay Krotkov, Lok Lamsal, Robert Spurr, David Haffner, Joanna Joiner, Eun-Su Yang, and Sergey Marchenko
Atmos. Meas. Tech., 10, 333–349, https://doi.org/10.5194/amt-10-333-2017, https://doi.org/10.5194/amt-10-333-2017, 2017
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We show how the surface reflection can vary day to day in the blue part of the sun's spectrum where we measure the pollutant gas nitrogen dioxide using a satellite instrument called OMI. We use information from an imaging spectrometer on another satellite, MODIS, to estimate the angular surface effects. We can then use models of how the sunlight travels through the atmosphere to predict how the angle-dependent surface reflection will impact the values of pollutant levels inferred by OMI.
Brian M. Lerner, Jessica B. Gilman, Kenneth C. Aikin, Elliot L. Atlas, Paul D. Goldan, Martin Graus, Roger Hendershot, Gabriel A. Isaacman-VanWertz, Abigail Koss, William C. Kuster, Richard A. Lueb, Richard J. McLaughlin, Jeff Peischl, Donna Sueper, Thomas B. Ryerson, Travis W. Tokarek, Carsten Warneke, Bin Yuan, and Joost A. de Gouw
Atmos. Meas. Tech., 10, 291–313, https://doi.org/10.5194/amt-10-291-2017, https://doi.org/10.5194/amt-10-291-2017, 2017
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Whole air sampling followed by analysis by gas chromatography is a common technique for characterization of trace volatile organic compounds in the atmosphere. We describe a new automated gas chromatograph–mass spectrograph which uses a Stirling cooler for sample preconcentration at −165 °C without the need for a cryogen such as liquid nitrogen. We also discuss potential sources of artifacts from our electropolished stainless steel sampling system and present results from two field campaigns.
Havala O. T. Pye, Benjamin N. Murphy, Lu Xu, Nga L. Ng, Annmarie G. Carlton, Hongyu Guo, Rodney Weber, Petros Vasilakos, K. Wyat Appel, Sri Hapsari Budisulistiorini, Jason D. Surratt, Athanasios Nenes, Weiwei Hu, Jose L. Jimenez, Gabriel Isaacman-VanWertz, Pawel K. Misztal, and Allen H. Goldstein
Atmos. Chem. Phys., 17, 343–369, https://doi.org/10.5194/acp-17-343-2017, https://doi.org/10.5194/acp-17-343-2017, 2017
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We use a chemical transport model to examine how organic compounds in the atmosphere interact with water present in particles. Organic compounds themselves lead to water uptake, and organic compounds interact with water associated with inorganic compounds in the rural southeast atmosphere. Including interactions of organic compounds with water requires a treatment of nonideality to more accurately represent aerosol observations during the Southern Oxidant and Aerosol Study (SOAS) 2013.
Joshua L. Laughner, Azimeh Zare, and Ronald C. Cohen
Atmos. Chem. Phys., 16, 15247–15264, https://doi.org/10.5194/acp-16-15247-2016, https://doi.org/10.5194/acp-16-15247-2016, 2016
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Satellite measurements of the atmosphere provide global information on pollutants that play an important role in air quality. These measurements require assumed knowledge about the vertical profile of these pollutants, which are often simulated at coarse resolution in space and time. We find that simulating these inputs with better spatial and temporal resolution alters individual measurements by up to 40 % and the average measurement by up to 13 %, and increases derived emissions by up to 100 %.
Yaping Zhang, Brent J. Williams, Allen H. Goldstein, Kenneth S. Docherty, and Jose L. Jimenez
Atmos. Meas. Tech., 9, 5637–5653, https://doi.org/10.5194/amt-9-5637-2016, https://doi.org/10.5194/amt-9-5637-2016, 2016
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The binning method provides an alternate way to process GC–MS data in a very fast manner. It only takes a very small portion of time (days versus years) compared to the traditional GC–MS data analysis method (peak identification and integration). Furthermore, the binning method can also be applied to any data set from a measurement (mass spectrometry, spectroscopy, etc.) with additional separations (volatility, polarity, size, etc.).
Daniel J. Jacob, Alexander J. Turner, Joannes D. Maasakkers, Jianxiong Sheng, Kang Sun, Xiong Liu, Kelly Chance, Ilse Aben, Jason McKeever, and Christian Frankenberg
Atmos. Chem. Phys., 16, 14371–14396, https://doi.org/10.5194/acp-16-14371-2016, https://doi.org/10.5194/acp-16-14371-2016, 2016
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Methane is a greenhouse gas emitted by a range of natural and anthropogenic sources. Atmospheric methane has been measured continuously from space since 2003, and new instruments are planned to launch in the near future that will greatly expand the capabilities of space-based observations. We review the value of current, future, and proposed satellite observations to better quantify methane emissions from the global scale down to the scale of point sources.
Katherine R. Travis, Daniel J. Jacob, Jenny A. Fisher, Patrick S. Kim, Eloise A. Marais, Lei Zhu, Karen Yu, Christopher C. Miller, Robert M. Yantosca, Melissa P. Sulprizio, Anne M. Thompson, Paul O. Wennberg, John D. Crounse, Jason M. St. Clair, Ronald C. Cohen, Joshua L. Laughner, Jack E. Dibb, Samuel R. Hall, Kirk Ullmann, Glenn M. Wolfe, Illana B. Pollack, Jeff Peischl, Jonathan A. Neuman, and Xianliang Zhou
Atmos. Chem. Phys., 16, 13561–13577, https://doi.org/10.5194/acp-16-13561-2016, https://doi.org/10.5194/acp-16-13561-2016, 2016
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Ground-level ozone pollution in the Southeast US involves complex chemistry driven by anthropogenic emissions of nitrogen oxides (NOx) and biogenic emissions of isoprene. We find that US NOx emissions are overestimated nationally by as much as 50 % and that reducing model emissions by this amount results in good agreement with SEAC4RS aircraft measurements in August and September 2013. Observations of nitrate wet deposition fluxes and satellite NO2 columns further support this result.
Lei Zhu, Daniel J. Jacob, Patrick S. Kim, Jenny A. Fisher, Karen Yu, Katherine R. Travis, Loretta J. Mickley, Robert M. Yantosca, Melissa P. Sulprizio, Isabelle De Smedt, Gonzalo González Abad, Kelly Chance, Can Li, Richard Ferrare, Alan Fried, Johnathan W. Hair, Thomas F. Hanisco, Dirk Richter, Amy Jo Scarino, James Walega, Petter Weibring, and Glenn M. Wolfe
Atmos. Chem. Phys., 16, 13477–13490, https://doi.org/10.5194/acp-16-13477-2016, https://doi.org/10.5194/acp-16-13477-2016, 2016
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HCHO column data are widely used as a proxy for VOCs emissions, but validation of the data has been extremely limited. We use accurate aircraft observations to validate and intercompare 6 HCHO retrievals with GEOS-Chem as the intercomparison platform. Retrievals are interconsistent in spatial variability over the SE US and in daily variability, but are biased low by 20–51 %. Our work supports the use of HCHO column as a quantitative proxy for isoprene emission after correction of the low bias.
Alexander J. Turner, Alexis A. Shusterman, Brian C. McDonald, Virginia Teige, Robert A. Harley, and Ronald C. Cohen
Atmos. Chem. Phys., 16, 13465–13475, https://doi.org/10.5194/acp-16-13465-2016, https://doi.org/10.5194/acp-16-13465-2016, 2016
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Our paper investigates the ability of different types of observational networks to estimate urban CO2 emissions. We have quantified the trade-off between precision and network density for estimating urban greenhouse gas emissions. Our results show that different observing systems may fall into noise- or site-limited regimes where reducing the uncertainty in the estimated emissions is governed by a single factor.
Alexis A. Shusterman, Virginia E. Teige, Alexander J. Turner, Catherine Newman, Jinsol Kim, and Ronald C. Cohen
Atmos. Chem. Phys., 16, 13449–13463, https://doi.org/10.5194/acp-16-13449-2016, https://doi.org/10.5194/acp-16-13449-2016, 2016
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We describe the design of and first results from the BErkeley Atmospheric CO2 Observation Network, a distributed instrument of 28 CO2 sensors stationed across and around the city of Oakland, California at ~ 2 km intervals. We evaluate the network via 4 performance parameters (cost, reliability, precision, systematic uncertainty) and find this high density technique to be sufficiently cost-effective and rigorous to inform understanding of small-scale urban emissions relevant to climate regulation.
Iolanda Ialongo, Jay Herman, Nick Krotkov, Lok Lamsal, K. Folkert Boersma, Jari Hovila, and Johanna Tamminen
Atmos. Meas. Tech., 9, 5203–5212, https://doi.org/10.5194/amt-9-5203-2016, https://doi.org/10.5194/amt-9-5203-2016, 2016
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We present the comparison between satellite- and ground-based atmospheric NO2 observations in Helsinki (Finland). The results show that, despite some limitations due to cloud contamination and low solar angles, satellite data are able to describe urban air quality features such as the weekly and seasonal cycles. The results support air quality satellite data exploitation at high latitudes and prepare for similar applications for future missions.
Xuan Zhang, Jordan E. Krechmer, Michael Groessl, Wen Xu, Stephan Graf, Michael Cubison, John T. Jayne, Jose L. Jimenez, Douglas R. Worsnop, and Manjula R. Canagaratna
Atmos. Chem. Phys., 16, 12945–12959, https://doi.org/10.5194/acp-16-12945-2016, https://doi.org/10.5194/acp-16-12945-2016, 2016
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We develop a novel two-dimensional space to probe the molecular composition of atmospheric organic aerosols.
Tomás Sherwen, Johan A. Schmidt, Mat J. Evans, Lucy J. Carpenter, Katja Großmann, Sebastian D. Eastham, Daniel J. Jacob, Barbara Dix, Theodore K. Koenig, Roman Sinreich, Ivan Ortega, Rainer Volkamer, Alfonso Saiz-Lopez, Cristina Prados-Roman, Anoop S. Mahajan, and Carlos Ordóñez
Atmos. Chem. Phys., 16, 12239–12271, https://doi.org/10.5194/acp-16-12239-2016, https://doi.org/10.5194/acp-16-12239-2016, 2016
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We present a simulation of tropospheric Cl, Br, I chemistry within the GEOS-Chem CTM. We find a decrease in tropospheric ozone burden of 18.6 % and a 8.2 % decrease in global mean OH concentrations. Cl oxidation of some VOCs range from 15 to 27 % of the total loss. Bromine plays a small role in oxidising oVOCs. Surface ozone, ozone sondes, and methane lifetime are in general improved by the inclusion of halogens. We argue that simulated bromine and chlorine represent a lower limit.
Weiwei Hu, Brett B. Palm, Douglas A. Day, Pedro Campuzano-Jost, Jordan E. Krechmer, Zhe Peng, Suzane S. de Sá, Scot T. Martin, M. Lizabeth Alexander, Karsten Baumann, Lina Hacker, Astrid Kiendler-Scharr, Abigail R. Koss, Joost A. de Gouw, Allen H. Goldstein, Roger Seco, Steven J. Sjostedt, Jeong-Hoo Park, Alex B. Guenther, Saewung Kim, Francesco Canonaco, André S. H. Prévôt, William H. Brune, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 11563–11580, https://doi.org/10.5194/acp-16-11563-2016, https://doi.org/10.5194/acp-16-11563-2016, 2016
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IEPOX-SOA is biogenically derived secondary organic aerosol under anthropogenic influence, which has been shown to comprise a substantial fraction of OA globally. We investigated the lifetime of ambient IEPOX-SOA in the SE US and Amazonia, with an oxidation flow reactor and thermodenuder coupled with MS-based instrumentation. The low volatility and long lifetime of IEPOX-SOA against OH radicals' oxidation (> 2 weeks) was observed, which can help to constrain OA impact on air quality and climate.
Quazi Z. Rasool, Rui Zhang, Benjamin Lash, Daniel S. Cohan, Ellen J. Cooter, Jesse O. Bash, and Lok N. Lamsal
Geosci. Model Dev., 9, 3177–3197, https://doi.org/10.5194/gmd-9-3177-2016, https://doi.org/10.5194/gmd-9-3177-2016, 2016
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This study updates the representation of soil NO emissions in a regional air quality model. The implementation enhances the representation of biome types and dynamic fertilizer use. Previous modeling of soil NO in CMAQ had tended to under-estimate emissions and misrepresent their response to soil conditions and meteorology. We evaluate results against satellite observations of NO2, and quantify the impacts of the new parameterization on simulations of ozone and particulate matter.
Aki Pajunoja, Weiwei Hu, Yu J. Leong, Nathan F. Taylor, Pasi Miettinen, Brett B. Palm, Santtu Mikkonen, Don R. Collins, Jose L. Jimenez, and Annele Virtanen
Atmos. Chem. Phys., 16, 11163–11176, https://doi.org/10.5194/acp-16-11163-2016, https://doi.org/10.5194/acp-16-11163-2016, 2016
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The phase state of ambient particles was inferred from bounce measurements conducted at a rural site in central Alabama during the SOAS campaign. The organic-dominated ambient particles are mostly in the liquid phase at summertime conditions but they turn semisolid when dried in the measurement setup. Bounce humidograms reveal that the hygroscopicity and oxidation of the particles decreases the liquefying RH. The effect of oxidation is emphasized by oxidation flow reactor measurements.
Giancarlo Ciarelli, Sebnem Aksoyoglu, Monica Crippa, Jose-Luis Jimenez, Eriko Nemitz, Karine Sellegri, Mikko Äijälä, Samara Carbone, Claudia Mohr, Colin O'Dowd, Laurent Poulain, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 16, 10313–10332, https://doi.org/10.5194/acp-16-10313-2016, https://doi.org/10.5194/acp-16-10313-2016, 2016
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Recent studies based on aerosol mass spectrometer measurements revealed that the organic fraction dominates the non-refractory PM1 composition. However its representation in chemical transport models is still very challenging due to uncertainties in emission sources and formation pathways. In this study, a novel organic aerosol scheme was tested in the regional air quality model CAMx and results were compared with ambient measurements at 11 different sites in Europe.
Raquel A. Silva, J. Jason West, Jean-François Lamarque, Drew T. Shindell, William J. Collins, Stig Dalsoren, Greg Faluvegi, Gerd Folberth, Larry W. Horowitz, Tatsuya Nagashima, Vaishali Naik, Steven T. Rumbold, Kengo Sudo, Toshihiko Takemura, Daniel Bergmann, Philip Cameron-Smith, Irene Cionni, Ruth M. Doherty, Veronika Eyring, Beatrice Josse, Ian A. MacKenzie, David Plummer, Mattia Righi, David S. Stevenson, Sarah Strode, Sophie Szopa, and Guang Zengast
Atmos. Chem. Phys., 16, 9847–9862, https://doi.org/10.5194/acp-16-9847-2016, https://doi.org/10.5194/acp-16-9847-2016, 2016
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Using ozone and PM2.5 concentrations from the ACCMIP ensemble of chemistry-climate models for the four Representative Concentration Pathway scenarios (RCPs), together with projections of future population and baseline mortality rates, we quantify the human premature mortality impacts of future ambient air pollution in 2030, 2050 and 2100, relative to 2000 concentrations. We also estimate the global mortality burden of ozone and PM2.5 in 2000 and each future period.
Matthew J. Alvarado, Chantelle R. Lonsdale, Helen L. Macintyre, Huisheng Bian, Mian Chin, David A. Ridley, Colette L. Heald, Kenneth L. Thornhill, Bruce E. Anderson, Michael J. Cubison, Jose L. Jimenez, Yutaka Kondo, Lokesh K. Sahu, Jack E. Dibb, and Chien Wang
Atmos. Chem. Phys., 16, 9435–9455, https://doi.org/10.5194/acp-16-9435-2016, https://doi.org/10.5194/acp-16-9435-2016, 2016
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Understanding the scattering and absorption of light by aerosols is necessary for understanding air quality and climate change. We used data from the 2008 ARCTAS campaign to evaluate aerosol optical property models using a closure methodology that separates errors in these models from other errors in aerosol emissions, chemistry, or transport. We find that the models on average perform reasonably well, and make suggestions for how remaining biases could be reduced.
Carsten Warneke, Michael Trainer, Joost A. de Gouw, David D. Parrish, David W. Fahey, A. R. Ravishankara, Ann M. Middlebrook, Charles A. Brock, James M. Roberts, Steven S. Brown, Jonathan A. Neuman, Brian M. Lerner, Daniel Lack, Daniel Law, Gerhard Hübler, Iliana Pollack, Steven Sjostedt, Thomas B. Ryerson, Jessica B. Gilman, Jin Liao, John Holloway, Jeff Peischl, John B. Nowak, Kenneth C. Aikin, Kyung-Eun Min, Rebecca A. Washenfelder, Martin G. Graus, Mathew Richardson, Milos Z. Markovic, Nick L. Wagner, André Welti, Patrick R. Veres, Peter Edwards, Joshua P. Schwarz, Timothy Gordon, William P. Dube, Stuart A. McKeen, Jerome Brioude, Ravan Ahmadov, Aikaterini Bougiatioti, Jack J. Lin, Athanasios Nenes, Glenn M. Wolfe, Thomas F. Hanisco, Ben H. Lee, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Frank N. Keutsch, Jennifer Kaiser, Jingqiu Mao, and Courtney D. Hatch
Atmos. Meas. Tech., 9, 3063–3093, https://doi.org/10.5194/amt-9-3063-2016, https://doi.org/10.5194/amt-9-3063-2016, 2016
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In this paper we describe the experimental approach, the science goals and early results of the NOAA SENEX campaign, which was focused on studying the interactions between biogenic and anthropogenic emissions to form secondary pollutants.
During SENEX, the NOAA WP-3D aircraft conducted 20 research flights between 27 May and 10 July 2013 based out of Smyrna, TN. The SENEX flights included day- and nighttime flights in the Southeast as well as flights over areas with intense shale gas extraction.
Dene R. Bowdalo, Mathew J. Evans, and Eric D. Sofen
Atmos. Chem. Phys., 16, 8295–8308, https://doi.org/10.5194/acp-16-8295-2016, https://doi.org/10.5194/acp-16-8295-2016, 2016
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We introduce a new methodology for the assessment of atmospheric models with observations. We apply a spectral analysis methodology to hourly ozone observations and the equivalent model output. The spectrally transformed observational data show significant peaks on daily and annual timescales. Comparison between the amplitude and phase of these peaks introduces a new comparison methodology between model and measurements. We find the model shows significant biases on an annual timescale.
Alma Hodzic, Prasad S. Kasibhatla, Duseong S. Jo, Christopher D. Cappa, Jose L. Jimenez, Sasha Madronich, and Rokjin J. Park
Atmos. Chem. Phys., 16, 7917–7941, https://doi.org/10.5194/acp-16-7917-2016, https://doi.org/10.5194/acp-16-7917-2016, 2016
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The global budget and spatial distribution of secondary organic aerosol (SOA) are highly uncertain in chemistry-climate models, which reflects our inability to characterize all phases of the OA lifecycle. We have performed global model simulations with the newly proposed formation and removal processes (photolysis and heterogeneous chemistry) and shown that SOA is a far more dynamic system, with 4 times stronger production rates and more efficient removal mechanisms, than assumed in models.
Paul S. Romer, Kaitlin C. Duffey, Paul J. Wooldridge, Hannah M. Allen, Benjamin R. Ayres, Steven S. Brown, William H. Brune, John D. Crounse, Joost de Gouw, Danielle C. Draper, Philip A. Feiner, Juliane L. Fry, Allen H. Goldstein, Abigail Koss, Pawel K. Misztal, Tran B. Nguyen, Kevin Olson, Alex P. Teng, Paul O. Wennberg, Robert J. Wild, Li Zhang, and Ronald C. Cohen
Atmos. Chem. Phys., 16, 7623–7637, https://doi.org/10.5194/acp-16-7623-2016, https://doi.org/10.5194/acp-16-7623-2016, 2016
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The lifetime of nitrogen oxides (NOx) is evaluated by analysis of field measurements from the southeastern United States. At warm temperatures in the daytime boundary layer, NOx interconverts rapidly with both PAN and alkyl and multifunctional nitrates (RONO2), and the relevant lifetime is the combined lifetime of these three classes. We find that the production of RONO2, followed by hydrolysis to produce nitric acid, is the dominant pathway for NOx removal in an isoprene dominated forest.
Amber M. Ortega, Patrick L. Hayes, Zhe Peng, Brett B. Palm, Weiwei Hu, Douglas A. Day, Rui Li, Michael J. Cubison, William H. Brune, Martin Graus, Carsten Warneke, Jessica B. Gilman, William C. Kuster, Joost de Gouw, Cándido Gutiérrez-Montes, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 7411–7433, https://doi.org/10.5194/acp-16-7411-2016, https://doi.org/10.5194/acp-16-7411-2016, 2016
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An oxidation flow reactor (OFR) was deployed to study secondary organic aerosol (SOA) formation and aging of urban emissions at a wide range of OH exposures during the CalNex campaign in Pasadena, CA, in 2010. Results include linking SOA formation to short-lived reactive compounds, similar elemental composition of reactor-aged emissions to atmospheric aging, changes in OA mass due to condensation of oxidized gas-phase species and heterogeneous oxidation of particle-phase species.
Sarah A. Strode, Helen M. Worden, Megan Damon, Anne R. Douglass, Bryan N. Duncan, Louisa K. Emmons, Jean-Francois Lamarque, Michael Manyin, Luke D. Oman, Jose M. Rodriguez, Susan E. Strahan, and Simone Tilmes
Atmos. Chem. Phys., 16, 7285–7294, https://doi.org/10.5194/acp-16-7285-2016, https://doi.org/10.5194/acp-16-7285-2016, 2016
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We use global models to interpret trends in MOPITT observations of CO. Simulations with time-dependent emissions reproduce the observed trends over the eastern USA and Europe, suggesting that the emissions are reasonable for these regions. The simulations produce a positive trend over eastern China, contrary to the observed negative trend. This may indicate that the assumed emission trend over China is too positive. However, large variability in the overhead ozone column also contributes.
Jenny A. Fisher, Daniel J. Jacob, Katherine R. Travis, Patrick S. Kim, Eloise A. Marais, Christopher Chan Miller, Karen Yu, Lei Zhu, Robert M. Yantosca, Melissa P. Sulprizio, Jingqiu Mao, Paul O. Wennberg, John D. Crounse, Alex P. Teng, Tran B. Nguyen, Jason M. St. Clair, Ronald C. Cohen, Paul Romer, Benjamin A. Nault, Paul J. Wooldridge, Jose L. Jimenez, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Paul B. Shepson, Fulizi Xiong, Donald R. Blake, Allen H. Goldstein, Pawel K. Misztal, Thomas F. Hanisco, Glenn M. Wolfe, Thomas B. Ryerson, Armin Wisthaler, and Tomas Mikoviny
Atmos. Chem. Phys., 16, 5969–5991, https://doi.org/10.5194/acp-16-5969-2016, https://doi.org/10.5194/acp-16-5969-2016, 2016
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We use new airborne and ground-based observations from two summer 2013 campaigns in the southeastern US, interpreted with a chemical transport model, to understand the impact of isoprene and monoterpene chemistry on the atmospheric NOx budget via production of organic nitrates (RONO2). We find that a diversity of species contribute to observed RONO2. Our work implies that the NOx sink to RONO2 production is only sensitive to NOx emissions in regions where they are already low.
Alicia Gressent, Bastien Sauvage, Daniel Cariolle, Mathew Evans, Maud Leriche, Céline Mari, and Valérie Thouret
Atmos. Chem. Phys., 16, 5867–5889, https://doi.org/10.5194/acp-16-5867-2016, https://doi.org/10.5194/acp-16-5867-2016, 2016
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In chemical transport models, NOx emitted by lightning (LNOx) is instantaneously diluted into the grid. A plume-in-grid parameterization to account for the sub-grid chemistry of LNOx is presented. This approach was implemented into the GEOS-Chem model and leads to a relative increase of NOx and O3 (18 % and 2 %, respectively, in July) on a large scale downwind of lightning emissions and a relative decrease (25 % and 8 %, respectively, over central Africa in July) over the regions of emissions.
Charles A. Brock, Nicholas L. Wagner, Bruce E. Anderson, Alexis R. Attwood, Andreas Beyersdorf, Pedro Campuzano-Jost, Annmarie G. Carlton, Douglas A. Day, Glenn S. Diskin, Timothy D. Gordon, Jose L. Jimenez, Daniel A. Lack, Jin Liao, Milos Z. Markovic, Ann M. Middlebrook, Nga L. Ng, Anne E. Perring, Matthews S. Richardson, Joshua P. Schwarz, Rebecca A. Washenfelder, Andre Welti, Lu Xu, Luke D. Ziemba, and Daniel M. Murphy
Atmos. Chem. Phys., 16, 4987–5007, https://doi.org/10.5194/acp-16-4987-2016, https://doi.org/10.5194/acp-16-4987-2016, 2016
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Microscopic pollution particles make the atmosphere look hazy and also cool the earth by sending sunlight back to space. When the air is moist, these particles swell with water and scatter even more sunlight. We showed that particles formed from organic material – which dominates particulate pollution in the southeastern U.S. – does not take up water very effectively, toward the low end of most previous studies. We also found a better way to mathematically describe this swelling process.
Charles A. Brock, Nicholas L. Wagner, Bruce E. Anderson, Andreas Beyersdorf, Pedro Campuzano-Jost, Douglas A. Day, Glenn S. Diskin, Timothy D. Gordon, Jose L. Jimenez, Daniel A. Lack, Jin Liao, Milos Z. Markovic, Ann M. Middlebrook, Anne E. Perring, Matthews S. Richardson, Joshua P. Schwarz, Andre Welti, Luke D. Ziemba, and Daniel M. Murphy
Atmos. Chem. Phys., 16, 5009–5019, https://doi.org/10.5194/acp-16-5009-2016, https://doi.org/10.5194/acp-16-5009-2016, 2016
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Two research aircraft made dozens of vertical profiles over rural areas in the southeastern US in summer 2013. These measurements show that, in addition to how much pollution was present and how moist the atmosphere was, the size of the pollutant particles affected how much sunlight was reflected back to space. These measurements will help climate modelers determine which characteristics of pollution are important to predict with accuracy.
S. T. Martin, P. Artaxo, L. A. T. Machado, A. O. Manzi, R. A. F. Souza, C. Schumacher, J. Wang, M. O. Andreae, H. M. J. Barbosa, J. Fan, G. Fisch, A. H. Goldstein, A. Guenther, J. L. Jimenez, U. Pöschl, M. A. Silva Dias, J. N. Smith, and M. Wendisch
Atmos. Chem. Phys., 16, 4785–4797, https://doi.org/10.5194/acp-16-4785-2016, https://doi.org/10.5194/acp-16-4785-2016, 2016
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The Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) Experiment took place in central Amazonia throughout 2014 and 2015. The experiment focused on the complex links among vegetation, atmospheric chemistry, and aerosol production on the one hand and their connections to aerosols, clouds, and precipitation on the other, especially when altered by urban pollution. This article serves as an introduction to the special issue of publications presenting findings of this experiment.
Chris Reed, Mathew J. Evans, Piero Di Carlo, James D. Lee, and Lucy J. Carpenter
Atmos. Chem. Phys., 16, 4707–4724, https://doi.org/10.5194/acp-16-4707-2016, https://doi.org/10.5194/acp-16-4707-2016, 2016
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The self-cleaning capacity of the atmosphere in places like Antarctica can be measured by quantifying very low amounts of combustion products that exist in a well-known ratio. When this ratio deviates from 1 it points to the existence of unknown compounds. Several unknown compounds have been theorized to exist but never measured. We have found the method for measuring the ratio of combustion products suffers a bias in remote places, which when taken into account disproves any unknown compounds.
Nickolay A. Krotkov, Chris A. McLinden, Can Li, Lok N. Lamsal, Edward A. Celarier, Sergey V. Marchenko, William H. Swartz, Eric J. Bucsela, Joanna Joiner, Bryan N. Duncan, K. Folkert Boersma, J. Pepijn Veefkind, Pieternel F. Levelt, Vitali E. Fioletov, Russell R. Dickerson, Hao He, Zifeng Lu, and David G. Streets
Atmos. Chem. Phys., 16, 4605–4629, https://doi.org/10.5194/acp-16-4605-2016, https://doi.org/10.5194/acp-16-4605-2016, 2016
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We examine changes in SO2 and NO2 over the world's most polluted regions during the first decade of Aura OMI observations. Over the eastern US, both NO2 and SO2 levels decreased by 40 % and 80 %, respectively. OMI confirmed large reductions in SO2 over eastern Europe's largest coal power plants. The North China Plain has the world's most severe SO2 pollution, but a decreasing trend been observed since 2011, with a 50 % reduction in 2012–2014. India's SO2 and NO2 levels are growing at a fast pace.
Christopher Chan Miller, Daniel J. Jacob, Gonzalo González Abad, and Kelly Chance
Atmos. Chem. Phys., 16, 4631–4639, https://doi.org/10.5194/acp-16-4631-2016, https://doi.org/10.5194/acp-16-4631-2016, 2016
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Volatile organic compounds (VOCs) are important precursors for photochemical smog.
Glyoxal is an organic compound produced in the atmosphere from reactions of larger VOCs. OMI satellite observations of glyoxal show a large hotspot over the Pearl River delta. The hotspot can be explained by industrial paint and solvent emissions of aromatic VOCs. Our work shows OMI observations are consistent with current VOC emissions estimates, whereas previous work has suggested large underestimates.
Brent J. Williams, Yaping Zhang, Xiaochen Zuo, Raul E. Martinez, Michael J. Walker, Nathan M. Kreisberg, Allen H. Goldstein, Kenneth S. Docherty, and Jose L. Jimenez
Atmos. Meas. Tech., 9, 1569–1586, https://doi.org/10.5194/amt-9-1569-2016, https://doi.org/10.5194/amt-9-1569-2016, 2016
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The thermal desorption aerosol gas chromatograph (TAG) has been used for in situ measurements of organic marker compounds to identify atmospheric particle sources and transformation processes. Here we identify that inorganic aerosol components (e.g., nitrate and sulfate) and highly oxygenated organic components experience thermal decomposition upon sample heating. This thermal decomposition signal in the TAG system is investigated through laboratory and field data.
Karen Yu, Daniel J. Jacob, Jenny A. Fisher, Patrick S. Kim, Eloise A. Marais, Christopher C. Miller, Katherine R. Travis, Lei Zhu, Robert M. Yantosca, Melissa P. Sulprizio, Ron C. Cohen, Jack E. Dibb, Alan Fried, Tomas Mikoviny, Thomas B. Ryerson, Paul O. Wennberg, and Armin Wisthaler
Atmos. Chem. Phys., 16, 4369–4378, https://doi.org/10.5194/acp-16-4369-2016, https://doi.org/10.5194/acp-16-4369-2016, 2016
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Increasing the spatial resolution of a chemical transport model may improve simulations but can be computationally expensive. Using observations from the SEAC4RS aircraft campaign, we find that at higher spatial resolutions, models are better able to simulate the chemical pathways of ozone precursors, but the overall effect on regional mean concentrations is small. This implies that for continental boundary layer applications, coarse resolution models are adequate.
Zhe Peng, Douglas A. Day, Amber M. Ortega, Brett B. Palm, Weiwei Hu, Harald Stark, Rui Li, Kostas Tsigaridis, William H. Brune, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 4283–4305, https://doi.org/10.5194/acp-16-4283-2016, https://doi.org/10.5194/acp-16-4283-2016, 2016
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Oxidation flow reactors (OFRs) are promising tools of studying atmospheric oxidation processes. Elevated concentrations of both OH and non-OH oxidants in OFRs leave room for speculation that non-OH chemistry can play a major role. Through systematic modeling, we find conditions where non-OH VOC fate is significant and show that, in most field studies of SOA using OFRs, non-OH VOC fate in OFRs was insignificant. We also provide guidelines helping OFR users avoid significant non-OH VOC oxidation.
Matthew C. Woody, Kirk R. Baker, Patrick L. Hayes, Jose L. Jimenez, Bonyoung Koo, and Havala O. T. Pye
Atmos. Chem. Phys., 16, 4081–4100, https://doi.org/10.5194/acp-16-4081-2016, https://doi.org/10.5194/acp-16-4081-2016, 2016
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In this work, organic aerosol (OA) predictions from the volatility basis set (VBS) module in the CMAQ photochemical transport model were evaluated against routine monitoring data and measurements collected during the 2010 CalNex field study. We found that the VBS module more accurately reproduced the observed primary/secondary OA split and secondary OA (SOA) mass at the CalNex Pasadena ground site compared to the traditional CMAQ OA module but still underpredicted observed SOA by ~ 5.2 ×.
Frank A. F. Winiberg, Terry J. Dillon, Stephanie C. Orr, Christoph B. M Groß, Iustinian Bejan, Charlotte A. Brumby, Matthew J. Evans, Shona C. Smith, Dwayne E. Heard, and Paul W. Seakins
Atmos. Chem. Phys., 16, 4023–4042, https://doi.org/10.5194/acp-16-4023-2016, https://doi.org/10.5194/acp-16-4023-2016, 2016
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OH radicals are important intermediates in the atmosphere, and the high concentrations observed in tropical regions are yet to be fully explained. Radical-radical reactions such as the title reaction can contribute to OH formation. This is the most fully comprehensive study of the CH3C(O)O2 + HO2 reaction with direct observation of products in all reaction channels. The implications of the new measurements on OH, PAN and NOx concentrations are considered via global models.
Christopher D. Cappa, Shantanu H. Jathar, Michael J. Kleeman, Kenneth S. Docherty, Jose L. Jimenez, John H. Seinfeld, and Anthony S. Wexler
Atmos. Chem. Phys., 16, 3041–3059, https://doi.org/10.5194/acp-16-3041-2016, https://doi.org/10.5194/acp-16-3041-2016, 2016
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Losses of vapors to walls of chambers can negatively bias SOA formation measurements, consequently leading to low predicted SOA concentrations in air quality models. Here, we show that accounting for such vapor losses leads to substantial increases in the predicted amount of SOA formed from VOCs and to notable increases in the O : C atomic ratio in two US regions. Comparison with a variety of observational data suggests generally improved model performance when vapor wall losses are accounted for.
Brett B. Palm, Pedro Campuzano-Jost, Amber M. Ortega, Douglas A. Day, Lisa Kaser, Werner Jud, Thomas Karl, Armin Hansel, James F. Hunter, Eben S. Cross, Jesse H. Kroll, Zhe Peng, William H. Brune, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 2943–2970, https://doi.org/10.5194/acp-16-2943-2016, https://doi.org/10.5194/acp-16-2943-2016, 2016
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Ambient pine forest air was oxidized by OH radicals in a PAM oxidation flow reactor during the BEACHON-RoMBAS campaign to study secondary organic aerosol formation. Approximately 4.4 times more secondary organic aerosol was formed in the reactor than could be explained by the volatile organic gases (VOCs) measured in ambient air. The organic aerosol formation can be explained by including an SOA yield from typically unmeasured semivolatile and intermediate-volatility organic gases (S/IVOCs).
S. E. Pusede, K. C. Duffey, A. A. Shusterman, A. Saleh, J. L. Laughner, P. J. Wooldridge, Q. Zhang, C. L. Parworth, H. Kim, S. L. Capps, L. C. Valin, C. D. Cappa, A. Fried, J. Walega, J. B. Nowak, A. J. Weinheimer, R. M. Hoff, T. A. Berkoff, A. J. Beyersdorf, J. Olson, J. H. Crawford, and R. C. Cohen
Atmos. Chem. Phys., 16, 2575–2596, https://doi.org/10.5194/acp-16-2575-2016, https://doi.org/10.5194/acp-16-2575-2016, 2016
G. M. Wolfe, J. Kaiser, T. F. Hanisco, F. N. Keutsch, J. A. de Gouw, J. B. Gilman, M. Graus, C. D. Hatch, J. Holloway, L. W. Horowitz, B. H. Lee, B. M. Lerner, F. Lopez-Hilifiker, J. Mao, M. R. Marvin, J. Peischl, I. B. Pollack, J. M. Roberts, T. B. Ryerson, J. A. Thornton, P. R. Veres, and C. Warneke
Atmos. Chem. Phys., 16, 2597–2610, https://doi.org/10.5194/acp-16-2597-2016, https://doi.org/10.5194/acp-16-2597-2016, 2016
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This study uses airborne trace gas observations acquired over the southeast US to examine how both natural (isoprene) and anthropogenic (NOx) emissions influence the production of formaldehyde (HCHO). We find a 3-fold increase in HCHO yield between rural and polluted environments. State-of-the-science chemical mechanisms are generally able to reproduce this behavior. These results add confidence to global hydrocarbon emission inventories constrained by spaceborne HCHO observations.
K. F. Boersma, G. C. M. Vinken, and H. J. Eskes
Geosci. Model Dev., 9, 875–898, https://doi.org/10.5194/gmd-9-875-2016, https://doi.org/10.5194/gmd-9-875-2016, 2016
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Satellite measurements of pollutants and greenhouse gases are useful to test and improve atmospheric models. But this requires that modellers account for the spatial and temporal representativeness and the vertical sensitivity of the satellite measurements. This paper provides guidelines on how to carry out a faithful model-satellite comparison for species such as nitrogen dioxide, sulfur dioxide, and formaldehyde that play a key role in air pollution studies.
E. D. Sofen, D. Bowdalo, M. J. Evans, F. Apadula, P. Bonasoni, M. Cupeiro, R. Ellul, I. E. Galbally, R. Girgzdiene, S. Luppo, M. Mimouni, A. C. Nahas, M. Saliba, and K. Tørseth
Earth Syst. Sci. Data, 8, 41–59, https://doi.org/10.5194/essd-8-41-2016, https://doi.org/10.5194/essd-8-41-2016, 2016
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We have brought together all publicly available surface ozone observations from online databases from 1971–2015, with 2200 sites representing regional background conditions appropriate for the evaluation of chemical transport and chemistry-climate models for projects such as the Chemistry-Climate Model Initiative. Gridded data sets of ozone metrics (mean, percentiles, MDA8, SOMO35, etc.) are available from the British Atmospheric Data Centre.
E. A. Marais, D. J. Jacob, J. L. Jimenez, P. Campuzano-Jost, D. A. Day, W. Hu, J. Krechmer, L. Zhu, P. S. Kim, C. C. Miller, J. A. Fisher, K. Travis, K. Yu, T. F. Hanisco, G. M. Wolfe, H. L. Arkinson, H. O. T. Pye, K. D. Froyd, J. Liao, and V. F. McNeill
Atmos. Chem. Phys., 16, 1603–1618, https://doi.org/10.5194/acp-16-1603-2016, https://doi.org/10.5194/acp-16-1603-2016, 2016
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Isoprene secondary organic aerosol (SOA) is a dominant aerosol component in the southeast US, but models routinely underestimate isoprene SOA with traditional schemes based on chamber studies operated under conditions not representative of isoprene-emitting forests. We develop a new irreversible uptake mechanism to reproduce isoprene SOA yields (3.3 %) and composition, and find a factor of 2 co-benefit of SO2 emission controls on reducing sulfate and organic aerosol in the southeast US.
V. Shah, L. Jaeglé, L. E. Gratz, J. L. Ambrose, D. A. Jaffe, N. E. Selin, S. Song, T. L. Campos, F. M. Flocke, M. Reeves, D. Stechman, M. Stell, J. Festa, J. Stutz, A. J. Weinheimer, D. J. Knapp, D. D. Montzka, G. S. Tyndall, E. C. Apel, R. S. Hornbrook, A. J. Hills, D. D. Riemer, N. J. Blake, C. A. Cantrell, and R. L. Mauldin III
Atmos. Chem. Phys., 16, 1511–1530, https://doi.org/10.5194/acp-16-1511-2016, https://doi.org/10.5194/acp-16-1511-2016, 2016
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We present airborne observations of mercury over the southeastern USA during summer. Higher concentrations of oxidized mercury were observed in clean, dry air masses descending in the subtropical anti-cyclones. We used an atmospheric model to simulate the chemistry and transport of mercury. We found reasonable agreement with the observations when the modeled oxidation of elemental mercury was increased, suggesting fast cycling between elemental and oxidized mercury.
E. D. Sofen, D. Bowdalo, and M. J. Evans
Atmos. Chem. Phys., 16, 1445–1457, https://doi.org/10.5194/acp-16-1445-2016, https://doi.org/10.5194/acp-16-1445-2016, 2016
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We explore the global representativeness of a global surface ozone data set from a range of perspectives (area, biomes, chemical regimes, model uncertainty, model trends). We conclude that the current network fails to provide sufficient constraints for important regions/regimes, leading to uncertainty for a range of atmospheric composition challenges. We suggest 20 new locations for making surface ozone observations, which would significantly enhance our observational capability.
T. Sherwen, M. J. Evans, L. J. Carpenter, S. J. Andrews, R. T. Lidster, B. Dix, T. K. Koenig, R. Sinreich, I. Ortega, R. Volkamer, A. Saiz-Lopez, C. Prados-Roman, A. S. Mahajan, and C. Ordóñez
Atmos. Chem. Phys., 16, 1161–1186, https://doi.org/10.5194/acp-16-1161-2016, https://doi.org/10.5194/acp-16-1161-2016, 2016
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Using a global chemical transport model (GEOS-Chem) with additional iodine emissions, chemistry, and deposition we show that iodine is responsible for ~ 9 % of global ozone loss but has negligible impacts on global OH. Uncertainties are large in the chemistry and emissions and future research is needed in both. Measurements of iodine species (especially HOI) would be useful. We believe iodine chemistry should be considered in future chemistry-climate and in air quality modelling.
A. W. H. Chan, N. M. Kreisberg, T. Hohaus, P. Campuzano-Jost, Y. Zhao, D. A. Day, L. Kaser, T. Karl, A. Hansel, A. P. Teng, C. R. Ruehl, D. T. Sueper, J. T. Jayne, D. R. Worsnop, J. L. Jimenez, S. V. Hering, and A. H. Goldstein
Atmos. Chem. Phys., 16, 1187–1205, https://doi.org/10.5194/acp-16-1187-2016, https://doi.org/10.5194/acp-16-1187-2016, 2016
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Using a novel instrument, we have made measurements of organic compounds that can exist as a gas or particle in the rural atmosphere. Through hourly measurements, we have identified the sources and atmospheric processes of these compounds, which are important for modeling the climate and health impact of these emissions.
L. M. Zamora, R. A. Kahn, M. J. Cubison, G. S. Diskin, J. L. Jimenez, Y. Kondo, G. M. McFarquhar, A. Nenes, K. L. Thornhill, A. Wisthaler, A. Zelenyuk, and L. D. Ziemba
Atmos. Chem. Phys., 16, 715–738, https://doi.org/10.5194/acp-16-715-2016, https://doi.org/10.5194/acp-16-715-2016, 2016
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Based on extensive aircraft campaigns, we quantify how biomass burning smoke affects subarctic and Arctic liquid cloud microphysical properties. Enhanced cloud albedo may decrease short-wave radiative flux by between 2 and 4 Wm2 or more in some subarctic conditions. Smoke halved average cloud droplet diameter. In one case study, it also appeared to limit droplet formation. Numerous Arctic background Aitken particles can also interact with combustion particles, perhaps affecting their properties.
R. J. Wild, P. M. Edwards, T. S. Bates, R. C. Cohen, J. A. de Gouw, W. P. Dubé, J. B. Gilman, J. Holloway, J. Kercher, A. R. Koss, L. Lee, B. M. Lerner, R. McLaren, P. K. Quinn, J. M. Roberts, J. Stutz, J. A. Thornton, P. R. Veres, C. Warneke, E. Williams, C. J. Young, B. Yuan, K. J. Zarzana, and S. S. Brown
Atmos. Chem. Phys., 16, 573–583, https://doi.org/10.5194/acp-16-573-2016, https://doi.org/10.5194/acp-16-573-2016, 2016
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High wintertime ozone levels have been observed in the Uintah Basin, Utah, a sparsely populated rural region with intensive oil and gas operations. The reactive nitrogen budget plays an important role in tropospheric ozone formation, and we find that nighttime chemistry has a large effect on its partitioning. Much of the oxidation of reactive nitrogen during a high-ozone year occurred via heterogeneous uptake onto aerosol at night, keeping NOx at concentrations comparable to a low-ozone year.
H.-M. Lee, F. Paulot, D. K. Henze, K. Travis, D. J. Jacob, L. H. Pardo, and B. A. Schichtel
Atmos. Chem. Phys., 16, 525–540, https://doi.org/10.5194/acp-16-525-2016, https://doi.org/10.5194/acp-16-525-2016, 2016
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Sources of nitrogen deposition (Ndep) in Federal Class I areas in the US are investigated, identifying unique features in contributions from different species, sectors and locations. Ndep in many parks is impacted by emissions several hundred km away; the role of oxidized vs reduced sources varies regionally. Emissions reductions in the western US most effectively reduce the extent of areas in critical load exceedance, while reductions in the east most effectively reduce exceedance magnitudes.
E. D. Sofen, M. J. Evans, and A. C. Lewis
Atmos. Chem. Phys., 15, 13627–13632, https://doi.org/10.5194/acp-15-13627-2015, https://doi.org/10.5194/acp-15-13627-2015, 2015
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As an air pollutant, O3 is monitored photometrically to assess compliance with air quality legislation. A recent study found a 1.8% reduction in its absorption cross section, which would lead to an equivalent increase in observed O3 concentrations. We estimate this would increase the number of sites out of compliance with air quality regulations in the EU and US by 20%. We draw attention to how small changes in gas metrology impacts attainment and compliance with legal air quality standards.
B. R. Ayres, H. M. Allen, D. C. Draper, S. S. Brown, R. J. Wild, J. L. Jimenez, D. A. Day, P. Campuzano-Jost, W. Hu, J. de Gouw, A. Koss, R. C. Cohen, K. C. Duffey, P. Romer, K. Baumann, E. Edgerton, S. Takahama, J. A. Thornton, B. H. Lee, F. D. Lopez-Hilfiker, C. Mohr, P. O. Wennberg, T. B. Nguyen, A. Teng, A. H. Goldstein, K. Olson, and J. L. Fry
Atmos. Chem. Phys., 15, 13377–13392, https://doi.org/10.5194/acp-15-13377-2015, https://doi.org/10.5194/acp-15-13377-2015, 2015
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This paper reports atmospheric gas- and aerosol-phase field measurements from the southeastern United States in summer 2013 to demonstrate that the oxidation of biogenic volatile organic compounds by nitrate radical produces a substantial amount of secondary organic aerosol in this region. This process, driven largely by monoterpenes, results in a comparable aerosol nitrate production rate to inorganic nitrate formation by heterogeneous uptake of HNO3 onto dust particles.
Z. Peng, D. A. Day, H. Stark, R. Li, J. Lee-Taylor, B. B. Palm, W. H. Brune, and J. L. Jimenez
Atmos. Meas. Tech., 8, 4863–4890, https://doi.org/10.5194/amt-8-4863-2015, https://doi.org/10.5194/amt-8-4863-2015, 2015
W. W. Hu, P. Campuzano-Jost, B. B. Palm, D. A. Day, A. M. Ortega, P. L. Hayes, J. E. Krechmer, Q. Chen, M. Kuwata, Y. J. Liu, S. S. de Sá, K. McKinney, S. T. Martin, M. Hu, S. H. Budisulistiorini, M. Riva, J. D. Surratt, J. M. St. Clair, G. Isaacman-Van Wertz, L. D. Yee, A. H. Goldstein, S. Carbone, J. Brito, P. Artaxo, J. A. de Gouw, A. Koss, A. Wisthaler, T. Mikoviny, T. Karl, L. Kaser, W. Jud, A. Hansel, K. S. Docherty, M. L. Alexander, N. H. Robinson, H. Coe, J. D. Allan, M. R. Canagaratna, F. Paulot, and J. L. Jimenez
Atmos. Chem. Phys., 15, 11807–11833, https://doi.org/10.5194/acp-15-11807-2015, https://doi.org/10.5194/acp-15-11807-2015, 2015
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This work summarized all the studies reporting isoprene epoxydiols-derived secondary organic aerosol (IEPOX-SOA) measured globally by aerosol mass spectrometer and compare them with modeled gas-phase IEPOX, with results suggestive of the importance of IEPOX-SOA for regional and global OA budgets. A real-time tracer of IEPOX-SOA is thoroughly evaluated for the first time by combing multiple field and chamber studies. A quick and easy empirical method on IEPOX-SOA estimation is also presented.
S. A. Strode, B. N. Duncan, E. A. Yegorova, J. Kouatchou, J. R. Ziemke, and A. R. Douglass
Atmos. Chem. Phys., 15, 11789–11805, https://doi.org/10.5194/acp-15-11789-2015, https://doi.org/10.5194/acp-15-11789-2015, 2015
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A low bias in carbon monoxide (CO) at northern latitudes is a common feature of chemistry climate models. We find that increasing Northern Hemisphere (NH) CO emissions or reducing NH OH concentrations improves the agreement with CO surface observations, but reducing NH OH leads to a better comparison with MOPITT. Removing model biases in ozone and water vapor increases the simulated methane lifetime, but it does not give the 20% reduction in NH OH suggested by our analysis of the CO bias.
K. D. Custard, C. R. Thompson, K. A. Pratt, P B. Shepson, J. Liao, L. G. Huey, J. J. Orlando, A. J. Weinheimer, E. Apel, S. R. Hall, F. Flocke, L. Mauldin, R. S. Hornbrook, D. Pöhler, S. General, J. Zielcke, W. R. Simpson, U. Platt, A. Fried, P. Weibring, B. C. Sive, K. Ullmann, C. Cantrell, D. J. Knapp, and D. D. Montzka
Atmos. Chem. Phys., 15, 10799–10809, https://doi.org/10.5194/acp-15-10799-2015, https://doi.org/10.5194/acp-15-10799-2015, 2015
J. L. Schnell, M. J. Prather, B. Josse, V. Naik, L. W. Horowitz, P. Cameron-Smith, D. Bergmann, G. Zeng, D. A. Plummer, K. Sudo, T. Nagashima, D. T. Shindell, G. Faluvegi, and S. A. Strode
Atmos. Chem. Phys., 15, 10581–10596, https://doi.org/10.5194/acp-15-10581-2015, https://doi.org/10.5194/acp-15-10581-2015, 2015
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We test global chemistry--climate models in their ability to simulate present-day surface ozone. Models are tested against observed hourly ozone from 4217 stations in North America and Europe that are averaged over 1°x1° grid cells. Using novel metrics, we find most models match the shape but not the amplitude of regional summertime diurnal and annual cycles and match the pattern but not the magnitude of summer ozone enhancement. Most also match the observed distribution of extreme episode sizes
P. S. Kim, D. J. Jacob, J. A. Fisher, K. Travis, K. Yu, L. Zhu, R. M. Yantosca, M. P. Sulprizio, J. L. Jimenez, P. Campuzano-Jost, K. D. Froyd, J. Liao, J. W. Hair, M. A. Fenn, C. F. Butler, N. L. Wagner, T. D. Gordon, A. Welti, P. O. Wennberg, J. D. Crounse, J. M. St. Clair, A. P. Teng, D. B. Millet, J. P. Schwarz, M. Z. Markovic, and A. E. Perring
Atmos. Chem. Phys., 15, 10411–10433, https://doi.org/10.5194/acp-15-10411-2015, https://doi.org/10.5194/acp-15-10411-2015, 2015
Z. Lu, D. G. Streets, B. de Foy, L. N. Lamsal, B. N. Duncan, and J. Xing
Atmos. Chem. Phys., 15, 10367–10383, https://doi.org/10.5194/acp-15-10367-2015, https://doi.org/10.5194/acp-15-10367-2015, 2015
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Using an exponentially modified Gaussian method and taking into account the effect of wind on NO2 distributions, we estimate 3-year moving-average emissions of summertime NOx from 35 US urban areas directly from NO2 retrievals of the OMI during 2005−2014. Total OMI-derived NOx emissions over US urban areas decreased by 49%, consistent with reductions of 43, 49, and 44% in the bottom-up NOx emissions, the weak-wind OMI NO2 burdens, and the averaged NO2 concentrations, respectively.
P. Castellanos, K. F. Boersma, O. Torres, and J. F. de Haan
Atmos. Meas. Tech., 8, 3831–3849, https://doi.org/10.5194/amt-8-3831-2015, https://doi.org/10.5194/amt-8-3831-2015, 2015
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Inaccuracies in the retrieval of NO2 tropospheric columns due to the radiative effects of light-absorbing aerosols are not well understood. Here we explicitly account for the effects of aerosols in the Dutch OMI NO2 (DOMINO) tropospheric AMF calculation by including aerosol observations collocated with OMI pixels. The AMF calculations that included aerosol absorption and scattering were on average 10% higher than traditional AMFs. Errors can reach a factor of 2 for individual pixels.
R. E. Dunmore, J. R. Hopkins, R. T. Lidster, J. D. Lee, M. J. Evans, A. R. Rickard, A. C. Lewis, and J. F. Hamilton
Atmos. Chem. Phys., 15, 9983–9996, https://doi.org/10.5194/acp-15-9983-2015, https://doi.org/10.5194/acp-15-9983-2015, 2015
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Technological shifts between fuel sources have had unexpected impacts on atmospheric composition and these significant changes can go undetected if source-specific monitoring infrastructure is not in place. We present chemically comprehensive, continuous measurements of organic compounds in a developed megacity (London), that show diesel-related hydrocarbons can dominate reactive carbon and ozone formation potential, highlighting a serious underestimation of this source in emission inventories.
C. R. Thompson, P. B. Shepson, J. Liao, L. G. Huey, E. C. Apel, C. A. Cantrell, F. Flocke, J. Orlando, A. Fried, S. R. Hall, R. S. Hornbrook, D. J. Knapp, R. L. Mauldin III, D. D. Montzka, B. C. Sive, K. Ullmann, P. Weibring, and A. Weinheimer
Atmos. Chem. Phys., 15, 9651–9679, https://doi.org/10.5194/acp-15-9651-2015, https://doi.org/10.5194/acp-15-9651-2015, 2015
L. Lee, P. J. Wooldridge, J. deGouw, S. S. Brown, T. S. Bates, P. K. Quinn, and R. C. Cohen
Atmos. Chem. Phys., 15, 9313–9325, https://doi.org/10.5194/acp-15-9313-2015, https://doi.org/10.5194/acp-15-9313-2015, 2015
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Secondary organic aerosol affects both the environment and human health. We characterized the aerosol composition in Uintah Basin by measuring the concentration of nitrooxy group moiety which is produced through chemical interaction of volatile organic compounds and NOx emitted largely from local human activity. We found nitrooxy compounds to be a persistent, if not dominant, portion of fine aerosol mass. Similar results may be expected from emissions due to traffic in cities.
A. Hodzic, S. Madronich, P. S. Kasibhatla, G. Tyndall, B. Aumont, J. L. Jimenez, J. Lee-Taylor, and J. Orlando
Atmos. Chem. Phys., 15, 9253–9269, https://doi.org/10.5194/acp-15-9253-2015, https://doi.org/10.5194/acp-15-9253-2015, 2015
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Our study combines process and global chemistry modeling to investigate the potential effect of gas- and particle-phase organic photolysis reactions on the formation and lifetime of secondary organic aerosols (SOAs). Photolysis of the oxidation intermediates that partition between gas and particle phases to form SOA is not included in 3D models. Our results suggest that exposure to UV light can suppress the formation of SOA or even lead to its substantial loss (comparable to wet deposition).
H. M. Walker, D. Stone, T. Ingham, S. Vaughan, M. Cain, R. L. Jones, O. J. Kennedy, M. McLeod, B. Ouyang, J. Pyle, S. Bauguitte, B. Bandy, G. Forster, M. J. Evans, J. F. Hamilton, J. R. Hopkins, J. D. Lee, A. C. Lewis, R. T. Lidster, S. Punjabi, W. T. Morgan, and D. E. Heard
Atmos. Chem. Phys., 15, 8179–8200, https://doi.org/10.5194/acp-15-8179-2015, https://doi.org/10.5194/acp-15-8179-2015, 2015
J. Liu, E. Scheuer, J. Dibb, G. S. Diskin, L. D. Ziemba, K. L. Thornhill, B. E. Anderson, A. Wisthaler, T. Mikoviny, J. J. Devi, M. Bergin, A. E. Perring, M. Z. Markovic, J. P. Schwarz, P. Campuzano-Jost, D. A. Day, J. L. Jimenez, and R. J. Weber
Atmos. Chem. Phys., 15, 7841–7858, https://doi.org/10.5194/acp-15-7841-2015, https://doi.org/10.5194/acp-15-7841-2015, 2015
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Brown carbon (BrC) is found throughout the US continental troposphere during a summer of extensive biomass burning and its prevalence relative to black carbon (BC) increases with altitude. A radiative transfer model based on direct measurements of aerosol scattering and absorption by BC and BrC shows BrC reduces top-of-atmosphere forcing by 20%. A method to estimate BrC radiative forcing efficiencies from surface-based measurements is provided.
J. Kaiser, G. M. Wolfe, K. E. Min, S. S. Brown, C. C. Miller, D. J. Jacob, J. A. deGouw, M. Graus, T. F. Hanisco, J. Holloway, J. Peischl, I. B. Pollack, T. B. Ryerson, C. Warneke, R. A. Washenfelder, and F. N. Keutsch
Atmos. Chem. Phys., 15, 7571–7583, https://doi.org/10.5194/acp-15-7571-2015, https://doi.org/10.5194/acp-15-7571-2015, 2015
A. J. Turner and D. J. Jacob
Atmos. Chem. Phys., 15, 7039–7048, https://doi.org/10.5194/acp-15-7039-2015, https://doi.org/10.5194/acp-15-7039-2015, 2015
A. J. Turner, D. J. Jacob, K. J. Wecht, J. D. Maasakkers, E. Lundgren, A. E. Andrews, S. C. Biraud, H. Boesch, K. W. Bowman, N. M. Deutscher, M. K. Dubey, D. W. T. Griffith, F. Hase, A. Kuze, J. Notholt, H. Ohyama, R. Parker, V. H. Payne, R. Sussmann, C. Sweeney, V. A. Velazco, T. Warneke, P. O. Wennberg, and D. Wunch
Atmos. Chem. Phys., 15, 7049–7069, https://doi.org/10.5194/acp-15-7049-2015, https://doi.org/10.5194/acp-15-7049-2015, 2015
N. L. Wagner, C. A. Brock, W. M. Angevine, A. Beyersdorf, P. Campuzano-Jost, D. Day, J. A. de Gouw, G. S. Diskin, T. D. Gordon, M. G. Graus, J. S. Holloway, G. Huey, J. L. Jimenez, D. A. Lack, J. Liao, X. Liu, M. Z. Markovic, A. M. Middlebrook, T. Mikoviny, J. Peischl, A. E. Perring, M. S. Richardson, T. B. Ryerson, J. P. Schwarz, C. Warneke, A. Welti, A. Wisthaler, L. D. Ziemba, and D. M. Murphy
Atmos. Chem. Phys., 15, 7085–7102, https://doi.org/10.5194/acp-15-7085-2015, https://doi.org/10.5194/acp-15-7085-2015, 2015
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This paper investigates the summertime vertical profile of aerosol over the southeastern US using in situ measurements collected from aircraft. We use a vertical mixing model and measurements of CO to predict the vertical profile of aerosol that we would expect from vertical mixing alone and compare with the observed aerosol profile. We found a modest enhancement of aerosol in the cloudy transition layer during shallow cumulus convection and attribute the enhancement to local aerosol formation.
L. K. Emmons, S. R. Arnold, S. A. Monks, V. Huijnen, S. Tilmes, K. S. Law, J. L. Thomas, J.-C. Raut, I. Bouarar, S. Turquety, Y. Long, B. Duncan, S. Steenrod, S. Strode, J. Flemming, J. Mao, J. Langner, A. M. Thompson, D. Tarasick, E. C. Apel, D. R. Blake, R. C. Cohen, J. Dibb, G. S. Diskin, A. Fried, S. R. Hall, L. G. Huey, A. J. Weinheimer, A. Wisthaler, T. Mikoviny, J. Nowak, J. Peischl, J. M. Roberts, T. Ryerson, C. Warneke, and D. Helmig
Atmos. Chem. Phys., 15, 6721–6744, https://doi.org/10.5194/acp-15-6721-2015, https://doi.org/10.5194/acp-15-6721-2015, 2015
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Eleven 3-D tropospheric chemistry models have been compared and evaluated with observations in the Arctic during the International Polar Year (IPY 2008). Large differences are seen among the models, particularly related to the model chemistry of volatile organic compounds (VOCs) and reactive nitrogen (NOx, PAN, HNO3) partitioning. Consistency among the models in the underestimation of CO, ethane and propane indicates the emission inventory is too low for these compounds.
D. B. Millet, M. Baasandorj, D. K. Farmer, J. A. Thornton, K. Baumann, P. Brophy, S. Chaliyakunnel, J. A. de Gouw, M. Graus, L. Hu, A. Koss, B. H. Lee, F. D. Lopez-Hilfiker, J. A. Neuman, F. Paulot, J. Peischl, I. B. Pollack, T. B. Ryerson, C. Warneke, B. J. Williams, and J. Xu
Atmos. Chem. Phys., 15, 6283–6304, https://doi.org/10.5194/acp-15-6283-2015, https://doi.org/10.5194/acp-15-6283-2015, 2015
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Formic acid (HCOOH) is an abundant atmospheric acid that affects precipitation chemistry and acidity. HCOOH measurements over the USA are 2-3× larger than can be explained by known sources and sinks, revealing a key gap in current understanding. Observations indicate a large biogenic source plus chemical production across a range of precursors. Model simulations cannot capture the HCOOH diurnal amplitude or nocturnal profile, implying a deposition bias and possibly even larger missing source.
M. J. Cubison and J. L. Jimenez
Atmos. Meas. Tech., 8, 2333–2345, https://doi.org/10.5194/amt-8-2333-2015, https://doi.org/10.5194/amt-8-2333-2015, 2015
P. L. Hayes, A. G. Carlton, K. R. Baker, R. Ahmadov, R. A. Washenfelder, S. Alvarez, B. Rappenglück, J. B. Gilman, W. C. Kuster, J. A. de Gouw, P. Zotter, A. S. H. Prévôt, S. Szidat, T. E. Kleindienst, J. H. Offenberg, P. K. Ma, and J. L. Jimenez
Atmos. Chem. Phys., 15, 5773–5801, https://doi.org/10.5194/acp-15-5773-2015, https://doi.org/10.5194/acp-15-5773-2015, 2015
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(1) Four different parameterizations for the formation and chemical evolution of secondary organic aerosol (SOA) are evaluated using a box model representing the Los Angeles region during the CalNex campaign.
(2) The SOA formed only from the oxidation of VOCs is insufficient to explain the observed SOA concentrations.
(3) The amount of SOA mass formed from diesel vehicle emissions is estimated to be 16-27%.
(4) Modeled SOA depends strongly on the P-S/IVOC volatility distribution.
K. R. Baker, A. G. Carlton, T. E. Kleindienst, J. H. Offenberg, M. R. Beaver, D. R. Gentner, A. H. Goldstein, P. L. Hayes, J. L. Jimenez, J. B. Gilman, J. A. de Gouw, M. C. Woody, H. O. T. Pye, J. T. Kelly, M. Lewandowski, M. Jaoui, P. S. Stevens, W. H. Brune, Y.-H. Lin, C. L. Rubitschun, and J. D. Surratt
Atmos. Chem. Phys., 15, 5243–5258, https://doi.org/10.5194/acp-15-5243-2015, https://doi.org/10.5194/acp-15-5243-2015, 2015
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This work details the evaluation of PM2.5 carbon, VOC precursors, and OH estimated by the CMAQ photochemical transport model using routine and special measurements from the 2010 CalNex field study. Here, CMAQ and most recent emissions inventory (2011 NEI) are used to generate model PM2.5 OC estimates that are examined in novel ways including primary vs. secondary formation, fossil vs. contemporary carbon, OH and HO2 evaluation, and the relationship between key VOC precursors and SOC tracers.
A. P. Teng, J. D. Crounse, L. Lee, J. M. St. Clair, R. C. Cohen, and P. O. Wennberg
Atmos. Chem. Phys., 15, 4297–4316, https://doi.org/10.5194/acp-15-4297-2015, https://doi.org/10.5194/acp-15-4297-2015, 2015
J. H. G. M. van Geffen, K. F. Boersma, M. Van Roozendael, F. Hendrick, E. Mahieu, I. De Smedt, M. Sneep, and J. P. Veefkind
Atmos. Meas. Tech., 8, 1685–1699, https://doi.org/10.5194/amt-8-1685-2015, https://doi.org/10.5194/amt-8-1685-2015, 2015
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The paper describes improvements to the algorithm for the retrieval of nitrogen dioxide (NO2) concentration from measurements of the Ozone Monitoring Instrument (OMI), launched on board NASA's EOS-Aura satellite in 2004. With these improvements - updates of the wavelength calibration and the reference spectra - the OMI results are consistent with independent NO2 measurements and the overall quality of the spectral fit is improved considerably.
Q. Chen, D. K. Farmer, L. V. Rizzo, T. Pauliquevis, M. Kuwata, T. G. Karl, A. Guenther, J. D. Allan, H. Coe, M. O. Andreae, U. Pöschl, J. L. Jimenez, P. Artaxo, and S. T. Martin
Atmos. Chem. Phys., 15, 3687–3701, https://doi.org/10.5194/acp-15-3687-2015, https://doi.org/10.5194/acp-15-3687-2015, 2015
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Submicron particle mass concentration in the Amazon during the wet season of 2008 was dominated by organic material. The PMF analysis finds a comparable importance of gas-phase (gas-to-particle condensation) and particle-phase (reactive uptake of isoprene oxidation products, especially of epoxydiols to acidic haze, fog, or cloud droplets) production of secondary organic material during the study period, together accounting for >70% of the organic-particle mass concentration.
L. K. Whalley, D. Stone, I. J. George, S. Mertes, D. van Pinxteren, A. Tilgner, H. Herrmann, M. J. Evans, and D. E. Heard
Atmos. Chem. Phys., 15, 3289–3301, https://doi.org/10.5194/acp-15-3289-2015, https://doi.org/10.5194/acp-15-3289-2015, 2015
A. Ripoll, M. C. Minguillón, J. Pey, J. L. Jimenez, D. A. Day, Y. Sosedova, F. Canonaco, A. S. H. Prévôt, X. Querol, and A. Alastuey
Atmos. Chem. Phys., 15, 2935–2951, https://doi.org/10.5194/acp-15-2935-2015, https://doi.org/10.5194/acp-15-2935-2015, 2015
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Real-time measurements of inorganic (sulfate, nitrate, ammonium, chloride and black carbon (BC)) and organic submicron aerosols from a continental background site (Montsec, MSC, 1570m a.s.l.) in the western Mediterranean Basin (WMB) were conducted for 10 months (July 2011 - April 2012) with an aerosol chemical speciation monitor (ACSM). The ACSM was co-located with other online and offline PM1 measurements. Analyses of the hourly, diurnal, and seasonal variations are presented here.
M. S. Long, R. Yantosca, J. E. Nielsen, C. A. Keller, A. da Silva, M. P. Sulprizio, S. Pawson, and D. J. Jacob
Geosci. Model Dev., 8, 595–602, https://doi.org/10.5194/gmd-8-595-2015, https://doi.org/10.5194/gmd-8-595-2015, 2015
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This paper presents results from the modularization of the GEOS-Chem chemical transport model, and its coupling as the chemical operator within the NASA-GMAO GEOS-5 Earth system model (ESM). The key findings are that chemistry within the modular GEOS-Chem system shows consistent, high strong-scaling properties across the range of distributed processors, transport is the limiting component prohibiting efficient scalability, and GEOS-Chem is able to generate suitable chemical results in an ESM.
B. A. Nault, C. Garland, S. E. Pusede, P. J. Wooldridge, K. Ullmann, S. R. Hall, and R. C. Cohen
Atmos. Meas. Tech., 8, 987–997, https://doi.org/10.5194/amt-8-987-2015, https://doi.org/10.5194/amt-8-987-2015, 2015
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We report the first atmospheric measurement of methyl peroxy nitrate (CH3O2NO2) and describe an experimental strategy to obtain NO2 observations free of methyl peroxy nitrate (CH3O2NO2). The accuracy of the CH3O2NO2 measurements are (+/- 40%) with a LOD of 15 pptv/min. We observe that CH3O2NO2 is ubiquitous in the upper troposphere with median mixing ratios of 100 to 200 pptv, and its composition to the total NOy budget is comparable to HNO3.
B. Yuan, P. R. Veres, C. Warneke, J. M. Roberts, J. B. Gilman, A. Koss, P. M. Edwards, M. Graus, W. C. Kuster, S.-M. Li, R. J. Wild, S. S. Brown, W. P. Dubé, B. M. Lerner, E. J. Williams, J. E. Johnson, P. K. Quinn, T. S. Bates, B. Lefer, P. L. Hayes, J. L. Jimenez, R. J. Weber, R. Zamora, B. Ervens, D. B. Millet, B. Rappenglück, and J. A. de Gouw
Atmos. Chem. Phys., 15, 1975–1993, https://doi.org/10.5194/acp-15-1975-2015, https://doi.org/10.5194/acp-15-1975-2015, 2015
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In this work, secondary formation of formic acid at an urban site and a site in an oil and gas production region is studied. We investigated various gas phase formation pathways of formic acid, including those recently proposed, using a box model. The contributions from aerosol-related processes, fog events and air-snow exchange to formic acid are also quantified.
W. Tang, D. S. Cohan, A. Pour-Biazar, L. N. Lamsal, A. T. White, X. Xiao, W. Zhou, B. H. Henderson, and B. F. Lash
Atmos. Chem. Phys., 15, 1601–1619, https://doi.org/10.5194/acp-15-1601-2015, https://doi.org/10.5194/acp-15-1601-2015, 2015
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A joint application of multiple satellite-derived model inputs to improve Texas O3 SIP modeling is demonstrated in this study. The GOES-retrieved clouds are applied to correct the modeled photolysis rates, and the DKF inversion approach is incorporated into the CAMx-DDM model to adjust NOx emissions using OMI NO2. Using both GOES-derived photolysis rates and OMI-constrained NOx emissions together improves O3 simulations and makes O3 more sensitive to NOx emissions in the O3 non-attainment areas.
C. Liu, X. Liu, M. G. Kowalewski, S. J. Janz, G. González Abad, K. E. Pickering, K. Chance, and L. N. Lamsal
Atmos. Meas. Tech., 8, 751–759, https://doi.org/10.5194/amt-8-751-2015, https://doi.org/10.5194/amt-8-751-2015, 2015
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We characterize the wavelengths and slit functions of Airborne Compact Atmospheric Mapper (ACAM) measurements in ~304--500 nm through the cross-correlation technique. It is necessary to account for atmospheric gas absorption and the ring effect. The derived broadened Gaussian slit functions agree very well with laboratory measurements. Trace gas retrieval comparisons demonstrate that the cross-correlation technique can be reliably used to characterize slit functions.
R. Ahmadov, S. McKeen, M. Trainer, R. Banta, A. Brewer, S. Brown, P. M. Edwards, J. A. de Gouw, G. J. Frost, J. Gilman, D. Helmig, B. Johnson, A. Karion, A. Koss, A. Langford, B. Lerner, J. Olson, S. Oltmans, J. Peischl, G. Pétron, Y. Pichugina, J. M. Roberts, T. Ryerson, R. Schnell, C. Senff, C. Sweeney, C. Thompson, P. R. Veres, C. Warneke, R. Wild, E. J. Williams, B. Yuan, and R. Zamora
Atmos. Chem. Phys., 15, 411–429, https://doi.org/10.5194/acp-15-411-2015, https://doi.org/10.5194/acp-15-411-2015, 2015
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High 2013 wintertime O3 pollution events associated with oil/gas production within the Uinta Basin are studied using a 3D model. It's able quantitatively to reproduce these events using emission estimates of O3 precursors based on ambient measurements (top-down approach), but unable to reproduce them using a recent bottom-up emission inventory for the oil/gas industry. The role of various physical and meteorological processes, chemical species and pathways contributing to high O3 are quantified.
M. R. Canagaratna, J. L. Jimenez, J. H. Kroll, Q. Chen, S. H. Kessler, P. Massoli, L. Hildebrandt Ruiz, E. Fortner, L. R. Williams, K. R. Wilson, J. D. Surratt, N. M. Donahue, J. T. Jayne, and D. R. Worsnop
Atmos. Chem. Phys., 15, 253–272, https://doi.org/10.5194/acp-15-253-2015, https://doi.org/10.5194/acp-15-253-2015, 2015
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Atomic oxygen-to-carbon (O:C), hydrogen-to-carbon (H:C), and organic mass-to-organic carbon (OM:OC) ratios of ambient organic aerosol (OA) species provide key constraints for understanding their sources and impacts. Here an improved method for obtaining accurate O:C, H:C, and OM:OC with a widely used aerosol mass spectrometer is developed. These results imply that OA is more oxidized than previously estimated and indicate the need for new chemical mechanisms that simulate ambient oxidation.
C. Knote, A. Hodzic, and J. L. Jimenez
Atmos. Chem. Phys., 15, 1–18, https://doi.org/10.5194/acp-15-1-2015, https://doi.org/10.5194/acp-15-1-2015, 2015
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Organic material found in ambient aerosol is mostly formed through the oxidation of gaseous precursors. It is semi-volatile under atmospheric conditions, and it continuously partitions between the gas and particle phases. At the same time, it is also highly water soluble. We show that wet and especially dry deposition of semi-volatile organic compounds in the gas phase are major indirect removal pathways for the particle phase, and hence need to be accurately accounted for in modeling studies.
L. Lee, P. J. Wooldridge, J. B. Gilman, C. Warneke, J. de Gouw, and R. C. Cohen
Atmos. Chem. Phys., 14, 12441–12454, https://doi.org/10.5194/acp-14-12441-2014, https://doi.org/10.5194/acp-14-12441-2014, 2014
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Alkyl nitrate formation is known to be an important sink of NOx in a wide range of environments. In a study in the Uintah basin in 2012, we find that formation of these compounds represents a more rapid NOx (NO + NO2) sink than does nitric acid formation. This rapid formation is in large part due to the low mean temperature (~0°C) during the study and is consistent with laboratory observations.
C. Chan Miller, G. Gonzalez Abad, H. Wang, X. Liu, T. Kurosu, D. J. Jacob, and K. Chance
Atmos. Meas. Tech., 7, 3891–3907, https://doi.org/10.5194/amt-7-3891-2014, https://doi.org/10.5194/amt-7-3891-2014, 2014
L. N. Lamsal, N. A. Krotkov, E. A. Celarier, W. H. Swartz, K. E. Pickering, E. J. Bucsela, J. F. Gleason, R. V. Martin, S. Philip, H. Irie, A. Cede, J. Herman, A. Weinheimer, J. J. Szykman, and T. N. Knepp
Atmos. Chem. Phys., 14, 11587–11609, https://doi.org/10.5194/acp-14-11587-2014, https://doi.org/10.5194/acp-14-11587-2014, 2014
C. Warneke, F. Geiger, P. M. Edwards, W. Dube, G. Pétron, J. Kofler, A. Zahn, S. S. Brown, M. Graus, J. B. Gilman, B. M. Lerner, J. Peischl, T. B. Ryerson, J. A. de Gouw, and J. M. Roberts
Atmos. Chem. Phys., 14, 10977–10988, https://doi.org/10.5194/acp-14-10977-2014, https://doi.org/10.5194/acp-14-10977-2014, 2014
K. Tsigaridis, N. Daskalakis, M. Kanakidou, P. J. Adams, P. Artaxo, R. Bahadur, Y. Balkanski, S. E. Bauer, N. Bellouin, A. Benedetti, T. Bergman, T. K. Berntsen, J. P. Beukes, H. Bian, K. S. Carslaw, M. Chin, G. Curci, T. Diehl, R. C. Easter, S. J. Ghan, S. L. Gong, A. Hodzic, C. R. Hoyle, T. Iversen, S. Jathar, J. L. Jimenez, J. W. Kaiser, A. Kirkevåg, D. Koch, H. Kokkola, Y. H Lee, G. Lin, X. Liu, G. Luo, X. Ma, G. W. Mann, N. Mihalopoulos, J.-J. Morcrette, J.-F. Müller, G. Myhre, S. Myriokefalitakis, N. L. Ng, D. O'Donnell, J. E. Penner, L. Pozzoli, K. J. Pringle, L. M. Russell, M. Schulz, J. Sciare, Ø. Seland, D. T. Shindell, S. Sillman, R. B. Skeie, D. Spracklen, T. Stavrakou, S. D. Steenrod, T. Takemura, P. Tiitta, S. Tilmes, H. Tost, T. van Noije, P. G. van Zyl, K. von Salzen, F. Yu, Z. Wang, Z. Wang, R. A. Zaveri, H. Zhang, K. Zhang, Q. Zhang, and X. Zhang
Atmos. Chem. Phys., 14, 10845–10895, https://doi.org/10.5194/acp-14-10845-2014, https://doi.org/10.5194/acp-14-10845-2014, 2014
G. C. M. Vinken, K. F. Boersma, J. D. Maasakkers, M. Adon, and R. V. Martin
Atmos. Chem. Phys., 14, 10363–10381, https://doi.org/10.5194/acp-14-10363-2014, https://doi.org/10.5194/acp-14-10363-2014, 2014
J. D. Fast, J. Allan, R. Bahreini, J. Craven, L. Emmons, R. Ferrare, P. L. Hayes, A. Hodzic, J. Holloway, C. Hostetler, J. L. Jimenez, H. Jonsson, S. Liu, Y. Liu, A. Metcalf, A. Middlebrook, J. Nowak, M. Pekour, A. Perring, L. Russell, A. Sedlacek, J. Seinfeld, A. Setyan, J. Shilling, M. Shrivastava, S. Springston, C. Song, R. Subramanian, J. W. Taylor, V. Vinoj, Q. Yang, R. A. Zaveri, and Q. Zhang
Atmos. Chem. Phys., 14, 10013–10060, https://doi.org/10.5194/acp-14-10013-2014, https://doi.org/10.5194/acp-14-10013-2014, 2014
K. J. Wecht, D. J. Jacob, M. P. Sulprizio, G. W. Santoni, S. C. Wofsy, R. Parker, H. Bösch, and J. Worden
Atmos. Chem. Phys., 14, 8173–8184, https://doi.org/10.5194/acp-14-8173-2014, https://doi.org/10.5194/acp-14-8173-2014, 2014
M. Belmonte Rivas, P. Veefkind, F. Boersma, P. Levelt, H. Eskes, and J. Gille
Atmos. Meas. Tech., 7, 2203–2225, https://doi.org/10.5194/amt-7-2203-2014, https://doi.org/10.5194/amt-7-2203-2014, 2014
S. Saarikoski, S. Carbone, M. J. Cubison, R. Hillamo, P. Keronen, C. Sioutas, D. R. Worsnop, and J. L. Jimenez
Atmos. Meas. Tech., 7, 2121–2135, https://doi.org/10.5194/amt-7-2121-2014, https://doi.org/10.5194/amt-7-2121-2014, 2014
C. A. Keller, M. S. Long, R. M. Yantosca, A. M. Da Silva, S. Pawson, and D. J. Jacob
Geosci. Model Dev., 7, 1409–1417, https://doi.org/10.5194/gmd-7-1409-2014, https://doi.org/10.5194/gmd-7-1409-2014, 2014
J. Ortega, A. Turnipseed, A. B. Guenther, T. G. Karl, D. A. Day, D. Gochis, J. A. Huffman, A. J. Prenni, E. J. T. Levin, S. M. Kreidenweis, P. J. DeMott, Y. Tobo, E. G. Patton, A. Hodzic, Y. Y. Cui, P. C. Harley, R. S. Hornbrook, E. C. Apel, R. K. Monson, A. S. D. Eller, J. P. Greenberg, M. C. Barth, P. Campuzano-Jost, B. B. Palm, J. L. Jimenez, A. C. Aiken, M. K. Dubey, C. Geron, J. Offenberg, M. G. Ryan, P. J. Fornwalt, S. C. Pryor, F. N. Keutsch, J. P. DiGangi, A. W. H. Chan, A. H. Goldstein, G. M. Wolfe, S. Kim, L. Kaser, R. Schnitzhofer, A. Hansel, C. A. Cantrell, R. L. Mauldin, and J. N. Smith
Atmos. Chem. Phys., 14, 6345–6367, https://doi.org/10.5194/acp-14-6345-2014, https://doi.org/10.5194/acp-14-6345-2014, 2014
P. Zoogman, D. J. Jacob, K. Chance, X. Liu, M. Lin, A. Fiore, and K. Travis
Atmos. Chem. Phys., 14, 6261–6271, https://doi.org/10.5194/acp-14-6261-2014, https://doi.org/10.5194/acp-14-6261-2014, 2014
C. Knote, A. Hodzic, J. L. Jimenez, R. Volkamer, J. J. Orlando, S. Baidar, J. Brioude, J. Fast, D. R. Gentner, A. H. Goldstein, P. L. Hayes, W. B. Knighton, H. Oetjen, A. Setyan, H. Stark, R. Thalman, G. Tyndall, R. Washenfelder, E. Waxman, and Q. Zhang
Atmos. Chem. Phys., 14, 6213–6239, https://doi.org/10.5194/acp-14-6213-2014, https://doi.org/10.5194/acp-14-6213-2014, 2014
M. Crippa, F. Canonaco, V. A. Lanz, M. Äijälä, J. D. Allan, S. Carbone, G. Capes, D. Ceburnis, M. Dall'Osto, D. A. Day, P. F. DeCarlo, M. Ehn, A. Eriksson, E. Freney, L. Hildebrandt Ruiz, R. Hillamo, J. L. Jimenez, H. Junninen, A. Kiendler-Scharr, A.-M. Kortelainen, M. Kulmala, A. Laaksonen, A. A. Mensah, C. Mohr, E. Nemitz, C. O'Dowd, J. Ovadnevaite, S. N. Pandis, T. Petäjä, L. Poulain, S. Saarikoski, K. Sellegri, E. Swietlicki, P. Tiitta, D. R. Worsnop, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 14, 6159–6176, https://doi.org/10.5194/acp-14-6159-2014, https://doi.org/10.5194/acp-14-6159-2014, 2014
K.-E. Min, S. E. Pusede, E. C. Browne, B. W. LaFranchi, and R. C. Cohen
Atmos. Chem. Phys., 14, 5495–5512, https://doi.org/10.5194/acp-14-5495-2014, https://doi.org/10.5194/acp-14-5495-2014, 2014
L. Zhang, D. J. Jacob, X. Yue, N. V. Downey, D. A. Wood, and D. Blewitt
Atmos. Chem. Phys., 14, 5295–5309, https://doi.org/10.5194/acp-14-5295-2014, https://doi.org/10.5194/acp-14-5295-2014, 2014
G. W. Santoni, B. C. Daube, E. A. Kort, R. Jiménez, S. Park, J. V. Pittman, E. Gottlieb, B. Xiang, M. S. Zahniser, D. D. Nelson, J. B. McManus, J. Peischl, T. B. Ryerson, J. S. Holloway, A. E. Andrews, C. Sweeney, B. Hall, E. J. Hintsa, F. L. Moore, J. W. Elkins, D. F. Hurst, B. B. Stephens, J. Bent, and S. C. Wofsy
Atmos. Meas. Tech., 7, 1509–1526, https://doi.org/10.5194/amt-7-1509-2014, https://doi.org/10.5194/amt-7-1509-2014, 2014
S. G. Howell, A. D. Clarke, S. Freitag, C. S. McNaughton, V. Kapustin, V. Brekovskikh, J.-L. Jimenez, and M. J. Cubison
Atmos. Chem. Phys., 14, 5073–5087, https://doi.org/10.5194/acp-14-5073-2014, https://doi.org/10.5194/acp-14-5073-2014, 2014
D. R. Gentner, T. B. Ford, A. Guha, K. Boulanger, J. Brioude, W. M. Angevine, J. A. de Gouw, C. Warneke, J. B. Gilman, T. B. Ryerson, J. Peischl, S. Meinardi, D. R. Blake, E. Atlas, W. A. Lonneman, T. E. Kleindienst, M. R. Beaver, J. M. St. Clair, P. O. Wennberg, T. C. VandenBoer, M. Z. Markovic, J. G. Murphy, R. A. Harley, and A. H. Goldstein
Atmos. Chem. Phys., 14, 4955–4978, https://doi.org/10.5194/acp-14-4955-2014, https://doi.org/10.5194/acp-14-4955-2014, 2014
P. Castellanos, K. F. Boersma, and G. R. van der Werf
Atmos. Chem. Phys., 14, 3929–3943, https://doi.org/10.5194/acp-14-3929-2014, https://doi.org/10.5194/acp-14-3929-2014, 2014
M. Chin, T. Diehl, Q. Tan, J. M. Prospero, R. A. Kahn, L. A. Remer, H. Yu, A. M. Sayer, H. Bian, I. V. Geogdzhayev, B. N. Holben, S. G. Howell, B. J. Huebert, N. C. Hsu, D. Kim, T. L. Kucsera, R. C. Levy, M. I. Mishchenko, X. Pan, P. K. Quinn, G. L. Schuster, D. G. Streets, S. A. Strode, O. Torres, and X.-P. Zhao
Atmos. Chem. Phys., 14, 3657–3690, https://doi.org/10.5194/acp-14-3657-2014, https://doi.org/10.5194/acp-14-3657-2014, 2014
C. A. McLinden, V. Fioletov, K. F. Boersma, S. K. Kharol, N. Krotkov, L. Lamsal, P. A. Makar, R. V. Martin, J. P. Veefkind, and K. Yang
Atmos. Chem. Phys., 14, 3637–3656, https://doi.org/10.5194/acp-14-3637-2014, https://doi.org/10.5194/acp-14-3637-2014, 2014
C. J. Young, R. A. Washenfelder, P. M. Edwards, D. D. Parrish, J. B. Gilman, W. C. Kuster, L. H. Mielke, H. D. Osthoff, C. Tsai, O. Pikelnaya, J. Stutz, P. R. Veres, J. M. Roberts, S. Griffith, S. Dusanter, P. S. Stevens, J. Flynn, N. Grossberg, B. Lefer, J. S. Holloway, J. Peischl, T. B. Ryerson, E. L. Atlas, D. R. Blake, and S. S. Brown
Atmos. Chem. Phys., 14, 3427–3440, https://doi.org/10.5194/acp-14-3427-2014, https://doi.org/10.5194/acp-14-3427-2014, 2014
S. E. Pusede, D. R. Gentner, P. J. Wooldridge, E. C. Browne, A. W. Rollins, K.-E. Min, A. R. Russell, J. Thomas, L. Zhang, W. H. Brune, S. B. Henry, J. P. DiGangi, F. N. Keutsch, S. A. Harrold, J. A. Thornton, M. R. Beaver, J. M. St. Clair, P. O. Wennberg, J. Sanders, X. Ren, T. C. VandenBoer, M. Z. Markovic, A. Guha, R. Weber, A. H. Goldstein, and R. C. Cohen
Atmos. Chem. Phys., 14, 3373–3395, https://doi.org/10.5194/acp-14-3373-2014, https://doi.org/10.5194/acp-14-3373-2014, 2014
E. J. T. Levin, A. J. Prenni, B. B. Palm, D. A. Day, P. Campuzano-Jost, P. M. Winkler, S. M. Kreidenweis, P. J. DeMott, J. L. Jimenez, and J. N. Smith
Atmos. Chem. Phys., 14, 2657–2667, https://doi.org/10.5194/acp-14-2657-2014, https://doi.org/10.5194/acp-14-2657-2014, 2014
E. V. Fischer, D. J. Jacob, R. M. Yantosca, M. P. Sulprizio, D. B. Millet, J. Mao, F. Paulot, H. B. Singh, A. Roiger, L. Ries, R.W. Talbot, K. Dzepina, and S. Pandey Deolal
Atmos. Chem. Phys., 14, 2679–2698, https://doi.org/10.5194/acp-14-2679-2014, https://doi.org/10.5194/acp-14-2679-2014, 2014
A. K. Mebust and R. C. Cohen
Atmos. Chem. Phys., 14, 2509–2524, https://doi.org/10.5194/acp-14-2509-2014, https://doi.org/10.5194/acp-14-2509-2014, 2014
J. J. Ensberg, P. L. Hayes, J. L. Jimenez, J. B. Gilman, W. C. Kuster, J. A. de Gouw, J. S. Holloway, T. D. Gordon, S. Jathar, A. L. Robinson, and J. H. Seinfeld
Atmos. Chem. Phys., 14, 2383–2397, https://doi.org/10.5194/acp-14-2383-2014, https://doi.org/10.5194/acp-14-2383-2014, 2014
R. L. N. Yatavelli, H. Stark, S. L. Thompson, J. R. Kimmel, M. J. Cubison, D. A. Day, P. Campuzano-Jost, B. B. Palm, A. Hodzic, J. A. Thornton, J. T. Jayne, D. R. Worsnop, and J. L. Jimenez
Atmos. Chem. Phys., 14, 1527–1546, https://doi.org/10.5194/acp-14-1527-2014, https://doi.org/10.5194/acp-14-1527-2014, 2014
D. Stone, M. J. Evans, H. Walker, T. Ingham, S. Vaughan, B. Ouyang, O. J. Kennedy, M. W. McLeod, R. L. Jones, J. Hopkins, S. Punjabi, R. Lidster, J. F. Hamilton, J. D. Lee, A. C. Lewis, L. J. Carpenter, G. Forster, D. E. Oram, C. E. Reeves, S. Bauguitte, W. Morgan, H. Coe, E. Aruffo, C. Dari-Salisburgo, F. Giammaria, P. Di Carlo, and D. E. Heard
Atmos. Chem. Phys., 14, 1299–1321, https://doi.org/10.5194/acp-14-1299-2014, https://doi.org/10.5194/acp-14-1299-2014, 2014
G. C. M. Vinken, K. F. Boersma, A. van Donkelaar, and L. Zhang
Atmos. Chem. Phys., 14, 1353–1369, https://doi.org/10.5194/acp-14-1353-2014, https://doi.org/10.5194/acp-14-1353-2014, 2014
E. C. Browne, P. J. Wooldridge, K.-E. Min, and R. C. Cohen
Atmos. Chem. Phys., 14, 1225–1238, https://doi.org/10.5194/acp-14-1225-2014, https://doi.org/10.5194/acp-14-1225-2014, 2014
L. C. Valin, A. R. Russell, and R. C. Cohen
Atmos. Chem. Phys., 14, 1–9, https://doi.org/10.5194/acp-14-1-2014, https://doi.org/10.5194/acp-14-1-2014, 2014
A. M. Ortega, D. A. Day, M. J. Cubison, W. H. Brune, D. Bon, J. A. de Gouw, and J. L. Jimenez
Atmos. Chem. Phys., 13, 11551–11571, https://doi.org/10.5194/acp-13-11551-2013, https://doi.org/10.5194/acp-13-11551-2013, 2013
S. S. Brown, W. P. Dubé, R. Bahreini, A. M. Middlebrook, C. A. Brock, C. Warneke, J. A. de Gouw, R. A. Washenfelder, E. Atlas, J. Peischl, T. B. Ryerson, J. S. Holloway, J. P. Schwarz, R. Spackman, M. Trainer, D. D. Parrish, F. C. Fehshenfeld, and A. R. Ravishankara
Atmos. Chem. Phys., 13, 11317–11337, https://doi.org/10.5194/acp-13-11317-2013, https://doi.org/10.5194/acp-13-11317-2013, 2013
W. Tang, D. S. Cohan, L. N. Lamsal, X. Xiao, and W. Zhou
Atmos. Chem. Phys., 13, 11005–11018, https://doi.org/10.5194/acp-13-11005-2013, https://doi.org/10.5194/acp-13-11005-2013, 2013
E. J. Bucsela, N. A. Krotkov, E. A. Celarier, L. N. Lamsal, W. H. Swartz, P. K. Bhartia, K. F. Boersma, J. P. Veefkind, J. F. Gleason, and K. E. Pickering
Atmos. Meas. Tech., 6, 2607–2626, https://doi.org/10.5194/amt-6-2607-2013, https://doi.org/10.5194/amt-6-2607-2013, 2013
P. M. Edwards, M. J. Evans, K. L. Furneaux, J. Hopkins, T. Ingham, C. Jones, J. D. Lee, A. C. Lewis, S. J. Moller, D. Stone, L. K. Whalley, and D. E. Heard
Atmos. Chem. Phys., 13, 9497–9514, https://doi.org/10.5194/acp-13-9497-2013, https://doi.org/10.5194/acp-13-9497-2013, 2013
P. S. Kim, D. J. Jacob, X. Liu, J. X. Warner, K. Yang, K. Chance, V. Thouret, and P. Nedelec
Atmos. Chem. Phys., 13, 9321–9335, https://doi.org/10.5194/acp-13-9321-2013, https://doi.org/10.5194/acp-13-9321-2013, 2013
T. Stavrakou, J.-F. Müller, K. F. Boersma, R. J. van der A, J. Kurokawa, T. Ohara, and Q. Zhang
Atmos. Chem. Phys., 13, 9057–9082, https://doi.org/10.5194/acp-13-9057-2013, https://doi.org/10.5194/acp-13-9057-2013, 2013
P. M. Edwards, C. J. Young, K. Aikin, J. deGouw, W. P. Dubé, F. Geiger, J. Gilman, D. Helmig, J. S. Holloway, J. Kercher, B. Lerner, R. Martin, R. McLaren, D. D. Parrish, J. Peischl, J. M. Roberts, T. B. Ryerson, J. Thornton, C. Warneke, E. J. Williams, and S. S. Brown
Atmos. Chem. Phys., 13, 8955–8971, https://doi.org/10.5194/acp-13-8955-2013, https://doi.org/10.5194/acp-13-8955-2013, 2013
J. L. Fry, D. C. Draper, K. J. Zarzana, P. Campuzano-Jost, D. A. Day, J. L. Jimenez, S. S. Brown, R. C. Cohen, L. Kaser, A. Hansel, L. Cappellin, T. Karl, A. Hodzic Roux, A. Turnipseed, C. Cantrell, B. L. Lefer, and N. Grossberg
Atmos. Chem. Phys., 13, 8585–8605, https://doi.org/10.5194/acp-13-8585-2013, https://doi.org/10.5194/acp-13-8585-2013, 2013
Y. Xie, F. Paulot, W. P. L. Carter, C. G. Nolte, D. J. Luecken, W. T. Hutzell, P. O. Wennberg, R. C. Cohen, and R. W. Pinder
Atmos. Chem. Phys., 13, 8439–8455, https://doi.org/10.5194/acp-13-8439-2013, https://doi.org/10.5194/acp-13-8439-2013, 2013
J.-F. Lamarque, F. Dentener, J. McConnell, C.-U. Ro, M. Shaw, R. Vet, D. Bergmann, P. Cameron-Smith, S. Dalsoren, R. Doherty, G. Faluvegi, S. J. Ghan, B. Josse, Y. H. Lee, I. A. MacKenzie, D. Plummer, D. T. Shindell, R. B. Skeie, D. S. Stevenson, S. Strode, G. Zeng, M. Curran, D. Dahl-Jensen, S. Das, D. Fritzsche, and M. Nolan
Atmos. Chem. Phys., 13, 7997–8018, https://doi.org/10.5194/acp-13-7997-2013, https://doi.org/10.5194/acp-13-7997-2013, 2013
J. A. Huffman, A. J. Prenni, P. J. DeMott, C. Pöhlker, R. H. Mason, N. H. Robinson, J. Fröhlich-Nowoisky, Y. Tobo, V. R. Després, E. Garcia, D. J. Gochis, E. Harris, I. Müller-Germann, C. Ruzene, B. Schmer, B. Sinha, D. A. Day, M. O. Andreae, J. L. Jimenez, M. Gallagher, S. M. Kreidenweis, A. K. Bertram, and U. Pöschl
Atmos. Chem. Phys., 13, 6151–6164, https://doi.org/10.5194/acp-13-6151-2013, https://doi.org/10.5194/acp-13-6151-2013, 2013
V. Naik, A. Voulgarakis, A. M. Fiore, L. W. Horowitz, J.-F. Lamarque, M. Lin, M. J. Prather, P. J. Young, D. Bergmann, P. J. Cameron-Smith, I. Cionni, W. J. Collins, S. B. Dalsøren, R. Doherty, V. Eyring, G. Faluvegi, G. A. Folberth, B. Josse, Y. H. Lee, I. A. MacKenzie, T. Nagashima, T. P. C. van Noije, D. A. Plummer, M. Righi, S. T. Rumbold, R. Skeie, D. T. Shindell, D. S. Stevenson, S. Strode, K. Sudo, S. Szopa, and G. Zeng
Atmos. Chem. Phys., 13, 5277–5298, https://doi.org/10.5194/acp-13-5277-2013, https://doi.org/10.5194/acp-13-5277-2013, 2013
W. W. Verstraeten, K. F. Boersma, J. Zörner, M. A. F. Allaart, K. W. Bowman, and J. R. Worden
Atmos. Meas. Tech., 6, 1413–1423, https://doi.org/10.5194/amt-6-1413-2013, https://doi.org/10.5194/amt-6-1413-2013, 2013
T. H. Bertram, A. E. Perring, P. J. Wooldridge, J. Dibb, M. A. Avery, and R. C. Cohen
Atmos. Chem. Phys., 13, 4617–4630, https://doi.org/10.5194/acp-13-4617-2013, https://doi.org/10.5194/acp-13-4617-2013, 2013
E. C. Browne, K.-E. Min, P. J. Wooldridge, E. Apel, D. R. Blake, W. H. Brune, C. A. Cantrell, M. J. Cubison, G. S. Diskin, J. L. Jimenez, A. J. Weinheimer, P. O. Wennberg, A. Wisthaler, and R. C. Cohen
Atmos. Chem. Phys., 13, 4543–4562, https://doi.org/10.5194/acp-13-4543-2013, https://doi.org/10.5194/acp-13-4543-2013, 2013
K. W. Bowman, D. T. Shindell, H. M. Worden, J.F. Lamarque, P. J. Young, D. S. Stevenson, Z. Qu, M. de la Torre, D. Bergmann, P. J. Cameron-Smith, W. J. Collins, R. Doherty, S. B. Dalsøren, G. Faluvegi, G. Folberth, L. W. Horowitz, B. M. Josse, Y. H. Lee, I. A. MacKenzie, G. Myhre, T. Nagashima, V. Naik, D. A. Plummer, S. T. Rumbold, R. B. Skeie, S. A. Strode, K. Sudo, S. Szopa, A. Voulgarakis, G. Zeng, S. S. Kulawik, A. M. Aghedo, and J. R. Worden
Atmos. Chem. Phys., 13, 4057–4072, https://doi.org/10.5194/acp-13-4057-2013, https://doi.org/10.5194/acp-13-4057-2013, 2013
J. Brioude, W. M. Angevine, R. Ahmadov, S.-W. Kim, S. Evan, S. A. McKeen, E.-Y. Hsie, G. J. Frost, J. A. Neuman, I. B. Pollack, J. Peischl, T. B. Ryerson, J. Holloway, S. S. Brown, J. B. Nowak, J. M. Roberts, S. C. Wofsy, G. W. Santoni, T. Oda, and M. Trainer
Atmos. Chem. Phys., 13, 3661–3677, https://doi.org/10.5194/acp-13-3661-2013, https://doi.org/10.5194/acp-13-3661-2013, 2013
D. S. Stevenson, P. J. Young, V. Naik, J.-F. Lamarque, D. T. Shindell, A. Voulgarakis, R. B. Skeie, S. B. Dalsoren, G. Myhre, T. K. Berntsen, G. A. Folberth, S. T. Rumbold, W. J. Collins, I. A. MacKenzie, R. M. Doherty, G. Zeng, T. P. C. van Noije, A. Strunk, D. Bergmann, P. Cameron-Smith, D. A. Plummer, S. A. Strode, L. Horowitz, Y. H. Lee, S. Szopa, K. Sudo, T. Nagashima, B. Josse, I. Cionni, M. Righi, V. Eyring, A. Conley, K. W. Bowman, O. Wild, and A. Archibald
Atmos. Chem. Phys., 13, 3063–3085, https://doi.org/10.5194/acp-13-3063-2013, https://doi.org/10.5194/acp-13-3063-2013, 2013
J. R. Pierce, M. J. Evans, C. E. Scott, S. D. D'Andrea, D. K. Farmer, E. Swietlicki, and D. V. Spracklen
Atmos. Chem. Phys., 13, 3163–3176, https://doi.org/10.5194/acp-13-3163-2013, https://doi.org/10.5194/acp-13-3163-2013, 2013
T. L. Lathem, A. J. Beyersdorf, K. L. Thornhill, E. L. Winstead, M. J. Cubison, A. Hecobian, J. L. Jimenez, R. J. Weber, B. E. Anderson, and A. Nenes
Atmos. Chem. Phys., 13, 2735–2756, https://doi.org/10.5194/acp-13-2735-2013, https://doi.org/10.5194/acp-13-2735-2013, 2013
A. Voulgarakis, V. Naik, J.-F. Lamarque, D. T. Shindell, P. J. Young, M. J. Prather, O. Wild, R. D. Field, D. Bergmann, P. Cameron-Smith, I. Cionni, W. J. Collins, S. B. Dalsøren, R. M. Doherty, V. Eyring, G. Faluvegi, G. A. Folberth, L. W. Horowitz, B. Josse, I. A. MacKenzie, T. Nagashima, D. A. Plummer, M. Righi, S. T. Rumbold, D. S. Stevenson, S. A. Strode, K. Sudo, S. Szopa, and G. Zeng
Atmos. Chem. Phys., 13, 2563–2587, https://doi.org/10.5194/acp-13-2563-2013, https://doi.org/10.5194/acp-13-2563-2013, 2013
P. J. Young, A. T. Archibald, K. W. Bowman, J.-F. Lamarque, V. Naik, D. S. Stevenson, S. Tilmes, A. Voulgarakis, O. Wild, D. Bergmann, P. Cameron-Smith, I. Cionni, W. J. Collins, S. B. Dalsøren, R. M. Doherty, V. Eyring, G. Faluvegi, L. W. Horowitz, B. Josse, Y. H. Lee, I. A. MacKenzie, T. Nagashima, D. A. Plummer, M. Righi, S. T. Rumbold, R. B. Skeie, D. T. Shindell, S. A. Strode, K. Sudo, S. Szopa, and G. Zeng
Atmos. Chem. Phys., 13, 2063–2090, https://doi.org/10.5194/acp-13-2063-2013, https://doi.org/10.5194/acp-13-2063-2013, 2013
J.-F. Lamarque, D. T. Shindell, B. Josse, P. J. Young, I. Cionni, V. Eyring, D. Bergmann, P. Cameron-Smith, W. J. Collins, R. Doherty, S. Dalsoren, G. Faluvegi, G. Folberth, S. J. Ghan, L. W. Horowitz, Y. H. Lee, I. A. MacKenzie, T. Nagashima, V. Naik, D. Plummer, M. Righi, S. T. Rumbold, M. Schulz, R. B. Skeie, D. S. Stevenson, S. Strode, K. Sudo, S. Szopa, A. Voulgarakis, and G. Zeng
Geosci. Model Dev., 6, 179–206, https://doi.org/10.5194/gmd-6-179-2013, https://doi.org/10.5194/gmd-6-179-2013, 2013
A. C. Lewis, M. J. Evans, J. R. Hopkins, S. Punjabi, K. A. Read, R. M. Purvis, S. J. Andrews, S. J. Moller, L. J. Carpenter, J. D. Lee, A. R. Rickard, P. I. Palmer, and M. Parrington
Atmos. Chem. Phys., 13, 851–867, https://doi.org/10.5194/acp-13-851-2013, https://doi.org/10.5194/acp-13-851-2013, 2013
J. Mao, S. Fan, D. J. Jacob, and K. R. Travis
Atmos. Chem. Phys., 13, 509–519, https://doi.org/10.5194/acp-13-509-2013, https://doi.org/10.5194/acp-13-509-2013, 2013
A. R. Russell, L. C. Valin, and R. C. Cohen
Atmos. Chem. Phys., 12, 12197–12209, https://doi.org/10.5194/acp-12-12197-2012, https://doi.org/10.5194/acp-12-12197-2012, 2012
E. C. Browne and R. C. Cohen
Atmos. Chem. Phys., 12, 11917–11932, https://doi.org/10.5194/acp-12-11917-2012, https://doi.org/10.5194/acp-12-11917-2012, 2012
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Seasonal, regional, and vertical characteristics of high-carbon-monoxide plumes along with their associated ozone anomalies, as seen by IAGOS between 2002 and 2019
The potential of drone observations to improve air quality predictions by 4D-Var
Process analysis of elevated concentrations of organic acids at Whiteface Mountain, New York
Ozone source attribution in polluted European areas during summer 2017 as simulated with MECO(n)
Opinion: Challenges and needs of tropospheric chemical mechanism development
The atmospheric oxidizing capacity in China – Part 2: Sensitivity to emissions of primary pollutants
Role of chemical production and depositional losses on formaldehyde in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM)
Review of source analyses of ambient volatile organic compounds considering reactive losses: methods of reducing loss effects, impacts of losses, and sources
Interpreting summertime hourly variation of NO2 columns with implications for geostationary satellite applications
An investigation into atmospheric nitrous acid (HONO) processes in South Korea
Performance evaluation of UKESM1 for surface ozone across the pan-tropics
Constraining light dependency in modeled emissions through comparison to observed biogenic volatile organic compound (BVOC) concentrations in a southeastern US forest
A global re-analysis of regionally resolved emissions and atmospheric mole fractions of SF6 for the period 2005–2021
Tropospheric ozone precursors: global and regional distributions, trends, and variability
The contribution of transport emissions to ozone mixing ratios and methane lifetime in 2015 and 2050 in the Shared Socioeconomic Pathways (SSPs)
Ether and ester formation from peroxy radical recombination: a qualitative reaction channel analysis
ACEIC: a comprehensive anthropogenic chlorine emission inventory for China
Impact of methane and other precursor emission reductions on surface ozone in Europe: scenario analysis using the European Monitoring and Evaluation Programme (EMEP) Meteorological Synthesizing Centre – West (MSC-W) model
Verifying national inventory-based combustion emissions of CO2 across the UK and mainland Europe using satellite observations of atmospheric CO and CO2
An improved estimate of inorganic iodine emissions from the ocean using a coupled surface microlayer box model
Impact of improved representation of volatile organic compound emissions and production of NOx reservoirs on modeled urban ozone production
The effect of different climate and air quality policies in China on in situ ozone production in Beijing
Assessing the relative impacts of satellite ozone and its precursor observations to improve global tropospheric ozone analysis using multiple chemical reanalysis systems
Evaluating present-day and future impacts of agricultural ammonia emissions on atmospheric chemistry and climate
Enhancing long-term trend simulation of the global tropospheric hydroxyl (TOH) and its drivers from 2005 to 2019: a synergistic integration of model simulations and satellite observations
Intercomparison of GEOS-Chem and CAM-chem tropospheric oxidant chemistry within the Community Earth System Model version 2 (CESM2)
Development of a detailed gaseous oxidation scheme of naphthalene for secondary organic aerosol (SOA) formation and speciation
Air pollution satellite-based CO2 emission inversion: system evaluation, sensitivity analysis, and future perspective
Anthropogenic emission controls reduce summertime ozone-temperature sensitivity in the United States
Large contributions of soil emissions to the atmospheric nitrogen budget and their impacts on air quality and temperature rise in North China
Why did ozone concentrations remain high during Shanghai's static management? A statistical and radical-chemistry perspective
Impact of introducing electric vehicles on ground-level O3 and PM2.5 in the Greater Tokyo Area: Yearly trends and the importance of changes in the Urban Heat Island effect
Revising VOC emissions speciation improves the simulation of global background ethane and propane
Changes in South American surface ozone trends: exploring the influences of precursors and extreme events
Evaluating NOx stack plume emissions using a high-resolution atmospheric chemistry model and satellite-derived NO2 columns
NOx emissions in France in 2019–2021 as estimated by the high-spatial-resolution assimilation of TROPOMI NO2 observations
Urban ozone formation and sensitivities to volatile chemical products, cooking emissions, and NOx across the Los Angeles Basin
Aggravated surface O3 pollution primarily driven by meteorological variations in China during the 2020 COVID-19 pandemic lockdown period
Identifying decadal trends in deweathered concentrations of criteria air pollutants in Canadian urban atmospheres with machine learning approaches
Evaluation of modelled versus observed non-methane volatile organic compounds at European Monitoring and Evaluation Programme sites in Europe
Constraining non-methane VOC emissions with TROPOMI HCHO observations: impact on summertime ozone simulation in August 2022 in China
Insights on ozone pollution control in urban areas by decoupling meteorological factors based on machine learning
Revealing the significant acceleration of hydrofluorocarbon (HFC) emissions in eastern Asia through long-term atmospheric observations
Interpreting Geostationary Environment Monitoring Spectrometer (GEMS) geostationary satellite observations of the diurnal variation in nitrogen dioxide (NO2) over East Asia
An intercomparison of satellite, airborne, and ground-level observations with WRF–CAMx simulations of NO2 columns over Houston, Texas, during the September 2021 TRACER-AQ campaign
Investigating processes influencing simulation of local Arctic wintertime anthropogenic pollution in Fairbanks, Alaska during ALPACA-2022
Interannual variability of summertime formaldehyde (HCHO) vertical column density and its main drivers at northern high latitudes
The impact of multi-decadal changes in VOC speciation on urban ozone chemistry: a case study in Birmingham, United Kingdom
Technical note: Challenges in detecting free tropospheric ozone trends in a sparsely sampled environment
Combined assimilation of NOAA surface and MIPAS satellite observations to constrain the global budget of carbonyl sulfide
Thibaut Lebourgeois, Bastien Sauvage, Pawel Wolff, Béatrice Josse, Virginie Marécal, Yasmine Bennouna, Romain Blot, Damien Boulanger, Hannah Clark, Jean-Marc Cousin, Philippe Nedelec, and Valérie Thouret
Atmos. Chem. Phys., 24, 13975–14004, https://doi.org/10.5194/acp-24-13975-2024, https://doi.org/10.5194/acp-24-13975-2024, 2024
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Our study examines intense-carbon-monoxide (CO) pollution events measured by commercial aircraft from the In-service Aircraft for a Global Observing System (IAGOS) research infrastructure. We combine these measurements with the SOFT-IO model to trace the origin of the observed CO. A comprehensive analysis of the geographical origin, source type, seasonal variation, and ozone levels of these pollution events is provided.
Hassnae Erraji, Philipp Franke, Astrid Lampert, Tobias Schuldt, Ralf Tillmann, Andreas Wahner, and Anne Caroline Lange
Atmos. Chem. Phys., 24, 13913–13934, https://doi.org/10.5194/acp-24-13913-2024, https://doi.org/10.5194/acp-24-13913-2024, 2024
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Four-dimensional variational data assimilation allows for the simultaneous optimisation of initial values and emission rates by using trace-gas profiles from drone observations in a regional air quality model. Assimilated profiles positively impact the representation of air pollutants in the model by improving their vertical distribution and ground-level concentrations. This case study highlights the potential of drone data to enhance air quality analyses including local emission evaluation.
Christopher Lawrence, Mary Barth, John Orlando, Paul Casson, Richard Brandt, Daniel Kelting, Elizabeth Yerger, and Sara Lance
Atmos. Chem. Phys., 24, 13693–13713, https://doi.org/10.5194/acp-24-13693-2024, https://doi.org/10.5194/acp-24-13693-2024, 2024
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This work uses chemical transport and box modeling to study the gas- and aqueous-phase production of organic acid concentrations measured in cloud water at the summit of Whiteface Mountain on 1 July 2018. Isoprene was the major source of formic, acetic, and oxalic acid. Gas-phase chemistry greatly underestimated formic and acetic acid, indicating missing sources, while cloud chemistry was a key source of oxalic acid. More studies of organic acids are required to better constrain their sources.
Markus Kilian, Volker Grewe, Patrick Jöckel, Astrid Kerkweg, Mariano Mertens, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 24, 13503–13523, https://doi.org/10.5194/acp-24-13503-2024, https://doi.org/10.5194/acp-24-13503-2024, 2024
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Anthropogenic emissions are a major source of precursors of tropospheric ozone. As ozone formation is highly non-linear, we apply a global–regional chemistry–climate model with a source attribution method (tagging) to quantify the contribution of anthropogenic emissions to ozone. Our analysis shows that the contribution of European anthropogenic emissions largely increases during large ozone periods, indicating that emissions from these sectors drive ozone values.
Barbara Ervens, Andrew Rickard, Bernard Aumont, William P. L. Carter, Max McGillen, Abdelwahid Mellouki, John Orlando, Bénédicte Picquet-Varrault, Paul Seakins, William R. Stockwell, Luc Vereecken, and Timothy J. Wallington
Atmos. Chem. Phys., 24, 13317–13339, https://doi.org/10.5194/acp-24-13317-2024, https://doi.org/10.5194/acp-24-13317-2024, 2024
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Chemical mechanisms describe the chemical processes in atmospheric models that are used to describe the changes in the atmospheric composition. Therefore, accurate chemical mechanisms are necessary to predict the evolution of air pollution and climate change. The article describes all steps that are needed to build chemical mechanisms and discusses the advances and needs of experimental and theoretical research activities needed to build reliable chemical mechanisms.
Jianing Dai, Guy P. Brasseur, Mihalis Vrekoussis, Maria Kanakidou, Kun Qu, Yijuan Zhang, Hongliang Zhang, and Tao Wang
Atmos. Chem. Phys., 24, 12943–12962, https://doi.org/10.5194/acp-24-12943-2024, https://doi.org/10.5194/acp-24-12943-2024, 2024
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This paper employs a regional chemical transport model to quantify the sensitivity of air pollutants and photochemical parameters to specified emission reductions in China for representative winter and summer conditions. The study provides insights into further air quality control in China with reduced primary emissions.
T. Nash Skipper, Emma L. D'Ambro, Forwood C. Wiser, V. Faye McNeill, Rebecca H. Schwantes, Barron H. Henderson, Ivan R. Piletic, Colleen B. Baublitz, Jesse O. Bash, Andrew R. Whitehill, Lukas C. Valin, Asher P. Mouat, Jennifer Kaiser, Glenn M. Wolfe, Jason M. St. Clair, Thomas F. Hanisco, Alan Fried, Bryan K. Place, and Havala O.T. Pye
Atmos. Chem. Phys., 24, 12903–12924, https://doi.org/10.5194/acp-24-12903-2024, https://doi.org/10.5194/acp-24-12903-2024, 2024
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We develop the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM) version 2 to improve predictions of formaldehyde in ambient air compared to satellite-, aircraft-, and ground-based observations. With the updated chemistry, we estimate the cancer risk from inhalation exposure to ambient formaldehyde across the contiguous USA and predict that 40 % of this risk is controllable through reductions in anthropogenic emissions of nitrogen oxides and reactive organic carbon.
Baoshuang Liu, Yao Gu, Yutong Wu, Qili Dai, Shaojie Song, Yinchang Feng, and Philip K. Hopke
Atmos. Chem. Phys., 24, 12861–12879, https://doi.org/10.5194/acp-24-12861-2024, https://doi.org/10.5194/acp-24-12861-2024, 2024
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Reactive loss of volatile organic compounds (VOCs) is a long-term issue yet to be resolved in VOC source analyses. We assess common methods of, and existing issues in, reducing losses, impacts of losses, and sources in current source analyses. We offer a potential supporting role for solving issues of VOC conversion. Source analyses of consumed VOCs that reacted to produce ozone and secondary organic aerosols can play an important role in the effective control of secondary pollution in air.
Deepangsu Chatterjee, Randall V. Martin, Chi Li, Dandan Zhang, Haihui Zhu, Daven K. Henze, James H. Crawford, Ronald C. Cohen, Lok N. Lamsal, and Alexander M. Cede
Atmos. Chem. Phys., 24, 12687–12706, https://doi.org/10.5194/acp-24-12687-2024, https://doi.org/10.5194/acp-24-12687-2024, 2024
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We investigate the hourly variation of NO2 columns and surface concentrations by applying the GEOS-Chem model to interpret aircraft and ground-based measurements over the US and Pandora sun photometer measurements over the US, Europe, and Asia. Corrections to the Pandora columns and finer model resolution improve the modeled representation of the summertime hourly variation of total NO2 columns to explain the weaker hourly variation in NO2 columns than at the surface.
Kiyeon Kim, Kyung Man Han, Chul Han Song, Hyojun Lee, Ross Beardsley, Jinhyeok Yu, Greg Yarwood, Bonyoung Koo, Jasper Madalipay, Jung-Hun Woo, and Seogju Cho
Atmos. Chem. Phys., 24, 12575–12593, https://doi.org/10.5194/acp-24-12575-2024, https://doi.org/10.5194/acp-24-12575-2024, 2024
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We incorporated each HONO process into the current CMAQ modeling framework to enhance the accuracy of HONO mixing ratio predictions. These results expand our understanding of HONO photochemistry and identify crucial sources of HONO that impact the total HONO budget in Seoul, South Korea. Through this investigation, we contribute to resolving discrepancies in understanding chemical transport models, with implications for better air quality management and environmental protection in the region.
Flossie Brown, Gerd Folberth, Stephen Sitch, Paulo Artaxo, Marijn Bauters, Pascal Boeckx, Alexander W. Cheesman, Matteo Detto, Ninong Komala, Luciana Rizzo, Nestor Rojas, Ines dos Santos Vieira, Steven Turnock, Hans Verbeeck, and Alfonso Zambrano
Atmos. Chem. Phys., 24, 12537–12555, https://doi.org/10.5194/acp-24-12537-2024, https://doi.org/10.5194/acp-24-12537-2024, 2024
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Ozone is a pollutant that is detrimental to human and plant health. Ozone monitoring sites in the tropics are limited, so models are often used to understand ozone exposure. We use measurements from the tropics to evaluate ozone from the UK Earth system model, UKESM1. UKESM1 is able to capture the pattern of ozone in the tropics, except in southeast Asia, although it systematically overestimates it at all sites. This work highlights that UKESM1 can capture seasonal and hourly variability.
Namrata Shanmukh Panji, Deborah F. McGlynn, Laura E. R. Barry, Todd M. Scanlon, Manuel T. Lerdau, Sally E. Pusede, and Gabriel Isaacman-VanWertz
Atmos. Chem. Phys., 24, 12495–12507, https://doi.org/10.5194/acp-24-12495-2024, https://doi.org/10.5194/acp-24-12495-2024, 2024
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Climate change will bring about changes in parameters that are currently used in global-scale models to calculate biogenic emissions. This study seeks to understand the factors driving these models by comparing long-term datasets of biogenic compounds to modeled emissions. We note that the light-dependent fractions currently used in models do not accurately represent regional observations. We provide evidence for the time-dependent variation in this parameter for future modifications to models.
Martin Vojta, Andreas Plach, Saurabh Annadate, Sunyoung Park, Gawon Lee, Pallav Purohit, Florian Lindl, Xin Lan, Jens Mühle, Rona L. Thompson, and Andreas Stohl
Atmos. Chem. Phys., 24, 12465–12493, https://doi.org/10.5194/acp-24-12465-2024, https://doi.org/10.5194/acp-24-12465-2024, 2024
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We constrain the global emissions of the very potent greenhouse gas sulfur hexafluoride (SF6) between 2005 and 2021. We show that SF6 emissions are decreasing in the USA and in the EU, while they are substantially growing in China, leading overall to an increasing global emission trend. The national reports for the USA, EU, and China all underestimated their SF6 emissions. However, stringent mitigation measures can successfully reduce SF6 emissions, as can be seen in the EU emission trend.
Yasin Elshorbany, Jerald R. Ziemke, Sarah Strode, Hervé Petetin, Kazuyuki Miyazaki, Isabelle De Smedt, Kenneth Pickering, Rodrigo J. Seguel, Helen Worden, Tamara Emmerichs, Domenico Taraborrelli, Maria Cazorla, Suvarna Fadnavis, Rebecca R. Buchholz, Benjamin Gaubert, Néstor Y. Rojas, Thiago Nogueira, Thérèse Salameh, and Min Huang
Atmos. Chem. Phys., 24, 12225–12257, https://doi.org/10.5194/acp-24-12225-2024, https://doi.org/10.5194/acp-24-12225-2024, 2024
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We investigated tropospheric ozone spatial variability and trends from 2005 to 2019 and related those to ozone precursors on global and regional scales. We also investigate the spatiotemporal characteristics of the ozone formation regime in relation to ozone chemical sources and sinks. Our analysis is based on remote sensing products of the tropospheric column of ozone and its precursors, nitrogen dioxide, formaldehyde, and total column CO, as well as ozonesonde data and model simulations.
Mariano Mertens, Sabine Brinkop, Phoebe Graf, Volker Grewe, Johannes Hendricks, Patrick Jöckel, Anna Lanteri, Sigrun Matthes, Vanessa S. Rieger, Mattia Righi, and Robin N. Thor
Atmos. Chem. Phys., 24, 12079–12106, https://doi.org/10.5194/acp-24-12079-2024, https://doi.org/10.5194/acp-24-12079-2024, 2024
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We quantified the contributions of land transport, shipping, and aviation emissions to tropospheric ozone; its radiative forcing; and the reductions of the methane lifetime using chemistry-climate model simulations. The contributions were analysed for the conditions of 2015 and for three projections for the year 2050. The results highlight the challenges of mitigating ozone formed by emissions of the transport sector, caused by the non-linearitiy of the ozone chemistry and the long lifetime.
Lauri Franzon, Marie Camredon, Richard Valorso, Bernard Aumont, and Theo Kurtén
Atmos. Chem. Phys., 24, 11679–11699, https://doi.org/10.5194/acp-24-11679-2024, https://doi.org/10.5194/acp-24-11679-2024, 2024
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In this article we investigate the formation of large, sticky molecules from various organic compounds entering the atmosphere as primary emissions and the degree to which these processes may contribute to organic aerosol particle mass. More specifically, we qualitatively investigate a recently discovered chemical reaction channel for one of the most important short-lived radical compounds, peroxy radicals, and discover which of these reactions are most atmospherically important.
Siting Li, Yiming Liu, Yuqi Zhu, Yinbao Jin, Yingying Hong, Ao Shen, Yifei Xu, Haofan Wang, Haichao Wang, Xiao Lu, Shaojia Fan, and Qi Fan
Atmos. Chem. Phys., 24, 11521–11544, https://doi.org/10.5194/acp-24-11521-2024, https://doi.org/10.5194/acp-24-11521-2024, 2024
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This study establishes an inventory of anthropogenic chlorine emissions in China in 2019 with expanded species (HCl, Cl-, Cl2, HOCl) and sources (41 specific sources). The inventory is validated by a modeling study against the observations. This study enhances the understanding of anthropogenic chlorine emissions in the atmosphere, identifies key sources, and provides scientific support for pollution control and climate change.
Willem E. van Caspel, Zbigniew Klimont, Chris Heyes, and Hilde Fagerli
Atmos. Chem. Phys., 24, 11545–11563, https://doi.org/10.5194/acp-24-11545-2024, https://doi.org/10.5194/acp-24-11545-2024, 2024
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Methane in the atmosphere contributes to the production of ozone gas – an air pollutant and greenhouse gas. Our results highlight that simultaneous reductions in methane emissions help avoid offsetting the air pollution benefits already achieved by the already-approved precursor emission reductions by 2050 in the European Monitoring and Evaluation Programme region, while also playing an important role in bringing air pollution further down towards World Health Organization guideline limits.
Tia R. Scarpelli, Paul I. Palmer, Mark Lunt, Ingrid Super, and Arjan Droste
Atmos. Chem. Phys., 24, 10773–10791, https://doi.org/10.5194/acp-24-10773-2024, https://doi.org/10.5194/acp-24-10773-2024, 2024
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Under the Paris Agreement, countries must track their anthropogenic greenhouse gas emissions. This study describes a method to determine self-consistent estimates for combustion emissions and natural fluxes of CO2 from atmospheric data. We report consistent estimates inferred using this approach from satellite data and ground-based data over Europe, suggesting that satellite data can be used to determine national anthropogenic CO2 emissions for countries where ground-based CO2 data are absent.
Ryan J. Pound, Lucy V. Brown, Mat J. Evans, and Lucy J. Carpenter
Atmos. Chem. Phys., 24, 9899–9921, https://doi.org/10.5194/acp-24-9899-2024, https://doi.org/10.5194/acp-24-9899-2024, 2024
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Iodine-mediated loss of ozone to the ocean surface and the subsequent emission of iodine species has a large effect on the troposphere. Here we combine recent experimental insights to develop a box model of the process, which we then parameterize and incorporate into the GEOS-Chem transport model. We find that these new insights have a small impact on the total emission of iodine but significantly change its distribution.
Katherine R. Travis, Benjamin A. Nault, James H. Crawford, Kelvin H. Bates, Donald R. Blake, Ronald C. Cohen, Alan Fried, Samuel R. Hall, L. Gregory Huey, Young Ro Lee, Simone Meinardi, Kyung-Eun Min, Isobel J. Simpson, and Kirk Ullman
Atmos. Chem. Phys., 24, 9555–9572, https://doi.org/10.5194/acp-24-9555-2024, https://doi.org/10.5194/acp-24-9555-2024, 2024
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Human activities result in the emission of volatile organic compounds (VOCs) that contribute to air pollution. Detailed VOC measurements were taken during a field study in South Korea. When compared to VOC inventories, large discrepancies showed underestimates from chemical products, liquefied petroleum gas, and long-range transport. Improved emissions and chemistry of these VOCs better described urban pollution. The new chemical scheme is relevant to urban areas and other VOC sources.
Beth S. Nelson, Zhenze Liu, Freya A. Squires, Marvin Shaw, James R. Hopkins, Jacqueline F. Hamilton, Andrew R. Rickard, Alastair C. Lewis, Zongbo Shi, and James D. Lee
Atmos. Chem. Phys., 24, 9031–9044, https://doi.org/10.5194/acp-24-9031-2024, https://doi.org/10.5194/acp-24-9031-2024, 2024
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The impact of combined air quality and carbon neutrality policies on O3 formation in Beijing was investigated. Emissions inventory data were used to estimate future pollutant mixing ratios relative to ground-level observations. O3 production was found to be most sensitive to changes in alkenes, but large reductions in less reactive compounds led to larger reductions in future O3 production. This study highlights the importance of understanding the emissions of organic pollutants.
Takashi Sekiya, Emanuele Emili, Kazuyuki Miyazaki, Antje Inness, Zhen Qu, R. Bradley Pierce, Dylan Jones, Helen Worden, William Y. Y. Cheng, Vincent Huijnen, and Gerbrand Koren
EGUsphere, https://doi.org/10.5194/egusphere-2024-2426, https://doi.org/10.5194/egusphere-2024-2426, 2024
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Five global chemical reanalysis datasets were used to assess the relative impacts of assimilating satellite ozone and its precursors measurements on tropospheric ozone analyses for 2010. The multiple reanalysis system comparison allows for evaluating dependency of the impacts on different reanalysis systems. The results suggested the importance of satellite ozone and its precursor measurements for improving ozone analysis in the whole troposphere, with varying the magnitudes among the systems.
Maureen Beaudor, Didier Hauglustaine, Juliette Lathière, Martin Van Damme, Lieven Clarisse, and Nicolas Vuichard
EGUsphere, https://doi.org/10.5194/egusphere-2024-2022, https://doi.org/10.5194/egusphere-2024-2022, 2024
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Agriculture is the biggest ammonia (NH3) source, impacting air quality, climate, and ecosystems. Because of food demand, NH3 emissions are projected to rise by 2100. Using a global model, we analyzed the impact of present and future NH3 emissions generated from a land model. Our results show improved ammonia patterns compared to a reference inventory. Future scenarios predict up to 70 % increase in global NH3 burden, significant changes in radiative forcing, and could significantly elevate N2O.
Amir H. Souri, Bryan N. Duncan, Sarah A. Strode, Daniel C. Anderson, Michael E. Manyin, Junhua Liu, Luke D. Oman, Zhen Zhang, and Brad Weir
Atmos. Chem. Phys., 24, 8677–8701, https://doi.org/10.5194/acp-24-8677-2024, https://doi.org/10.5194/acp-24-8677-2024, 2024
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We explore a new method of using the wealth of information obtained from satellite observations of Aura OMI NO2, HCHO, and MERRA-2 reanalysis in NASA’s GEOS model equipped with an efficient tropospheric OH (TOH) estimator to enhance the representation of TOH spatial distribution and its long-term trends. This new framework helps us pinpoint regional inaccuracies in TOH and differentiate between established prior knowledge and newly acquired information from satellites on TOH trends.
Haipeng Lin, Louisa K. Emmons, Elizabeth W. Lundgren, Laura Hyesung Yang, Xu Feng, Ruijun Dang, Shixian Zhai, Yunxiao Tang, Makoto M. Kelp, Nadia K. Colombi, Sebastian D. Eastham, Thibaud M. Fritz, and Daniel J. Jacob
Atmos. Chem. Phys., 24, 8607–8624, https://doi.org/10.5194/acp-24-8607-2024, https://doi.org/10.5194/acp-24-8607-2024, 2024
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Tropospheric ozone is a major air pollutant, a greenhouse gas, and a major indicator of model skill. Global atmospheric chemistry models show large differences in simulations of tropospheric ozone, but isolating sources of differences is complicated by different model environments. By implementing the GEOS-Chem model side by side to CAM-chem within a common Earth system model, we identify and evaluate specific differences between the two models and their impacts on key chemical species.
Victor Lannuque and Karine Sartelet
Atmos. Chem. Phys., 24, 8589–8606, https://doi.org/10.5194/acp-24-8589-2024, https://doi.org/10.5194/acp-24-8589-2024, 2024
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Large uncertainties remain in understanding secondary organic aerosol (SOA) formation and speciation from naphthalene oxidation. This study details the development of the first near-explicit chemical scheme for naphthalene oxidation by OH, which includes kinetic and mechanistic data, and is able to reproduce most of the experimentally identified products in both gas and particle phases.
Hui Li, Jiaxin Qiu, and Bo Zheng
EGUsphere, https://doi.org/10.5194/egusphere-2024-1986, https://doi.org/10.5194/egusphere-2024-1986, 2024
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We conduct a sensitivity analysis on various factors including prior, model resolution, satellite constraint, and inversion system configuration to assess the vulnerability of emission estimates across temporal, sectoral, and regional dimensions. Our analysis first reveals the robustness of emissions estimated by this air pollution satellite sensor-based CO2 emission inversion system, with relative change between tests and Base inversion below 4.0 % for national annual NOx and CO2 emissions.
Shuai Li, Xiao Lu, and Haolin Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-1889, https://doi.org/10.5194/egusphere-2024-1889, 2024
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We report that the summertime ozone-temperature sensitivity decreased by 50 % from 3.0 ppbv/K in 1990 to 1.5 ppb/K in 2021 in the US. GEOS-Chem simulations show that anthropogenic NOx emission reduction is the dominant driver of the ozone-temperature sensitivity decline, through influencing both the temperature-direct and temperature-indirect processes. Reduced ozone-temperature sensitivity has decreased the ozone enhancement from low to high temperatures by an average of 6.8 ppbv across the US.
Tong Sha, Siyu Yang, Qingcai Chen, Liangqing Li, Xiaoyan Ma, Yan-Lin Zhang, Zhaozhong Feng, K. Folkert Boersma, and Jun Wang
Atmos. Chem. Phys., 24, 8441–8455, https://doi.org/10.5194/acp-24-8441-2024, https://doi.org/10.5194/acp-24-8441-2024, 2024
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Using an updated soil reactive nitrogen emission scheme in the Unified Inputs for Weather Research and Forecasting coupled with Chemistry (UI-WRF-Chem) model, we investigate the role of soil NO and HONO (Nr) emissions in air quality and temperature in North China. Contributions of soil Nr emissions to O3 and secondary pollutants are revealed, exceeding effects of soil NOx or HONO emission. Soil Nr emissions play an important role in mitigating O3 pollution and addressing climate change.
Jian Zhu, Shanshan Wang, Chuanqi Gu, Zhiwen Jiang, Sanbao Zhang, Ruibin Xue, Yuhao Yan, and Bin Zhou
Atmos. Chem. Phys., 24, 8383–8395, https://doi.org/10.5194/acp-24-8383-2024, https://doi.org/10.5194/acp-24-8383-2024, 2024
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In 2022, Shanghai implemented city-wide static management measures during the high-ozone season in April and May, providing a chance to study ozone pollution control. Despite significant emissions reductions, ozone levels increased by 23 %. Statistically, the number of days with higher ozone diurnal variation types increased during the lockdown period. The uneven decline in VOC and NO2 emissions led to heightened photochemical processes, resulting in the observed ozone level rise.
Hiroo Hata, Norifumi Mizushima, and Tomohiko Ihara
EGUsphere, https://doi.org/10.5194/egusphere-2024-1961, https://doi.org/10.5194/egusphere-2024-1961, 2024
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The introduction of battery electric vehicles (BEV) is expected to reduce the primary air pollutants from vehicular exhaust and evaporative emissions while reducing the anthropogenic heat produced by vehicles, ultimately decreasing the urban heat island effect (UHI). This study revealed the impact of introducing BEVs on the decrease in UHI and the effects of BEVs on the formation of tropospheric ozone and fine particulate matter in the Greater Tokyo Area of Japan.
Matthew J. Rowlinson, Mat J. Evans, Lucy J. Carpenter, Katie A. Read, Shalini Punjabi, Adedayo Adedeji, Luke Fakes, Ally Lewis, Ben Richmond, Neil Passant, Tim Murrells, Barron Henderson, Kelvin H. Bates, and Detlev Helmig
Atmos. Chem. Phys., 24, 8317–8342, https://doi.org/10.5194/acp-24-8317-2024, https://doi.org/10.5194/acp-24-8317-2024, 2024
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Ethane and propane are volatile organic compounds emitted from human activities which help to form ozone, a pollutant and greenhouse gas, and also affect the chemistry of the lower atmosphere. Atmospheric models tend to do a poor job of reproducing the abundance of these compounds in the atmosphere. By using regional estimates of their emissions, rather than globally consistent estimates, we can significantly improve the simulation of ethane in the model and make some improvement for propane.
Rodrigo J. Seguel, Lucas Castillo, Charlie Opazo, Néstor Y. Rojas, Thiago Nogueira, María Cazorla, Mario Gavidia-Calderón, Laura Gallardo, René Garreaud, Tomás Carrasco-Escaff, and Yasin Elshorbany
Atmos. Chem. Phys., 24, 8225–8242, https://doi.org/10.5194/acp-24-8225-2024, https://doi.org/10.5194/acp-24-8225-2024, 2024
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Trends of surface ozone were examined across South America. Our findings indicate that ozone trends in major South American cities either increase or remain steady, with no signs of decline. The upward trends can be attributed to chemical regimes that efficiently convert nitric oxide into nitrogen dioxide. Additionally, our results suggest a climate penalty for ozone driven by meteorological conditions that favor wildfire propagation in Chile and extensive heat waves in southern Brazil.
Maarten Krol, Bart van Stratum, Isidora Anglou, and Klaas Folkert Boersma
Atmos. Chem. Phys., 24, 8243–8262, https://doi.org/10.5194/acp-24-8243-2024, https://doi.org/10.5194/acp-24-8243-2024, 2024
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This paper presents detailed plume simulations of nitrogen oxides and carbon dioxide that are emitted from four large industrial facilities world-wide. Results from the high-resolution simulations that include atmospheric chemistry are compared to nitrogen dioxide observations from satellites. We find good performance of the model and show that common assumptions that are used in simplified models need revision. This work is important for the monitoring of emissions using satellite data.
Robin Plauchu, Audrey Fortems-Cheiney, Grégoire Broquet, Isabelle Pison, Antoine Berchet, Elise Potier, Gaëlle Dufour, Adriana Coman, Dilek Savas, Guillaume Siour, and Henk Eskes
Atmos. Chem. Phys., 24, 8139–8163, https://doi.org/10.5194/acp-24-8139-2024, https://doi.org/10.5194/acp-24-8139-2024, 2024
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This study uses the Community Inversion Framework and CHIMERE model to assess the potential of TROPOMI-S5P PAL NO2 tropospheric column data to estimate NOx emissions in France (2019–2021). Results show a 3 % decrease in average emissions compared to the 2016 CAMS-REG/INS, lower than the 14 % decrease from CITEPA. The study highlights challenges in capturing emission anomalies due to limited data coverage and error levels but shows promise for local inventory improvements.
Chelsea E. Stockwell, Matthew M. Coggon, Rebecca H. Schwantes, Colin Harkins, Bert Verreyken, Congmeng Lyu, Qindan Zhu, Lu Xu, Jessica B. Gilman, Aaron Lamplugh, Jeff Peischl, Michael A. Robinson, Patrick R. Veres, Meng Li, Andrew W. Rollins, Kristen Zuraski, Sunil Baidar, Shang Liu, Toshihiro Kuwayama, Steven S. Brown, Brian C. McDonald, and Carsten Warneke
EGUsphere, https://doi.org/10.5194/egusphere-2024-1899, https://doi.org/10.5194/egusphere-2024-1899, 2024
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In urban areas, emissions from everyday products like paints, cleaners, and personal care products, along with non-traditional sources such as cooking are important sources that impact air quality. This study used a model to evaluate how these emissions impact ozone in the Los Angeles Basin, and quantifies the impact of gaseous cooking emissions for the first time. Accurate representation of these and other man-made sources in inventories is crucial to inform effective air quality policies.
Zhendong Lu, Jun Wang, Yi Wang, Daven K. Henze, Xi Chen, Tong Sha, and Kang Sun
Atmos. Chem. Phys., 24, 7793–7813, https://doi.org/10.5194/acp-24-7793-2024, https://doi.org/10.5194/acp-24-7793-2024, 2024
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In contrast with past work showing that the reduction of emissions was the dominant factor for the nationwide increase of surface O3 during the lockdown in China, this study finds that the variation in meteorology (temperature and other parameters) plays a more important role. This result is obtained through sensitivity simulations using a chemical transport model constrained by satellite (TROPOMI) data and calibrated with surface observations.
Xiaohong Yao and Leiming Zhang
Atmos. Chem. Phys., 24, 7773–7791, https://doi.org/10.5194/acp-24-7773-2024, https://doi.org/10.5194/acp-24-7773-2024, 2024
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This study investigates long-term trends of criteria air pollutants, including NO2, CO, SO2, O3 and PM2.5, and NO2+O3 measured in 10 Canadian cities during the last 2 to 3 decades. We also investigate associated driving forces in terms of emission reductions, perturbations from varying weather conditions and large-scale wildfires, as well as changes in O3 sources and sinks.
Yao Ge, Sverre Solberg, Mathew R. Heal, Stefan Reimann, Willem van Caspel, Bryan Hellack, Thérèse Salameh, and David Simpson
Atmos. Chem. Phys., 24, 7699–7729, https://doi.org/10.5194/acp-24-7699-2024, https://doi.org/10.5194/acp-24-7699-2024, 2024
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Atmospheric volatile organic compounds (VOCs) constitute many species, acting as precursors to ozone and aerosol. Given the uncertainties in VOC emissions, lack of evaluation studies, and recent changes in emissions, this work adapts the EMEP MSC-W to evaluate emission inventories in Europe. We focus on the varying agreement between modelled and measured VOCs across different species and underscore potential inaccuracies in total and sector-specific emission estimates.
Shuzhuang Feng, Fei Jiang, Tianlu Qian, Nan Wang, Mengwei Jia, Songci Zheng, Jiansong Chen, Fang Ying, and Weimin Ju
Atmos. Chem. Phys., 24, 7481–7498, https://doi.org/10.5194/acp-24-7481-2024, https://doi.org/10.5194/acp-24-7481-2024, 2024
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We developed a multi-air-pollutant inversion system to estimate non-methane volatile organic compound (NMVOC) emissions using TROPOMI formaldehyde retrievals. We found that the inversion significantly improved formaldehyde simulations and reduced NMVOC emission uncertainties. The optimized NMVOC emissions effectively corrected the overestimation of O3 levels, mainly by decreasing the rate of the RO2 + NO reaction and increasing the rate of the NO2 + OH reaction.
Yuqing Qiu, Xin Li, Wenxuan Chai, Yi Liu, Mengdi Song, Xudong Tian, Qiaoli Zou, Wenjun Lou, Wangyao Zhang, Juan Li, and Yuanhang Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2024-1576, https://doi.org/10.5194/egusphere-2024-1576, 2024
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The chemical reactions of ozone (O3) formation are related to meteorology and local emissions. Here, a random forest approach was used to eliminate the effects of meteorological factors (dispersion or transport) on O3 and its precursors. Variations in the sensitivity of O3 formation and the apportionment of emission sources were revealed after meteorological normalization. Our results suggest that meteorological variations should be considered when diagnosing O3 formation.
Haklim Choi, Alison L. Redington, Hyeri Park, Jooil Kim, Rona L. Thompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Ray F. Weiss, Alistair J. Manning, and Sunyoung Park
Atmos. Chem. Phys., 24, 7309–7330, https://doi.org/10.5194/acp-24-7309-2024, https://doi.org/10.5194/acp-24-7309-2024, 2024
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We analyzed with an inversion model the atmospheric abundance of hydrofluorocarbons (HFCs), potent greenhouse gases, from 2008 to 2020 at Gosan station in South Korea and revealed a significant increase in emissions, especially from eastern China and Japan. This increase contradicts reported data, underscoring the need for accurate monitoring and reporting. Our findings are crucial for understanding and managing global HFCs emissions, highlighting the importance of efforts to reduce HFCs.
Laura Hyesung Yang, Daniel J. Jacob, Ruijun Dang, Yujin J. Oak, Haipeng Lin, Jhoon Kim, Shixian Zhai, Nadia K. Colombi, Drew C. Pendergrass, Ellie Beaudry, Viral Shah, Xu Feng, Robert M. Yantosca, Heesung Chong, Junsung Park, Hanlim Lee, Won-Jin Lee, Soontae Kim, Eunhye Kim, Katherine R. Travis, James H. Crawford, and Hong Liao
Atmos. Chem. Phys., 24, 7027–7039, https://doi.org/10.5194/acp-24-7027-2024, https://doi.org/10.5194/acp-24-7027-2024, 2024
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The Geostationary Environment Monitoring Spectrometer (GEMS) provides hourly measurements of NO2. We use the chemical transport model to find how emissions, chemistry, and transport drive the changes in NO2 observed by GEMS at different times of the day. In winter, the chemistry plays a minor role, and high daytime emissions dominate the diurnal variation in NO2, balanced by transport. In summer, emissions, chemistry, and transport play an important role in shaping the diurnal variation in NO2.
M. Omar Nawaz, Jeremiah Johnson, Greg Yarwood, Benjamin de Foy, Laura Judd, and Daniel L. Goldberg
Atmos. Chem. Phys., 24, 6719–6741, https://doi.org/10.5194/acp-24-6719-2024, https://doi.org/10.5194/acp-24-6719-2024, 2024
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NO2 is a gas with implications for air pollution. A campaign conducted in Houston provided an opportunity to compare NO2 from different instruments and a model. Aircraft and satellite observations agreed well with measurements on the ground; however, the latter estimated lower values. We find that model-simulated NO2 was lower than observations, especially downtown, suggesting that NO2 sources associated with the urban core of Houston, such as vehicle emissions, may be underestimated.
Natalie Brett, Kathy S. Law, Steve R. Arnold, Javier G. Fochesatto, Jean-Christophe Raut, Tatsuo Onishi, Robert Gilliam, Kathleen Fahey, Deanna Huff, George Pouliot, Brice Barret, Elsa Dieudonne, Roman Pohorsky, Julia Schmale, Andrea Baccarini, Slimane Bekki, Gianluca Pappaccogli, Federico Scoto, Stefano Decesari, Antonio Donateo, Meeta Cesler-Maloney, William Simpson, Patrice Medina, Barbara D'Anna, Brice Temime-Roussel, Joel Savarino, Sarah Albertin, Jingqiu Mao, Becky Alexander, Allison Moon, Peter F. DeCarlo, Vanessa Selimovic, Robert Yokelson, and Ellis S. Robinson
EGUsphere, https://doi.org/10.5194/egusphere-2024-1450, https://doi.org/10.5194/egusphere-2024-1450, 2024
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Processes influencing dispersion of local anthropogenic emissions in Arctic wintertime are investigated with dispersion model simulations. Modelled power plant plume rise that considers surface and elevated temperature inversions improves results compared to observations. Modelled near-surface concentrations are improved by representation of vertical mixing and emission estimates. Large increases in diesel vehicle emissions at temperatures reaching -35 °C are required to reproduce observed NOx.
Tianlang Zhao, Jingqiu Mao, Zolal Ayazpour, Gonzalo González Abad, Caroline R. Nowlan, and Yiqi Zheng
Atmos. Chem. Phys., 24, 6105–6121, https://doi.org/10.5194/acp-24-6105-2024, https://doi.org/10.5194/acp-24-6105-2024, 2024
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HCHO variability is a key tracer in understanding VOC emissions in response to climate change. We investigate the role of methane oxidation and biogenic and wildfire emissions in HCHO interannual variability over northern high latitudes in summer, emphasizing wildfires as a key driver of HCHO interannual variability in Alaska, Siberia and northern Canada using satellite HCHO and SIF retrievals and then GEOS-Chem model. We show SIF is a tool to understand biogenic HCHO variability in this region.
Jianghao Li, Alastair C. Lewis, Jim R. Hopkins, Stephen J. Andrews, Tim Murrells, Neil Passant, Ben Richmond, Siqi Hou, William J. Bloss, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 24, 6219–6231, https://doi.org/10.5194/acp-24-6219-2024, https://doi.org/10.5194/acp-24-6219-2024, 2024
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A summertime ozone event at an urban site in Birmingham is sensitive to volatile organic compounds (VOCs) – particularly those of oxygenated VOCs. The roles of anthropogenic VOC sources in urban ozone chemistry are examined by integrating the 1990–2019 national atmospheric emission inventory into model scenarios. Road transport remains the most powerful means of further reducing ozone in this case study, but the benefits may be offset if solvent emissions of VOCs continue to increase.
Kai-Lan Chang, Owen R. Cooper, Audrey Gaudel, Irina Petropavlovskikh, Peter Effertz, Gary Morris, and Brian C. McDonald
Atmos. Chem. Phys., 24, 6197–6218, https://doi.org/10.5194/acp-24-6197-2024, https://doi.org/10.5194/acp-24-6197-2024, 2024
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A great majority of observational trend studies of free tropospheric ozone use sparsely sampled ozonesonde and aircraft measurements as reference data sets. A ubiquitous assumption is that trends are accurate and reliable so long as long-term records are available. We show that sampling bias due to sparse samples can persistently reduce the trend accuracy, and we highlight the importance of maintaining adequate frequency and continuity of observations.
Jin Ma, Linda M. J. Kooijmans, Norbert Glatthor, Stephen A. Montzka, Marc von Hobe, Thomas Röckmann, and Maarten C. Krol
Atmos. Chem. Phys., 24, 6047–6070, https://doi.org/10.5194/acp-24-6047-2024, https://doi.org/10.5194/acp-24-6047-2024, 2024
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The global budget of atmospheric COS can be optimised by inverse modelling using TM5-4DVAR, with the co-constraints of NOAA surface observations and MIPAS satellite data. We found reduced COS biosphere uptake from inversions and improved land and ocean separation using MIPAS satellite data assimilation. Further improvements are expected from better quantification of COS ocean and biosphere fluxes.
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Short summary
NOx in the free troposphere (above 2 km) affects global tropospheric chemistry and the retrieval and interpretation of satellite NO2 measurements. We evaluate free tropospheric NOx in global atmospheric chemistry models and find that recycling NOx from its reservoirs over the oceans is faster than that simulated in the models, resulting in increases in simulated tropospheric ozone and OH. Over the U.S., free tropospheric NO2 contributes the majority of the tropospheric NO2 column in summer.
NOx in the free troposphere (above 2 km) affects global tropospheric chemistry and the retrieval...
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