Articles | Volume 19, issue 13
https://doi.org/10.5194/acp-19-8863-2019
© Author(s) 2019. 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-19-8863-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
12 Jul 2019
Research article |
| 12 Jul 2019
| 12 Jul 2019
Using satellite observations of tropospheric NO2 columns to infer long-term trends in US NOx emissions: the importance of accounting for the free tropospheric NO2 background
Department of Earth and Planetary Sciences, Harvard University,
Cambridge, MA, USA
Daniel J. Jacob
Department of Earth and Planetary Sciences, Harvard University,
Cambridge, MA, USA
School of Engineering and Applied Sciences, Harvard University,
Cambridge, MA, USA
Loretta J. Mickley
School of Engineering and Applied Sciences, Harvard University,
Cambridge, MA, USA
Melissa P. Sulprizio
School of Engineering and Applied Sciences, Harvard University,
Cambridge, MA, USA
Katherine R. Travis
Department of Civil and Environmental Engineering, Massachusetts
Institute of Technology, Cambridge, MA, USA
now at: NASA Langley Research Center, Hampton, VA, USA
Eloise A. Marais
Department of Physics and Astronomy, University of Leicester,
Leicester, UK
Ronald C. Cohen
Department of Chemistry, University of California, Berkeley, CA, USA
Department of Earth and Planetary Science, University of California,
Berkeley, CA, USA
Joshua L. Laughner
Department of Chemistry, University of California, Berkeley, CA, USA
now at: Division of Geological and Planetary Sciences, California
Institute of Technology, Pasadena, CA, USA
Sungyeon Choi
Science Systems and Applications Inc., Lanham, MD, USA
Joanna Joiner
Science Systems and Applications Inc., Lanham, MD, USA
NASA Goddard Space Flight Center, Greenbelt, MD, USA
Lok N. Lamsal
NASA Goddard Space Flight Center, Greenbelt, MD, USA
Goddard Earth Sciences Technology and Research, Universities Space
Research Association, Columbia, MD, USA
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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.
Harrison A. Parker, Joshua L. Laughner, Geoffrey C. Toon, Debra Wunch, Coleen M. Roehl, Laura T. Iraci, James R. Podolske, Kathryn McKain, Bianca C. Baier, and Paul O. Wennberg
Atmos. Meas. Tech., 16, 2601–2625, https://doi.org/10.5194/amt-16-2601-2023, https://doi.org/10.5194/amt-16-2601-2023, 2023
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We describe a retrieval algorithm for determining limited information about the vertical distribution of carbon monoxide (CO) and carbon dioxide (CO2) from total column observations from ground-based observations. Our retrieved partial column values compare well with integrated in situ data. The average error for our retrieval is 1.51 ppb (~ 2 %) for CO and 5.09 ppm (~ 1.25 %) for CO2. We anticipate that this approach will find broad application for use in carbon cycle science.
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.
Yu Someya, Yukio Yoshida, Hirofumi Ohyama, Shohei Nomura, Akihide Kamei, Isamu Morino, Hitoshi Mukai, Tsuneo Matsunaga, Joshua L. Laughner, Voltaire A. Velazco, Benedikt Herkommer, Yao Té, Mahesh Kumar Sha, Rigel Kivi, Minqiang Zhou, Young Suk Oh, Nicholas M. Deutscher, and David W. T. Griffith
Atmos. Meas. Tech., 16, 1477–1501, https://doi.org/10.5194/amt-16-1477-2023, https://doi.org/10.5194/amt-16-1477-2023, 2023
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The updated retrieval algorithm for the Greenhouse gases Observing SATellite level 2 product is presented. The main changes in the algorithm from the previous one are the treatment of cirrus clouds, the degradation model of the sensor, solar irradiance, and gas absorption coefficient tables. The retrieval results showed improvements in fitting accuracy and an increase in the data amount over land. On the other hand, there are still large biases of XCO2 which should be corrected over the ocean.
Cameron G. MacDonald, Jon-Paul Mastrogiacomo, Joshua L. Laughner, Jacob K. Hedelius, Ray Nassar, and Debra Wunch
Atmos. Chem. Phys., 23, 3493–3516, https://doi.org/10.5194/acp-23-3493-2023, https://doi.org/10.5194/acp-23-3493-2023, 2023
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We use three satellites measuring carbon dioxide (CO2), carbon monoxide (CO) and nitrogen dioxide (NO2) to calculate atmospheric enhancements of these gases from 27 urban areas. We calculate enhancement ratios between the species and compare those to ratios derived from four globally gridded anthropogenic emission inventories. We find that the global inventories generally underestimate CO emissions in many North American and European cities relative to our observed enhancement ratios.
Nasrin Mostafavi Pak, Jacob K. Hedelius, Sébastien Roche, Liz Cunningham, Bianca Baier, Colm Sweeney, Coleen Roehl, Joshua Laughner, Geoffrey Toon, Paul Wennberg, Harrison Parker, Colin Arrowsmith, Joseph Mendonca, Pierre Fogal, Tyler Wizenberg, Beatriz Herrera, Kimberly Strong, Kaley A. Walker, Felix Vogel, and Debra Wunch
Atmos. Meas. Tech., 16, 1239–1261, https://doi.org/10.5194/amt-16-1239-2023, https://doi.org/10.5194/amt-16-1239-2023, 2023
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Ground-based remote sensing instruments in the Total Carbon Column Observing Network (TCCON) measure greenhouse gases in the atmosphere. Consistency between TCCON measurements is crucial to accurately infer changes in atmospheric composition. We use portable remote sensing instruments (EM27/SUN) to evaluate biases between TCCON stations in North America. We also improve the retrievals of EM27/SUN instruments and evaluate the previous (GGG2014) and newest (GGG2020) retrieval algorithms.
Joshua L. Laughner, Sébastien Roche, Matthäus Kiel, Geoffrey C. Toon, Debra Wunch, Bianca C. Baier, Sébastien Biraud, Huilin Chen, Rigel Kivi, Thomas Laemmel, Kathryn McKain, Pierre-Yves Quéhé, Constantina Rousogenous, Britton B. Stephens, Kaley Walker, and Paul O. Wennberg
Atmos. Meas. Tech., 16, 1121–1146, https://doi.org/10.5194/amt-16-1121-2023, https://doi.org/10.5194/amt-16-1121-2023, 2023
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Observations using sunlight to measure surface-to-space total column of greenhouse gases in the atmosphere need an initial guess of the vertical distribution of those gases to start from. We have developed an approach to provide those initial guess profiles that uses readily available meteorological data as input. This lets us make these guesses without simulating them with a global model. The profiles generated this way match independent observations well.
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.
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.
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.
Viral Shah, Daniel J. Jacob, Ruijun Dang, Lok N. Lamsal, Sarah A. Strode, Stephen D. Steenrod, K. Folkert Boersma, Sebastian D. Eastham, Thibaud M. Fritz, Chelsea Thompson, Jeff Peischl, Ilann Bourgeois, Ilana B. Pollack, Benjamin A. Nault, Ronald C. Cohen, Pedro Campuzano-Jost, Jose L. Jimenez, Simone T. Andersen, Lucy J. Carpenter, Tomás Sherwen, and Mat J. Evans
Atmos. Chem. Phys., 23, 1227–1257, https://doi.org/10.5194/acp-23-1227-2023, https://doi.org/10.5194/acp-23-1227-2023, 2023
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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.
Vitali E. Fioletov, Chris A. McLinden, Debora Griffin, Ihab Abboud, Nickolay Krotkov, Peter J. T. Leonard, Can Li, Joanna Joiner, Nicolas Theys, and Simon Carn
Earth Syst. Sci. Data, 15, 75–93, https://doi.org/10.5194/essd-15-75-2023, https://doi.org/10.5194/essd-15-75-2023, 2023
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Sulfur dioxide (SO2) measurements from three satellite instruments were used to update and extend the previously developed global catalogue of large SO2 emission sources. This version 2 of the global catalogue covers the period of 2005–2021 and includes a total of 759 continuously emitting point sources. The catalogue data show an approximate 50 % decline in global SO2 emissions between 2005 and 2021, although emissions were relatively stable during the last 3 years.
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.
Amy Christiansen, Loretta J. Mickley, Junhua Liu, Luke D. Oman, and Lu Hu
Atmos. Chem. Phys., 22, 14751–14782, https://doi.org/10.5194/acp-22-14751-2022, https://doi.org/10.5194/acp-22-14751-2022, 2022
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Understanding tropospheric ozone trends is crucial for accurate predictions of future air quality and climate, but drivers of trends are not well understood. We analyze global tropospheric ozone trends since 1980 using ozonesonde and surface measurements, and we evaluate two models for their ability to reproduce trends. We find observational evidence of increasing tropospheric ozone, but models underestimate these increases. This hinders our ability to estimate ozone radiative forcing.
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.
Can Li, Joanna Joiner, Fei Liu, Nickolay A. Krotkov, Vitali Fioletov, and Chris McLinden
Atmos. Meas. Tech., 15, 5497–5514, https://doi.org/10.5194/amt-15-5497-2022, https://doi.org/10.5194/amt-15-5497-2022, 2022
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Satellite observations provide information on the sources of SO2, an important pollutant that affects both air quality and climate. However, these observations suffer from relatively poor data quality due to weak signals of SO2. Here, we use a machine learning technique to analyze satellite SO2 observations in order to reduce the noise and artifacts over relatively clean areas while keeping the signals near pollution sources. This leads to significant improvement in satellite SO2 data.
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.
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.
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.
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.
Joseph S. Schlosser, Connor Stahl, Armin Sorooshian, Yen Thi-Hoang Le, Ki-Joon Jeon, Peng Xian, Carolyn E. Jordan, Katherine R. Travis, James H. Crawford, Sung Yong Gong, Hye-Jung Shin, In-Ho Song, and Jong-sang Youn
Atmos. Chem. Phys., 22, 7505–7522, https://doi.org/10.5194/acp-22-7505-2022, https://doi.org/10.5194/acp-22-7505-2022, 2022
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During a major haze pollution episode in March 2019, anthropogenic emissions were dominant in the boundary layer over Incheon and Seoul, South Korea. Using supermicrometer and submicrometer size- and chemistry-resolved aerosol particle measurements taken during this haze pollution period, this work shows that local emissions and a shallow boundary layer, enhanced humidity, and low temperature promoted local heterogeneous formation of secondary inorganic and organic aerosol species.
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.
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 %.
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.
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.
Fei Liu, Zhining Tao, Steffen Beirle, Joanna Joiner, Yasuko Yoshida, Steven J. Smith, K. Emma Knowland, and Thomas Wagner
Atmos. Chem. Phys., 22, 1333–1349, https://doi.org/10.5194/acp-22-1333-2022, https://doi.org/10.5194/acp-22-1333-2022, 2022
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In this work, we present a novel method to infer NOx emissions and lifetimes based on tropospheric NO2 observations together with reanalysis wind fields for cities located in polluted backgrounds. We evaluate the accuracy of the method using synthetic NO2 observations derived from a high-resolution model simulation. Our work provides an estimate for uncertainties in satellite-derived emissions inferred from chemical transport model (CTM)-independent approaches.
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.
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.
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.
Nick Gorkavyi, Nickolay Krotkov, Can Li, Leslie Lait, Peter Colarco, Simon Carn, Matthew DeLand, Paul Newman, Mark Schoeberl, Ghassan Taha, Omar Torres, Alexander Vasilkov, and Joanna Joiner
Atmos. Meas. Tech., 14, 7545–7563, https://doi.org/10.5194/amt-14-7545-2021, https://doi.org/10.5194/amt-14-7545-2021, 2021
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The 21 June 2019 eruption of the Raikoke volcano produced significant amounts of volcanic aerosols (sulfate and ash) and sulfur dioxide (SO2) gas that penetrated into the lower stratosphere. We showed that the amount of SO2 decreases with a characteristic period of 8–18 d and the peak of sulfate aerosol lags the initial peak of SO2 by 1.5 months. We also examined the dynamics of an unusual stratospheric coherent circular cloud of SO2 and aerosol observed from 18 July to 22 September 2019.
Luis Guanter, Cédric Bacour, Andreas Schneider, Ilse Aben, Tim A. van Kempen, Fabienne Maignan, Christian Retscher, Philipp Köhler, Christian Frankenberg, Joanna Joiner, and Yongguang Zhang
Earth Syst. Sci. Data, 13, 5423–5440, https://doi.org/10.5194/essd-13-5423-2021, https://doi.org/10.5194/essd-13-5423-2021, 2021
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Sun-induced chlorophyll fluorescence (SIF) is an electromagnetic signal emitted by plants in the red and far-red parts of the spectrum. It has a functional link to photosynthesis and can be measured by satellite instruments, which makes it an important variable for the remote monitoring of the photosynthetic activity of vegetation ecosystems around the world. In this contribution we present a SIF dataset derived from the new Sentinel-5P TROPOMI missions.
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.
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.
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.
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.
Lee T. Murray, Eric M. Leibensperger, Clara Orbe, Loretta J. Mickley, and Melissa Sulprizio
Geosci. Model Dev., 14, 5789–5823, https://doi.org/10.5194/gmd-14-5789-2021, https://doi.org/10.5194/gmd-14-5789-2021, 2021
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Chemical-transport models are tools used to study air pollution and inform public policy. However, they are limited by the availability of archived meteorology. Here, we describe how the GEOS-Chem chemical-transport model may now be driven by meteorology archived from a state-of-the-art general circulation model for past and future climates, allowing it to be used to explore the impact of climate change on air pollution and atmospheric composition.
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 %.
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.
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.
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.
Jun Meng, Randall V. Martin, Paul Ginoux, Melanie Hammer, Melissa P. Sulprizio, David A. Ridley, and Aaron van Donkelaar
Geosci. Model Dev., 14, 4249–4260, https://doi.org/10.5194/gmd-14-4249-2021, https://doi.org/10.5194/gmd-14-4249-2021, 2021
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Dust emissions in models, for example, GEOS-Chem, have a strong nonlinear dependence on meteorology, which means dust emission strengths calculated from different resolution meteorological fields are different. Offline high-resolution dust emissions with an optimized global dust strength, presented in this work, can be implemented into GEOS-Chem as offline emission inventory so that it could promote model development by harmonizing dust emissions across simulations of different resolutions.
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.
Astrid Müller, Hiroshi Tanimoto, Takafumi Sugita, Toshinobu Machida, Shin-ichiro Nakaoka, Prabir K. Patra, Joshua Laughner, and David Crisp
Atmos. Chem. Phys., 21, 8255–8271, https://doi.org/10.5194/acp-21-8255-2021, https://doi.org/10.5194/acp-21-8255-2021, 2021
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Over oceans, high uncertainties in satellite CO2 retrievals exist due to limited reference data. We combine commercial ship and aircraft observations and, with the aid of model calculations, obtain column-averaged mixing ratios of CO2 (XCO2) data over the Pacific Ocean. This new dataset has great potential as a robust reference for XCO2 measured from space and can help to better understand changes in the carbon cycle in response to climate change using satellite observations.
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.
Sébastien Roche, Kimberly Strong, Debra Wunch, Joseph Mendonca, Colm Sweeney, Bianca Baier, Sébastien C. Biraud, Joshua L. Laughner, Geoffrey C. Toon, and Brian J. Connor
Atmos. Meas. Tech., 14, 3087–3118, https://doi.org/10.5194/amt-14-3087-2021, https://doi.org/10.5194/amt-14-3087-2021, 2021
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We evaluate CO2 profile retrievals from ground-based near-infrared solar absorption spectra after implementing several improvements to the GFIT2 retrieval algorithm. Realistic errors in the a priori temperature profile (~ 2 °C in the lower troposphere) are found to be the leading source of differences between the retrieved and true CO2 profiles, differences that are larger than typical CO2 variability. A temperature retrieval or correction is critical to improve CO2 profile retrieval results.
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.
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.
Junjie Liu, Latha Baskaran, Kevin Bowman, David Schimel, A. Anthony Bloom, Nicholas C. Parazoo, Tomohiro Oda, Dustin Carroll, Dimitris Menemenlis, Joanna Joiner, Roisin Commane, Bruce Daube, Lucianna V. Gatti, Kathryn McKain, John Miller, Britton B. Stephens, Colm Sweeney, and Steven Wofsy
Earth Syst. Sci. Data, 13, 299–330, https://doi.org/10.5194/essd-13-299-2021, https://doi.org/10.5194/essd-13-299-2021, 2021
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On average, the terrestrial biosphere carbon sink is equivalent to ~ 20 % of fossil fuel emissions. Understanding where and why the terrestrial biosphere absorbs carbon from the atmosphere is pivotal to any mitigation policy. Here we present a regionally resolved satellite-constrained net biosphere exchange (NBE) dataset with corresponding uncertainties between 2010–2018: CMS-Flux NBE 2020. The dataset provides a unique perspective on monitoring regional contributions to the CO2 growth rate.
Bo Zhang, Hongyu Liu, James H. Crawford, Gao Chen, T. Duncan Fairlie, Scott Chambers, Chang-Hee Kang, Alastair G. Williams, Kai Zhang, David B. Considine, Melissa P. Sulprizio, and Robert M. Yantosca
Atmos. Chem. Phys., 21, 1861–1887, https://doi.org/10.5194/acp-21-1861-2021, https://doi.org/10.5194/acp-21-1861-2021, 2021
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We simulate atmospheric 222Rn using the GEOS-Chem model to improve understanding of 222Rn emissions and characterize convective transport in the model. We demonstrate the potential of a customized global 222Rn emission scenario to improve simulated surface 222Rn concentrations and seasonality. We assess convective transport using observed 222Rn vertical profiles. Results have important implications for using chemical transport models to interpret the transport of trace gases and aerosols.
Nick Gorkavyi, Zachary Fasnacht, David Haffner, Sergey Marchenko, Joanna Joiner, and Alexander Vasilkov
Atmos. Meas. Tech., 14, 961–974, https://doi.org/10.5194/amt-14-961-2021, https://doi.org/10.5194/amt-14-961-2021, 2021
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Various instrumental or geophysical artifacts, such as saturation, stray light or obstruction of light, negatively impact satellite measured ultraviolet and visible Earthshine radiance spectra. Here, we introduce a straightforward detection method that is based on the correlation, r, between the observed Earthshine radiance and solar irradiance spectra over a 10 nm spectral range; our decorrelation index (DI for brevity) is simply defined as DI of 1–r.
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.
Yang Li, Loretta J. Mickley, and Jed O. Kaplan
Atmos. Chem. Phys., 21, 57–68, https://doi.org/10.5194/acp-21-57-2021, https://doi.org/10.5194/acp-21-57-2021, 2021
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Climate models predict a shift toward warmer, drier environments in southwestern North America. Under future climate, the two main drivers of dust trends play opposing roles: (1) CO2 fertilization enhances vegetation and, in turn, decreases dust, and (2) increasing land use enhances dust emissions from northern Mexico. In the worst-case scenario, elevated dust concentrations spread widely over the domain by 2100 in spring, suggesting a large climate penalty on air quality and human health.
Erin E. McDuffie, Steven J. Smith, Patrick O'Rourke, Kushal Tibrewal, Chandra Venkataraman, Eloise A. Marais, Bo Zheng, Monica Crippa, Michael Brauer, and Randall V. Martin
Earth Syst. Sci. Data, 12, 3413–3442, https://doi.org/10.5194/essd-12-3413-2020, https://doi.org/10.5194/essd-12-3413-2020, 2020
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Global emission inventories are vital to understanding the impacts of air pollution on the environment, human health, and society. We update the open-source Community Emissions Data System (CEDS) to provide global gridded emissions of seven key air pollutants from 1970–2017 for 11 source sectors and multiple fuel types, including coal, solid biofuel, and liquid oil and natural gas. This dataset includes both monthly global gridded emissions and annual national totals.
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.
Can Li, Nickolay A. Krotkov, Peter J. T. Leonard, Simon Carn, Joanna Joiner, Robert J. D. Spurr, and Alexander Vasilkov
Atmos. Meas. Tech., 13, 6175–6191, https://doi.org/10.5194/amt-13-6175-2020, https://doi.org/10.5194/amt-13-6175-2020, 2020
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Sulfur dioxide (SO2) is an important pollutant that causes haze and acid rain. The Ozone Monitoring Instrument (OMI) has been providing global observation of SO2 from space for over 15 years. In this paper, we introduce a new OMI SO2 dataset for global pollution monitoring. The dataset better accounts for the influences of different factors such as location and sun and satellite angles, leading to improved data quality. The new OMI SO2 dataset is publicly available through NASA's data center.
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.
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.
Priyanka deSouza, Ralph A. Kahn, James A. Limbacher, Eloise A. Marais, Fábio Duarte, and Carlo Ratti
Atmos. Meas. Tech., 13, 5319–5334, https://doi.org/10.5194/amt-13-5319-2020, https://doi.org/10.5194/amt-13-5319-2020, 2020
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This paper presents a novel method to constrain the size distribution derived from low-cost optical particle counters (OPCs) using satellite data to develop higher-quality particulate matter (PM) estimates. Such estimates can enable cities that do not have access to expensive reference air quality monitors, especially those in the global south, to develop effective air quality management plans.
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.
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.
Yang Li, Loretta J. Mickley, Pengfei Liu, and Jed O. Kaplan
Atmos. Chem. Phys., 20, 8827–8838, https://doi.org/10.5194/acp-20-8827-2020, https://doi.org/10.5194/acp-20-8827-2020, 2020
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Using a coupled vegetation–fire–climate modeling framework, we show a northward shift in forests and increased lightning fire activity in northern US states, including Idaho, Montana, and Wyoming. Our findings suggest a large climate penalty on ecosystem, air quality, visibility, and human health in a region valued for its national forests and parks. The fine-scale smoke PM predictions provided in this study should prove useful to human health and environmental assessments.
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.
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.
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.
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
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.
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.
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.
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.
Zachary Fasnacht, Alexander Vasilkov, David Haffner, Wenhan Qin, Joanna Joiner, Nickolay Krotkov, Andrew M. Sayer, and Robert Spurr
Atmos. Meas. Tech., 12, 6749–6769, https://doi.org/10.5194/amt-12-6749-2019, https://doi.org/10.5194/amt-12-6749-2019, 2019
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The anisotropy of Earth's surface reflection plays an important role in satellite-based retrievals of cloud, aerosol, and trace gases. Most current ultraviolet and visible satellite retrievals utilize climatological surface reflectivity databases that do not account for surface anisotropy. The GLER concept was introduced to account for such features. Here we evaluate GLER for water surfaces by comparing with OMI measurements and show that it captures these surface anisotropy features.
Helen M. Worden, A. Anthony Bloom, John R. Worden, Zhe Jiang, Eloise A. Marais, Trissevgeni Stavrakou, Benjamin Gaubert, and Forrest Lacey
Atmos. Chem. Phys., 19, 13569–13579, https://doi.org/10.5194/acp-19-13569-2019, https://doi.org/10.5194/acp-19-13569-2019, 2019
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Biogenic non-methane volatile organic compounds (NMVOCs) emitted from vegetation play a significant role in air quality and climate. However, there are large uncertainties in their role for climate. We present a Bayesian approach to estimate carbon monoxide fluxes that are chemically produced from biogenic sources. This provides independent constraints on models that predict biogenic emissions in order improve their capability for predicting air quality and future climate scenarios.
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.
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.
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.
Wenhan Qin, Zachary Fasnacht, David Haffner, Alexander Vasilkov, Joanna Joiner, Nickolay Krotkov, Bradford Fisher, and Robert Spurr
Atmos. Meas. Tech., 12, 3997–4017, https://doi.org/10.5194/amt-12-3997-2019, https://doi.org/10.5194/amt-12-3997-2019, 2019
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Satellite observations depend on Sun and view angles due to anisotropy of the Earth's atmosphere and surface reflection. But most of the ultraviolet and visible cloud, aerosol, and trace-gas algorithms utilize surface reflectivity databases that do not account for surface anisotropy. We create a surface database using the GLER concept which adequately accounts for surface anisotropy, validate it with independent satellite data, and provide a simple implementation to the current algorithms.
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.
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.
Yuekui Yang, Kerry Meyer, Galina Wind, Yaping Zhou, Alexander Marshak, Steven Platnick, Qilong Min, Anthony B. Davis, Joanna Joiner, Alexander Vasilkov, David Duda, and Wenying Su
Atmos. Meas. Tech., 12, 2019–2031, https://doi.org/10.5194/amt-12-2019-2019, https://doi.org/10.5194/amt-12-2019-2019, 2019
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The physical basis of the EPIC cloud product algorithms and an initial evaluation of their performance are presented. EPIC cloud products include cloud mask, effective height, and optical depth. Comparison with co-located retrievals from geosynchronous earth orbit (GEO) and low earth orbit (LEO) satellites shows that the algorithms are performing well and are consistent with theoretical expectations. These products are publicly available at the NASA Langley Atmospheric Sciences Data Center.
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.
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.
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.
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).
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.
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.
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.
Fei Liu, Sungyeon Choi, Can Li, Vitali E. Fioletov, Chris A. McLinden, Joanna Joiner, Nickolay A. Krotkov, Huisheng Bian, Greet Janssens-Maenhout, Anton S. Darmenov, and Arlindo M. da Silva
Atmos. Chem. Phys., 18, 16571–16586, https://doi.org/10.5194/acp-18-16571-2018, https://doi.org/10.5194/acp-18-16571-2018, 2018
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Sulfur dioxide measurements from space have been used to detect emissions from large sources. We developed a new emission inventory by combining the satellite-based emission estimates and the conventional bottom-up inventory for smaller sources. The new inventory improves the model agreement with in situ observations and offers the possibility of rapid updates to emissions.
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.
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.
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.
Yao Zhang, Joanna Joiner, Seyed Hamed Alemohammad, Sha Zhou, and Pierre Gentine
Biogeosciences, 15, 5779–5800, https://doi.org/10.5194/bg-15-5779-2018, https://doi.org/10.5194/bg-15-5779-2018, 2018
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Using satellite reflectance measurements and a machine learning algorithm, we generated a new solar-induced chlorophyll fluorescence (SIF) dataset that is closely linked to plant photosynthesis. This new dataset has higher spatial and temporal resolutions, and lower uncertainty compared to the existing satellite retrievals. We also demonstrated its application in monitoring drought and improving the understanding of the SIF–photosynthesis relationship.
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.
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.
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.
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.
Alexander Vasilkov, Eun-Su Yang, Sergey Marchenko, Wenhan Qin, Lok Lamsal, Joanna Joiner, Nickolay Krotkov, David Haffner, Pawan K. Bhartia, and Robert Spurr
Atmos. Meas. Tech., 11, 4093–4107, https://doi.org/10.5194/amt-11-4093-2018, https://doi.org/10.5194/amt-11-4093-2018, 2018
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We discuss a new cloud algorithm that retrieves effective cloud fraction and cloud altitude and pressure from the oxygen dimer absorption band at 477 nm. The algorithm accounts for how changes in the sun–satellite geometry affect the surface reflection. The cloud fraction and pressure are used as inputs to the OMI algorithm that retrieves a pollutant gas called nitrogen dioxide. Impacts of the application of the newly developed cloud algorithm on the OMI nitrogen dioxide retrieval are discussed.
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.
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.
Danny M. Leung, Amos P. K. Tai, Loretta J. Mickley, Jonathan M. Moch, Aaron van Donkelaar, Lu Shen, and Randall V. Martin
Atmos. Chem. Phys., 18, 6733–6748, https://doi.org/10.5194/acp-18-6733-2018, https://doi.org/10.5194/acp-18-6733-2018, 2018
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This paper investigates how large-scale weather systems control fine particulate matter (PM2.5) air quality in China. We show that winter monsoons, onshore winds and frontal rains can drive daily PM2.5 variability in different regions of China. We further project future PM2.5 concentration change by 2050s due to climate change, and verify that climate change has little benefit on future PM2.5 in Beijing, implying cutting down emissions is necessary to mitigate pollutions in megacities of China.
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.
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.
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.
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.
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.
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.
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.
Daniel H. Cusworth, Loretta J. Mickley, Eric M. Leibensperger, and Michael J. Iacono
Atmos. Chem. Phys., 17, 13559–13572, https://doi.org/10.5194/acp-17-13559-2017, https://doi.org/10.5194/acp-17-13559-2017, 2017
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Since 1990, light-scattering pollution known as aerosols have declined as a result of tightening US air quality regulations. Our study finds that US surface solar radiation has increased simultaneously. We establish a link between aerosols and radiation through physical and statistical models. We find the strongest relationship between aerosols, radiation, and climate at a site in the Midwest. Our work underscores the importance of regional pollution on climate in the US and abroad.
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.
Vitali Fioletov, Chris A. McLinden, Shailesh K. Kharol, Nickolay A. Krotkov, Can Li, Joanna Joiner, Michael D. Moran, Robert Vet, Antoon J. H. Visschedijk, and Hugo A. C. Denier van der Gon
Atmos. Chem. Phys., 17, 12597–12616, https://doi.org/10.5194/acp-17-12597-2017, https://doi.org/10.5194/acp-17-12597-2017, 2017
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.
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.
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.
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.
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.
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.
Yan Zhang, Can Li, Nickolay A. Krotkov, Joanna Joiner, Vitali Fioletov, and Chris McLinden
Atmos. Meas. Tech., 10, 1495–1509, https://doi.org/10.5194/amt-10-1495-2017, https://doi.org/10.5194/amt-10-1495-2017, 2017
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In this study, we demonstrate a very good consistency of the SO2 retrievals from OMI and OMPS using our state-of-the-art principal component analysis technique. Four full years of OMI and OMPS SO2 retrievals, during 2012–2015 have been analyzed over some of the world’s most polluted regions: eastern China, Mexico, and South Africa. The consistency of retrievals between OMI and OMPS make it possible to continue the long-term global SO2 pollution monitoring.
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.
Lu Shen, Loretta J. Mickley, and Lee T. Murray
Atmos. Chem. Phys., 17, 4355–4367, https://doi.org/10.5194/acp-17-4355-2017, https://doi.org/10.5194/acp-17-4355-2017, 2017
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We introduce a new method to characterize the influence of atmospheric circulation on surface PM2.5 concentrations. Applying our statistical model to climate projections, we find a strong influence of 2000–2050 climate change on PM2.5 air quality in the United States. We find that current atmospheric chemistry models may underestimate the strong positive sensitivity of PM2.5 to temperature in the eastern United States in summer, and so may underestimate PM2.5 changes in a warmer climate.
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.
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.
Can Li, Nickolay A. Krotkov, Simon Carn, Yan Zhang, Robert J. D. Spurr, and Joanna Joiner
Atmos. Meas. Tech., 10, 445–458, https://doi.org/10.5194/amt-10-445-2017, https://doi.org/10.5194/amt-10-445-2017, 2017
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In this paper, we describe the new-generation OMI volcanic SO2 algorithm based on our principal component analysis (PCA) retrieval technique. We demonstrate significant improvement in the our new OMI volcanic SO2 data, with the retrieval noise reduced by a factor of 2 as compared with the previous dataset. The algorithm also improves the accuracy for large volcanic eruptions. It is also capable of producing consistent retrievals between different instruments.
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.
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 %.
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.
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.
Glenn M. Wolfe, Margaret R. Marvin, Sandra J. Roberts, Katherine R. Travis, and Jin Liao
Geosci. Model Dev., 9, 3309–3319, https://doi.org/10.5194/gmd-9-3309-2016, https://doi.org/10.5194/gmd-9-3309-2016, 2016
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The Framework for 0-D Atmospheric Modeling (F0AM) is a new, user-friendly platform for simulation of atmospheric chemistry systems. It incorporates a suite of commonly used mechanisms and is adaptable to photochemical chambers, Lagrangian plumes, and steady-state or time-varying diurnal cycles. We provide a detailed model description, demonstrate several common applications, and highlight some of the advantages and challenges of the 0-D box modeling approach.
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.
Vitali E. Fioletov, Chris A. McLinden, Nickolay Krotkov, Can Li, Joanna Joiner, Nicolas Theys, Simon Carn, and Mike D. Moran
Atmos. Chem. Phys., 16, 11497–11519, https://doi.org/10.5194/acp-16-11497-2016, https://doi.org/10.5194/acp-16-11497-2016, 2016
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We introduce the first space-based catalogue of SO2 emission sources seen by OMI. The inventory contains about 500 sources. They account for about a half of all SO2 emissions; the remaining half is likely related to sources emitting less than 30 kt yr−1 and not detected by OMI. The sources are grouped by type (volcanoes, power plants, oil- and gas-related sources, and smelters) and country. The catalogue presented herein can be used for verification of available SO2 emission inventories.
Joanna Joiner, Yasuko Yoshida, Luis Guanter, and Elizabeth M. Middleton
Atmos. Meas. Tech., 9, 3939–3967, https://doi.org/10.5194/amt-9-3939-2016, https://doi.org/10.5194/amt-9-3939-2016, 2016
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We examine new ways to use existing satellite instruments to retrieve red solar-induced fluorescence (SIF) over land and ocean. Our 8-year record of red SIF observations over land with the Global Ozone Monitoring Instrument 2 (GOME-2) shows for the first time reductions in response to drought. High-quality ocean fluorescence can also be derived with GOME-2 and similar instruments by utilizing their rich measurements of different colors.
Pawan Gupta, Joanna Joiner, Alexander Vasilkov, and Pawan K. Bhartia
Atmos. Meas. Tech., 9, 2813–2826, https://doi.org/10.5194/amt-9-2813-2016, https://doi.org/10.5194/amt-9-2813-2016, 2016
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The A-train constellation of satellites provides a unique opportunity to analyze near-simultaneous data from several of these sensors. In this paper, retrievals of cloud/aerosols parameters and total column ozone (TCO) from the Aura Ozone Monitoring Instrument (OMI) have been used to develop a variety of neural networks that estimate TOA SWF globally over ocean and land using only OMI data as inputs. Application of our method to other ultraviolet sensors may provide unique estimates of TOA SWF.
Jinfeng Chang, Philippe Ciais, Mario Herrero, Petr Havlik, Matteo Campioli, Xianzhou Zhang, Yongfei Bai, Nicolas Viovy, Joanna Joiner, Xuhui Wang, Shushi Peng, Chao Yue, Shilong Piao, Tao Wang, Didier A. Hauglustaine, Jean-Francois Soussana, Anna Peregon, Natalya Kosykh, and Nina Mironycheva-Tokareva
Biogeosciences, 13, 3757–3776, https://doi.org/10.5194/bg-13-3757-2016, https://doi.org/10.5194/bg-13-3757-2016, 2016
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We derived the global maps of grassland management intensity of 1901–2012, including the minimum area of managed grassland with fraction of mown/grazed part. These maps, to our knowledge for the first time, provide global, time-dependent information for drawing up global estimates of management impact on biomass production and yields and for global vegetation models to enable simulations of carbon stocks and GHG budgets beyond simple tuning of grassland productivities to account for management.
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.
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.
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.
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.
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
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.
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.
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.
L. Shen, L. J. Mickley, and A. P. K. Tai
Atmos. Chem. Phys., 15, 10925–10938, https://doi.org/10.5194/acp-15-10925-2015, https://doi.org/10.5194/acp-15-10925-2015, 2015
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In this study, we have examined the effect of polar jet and Bermuda High on ozone air quality in the eastern United States. In the Midwest and northeast, the poleward shift of jet wind leads to reduced polar jet frequency, resulting in increased ozone there. In the southeast, the influence of Bermuda High on ozone variability depends on the location of its west edge. Westward movement increases the ozone only when the JJA Bermuda High west edge is located west of 85.4°W.
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.
X. Yue, L. J. Mickley, J. A. Logan, R. C. Hudman, M. V. Martin, and R. M. Yantosca
Atmos. Chem. Phys., 15, 10033–10055, https://doi.org/10.5194/acp-15-10033-2015, https://doi.org/10.5194/acp-15-10033-2015, 2015
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Based on simulated meteorology from 13 GCMs, we projected future wildfire activity in Alaskan and Canadian ecoregions by the mid-century. The most robust change is the increase of 150-390% in area burned over Alaska and western Canada. The models also predict an increase of 45-90% in the central and southern Canadian ecoregions, but a decrease of up to 50% in northern Canada. We further quantify how the changes in wildfire emissions may affect ozone concentrations in North America.
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.
P. Achakulwisut, L. J. Mickley, L. T. Murray, A. P. K. Tai, J. O. Kaplan, and B. Alexander
Atmos. Chem. Phys., 15, 7977–7998, https://doi.org/10.5194/acp-15-7977-2015, https://doi.org/10.5194/acp-15-7977-2015, 2015
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The atmosphere’s oxidative capacity determines the lifetime of many trace gases important to climate, chemistry, and human health. Yet uncertainties remain about its past variations, its controlling factors, and the radiative forcing of short-lived species it influences. To reduce these uncertainties, we must better quantify the natural emissions and chemical reaction mechanisms of organic compounds in the atmosphere, which play a role in governing the oxidative capacity.
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
P. Köhler, L. Guanter, and J. Joiner
Atmos. Meas. Tech., 8, 2589–2608, https://doi.org/10.5194/amt-8-2589-2015, https://doi.org/10.5194/amt-8-2589-2015, 2015
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The paper presents recent developments for the retrieval of sun-induced fluorescence (SIF) from medium spectral resolution space-borne spectrometers such as the Global Ozone Monitoring Experiment (GOME-2) and the Scanning Imaging Absorption SpectroMeter for Atmospheric ChartographY (SCIAMACHY). Beside using simulated radiances to evaluate the retrieval performance, the method has also been used to estimate SIF at 740 nm using real spectra from GOME-2 and for the first time, from SCIAMACHY.
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.
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
L. Guanter, I. Aben, P. Tol, J. M. Krijger, A. Hollstein, P. Köhler, A. Damm, J. Joiner, C. Frankenberg, and J. Landgraf
Atmos. Meas. Tech., 8, 1337–1352, https://doi.org/10.5194/amt-8-1337-2015, https://doi.org/10.5194/amt-8-1337-2015, 2015
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This paper investigates the potential of the upcoming TROPOspheric Monitoring Instrument (TROPOMI) instrument for the retrieval of the chlorophyll fluorescence signal emitted in the 650–850nm spectral range by the photosynthetic machinery of green plants. We find that TROPOMI will allow substantial improvements in the space monitoring of fluorescence with respect to current spaceborne instruments such as GOME-2 and SCIAMACHY.
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.
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.
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
S. Choi, J. Joiner, Y. Choi, B. N. Duncan, A. Vasilkov, N. Krotkov, and E. Bucsela
Atmos. Chem. Phys., 14, 10565–10588, https://doi.org/10.5194/acp-14-10565-2014, https://doi.org/10.5194/acp-14-10565-2014, 2014
A. Vasilkov, J. Joiner, and C. Seftor
Atmos. Meas. Tech., 7, 2897–2906, https://doi.org/10.5194/amt-7-2897-2014, https://doi.org/10.5194/amt-7-2897-2014, 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
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
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
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
L. T. Murray, L. J. Mickley, J. O. Kaplan, E. D. Sofen, M. Pfeiffer, and B. Alexander
Atmos. Chem. Phys., 14, 3589–3622, https://doi.org/10.5194/acp-14-3589-2014, https://doi.org/10.5194/acp-14-3589-2014, 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
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. 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
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
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
J. Joiner, L. Guanter, R. Lindstrot, M. Voigt, A. P. Vasilkov, E. M. Middleton, K. F. Huemmrich, Y. Yoshida, and C. Frankenberg
Atmos. Meas. Tech., 6, 2803–2823, https://doi.org/10.5194/amt-6-2803-2013, https://doi.org/10.5194/amt-6-2803-2013, 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. 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
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
H. Jiang, H. Liao, H. O. T. Pye, S. Wu, L. J. Mickley, J. H. Seinfeld, and X. Y. Zhang
Atmos. Chem. Phys., 13, 7937–7960, https://doi.org/10.5194/acp-13-7937-2013, https://doi.org/10.5194/acp-13-7937-2013, 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
A. Vasilkov, J. Joiner, and R. Spurr
Atmos. Meas. Tech., 6, 981–990, https://doi.org/10.5194/amt-6-981-2013, https://doi.org/10.5194/amt-6-981-2013, 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)
CO anthropogenic emissions in Europe from 2011 to 2021: insights from Measurement of Pollution in the Troposphere (MOPITT) satellite data
Constraining long-term NOx emissions over the United States and Europe using nitrate wet deposition monitoring networks
Analysis of an intense O3 pollution episode on the Atlantic coast of the Iberian Peninsula using photochemical modeling: characterization of transport pathways and accumulation processes
Atmospheric oxygen as a tracer for fossil fuel carbon dioxide: a sensitivity study in the UK
MIXv2: a long-term mosaic emission inventory for Asia (2010–2017)
Organosulfate produced from consumption of SO3 speeds up sulfuric acid–dimethylamine atmospheric nucleation
Contribution of expanded marine sulfur chemistry to the seasonal variability of dimethyl sulfide oxidation products and size-resolved sulfate aerosol
Spatial disparities of ozone pollution in the Sichuan Basin spurred by extreme, hot weather
Global impacts of aviation on air quality evaluated at high resolution
Bias correction of OMI HCHO columns based on FTIR and aircraft measurements and impact on top-down emission estimates
Investigation of the renewed methane growth post-2007 with high-resolution 3-D variational inverse modeling and isotopic constraints
Revisiting day-of-week ozone patterns in an era of evolving US air quality
Air quality and radiative impacts of downward-propagating sudden stratospheric warmings (SSWs)
Estimation of the atmospheric hydroxyl radical oxidative capacity using multiple hydrofluorocarbons (HFCs)
Investigating the differences in calculating global mean surface CO2 abundance: the impact of analysis methodologies and site selection
Meteorological characteristics of extreme ozone pollution events in China and their future predictions
Evaluating modelled tropospheric columns of CH4, CO, and O3 in the Arctic using ground-based Fourier transform infrared (FTIR) measurements
The high-resolution Global Aviation emissions Inventory based on ADS-B (GAIA) for 2019–2021
Zonal variability of methane trends derived from satellite data
Weekly derived top-down volatile-organic-compound fluxes over Europe from TROPOMI HCHO data from 2018 to 2021
Technical note: Challenges of detecting free tropospheric ozone trends in a sparsely sampled environment
Current status of model predictions of volatile organic compounds and impacts on surface ozone predictions during summer in China
Utility of Geostationary Lightning Mapper-derived lightning NO emission estimates in air quality modeling studies
The suitability of atmospheric oxygen measurements to constrain western European fossil-fuel CO2 emissions and their trends
Future tropospheric ozone budget and distribution over east Asia under a net-zero scenario
Comprehensive multiphase chlorine chemistry in the box model CAABA/MECCA: implications for atmospheric oxidative capacity
Insights into soil NO emissions and the contribution to surface ozone formation in China
The impact of gaseous degradation on the equilibrium state of gas/particle partitioning of semi-volatile organic compounds
An intercomparison of satellite, airborne, and ground-level observations with WRF-CAMx simulations of NO2 columns over Houston, TX during the September 2021 TRACER-AQ campaign
Development, intercomparison, and evaluation of an improved mechanism for the oxidation of dimethyl sulfide in the UKCA model
A better representation of VOC chemistry in WRF-Chem and its impact on ozone over Los Angeles
Technical note: An assessment of the performance of statistical bias correction techniques for global chemistry-climate model surface ozone fields
The atmospheric oxidizing capacity in China – Part 1: Roles of different photochemical processes
Benefits of net-zero policies for future ozone pollution in China
Simulating impacts on UK air quality from net-zero forest planting scenarios
Understanding offshore high-ozone events during TRACER-AQ 2021 in Houston: insights from WRF–CAMx photochemical modeling
Opinion: Establishing a science-into-policy process for tropospheric ozone assessment
Atmospheric composition and climate impacts of a future hydrogen economy
Assessment of isoprene and near-surface ozone sensitivities to water stress over the Euro-Mediterranean region
The impact multi-decadal of changes in VOCs speciation on urban ozone chemistry: A case study in Birmingham, United Kingdom
Nighttime ozone in the lower boundary layer: insights from 3-year tower-based measurements in South China and regional air quality modeling
What controls ozone sensitivity in the upper tropical troposphere?
Summertime tropospheric ozone source apportionment study in Madrid (Spain)
Modelling the impacts of emission changes on O3 sensitivity, atmospheric oxidation capacity, and pollution transport over the Catalonia region
A regional modelling study of halogen chemistry within a volcanic plume of Mt Etna's Christmas 2018 eruption
Constraining the budget of atmospheric carbonyl sulfide using a 3-D chemical transport model
Atmospheric CO2 inversion reveals the Amazon as a minor carbon source caused by fire emissions, with forest uptake offsetting about half of these emissions
Rapid O3 assimilations – Part 2: Tropospheric O3 changes accompanied by declining NOx emissions in the USA and Europe in 2005–2020
High-resolution air quality simulations of ozone exceedance events during the Lake Michigan Ozone Study
Simulations of winter ozone in the Upper Green River basin, Wyoming, using WRF-Chem
Audrey Fortems-Cheiney, Gregoire Broquet, Elise Potier, Robin Plauchu, Antoine Berchet, Isabelle Pison, Hugo Denier van der Gon, and Stijn Dellaert
Atmos. Chem. Phys., 24, 4635–4649, https://doi.org/10.5194/acp-24-4635-2024, https://doi.org/10.5194/acp-24-4635-2024, 2024
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We have estimated the carbon monixide (CO) European emissions from satellite observations of the MOPITT instrument at the relatively high resolution of 0.5° for a period of over 10 years from 2011 to 2021. The analysis of the inversion results reveals the challenges associated with the inversion of CO emissions at the regional scale over Europe.
Amy Christiansen, Loretta J. Mickley, and Lu Hu
Atmos. Chem. Phys., 24, 4569–4589, https://doi.org/10.5194/acp-24-4569-2024, https://doi.org/10.5194/acp-24-4569-2024, 2024
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In this work, we provide an additional constraint on emissions and trends of nitrogen oxides using nitrate wet deposition (NWD) fluxes over the United States and Europe from 1980–2020. We find that NWD measurements constrain total NOx emissions well. We also find evidence of NOx emission overestimates in both domains, but especially over Europe, where NOx emissions are overestimated by a factor of 2. Reducing NOx emissions over Europe improves model representation of ozone at the surface.
Eduardo Torre-Pascual, Gotzon Gangoiti, Ana Rodríguez-García, Estibaliz Sáez de Cámara, Joana Ferreira, Carla Gama, María Carmen Gómez, Iñaki Zuazo, Jose Antonio García, and Maite de Blas
Atmos. Chem. Phys., 24, 4305–4329, https://doi.org/10.5194/acp-24-4305-2024, https://doi.org/10.5194/acp-24-4305-2024, 2024
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We present an analysis of an intense air pollution episode of tropospheric ozone (O3) along the Atlantic coast of the Iberian Peninsula, incorporating both measured and simulated parameters. Our study extends beyond surface-level factors to include altitude-related parameters. These episodes stem from upper-atmosphere O3 accumulation in preceding days, transported to surface layers, causing rapid O3 concentration increase.
Hannah Chawner, Eric Saboya, Karina E. Adcock, Tim Arnold, Yuri Artioli, Caroline Dylag, Grant L. Forster, Anita Ganesan, Heather Graven, Gennadi Lessin, Peter Levy, Ingrid T. Luijkx, Alistair Manning, Penelope A. Pickers, Chris Rennick, Christian Rödenbeck, and Matthew Rigby
Atmos. Chem. Phys., 24, 4231–4252, https://doi.org/10.5194/acp-24-4231-2024, https://doi.org/10.5194/acp-24-4231-2024, 2024
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The quantity of atmospheric potential oxygen (APO), derived from coincident measurements of carbon dioxide (CO2) and oxygen (O2), has been proposed as a tracer for fossil fuel CO2 emissions. In this model sensitivity study, we examine the use of APO for this purpose in the UK and compare our model to observations. We find that our model simulations are most sensitive to uncertainties relating to ocean fluxes and boundary conditions.
Meng Li, Junichi Kurokawa, Qiang Zhang, Jung-Hun Woo, Tazuko Morikawa, Satoru Chatani, Zifeng Lu, Yu Song, Guannan Geng, Hanwen Hu, Jinseok Kim, Owen R. Cooper, and Brian C. McDonald
Atmos. Chem. Phys., 24, 3925–3952, https://doi.org/10.5194/acp-24-3925-2024, https://doi.org/10.5194/acp-24-3925-2024, 2024
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In this work, we developed MIXv2, a mosaic Asian emission inventory for 2010–2017. With high spatial (0.1°) and monthly temporal resolution, MIXv2 integrates anthropogenic and open biomass burning emissions across seven sectors following a mosaic methodology. It provides CO2 emissions data alongside nine key pollutants and three chemical mechanisms. Our publicly accessible gridded monthly emissions data can facilitate long-term atmospheric and climate model analyses.
Xiaomeng Zhang, Yongjian Lian, Shendong Tan, and Shi Yin
Atmos. Chem. Phys., 24, 3593–3612, https://doi.org/10.5194/acp-24-3593-2024, https://doi.org/10.5194/acp-24-3593-2024, 2024
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Atmospheric new particle formation (NPF) has a significant influence on the global climate, local air quality and human health. Using a combination of quantum chemical calculations and kinetics modeling, we find that thhe gas-phase organosulfate produced from consumption of SO3 can significantly enhance SA–DMA nucleation in the polluted boundary layer, resulting in non-negligible contributions to NPF. Our findings provide important insights into organic sulfur in atmospheric aerosol formation.
Linia Tashmim, William C. Porter, Qianjie Chen, Becky Alexander, Charles H. Fite, Christopher D. Holmes, Jeffrey R. Pierce, Betty Croft, and Sakiko Ishino
Atmos. Chem. Phys., 24, 3379–3403, https://doi.org/10.5194/acp-24-3379-2024, https://doi.org/10.5194/acp-24-3379-2024, 2024
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Dimethyl sulfide (DMS) is mostly emitted from ocean surfaces and represents the largest natural source of sulfur for the atmosphere. Once in the atmosphere, DMS forms stable oxidation products such as SO2 and H2SO4, which can subsequently contribute to airborne particle formation and growth. In this study, we update the DMS oxidation mechanism in the chemical transport model GEOS-Chem and describe resulting changes in particle growth as well as the overall global sulfur budget.
Nan Wang, Yunsong Du, Dongyang Chen, Haiyan Meng, Xi Chen, Li Zhou, Guangming Shi, Yu Zhan, Miao Feng, Wei Li, Mulan Chen, Zhenliang Li, and Fumo Yang
Atmos. Chem. Phys., 24, 3029–3042, https://doi.org/10.5194/acp-24-3029-2024, https://doi.org/10.5194/acp-24-3029-2024, 2024
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In the scorching August 2022 heatwave, China's Sichuan Basin saw a stark contrast in ozone (O3) levels between Chengdu and Chongqing. The regional disparities were studied considering meteorology, precursors, photochemistry, and transportation. The study highlighted the importance of tailored pollution control measures and underlined the necessity for region-specific strategies to combat O3 pollution on a regional scale.
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.
Jean-François Müller, Trissevgeni Stavrakou, Glenn-Michael Oomen, Beata Opacka, Isabelle De Smedt, Alex Guenther, Corinne Vigouroux, Bavo Langerock, Carlos Augusto Bauer Aquino, Michel Grutter, James Hannigan, Frank Hase, Rigel Kivi, Erik Lutsch, Emmanuel Mahieu, Maria Makarova, Jean-Marc Metzger, Isamu Morino, Isao Murata, Tomoo Nagahama, Justus Notholt, Ivan Ortega, Mathias Palm, Amelie Röhling, Wolfgang Stremme, Kimberly Strong, Ralf Sussmann, Yao Té, and Alan Fried
Atmos. Chem. Phys., 24, 2207–2237, https://doi.org/10.5194/acp-24-2207-2024, https://doi.org/10.5194/acp-24-2207-2024, 2024
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Formaldehyde observations from satellites can be used to constrain the emissions of volatile organic compounds, but those observations have biases. Using an atmospheric model, aircraft and ground-based remote sensing data, we quantify these biases, propose a correction to the data, and assess the consequence of this correction for the evaluation of emissions.
Joël Thanwerdas, Marielle Saunois, Antoine Berchet, Isabelle Pison, and Philippe Bousquet
Atmos. Chem. Phys., 24, 2129–2167, https://doi.org/10.5194/acp-24-2129-2024, https://doi.org/10.5194/acp-24-2129-2024, 2024
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We investigate the causes of the renewed growth of atmospheric methane (CH4) after 2007 using inverse modeling. We use the additional information provided by observations of CH4 isotopic compositions to better differentiate between the emission categories. Accounting for the large uncertainties in source signatures, our results suggest that the post-2007 increase in atmospheric CH4 was caused by similar increases in emissions from (1) fossil fuels and (2) agriculture and waste.
Heather Simon, Christian Hogrefe, Andrew Whitehill, Kristen M. Foley, Jennifer Liljegren, Norm Possiel, Benjamin Wells, Barron H. Henderson, Lukas C. Valin, Gail Tonnesen, K. Wyat Appel, and Shannon Koplitz
Atmos. Chem. Phys., 24, 1855–1871, https://doi.org/10.5194/acp-24-1855-2024, https://doi.org/10.5194/acp-24-1855-2024, 2024
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We assess observed and modeled ozone weekend–weekday differences in the USA from 2002–2019. A subset of urban areas that were NOx-saturated at the beginning of the period transitioned to NOx-limited conditions. Multiple rural areas of California were NOx-limited for the entire period but become less influenced by local day-of-week emission patterns in more recent years. The model produces more NOx-saturated conditions than the observations but captures trends in weekend–weekday ozone patterns.
Ryan S. Williams, Michaela I. Hegglin, Patrick Jöckel, Hella Garny, and Keith P. Shine
Atmos. Chem. Phys., 24, 1389–1413, https://doi.org/10.5194/acp-24-1389-2024, https://doi.org/10.5194/acp-24-1389-2024, 2024
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During winter, a brief but abrupt reversal of the mean stratospheric westerly flow (~30 km high) around the Arctic occurs ~6 times a decade. Using a chemistry–climate model, about half of these events are shown to induce large anomalies in Arctic ozone (>25 %) and water vapour (>±25 %) around ~8–12 km altitude for up to 2–3 months, important for weather forecasting. We also calculate a doubling to trebling of the risk in breaches of mid-latitude surface air quality (ozone) standards (~60 ppbv).
Rona L. Thompson, Stephen A. Montzka, Martin K. Vollmer, Jgor Arduini, Molly Crotwell, Paul B. Krummel, Chris Lunder, Jens Mühle, Simon O'Doherty, Ronald G. Prinn, Stefan Reimann, Isaac Vimont, Hsiang Wang, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 24, 1415–1427, https://doi.org/10.5194/acp-24-1415-2024, https://doi.org/10.5194/acp-24-1415-2024, 2024
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The hydroxyl radical determines the atmospheric lifetimes of numerous species including methane. Since OH is very short-lived, it is not possible to directly measure its concentration on scales relevant for understanding its effect on other species. Here, OH is inferred by looking at changes in hydrofluorocarbons (HFCs). We find that OH levels have been fairly stable over our study period (2004 to 2021), suggesting that OH is not the main driver of the recent increase in atmospheric methane.
Zhendong Wu, Alex Vermeulen, Yousuke Sawa, Ute Karstens, Wouter Peters, Remco de Kok, Xin Lan, Yasuyuki Nagai, Akinori Ogi, and Oksana Tarasova
Atmos. Chem. Phys., 24, 1249–1264, https://doi.org/10.5194/acp-24-1249-2024, https://doi.org/10.5194/acp-24-1249-2024, 2024
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This study focuses on exploring the differences in calculating global surface CO2 and its growth rate, considering the impact of analysis methodologies and site selection. Our study reveals that the current global CO2 network has a good capacity to represent global surface CO2 and its growth rate, as well as trends in atmospheric CO2 mass changes. However, small differences exist in different analyses due to the impact of methodology and site selection.
Yang Yang, Yang Zhou, Hailong Wang, Mengyun Li, Huimin Li, Pinya Wang, Xu Yue, Ke Li, Jia Zhu, and Hong Liao
Atmos. Chem. Phys., 24, 1177–1191, https://doi.org/10.5194/acp-24-1177-2024, https://doi.org/10.5194/acp-24-1177-2024, 2024
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This study reveals that extreme ozone pollution over the North China Plain and Yangtze River Delta is due to the chemical production related to hot and dry conditions, and the regional transport explains the ozone pollution over the Sichuan Basin and Pearl River Delta. The frequency of meteorological conditions of the extreme ozone pollution increases from the past to the future. The sustainable scenario is the optimal path to retaining clean air in China in the future.
Victoria A. Flood, Kimberly Strong, Cynthia H. Whaley, Kaley A. Walker, Thomas Blumenstock, James W. Hannigan, Johan Mellqvist, Justus Notholt, Mathias Palm, Amelie N. Röhling, Stephen Arnold, Stephen Beagley, Rong-You Chien, Jesper Christensen, Makoto Deushi, Srdjan Dobricic, Xinyi Dong, Joshua S. Fu, Michael Gauss, Wanmin Gong, Joakim Langner, Kathy S. Law, Louis Marelle, Tatsuo Onishi, Naga Oshima, David A. Plummer, Luca Pozzoli, Jean-Christophe Raut, Manu A. Thomas, Svetlana Tsyro, and Steven Turnock
Atmos. Chem. Phys., 24, 1079–1118, https://doi.org/10.5194/acp-24-1079-2024, https://doi.org/10.5194/acp-24-1079-2024, 2024
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It is important to understand the composition of the Arctic atmosphere and how it is changing. Atmospheric models provide simulations that can inform policy. This study examines simulations of CH4, CO, and O3 by 11 models. Model performance is assessed by comparing results matched in space and time to measurements from five high-latitude ground-based infrared spectrometers. This work finds that models generally underpredict the concentrations of these gases in the Arctic troposphere.
Roger Teoh, Zebediah Engberg, Marc Shapiro, Lynnette Dray, and Marc E. J. Stettler
Atmos. Chem. Phys., 24, 725–744, https://doi.org/10.5194/acp-24-725-2024, https://doi.org/10.5194/acp-24-725-2024, 2024
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Emissions from aircraft contribute to climate change and degrade air quality. We describe an up-to-date 4D emissions inventory of global aviation from 2019 to 2021 based on actual flown trajectories. In 2019, 40.2 million flights collectively travelled 61 billion kilometres using 283 Tg of fuel. Long-haul flights were responsible for 43 % of CO2. The emissions inventory is made available for use in future studies to evaluate the negative externalities arising from global aviation.
Jonas Hachmeister, Oliver Schneising, Michael Buchwitz, John P. Burrows, Justus Notholt, and Matthias Buschmann
Atmos. Chem. Phys., 24, 577–595, https://doi.org/10.5194/acp-24-577-2024, https://doi.org/10.5194/acp-24-577-2024, 2024
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We quantified changes in atmospheric methane concentrations using satellite data and a dynamic linear model approach. We calculated global annual methane increases for the years 2019–2022, which are in good agreement with other sources. For zonal methane growth rates, we identified strong inter-hemispheric differences in 2019 and 2022. For 2022, we could attribute decreases in the global growth rate to the Northern Hemisphere, possibly related to a reduction in anthropogenic emissions.
Glenn-Michael Oomen, Jean-François Müller, Trissevgeni Stavrakou, Isabelle De Smedt, Thomas Blumenstock, Rigel Kivi, Maria Makarova, Mathias Palm, Amelie Röhling, Yao Té, Corinne Vigouroux, Martina M. Friedrich, Udo Frieß, François Hendrick, Alexis Merlaud, Ankie Piters, Andreas Richter, Michel Van Roozendael, and Thomas Wagner
Atmos. Chem. Phys., 24, 449–474, https://doi.org/10.5194/acp-24-449-2024, https://doi.org/10.5194/acp-24-449-2024, 2024
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Natural emissions from vegetation have a profound impact on air quality for their role in the formation of harmful tropospheric ozone and organic aerosols, yet these emissions are highly uncertain. In this study, we quantify emissions of organic gases over Europe using high-quality satellite measurements of formaldehyde. These satellite observations suggest that emissions from vegetation are much higher than predicted by models, especially in southern Europe.
Kai-Lan Chang, Owen R. Cooper, Audrey Gaudel, Irina Petropavlovskikh, Peter Effertz, Gary Morris, and Brian C. McDonald
EGUsphere, https://doi.org/10.5194/egusphere-2023-2739, https://doi.org/10.5194/egusphere-2023-2739, 2024
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The great majority of observational trend studies of free tropospheric ozone use sparsely sampled ozonesonde and aircraft measurements as reference datasets. 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 highlight the importance of maintaining adequate frequency and continuity of observations.
Yongliang She, Jingyi Li, Xiaopu Lyu, Hai Guo, Momei Qin, Xiaodong Xie, Kangjia Gong, Fei Ye, Jianjiong Mao, Lin Huang, and Jianlin Hu
Atmos. Chem. Phys., 24, 219–233, https://doi.org/10.5194/acp-24-219-2024, https://doi.org/10.5194/acp-24-219-2024, 2024
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In this study, we use multi-site volatile organic compound (VOC) measurements to evaluate the CMAQ-model-predicted VOCs and assess the impacts of VOC bias on O3 simulation. Our results demonstrate that current modeling setups and emission inventories are likely to underpredict VOC concentrations, and this underprediction of VOCs contributes to lower O3 predictions in China.
Peiyang Cheng, Arastoo Pour-Biazar, Yuling Wu, Shi Kuang, Richard T. McNider, and William J. Koshak
Atmos. Chem. Phys., 24, 41–63, https://doi.org/10.5194/acp-24-41-2024, https://doi.org/10.5194/acp-24-41-2024, 2024
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Lightning-induced nitrogen monoxide (LNO) emission can be estimated from geostationary satellite observations. The present study uses the LNO emission estimates derived from geostationary satellite observations in an air quality modeling system to investigate the impact of LNO on air quality. Results indicate that significant ozone increase could be due to long-distance chemical transport, lightning activity in the upwind direction, and the mixing of high LNO (or ozone) plumes.
Christian Rödenbeck, Karina E. Adcock, Markus Eritt, Maksym Gachkivskyi, Christoph Gerbig, Samuel Hammer, Armin Jordan, Ralph F. Keeling, Ingeborg Levin, Fabian Maier, Andrew C. Manning, Heiko Moossen, Saqr Munassar, Penelope A. Pickers, Michael Rothe, Yasunori Tohjima, and Sönke Zaehle
Atmos. Chem. Phys., 23, 15767–15782, https://doi.org/10.5194/acp-23-15767-2023, https://doi.org/10.5194/acp-23-15767-2023, 2023
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The carbon dioxide content of the Earth atmosphere is increasing due to human emissions from burning of fossil fuels, causing global climate change. The strength of the fossil-fuel emissions is estimated by inventories based on energy data, but independent validation of these inventories has been recommended by the Intergovernmental Panel on Climate Change. Here we investigate the potential to validate inventories based on measurements of small changes in the atmospheric oxygen content.
Xuewei Hou, Oliver Wild, Bin Zhu, and James Lee
Atmos. Chem. Phys., 23, 15395–15411, https://doi.org/10.5194/acp-23-15395-2023, https://doi.org/10.5194/acp-23-15395-2023, 2023
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In response to the climate crisis, many countries have committed to net zero in a certain future year. The impacts of net-zero scenarios on tropospheric O3 are less well studied and remain unclear. In this study, we quantified the changes of tropospheric O3 budgets, spatiotemporal distributions of future surface O3 in east Asia and regional O3 source contributions for 2060 under a net-zero scenario using the NCAR Community Earth System Model (CESM) and online O3-tagging methods.
Meghna Soni, Rolf Sander, Lokesh K. Sahu, Domenico Taraborrelli, Pengfei Liu, Ankit Patel, Imran A. Girach, Andrea Pozzer, Sachin S. Gunthe, and Narendra Ojha
Atmos. Chem. Phys., 23, 15165–15180, https://doi.org/10.5194/acp-23-15165-2023, https://doi.org/10.5194/acp-23-15165-2023, 2023
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The study presents the implementation of comprehensive multiphase chlorine chemistry in the box model CAABA/MECCA. Simulations for contrasting urban environments of Asia and Europe highlight the significant impacts of chlorine on atmospheric oxidation capacity and composition. Chemical processes governing the production and loss of chlorine-containing species has been discussed. The updated chemical mechanism will be useful to interpret field measurements and for future air quality studies.
Ling Huang, Jiong Fang, Jiaqiang Liao, Greg Yarwood, Hui Chen, Yangjun Wang, and Li Li
Atmos. Chem. Phys., 23, 14919–14932, https://doi.org/10.5194/acp-23-14919-2023, https://doi.org/10.5194/acp-23-14919-2023, 2023
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Surface ozone concentrations have emerged as a major environmental issue in China. Although control strategies aimed at reducing NOx emissions from conventional combustion sources are widely recognized, soil NOx emissions have received little attention. The impact of soil NO emissions on ground-level ozone concentration is yet to be evaluated. In this study, we estimated the soil NO emissions and evaluated its impact on ozone formation in China.
Fu-Jie Zhu, Zi-Feng Zhang, Li-Yan Liu, Pu-Fei Yang, Peng-Tuan Hu, Geng-Bo Ren, Meng Qin, and Wan-Li Ma
EGUsphere, https://doi.org/10.5194/egusphere-2023-2376, https://doi.org/10.5194/egusphere-2023-2376, 2023
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Gas/particle partitioning is an important atmospheric behavior for SVOCs. The observation of that the gaseous degradation could disrupt the equilibrium state of gas/particle partitioning of low molecular weight SVOCs, was demonstrated and evaluated by a steady-state model, with increasing gas/particle partitioning quotients about 1 to 8.4 times. The present study suggested the interplay between degradation and G/P partitioning of SVOCs.
M. Omar Nawaz, Jeremiah Johnson, Greg Yarwood, Benjamin de Foy, Laura M. Judd, and Daniel L. Goldberg
EGUsphere, https://doi.org/10.5194/egusphere-2023-2844, https://doi.org/10.5194/egusphere-2023-2844, 2023
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NO2 is a gas with implications for air pollution. An air campaign conducted in Houston provided an opportunity to compare NO2 from different instruments and a model. Observations from aircrafts and the TROPOMI satellite instrument agreed well with measurements on the ground, however the latter estimated lower values. We find that NO2 simulated in our model performed worse and find the worst performance in downtown Houston, suggesting that vehicle emissions of NO2 may be underestimated.
Ben A. Cala, Scott Archer-Nicholls, James Weber, N. Luke Abraham, Paul T. Griffiths, Lorrie Jacob, Y. Matthew Shin, Laura E. Revell, Matthew Woodhouse, and Alexander T. Archibald
Atmos. Chem. Phys., 23, 14735–14760, https://doi.org/10.5194/acp-23-14735-2023, https://doi.org/10.5194/acp-23-14735-2023, 2023
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Dimethyl sulfide (DMS) is an important trace gas emitted from the ocean recognised as setting the sulfate aerosol background, but its oxidation is complex. As a result representation in chemistry-climate models is greatly simplified. We develop and compare a new mechanism to existing mechanisms via a series of global and box model experiments. Our studies show our updated DMS scheme is a significant improvement but significant variance exists between mechanisms.
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, Andy Neuman, Patrick R. Veres, Jeff Peischl, Steven S. Brown, Allen H. Goldstein, Ronald C. Cohen, and Brian C. McDonald
EGUsphere, https://doi.org/10.5194/egusphere-2023-2742, https://doi.org/10.5194/egusphere-2023-2742, 2023
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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 represent VOCs 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.
Christoph Staehle, Harald E. Rieder, and Arlene M. Fiore
EGUsphere, https://doi.org/10.5194/egusphere-2023-2743, https://doi.org/10.5194/egusphere-2023-2743, 2023
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Chemistry-climate models show biases compared to surface ozone observations, and thus require bias-correction for impact studies and the assessment of air quality changes. We compare the performance of commonly used correction techniques for model outputs available via CMIP6. While all methods can reduce model biases, better results are obtained for more complex approaches. Thus, our study suggests broader use of these techniques in studies seeking to inform air quality management and policy.
Jianing Dai, Guy P. Brasseur, Mihalis Vrekoussis, Maria Kanakidou, Kun Qu, Yijuan Zhang, Hongliang Zhang, and Tao Wang
Atmos. Chem. Phys., 23, 14127–14158, https://doi.org/10.5194/acp-23-14127-2023, https://doi.org/10.5194/acp-23-14127-2023, 2023
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In this study, we used a regional chemical transport model to characterize the different parameters of atmospheric oxidative capacity in recent chemical environments in China. These parameters include the production and destruction rates of ozone and other oxidants, the ozone production efficiency, the OH reactivity, and the length of the reaction chain responsible for the formation of ozone and ROx. They are also affected by the aerosol burden in the atmosphere.
Zhenze Liu, Oliver Wild, Ruth M. Doherty, Fiona M. O'Connor, and Steven T. Turnock
Atmos. Chem. Phys., 23, 13755–13768, https://doi.org/10.5194/acp-23-13755-2023, https://doi.org/10.5194/acp-23-13755-2023, 2023
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We investigate the impact of net-zero policies on surface ozone pollution in China. A chemistry–climate model is used to simulate ozone changes driven by local and external emissions, methane, and warmer climates. A deep learning model is applied to generate more robust ozone projection, and we find that the benefits of net-zero policies may be overestimated with the chemistry–climate model. Nevertheless, it is clear that the policies can still substantially reduce ozone pollution in future.
Gemma Purser, Mathew R. Heal, Edward J. Carnell, Stephen Bathgate, Julia Drewer, James I. L. Morison, and Massimo Vieno
Atmos. Chem. Phys., 23, 13713–13733, https://doi.org/10.5194/acp-23-13713-2023, https://doi.org/10.5194/acp-23-13713-2023, 2023
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Forest expansion is a ″net-zero“ pathway, but change in land cover alters air quality in many ways. This study combines tree planting suitability data with UK measured emissions of biogenic volatile organic compounds to simulate spatial and temporal changes in atmospheric composition for planting scenarios of four species. Decreases in fine particulate matter are relatively larger than increases in ozone, which may indicate a net benefit of tree planting on human health aspects of air quality.
Wei Li, Yuxuan Wang, Xueying Liu, Ehsan Soleimanian, Travis Griggs, James Flynn, and Paul Walter
Atmos. Chem. Phys., 23, 13685–13699, https://doi.org/10.5194/acp-23-13685-2023, https://doi.org/10.5194/acp-23-13685-2023, 2023
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This study examined high offshore ozone events in Galveston Bay and the Gulf of Mexico, using boat data and WRF–CAMx modeling during the TRACER-AQ 2021 field campaign. On average, high ozone is caused by chemistry due to the regional transport of volatile organic compounds and downwind advection of NOx from the ship channel. Two case studies show advection of ozone can be another process leading to high ozone, and accurate wind prediction is crucial for air quality forecasting in coastal areas.
Richard G. Derwent, David D. Parrish, and Ian C. Faloona
Atmos. Chem. Phys., 23, 13613–13623, https://doi.org/10.5194/acp-23-13613-2023, https://doi.org/10.5194/acp-23-13613-2023, 2023
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Elevated tropospheric ozone concentrations driven by anthropogenic precursor emissions are a world-wide health and environmental concern; however, this issue lacks a generally accepted understanding of the scientific issues. Here, we briefly outline the elements required to conduct an international assessment process to establish a conceptual model of the underpinning science and motivate international policy forums for regulating ozone production over hemispheric and global scales.
Nicola J. Warwick, Alex T. Archibald, Paul T. Griffiths, James Keeble, Fiona M. O'Connor, John A. Pyle, and Keith P. Shine
Atmos. Chem. Phys., 23, 13451–13467, https://doi.org/10.5194/acp-23-13451-2023, https://doi.org/10.5194/acp-23-13451-2023, 2023
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A chemistry–climate model has been used to explore the atmospheric response to changes in emissions of hydrogen and other species associated with a shift from fossil fuel to hydrogen use. Leakage of hydrogen results in indirect global warming, offsetting greenhouse gas emission reductions from reduced fossil fuel use. To maximise the benefit of hydrogen as an energy source, hydrogen leakage and emissions of methane, carbon monoxide and nitrogen oxides should be minimised.
Susanna Strada, Andrea Pozzer, Graziano Giuliani, Erika Coppola, Fabien Solmon, Xiaoyan Jiang, Alex Guenther, Efstratios Bourtsoukidis, Dominique Serça, Jonathan Williams, and Filippo Giorgi
Atmos. Chem. Phys., 23, 13301–13327, https://doi.org/10.5194/acp-23-13301-2023, https://doi.org/10.5194/acp-23-13301-2023, 2023
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Water deficit modifies emissions of isoprene, an aromatic compound released by plants that influences the production of an air pollutant such as ozone. Numerical modelling shows that, during the warmest and driest summers, isoprene decreases between −20 and −60 % over the Euro-Mediterranean region, while near-surface ozone only diminishes by a few percent. Decreases in isoprene emissions not only happen under dry conditions, but also could occur after prolonged or repeated water deficits.
Jianghao Li, Alastair C. Lewis, Jim R. Hopkins, Stephen J. Andrews, Tim Murrells, Neil Passant, Ben Richmond, Siqi Hou, William Bloss, Roy Harrison, and Zongbo Shi
EGUsphere, https://doi.org/10.5194/egusphere-2023-2294, https://doi.org/10.5194/egusphere-2023-2294, 2023
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A summertime ozone event at an urban site in Birmingham is sensitive to volatile organic compound (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 to further reduce ozone in this case study, but the benefits maybe offset if solvent emission of VOCs were to continue to increase.
Guowen He, Cheng He, Haofan Wang, Xiao Lu, Chenglei Pei, Xiaonuan Qiu, Chenxi Liu, Yiming Wang, Nanxi Liu, Jinpu Zhang, Lei Lei, Yiming Liu, Haichao Wang, Tao Deng, Qi Fan, and Shaojia Fan
Atmos. Chem. Phys., 23, 13107–13124, https://doi.org/10.5194/acp-23-13107-2023, https://doi.org/10.5194/acp-23-13107-2023, 2023
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We analyze nighttime ozone in the lower boundary layer (up to 500 m) from the 2017–2019 measurements at the Canton Tower and the WRF-CMAQ model. We identify a strong ability of the residual layer to store daytime ozone in the convective mixing layer, investigate the chemical and meteorological factors controlling nighttime ozone in the residual layer, and quantify the contribution of nighttime ozone in the residual layer to both the nighttime and the following day’s surface ozone air quality.
Clara M. Nussbaumer, Horst Fischer, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 23, 12651–12669, https://doi.org/10.5194/acp-23-12651-2023, https://doi.org/10.5194/acp-23-12651-2023, 2023
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Ozone is a greenhouse gas and contributes to the earth’s radiative energy budget and therefore to global warming. This effect is the largest in the upper troposphere. In this study, we investigate the processes controlling ozone formation and the sensitivity to its precursors in the upper tropical troposphere based on model simulations by the ECHAM5/MESSy2 Atmospheric Chemistry (EMAC) model. We find that NO𝑥 emissions from lightning most importantly affect ozone chemistry at these altitudes.
David de la Paz, Rafael Borge, Juan Manuel de Andrés, Luis Miguel Tovar, Golam Sarwar, and Sergey L. Napelenok
EGUsphere, https://doi.org/10.5194/egusphere-2023-2056, https://doi.org/10.5194/egusphere-2023-2056, 2023
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This modelling study shows that around 70 % of ground-level ozone (O3) in Madrid (Spain) is transported from other regions. Nonetheless, local sources, mainly road traffic, play a significant role, specially under stagnation conditions associated to regional air recirculation. Our results suggest that local measures may be effective to reduce O3 peaks (potentially, up to 30 %) and thus, reduce impacts from high-O3 episodes in the Madrid metropolitan area.
Alba Badia, Veronica Vidal, Sergi Ventura, Roger Curcoll, Ricard Segura, and Gara Villalba
Atmos. Chem. Phys., 23, 10751–10774, https://doi.org/10.5194/acp-23-10751-2023, https://doi.org/10.5194/acp-23-10751-2023, 2023
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Improving air quality is a top priority in urban areas. In this study, we used an air quality model to analyse the air quality changes occurring over the metropolitan area of Barcelona and other rural areas affected by transport of the atmospheric plume from the city during mobility restrictions. Our results show that mitigation strategies intended to reduce O3 should be designed according to the local meteorology, air transport, and particular ozone chemistry of the urban area.
Herizo Narivelo, Paul David Hamer, Virginie Marécal, Luke Surl, Tjarda Roberts, Sophie Pelletier, Béatrice Josse, Jonathan Guth, Mickaël Bacles, Simon Warnach, Thomas Wagner, Stefano Corradini, Giuseppe Salerno, and Lorenzo Guerrieri
Atmos. Chem. Phys., 23, 10533–10561, https://doi.org/10.5194/acp-23-10533-2023, https://doi.org/10.5194/acp-23-10533-2023, 2023
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Volcanic emissions emit large quantities of gases and primary aerosols that can play an important role in atmospheric chemistry. We present a study of the fate of volcanic bromine emissions from the eruption of Mount Etna around Christmas 2018. Using a numerical model and satellite observations, we analyse the impact of the volcanic plume and how it modifies the composition of the air over the whole Mediterranean basin, in particular on tropospheric ozone through the bromine-explosion cycle.
Michael P. Cartwright, Richard J. Pope, Jeremy J. Harrison, Martyn P. Chipperfield, Chris Wilson, Wuhu Feng, David P. Moore, and Parvadha Suntharalingam
Atmos. Chem. Phys., 23, 10035–10056, https://doi.org/10.5194/acp-23-10035-2023, https://doi.org/10.5194/acp-23-10035-2023, 2023
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A 3-D chemical transport model, TOMCAT, is used to simulate global atmospheric carbonyl sulfide (OCS) distribution. Modelled OCS compares well with satellite observations of OCS from limb-sounding satellite observations. Model simulations also compare adequately with surface and atmospheric observations and suitably capture the seasonality of OCS and background concentrations.
Luana S. Basso, Chris Wilson, Martyn P. Chipperfield, Graciela Tejada, Henrique L. G. Cassol, Egídio Arai, Mathew Williams, T. Luke Smallman, Wouter Peters, Stijn Naus, John B. Miller, and Manuel Gloor
Atmos. Chem. Phys., 23, 9685–9723, https://doi.org/10.5194/acp-23-9685-2023, https://doi.org/10.5194/acp-23-9685-2023, 2023
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The Amazon’s carbon balance may have changed due to forest degradation, deforestation and warmer climate. We used an atmospheric model and atmospheric CO2 observations to quantify Amazonian carbon emissions (2010–2018). The region was a small carbon source to the atmosphere, mostly due to fire emissions. Forest uptake compensated for ~ 50 % of the fire emissions, meaning that the remaining forest is still a small carbon sink. We found no clear evidence of weakening carbon uptake over the period.
Rui Zhu, Zhaojun Tang, Xiaokang Chen, Xiong Liu, and Zhe Jiang
Atmos. Chem. Phys., 23, 9745–9763, https://doi.org/10.5194/acp-23-9745-2023, https://doi.org/10.5194/acp-23-9745-2023, 2023
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Ozone Monitoring Instrument (OMI) and surface O3 observations are used to investigate the changes in tropospheric O3 in the USA and Europe in 2005–2020. The surface-based assimilations show limited changes in surface and tropospheric column O3. The OMI-based assimilations show larger decreases in tropospheric O3 columns in 2010–2014, related to a decline in free-tropospheric NO2. Analysis suggests limited impacts of local emissions decline on tropospheric O3 over the USA and Europe in 2005–2020.
R. Bradley Pierce, Monica Harkey, Allen Lenzen, Lee M. Cronce, Jason A. Otkin, Jonathan L. Case, David S. Henderson, Zac Adelman, Tsengel Nergui, and Christopher R. Hain
Atmos. Chem. Phys., 23, 9613–9635, https://doi.org/10.5194/acp-23-9613-2023, https://doi.org/10.5194/acp-23-9613-2023, 2023
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We evaluate two high-resolution model simulations with different meteorological inputs but identical chemistry and anthropogenic emissions, with the goal of identifying a model configuration best suited for characterizing air quality in locations where lake breezes commonly affect local air quality along the Lake Michigan shoreline. This analysis complements other studies in evaluating the impact of meteorological inputs and parameterizations on air quality in a complex environment.
Shreta Ghimire, Zachary J. Lebo, Shane Murphy, Stefan Rahimi, and Trang Tran
Atmos. Chem. Phys., 23, 9413–9438, https://doi.org/10.5194/acp-23-9413-2023, https://doi.org/10.5194/acp-23-9413-2023, 2023
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High wintertime ozone levels have occurred often in recent years in mountain basins with oil and gas production facilities. Photochemical modeling of ozone production serves as a basis for understanding the mechanism by which it occurs and for predictive capability. We present photochemical model simulations of ozone formation and accumulation in the Upper Green River basin, Wyoming, demonstrating the model's ability to simulate wintertime ozone and the sensitivity of ozone to its precursors.
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Brioude, J., Angevine, W. M., Ahmadov, R., Kim, S.-W., Evan, S., McKeen, S. A., Hsie, E.-Y., Frost, G. J., Neuman, J. A., Pollack, I. B., Peischl, J., Ryerson, T. B., Holloway, J., Brown, S. S., Nowak, J. B., Roberts, J. M., Wofsy, S. C., Santoni, G. W., Oda, T., and Trainer, M.: Top-down estimate of surface flux in the Los Angeles Basin using a mesoscale inverse modeling technique: assessing anthropogenic emissions of CO, NOx and CO2 and their impacts, Atmos. Chem. Phys., 13, 3661–3677, https://doi.org/10.5194/acp-13-3661-2013, 2013.
Bucsela, E. J., Krotkov, N. A., Celarier, E. A., Lamsal, L. N., Swartz, W. H., Bhartia, P. K., Boersma, K. F., Veefkind, J. P., Gleason, J. F., and Pickering, K. E.: A new stratospheric and tropospheric NO2 retrieval algorithm for nadir-viewing satellite instruments: applications to OMI, Atmos. Meas. Tech., 6, 2607–2626, https://doi.org/10.5194/amt-6-2607-2013, 2013.
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Short summary
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.
The US EPA reports a steady decrease in nitrogen oxide (NOx) emissions from fuel combustion over...
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