Articles | Volume 23, issue 5
https://doi.org/10.5194/acp-23-3031-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-23-3031-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
07 Mar 2023
Research article |
| 07 Mar 2023
| 07 Mar 2023
Variable effects of spatial resolution on modeling of nitrogen oxides
Department of Energy, Environmental & Chemical Engineering, Washington University in St. Louis, St. Louis, MO, USA
Randall V. Martin
Department of Energy, Environmental & Chemical Engineering, Washington University in St. Louis, St. Louis, MO, USA
Ronald C. Cohen
Department of Chemistry, University of California, Berkeley, Berkeley, CA, USA
Department of Earth and Planetary Science, University of California, Berkeley, Berkeley, CA, USA
Liam Bindle
Department of Energy, Environmental & Chemical Engineering, Washington University in St. Louis, St. Louis, MO, USA
Dandan Zhang
Department of Energy, Environmental & Chemical Engineering, Washington University in St. Louis, St. Louis, MO, USA
Deepangsu Chatterjee
Department of Energy, Environmental & Chemical Engineering, Washington University in St. Louis, St. Louis, MO, USA
Hongjian Weng
Laboratory for Climate and Ocean-Atmosphere Studies, Department of Atmospheric and Oceanic Sciences, School of Physics, Peking University, Beijing, China
Jintai Lin
Laboratory for Climate and Ocean-Atmosphere Studies, Department of Atmospheric and Oceanic Sciences, School of Physics, Peking University, Beijing, China
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Yanshun Li, Randall V. Martin, Chi Li, Brian L. Boys, Aaron van Donkelaar, Jun Meng, and Jeffrey R. Pierce
Atmos. Chem. Phys., 23, 12525–12543, https://doi.org/10.5194/acp-23-12525-2023, https://doi.org/10.5194/acp-23-12525-2023, 2023
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We developed and evaluated processes affecting within-day (diel) variability in PM2.5 concentrations in a chemical transport model over the contiguous US. Diel variability in PM2.5 for the contiguous US is driven by early-morning accumulation into a shallow mixed layer, decreases from mid-morning through afternoon with mixed-layer growth, increases from mid-afternoon through evening as the mixed-layer collapses, and decreases overnight as emissions decrease.
Jun-Wei Xu, Jintai Lin, Dan Tong, and Lulu Chen
Atmos. Chem. Phys., 23, 10075–10089, https://doi.org/10.5194/acp-23-10075-2023, https://doi.org/10.5194/acp-23-10075-2023, 2023
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This study highlights the necessity of a low-carbon pathway in foreign countries for China to achieve air quality goals and to protect public health. We find that adopting the low-carbon instead of the fossil-fuel-intensive pathway in foreign countries would prevent 63 000–270 000 transboundary PM2.5-associated mortalities in China in 2060. Our study provides direct evidence of the necessity of inter-regional cooperation for air quality improvement.
Qindan Zhu, Bryan Place, Eva Y. Pfannerstill, Sha Tong, Huanxin Zhang, Jun Wang, Clara M. Nussbaumer, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Anthony Bucholtz, John H. Seinfeld, Allen H. Goldstein, and Ronald C. Cohen
Atmos. Chem. Phys., 23, 9669–9683, https://doi.org/10.5194/acp-23-9669-2023, https://doi.org/10.5194/acp-23-9669-2023, 2023
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Haihui Zhu, Randall V. Martin, Betty Croft, Shixian Zhai, Chi Li, Liam Bindle, Jeffrey R. Pierce, Rachel Y.-W. Chang, Bruce E. Anderson, Luke D. Ziemba, Johnathan W. Hair, Richard A. Ferrare, Chris A. Hostetler, Inderjeet Singh, Deepangsu Chatterjee, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jack E. Dibb, Joshua S. Schwarz, and Andrew Weinheimer
Atmos. Chem. Phys., 23, 5023–5042, https://doi.org/10.5194/acp-23-5023-2023, https://doi.org/10.5194/acp-23-5023-2023, 2023
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Jun-Wei Xu, Jintai Lin, Gan Luo, Jamiu Adeniran, and Hao Kong
Atmos. Chem. Phys., 23, 4149–4163, https://doi.org/10.5194/acp-23-4149-2023, https://doi.org/10.5194/acp-23-4149-2023, 2023
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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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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.
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.
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 %.
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.
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.
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.
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.
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.
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.
Yingying Yan, Yue Zhou, Shaofei Kong, Jintai Lin, Jian Wu, Huang Zheng, Zexuan Zhang, Aili Song, Yongqing Bai, Zhang Ling, Dantong Liu, and Tianliang Zhao
Atmos. Chem. Phys., 21, 3143–3162, https://doi.org/10.5194/acp-21-3143-2021, https://doi.org/10.5194/acp-21-3143-2021, 2021
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We analyze the effectiveness of emission reduction for local and upwind regions during winter haze episodes controlled by the main potential synoptic patterns over central China, a regional pollutant transport hub with sub-basin topography. Our results provide an opportunity to effectively mitigate haze pollution via local emission control actions in coordination with regional collaborative actions according to different synoptic patterns.
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.
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.
Mengyao Liu, Jintai Lin, Hao Kong, K. Folkert Boersma, Henk Eskes, Yugo Kanaya, Qin He, Xin Tian, Kai Qin, Pinhua Xie, Robert Spurr, Ruijing Ni, Yingying Yan, Hongjian Weng, and Jingxu Wang
Atmos. Meas. Tech., 13, 4247–4259, https://doi.org/10.5194/amt-13-4247-2020, https://doi.org/10.5194/amt-13-4247-2020, 2020
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Nitrogen oxides (NOx = NO + NO2) are important air pollutants in the troposphere and play crucial roles in the formation of ozone and particulate matter. The recently launched TROPOspheric Monitoring Instrument (TROPOMI) provides an opportunity to retrieve tropospheric concentrations of nitrogen dioxide (NO2) at an unprecedented high horizontal resolution. This work presents a new NO2 retrieval product over East Asia and further quantifies key factors affecting the retrieval, including aerosol.
Matthew J. Cooper, Randall V. Martin, Daven K. Henze, and Dylan B. A. Jones
Atmos. Chem. Phys., 20, 7231–7241, https://doi.org/10.5194/acp-20-7231-2020, https://doi.org/10.5194/acp-20-7231-2020, 2020
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Comparisons between satellite-retrieved and model-simulated NO2 columns are affected by differences between the model vertical profile and the assumed profile used in the retrieval process. We examine how such differences impact NOx emission estimates from satellite observations. Larger differences between the simulated and assumed profile shape correspond to larger emission errors. This reveals the importance of using consistent profile information when comparing satellite columns to models.
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
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.
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.
Hao Kong, Jintai Lin, Ruixiong Zhang, Mengyao Liu, Hongjian Weng, Ruijing Ni, Lulu Chen, Jingxu Wang, Yingying Yan, and Qiang Zhang
Atmos. Chem. Phys., 19, 12835–12856, https://doi.org/10.5194/acp-19-12835-2019, https://doi.org/10.5194/acp-19-12835-2019, 2019
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We develop a computationally efficient space-based top-down method to inverting NOx emissions in major urban areas at high resolution. The inversion method uses long-term OMI NO2 data to enhance the horizontal resolution, and it accounts for the nonlinear effects of horizontal transport, chemical loss, and deposition on NOx. The inversion results reveal fine-scale spatial information of emissions which is hardly captured by bottom-up inventories.
Rachel F. Silvern, Daniel J. Jacob, Loretta J. Mickley, Melissa P. Sulprizio, Katherine R. Travis, Eloise A. Marais, Ronald C. Cohen, Joshua L. Laughner, Sungyeon Choi, Joanna Joiner, and Lok N. Lamsal
Atmos. Chem. Phys., 19, 8863–8878, https://doi.org/10.5194/acp-19-8863-2019, https://doi.org/10.5194/acp-19-8863-2019, 2019
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The US EPA reports a steady decrease in nitrogen oxide (NOx) emissions from fuel combustion over the 2005–2017 period, while satellite observations show a leveling off after 2009, suggesting emission reductions and related air quality gains have halted. We show the sustained decrease in NOx emissions is in fact consistent with observed trends in surface NO2 and ozone concentrations and that the flattening of the satellite trend reflects a growing influence from the non-anthropogenic background.
Xiao Lu, Lin Zhang, Youfan Chen, Mi Zhou, Bo Zheng, Ke Li, Yiming Liu, Jintai Lin, Tzung-May Fu, and Qiang Zhang
Atmos. Chem. Phys., 19, 8339–8361, https://doi.org/10.5194/acp-19-8339-2019, https://doi.org/10.5194/acp-19-8339-2019, 2019
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Severe and deteriorating surface ozone pollution over major Chinese cities has become an emerging environmental concern in China. This study assesses the source contributions (including anthropogenic, background, and individual natural sources) and meteorological influences of surface ozone over China in 2016–2017 using the GEOS-Chem chemical transport model at high horizontal resolution with the most up-to-date Chinese anthropogenic emission inventory.
Jingyuan Shao, Qianjie Chen, Yuxuan Wang, Xiao Lu, Pengzhen He, Yele Sun, Viral Shah, Randall V. Martin, Sajeev Philip, Shaojie Song, Yue Zhao, Zhouqing Xie, Lin Zhang, and Becky Alexander
Atmos. Chem. Phys., 19, 6107–6123, https://doi.org/10.5194/acp-19-6107-2019, https://doi.org/10.5194/acp-19-6107-2019, 2019
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Sulfate is a key species contributing to particle formation and growth during wintertime Chinese haze events. This study combines observations and modeling of oxygen isotope signatures in sulfate aerosol to investigate its formation mechanisms, with a focus on heterogeneous production on aerosol surface via H2O2, O3, and NO2 and trace metal catalyzed oxidation. Contributions from different formation pathways are presented.
Betty Croft, Randall V. Martin, W. Richard Leaitch, Julia Burkart, Rachel Y.-W. Chang, Douglas B. Collins, Patrick L. Hayes, Anna L. Hodshire, Lin Huang, John K. Kodros, Alexander Moravek, Emma L. Mungall, Jennifer G. Murphy, Sangeeta Sharma, Samantha Tremblay, Gregory R. Wentworth, Megan D. Willis, Jonathan P. D. Abbatt, and Jeffrey R. Pierce
Atmos. Chem. Phys., 19, 2787–2812, https://doi.org/10.5194/acp-19-2787-2019, https://doi.org/10.5194/acp-19-2787-2019, 2019
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Summertime Arctic atmospheric aerosols are strongly controlled by processes related to natural regional sources. We use a chemical transport model with size-resolved aerosol microphysics to interpret measurements made during summertime 2016 in the Canadian Arctic Archipelago. Our results explore the processes that control summertime aerosol size distributions and support a climate-relevant role for Arctic marine secondary organic aerosol formed from precursor vapors with Arctic marine sources.
Robyn N. C. Latimer and Randall V. Martin
Atmos. Chem. Phys., 19, 2635–2653, https://doi.org/10.5194/acp-19-2635-2019, https://doi.org/10.5194/acp-19-2635-2019, 2019
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Long-term aerosol measurements from the IMPROVE network were used to investigate the simulation of mass scattering efficiency in the GEOS-Chem chemical transport model. The simulation of mass scattering efficiency was developed to better represent observations by refining the representation of aerosol size and hygroscopicity. Simulated average mass scattering efficiency over North America increased by 16 %, with larger increases in northern regions and reductions in the southwest.
Jonathan P. D. Abbatt, W. Richard Leaitch, Amir A. Aliabadi, Allan K. Bertram, Jean-Pierre Blanchet, Aude Boivin-Rioux, Heiko Bozem, Julia Burkart, Rachel Y. W. Chang, Joannie Charette, Jai P. Chaubey, Robert J. Christensen, Ana Cirisan, Douglas B. Collins, Betty Croft, Joelle Dionne, Greg J. Evans, Christopher G. Fletcher, Martí Galí, Roya Ghahreman, Eric Girard, Wanmin Gong, Michel Gosselin, Margaux Gourdal, Sarah J. Hanna, Hakase Hayashida, Andreas B. Herber, Sareh Hesaraki, Peter Hoor, Lin Huang, Rachel Hussherr, Victoria E. Irish, Setigui A. Keita, John K. Kodros, Franziska Köllner, Felicia Kolonjari, Daniel Kunkel, Luis A. Ladino, Kathy Law, Maurice Levasseur, Quentin Libois, John Liggio, Martine Lizotte, Katrina M. Macdonald, Rashed Mahmood, Randall V. Martin, Ryan H. Mason, Lisa A. Miller, Alexander Moravek, Eric Mortenson, Emma L. Mungall, Jennifer G. Murphy, Maryam Namazi, Ann-Lise Norman, Norman T. O'Neill, Jeffrey R. Pierce, Lynn M. Russell, Johannes Schneider, Hannes Schulz, Sangeeta Sharma, Meng Si, Ralf M. Staebler, Nadja S. Steiner, Jennie L. Thomas, Knut von Salzen, Jeremy J. B. Wentzell, Megan D. Willis, Gregory R. Wentworth, Jun-Wei Xu, and Jacqueline D. Yakobi-Hancock
Atmos. Chem. Phys., 19, 2527–2560, https://doi.org/10.5194/acp-19-2527-2019, https://doi.org/10.5194/acp-19-2527-2019, 2019
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The Arctic is experiencing considerable environmental change with climate warming, illustrated by the dramatic decrease in sea-ice extent. It is important to understand both the natural and perturbed Arctic systems to gain a better understanding of how they will change in the future. This paper summarizes new insights into the relationships between Arctic aerosol particles and climate, as learned over the past five or so years by a large Canadian research consortium, NETCARE.
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.
Lei Sun, Likun Xue, Yuhang Wang, Longlei Li, Jintai Lin, Ruijing Ni, Yingying Yan, Lulu Chen, Juan Li, Qingzhu Zhang, and Wenxing Wang
Atmos. Chem. Phys., 19, 1455–1469, https://doi.org/10.5194/acp-19-1455-2019, https://doi.org/10.5194/acp-19-1455-2019, 2019
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We quantified the detailed impacts of meteorology and anthropogenic emissions on surface O3 increase in central eastern China between 2003 and 2015 using GEOS-Chem. The emission change plays a more important role than the meteorological change, while the regions with a larger O3 increase are more sensitive to meteorology. NMVOC emission change dominated the O3 increase in eastern CEC, while NOx emission change led to an O3 increase in western and central CEC and O3 decrease in urban areas.
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.
Yingying Yan, David Cabrera-Perez, Jintai Lin, Andrea Pozzer, Lu Hu, Dylan B. Millet, William C. Porter, and Jos Lelieveld
Geosci. Model Dev., 12, 111–130, https://doi.org/10.5194/gmd-12-111-2019, https://doi.org/10.5194/gmd-12-111-2019, 2019
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The GEOS-Chem model has been updated with the SAPRC-11 aromatics chemical mechanism to evaluate global and regional effects of aromatics on tropospheric oxidation capacity. Our results reveal relatively slight changes in ozone, hydroxyl radical, and nitrogen oxides on a global mean basis (1–4 %), although remarkable regional differences (5–20 %) exist near the source regions. Improved representation of aromatics is important to simulate the tropospheric oxidation.
Mengyao Liu, Jintai Lin, K. Folkert Boersma, Gaia Pinardi, Yang Wang, Julien Chimot, Thomas Wagner, Pinhua Xie, Henk Eskes, Michel Van Roozendael, François Hendrick, Pucai Wang, Ting Wang, Yingying Yan, Lulu Chen, and Ruijing Ni
Atmos. Meas. Tech., 12, 1–21, https://doi.org/10.5194/amt-12-1-2019, https://doi.org/10.5194/amt-12-1-2019, 2019
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China has become the world’s largest emitter of NOx, which mainly comes from vehicle exhaust, power plants, etc. However, there are no official ground-based measurements before 2013, so satellites have been widely used to monitor and analyze NOx pollution here. Aerosol is the key factor influencing the accuracy of the satellite NOx product. Our study provides a more accurate way to account for aerosol's influence compared to current widely used products.
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.
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.
Jeffrey A. Geddes, Randall V. Martin, Eric J. Bucsela, Chris A. McLinden, and Daniel J. M. Cunningham
Atmos. Meas. Tech., 11, 6271–6287, https://doi.org/10.5194/amt-11-6271-2018, https://doi.org/10.5194/amt-11-6271-2018, 2018
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This paper describes an approach for separating the stratospheric and tropospheric contributions in geostationary observations of nitrogen dioxide from the upcoming TEMPO instrument. We find minimal impact of the limited field of observation compared to previous low-Earth-observing systems with global coverage. We find that continued development of low-Earth-orbit retrievals will benefit geostationary data by providing important context outside the field of regard.
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.
William H. Brune, Xinrong Ren, Li Zhang, Jingqiu Mao, David O. Miller, Bruce E. Anderson, Donald R. Blake, Ronald C. Cohen, Glenn S. Diskin, Samuel R. Hall, Thomas F. Hanisco, L. Gregory Huey, Benjamin A. Nault, Jeff Peischl, Ilana Pollack, Thomas B. Ryerson, Taylor Shingler, Armin Sorooshian, Kirk Ullmann, Armin Wisthaler, and Paul J. Wooldridge
Atmos. Chem. Phys., 18, 14493–14510, https://doi.org/10.5194/acp-18-14493-2018, https://doi.org/10.5194/acp-18-14493-2018, 2018
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Thunderstorms pull in polluted air from near the ground, transport it up through clouds containing lightning, and deposit it at altitudes where airplanes fly. The resulting chemical mixture in this air reacts to form ozone and particles, which affect climate. In this study, aircraft observations of the reactive gases responsible for this chemistry generally agree with modeled values, even in ice clouds. Thus, atmospheric oxidation chemistry appears to be mostly understood for this environment.
Erin R. Delaria, Megan Vieira, Julie Cremieux, and Ronald C. Cohen
Atmos. Chem. Phys., 18, 14161–14173, https://doi.org/10.5194/acp-18-14161-2018, https://doi.org/10.5194/acp-18-14161-2018, 2018
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Observations of NOx exchange between the atmosphere and vegetation have been widely reported. However, the magnitude, direction, and mechanism of this atmosphere–biosphere exchange remain uncertain across different ecosystems. We use laboratory measurements to study the rates of NOx deposition to the leaves of a California oak tree species. We detect no evidence of NOx emission and find that NOx loss to oak leaves is substantial even at low NOx concentrations relevant to forested environments.
Alexis A. Shusterman, Jinsol Kim, Kaitlyn J. Lieschke, Catherine Newman, Paul J. Wooldridge, and Ronald C. Cohen
Atmos. Chem. Phys., 18, 13773–13785, https://doi.org/10.5194/acp-18-13773-2018, https://doi.org/10.5194/acp-18-13773-2018, 2018
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We describe the diversity and heterogeneity of urban CO2 levels observed using the BErkeley Atmospheric CO2 Observation Network, a distributed instrument of > 50 CO2 sensors stationed every ~ 2 km across the San Francisco Bay Area. We demonstrate that relatively simple mathematical techniques, applied to these observations, can be used to detect the small changes in highway CO2 emissions expected to result from upcoming fuel economy regulations, affirming the policy relevance of low-cost sensors.
Mengyao Liu, Jintai Lin, Yuchen Wang, Yang Sun, Bo Zheng, Jingyuan Shao, Lulu Chen, Yixuan Zheng, Jinxuan Chen, Tzung-May Fu, Yingying Yan, Qiang Zhang, and Zhaohua Wu
Atmos. Chem. Phys., 18, 12933–12952, https://doi.org/10.5194/acp-18-12933-2018, https://doi.org/10.5194/acp-18-12933-2018, 2018
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Eastern China is heavily polluted by NO2, PM2.5, and other air pollutants. Our study uses EOF–EEMD to analyze the spatiotemporal variability of ground-level NO2, PM2.5, and their associations with meteorological processes. Their regular diurnal cycles are mainly affected by human activities, while irregular day-to-day variations are dominated by weather processes representing synchronous variation or north–south opposing changes over Eastern China.
Ruijing Ni, Jintai Lin, Yingying Yan, and Weili Lin
Atmos. Chem. Phys., 18, 11447–11469, https://doi.org/10.5194/acp-18-11447-2018, https://doi.org/10.5194/acp-18-11447-2018, 2018
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By integrating several modeling methods, we find considerable contributions of foreign anthropogenic emissions to surface ozone over China (2–11 ppb). For anthropogenic ozone over China, the foreign contribution is 40–50 % below 2 km and 85 % in the upper troposphere. For total foreign anthropogenic ozone over China, the portion of transboundary ozone produced within foreign emission source regions is less than 50 %, with the rest produced by precursors transported out of those source regions.
Melanie S. Hammer, Randall V. Martin, Chi Li, Omar Torres, Max Manning, and Brian L. Boys
Atmos. Chem. Phys., 18, 8097–8112, https://doi.org/10.5194/acp-18-8097-2018, https://doi.org/10.5194/acp-18-8097-2018, 2018
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We apply a simulation of the Ultraviolet Aerosol Index (UVAI), a method of detecting aerosol absorption from satellite observations, to interpret UVAI values observed by the Ozone Monitoring Instrument (OMI) from 2005 to 2015 to understand global trends in aerosol composition. We find that global trends in the UVAI are largely explained by trends in absorption by mineral dust, absorption by brown carbon, and scattering by secondary inorganic aerosol.
Chandra Venkataraman, Michael Brauer, Kushal Tibrewal, Pankaj Sadavarte, Qiao Ma, Aaron Cohen, Sreelekha Chaliyakunnel, Joseph Frostad, Zbigniew Klimont, Randall V. Martin, Dylan B. Millet, Sajeev Philip, Katherine Walker, and Shuxiao Wang
Atmos. Chem. Phys., 18, 8017–8039, https://doi.org/10.5194/acp-18-8017-2018, https://doi.org/10.5194/acp-18-8017-2018, 2018
Matthew J. Cooper, Randall V. Martin, Alexei I. Lyapustin, and Chris A. McLinden
Atmos. Meas. Tech., 11, 2983–2994, https://doi.org/10.5194/amt-11-2983-2018, https://doi.org/10.5194/amt-11-2983-2018, 2018
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To accurately infer air pollutant concentrations from satellite observations, we must first know the reflectivity of the Earth’s surface. Using a model, we show that satellite observations are better able to observe NO2 near the surface if snow is present. However, knowing when snow is present is difficult due to its variability. We test seven existing snow cover data sets to assess their ability to inform future satellite observations and find that the IMS data set is best suited for this task.
Yingying Yan, Andrea Pozzer, Narendra Ojha, Jintai Lin, and Jos Lelieveld
Atmos. Chem. Phys., 18, 5589–5605, https://doi.org/10.5194/acp-18-5589-2018, https://doi.org/10.5194/acp-18-5589-2018, 2018
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Surface-based measurements from the EMEP network and EMAC model simulations are used to estimate the European surface ozone changes over 1995–2014. It shows a significantly decreasing trend in the 95th percentile ozone concentrations, while increasing in the 5th percentile ozone. Sensitivity simulations and statistical analysis show that a decrease in European anthropogenic emissions had contrasting effects on surface ozone trends between the 95th and 5th percentile levels.
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.
Meng Li, Zbigniew Klimont, Qiang Zhang, Randall V. Martin, Bo Zheng, Chris Heyes, Janusz Cofala, Yuxuan Zhang, and Kebin He
Atmos. Chem. Phys., 18, 3433–3456, https://doi.org/10.5194/acp-18-3433-2018, https://doi.org/10.5194/acp-18-3433-2018, 2018
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In this paper, we conducted a comprehensive evaluation of two widely used anthropogenic emission inventories over China, ECLIPSE and MIX, to explore the potential sources of uncertainties and find clues to improving emission inventories. We found that SO2 emission estimates are consistent between the two inventories (with 1 % differences), while NOx emissions in ECLIPSE's estimates are 16 % lower than those in MIX. Discrepancies at the sector and provincial levels are much higher.
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.
Yingying Yan, Jintai Lin, and Cenlin He
Atmos. Chem. Phys., 18, 1185–1202, https://doi.org/10.5194/acp-18-1185-2018, https://doi.org/10.5194/acp-18-1185-2018, 2018
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Examining observed and simulated ozone at about 1000 sites during 1990–2014, we find a clear diurnal cycle both in the magnitude of ozone trends and in the relative importance of climate variability versus anthropogenic emissions to ozone changes, which has policy implications to mitigate ozone at night and other non-peak hours.
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.
Hongyan Zhao, Xin Li, Qiang Zhang, Xujia Jiang, Jintai Lin, Glen P. Peters, Meng Li, Guannan Geng, Bo Zheng, Hong Huo, Lin Zhang, Haikun Wang, Steven J. Davis, and Kebin He
Atmos. Chem. Phys., 17, 10367–10381, https://doi.org/10.5194/acp-17-10367-2017, https://doi.org/10.5194/acp-17-10367-2017, 2017
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Effective and efficient control of air pollution relies upon an understanding of the pollution sources. We conduct an interdisciplinary study and find that 33 % of China’s PM2.5-related premature mortality in 2010 were caused by production emission in other regions; 56 % of the mortality was related to consumption in other regions. Multilateral and multi-stage cooperation under a regional sustainable development framework is in urgent need to mitigate air pollution and related health impacts.
Jeffrey A. Geddes and Randall V. Martin
Atmos. Chem. Phys., 17, 10071–10091, https://doi.org/10.5194/acp-17-10071-2017, https://doi.org/10.5194/acp-17-10071-2017, 2017
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We use observations of nitrogen dioxide columns from multiple satellite instruments with the help of a chemical transport model to constrain the global deposition of reactive nitrogen oxides (NOy) over the last 2 decades. NOy deposition decreased by up to 60 % in eastern North America, doubled in regions of East Asia, and declined by 20 % in parts of Western Europe. We also find changes in the export of NOy via atmospheric transport, with direct impacts on countries downwind of source regions.
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.
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.
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.
Guannan Geng, Qiang Zhang, Randall V. Martin, Jintai Lin, Hong Huo, Bo Zheng, Siwen Wang, and Kebin He
Atmos. Chem. Phys., 17, 4131–4145, https://doi.org/10.5194/acp-17-4131-2017, https://doi.org/10.5194/acp-17-4131-2017, 2017
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We investigated the impact of spatial proxies on the representation of gridded emissions by comparing six gridded NOx emission datasets over China developed from the same magnitude of emissions and different spatial proxies. GEOS-Chem-modeled NO2 columns from the six gridded emissions are compared with satellite-based columns from OMI. Results show that differences between modeled and satellite-based NO2 columns are sensitive to the spatial proxies used in the gridded emission inventories.
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.
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.
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 %.
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.
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.
Graydon Snider, Crystal L. Weagle, Kalaivani K. Murdymootoo, Amanda Ring, Yvonne Ritchie, Emily Stone, Ainsley Walsh, Clement Akoshile, Nguyen Xuan Anh, Rajasekhar Balasubramanian, Jeff Brook, Fatimah D. Qonitan, Jinlu Dong, Derek Griffith, Kebin He, Brent N. Holben, Ralph Kahn, Nofel Lagrosas, Puji Lestari, Zongwei Ma, Amit Misra, Leslie K. Norford, Eduardo J. Quel, Abdus Salam, Bret Schichtel, Lior Segev, Sachchida Tripathi, Chien Wang, Chao Yu, Qiang Zhang, Yuxuan Zhang, Michael Brauer, Aaron Cohen, Mark D. Gibson, Yang Liu, J. Vanderlei Martins, Yinon Rudich, and Randall V. Martin
Atmos. Chem. Phys., 16, 9629–9653, https://doi.org/10.5194/acp-16-9629-2016, https://doi.org/10.5194/acp-16-9629-2016, 2016
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We examine the chemical composition of fine particulate matter (PM2.5) collected on filters at traditionally undersampled, globally dispersed urban locations. Several PM2.5 chemical components (e.g. ammonium sulfate, ammonium nitrate, and black carbon) vary by more than an order of magnitude between sites while aerosol hygroscopicity varies by a factor of 2. Enhanced anthropogenic dust fractions in large urban areas are apparent from high Zn : Al ratios.
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.
Emma L. Mungall, Betty Croft, Martine Lizotte, Jennie L. Thomas, Jennifer G. Murphy, Maurice Levasseur, Randall V. Martin, Jeremy J. B. Wentzell, John Liggio, and Jonathan P. D. Abbatt
Atmos. Chem. Phys., 16, 6665–6680, https://doi.org/10.5194/acp-16-6665-2016, https://doi.org/10.5194/acp-16-6665-2016, 2016
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Previous work has suggested that marine emissions of dimethyl sulfide (DMS) could impact the Arctic climate through interactions with clouds. We made the first high-time-resolution measurements of summertime atmospheric DMS in the Canadian Arctic, and performed source sensitivity simulations. We found that regional marine sources dominated, but do not appear to be sufficient to explain our observations. Understanding DMS sources in the Arctic is necessary to model future climate in the region.
Yuanzheng Cui, Jintai Lin, Chunqiao Song, Mengyao Liu, Yingying Yan, Yuan Xu, and Bo Huang
Atmos. Chem. Phys., 16, 6207–6221, https://doi.org/10.5194/acp-16-6207-2016, https://doi.org/10.5194/acp-16-6207-2016, 2016
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We find rapid NO2 growth over Western China over 2005–2013 at a rate which exceeds the rates over the well-known polluted regions in the east. A nested GEOS-Chem simulation and Chinese official emission data confirm that anthropogenic emissions are the main driver of NO2 variations. Additional socioeconomic analysis suggests that this rapid NO2 growth is likely related to the fast industrialization and urbanization along with the "Go West" movement as well as relatively weak emission controls.
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.
Sajeev Philip, Randall V. Martin, and Christoph A. Keller
Geosci. Model Dev., 9, 1683–1695, https://doi.org/10.5194/gmd-9-1683-2016, https://doi.org/10.5194/gmd-9-1683-2016, 2016
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We assessed the sensitivity of simulation accuracy to the duration of chemical and transport operators in a chemistry-transport model.
Longer continuous transport operator duration increases concentrations of emitted species.
Chemical operator duration twice that of the transport operator duration offers more simulation accuracy per unit computation.
The simulation error from coarser spatial resolution generally exceeds that from longer operator duration.
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.
Betty Croft, Randall V. Martin, W. Richard Leaitch, Peter Tunved, Thomas J. Breider, Stephen D. D'Andrea, and Jeffrey R. Pierce
Atmos. Chem. Phys., 16, 3665–3682, https://doi.org/10.5194/acp-16-3665-2016, https://doi.org/10.5194/acp-16-3665-2016, 2016
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Measurements at high-Arctic sites show a strong annual cycle in atmospheric particle number and size. Previous studies identified poor scientific understanding related to global model representation of Arctic particle number and size, limiting ability to simulate this environment. Here we evaluate state-of-science ability to simulate Arctic particles using GEOS-Chem-TOMAS model, documenting key roles and interconnections of particle formation, cloud-related processes and remaining uncertainties.
N. I. Kristiansen, A. Stohl, D. J. L. Olivié, B. Croft, O. A. Søvde, H. Klein, T. Christoudias, D. Kunkel, S. J. Leadbetter, Y. H. Lee, K. Zhang, K. Tsigaridis, T. Bergman, N. Evangeliou, H. Wang, P.-L. Ma, R. C. Easter, P. J. Rasch, X. Liu, G. Pitari, G. Di Genova, S. Y. Zhao, Y. Balkanski, S. E. Bauer, G. S. Faluvegi, H. Kokkola, R. V. Martin, J. R. Pierce, M. Schulz, D. Shindell, H. Tost, and H. Zhang
Atmos. Chem. Phys., 16, 3525–3561, https://doi.org/10.5194/acp-16-3525-2016, https://doi.org/10.5194/acp-16-3525-2016, 2016
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Processes affecting aerosol removal from the atmosphere are not fully understood. In this study we investigate to what extent atmospheric transport models can reproduce observed loss of aerosols. We compare measurements of radioactive isotopes, that attached to ambient sulfate aerosols during the 2011 Fukushima nuclear accident, to 19 models using identical emissions. Results indicate aerosol removal that is too fast in most models, and apply to aerosols that have undergone long-range transport.
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
Chi Li, Randall V. Martin, Brian L. Boys, Aaron van Donkelaar, and Sacha Ruzzante
Atmos. Chem. Phys., 16, 2435–2457, https://doi.org/10.5194/acp-16-2435-2016, https://doi.org/10.5194/acp-16-2435-2016, 2016
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We comprehensively screen and process global hourly visibility data to construct a more reliable monthly inverse visibility (1/Vis) data set, and to infer trends in atmospheric haze. Consistency is found for the inferred 1/Vis seasonality and trends with other collocated in situ aerosol measurements over the US and Europe. Trends of 1/Vis over 1945–1996 for the eastern US, and over 1973–2013 for Europe and eastern Asia are significantly associated with the variation of SO2 emission.
Yingying Yan, Jintai Lin, Jinxuan Chen, and Lu Hu
Atmos. Chem. Phys., 16, 2381–2400, https://doi.org/10.5194/acp-16-2381-2016, https://doi.org/10.5194/acp-16-2381-2016, 2016
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We use a newly built two-way coupling system of the GEOS-Chem CTM to simulate the global tropospheric O3 in 2009. It significantly improves the simulation upon the global model by comparisons with a suite of ground, aircraft, and satellite measurements, also reduces the global OH by 5 % with enhancements by 5 % in the lifetimes of MCF and methane. Therefore, improving model representations of small-scale processes is a critical step forward to understanding the global tropospheric chemistry.
Jeffrey A. Geddes, Colette L. Heald, Sam J. Silva, and Randall V. Martin
Atmos. Chem. Phys., 16, 2323–2340, https://doi.org/10.5194/acp-16-2323-2016, https://doi.org/10.5194/acp-16-2323-2016, 2016
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Land use and land cover changes driven by anthropogenic activities or natural causes (e.g., forestry management, agriculture, wildfires) can impact climate and air quality in many complex ways. Using a state-of-the-art chemistry model, we investigate how tree mortality in the US due to insect infestation and disease outbreak may impact atmospheric composition. We find that the surface concentrations of ozone and aerosol can be altered due to changing background emissions and loss processes.
Gregory R. Wentworth, Jennifer G. Murphy, Betty Croft, Randall V. Martin, Jeffrey R. Pierce, Jean-Sébastien Côté, Isabelle Courchesne, Jean-Éric Tremblay, Jonathan Gagnon, Jennie L. Thomas, Sangeeta Sharma, Desiree Toom-Sauntry, Alina Chivulescu, Maurice Levasseur, and Jonathan P. D. Abbatt
Atmos. Chem. Phys., 16, 1937–1953, https://doi.org/10.5194/acp-16-1937-2016, https://doi.org/10.5194/acp-16-1937-2016, 2016
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Air near the surface in the summertime Arctic is extremely clean and typically has very low concentrations of both gases and particles. However, atmospheric measurements taken throughout the Canadian Arctic in the summer of 2014 revealed higher-than-expected amounts of gaseous ammonia. It is likely the majority of this ammonia is coming from migratory seabird colonies throughout the Arctic. Seabird guano (dung) releases ammonia which could impact climate and sensitive Arctic ecosystems.
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.
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.
J.-T. Lin, M.-Y. Liu, J.-Y. Xin, K. F. Boersma, R. Spurr, R. Martin, and Q. Zhang
Atmos. Chem. Phys., 15, 11217–11241, https://doi.org/10.5194/acp-15-11217-2015, https://doi.org/10.5194/acp-15-11217-2015, 2015
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We conduct an improved OMI-based retrieval of tropospheric NO2 VCDs (POMINO) over China by explicitly accounting for aerosol optical effects and surface reflectance anisotropy. Compared to the traditional implicit aerosol treatment, an explicit treatment greatly lowers NO2 VCDs and subsequently estimated NOx emissions over eastern China, but with large spatiotemporal dependence. An explicit treatment also better captures high-pollution days. Effects of surface reflectance treatments are smaller.
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.
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.
J. R. Pierce, B. Croft, J. K. Kodros, S. D. D'Andrea, and R. V. Martin
Atmos. Chem. Phys., 15, 6147–6158, https://doi.org/10.5194/acp-15-6147-2015, https://doi.org/10.5194/acp-15-6147-2015, 2015
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In this paper we show that coagulation of cloud droplets with interstitial aerosol particles, a process often neglected in atmospheric aerosol models, has a significant impact on aerosol size distributions and radiative forcings.
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
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.
G. Snider, C. L. Weagle, R. V. Martin, A. van Donkelaar, K. Conrad, D. Cunningham, C. Gordon, M. Zwicker, C. Akoshile, P. Artaxo, N. X. Anh, J. Brook, J. Dong, R. M. Garland, R. Greenwald, D. Griffith, K. He, B. N. Holben, R. Kahn, I. Koren, N. Lagrosas, P. Lestari, Z. Ma, J. Vanderlei Martins, E. J. Quel, Y. Rudich, A. Salam, S. N. Tripathi, C. Yu, Q. Zhang, Y. Zhang, M. Brauer, A. Cohen, M. D. Gibson, and Y. Liu
Atmos. Meas. Tech., 8, 505–521, https://doi.org/10.5194/amt-8-505-2015, https://doi.org/10.5194/amt-8-505-2015, 2015
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We have initiated a global network of ground-level monitoring stations to measure concentrations of fine aerosols in urban environments. Our findings include major ions species, total mass, and total scatter at three wavelengths. Results will be used to further evaluate and enhance satellite remote sensing estimates.
Z. Jiang, J. R. Worden, D. B. A. Jones, J.-T. Lin, W. W. Verstraeten, and D. K. Henze
Atmos. Chem. Phys., 15, 99–112, https://doi.org/10.5194/acp-15-99-2015, https://doi.org/10.5194/acp-15-99-2015, 2015
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We use satellite measurements of O3, CO and NO2 from TES, MOPITT and OMI to quantify O3 precursor emissions for 2006 and their impact on free tropospheric O3 over northeastern Asia. Using the adjoint of GEOS-Chem, we found that Chinese emissions have the largest influence on the free tropospheric O3. The contributions from lightning NOx in summer and India and southeastern Asia emissions in winter are sizable, comparable with Chinese emissions.
Y.-Y. Yan, J.-T. Lin, Y. Kuang, D. Yang, and L. Zhang
Atmos. Chem. Phys., 14, 12649–12663, https://doi.org/10.5194/acp-14-12649-2014, https://doi.org/10.5194/acp-14-12649-2014, 2014
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Limited by coarse resolutions, global chemical transport models cannot well capture small-scale nonlinear processes. To alleviate the problem, we develop a two-way coupled system to integrate the global GEOS-Chem model and its three high-resolution nested models covering Asia, Europe and North America. Confirmed by comparisons with observations, the coupled system improves upon the global model with a 10% increase in global tropospheric CO, a 4% decrease in OH and a 4% increase in MCF lifetime.
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.
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
G. C. M. Vinken, K. F. Boersma, J. D. Maasakkers, M. Adon, and R. V. Martin
Atmos. Chem. Phys., 14, 10363–10381, https://doi.org/10.5194/acp-14-10363-2014, https://doi.org/10.5194/acp-14-10363-2014, 2014
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
B. Croft, J. R. Pierce, and R. V. Martin
Atmos. Chem. Phys., 14, 4313–4325, https://doi.org/10.5194/acp-14-4313-2014, https://doi.org/10.5194/acp-14-4313-2014, 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
A. K. Mebust and R. C. Cohen
Atmos. Chem. Phys., 14, 2509–2524, https://doi.org/10.5194/acp-14-2509-2014, https://doi.org/10.5194/acp-14-2509-2014, 2014
J.-T. Lin, R. V. Martin, K. F. Boersma, M. Sneep, P. Stammes, R. Spurr, P. Wang, M. Van Roozendael, K. Clémer, and H. Irie
Atmos. Chem. Phys., 14, 1441–1461, https://doi.org/10.5194/acp-14-1441-2014, https://doi.org/10.5194/acp-14-1441-2014, 2014
E. C. Browne, P. J. Wooldridge, K.-E. Min, and R. C. Cohen
Atmos. Chem. Phys., 14, 1225–1238, https://doi.org/10.5194/acp-14-1225-2014, https://doi.org/10.5194/acp-14-1225-2014, 2014
L. C. Valin, A. R. Russell, and R. C. Cohen
Atmos. Chem. Phys., 14, 1–9, https://doi.org/10.5194/acp-14-1-2014, https://doi.org/10.5194/acp-14-1-2014, 2014
A. Wiacek, R. V. Martin, A. E. Bourassa, N. D. Lloyd, and D. A. Degenstein
Atmos. Meas. Tech., 6, 2761–2776, https://doi.org/10.5194/amt-6-2761-2013, https://doi.org/10.5194/amt-6-2761-2013, 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
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
J.-T. Lin, Z. Liu, Q. Zhang, H. Liu, J. Mao, and G. Zhuang
Atmos. Chem. Phys., 12, 12255–12275, https://doi.org/10.5194/acp-12-12255-2012, https://doi.org/10.5194/acp-12-12255-2012, 2012
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)
An improved estimate of inorganic iodine emissions from the ocean using a coupled surface microlayer box model
Impact of improved representation of volatile organic compound emissions and production of NOx reservoirs on modeled urban ozone production
The effect of different climate and air quality policies in China on in situ ozone production in Beijing
Enhancing long-term trend simulation of the global tropospheric hydroxyl (TOH) and its drivers from 2005 to 2019: a synergistic integration of model simulations and satellite observations
Intercomparison of GEOS-Chem and CAM-chem tropospheric oxidant chemistry within the Community Earth System Model version 2 (CESM2)
Development of a detailed gaseous oxidation scheme of naphthalene for secondary organic aerosol (SOA) formation and speciation
Large contributions of soil emissions to the atmospheric nitrogen budget and their impacts on air quality and temperature rise in North China
Why did ozone concentrations remain high during Shanghai's static management? A statistical and radical-chemistry perspective
Revising VOC emissions speciation improves the simulation of global background ethane and propane
Changes in South American surface ozone trends: exploring the influences of precursors and extreme events
Evaluating NOx stack plume emissions using a high-resolution atmospheric chemistry model and satellite-derived NO2 columns
NOx emissions in France in 2019–2021 as estimated by the high-spatial-resolution assimilation of TROPOMI NO2 observations
Aggravated surface O3 pollution primarily driven by meteorological variations in China during the 2020 COVID-19 pandemic lockdown period
Identifying decadal trends in deweathered concentrations of criteria air pollutants in Canadian urban atmospheres with machine learning approaches
Evaluation of modelled versus observed non-methane volatile organic compounds at European Monitoring and Evaluation Programme sites in Europe
Constraining non-methane VOC emissions with TROPOMI HCHO observations: impact on summertime ozone simulation in August 2022 in China
Revealing the significant acceleration of hydrofluorocarbon (HFC) emissions in eastern Asia through long-term atmospheric observations
Interpreting Geostationary Environment Monitoring Spectrometer (GEMS) geostationary satellite observations of the diurnal variation in nitrogen dioxide (NO2) over East Asia
An intercomparison of satellite, airborne, and ground-level observations with WRF–CAMx simulations of NO2 columns over Houston, Texas, during the September 2021 TRACER-AQ campaign
Impact of methane and other precursor emission reductions on surface ozone in Europe: Scenario analysis using the EMEP MSC-W model
Interannual variability of summertime formaldehyde (HCHO) vertical column density and its main drivers at northern high latitudes
The impact of multi-decadal changes in VOC speciation on urban ozone chemistry: a case study in Birmingham, United Kingdom
Technical note: Challenges in detecting free tropospheric ozone trends in a sparsely sampled environment
Combined assimilation of NOAA surface and MIPAS satellite observations to constrain the global budget of carbonyl sulfide
The impact of gaseous degradation on the gas–particle partitioning of methylated polycyclic aromatic hydrocarbons
Technical note: An assessment of the performance of statistical bias correction techniques for global chemistry–climate model surface ozone fields
A better representation of volatile organic compound chemistry in WRF-Chem and its impact on ozone over Los Angeles
High-resolution US methane emissions inferred from an inversion of 2019 TROPOMI satellite data: contributions from individual states, urban areas, and landfills
Summertime tropospheric ozone source apportionment study in the Madrid region (Spain)
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
An investigation into atmospheric nitrous acid (HONO) processes in South Korea
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
A global re-analysis of regionally resolved emissions and atmospheric mole fractions of SF6 for the period 2005–2021
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)
Ether and ester formation from peroxy radical recombination: A qualitative reaction channel analysis
Organosulfate produced from consumption of SO3 speeds up sulfuric acid–dimethylamine atmospheric nucleation
Tropospheric Ozone Precursors: Global and Regional Distributions, Trends and Variability
Contribution of expanded marine sulfur chemistry to the seasonal variability of dimethyl sulfide oxidation products and size-resolved sulfate aerosol
Verifying national inventory-based combustion emissions of CO2 across the UK and mainland Europe using satellite observations of atmospheric CO and CO2
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
The contribution of transport emissions to ozone mixing ratios and methane lifetime in 2015 and 2050 in the Shared Socioeconomic Pathways (SSPs)
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
Ryan J. Pound, Lucy V. Brown, Mat J. Evans, and Lucy J. Carpenter
Atmos. Chem. Phys., 24, 9899–9921, https://doi.org/10.5194/acp-24-9899-2024, https://doi.org/10.5194/acp-24-9899-2024, 2024
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Iodine-mediated loss of ozone to the ocean surface and the subsequent emission of iodine species has a large effect on the troposphere. Here we combine recent experimental insights to develop a box model of the process, which we then parameterize and incorporate into the GEOS-Chem transport model. We find that these new insights have a small impact on the total emission of iodine but significantly change its distribution.
Katherine R. Travis, Benjamin A. Nault, James H. Crawford, Kelvin H. Bates, Donald R. Blake, Ronald C. Cohen, Alan Fried, Samuel R. Hall, L. Gregory Huey, Young Ro Lee, Simone Meinardi, Kyung-Eun Min, Isobel J. Simpson, and Kirk Ullman
Atmos. Chem. Phys., 24, 9555–9572, https://doi.org/10.5194/acp-24-9555-2024, https://doi.org/10.5194/acp-24-9555-2024, 2024
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Human activities result in the emission of volatile organic compounds (VOCs) that contribute to air pollution. Detailed VOC measurements were taken during a field study in South Korea. When compared to VOC inventories, large discrepancies showed underestimates from chemical products, liquefied petroleum gas, and long-range transport. Improved emissions and chemistry of these VOCs better described urban pollution. The new chemical scheme is relevant to urban areas and other VOC sources.
Beth S. Nelson, Zhenze Liu, Freya A. Squires, Marvin Shaw, James R. Hopkins, Jacqueline F. Hamilton, Andrew R. Rickard, Alastair C. Lewis, Zongbo Shi, and James D. Lee
Atmos. Chem. Phys., 24, 9031–9044, https://doi.org/10.5194/acp-24-9031-2024, https://doi.org/10.5194/acp-24-9031-2024, 2024
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The impact of combined air quality and carbon neutrality policies on O3 formation in Beijing was investigated. Emissions inventory data were used to estimate future pollutant mixing ratios relative to ground-level observations. O3 production was found to be most sensitive to changes in alkenes, but large reductions in less reactive compounds led to larger reductions in future O3 production. This study highlights the importance of understanding the emissions of organic pollutants.
Amir H. Souri, Bryan N. Duncan, Sarah A. Strode, Daniel C. Anderson, Michael E. Manyin, Junhua Liu, Luke D. Oman, Zhen Zhang, and Brad Weir
Atmos. Chem. Phys., 24, 8677–8701, https://doi.org/10.5194/acp-24-8677-2024, https://doi.org/10.5194/acp-24-8677-2024, 2024
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We explore a new method of using the wealth of information obtained from satellite observations of Aura OMI NO2, HCHO, and MERRA-2 reanalysis in NASA’s GEOS model equipped with an efficient tropospheric OH (TOH) estimator to enhance the representation of TOH spatial distribution and its long-term trends. This new framework helps us pinpoint regional inaccuracies in TOH and differentiate between established prior knowledge and newly acquired information from satellites on TOH trends.
Haipeng Lin, Louisa K. Emmons, Elizabeth W. Lundgren, Laura Hyesung Yang, Xu Feng, Ruijun Dang, Shixian Zhai, Yunxiao Tang, Makoto M. Kelp, Nadia K. Colombi, Sebastian D. Eastham, Thibaud M. Fritz, and Daniel J. Jacob
Atmos. Chem. Phys., 24, 8607–8624, https://doi.org/10.5194/acp-24-8607-2024, https://doi.org/10.5194/acp-24-8607-2024, 2024
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Tropospheric ozone is a major air pollutant, a greenhouse gas, and a major indicator of model skill. Global atmospheric chemistry models show large differences in simulations of tropospheric ozone, but isolating sources of differences is complicated by different model environments. By implementing the GEOS-Chem model side by side to CAM-chem within a common Earth system model, we identify and evaluate specific differences between the two models and their impacts on key chemical species.
Victor Lannuque and Karine Sartelet
Atmos. Chem. Phys., 24, 8589–8606, https://doi.org/10.5194/acp-24-8589-2024, https://doi.org/10.5194/acp-24-8589-2024, 2024
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Large uncertainties remain in understanding secondary organic aerosol (SOA) formation and speciation from naphthalene oxidation. This study details the development of the first near-explicit chemical scheme for naphthalene oxidation by OH, which includes kinetic and mechanistic data, and is able to reproduce most of the experimentally identified products in both gas and particle phases.
Tong Sha, Siyu Yang, Qingcai Chen, Liangqing Li, Xiaoyan Ma, Yan-Lin Zhang, Zhaozhong Feng, K. Folkert Boersma, and Jun Wang
Atmos. Chem. Phys., 24, 8441–8455, https://doi.org/10.5194/acp-24-8441-2024, https://doi.org/10.5194/acp-24-8441-2024, 2024
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Using an updated soil reactive nitrogen emission scheme in the Unified Inputs for Weather Research and Forecasting coupled with Chemistry (UI-WRF-Chem) model, we investigate the role of soil NO and HONO (Nr) emissions in air quality and temperature in North China. Contributions of soil Nr emissions to O3 and secondary pollutants are revealed, exceeding effects of soil NOx or HONO emission. Soil Nr emissions play an important role in mitigating O3 pollution and addressing climate change.
Jian Zhu, Shanshan Wang, Chuanqi Gu, Zhiwen Jiang, Sanbao Zhang, Ruibin Xue, Yuhao Yan, and Bin Zhou
Atmos. Chem. Phys., 24, 8383–8395, https://doi.org/10.5194/acp-24-8383-2024, https://doi.org/10.5194/acp-24-8383-2024, 2024
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In 2022, Shanghai implemented city-wide static management measures during the high-ozone season in April and May, providing a chance to study ozone pollution control. Despite significant emissions reductions, ozone levels increased by 23 %. Statistically, the number of days with higher ozone diurnal variation types increased during the lockdown period. The uneven decline in VOC and NO2 emissions led to heightened photochemical processes, resulting in the observed ozone level rise.
Matthew J. Rowlinson, Mat J. Evans, Lucy J. Carpenter, Katie A. Read, Shalini Punjabi, Adedayo Adedeji, Luke Fakes, Ally Lewis, Ben Richmond, Neil Passant, Tim Murrells, Barron Henderson, Kelvin H. Bates, and Detlev Helmig
Atmos. Chem. Phys., 24, 8317–8342, https://doi.org/10.5194/acp-24-8317-2024, https://doi.org/10.5194/acp-24-8317-2024, 2024
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Ethane and propane are volatile organic compounds emitted from human activities which help to form ozone, a pollutant and greenhouse gas, and also affect the chemistry of the lower atmosphere. Atmospheric models tend to do a poor job of reproducing the abundance of these compounds in the atmosphere. By using regional estimates of their emissions, rather than globally consistent estimates, we can significantly improve the simulation of ethane in the model and make some improvement for propane.
Rodrigo J. Seguel, Lucas Castillo, Charlie Opazo, Néstor Y. Rojas, Thiago Nogueira, María Cazorla, Mario Gavidia-Calderón, Laura Gallardo, René Garreaud, Tomás Carrasco-Escaff, and Yasin Elshorbany
Atmos. Chem. Phys., 24, 8225–8242, https://doi.org/10.5194/acp-24-8225-2024, https://doi.org/10.5194/acp-24-8225-2024, 2024
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Trends of surface ozone were examined across South America. Our findings indicate that ozone trends in major South American cities either increase or remain steady, with no signs of decline. The upward trends can be attributed to chemical regimes that efficiently convert nitric oxide into nitrogen dioxide. Additionally, our results suggest a climate penalty for ozone driven by meteorological conditions that favor wildfire propagation in Chile and extensive heat waves in southern Brazil.
Maarten Krol, Bart van Stratum, Isidora Anglou, and Klaas Folkert Boersma
Atmos. Chem. Phys., 24, 8243–8262, https://doi.org/10.5194/acp-24-8243-2024, https://doi.org/10.5194/acp-24-8243-2024, 2024
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This paper presents detailed plume simulations of nitrogen oxides and carbon dioxide that are emitted from four large industrial facilities world-wide. Results from the high-resolution simulations that include atmospheric chemistry are compared to nitrogen dioxide observations from satellites. We find good performance of the model and show that common assumptions that are used in simplified models need revision. This work is important for the monitoring of emissions using satellite data.
Robin Plauchu, Audrey Fortems-Cheiney, Grégoire Broquet, Isabelle Pison, Antoine Berchet, Elise Potier, Gaëlle Dufour, Adriana Coman, Dilek Savas, Guillaume Siour, and Henk Eskes
Atmos. Chem. Phys., 24, 8139–8163, https://doi.org/10.5194/acp-24-8139-2024, https://doi.org/10.5194/acp-24-8139-2024, 2024
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This study uses the Community Inversion Framework and CHIMERE model to assess the potential of TROPOMI-S5P PAL NO2 tropospheric column data to estimate NOx emissions in France (2019–2021). Results show a 3 % decrease in average emissions compared to the 2016 CAMS-REG/INS, lower than the 14 % decrease from CITEPA. The study highlights challenges in capturing emission anomalies due to limited data coverage and error levels but shows promise for local inventory improvements.
Zhendong Lu, Jun Wang, Yi Wang, Daven K. Henze, Xi Chen, Tong Sha, and Kang Sun
Atmos. Chem. Phys., 24, 7793–7813, https://doi.org/10.5194/acp-24-7793-2024, https://doi.org/10.5194/acp-24-7793-2024, 2024
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In contrast with past work showing that the reduction of emissions was the dominant factor for the nationwide increase of surface O3 during the lockdown in China, this study finds that the variation in meteorology (temperature and other parameters) plays a more important role. This result is obtained through sensitivity simulations using a chemical transport model constrained by satellite (TROPOMI) data and calibrated with surface observations.
Xiaohong Yao and Leiming Zhang
Atmos. Chem. Phys., 24, 7773–7791, https://doi.org/10.5194/acp-24-7773-2024, https://doi.org/10.5194/acp-24-7773-2024, 2024
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This study investigates long-term trends of criteria air pollutants, including NO2, CO, SO2, O3 and PM2.5, and NO2+O3 measured in 10 Canadian cities during the last 2 to 3 decades. We also investigate associated driving forces in terms of emission reductions, perturbations from varying weather conditions and large-scale wildfires, as well as changes in O3 sources and sinks.
Yao Ge, Sverre Solberg, Mathew R. Heal, Stefan Reimann, Willem van Caspel, Bryan Hellack, Thérèse Salameh, and David Simpson
Atmos. Chem. Phys., 24, 7699–7729, https://doi.org/10.5194/acp-24-7699-2024, https://doi.org/10.5194/acp-24-7699-2024, 2024
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Atmospheric volatile organic compounds (VOCs) constitute many species, acting as precursors to ozone and aerosol. Given the uncertainties in VOC emissions, lack of evaluation studies, and recent changes in emissions, this work adapts the EMEP MSC-W to evaluate emission inventories in Europe. We focus on the varying agreement between modelled and measured VOCs across different species and underscore potential inaccuracies in total and sector-specific emission estimates.
Shuzhuang Feng, Fei Jiang, Tianlu Qian, Nan Wang, Mengwei Jia, Songci Zheng, Jiansong Chen, Fang Ying, and Weimin Ju
Atmos. Chem. Phys., 24, 7481–7498, https://doi.org/10.5194/acp-24-7481-2024, https://doi.org/10.5194/acp-24-7481-2024, 2024
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We developed a multi-air-pollutant inversion system to estimate non-methane volatile organic compound (NMVOC) emissions using TROPOMI formaldehyde retrievals. We found that the inversion significantly improved formaldehyde simulations and reduced NMVOC emission uncertainties. The optimized NMVOC emissions effectively corrected the overestimation of O3 levels, mainly by decreasing the rate of the RO2 + NO reaction and increasing the rate of the NO2 + OH reaction.
Haklim Choi, Alison L. Redington, Hyeri Park, Jooil Kim, Rona L. Thompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Ray F. Weiss, Alistair J. Manning, and Sunyoung Park
Atmos. Chem. Phys., 24, 7309–7330, https://doi.org/10.5194/acp-24-7309-2024, https://doi.org/10.5194/acp-24-7309-2024, 2024
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We analyzed with an inversion model the atmospheric abundance of hydrofluorocarbons (HFCs), potent greenhouse gases, from 2008 to 2020 at Gosan station in South Korea and revealed a significant increase in emissions, especially from eastern China and Japan. This increase contradicts reported data, underscoring the need for accurate monitoring and reporting. Our findings are crucial for understanding and managing global HFCs emissions, highlighting the importance of efforts to reduce HFCs.
Laura Hyesung Yang, Daniel J. Jacob, Ruijun Dang, Yujin J. Oak, Haipeng Lin, Jhoon Kim, Shixian Zhai, Nadia K. Colombi, Drew C. Pendergrass, Ellie Beaudry, Viral Shah, Xu Feng, Robert M. Yantosca, Heesung Chong, Junsung Park, Hanlim Lee, Won-Jin Lee, Soontae Kim, Eunhye Kim, Katherine R. Travis, James H. Crawford, and Hong Liao
Atmos. Chem. Phys., 24, 7027–7039, https://doi.org/10.5194/acp-24-7027-2024, https://doi.org/10.5194/acp-24-7027-2024, 2024
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The Geostationary Environment Monitoring Spectrometer (GEMS) provides hourly measurements of NO2. We use the chemical transport model to find how emissions, chemistry, and transport drive the changes in NO2 observed by GEMS at different times of the day. In winter, the chemistry plays a minor role, and high daytime emissions dominate the diurnal variation in NO2, balanced by transport. In summer, emissions, chemistry, and transport play an important role in shaping the diurnal variation in NO2.
M. Omar Nawaz, Jeremiah Johnson, Greg Yarwood, Benjamin de Foy, Laura Judd, and Daniel L. Goldberg
Atmos. Chem. Phys., 24, 6719–6741, https://doi.org/10.5194/acp-24-6719-2024, https://doi.org/10.5194/acp-24-6719-2024, 2024
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NO2 is a gas with implications for air pollution. A campaign conducted in Houston provided an opportunity to compare NO2 from different instruments and a model. Aircraft and satellite observations agreed well with measurements on the ground; however, the latter estimated lower values. We find that model-simulated NO2 was lower than observations, especially downtown, suggesting that NO2 sources associated with the urban core of Houston, such as vehicle emissions, may be underestimated.
Willem Elias van Caspel, Zbigniew Klimont, Chris Heyes, and Hilde Fagerli
EGUsphere, https://doi.org/10.5194/egusphere-2024-1422, https://doi.org/10.5194/egusphere-2024-1422, 2024
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Methane in the atmosphere contributes to the production of ozone gas, which is an air pollutant as well as a greenhouse gas. In this study, the impact of reducing methane emissions on surface ozone is investigated for the United Nations Economic Commission for Europe (UNECE) region excluding North America and Israel (the "EMEP region"), in particular in terms of its importance in reaching the ozone exposure guideline limits set by the World Health Organization.
Tianlang Zhao, Jingqiu Mao, Zolal Ayazpour, Gonzalo González Abad, Caroline R. Nowlan, and Yiqi Zheng
Atmos. Chem. Phys., 24, 6105–6121, https://doi.org/10.5194/acp-24-6105-2024, https://doi.org/10.5194/acp-24-6105-2024, 2024
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HCHO variability is a key tracer in understanding VOC emissions in response to climate change. We investigate the role of methane oxidation and biogenic and wildfire emissions in HCHO interannual variability over northern high latitudes in summer, emphasizing wildfires as a key driver of HCHO interannual variability in Alaska, Siberia and northern Canada using satellite HCHO and SIF retrievals and then GEOS-Chem model. We show SIF is a tool to understand biogenic HCHO variability in this region.
Jianghao Li, Alastair C. Lewis, Jim R. Hopkins, Stephen J. Andrews, Tim Murrells, Neil Passant, Ben Richmond, Siqi Hou, William J. Bloss, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 24, 6219–6231, https://doi.org/10.5194/acp-24-6219-2024, https://doi.org/10.5194/acp-24-6219-2024, 2024
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A summertime ozone event at an urban site in Birmingham is sensitive to volatile organic compounds (VOCs) – particularly those of oxygenated VOCs. The roles of anthropogenic VOC sources in urban ozone chemistry are examined by integrating the 1990–2019 national atmospheric emission inventory into model scenarios. Road transport remains the most powerful means of further reducing ozone in this case study, but the benefits may be offset if solvent emissions of VOCs continue to increase.
Kai-Lan Chang, Owen R. Cooper, Audrey Gaudel, Irina Petropavlovskikh, Peter Effertz, Gary Morris, and Brian C. McDonald
Atmos. Chem. Phys., 24, 6197–6218, https://doi.org/10.5194/acp-24-6197-2024, https://doi.org/10.5194/acp-24-6197-2024, 2024
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A great majority of observational trend studies of free tropospheric ozone use sparsely sampled ozonesonde and aircraft measurements as reference data sets. A ubiquitous assumption is that trends are accurate and reliable so long as long-term records are available. We show that sampling bias due to sparse samples can persistently reduce the trend accuracy, and we highlight the importance of maintaining adequate frequency and continuity of observations.
Jin Ma, Linda M. J. Kooijmans, Norbert Glatthor, Stephen A. Montzka, Marc von Hobe, Thomas Röckmann, and Maarten C. Krol
Atmos. Chem. Phys., 24, 6047–6070, https://doi.org/10.5194/acp-24-6047-2024, https://doi.org/10.5194/acp-24-6047-2024, 2024
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The global budget of atmospheric COS can be optimised by inverse modelling using TM5-4DVAR, with the co-constraints of NOAA surface observations and MIPAS satellite data. We found reduced COS biosphere uptake from inversions and improved land and ocean separation using MIPAS satellite data assimilation. Further improvements are expected from better quantification of COS ocean and biosphere fluxes.
Fu-Jie Zhu, Zi-Feng Zhang, Li-Yan Liu, Pu-Fei Yang, Peng-Tuan Hu, Geng-Bo Ren, Meng Qin, and Wan-Li Ma
Atmos. Chem. Phys., 24, 6095–6103, https://doi.org/10.5194/acp-24-6095-2024, https://doi.org/10.5194/acp-24-6095-2024, 2024
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Gas–particle (G–P) partitioning is an important atmospheric behavior for semi-volatile organic compounds (SVOCs). Diurnal variation in G–P partitioning of methylated polycyclic aromatic hydrocarbons (Me-PAHs) demonstrates the possible influence of gaseous degradation; the enhancement of gaseous degradation (1.10–5.58 times) on G–P partitioning is verified by a steady-state G–P partitioning model. The effect of gaseous degradation on G–P partitioning of (especially light) SVOCs is important.
Christoph Staehle, Harald E. Rieder, Arlene M. Fiore, and Jordan L. Schnell
Atmos. Chem. Phys., 24, 5953–5969, https://doi.org/10.5194/acp-24-5953-2024, https://doi.org/10.5194/acp-24-5953-2024, 2024
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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 from more complex approaches. Thus, our study suggests broader use of these techniques in studies seeking to inform air quality management and policy.
Qindan Zhu, Rebecca H. Schwantes, Matthew Coggon, Colin Harkins, Jordan Schnell, Jian He, Havala O. T. Pye, Meng Li, Barry Baker, Zachary Moon, Ravan Ahmadov, Eva Y. Pfannerstill, Bryan Place, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Anthony Bucholtz, John H. Seinfeld, Carsten Warneke, Chelsea E. Stockwell, Lu Xu, Kristen Zuraski, Michael A. Robinson, J. Andrew Neuman, Patrick R. Veres, Jeff Peischl, Steven S. Brown, Allen H. Goldstein, Ronald C. Cohen, and Brian C. McDonald
Atmos. Chem. Phys., 24, 5265–5286, https://doi.org/10.5194/acp-24-5265-2024, https://doi.org/10.5194/acp-24-5265-2024, 2024
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Volatile organic compounds (VOCs) fuel the production of air pollutants like ozone and particulate matter. The representation of VOC chemistry remains challenging due to its complexity in speciation and reactions. Here, we develop a chemical mechanism, RACM2B-VCP, that better represents VOC chemistry in urban areas such as Los Angeles. We also discuss the contribution of VOCs emitted from volatile chemical products and other anthropogenic sources to total VOC reactivity and O3.
Hannah Nesser, Daniel J. Jacob, Joannes D. Maasakkers, Alba Lorente, Zichong Chen, Xiao Lu, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Margaux Winter, Shuang Ma, A. Anthony Bloom, John R. Worden, Robert N. Stavins, and Cynthia A. Randles
Atmos. Chem. Phys., 24, 5069–5091, https://doi.org/10.5194/acp-24-5069-2024, https://doi.org/10.5194/acp-24-5069-2024, 2024
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We quantify 2019 methane emissions in the contiguous US (CONUS) at a ≈ 25 km × 25 km resolution using satellite methane observations. We find a 13 % upward correction to the 2023 US Environmental Protection Agency (EPA) Greenhouse Gas Emissions Inventory (GHGI) for 2019, with large corrections to individual states, urban areas, and landfills. This may present a challenge for US climate policies and goals, many of which target significant reductions in methane emissions.
David de la Paz, Rafael Borge, Juan Manuel de Andrés, Luis Tovar, Golam Sarwar, and Sergey L. Napelenok
Atmos. Chem. Phys., 24, 4949–4972, https://doi.org/10.5194/acp-24-4949-2024, https://doi.org/10.5194/acp-24-4949-2024, 2024
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This source apportionment modeling study shows that around 70 % of ground-level O3 in Madrid (Spain) is transported from other regions. Nonetheless, emissions from local sources, mainly road traffic, play a significant role, especially under atmospheric stagnation. Local measures during those conditions may be able to reduce O3 peaks by up to 30 % and, thus, lessen impacts from high-O3 episodes in the Madrid metropolitan area.
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.
Kiyeon Kim, Kyung Man Han, Chul Han Song, Hyojun Lee, Ross Beardsley, Jinhyeok Yu, Greg Yarwood, Bonyoung Koo, Jasper Madalipay, Jung-Hun Woo, and Seogju Cho
EGUsphere, https://doi.org/10.5194/egusphere-2024-886, https://doi.org/10.5194/egusphere-2024-886, 2024
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We incoporated each HONO process into the current CMAQ modeling framework to enhance the accuracy of HONO mixing ratios predictions. These results expand our understanding of HONO photochemistry and identify crucial sources of HONO that impact the total HONO budget in Seoul, South Korea. Through this investigation, we contribute to resolving discrepancies in understading chemical transport models, with implications for better air quality mangement and environmental protection in the region.
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.
Martin Vojta, Andreas Plach, Saurabh Annadate, Sunyong Park, Gawon Lee, Pallav Purohit, Florian Lindl, Xin Lan, Jens Mühle, Rona L. Thompson, and Andreas Stohl
EGUsphere, https://doi.org/10.5194/egusphere-2024-811, https://doi.org/10.5194/egusphere-2024-811, 2024
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We constrain the global emissions of the very potent greenhouse gas sulfur hexafluoride (SF6) between 2005 and 2021. We show, that SF6 emissions are decreasing in the USA and Europe, while they are substantially growing in China, leading overall to an increasing global emission trend. The national reports for the USA, Europe, and China all underestimated their SF6 emissions. However, stringent mitigation measures can successfully reduce SF6 emissions, as can be seen in the EU emission trend.
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.
Lauri Johannes Franzon, Marie Camredon, Richard Valorso, Bernard Aumont, and Theo Christian Kurtén
EGUsphere, https://doi.org/10.5194/egusphere-2024-920, https://doi.org/10.5194/egusphere-2024-920, 2024
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In this article we investigate the formation of large, sticky molecules from various organic compounds entering the atmosphere as primary emissions, and the degree to which these processes may contribute to organic aerosol particle mass. More specifically, we are qualitatively investigating a recently discovered chemical reaction channel for one of the most important short-lived radical compounds, peroxy radicals, and discovering which of these reactions are most atmospherically important.
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.
Yasin Elshorbany, Jerald Ziemke, Sarah Strode, Hervé Petetin, Kazuyuki Miyazaki, Isabelle De Smedt, Kenneth Pickering, Rodrigo Seguel, Helen Worden, Tamara Emmerichs, Domenico Taraborrelli, Maria Cazorla, Suvarna Fadnavis, Rebecca Buchholz, Benjamin Gaubert, Néstor Rojas, Thiago Nogueira, Thérèse Salameh, and Min Huang
EGUsphere, https://doi.org/10.5194/egusphere-2024-720, https://doi.org/10.5194/egusphere-2024-720, 2024
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We investigated tropospheric ozone spatial variability and trends from 2005 to 2019 and related those to ozone precursors on global and regional scales. We also investigate the spatiotemporal characteristics of the ozone formation regime in relation to ozone chemical sources and sinks. Our analysis is based on remote sensing products of the Tropospheric Column of Ozone and its precursors, nitrogen dioxide, formaldehyde, and total column of CO as well as ozonesonde data and model simulations.
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.
Tia Scarpelli, Paul Palmer, Mark Lunt, Ingrid Super, and Arjan Droste
EGUsphere, https://doi.org/10.5194/egusphere-2024-416, https://doi.org/10.5194/egusphere-2024-416, 2024
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Under the Paris Agreement, countries must track their anthropogenic greenhouse gas emissions. This study describes a method to determine self-consistent estimates for combustion emissions and natural fluxes of CO2 from atmospheric data We report consistent estimates inferred using this approach from satellite data and ground-based data over Europe, suggesting that satellite data can be used to determine national anthropogenic CO2 emissions for countries where ground-based CO2 data are absent.
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.
Mariano Mertens, Sabine Brinkop, Phoebe Graf, Volker Grewe, Johannes Hendricks, Patrick Jöckel, Anna Lanteri, Sigrun Matthes, Vanessa S. Rieger, Mattia Righi, and Robin N. Thor
EGUsphere, https://doi.org/10.5194/egusphere-2024-324, https://doi.org/10.5194/egusphere-2024-324, 2024
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We quantified the contributions of land transport, shipping and aviation emissions to tropospheric ozone and the reductions of the methane lifetime using chemistry-climate model simulations. The contributions were analysed for the conditions of 2015 and for three projections for the year 2050. The results highllight the challenges of mitigating ozone formed by emissions of the transport sector, caused by the non-linearitiy of the ozone chemistry and the long life-time.
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
Short summary
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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.
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Short summary
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.
Models are essential to diagnose the significant effects of nitrogen oxides (NOx) on air...
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