Articles | Volume 19, issue 9
https://doi.org/10.5194/acp-19-6107-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-19-6107-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| Highlight paper
| 
08 May 2019
Research article | Highlight paper |
| 08 May 2019
| 08 May 2019
Heterogeneous sulfate aerosol formation mechanisms during wintertime Chinese haze events: air quality model assessment using observations of sulfate oxygen isotopes in Beijing
Jingyuan Shao
Laboratory for Climate and Ocean-Atmosphere Studies, Department of Atmospheric and Oceanic Sciences, School of Physics, Peking University, Beijing 100871, China
Department of Atmospheric Sciences, University of Washington, Seattle, WA 98195, USA
Qianjie Chen
Department of Atmospheric Sciences, University of Washington, Seattle, WA 98195, USA
Department of Chemistry, University of Michigan, Ann Arbor, MI 48109, USA
Yuxuan Wang
Department of Earth and Atmospheric Sciences, University of Houston, Houston, TX 77204, USA
Laboratory for Climate and Ocean-Atmosphere Studies, Department of Atmospheric and Oceanic Sciences, School of Physics, Peking University, Beijing 100871, China
Pengzhen He
Anhui Province Key Laboratory of Polar Environment and Global Change, School of Earth and Space Sciences, University of Science and Technology of China, Hefei 230026, China
State Key Laboratory of Atmospheric Boundary Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China
Viral Shah
Department of Atmospheric Sciences, University of Washington, Seattle, WA 98195, USA
School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, USA
Randall V. Martin
Department of Physics and Atmospheric Science, Dalhousie University, Halifax, Nova Scotia, Canada
Sajeev Philip
NASA postdoctoral program, NASA Ames Research Center, Moffett Field, CA 94035, USA
Shaojie Song
School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, USA
School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China
Zhouqing Xie
CORRESPONDING AUTHOR
Anhui Province Key Laboratory of Polar Environment and Global Change, School of Earth and Space Sciences, University of Science and Technology of China, Hefei 230026, China
Lin Zhang
CORRESPONDING AUTHOR
Laboratory for Climate and Ocean-Atmosphere Studies, Department of Atmospheric and Oceanic Sciences, School of Physics, Peking University, Beijing 100871, China
Department of Atmospheric Sciences, University of Washington, Seattle, WA 98195, USA
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This study establishes an inventory of anthropogenic chlorine emissions in China in 2018 with expanded categories (HCl, Cl-, Cl2, HOCl) and sources (41 specific sources) with detailed spatial and temporal assignments, and emission factors based on localized survey data. This study enhances the understanding of anthropogenic chlorine emissions in the atmosphere, identifies key sources, and provides scientific support for pollution control and climate change.
Daniel J. Varon, Daniel J. Jacob, Benjamin Hmiel, Ritesh Gautam, David R. Lyon, Mark Omara, Melissa Sulprizio, Lu Shen, Drew Pendergrass, Hannah Nesser, Zhen Qu, Zachary R. Barkley, Natasha L. Miles, Scott J. Richardson, Kenneth J. Davis, Sudhanshu Pandey, Xiao Lu, Alba Lorente, Tobias Borsdorff, Joannes D. Maasakkers, and Ilse Aben
Atmos. Chem. Phys., 23, 7503–7520, https://doi.org/10.5194/acp-23-7503-2023, https://doi.org/10.5194/acp-23-7503-2023, 2023
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We use TROPOMI satellite observations to quantify weekly methane emissions from the US Permian oil and gas basin from May 2018 to October 2020. We find that Permian emissions are highly variable, with diverse economic and activity drivers. The most important drivers during our study period were new well development and natural gas price. Permian methane intensity averaged 4.6 % and decreased by 1 % per year.
Hang Liu, Xiaole Pan, Shandong Lei, Yuting Zhang, Aodong Du, Weijie Yao, Guiqian Tang, Tao Wang, Jinyuan Xin, Jie Li, Yele Sun, Junji Cao, and Zifa Wang
Atmos. Chem. Phys., 23, 7225–7239, https://doi.org/10.5194/acp-23-7225-2023, https://doi.org/10.5194/acp-23-7225-2023, 2023
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We provide the average vertical profiles of black carbon (BC) concentration, size distribution and coating thickness at different times of the day in an urban area based on 112 vertical profiles. In addition, it is found that BC in the residual layer generally has a thicker coating, higher absorption enhancement and hygroscopicity than on the surface. Such aged BC could enter into the boundary layer and influence the BC properties in the early morning.
Zhouxing Zou, Qianjie Chen, Men Xia, Qi Yuan, Yi Chen, Yanan Wang, Enyu Xiong, Zhe Wang, and Tao Wang
Atmos. Chem. Phys., 23, 7057–7074, https://doi.org/10.5194/acp-23-7057-2023, https://doi.org/10.5194/acp-23-7057-2023, 2023
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We present OH observation and model simulation results at a coastal site in Hong Kong. The model predicted the OH concentration under high-NOx well but overpredicted it under low-NOx conditions. This implies an insufficient understanding of OH chemistry under low-NOx conditions. We show evidence of missing OH sinks as a possible cause of the overprediction.
Zhuang Jiang, Becky Alexander, Joel Savarino, and Lei Geng
EGUsphere, https://doi.org/10.5194/egusphere-2023-1054, https://doi.org/10.5194/egusphere-2023-1054, 2023
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Ice-core nitrate could track the past atmospheric NOx and oxidant level, but its interpretation is hampered by the post-depositional processing. In this work, an inverse model was developed and tested against two polar sites, and was shown to well reproduce the observed nitrate signals in snow and atmosphere, suggesting that the model can properly correct for the effect of post-depositional processing. This model offers a very useful tool for future studies on ice-core nitrate records.
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
EGUsphere, https://doi.org/10.5194/egusphere-2023-946, https://doi.org/10.5194/egusphere-2023-946, 2023
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We quantify 2019 methane emissions in the contiguous U.S. (CONUS) at ≈25 km × 25 km resolution using satellite methane observations. We find a 13 % upward correction to the 2023 U.S. 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 U.S. climate policies and goals, many of which target significant reductions in methane emissions.
Lei Kong, Xiao Tang, Jiang Zhu, Zifa Wang, Yele Sun, Pingqing Fu, Meng Gao, Huangjian Wu, Miaomiao Lu, Qian Wu, Shuyuan Huang, Wenxuan Sui, Jie Li, Xiaole Pan, Lin Wu, Hajime Akimoto, and Gregory R. Carmichael
Atmos. Chem. Phys., 23, 6217–6240, https://doi.org/10.5194/acp-23-6217-2023, https://doi.org/10.5194/acp-23-6217-2023, 2023
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A multi-air-pollutant inversion system has been developed in this study to estimate emission changes in China during COVID-19 lockdown. The results demonstrate that the lockdown is largely a nationwide road traffic control measure with NOx emissions decreasing by ~40 %. Emissions of other species only decreased by ~10 % due to smaller effects of lockdown on other sectors. Assessment results further indicate that the lockdown only had limited effects on the control of PM2.5 and O3 in China.
Ruijun Dang, Daniel J. Jacob, Viral Shah, Sebastian D. Eastham, Thibaud M. Fritz, Loretta J. Mickley, Tianjia Liu, Yi Wang, and Jun Wang
Atmos. Chem. Phys., 23, 6271–6284, https://doi.org/10.5194/acp-23-6271-2023, https://doi.org/10.5194/acp-23-6271-2023, 2023
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We use the GEOS-Chem model to better understand the magnitude and trend in free tropospheric NO2 over the contiguous US. Model underestimate of background NO2 is largely corrected by considering aerosol nitrate photolysis. Increase in aircraft emissions affects satellite retrievals by altering the NO2 shape factor, and this effect is expected to increase in future. We show the importance of properly accounting for the free tropospheric background in interpreting NO2 observations from space.
Zichong Chen, Daniel J. Jacob, Ritesh Gautam, Mark Omara, Robert N. Stavins, Robert C. Stowe, Hannah Nesser, Melissa P. Sulprizio, Alba Lorente, Daniel J. Varon, Xiao Lu, Lu Shen, Zhen Qu, Drew C. Pendergrass, and Sarah Hancock
Atmos. Chem. Phys., 23, 5945–5967, https://doi.org/10.5194/acp-23-5945-2023, https://doi.org/10.5194/acp-23-5945-2023, 2023
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We quantify methane emissions from individual countries in the Middle East and North Africa by inverse analysis of 2019 TROPOMI satellite observations of atmospheric methane. We show that the ability to simply relate oil/gas emissions to activity metrics is compromised by stochastic nature of local infrastructure and management practices. We find that the industry target for oil/gas methane intensity is achievable through associated gas capture, modern infrastructure, and centralized operations.
Joanna E. Dyson, Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Stephen D. Worrall, Asan Bacak, Archit Mehra, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, C. Nicholas Hewitt, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, W. Joe F. Acton, William J. Bloss, Supattarachai Saksakulkrai, Jingsha Xu, Zongbo Shi, Roy M. Harrison, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lianfang Wei, Pingqing Fu, Xinming Wang, Stephen R. Arnold, and Dwayne E. Heard
Atmos. Chem. Phys., 23, 5679–5697, https://doi.org/10.5194/acp-23-5679-2023, https://doi.org/10.5194/acp-23-5679-2023, 2023
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The hydroxyl (OH) and closely coupled hydroperoxyl (HO2) radicals are vital for their role in the removal of atmospheric pollutants. In less polluted regions, atmospheric models over-predict HO2 concentrations. In this modelling study, the impact of heterogeneous uptake of HO2 onto aerosol surfaces on radical concentrations and the ozone production regime in Beijing in the summertime is investigated, and the implications for emissions policies across China are considered.
Haihui Zhu, Randall V. Martin, Betty Croft, Shixian Zhai, Chi Li, Liam Bindle, Jeffrey R. Pierce, Rachel Y.-W. Chang, Bruce E. Anderson, Luke D. Ziemba, Johnathan W. Hair, Richard A. Ferrare, Chris A. Hostetler, Inderjeet Singh, Deepangsu Chatterjee, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jack E. Dibb, Joshua S. Schwarz, and Andrew Weinheimer
Atmos. Chem. Phys., 23, 5023–5042, https://doi.org/10.5194/acp-23-5023-2023, https://doi.org/10.5194/acp-23-5023-2023, 2023
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Particle size of atmospheric aerosol is important for estimating its climate and health effects, but simulating atmospheric aerosol size is computationally demanding. This study derives a simple parameterization of the size of organic and secondary inorganic ambient aerosol that can be applied to atmospheric models. Applying this parameterization allows a better representation of the global spatial pattern of aerosol size, as verified by ground and airborne measurements.
Shixian Zhai, Daniel J. Jacob, Drew C. Pendergrass, Nadia K. Colombi, Viral Shah, Laura Hyesung Yang, Qiang Zhang, Shuxiao Wang, Hwajin Kim, Yele Sun, Jin-Soo Choi, Jin-Soo Park, Gan Luo, Fangqun Yu, Jung-Hun Woo, Younha Kim, Jack E. Dibb, Taehyoung Lee, Jin-Seok Han, Bruce E. Anderson, Ke Li, and Hong Liao
Atmos. Chem. Phys., 23, 4271–4281, https://doi.org/10.5194/acp-23-4271-2023, https://doi.org/10.5194/acp-23-4271-2023, 2023
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Anthropogenic fugitive dust in East Asia not only causes severe coarse particulate matter air pollution problems, but also affects fine particulate nitrate. Due to emission control efforts, coarse PM decreased steadily. We find that the decrease of coarse PM is a major driver for a lack of decrease of fine particulate nitrate, as it allows more nitric acid to form fine particulate nitrate. The continuing decrease of coarse PM requires more stringent ammonia and nitrogen oxides emission controls.
Nadia K. Colombi, Daniel J. Jacob, Laura Hyesung Yang, Shixian Zhai, Viral Shah, Stuart K. Grange, Robert M. Yantosca, Soontae Kim, and Hong Liao
Atmos. Chem. Phys., 23, 4031–4044, https://doi.org/10.5194/acp-23-4031-2023, https://doi.org/10.5194/acp-23-4031-2023, 2023
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Surface ozone, detrimental to human and ecosystem health, is very high and increasing in South Korea. Using a global model of the atmosphere, we found that emissions from South Korea and China contribute equally to the high ozone observed. We found that in the absence of all anthropogenic emissions over East Asia, ozone is still very high, implying that the air quality standard in South Korea is not practically achievable unless this background external to East Asia can be decreased.
Chi Li, Randall V. Martin, Ronald C. Cohen, Liam Bindle, Dandan Zhang, Deepangsu Chatterjee, Hongjian Weng, and Jintai Lin
Atmos. Chem. Phys., 23, 3031–3049, https://doi.org/10.5194/acp-23-3031-2023, https://doi.org/10.5194/acp-23-3031-2023, 2023
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Models are essential to diagnose the significant effects of nitrogen oxides (NOx) on air pollution. We use an air quality model to illustrate the variability of NOx resolution-dependent simulation biases; how these biases depend on specific chemical environments, driving mechanisms, and vertical variabilities; and how these biases affect the interpretation of satellite observations. High-resolution simulations are thus critical to accurately interpret NOx and its relevance to air quality.
Laura Hyesung Yang, Daniel J. Jacob, Nadia K. Colombi, Shixian Zhai, Kelvin H. Bates, Viral Shah, Ellie Beaudry, Robert M. Yantosca, Haipeng Lin, Jared F. Brewer, Heesung Chong, Katherine R. Travis, James H. Crawford, Lok N. Lamsal, Ja-Ho Koo, and Jhoon Kim
Atmos. Chem. Phys., 23, 2465–2481, https://doi.org/10.5194/acp-23-2465-2023, https://doi.org/10.5194/acp-23-2465-2023, 2023
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A geostationary satellite can now provide hourly NO2 vertical columns, and obtaining the NO2 vertical columns from space relies on NO2 vertical distribution from the chemical transport model (CTM). In this work, we update the CTM to better represent the chemistry environment so that the CTM can accurately provide NO2 vertical distribution. We also find that the changes in NO2 vertical distribution driven by a change in mixing depth play an important role in the NO2 column's diurnal variation.
Jiangchuan Tao, Biao Luo, Weiqi Xu, Gang Zhao, Hanbin Xu, Biao Xue, Miaomiao Zhai, Wanyun Xu, Huarong Zhao, Sanxue Ren, Guangsheng Zhou, Li Liu, Ye Kuang, and Yele Sun
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-840, https://doi.org/10.5194/acp-2022-840, 2023
Revised manuscript under review for ACP
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Using simultaneous measurements of DMA-CCNC, H/VTDMA and DMA-SP2, impacts of primary emissions and secondary aerosol formations on changes of aerosol physicochemical properties were comprehensively investigated. It was found that intercomparisons among aerosol mixing state parameters derived from different techniques can help getting more insights into aerosol physical properties which in turn will aid the investigation of emission characteristics and secondary aerosol formation pathways.
Shujun Zhong, Shuang Chen, Junjun Deng, Yanbing Fan, Qiang Zhang, Qiaorong Xie, Yulin Qi, Wei Hu, Libin Wu, Xiaodong Li, Chandra Mouli Pavuluri, Jialei Zhu, Xin Wang, Di Liu, Xiaole Pan, Yele Sun, Zifa Wang, Yisheng Xu, Haijie Tong, Hang Su, Yafang Cheng, Kimitaka Kawamura, and Pingqing Fu
Atmos. Chem. Phys., 23, 2061–2077, https://doi.org/10.5194/acp-23-2061-2023, https://doi.org/10.5194/acp-23-2061-2023, 2023
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This study investigated the role of the secondary organic aerosol (SOA) loading on the molecular composition of wintertime urban aerosols by ultrahigh-resolution mass spectrometry. Results demonstrate that the SOA loading is an important factor associated with the oxidation degree, nitrate group content, and chemodiversity of nitrooxy–organosulfates. Our study also found that the hydrolysis of nitrooxy–organosulfates is a possible pathway for the formation of organosulfates.
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.
Claudia Bernier, Yuxuan Wang, Guillaume Gronoff, Timothy Berkoff, K. Emma Knowland, John T. Sullivan, Ruben Delgado, Vanessa Caicedo, and Brian Carroll
Atmos. Chem. Phys., 22, 15313–15331, https://doi.org/10.5194/acp-22-15313-2022, https://doi.org/10.5194/acp-22-15313-2022, 2022
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Coastal regions are susceptible to variable and high ozone which is difficult to simulate. We developed a method to characterize large datasets of multi-dimensional measurements from lidar instruments taken in coastal regions. Using the clustered ozone groups, we evaluated model performance in simulating the coastal ozone variability vertically and diurnally. The approach allowed us to pinpoint areas where the models succeed in simulating coastal ozone and areas where there are still gaps.
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.
Qianjie Chen, Jessica A. Mirrielees, Sham Thanekar, Nicole A. Loeb, Rachel M. Kirpes, Lucia M. Upchurch, Anna J. Barget, Nurun Nahar Lata, Angela R. W. Raso, Stephen M. McNamara, Swarup China, Patricia K. Quinn, Andrew P. Ault, Aaron Kennedy, Paul B. Shepson, Jose D. Fuentes, and Kerri A. Pratt
Atmos. Chem. Phys., 22, 15263–15285, https://doi.org/10.5194/acp-22-15263-2022, https://doi.org/10.5194/acp-22-15263-2022, 2022
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During a spring field campaign in the coastal Arctic, ultrafine particles were enhanced during high wind speeds, and coarse-mode particles were reduced during blowing snow. Calculated periods blowing snow were overpredicted compared to observations. Sea spray aerosols produced by sea ice leads affected the composition of aerosols and snowpack. An improved understanding of aerosol emissions from leads and blowing snow is critical for predicting the future climate of the rapidly warming Arctic.
Cheng He, Xiao Lu, Haolin Wang, Haichao Wang, Yan Li, Guowen He, Yuanping He, Yurun Wang, Youlang Zhang, Yiming Liu, Qi Fan, and Shaojia Fan
Atmos. Chem. Phys., 22, 15243–15261, https://doi.org/10.5194/acp-22-15243-2022, https://doi.org/10.5194/acp-22-15243-2022, 2022
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We report that nocturnal ozone enhancement (NOE) events are observed at a high annual frequency of 41 % over 800 sites in China in 2014–2019 (about 50 % higher than that over Europe or the US). High daytime ozone provides a rich ozone source in the nighttime residual layer, determining the overall high frequency of NOE events in China, and enhanced atmospheric mixing then triggers NOE events by allowing the ozone-rich air in the residual layer to be mixed into the nighttime boundary layer.
William F. Swanson, Chris D. Holmes, William R. Simpson, Kaitlyn Confer, Louis Marelle, Jennie L. Thomas, Lyatt Jaeglé, Becky Alexander, Shuting Zhai, Qianjie Chen, Xuan Wang, and Tomás Sherwen
Atmos. Chem. Phys., 22, 14467–14488, https://doi.org/10.5194/acp-22-14467-2022, https://doi.org/10.5194/acp-22-14467-2022, 2022
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Radical bromine molecules are seen at higher concentrations during the Arctic spring. We use the global model GEOS-Chem to test whether snowpack and wind-blown snow sources can explain high bromine concentrations. We run this model for the entire year of 2015 and compare results to observations of bromine from floating platforms on the Arctic Ocean and at Utqiaġvik. We find that the model performs best when both sources are enabled but may overestimate bromine production in summer and fall.
Yuxuan Wang, Nan Lin, Wei Li, Alex Guenther, Joey C. Y. Lam, Amos P. K. Tai, Mark J. Potosnak, and Roger Seco
Atmos. Chem. Phys., 22, 14189–14208, https://doi.org/10.5194/acp-22-14189-2022, https://doi.org/10.5194/acp-22-14189-2022, 2022
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Drought can cause large changes in biogenic isoprene emissions. In situ field observations of isoprene emissions during droughts are confined by spatial coverage and, thus, provide limited constraints. We derived a drought stress factor based on satellite HCHO data for MEGAN2.1 in the GEOS-Chem model using water stress and temperature. This factor reduces the overestimation of isoprene emissions during severe droughts and improves the simulated O3 and organic aerosol responses to droughts.
Yuying Wang, Rong Hu, Qiuyan Wang, Zhanqing Li, Maureen Cribb, Yele Sun, Xiaorui Song, Yi Shang, Yixuan Wu, Xin Huang, and Yuxiang Wang
Atmos. Chem. Phys., 22, 14133–14146, https://doi.org/10.5194/acp-22-14133-2022, https://doi.org/10.5194/acp-22-14133-2022, 2022
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The mixing state of size-resolved soot particles and their influencing factors were investigated. The results suggest anthropogenic emissions and aging processes have diverse impacts on the mixing state of soot particles in different modes. Considering that the mixing state of soot particles is crucial to model aerosol absorption, this finding is important to study particle growth and the warming effect of black carbon aerosols.
Haolin Wang, Xiao Lu, Daniel J. Jacob, Owen R. Cooper, Kai-Lan Chang, Ke Li, Meng Gao, Yiming Liu, Bosi Sheng, Kai Wu, Tongwen Wu, Jie Zhang, Bastien Sauvage, Philippe Nédélec, Romain Blot, and Shaojia Fan
Atmos. Chem. Phys., 22, 13753–13782, https://doi.org/10.5194/acp-22-13753-2022, https://doi.org/10.5194/acp-22-13753-2022, 2022
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We report significant global tropospheric ozone increases in 1995–2017 based on extensive aircraft and ozonesonde observations. Using GEOS-Chem (Goddard Earth Observing System chemistry model) multi-decadal global simulations, we find that changes in global anthropogenic emissions, in particular the rapid increases in aircraft emissions, contribute significantly to the increases in tropospheric ozone and resulting radiative impact.
Futing Wang, Ting Yang, Zifa Wang, Haibo Wang, Xi Chen, Yele Sun, Jianjun Li, Guigang Tang, and Wenxuan Chai
Atmos. Meas. Tech., 15, 6127–6144, https://doi.org/10.5194/amt-15-6127-2022, https://doi.org/10.5194/amt-15-6127-2022, 2022
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We develop a new algorithm to get the vertical mass concentration profiles of fine aerosol components based on the synergy of ground-based remote sensing for the first time. The comparisons with in situ observations and chemistry transport models validate the performance of the algorithm. Uncertainties caused by input parameters are also assessed in this paper. We expected that the algorithm can provide a new idea for lidar inversion and promote the development of aerosol component profiles.
Yanzhi Cao, Zhuang Jiang, Becky Alexander, Jihong Cole-Dai, Joel Savarino, Joseph Erbland, and Lei Geng
Atmos. Chem. Phys., 22, 13407–13422, https://doi.org/10.5194/acp-22-13407-2022, https://doi.org/10.5194/acp-22-13407-2022, 2022
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We investigate the potential of ice-core preserved nitrate isotopes as proxies of stratospheric ozone variability by measuring nitrate isotopes in a shallow ice core from the South Pole. The large variability in the snow accumulation rate and its slight increase after the 1970s masked any signals caused by the ozone hole. Moreover, the nitrate oxygen isotope decrease may reflect changes in the atmospheric oxidation environment in the Southern Ocean.
Elizabeth Klovenski, Yuxuan Wang, Susanne E. Bauer, Kostas Tsigaridis, Greg Faluvegi, Igor Aleinov, Nancy Y. Kiang, Alex Guenther, Xiaoyan Jiang, Wei Li, and Nan Lin
Atmos. Chem. Phys., 22, 13303–13323, https://doi.org/10.5194/acp-22-13303-2022, https://doi.org/10.5194/acp-22-13303-2022, 2022
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Severe drought stresses vegetation and causes reduced emission of isoprene. We study the impact of including a new isoprene drought stress (yd) parameterization in NASA GISS ModelE called DroughtStress_ModelE, which is specifically tuned for ModelE. Inclusion of yd leads to better simulated isoprene emissions at the MOFLUX site during the severe drought of 2012, reduced overestimation of OMI satellite ΩHCHO (formaldehyde column), and improved simulated O3 (ozone) during drought.
Chao Yan, Yicheng Shen, Dominik Stolzenburg, Lubna Dada, Ximeng Qi, Simo Hakala, Anu-Maija Sundström, Yishuo Guo, Antti Lipponen, Tom V. Kokkonen, Jenni Kontkanen, Runlong Cai, Jing Cai, Tommy Chan, Liangduo Chen, Biwu Chu, Chenjuan Deng, Wei Du, Xiaolong Fan, Xu-Cheng He, Juha Kangasluoma, Joni Kujansuu, Mona Kurppa, Chang Li, Yiran Li, Zhuohui Lin, Yiliang Liu, Yuliang Liu, Yiqun Lu, Wei Nie, Jouni Pulliainen, Xiaohui Qiao, Yonghong Wang, Yifan Wen, Ye Wu, Gan Yang, Lei Yao, Rujing Yin, Gen Zhang, Shaojun Zhang, Feixue Zheng, Ying Zhou, Antti Arola, Johanna Tamminen, Pauli Paasonen, Yele Sun, Lin Wang, Neil M. Donahue, Yongchun Liu, Federico Bianchi, Kaspar R. Daellenbach, Douglas R. Worsnop, Veli-Matti Kerminen, Tuukka Petäjä, Aijun Ding, Jingkun Jiang, and Markku Kulmala
Atmos. Chem. Phys., 22, 12207–12220, https://doi.org/10.5194/acp-22-12207-2022, https://doi.org/10.5194/acp-22-12207-2022, 2022
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Atmospheric new particle formation (NPF) is a dominant source of atmospheric ultrafine particles. In urban environments, traffic emissions are a major source of primary pollutants, but their contribution to NPF remains under debate. During the COVID-19 lockdown, traffic emissions were significantly reduced, providing a unique chance to examine their relevance to NPF. Based on our comprehensive measurements, we demonstrate that traffic emissions alone are not able to explain the NPF in Beijing.
Mengying Li, Shaocai Yu, Xue Chen, Zhen Li, Yibo Zhang, Zhe Song, Weiping Liu, Pengfei Li, Xiaoye Zhang, Meigen Zhang, Yele Sun, Zirui Liu, Caiping Sun, Jingkun Jiang, Shuxiao Wang, Benjamin N. Murphy, Kiran Alapaty, Rohit Mathur, Daniel Rosenfeld, and John H. Seinfeld
Atmos. Chem. Phys., 22, 11845–11866, https://doi.org/10.5194/acp-22-11845-2022, https://doi.org/10.5194/acp-22-11845-2022, 2022
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This study constructed an emission inventory of condensable particulate matter (CPM) in China with a focus on organic aerosols (OAs), based on collected CPM emission information. The results show that OA emissions are enhanced twofold for the years 2014 and 2017 after the inclusion of CPM in the new inventory. Sensitivity cases demonstrated the significant contributions of CPM emissions from stationary combustion and mobile sources to primary, secondary, and total OA concentrations.
Lu Shen, Ritesh Gautam, Mark Omara, Daniel Zavala-Araiza, Joannes D. Maasakkers, Tia R. Scarpelli, Alba Lorente, David Lyon, Jianxiong Sheng, Daniel J. Varon, Hannah Nesser, Zhen Qu, Xiao Lu, Melissa P. Sulprizio, Steven P. Hamburg, and Daniel J. Jacob
Atmos. Chem. Phys., 22, 11203–11215, https://doi.org/10.5194/acp-22-11203-2022, https://doi.org/10.5194/acp-22-11203-2022, 2022
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We use 22 months of TROPOMI satellite observations to quantity methane emissions from the oil (O) and natural gas (G) sector in the US and Canada at the scale of both individual basins as well as country-wide aggregates. We find that O/G-related methane emissions are underestimated in these inventories by 80 % for the US and 40 % for Canada, and 70 % of the underestimate in the US is from five O/G basins, including Permian, Haynesville, Anadarko, Eagle Ford, and Barnett.
Zichong Chen, Daniel J. Jacob, Hannah Nesser, Melissa P. Sulprizio, Alba Lorente, Daniel J. Varon, Xiao Lu, Lu Shen, Zhen Qu, Elise Penn, and Xueying Yu
Atmos. Chem. Phys., 22, 10809–10826, https://doi.org/10.5194/acp-22-10809-2022, https://doi.org/10.5194/acp-22-10809-2022, 2022
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We quantify methane emissions in China and contributions from different sectors by inverse analysis of 2019 TROPOMI satellite observations of atmospheric methane. We find that anthropogenic methane emissions for China are underestimated in the national inventory. Our estimate of emissions indicates a small life-cycle loss rate, implying net climate benefits from the current
coal-to-gasenergy transition in China. However, this small loss rate can be misleading given China's high gas imports.
Zhiqiang Zhang, Yele Sun, Chun Chen, Bo You, Aodong Du, Weiqi Xu, Yan Li, Zhijie Li, Lu Lei, Wei Zhou, Jiaxing Sun, Yanmei Qiu, Lianfang Wei, Pingqing Fu, and Zifa Wang
Atmos. Chem. Phys., 22, 10409–10423, https://doi.org/10.5194/acp-22-10409-2022, https://doi.org/10.5194/acp-22-10409-2022, 2022
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We present a comprehensive characterization of water-soluble organic aerosol and the first mass spectral characterization of water-insoluble organic aerosol in the cold season in Beijing by integrating online and offline aerosol mass spectrometer measurements. WSOA comprised dominantly secondary OA and showed large changes during the transition season from autumn to winter. WIOA was characterized by prominent hydrocarbon ions series, low oxidation states, and significant day–night differences.
Xueyin Ruan, Chun Zhao, Rahul A. Zaveri, Pengzhen He, Xinming Wang, Jingyuan Shao, and Lei Geng
Geosci. Model Dev., 15, 6143–6164, https://doi.org/10.5194/gmd-15-6143-2022, https://doi.org/10.5194/gmd-15-6143-2022, 2022
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Accurate prediction of aerosol pH in chemical transport models is essential to aerosol modeling. This study examines the performance of the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) on aerosol pH predictions and the sensitivities to emissions of nonvolatile cations and NH3, aerosol-phase state assumption, and heterogeneous sulfate production. Temporal evolution of aerosol pH during haze cycles in Beijing and the driving factors are also presented and discussed.
Daniel J. Varon, Daniel J. Jacob, Melissa Sulprizio, Lucas A. Estrada, William B. Downs, Lu Shen, Sarah E. Hancock, Hannah Nesser, Zhen Qu, Elise Penn, Zichong Chen, Xiao Lu, Alba Lorente, Ashutosh Tewari, and Cynthia A. Randles
Geosci. Model Dev., 15, 5787–5805, https://doi.org/10.5194/gmd-15-5787-2022, https://doi.org/10.5194/gmd-15-5787-2022, 2022
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Reducing atmospheric methane emissions is critical to slow near-term climate change. Globally surveying satellite instruments like the TROPOspheric Monitoring Instrument (TROPOMI) have unique capabilities for monitoring atmospheric methane around the world. Here we present a user-friendly cloud-computing tool that enables researchers and stakeholders to quantify methane emissions across user-selected regions of interest using TROPOMI satellite observations.
Zhuang Jiang, Joel Savarino, Becky Alexander, Joseph Erbland, Jean-Luc Jaffrezo, and Lei Geng
The Cryosphere, 16, 2709–2724, https://doi.org/10.5194/tc-16-2709-2022, https://doi.org/10.5194/tc-16-2709-2022, 2022
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A record of year-round atmospheric nitrate isotopic composition along with snow nitrate isotopic data from Summit, Greenland, revealed apparent enrichments in nitrogen isotopes in snow nitrate compared to atmospheric nitrate, in addition to a relatively smaller degree of changes in oxygen isotopes. The results suggest that at this site post-depositional processing takes effect, which should be taken into account when interpreting ice-core nitrate isotope records.
Wei Li and Yuxuan Wang
Atmos. Chem. Phys., 22, 7843–7859, https://doi.org/10.5194/acp-22-7843-2022, https://doi.org/10.5194/acp-22-7843-2022, 2022
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Fine dust is an important component of PM2.5 and can be largely modulated by droughts. In contrast to the increase in dust in the southwest USA where major dust sources are located, dust in the southeast USA is affected more by long-range transport from Africa and decreases under droughts. Both the transport and emissions of African dust are weakened when the southeast USA is under droughts, which reveals how regional-scale droughts can influence aerosol abundance through long-range transport.
Jiaxing Sun, Yele Sun, Conghui Xie, Weiqi Xu, Chun Chen, Zhe Wang, Lei Li, Xubing Du, Fugui Huang, Yan Li, Zhijie Li, Xiaole Pan, Nan Ma, Wanyun Xu, Pingqing Fu, and Zifa Wang
Atmos. Chem. Phys., 22, 7619–7630, https://doi.org/10.5194/acp-22-7619-2022, https://doi.org/10.5194/acp-22-7619-2022, 2022
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We analyzed the chemical composition and mixing state of BC-containing particles at urban and rural sites in winter in the North China Plain and evaluated their impact on light absorption enhancement. BC was dominantly mixed with organic carbon, nitrate, and sulfate, and the mixing state evolved significantly as a function of relative humidity (RH) at both sites. The absorption enhancement depended strongly on coated secondary inorganic aerosol and was up to ~1.3–1.4 during aging processes.
Chenhong Zhou, Fan Wang, Yike Guo, Cheng Liu, Dongsheng Ji, Yuesi Wang, Xiaobin Xu, Xiao Lu, Yan Wang, Gregory Carmichael, and Meng Gao
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2022-187, https://doi.org/10.5194/essd-2022-187, 2022
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We develop an eXtreme Gradient Boosting (XGBoost) model integrating high-resolution meteorological data, satellite retrievals of trace gases, etc. to provide reconstructed daily ground-level O3 over 2005–2021 in China. It can facilitate climatological, ecological, and health research. The dataset is freely available at Zenodo (https://zenodo.org/record/6507706#.Yo8hKujP13g; Zhou, 2022).
Junjun Deng, Hao Ma, Xinfeng Wang, Shujun Zhong, Zhimin Zhang, Jialei Zhu, Yanbing Fan, Wei Hu, Libin Wu, Xiaodong Li, Lujie Ren, Chandra Mouli Pavuluri, Xiaole Pan, Yele Sun, Zifa Wang, Kimitaka Kawamura, and Pingqing Fu
Atmos. Chem. Phys., 22, 6449–6470, https://doi.org/10.5194/acp-22-6449-2022, https://doi.org/10.5194/acp-22-6449-2022, 2022
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Light-absorbing brown carbon (BrC) plays an important role in climate change and atmospheric chemistry. Here we investigated the seasonal and diurnal variations in water-soluble BrC in PM2.5 in the megacity Tianjin in coastal China. Results of the source apportionments from the combination with organic molecular compositions and optical properties of water-soluble BrC reveal a large contribution from primary bioaerosol particles to BrC in the urban atmosphere.
Jingnan Shi, Juan Hong, Nan Ma, Qingwei Luo, Yao He, Hanbing Xu, Haobo Tan, Qiaoqiao Wang, Jiangchuan Tao, Yaqing Zhou, Shuang Han, Long Peng, Linhong Xie, Guangsheng Zhou, Wanyun Xu, Yele Sun, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 22, 4599–4613, https://doi.org/10.5194/acp-22-4599-2022, https://doi.org/10.5194/acp-22-4599-2022, 2022
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In this study, we investigated the hygroscopicity of submicron aerosols at a rural site in the North China Plain during the winter of 2018, using a HTDMA and a CV-ToF-ACSM. We observed differences in aerosol hygroscopicity during two distinct episodes with different primary emissions and secondary aerosol formation processes. These results provide an improved understanding of the complex influence of sources and aerosol evolution processes on their hygroscopicity.
Han Zang, Yue Zhao, Juntao Huo, Qianbiao Zhao, Qingyan Fu, Yusen Duan, Jingyuan Shao, Cheng Huang, Jingyu An, Likun Xue, Ziyue Li, Chenxi Li, and Huayun Xiao
Atmos. Chem. Phys., 22, 4355–4374, https://doi.org/10.5194/acp-22-4355-2022, https://doi.org/10.5194/acp-22-4355-2022, 2022
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Particulate nitrate plays an important role in wintertime haze pollution in eastern China, yet quantitative constraints on detailed nitrate formation mechanisms remain limited. Here we quantified the contributions of the heterogeneous N2O5 hydrolysis (66 %) and gas-phase OH + NO2 reaction (32 %) to nitrate formation in this region and identified the atmospheric oxidation capacity (i.e., availability of O3 and OH radicals) as the driving factor of nitrate formation from both processes.
Tia R. Scarpelli, Daniel J. Jacob, Shayna Grossman, Xiao Lu, Zhen Qu, Melissa P. Sulprizio, Yuzhong Zhang, Frances Reuland, Deborah Gordon, and John R. Worden
Atmos. Chem. Phys., 22, 3235–3249, https://doi.org/10.5194/acp-22-3235-2022, https://doi.org/10.5194/acp-22-3235-2022, 2022
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We present a spatially explicit version of the national inventories of oil, gas, and coal methane emissions as submitted by individual countries to the United Nations Framework Convention on Climate Change (UNFCCC) in 2021. We then use atmospheric modeling to compare our inventory emissions to atmospheric methane observations with the goal of identifying potential under- and overestimates of oil–gas methane emissions in the national inventories.
Kathryn D. Kulju, Stephen M. McNamara, Qianjie Chen, Hannah S. Kenagy, Jacinta Edebeli, Jose D. Fuentes, Steven B. Bertman, and Kerri A. Pratt
Atmos. Chem. Phys., 22, 2553–2568, https://doi.org/10.5194/acp-22-2553-2022, https://doi.org/10.5194/acp-22-2553-2022, 2022
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N2O5 uptake by chloride-containing surfaces produces ClNO2, which photolyzes, producing NO2 and highly reactive Cl radicals that impact air quality. In the inland urban atmosphere, ClNO2 was elevated during lower air turbulence and over snow-covered ground, from snowpack ClNO2 production. N2O5 and ClNO2 levels were lowest, on average, during rainfall and fog because of scavenging, with N2O5 scavenging by fog droplets likely contributing to observed increased particulate nitrate concentrations.
Dianyi Li, Drew Shindell, Dian Ding, Xiao Lu, Lin Zhang, and Yuqiang Zhang
Atmos. Chem. Phys., 22, 2625–2638, https://doi.org/10.5194/acp-22-2625-2022, https://doi.org/10.5194/acp-22-2625-2022, 2022
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In this study, we applied chemical transport model simulation with the latest annual anthropogenic emission inventory to study the long-term trend of ozone-induced crop production losses from 2010 to 2017 in China. We find that overall the ozone-induced crop production loss in China is significant and the annual average economic losses for wheat, rice, maize, and soybean in China are USD 9.55 billion, USD 8.53 billion, USD 2.23 billion, and USD 1.16 billion respectively, over the 8 years.
Jing Cai, Cheng Wu, Jiandong Wang, Wei Du, Feixue Zheng, Simo Hakala, Xiaolong Fan, Biwu Chu, Lei Yao, Zemin Feng, Yongchun Liu, Yele Sun, Jun Zheng, Chao Yan, Federico Bianchi, Markku Kulmala, Claudia Mohr, and Kaspar R. Daellenbach
Atmos. Chem. Phys., 22, 1251–1269, https://doi.org/10.5194/acp-22-1251-2022, https://doi.org/10.5194/acp-22-1251-2022, 2022
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This study investigates the connection between organic aerosol (OA) molecular composition and particle absorptive properties in autumn in Beijing. We find that the molecular properties of OA compounds in different episodes influence particle light absorption properties differently: the light absorption enhancement of black carbon and light absorption coefficient of brown carbon were mostly related to more oxygenated OA (low C number and four O atoms) and aromatics/nitro-aromatics, respectively.
Haiyue Tan, Lin Zhang, Xiao Lu, Yuanhong Zhao, Bo Yao, Robert J. Parker, and Hartmut Boesch
Atmos. Chem. Phys., 22, 1229–1249, https://doi.org/10.5194/acp-22-1229-2022, https://doi.org/10.5194/acp-22-1229-2022, 2022
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Methane is the second most important anthropogenic greenhouse gas. Understanding methane emissions and concentration growth over China in the past decade is important to support its mitigation. This study analyzes the contributions of methane emissions from different regions and sources over the globe to methane changes over China in 2007–2018. Our results show strong international transport influences and emphasize the need of intensive methane measurements covering eastern China.
Jiaxing Sun, Zhe Wang, Wei Zhou, Conghui Xie, Cheng Wu, Chun Chen, Tingting Han, Qingqing Wang, Zhijie Li, Jie Li, Pingqing Fu, Zifa Wang, and Yele Sun
Atmos. Chem. Phys., 22, 561–575, https://doi.org/10.5194/acp-22-561-2022, https://doi.org/10.5194/acp-22-561-2022, 2022
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We analyzed 9-year measurements of BC and aerosol optical properties from 2012 to 2020 in Beijing, China. Our results showed large reductions in BC and light extinction coefficient due to the Clean Air Action Plan. As a response, both SSA and mass extinction efficiency (MEE) showed considerable increases, demonstrating a future challenge in visibility improvement. The primary and secondary BrC was also separated and quantified, and the changes in radiative forcing of BC and BrC were estimated.
Xiao Lu, Daniel J. Jacob, Haolin Wang, Joannes D. Maasakkers, Yuzhong Zhang, Tia R. Scarpelli, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Hannah Nesser, A. Anthony Bloom, Shuang Ma, John R. Worden, Shaojia Fan, Robert J. Parker, Hartmut Boesch, Ritesh Gautam, Deborah Gordon, Michael D. Moran, Frances Reuland, Claudia A. Octaviano Villasana, and Arlyn Andrews
Atmos. Chem. Phys., 22, 395–418, https://doi.org/10.5194/acp-22-395-2022, https://doi.org/10.5194/acp-22-395-2022, 2022
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We evaluate methane emissions and trends for 2010–2017 in the gridded national emission inventories for the United States, Canada, and Mexico by inversion of in situ and satellite methane observations. We find that anthropogenic methane emissions for all three countries are underestimated in the national inventories, largely driven by oil emissions. Anthropogenic methane emissions in the US peak in 2014, in contrast to the report of a steadily decreasing trend over 2010–2017 from the US EPA.
Youwen Sun, Hao Yin, Xiao Lu, Justus Notholt, Mathias Palm, Cheng Liu, Yuan Tian, and Bo Zheng
Atmos. Chem. Phys., 21, 18589–18608, https://doi.org/10.5194/acp-21-18589-2021, https://doi.org/10.5194/acp-21-18589-2021, 2021
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This study uses high-resolution nested-grid GEOS-Chem simulation, the eXtreme Gradient Boosting (XGBoost) machine learning method, and the exposure–response relationship to determine the drivers and evaluate the health risks of the unexpected surface O3 enhancements over the Sichuan Basin in 2020. These unexpected O3 enhancements were induced by meteorological anomalies and caused dramatically high health risks.
Yuting Zhang, Hang Liu, Shandong Lei, Wanyun Xu, Yu Tian, Weijie Yao, Xiaoyong Liu, Qi Liao, Jie Li, Chun Chen, Yele Sun, Pingqing Fu, Jinyuan Xin, Junji Cao, Xiaole Pan, and Zifa Wang
Atmos. Chem. Phys., 21, 17631–17648, https://doi.org/10.5194/acp-21-17631-2021, https://doi.org/10.5194/acp-21-17631-2021, 2021
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In this study, the authors used a single-particle soot photometer (SP2) to characterize the particle size, mixing state, and optical properties of black carbon aerosols in rural areas of the North China Plain in winter. Relatively warm and high-RH environments (RH > 50 %, −4° < T < 4 °) were more favorable to rBC aging than dry and cold environments (RH < 60 %, T < −8°). The paper emphasizes the importance of meteorological parameters in the mixing state of black carbon.
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.
Ruqian Miao, Qi Chen, Manish Shrivastava, Youfan Chen, Lin Zhang, Jianlin Hu, Yan Zheng, and Keren Liao
Atmos. Chem. Phys., 21, 16183–16201, https://doi.org/10.5194/acp-21-16183-2021, https://doi.org/10.5194/acp-21-16183-2021, 2021
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We apply process-based and observation-constrained schemes to simulate organic aerosol in China and conduct comprehensive model–observation comparisons. The results show that anthropogenic semivolatile and intermediate-volatility organic compounds (SVOCs and IVOCs) are the main sources of secondary organic aerosol (SOA) in polluted regions, for which the residential sector is perhaps the predominant contributor. The hydroxyl radical level is also important for SOA modeling in polluted regions.
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.
Sihui Jiang, Fang Zhang, Jingye Ren, Lu Chen, Xing Yan, Jieyao Liu, Yele Sun, and Zhanqing Li
Atmos. Chem. Phys., 21, 14293–14308, https://doi.org/10.5194/acp-21-14293-2021, https://doi.org/10.5194/acp-21-14293-2021, 2021
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New particle formation (NPF) can be a large source of CCN and affect weather and climate. Here we show that the NPF contributes largely to cloud droplet number concentration (Nd) but is suppressed at high particle number concentrations in Beijing due to water vapor competition. We also reveal a considerable impact of primary sources on the evaluation in the urban atmosphere. Our study has great significance for assessing NPF-associated effects on climate in polluted regions.
Zhen Qu, Daniel J. Jacob, Lu Shen, Xiao Lu, Yuzhong Zhang, Tia R. Scarpelli, Hannah Nesser, Melissa P. Sulprizio, Joannes D. Maasakkers, A. Anthony Bloom, John R. Worden, Robert J. Parker, and Alba L. Delgado
Atmos. Chem. Phys., 21, 14159–14175, https://doi.org/10.5194/acp-21-14159-2021, https://doi.org/10.5194/acp-21-14159-2021, 2021
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The recent launch of TROPOMI offers an unprecedented opportunity to quantify the methane budget from a top-down perspective. We use TROPOMI and the more mature GOSAT methane observations to estimate methane emissions and get consistent global budgets. However, TROPOMI shows biases over regions where surface albedo is small and provides less information for the coarse-resolution inversion due to the larger error correlations and spatial variations in the number of observations.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Andreas Tilgner, Thomas Schaefer, Becky Alexander, Mary Barth, Jeffrey L. Collett Jr., Kathleen M. Fahey, Athanasios Nenes, Havala O. T. Pye, Hartmut Herrmann, and V. Faye McNeill
Atmos. Chem. Phys., 21, 13483–13536, https://doi.org/10.5194/acp-21-13483-2021, https://doi.org/10.5194/acp-21-13483-2021, 2021
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Feedbacks of acidity and atmospheric multiphase chemistry in deliquesced particles and clouds are crucial for the tropospheric composition, depositions, climate, and human health. This review synthesizes the current scientific knowledge on these feedbacks using both inorganic and organic aqueous-phase chemistry. Finally, this review outlines atmospheric implications and highlights the need for future investigations with respect to reducing emissions of key acid precursors in a changing world.
Zhuang Jiang, Becky Alexander, Joel Savarino, Joseph Erbland, and Lei Geng
The Cryosphere, 15, 4207–4220, https://doi.org/10.5194/tc-15-4207-2021, https://doi.org/10.5194/tc-15-4207-2021, 2021
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We used a snow photochemistry model (TRANSITS) to simulate the seasonal nitrate snow profile at Summit, Greenland. Comparisons between model outputs and observations suggest that at Summit post-depositional processing is active and probably dominates the snowpack δ15N seasonality. We also used the model to assess the degree of snow nitrate loss and the consequences in its isotopes at present and in the past, which helps for quantitative interpretations of ice-core nitrate records.
Hong Ren, Wei Hu, Lianfang Wei, Siyao Yue, Jian Zhao, Linjie Li, Libin Wu, Wanyu Zhao, Lujie Ren, Mingjie Kang, Qiaorong Xie, Sihui Su, Xiaole Pan, Zifa Wang, Yele Sun, Kimitaka Kawamura, and Pingqing Fu
Atmos. Chem. Phys., 21, 12949–12963, https://doi.org/10.5194/acp-21-12949-2021, https://doi.org/10.5194/acp-21-12949-2021, 2021
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This study presents vertical profiles of biogenic and anthropogenic secondary organic aerosols (SOAs) in the urban boundary layer based on a 325 m tower in Beijing in late summer. The increases in the isoprene and toluene SOAs with height were found to be more related to regional transport, whereas the decrease in those from monoterpenes and sesquiterpene were more subject to local emissions. Such complicated vertical distributions of SOA should be considered in future modeling work.
Youwen Sun, Hao Yin, Cheng Liu, Emmanuel Mahieu, Justus Notholt, Yao Té, Xiao Lu, Mathias Palm, Wei Wang, Changgong Shan, Qihou Hu, Min Qin, Yuan Tian, and Bo Zheng
Atmos. Chem. Phys., 21, 11759–11779, https://doi.org/10.5194/acp-21-11759-2021, https://doi.org/10.5194/acp-21-11759-2021, 2021
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The variability, sources, and transport of ethane (C2H6) over eastern China from 2015 to 2020 were studied using ground-based Fourier transform infrared (FTIR) spectroscopy and GEOS-Chem simulations. C2H6 variability is driven by both meteorological and emission factors. The reduction in C2H6 in recent years over eastern China points to air quality improvement in China.
Yang Yang, Minqiang Zhou, Ting Wang, Bo Yao, Pengfei Han, Denghui Ji, Wei Zhou, Yele Sun, Gengchen Wang, and Pucai Wang
Atmos. Chem. Phys., 21, 11741–11757, https://doi.org/10.5194/acp-21-11741-2021, https://doi.org/10.5194/acp-21-11741-2021, 2021
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This study introduces the in situ CO2 measurement system installed in Beijing (urban), Xianghe (suburban), and Xinglong (rural) in North China for the first time. The spatial and temporal variations in CO2 mole fractions at the three sites between June 2018 and April 2020 are discussed on both seasonal and diurnal scales.
Yadong Lei, Xu Yue, Hong Liao, Lin Zhang, Yang Yang, Hao Zhou, Chenguang Tian, Cheng Gong, Yimian Ma, Lan Gao, and Yang Cao
Atmos. Chem. Phys., 21, 11531–11543, https://doi.org/10.5194/acp-21-11531-2021, https://doi.org/10.5194/acp-21-11531-2021, 2021
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We present the first estimate of ozone enhancement by fire emissions through ozone–vegetation interactions using a fully coupled chemistry–vegetation model (GC-YIBs). In fire-prone areas, fire-induced ozone causes a positive feedback to surface ozone mainly because of the inhibition effects on stomatal conductance.
Qiaorong Xie, Sihui Su, Jing Chen, Yuqing Dai, Siyao Yue, Hang Su, Haijie Tong, Wanyu Zhao, Lujie Ren, Yisheng Xu, Dong Cao, Ying Li, Yele Sun, Zifa Wang, Cong-Qiang Liu, Kimitaka Kawamura, Guibin Jiang, Yafang Cheng, and Pingqing Fu
Atmos. Chem. Phys., 21, 11453–11465, https://doi.org/10.5194/acp-21-11453-2021, https://doi.org/10.5194/acp-21-11453-2021, 2021
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This study investigated the role of nighttime chemistry during Chinese New Year's Eve that enhances the formation of nitrooxy organosulfates in the aerosol phase. Results show that anthropogenic precursors, together with biogenic ones, considerably contribute to the formation of low-volatility nitrooxy OSs. Our study provides detailed molecular composition of firework-related aerosols, which gives new insights into the physicochemical properties and potential health effects of urban aerosols.
Meng Gao, Yang Yang, Hong Liao, Bin Zhu, Yuxuan Zhang, Zirui Liu, Xiao Lu, Chen Wang, Qiming Zhou, Yuesi Wang, Qiang Zhang, Gregory R. Carmichael, and Jianlin Hu
Atmos. Chem. Phys., 21, 11405–11421, https://doi.org/10.5194/acp-21-11405-2021, https://doi.org/10.5194/acp-21-11405-2021, 2021
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Light absorption and radiative forcing of black carbon (BC) is influenced by both BC itself and its interactions with other aerosol chemical compositions. In this study, we used the online coupled WRF-Chem model to examine how emission control measures during the Asian-Pacific Economic Cooperation (APEC) conference affect the mixing state and light absorption of BC and the associated implications for BC-PBL interactions.
Ying Wei, Xueshun Chen, Huansheng Chen, Yele Sun, Wenyi Yang, Huiyun Du, Qizhong Wu, Dan Chen, Xiujuan Zhao, Jie Li, and Zifa Wang
Geosci. Model Dev., 14, 4411–4428, https://doi.org/10.5194/gmd-14-4411-2021, https://doi.org/10.5194/gmd-14-4411-2021, 2021
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The sub-grid particle formation (SGPF) in plumes plays an important role in air pollution and climate. We coupled an SGPF scheme to a chemical transport model with an aerosol microphysics module and applied it to investigate the SGPF impact over China. The scheme clearly improved the model performance in simulating aerosol components and particle number at typical sites influenced by point sources. The results indicate the significant effects of SGPF on aerosol particles in industrial areas.
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.
Xueshun Chen, Fangqun Yu, Wenyi Yang, Yele Sun, Huansheng Chen, Wei Du, Jian Zhao, Ying Wei, Lianfang Wei, Huiyun Du, Zhe Wang, Qizhong Wu, Jie Li, Junling An, and Zifa Wang
Atmos. Chem. Phys., 21, 9343–9366, https://doi.org/10.5194/acp-21-9343-2021, https://doi.org/10.5194/acp-21-9343-2021, 2021
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Atmospheric aerosol particles have significant climate and health effects that depend on aerosol size, composition, and mixing state. A new global-regional nested aerosol model with an advanced particle microphysics module and a volatility basis set organic aerosol module was developed to simulate aerosol microphysical processes. Simulations strongly suggest the important role of anthropogenic organic species in particle formation over the areas influenced by anthropogenic sources.
Youwen Sun, Hao Yin, Yuan Cheng, Qianggong Zhang, Bo Zheng, Justus Notholt, Xiao Lu, Cheng Liu, Yuan Tian, and Jianguo Liu
Atmos. Chem. Phys., 21, 9201–9222, https://doi.org/10.5194/acp-21-9201-2021, https://doi.org/10.5194/acp-21-9201-2021, 2021
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We quantified the variability, source, and transport of urban CO over the Himalayas and Tibetan Plateau (HTP) by using measurement, model simulation, and the analysis of meteorological fields. Urban CO over the HTP is dominated by anthropogenic and biomass burning emissions from local, South Asia and East Asia, and oxidation sources. The decreasing trends in surface CO since 2015 in most cities over the HTP are attributed to the reduction in local and transported CO emissions in recent years.
Kun Wang, Shohei Hattori, Mang Lin, Sakiko Ishino, Becky Alexander, Kazuki Kamezaki, Naohiro Yoshida, and Shichang Kang
Atmos. Chem. Phys., 21, 8357–8376, https://doi.org/10.5194/acp-21-8357-2021, https://doi.org/10.5194/acp-21-8357-2021, 2021
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Sulfate aerosols play an important climatic role and exert adverse effects on the ecological environment and human health. In this study, we present the triple oxygen isotopic composition of sulfate from the Mt. Everest region, southern Tibetan Plateau, and decipher the formation mechanisms of atmospheric sulfate in this pristine environment. The results indicate the important role of the S(IV) + O3 pathway in atmospheric sulfate formation promoted by conditions of high cloud water pH.
Siqi Hou, Di Liu, Jingsha Xu, Tuan V. Vu, Xuefang Wu, Deepchandra Srivastava, Pingqing Fu, Linjie Li, Yele Sun, Athanasia Vlachou, Vaios Moschos, Gary Salazar, Sönke Szidat, André S. H. Prévôt, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 21, 8273–8292, https://doi.org/10.5194/acp-21-8273-2021, https://doi.org/10.5194/acp-21-8273-2021, 2021
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This study provides a newly developed method which combines radiocarbon (14C) with organic tracers to enable source apportionment of primary and secondary fossil vs. non-fossil sources of carbonaceous aerosols at an urban and a rural site of Beijing. The source apportionment results were compared with those by chemical mass balance and AMS/ACSM-PMF methods. Correlations of WINSOC and WSOC with different sources of OC were also performed to elucidate the formation mechanisms of SOC.
Weiqi Xu, Masayuki Takeuchi, Chun Chen, Yanmei Qiu, Conghui Xie, Wanyun Xu, Nan Ma, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Meas. Tech., 14, 3693–3705, https://doi.org/10.5194/amt-14-3693-2021, https://doi.org/10.5194/amt-14-3693-2021, 2021
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Here we developed a method for estimation of particulate organic nitrates (pON) from the measurements of a high-resolution aerosol mass spectrometer coupled with a thermodenuder based on the volatility differences between inorganic nitrate and pON. The results generally had improvements in reducing negative values due to the influences of a high concentration of inorganic nitrate and a constant ratio of NO+ to NO2+ of organic nitrates (RON).
Jiangchuan Tao, Ye Kuang, Nan Ma, Juan Hong, Yele Sun, Wanyun Xu, Yanyan Zhang, Yao He, Qingwei Luo, Linhong Xie, Hang Su, and Yafang Cheng
Atmos. Chem. Phys., 21, 7409–7427, https://doi.org/10.5194/acp-21-7409-2021, https://doi.org/10.5194/acp-21-7409-2021, 2021
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The mechanism of secondary aerosol (SA) formation can be affected by relative humidity (RH) and has different influences on the particle CCN activity under different RH conditions. In the North China Plain, we find different responses of CCN activity and enhancements of CCN number concentration to SA formation under different RH conditions. In addition, variations of aerosol mixing state due to SA formation contribute some of the largest uncertainties in predicting CCN number concentration.
Jingsha Xu, Di Liu, Xuefang Wu, Tuan V. Vu, Yanli Zhang, Pingqing Fu, Yele Sun, Weiqi Xu, Bo Zheng, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 21, 7321–7341, https://doi.org/10.5194/acp-21-7321-2021, https://doi.org/10.5194/acp-21-7321-2021, 2021
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Source apportionment of fine aerosols in an urban site of Beijing used a chemical mass balance (CMB) model. Seven primary sources (industrial/residential coal burning, biomass burning, gasoline/diesel vehicles, cooking and vegetative detritus) explained an average of 75.7 % and 56.1 % of fine OC in winter and summer, respectively. CMB was found to resolve more primary OA sources than AMS-PMF, but the latter apportioned more secondary OA sources.
Youwen Sun, Hao Yin, Cheng Liu, Lin Zhang, Yuan Cheng, Mathias Palm, Justus Notholt, Xiao Lu, Corinne Vigouroux, Bo Zheng, Wei Wang, Nicholas Jones, Changong Shan, Min Qin, Yuan Tian, Qihou Hu, Fanhao Meng, and Jianguo Liu
Atmos. Chem. Phys., 21, 6365–6387, https://doi.org/10.5194/acp-21-6365-2021, https://doi.org/10.5194/acp-21-6365-2021, 2021
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This study mapped the drivers of HCHO variability from 2015 to 2019 over eastern China. Hydroxyl (OH) radical production rates from HCHO photolysis were evaluated. The relative contributions of emitted and photochemical sources to the observed HCHO abundance were analyzed. Contributions of various emission sources and geographical regions to the observed HCHO summertime enhancements were determined.
Athanasios Nenes, Spyros N. Pandis, Maria Kanakidou, Armistead G. Russell, Shaojie Song, Petros Vasilakos, and Rodney J. Weber
Atmos. Chem. Phys., 21, 6023–6033, https://doi.org/10.5194/acp-21-6023-2021, https://doi.org/10.5194/acp-21-6023-2021, 2021
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Ecosystems and air quality are affected by the dry deposition of inorganic reactive nitrogen (Nr, the sum of ammonium and nitrate). Its large variability is driven by the large difference in deposition velocity of N when in the gas or particle phase. Here we show that aerosol liquid water and acidity, by affecting gas–particle partitioning, modulate the dry deposition velocity of NH3, HNO3, and Nr worldwide. These effects explain the rapid accumulation of nitrate aerosol during haze events.
Steven J. Campbell, Kate Wolfer, Battist Utinger, Joe Westwood, Zhi-Hui Zhang, Nicolas Bukowiecki, Sarah S. Steimer, Tuan V. Vu, Jingsha Xu, Nicholas Straw, Steven Thomson, Atallah Elzein, Yele Sun, Di Liu, Linjie Li, Pingqing Fu, Alastair C. Lewis, Roy M. Harrison, William J. Bloss, Miranda Loh, Mark R. Miller, Zongbo Shi, and Markus Kalberer
Atmos. Chem. Phys., 21, 5549–5573, https://doi.org/10.5194/acp-21-5549-2021, https://doi.org/10.5194/acp-21-5549-2021, 2021
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In this study, we quantify PM2.5 oxidative potential (OP), a metric widely suggested as a potential measure of particle toxicity, in Beijing in summer and winter using four acellular assays. We correlate PM2.5 OP with a comprehensive range of atmospheric and particle composition measurements, demonstrating inter-assay differences and seasonal variation of PM2.5 OP. Using multivariate statistical analysis, we highlight specific particle chemical components and sources that influence OP.
Weiqi Xu, Chun Chen, Yanmei Qiu, Ying Li, Zhiqiang Zhang, Eleni Karnezi, Spyros N. Pandis, Conghui Xie, Zhijie Li, Jiaxing Sun, Nan Ma, Wanyun Xu, Pingqing Fu, Zifa Wang, Jiang Zhu, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Chem. Phys., 21, 5463–5476, https://doi.org/10.5194/acp-21-5463-2021, https://doi.org/10.5194/acp-21-5463-2021, 2021
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Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in the North China Plain (NCP) were investigated in summer and winter. Our results showed that organic aerosol (OA) in winter in the NCP is more volatile than that in summer due to enhanced primary emissions from coal combustion and biomass burning. We also found that OA existed mainly as a solid in winter in Beijing but as semisolids in Beijing in summer and Gucheng in winter.
Xiao Lu, Daniel J. Jacob, Yuzhong Zhang, Joannes D. Maasakkers, Melissa P. Sulprizio, Lu Shen, Zhen Qu, Tia R. Scarpelli, Hannah Nesser, Robert M. Yantosca, Jianxiong Sheng, Arlyn Andrews, Robert J. Parker, Hartmut Boesch, A. Anthony Bloom, and Shuang Ma
Atmos. Chem. Phys., 21, 4637–4657, https://doi.org/10.5194/acp-21-4637-2021, https://doi.org/10.5194/acp-21-4637-2021, 2021
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We use an analytical solution to the Bayesian inverse problem to quantitatively compare and combine the information from satellite and in situ observations, and to estimate global methane budget and their trends over the 2010–2017 period. We find that satellite and in situ observations are to a large extent complementary in the inversion for estimating global methane budget, and reveal consistent corrections of regional anthropogenic and wetland methane emissions relative to the prior inventory.
Joannes D. Maasakkers, Daniel J. Jacob, Melissa P. Sulprizio, Tia R. Scarpelli, Hannah Nesser, Jianxiong Sheng, Yuzhong Zhang, Xiao Lu, A. Anthony Bloom, Kevin W. Bowman, John R. Worden, and Robert J. Parker
Atmos. Chem. Phys., 21, 4339–4356, https://doi.org/10.5194/acp-21-4339-2021, https://doi.org/10.5194/acp-21-4339-2021, 2021
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We use 2010–2015 GOSAT satellite observations of atmospheric methane over North America in a high-resolution inversion to estimate methane emissions. We find general consistency with the gridded EPA inventory but higher oil and gas production emissions, with oil production emissions twice as large as in the latest EPA Greenhouse Gas Inventory. We find lower wetland emissions than predicted by WetCHARTs and a small increasing trend in the eastern US, apparently related to unconventional oil/gas.
Yuzhong Zhang, Daniel J. Jacob, Xiao Lu, Joannes D. Maasakkers, Tia R. Scarpelli, Jian-Xiong Sheng, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Jinfeng Chang, A. Anthony Bloom, Shuang Ma, John Worden, Robert J. Parker, and Hartmut Boesch
Atmos. Chem. Phys., 21, 3643–3666, https://doi.org/10.5194/acp-21-3643-2021, https://doi.org/10.5194/acp-21-3643-2021, 2021
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We use 2010–2018 satellite observations of atmospheric methane to interpret the factors controlling atmospheric methane and its accelerating increase during the period. The 2010–2018 increase in global methane emissions is driven by tropical and boreal wetlands and tropical livestock (South Asia, Africa, Brazil), with an insignificant positive trend in emissions from the fossil fuel sector. The peak methane growth rates in 2014–2015 are also contributed by low OH and high fire emissions.
Peter Sherman, Meng Gao, Shaojie Song, Alex T. Archibald, Nathan Luke Abraham, Jean-François Lamarque, Drew Shindell, Gregory Faluvegi, and Michael B. McElroy
Atmos. Chem. Phys., 21, 3593–3605, https://doi.org/10.5194/acp-21-3593-2021, https://doi.org/10.5194/acp-21-3593-2021, 2021
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The aims here are to assess the role of aerosols in India's monsoon precipitation and to determine the relative contributions from Chinese and Indian emissions using CMIP6 models. We find that increased sulfur emissions reduce precipitation, which is primarily dynamically driven due to spatial shifts in convection over the region. A significant increase in precipitation (up to ~ 20 %) is found only when both Indian and Chinese sulfate emissions are regulated.
Yao Wang, Yue Zhao, Yuchen Wang, Jian-Zhen Yu, Jingyuan Shao, Ping Liu, Wenfei Zhu, Zhen Cheng, Ziyue Li, Naiqiang Yan, and Huayun Xiao
Atmos. Chem. Phys., 21, 2959–2980, https://doi.org/10.5194/acp-21-2959-2021, https://doi.org/10.5194/acp-21-2959-2021, 2021
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Organosulfates (OSs) are important constituents and tracers of secondary organic aerosols (SOAs) in the atmosphere. Here we characterized the OS species in ambient aerosols in Shanghai, China. We find that the contributions of OSs and SOAs to organic aerosols have increased in recent years and that OS production was largely controlled by the oxidant level (Ox), particularly in summer. We infer that mitigation of Ox pollution can effectively reduce the production of OSs and SOAs in eastern China.
Zhongjing Jiang, Jing Li, Xiao Lu, Cheng Gong, Lin Zhang, and Hong Liao
Atmos. Chem. Phys., 21, 2601–2613, https://doi.org/10.5194/acp-21-2601-2021, https://doi.org/10.5194/acp-21-2601-2021, 2021
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This study demonstrates that the intensity of the western Pacific subtropical high (WPSH), a major synoptic pattern in the northern Pacific during summer, can induce a dipole change in surface ozone pollution over eastern China. Ozone concentration increases in the north and decreases in the south during the strong WPSH phase, and vice versa. The change in chemical processes associated with the WPSH change plays a decisive role, whereas the natural emission of ozone precursors accounts for ~ 30 %.
Lei Liu, Jian Zhang, Yinxiao Zhang, Yuanyuan Wang, Liang Xu, Qi Yuan, Dantong Liu, Yele Sun, Pingqing Fu, Zongbo Shi, and Weijun Li
Atmos. Chem. Phys., 21, 2251–2265, https://doi.org/10.5194/acp-21-2251-2021, https://doi.org/10.5194/acp-21-2251-2021, 2021
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We found that large numbers of light-absorbing primary organic particles with high viscosity, especially tarballs, from domestic coal and biomass burning occurred in rural and even urban hazes in the winter of North China. For the first time, we characterized the atmospheric aging process of these burning-related primary organic particles by microscopic analysis and further evaluated their light absorption enhancement resulting from the “lensing effect” of secondary inorganic coatings.
Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Archit Mehra, Stephen D. Worrall, Asan Bacak, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, William J. Bloss, Tuan Vu, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lujie Ren, W. Joe F. Acton, C. Nicholas Hewitt, Xinming Wang, Pingqing Fu, and Dwayne E. Heard
Atmos. Chem. Phys., 21, 2125–2147, https://doi.org/10.5194/acp-21-2125-2021, https://doi.org/10.5194/acp-21-2125-2021, 2021
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To understand how emission controls will impact ozone, an understanding of the sources and sinks of OH and the chemical cycling between peroxy radicals is needed. This paper presents measurements of OH, HO2 and total RO2 taken in central Beijing. The radical observations are compared to a detailed chemistry model, which shows that under low NO conditions, there is a missing OH source. Under high NOx conditions, the model under-predicts RO2 and impacts our ability to model ozone.
Shaojie Song, Tao Ma, Yuzhong Zhang, Lu Shen, Pengfei Liu, Ke Li, Shixian Zhai, Haotian Zheng, Meng Gao, Jonathan M. Moch, Fengkui Duan, Kebin He, and Michael B. McElroy
Atmos. Chem. Phys., 21, 457–481, https://doi.org/10.5194/acp-21-457-2021, https://doi.org/10.5194/acp-21-457-2021, 2021
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We simulate the atmospheric chemical processes of an important sulfur-containing organic aerosol species, which is produced by the reaction between sulfur dioxide and formaldehyde. We can predict its distribution on a global scale. We find it is particularly rich in East Asia. This aerosol species is more abundant in the colder season partly because of weaker sunlight.
Liya Ma, Yujiao Zhu, Mei Zheng, Yele Sun, Lei Huang, Xiaohuan Liu, Yang Gao, Yanjie Shen, Huiwang Gao, and Xiaohong Yao
Atmos. Chem. Phys., 21, 183–200, https://doi.org/10.5194/acp-21-183-2021, https://doi.org/10.5194/acp-21-183-2021, 2021
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In this study, we investigate three patterns of new particles growing to CCN (cloud condensation nuclei) size, i.e., one-stage growth and two-stage growth-A and growth-B patterns. Combining the observations of gaseous pollutants and measured or modeled particulate chemical species, the three growth patterns were discussed regarding the spatial heterogeneity, formation of secondary aerosols, and evaporation of semivolatile particulates as was the survival probability of new particles to CCN size.
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.
Zhuang Wang, Cheng Liu, Zhouqing Xie, Qihou Hu, Meinrat O. Andreae, Yunsheng Dong, Chun Zhao, Ting Liu, Yizhi Zhu, Haoran Liu, Chengzhi Xing, Wei Tan, Xiangguang Ji, Jinan Lin, and Jianguo Liu
Atmos. Chem. Phys., 20, 14917–14932, https://doi.org/10.5194/acp-20-14917-2020, https://doi.org/10.5194/acp-20-14917-2020, 2020
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Significant stratification of aerosols was observed in North China. Polluted dust dominated above the PBL, and anthropogenic aerosols prevailed within the PBL, which is mainly driven by meteorological conditions. The key role of the elevated dust is to alter atmospheric thermodynamics and stability, causing the suppression of turbulence exchange and a decrease in PBL height, especially during the dissipation stage, thereby inhibiting dissipation of persistent heavy surface haze pollution.
Eloise J. Slater, Lisa K. Whalley, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Leigh R. Crilley, Louisa Kramer, William Bloss, Tuan Vu, Yele Sun, Weiqi Xu, Siyao Yue, Lujie Ren, W. Joe F. Acton, C. Nicholas Hewitt, Xinming Wang, Pingqing Fu, and Dwayne E. Heard
Atmos. Chem. Phys., 20, 14847–14871, https://doi.org/10.5194/acp-20-14847-2020, https://doi.org/10.5194/acp-20-14847-2020, 2020
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The paper details atmospheric chemistry in a megacity (Beijing), focussing on radicals which mediate the formation of secondary pollutants such as ozone and particles. Highly polluted conditions were experienced, including the highest ever levels of nitric oxide (NO), with simultaneous radical measurements. Radical concentrations were large during "haze" events, demonstrating active photochemistry. Modelling showed that our understanding of the chemistry at high NOx levels is incomplete.
Jingsha Xu, Shaojie Song, Roy M. Harrison, Congbo Song, Lianfang Wei, Qiang Zhang, Yele Sun, Lu Lei, Chao Zhang, Xiaohong Yao, Dihui Chen, Weijun Li, Miaomiao Wu, Hezhong Tian, Lining Luo, Shengrui Tong, Weiran Li, Junling Wang, Guoliang Shi, Yanqi Huangfu, Yingze Tian, Baozhu Ge, Shaoli Su, Chao Peng, Yang Chen, Fumo Yang, Aleksandra Mihajlidi-Zelić, Dragana Đorđević, Stefan J. Swift, Imogen Andrews, Jacqueline F. Hamilton, Ye Sun, Agung Kramawijaya, Jinxiu Han, Supattarachai Saksakulkrai, Clarissa Baldo, Siqi Hou, Feixue Zheng, Kaspar R. Daellenbach, Chao Yan, Yongchun Liu, Markku Kulmala, Pingqing Fu, and Zongbo Shi
Atmos. Meas. Tech., 13, 6325–6341, https://doi.org/10.5194/amt-13-6325-2020, https://doi.org/10.5194/amt-13-6325-2020, 2020
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An interlaboratory comparison was conducted for the first time to examine differences in water-soluble inorganic ions (WSIIs) measured by 10 labs using ion chromatography (IC) and by two online aerosol chemical speciation monitor (ACSM) methods. Major ions including SO42−, NO3− and NH4+ agreed well in 10 IC labs and correlated well with ACSM data. WSII interlab variability strongly affected aerosol acidity results based on ion balance, but aerosol pH computed by ISORROPIA II was very similar.
Chaomin Wang, Bin Yuan, Caihong Wu, Sihang Wang, Jipeng Qi, Baolin Wang, Zelong Wang, Weiwei Hu, Wei Chen, Chenshuo Ye, Wenjie Wang, Yele Sun, Chen Wang, Shan Huang, Wei Song, Xinming Wang, Suxia Yang, Shenyang Zhang, Wanyun Xu, Nan Ma, Zhanyi Zhang, Bin Jiang, Hang Su, Yafang Cheng, Xuemei Wang, and Min Shao
Atmos. Chem. Phys., 20, 14123–14138, https://doi.org/10.5194/acp-20-14123-2020, https://doi.org/10.5194/acp-20-14123-2020, 2020
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We utilized a novel online mass spectrometry method to measure the total concentration of higher alkanes at each carbon number at two different sites in China, allowing us to take into account SOA contributions from all isomers for higher alkanes. We found that higher alkanes account for significant fractions of SOA formation at the two sites. The contributions are comparable to or even higher than single-ring aromatics, the most-recognized SOA precursors in urban air.
Junfeng Wang, Jianhuai Ye, Dantong Liu, Yangzhou Wu, Jian Zhao, Weiqi Xu, Conghui Xie, Fuzhen Shen, Jie Zhang, Paul E. Ohno, Yiming Qin, Xiuyong Zhao, Scot T. Martin, Alex K. Y. Lee, Pingqing Fu, Daniel J. Jacob, Qi Zhang, Yele Sun, Mindong Chen, and Xinlei Ge
Atmos. Chem. Phys., 20, 14091–14102, https://doi.org/10.5194/acp-20-14091-2020, https://doi.org/10.5194/acp-20-14091-2020, 2020
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We compared the organics in total submicron matter and those coated on BC cores during summertime in Beijing and found large differences between them. Traffic-related OA was associated significantly with BC, while cooking-related OA did not coat BC. In addition, a factor likely originated from primary biomass burning OA was only identified in BC-containing particles. Such a unique BBOA requires further field and laboratory studies to verify its presence and elucidate its properties and impacts.
Jing Cai, Biwu Chu, Lei Yao, Chao Yan, Liine M. Heikkinen, Feixue Zheng, Chang Li, Xiaolong Fan, Shaojun Zhang, Daoyuan Yang, Yonghong Wang, Tom V. Kokkonen, Tommy Chan, Ying Zhou, Lubna Dada, Yongchun Liu, Hong He, Pauli Paasonen, Joni T. Kujansuu, Tuukka Petäjä, Claudia Mohr, Juha Kangasluoma, Federico Bianchi, Yele Sun, Philip L. Croteau, Douglas R. Worsnop, Veli-Matti Kerminen, Wei Du, Markku Kulmala, and Kaspar R. Daellenbach
Atmos. Chem. Phys., 20, 12721–12740, https://doi.org/10.5194/acp-20-12721-2020, https://doi.org/10.5194/acp-20-12721-2020, 2020
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By applying both OA PMF and size PMF at the same urban measurement site in Beijing, similar particle source types, including vehicular emissions, cooking emissions and secondary formation-related sources, were resolved by both frameworks and agreed well. It is also found that in the absence of new particle formation, vehicular and cooking emissions dominate the particle number concentration, while secondary particulate matter governed PM2.5 mass during spring and summer in Beijing.
Ruqian Miao, Qi Chen, Yan Zheng, Xi Cheng, Yele Sun, Paul I. Palmer, Manish Shrivastava, Jianping Guo, Qiang Zhang, Yuhan Liu, Zhaofeng Tan, Xuefei Ma, Shiyi Chen, Limin Zeng, Keding Lu, and Yuanhang Zhang
Atmos. Chem. Phys., 20, 12265–12284, https://doi.org/10.5194/acp-20-12265-2020, https://doi.org/10.5194/acp-20-12265-2020, 2020
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In this study we evaluated the model performances for simulating secondary inorganic aerosol (SIA) and organic aerosol (OA) in PM2.5 in China against comprehensive datasets. The potential biases from factors related to meteorology, emission, chemistry, and atmospheric removal are systematically investigated. This study provides a comprehensive understanding of modeling PM2.5, which is important for studies on the effectiveness of emission control strategies.
Viral Shah, Daniel J. Jacob, Jonathan M. Moch, Xuan Wang, and Shixian Zhai
Atmos. Chem. Phys., 20, 12223–12245, https://doi.org/10.5194/acp-20-12223-2020, https://doi.org/10.5194/acp-20-12223-2020, 2020
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Cloud water pH affects atmospheric chemistry, and acid rain damages ecosystems. We use model simulations along with observations to present a global view of cloud water and precipitation pH. Sulfuric acid, nitric acid, and ammonia control the pH in the northern midlatitudes, but carboxylic acids and dust cations are important in the tropics and subtropics. The acid inputs to many nitrogen-saturated ecosystems are high enough to cause acidification, with ammonium as the main acidifying species.
Hwajin Kim, Qi Zhang, and Yele Sun
Atmos. Chem. Phys., 20, 11527–11550, https://doi.org/10.5194/acp-20-11527-2020, https://doi.org/10.5194/acp-20-11527-2020, 2020
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Severe spring haze and influences of long-range transport in the Seoul metropolitan area (SMA) in March 2019 were investigated. Simultaneous downwind (SMA) and upwind (Beijing) measurements using AMS and ACSM over the same period showed that PM species can be transported in approximately 2 d. Nitrate was the most responsible, and sulfate and two regional-transport-influenced SOAs also contributed. Enhancement of Pb also showed that the haze in the SMA was influenced by the regional transport.
Ke Li, Daniel J. Jacob, Lu Shen, Xiao Lu, Isabelle De Smedt, and Hong Liao
Atmos. Chem. Phys., 20, 11423–11433, https://doi.org/10.5194/acp-20-11423-2020, https://doi.org/10.5194/acp-20-11423-2020, 2020
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Surface summer ozone increased in China from 2013 to 2019 despite new governmental efforts targeting ozone pollution. We find that the ozone increase is mostly due to anthropogenic drivers, although meteorology also plays a role. Further analysis for the North China Plain shows that PM2.5 continued to decrease through 2019, while emissions of volatile organic compounds (VOCs) stayed flat. This could explain the anthropogenic increase in ozone, as PM2.5 scavenges the radical precursors of ozone.
Sally S.-C. Wang and Yuxuan Wang
Atmos. Chem. Phys., 20, 11065–11087, https://doi.org/10.5194/acp-20-11065-2020, https://doi.org/10.5194/acp-20-11065-2020, 2020
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A model consisting of multiple machine learning algorithms is developed to predict wildfire burned area over the south central US and explains key environmental drivers. The developed model alleviates the issue of unevenly distributed data and predicts burned grids and burned areas with good accuracy. The model reveals climate variability such as relative humidity anomalies and antecedent drought severity contributes the most to the total burned area for winter–spring and summer fire season.
Li Zhang, Meiyun Lin, Andrew O. Langford, Larry W. Horowitz, Christoph J. Senff, Elizabeth Klovenski, Yuxuan Wang, Raul J. Alvarez II, Irina Petropavlovskikh, Patrick Cullis, Chance W. Sterling, Jeff Peischl, Thomas B. Ryerson, Steven S. Brown, Zachary C. J. Decker, Guillaume Kirgis, and Stephen Conley
Atmos. Chem. Phys., 20, 10379–10400, https://doi.org/10.5194/acp-20-10379-2020, https://doi.org/10.5194/acp-20-10379-2020, 2020
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Measuring and quantifying the sources of elevated springtime ozone in the southwestern US is challenging but relevant to the implications for control policy. Here we use intensive field measurements and two global models to study ozone sources in the region. We find that ozone from the stratosphere, wildfires, and Asia is an important source of high-ozone events in the region. Our analysis also helps understand the uncertainties in ozone simulations with individual models.
Wanyu Zhao, Hong Ren, Kimitaka Kawamura, Huiyun Du, Xueshun Chen, Siyao Yue, Qiaorong Xie, Lianfang Wei, Ping Li, Xin Zeng, Shaofei Kong, Yele Sun, Zifa Wang, and Pingqing Fu
Atmos. Chem. Phys., 20, 10331–10350, https://doi.org/10.5194/acp-20-10331-2020, https://doi.org/10.5194/acp-20-10331-2020, 2020
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Our observations provide detailed information on the abundance and vertical distribution of dicarboxylic acids, oxoacids and α-dicarbonyls in PM2.5 collected at three heights based on a 325 m meteorological tower in Beijing in summer. Our results demonstrate that organic acids at the ground surface are largely associated with local traffic emissions, while long-range atmospheric transport followed by photochemical ageing contributes more in the urban boundary layer than the ground surface.
Xiao Lu, Lin Zhang, Tongwen Wu, Michael S. Long, Jun Wang, Daniel J. Jacob, Fang Zhang, Jie Zhang, Sebastian D. Eastham, Lu Hu, Lei Zhu, Xiong Liu, and Min Wei
Geosci. Model Dev., 13, 3817–3838, https://doi.org/10.5194/gmd-13-3817-2020, https://doi.org/10.5194/gmd-13-3817-2020, 2020
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This study presents the development and evaluation of a new climate chemistry model, BCC-GEOS-Chem v1.0, which couples the GEOS-Chem chemical transport model as an atmospheric chemistry component in the Beijing Climate Center atmospheric general circulation model. A 3-year (2012–2014) simulation of BCC-GEOS-Chem v1.0 shows that the model captures well the spatiotemporal distributions of tropospheric ozone, other gaseous pollutants, and aerosols.
Haipeng Lin, Xu Feng, Tzung-May Fu, Heng Tian, Yaping Ma, Lijuan Zhang, Daniel J. Jacob, Robert M. Yantosca, Melissa P. Sulprizio, Elizabeth W. Lundgren, Jiawei Zhuang, Qiang Zhang, Xiao Lu, Lin Zhang, Lu Shen, Jianping Guo, Sebastian D. Eastham, and Christoph A. Keller
Geosci. Model Dev., 13, 3241–3265, https://doi.org/10.5194/gmd-13-3241-2020, https://doi.org/10.5194/gmd-13-3241-2020, 2020
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Online coupling of meteorology and chemistry models often presents maintenance issues with hard-wired coding. We present WRF-GC, an one-way online coupling of the WRF meteorological model and GEOS-Chem atmospheric chemistry model for regional atmospheric chemistry and air quality modeling. Our coupling structure allows future versions of either parent model to be immediately integrated into WRF-GC. The WRF-GC model was able to well reproduce regional PM2.5 with greater computational efficiency.
Junchen Guo, Shengzhen Zhou, Mingfu Cai, Jun Zhao, Wei Song, Weixiong Zhao, Weiwei Hu, Yele Sun, Yao He, Chengqiang Yang, Xuezhe Xu, Zhisheng Zhang, Peng Cheng, Qi Fan, Jian Hang, Shaojia Fan, Xinming Wang, and Xuemei Wang
Atmos. Chem. Phys., 20, 7595–7615, https://doi.org/10.5194/acp-20-7595-2020, https://doi.org/10.5194/acp-20-7595-2020, 2020
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We characterized non-refractory submicron particulate matter (PM1.0) during winter in Guangzhou, south China. Chemical composition and key sources of ambient PM1.0 are revealed, highlighting the significant role of SOA. The relationship with SOA and peroxy radicals indicated gas-phase oxidation contributed predominantly to SOA formation during non-pollution periods, while heterogeneous/multiphase reactions played more important roles in SOA formation during pollution periods.
Jiayue Huang, Lyatt Jaeglé, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mat J. Evans, Nicolas Theys, and Sungyeon Choi
Atmos. Chem. Phys., 20, 7335–7358, https://doi.org/10.5194/acp-20-7335-2020, https://doi.org/10.5194/acp-20-7335-2020, 2020
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Large-scale enhancements of tropospheric BrO and the depletion of surface ozone are often observed in the springtime Arctic. Here, we use a chemical transport model to examine the role of sea salt aerosol from blowing snow in explaining these phenomena. We find that our simulation can account for the spatiotemporal variability of satellite observations of BrO. However, the model has difficulty in producing the magnitude of observed ozone depletion events.
Jingyi Li, Haowen Zhang, Qi Ying, Zhijun Wu, Yanli Zhang, Xinming Wang, Xinghua Li, Yele Sun, Min Hu, Yuanhang Zhang, and Jianlin Hu
Atmos. Chem. Phys., 20, 7291–7306, https://doi.org/10.5194/acp-20-7291-2020, https://doi.org/10.5194/acp-20-7291-2020, 2020
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Large gaps still exist in modeled and observed secondary organic aerosol (SOA) mass loading and properties. Here we investigated the impacts of water partitioning into organic aerosol and nonideality of the organic–water mixture on SOA over eastern China using a regional 3D model. SOA is increased more significantly in humid and hot environments. Increases in SOA further cause an enhancement of the cooling effects of aerosols. It is crucial to consider the above processes in modeling SOA.
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.
Weiqi Xu, Yao He, Yanmei Qiu, Chun Chen, Conghui Xie, Lu Lei, Zhijie Li, Jiaxing Sun, Junyao Li, Pingqing Fu, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Meas. Tech., 13, 3205–3219, https://doi.org/10.5194/amt-13-3205-2020, https://doi.org/10.5194/amt-13-3205-2020, 2020
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We characterized mass spectral features of organic aerosol (OA) and water-soluble OA (WSOA) from 21 cooking, crop straw, wood, and coal burning experiments using aerosol mass spectrometers with standard and capture vaporizers, and we demonstrated the applications of source spectral profiles in improving source apportionment of ambient OA at a highly polluted rural site in the North China Plain in winter.
Jing Yang, Wanyu Zhao, Lianfang Wei, Qiang Zhang, Yue Zhao, Wei Hu, Libin Wu, Xiaodong Li, Chandra Mouli Pavuluri, Xiaole Pan, Yele Sun, Zifa Wang, Cong-Qiang Liu, Kimitaka Kawamura, and Pingqing Fu
Atmos. Chem. Phys., 20, 6841–6860, https://doi.org/10.5194/acp-20-6841-2020, https://doi.org/10.5194/acp-20-6841-2020, 2020
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Our observations provide novel detailed information on the atmospheric abundances and spatial distributions of dicarboxylic acids, oxoacids, and α-dicarbonyls in marine aerosols collected from the South China Sea to the East Indian Ocean. Our results demonstrate that the continental outflow of both biogenic and anthropogenic precursors followed by photochemical aging is one of the main sources and formation processes of marine organic aerosols over the tropical oceanic regions.
Qiaorong Xie, Sihui Su, Shuang Chen, Yisheng Xu, Dong Cao, Jing Chen, Lujie Ren, Siyao Yue, Wanyu Zhao, Yele Sun, Zifa Wang, Haijie Tong, Hang Su, Yafang Cheng, Kimitaka Kawamura, Guibin Jiang, Cong-Qiang Liu, and Pingqing Fu
Atmos. Chem. Phys., 20, 6803–6820, https://doi.org/10.5194/acp-20-6803-2020, https://doi.org/10.5194/acp-20-6803-2020, 2020
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Current knowledge on firework-related organic aerosols is very limited. Here the detailed molecular composition of organics in urban aerosols was characterized using ultrahigh-resolution FT-ICR mass spectrometry. Our findings highlight that firework emission leads to a sharp increase in CHO, CHNO, and CHOS containing high-molecular-weight species, particularly aromatic-like substances, which affect the physicochemical properties such as the light absorption and health effects of urban aerosols.
Shengzhen Zhou, Luolin Wu, Junchen Guo, Weihua Chen, Xuemei Wang, Jun Zhao, Yafang Cheng, Zuzhao Huang, Jinpu Zhang, Yele Sun, Pingqing Fu, Shiguo Jia, Jun Tao, Yanning Chen, and Junxia Kuang
Atmos. Chem. Phys., 20, 6435–6453, https://doi.org/10.5194/acp-20-6435-2020, https://doi.org/10.5194/acp-20-6435-2020, 2020
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In this work, measurements of size-segregated aerosols were conducted at three altitudes (ground level, 118 m, and 488 m) on the 610 m high Canton Tower in southern China. Vertical variations of PM and size-segregated chemical compositions were investigated. The results indicated that meteorological parameters and atmospheric aqueous and heterogeneous reactions together led to aerosol formation and haze episodes in the Pearl River Delta region during the measurement periods.
Tao Ma, Hiroshi Furutani, Fengkui Duan, Takashi Kimoto, Jingkun Jiang, Qiang Zhang, Xiaobin Xu, Ying Wang, Jian Gao, Guannan Geng, Meng Li, Shaojie Song, Yongliang Ma, Fei Che, Jie Wang, Lidan Zhu, Tao Huang, Michisato Toyoda, and Kebin He
Atmos. Chem. Phys., 20, 5887–5897, https://doi.org/10.5194/acp-20-5887-2020, https://doi.org/10.5194/acp-20-5887-2020, 2020
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The formation mechanisms of organic matter and sulfate in winter haze in the North China Plain remain unclear. This paper presents the identification and quantification of hydroxymethanesulfonate (HMS) in PM2.5 in Beijing winter and elucidates the heterogeneous HMS chemistry in favorable winter haze conditions. We show that the HMS not only contributes a substantial mass of organic matter, but also leads to an overestimation of sulfate in conventional measurements.
Hang Liu, Xiaole Pan, Dantong Liu, Xiaoyong Liu, Xueshun Chen, Yu Tian, Yele Sun, Pingqing Fu, and Zifa Wang
Atmos. Chem. Phys., 20, 5771–5785, https://doi.org/10.5194/acp-20-5771-2020, https://doi.org/10.5194/acp-20-5771-2020, 2020
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The bare black carbon (BC) was in a fractal structure. With coating thickness increasing, BC changed from a fractal structure to a core–shell structure. In the ambient atmosphere, plenty of BC particles were not in a perfect core–shell structure. This study brought attention to the combined effects of morphology and coating thickness on the absorption enhancement of BC-containing particles, which is helpful for determining the climatic effects of BC.
Youwen Sun, Cheng Liu, Lin Zhang, Mathias Palm, Justus Notholt, Hao Yin, Corinne Vigouroux, Erik Lutsch, Wei Wang, Changong Shan, Thomas Blumenstock, Tomoo Nagahama, Isamu Morino, Emmanuel Mahieu, Kimberly Strong, Bavo Langerock, Martine De Mazière, Qihou Hu, Huifang Zhang, Christof Petri, and Jianguo Liu
Atmos. Chem. Phys., 20, 5437–5456, https://doi.org/10.5194/acp-20-5437-2020, https://doi.org/10.5194/acp-20-5437-2020, 2020
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We present multiyear time series of ground-based Fourier-transform infrared spectroscopy measurements of HCN in densely populated eastern China. The seasonality and interannual variability of tropospheric HCN columns were investigated. The potential sources that drive the observed HCN seasonality and interannual variability were determined using a GEOS-Chem tagged CO simulation, global fire maps, and potential source contribution function values calculated using HYSPLIT back trajectories.
Fanhao Meng, Min Qin, Ke Tang, Jun Duan, Wu Fang, Shuaixi Liang, Kaidi Ye, Pinhua Xie, Yele Sun, Conghui Xie, Chunxiang Ye, Pingqing Fu, Jianguo Liu, and Wenqing Liu
Atmos. Chem. Phys., 20, 5071–5092, https://doi.org/10.5194/acp-20-5071-2020, https://doi.org/10.5194/acp-20-5071-2020, 2020
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Nitrous acid (HONO), a major precursor of the OH radical, plays a key role in atmospheric chemistry, but its sources are still debated. The first high-resolution vertical measurements of HONO and NO2 were conducted in Beijing to investigate the nocturnal sources of HONO at different stages of pollution. The ground surface dominated HONO production by heterogeneous conversion of NO2 during clean episodes, but the aerosol production was an important nighttime HONO source during haze episodes.
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, https://doi.org/10.5194/acp-20-4809-2020, 2020
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Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
Meng Gao, Jinhui Gao, Bin Zhu, Rajesh Kumar, Xiao Lu, Shaojie Song, Yuzhong Zhang, Beixi Jia, Peng Wang, Gufran Beig, Jianlin Hu, Qi Ying, Hongliang Zhang, Peter Sherman, and Michael B. McElroy
Atmos. Chem. Phys., 20, 4399–4414, https://doi.org/10.5194/acp-20-4399-2020, https://doi.org/10.5194/acp-20-4399-2020, 2020
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A regional fully coupled meteorology–chemistry model, Weather Research and Forecasting model with Chemistry (WRF-Chem), was employed to study the seasonality of ozone (O3) pollution and its sources in both China and India.
Becky Alexander, Tomás Sherwen, Christopher D. Holmes, Jenny A. Fisher, Qianjie Chen, Mat J. Evans, and Prasad Kasibhatla
Atmos. Chem. Phys., 20, 3859–3877, https://doi.org/10.5194/acp-20-3859-2020, https://doi.org/10.5194/acp-20-3859-2020, 2020
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Nitrogen oxides are important for the formation of tropospheric oxidants and are removed from the atmosphere mainly through the formation of nitrate. We compare observations of the oxygen isotopes of nitrate with a global model to test our understanding of the chemistry nitrate formation. We use the model to quantify nitrate formation pathways in the atmosphere and identify key uncertainties and their relevance for the oxidation capacity of the atmosphere.
Chenjie Yu, Dantong Liu, Kurtis Broda, Rutambhara Joshi, Jason Olfert, Yele Sun, Pingqing Fu, Hugh Coe, and James D. Allan
Atmos. Chem. Phys., 20, 3645–3661, https://doi.org/10.5194/acp-20-3645-2020, https://doi.org/10.5194/acp-20-3645-2020, 2020
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This study presents the first atmospheric application of a new morphology-independent measurement for the quantification of the mixing state of rBC-containing particles in urban Beijing as part of the UK–China APHH campaign. An inversion method has been applied for better quantification of rBC mixing state. The mass-resolved rBC mixing state information presented here has implications for detailed models of BC, its optical properties and its atmospheric life cycle.
Shaofeng Xu, Lujie Ren, Yunchao Lang, Shengjie Hou, Hong Ren, Lianfang Wei, Libin Wu, Junjun Deng, Wei Hu, Xiaole Pan, Yele Sun, Zifa Wang, Hang Su, Yafang Cheng, and Pingqing Fu
Atmos. Chem. Phys., 20, 3623–3644, https://doi.org/10.5194/acp-20-3623-2020, https://doi.org/10.5194/acp-20-3623-2020, 2020
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Current knowledge on the size distribution of biogenic primary organic aerosols in urban regions with heavy haze pollution is very limited. Here we performed a year-round study focusing on the organic molecular composition of size-segregated aerosol samples collected in urban Beijing during haze and non-haze days to elucidate the seasonal contributions of biomass burning, fungal spores, and plant debris to organic carbon as well as the influences from local emissions and long-range transport.
Archana Dayalu, J. William Munger, Yuxuan Wang, Steven C. Wofsy, Yu Zhao, Thomas Nehrkorn, Chris Nielsen, Michael B. McElroy, and Rachel Chang
Atmos. Chem. Phys., 20, 3569–3588, https://doi.org/10.5194/acp-20-3569-2020, https://doi.org/10.5194/acp-20-3569-2020, 2020
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China has pledged to reduce carbon dioxide emissions per unit GDP by 60–65 % relative to 2005 levels, and to peak carbon emissions overall by 2030. Disagreement among available inventories of Chinese emissions makes it difficult for China to track progress toward its goals and evaluate the efficacy of regional control measures. This study uses a unique set of historical atmospheric observations for the key period from 2005 to 2009 to independently evaluate three different CO2 emission estimates.
Yadong Lei, Xu Yue, Hong Liao, Cheng Gong, and Lin Zhang
Geosci. Model Dev., 13, 1137–1153, https://doi.org/10.5194/gmd-13-1137-2020, https://doi.org/10.5194/gmd-13-1137-2020, 2020
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We coupled a dynamic vegetation model YIBs with the chemical transport model GEOS-Chem to develop a new tool for studying interactions between atmospheric chemistry and biosphere. Within this framework, leaf area index and stomatal conductance are predicted for chemical simulations. In turn, surface ozone causes negative impacts to plant growth and the consequent dry deposition. Such interactions are important for air pollution prediction but ignored in most of current chemical models.
Leigh R. Crilley, Ajit Singh, Louisa J. Kramer, Marvin D. Shaw, Mohammed S. Alam, Joshua S. Apte, William J. Bloss, Lea Hildebrandt Ruiz, Pingqing Fu, Weiqi Fu, Shahzad Gani, Michael Gatari, Evgenia Ilyinskaya, Alastair C. Lewis, David Ng'ang'a, Yele Sun, Rachel C. W. Whitty, Siyao Yue, Stuart Young, and Francis D. Pope
Atmos. Meas. Tech., 13, 1181–1193, https://doi.org/10.5194/amt-13-1181-2020, https://doi.org/10.5194/amt-13-1181-2020, 2020
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There is considerable interest in using low-cost optical particle counters (OPCs) for particle mass measurements; however, there is no agreed upon method with respect to calibration. Here we exploit a number of datasets globally to demonstrate that particle composition and relative humidity are the key factors affecting measured concentrations from a low-cost OPC, and we present a simple correction methodology that corrects for this influence.
Lu Lei, Conghui Xie, Dawei Wang, Yao He, Qingqing Wang, Wei Zhou, Wei Hu, Pingqing Fu, Yong Chen, Xiaole Pan, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Chem. Phys., 20, 2877–2890, https://doi.org/10.5194/acp-20-2877-2020, https://doi.org/10.5194/acp-20-2877-2020, 2020
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We characterized aerosol composition and sources near two steel plants in a coastal region in fall and spring seasons. Our results showed substantially different aerosol composition and sources between the two seasons. We observed significant impacts of steel plant emissions on aerosol chemistry nearby, and we found that aerosol particles emitted from the steel plants were dominated by ammonium sulfate/bisulfate; NOx/CO and NOx/SO2 were distinct from those in the absence of industrial plumes.
Tongwen Wu, Fang Zhang, Jie Zhang, Weihua Jie, Yanwu Zhang, Fanghua Wu, Laurent Li, Jinghui Yan, Xiaohong Liu, Xiao Lu, Haiyue Tan, Lin Zhang, Jun Wang, and Aixue Hu
Geosci. Model Dev., 13, 977–1005, https://doi.org/10.5194/gmd-13-977-2020, https://doi.org/10.5194/gmd-13-977-2020, 2020
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This paper describes the first version of the Beijing Climate Center (BCC) fully coupled Earth System Model with interactive atmospheric chemistry and aerosols (BCC-ESM1). It is one of the models at the BCC for the Coupled Model Intercomparison Project Phase 6 (CMIP6). The CMIP6 Aerosol Chemistry Model Intercomparison Project (AerChemMIP) experiment using BCC-ESM1 has been finished. The evaluations show an overall good agreement between BCC-ESM1 simulations and observations in the 20th century.
Meng Gao, Zirui Liu, Bo Zheng, Dongsheng Ji, Peter Sherman, Shaojie Song, Jinyuan Xin, Cheng Liu, Yuesi Wang, Qiang Zhang, Jia Xing, Jingkun Jiang, Zifa Wang, Gregory R. Carmichael, and Michael B. McElroy
Atmos. Chem. Phys., 20, 1497–1505, https://doi.org/10.5194/acp-20-1497-2020, https://doi.org/10.5194/acp-20-1497-2020, 2020
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We quantified the relative influences of anthropogenic emissions and meteorological conditions on PM2.5 concentrations in Beijing over the winters of 2002–2016. Meteorological conditions over the study period would have led to an increase of haze in Beijing, but the strict emission control measures have suppressed the unfavorable influences of the recent climate.
Viral Shah, Daniel J. Jacob, Ke Li, Rachel F. Silvern, Shixian Zhai, Mengyao Liu, Jintai Lin, and Qiang Zhang
Atmos. Chem. Phys., 20, 1483–1495, https://doi.org/10.5194/acp-20-1483-2020, https://doi.org/10.5194/acp-20-1483-2020, 2020
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We analyze 15 years of satellite observations of nitrogen dioxide (NO2) and use an atmospheric chemistry model to understand the seasonal changes and trends in nitrogen oxides (NOx) over China. We show that the seasonal changes in NO2 occur due to changes in the NOx oxidation lifetime. We find that Chinese NOx emissions peaked in 2011 and had decreased by about 25 % by 2018. But the decrease in NO2 in winter was larger, likely because of a simultaneous decrease in the NOx oxidation lifetime.
Xinxin Fan, Jieyao Liu, Fang Zhang, Lu Chen, Don Collins, Weiqi Xu, Xiaoai Jin, Jingye Ren, Yuying Wang, Hao Wu, Shangze Li, Yele Sun, and Zhanqing Li
Atmos. Chem. Phys., 20, 915–929, https://doi.org/10.5194/acp-20-915-2020, https://doi.org/10.5194/acp-20-915-2020, 2020
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Aerosol effects on visibility and climate are influenced by their hygroscopicity. By contrasting data from two techniques between summer and winter in Beijing, we investigate the effect of aerosol aging, mixing state, and local sources on its hygroscopicity. We revealed that inappropriate use of the density of BC and organics results in large uncertainty in calculating aerosols hygroscopicity. Our results are helpful for parameterization in models.
Xiaoai Jin, Yuying Wang, Zhanqing Li, Fang Zhang, Weiqi Xu, Yele Sun, Xinxin Fan, Guangyu Chen, Hao Wu, Jingye Ren, Qiuyan Wang, and Maureen Cribb
Atmos. Chem. Phys., 20, 901–914, https://doi.org/10.5194/acp-20-901-2020, https://doi.org/10.5194/acp-20-901-2020, 2020
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In this study the aerosol liquid water content (ALWC) is determined from aerosol hygroscopic growth factor (GF) measurement (ALWCHTDMA) and also simulated by the ISORROPIA II thermodynamic model (ALWCISO). We found that ALWC contributed by organics (ALWCOrg) accounts for 30 % ± 22 % of the total ALWC in winter in Beijing. A case study reveals that ALWCOrg plays an important role in the formation of secondary aerosols through multiphase reactions at the initial stage of a heavy-haze episode.
Ye Kuang, Yao He, Wanyun Xu, Pusheng Zhao, Yafang Cheng, Gang Zhao, Jiangchuan Tao, Nan Ma, Hang Su, Yanyan Zhang, Jiayin Sun, Peng Cheng, Wenda Yang, Shaobin Zhang, Cheng Wu, Yele Sun, and Chunsheng Zhao
Atmos. Chem. Phys., 20, 865–880, https://doi.org/10.5194/acp-20-865-2020, https://doi.org/10.5194/acp-20-865-2020, 2020
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A new method was developed to calculate hygroscopicity parameter κ of organic aerosols (κOA) based on aerosol light-scattering measurements and bulk aerosol chemical-composition measurements. Derived high-time-resolution κOA varied in a wide range (near 0 to 0.25), and the organic aerosol oxidation degree significantly impacts variations in κOA. Distinct diurnal variation in κOA is found, and its relationship with oxygenated organic aerosol is discussed.
Yanbing Fan, Cong-Qiang Liu, Linjie Li, Lujie Ren, Hong Ren, Zhimin Zhang, Qinkai Li, Shuang Wang, Wei Hu, Junjun Deng, Libin Wu, Shujun Zhong, Yue Zhao, Chandra Mouli Pavuluri, Xiaodong Li, Xiaole Pan, Yele Sun, Zifa Wang, Kimitaka Kawamura, Zongbo Shi, and Pingqing Fu
Atmos. Chem. Phys., 20, 117–137, https://doi.org/10.5194/acp-20-117-2020, https://doi.org/10.5194/acp-20-117-2020, 2020
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This study provides useful knowledge on the abundance, sources, and formation processes of organic aerosols in the coastal megacity of Tianjin, North China, based on the investigation of the molecular composition, diurnal variation, and winter/summer differences under the influence of land/sea breezes and the Asian summer monsoon.
Danhui Xu, Baozhu Ge, Xueshun Chen, Yele Sun, Nianliang Cheng, Mei Li, Xiaole Pan, Zhiqiang Ma, Yuepeng Pan, and Zifa Wang
Atmos. Chem. Phys., 19, 15569–15581, https://doi.org/10.5194/acp-19-15569-2019, https://doi.org/10.5194/acp-19-15569-2019, 2019
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Wet deposition is one of the most important and efficient removal mechanisms in the evolution of the air pollution. Due to the lack of a localized parameterization scheme and some mechanisms being neglected in theoretical estimations and modeling calculations, below-cloud wet scavenging coefficients (BWSC) have large uncertainties. We compare the BWSCs under the same conditions to perform a multi-method evaluation in order to describe their characteristics.
Hang Liu, Xiaole Pan, Yu Wu, Dawei Wang, Yu Tian, Xiaoyong Liu, Lu Lei, Yele Sun, Pingqing Fu, and Zifa Wang
Atmos. Chem. Phys., 19, 14791–14804, https://doi.org/10.5194/acp-19-14791-2019, https://doi.org/10.5194/acp-19-14791-2019, 2019
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The relationship among the effective density, rBC's coating thickness, and rBC's morphology was investigated. rBC with larger effective density adopted a more regular shape due to more coating thickness. The effective density distribution of ambient rBC was also measured. From the information of effective density, the ambient rBC mainly adopts an irregular shape, which can cause large uncertainties in the rBC's optical properties.
Xiaoxiao Li, Shaojie Song, Wei Zhou, Jiming Hao, Douglas R. Worsnop, and Jingkun Jiang
Atmos. Chem. Phys., 19, 12163–12174, https://doi.org/10.5194/acp-19-12163-2019, https://doi.org/10.5194/acp-19-12163-2019, 2019
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Aerosol liquid water is ubiquitous in ambient aerosol. Using long-term aerosol chemical composition to model the aerosol water in Beijing, we found that water absorbed by organics contributes a significant fraction to the total aerosol water. We emphasize the hygroscopicity of organics is highly variable and should be taken into consideration in modelling. A positive feedback loop between organic hygroscopicity and aerosol water was found as one of the driving factors of severe haze in Beijing.
Weiqi Xu, Conghui Xie, Eleni Karnezi, Qi Zhang, Junfeng Wang, Spyros N. Pandis, Xinlei Ge, Jingwei Zhang, Junling An, Qingqing Wang, Jian Zhao, Wei Du, Yanmei Qiu, Wei Zhou, Yao He, Ying Li, Jie Li, Pingqing Fu, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Chem. Phys., 19, 10205–10216, https://doi.org/10.5194/acp-19-10205-2019, https://doi.org/10.5194/acp-19-10205-2019, 2019
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We present the first aerosol volatility measurements in Beijing in summer using a thermodenuder coupled with aerosol mass spectrometers. Our results showed that organic aerosol (OA) comprised mainly semi-volatile organic compounds in summer, and the freshly oxidized secondary OA was the most volatile component. We also found quite different volatility distributions in black-carbon-containing primary and secondary OA, ambient OA, ambient secondary OA and the WRF-Chem model.
Michael Hollaway, Oliver Wild, Ting Yang, Yele Sun, Weiqi Xu, Conghui Xie, Lisa Whalley, Eloise Slater, Dwayne Heard, and Dantong Liu
Atmos. Chem. Phys., 19, 9699–9714, https://doi.org/10.5194/acp-19-9699-2019, https://doi.org/10.5194/acp-19-9699-2019, 2019
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This study, for the first time, uses combinations of aerosol and lidar data to drive an offline photolysis scheme. Absorbing species are shown to have the greatest impact on photolysis rate constants in the winter and scattering aerosol are shown to dominate responses in the summer. During haze episodes, aerosols are shown to produce a greater impact than cloud cover. The findings demonstrate the potential photochemical impacts of haze pollution in a highly polluted urban environment.
Huiyun Du, Jie Li, Xueshun Chen, Zifa Wang, Yele Sun, Pingqing Fu, Jianjun Li, Jian Gao, and Ying Wei
Atmos. Chem. Phys., 19, 9351–9370, https://doi.org/10.5194/acp-19-9351-2019, https://doi.org/10.5194/acp-19-9351-2019, 2019
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Regional transport and heterogeneous reactions play crucial roles in haze formation. Using a chemical transport model, we found that chemical transformation of SO2 along the transport pathway from source regions to Beijing was the major source of sulfate. Heterogeneous chemistry had a stronger effect under high humidity and high pollution levels. Aerosols underwent aging during transport which altered the aerosol size and the degree of aging.
Tabish Umar Ansari, Oliver Wild, Jie Li, Ting Yang, Weiqi Xu, Yele Sun, and Zifa Wang
Atmos. Chem. Phys., 19, 8651–8668, https://doi.org/10.5194/acp-19-8651-2019, https://doi.org/10.5194/acp-19-8651-2019, 2019
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We explore the effectiveness of short-term emission controls on haze events in Beijing in October–November 2014 with high-resolution model studies. The model captures observed hourly variation in key pollutants well, but representation of boundary layer processes remains a key constraint. The controls contributed to improved air quality in early November but would not have been sufficient had the meteorology been less favourable. We quantify the much more stringent controls needed in that case.
Xiaole Pan, Hang Liu, Yu Wu, Yu Tian, Yele Sun, Conghui Xie, Xiaoyong Liu, Tianhai Cheng, and Zifa Wang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-433, https://doi.org/10.5194/acp-2019-433, 2019
Revised manuscript not accepted
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.
Ying Wei, Xueshun Chen, Huansheng Chen, Jie Li, Zifa Wang, Wenyi Yang, Baozhu Ge, Huiyun Du, Jianqi Hao, Wei Wang, Jianjun Li, Yele Sun, and Huili Huang
Atmos. Chem. Phys., 19, 8269–8296, https://doi.org/10.5194/acp-19-8269-2019, https://doi.org/10.5194/acp-19-8269-2019, 2019
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This study presents a full description and evaluation of a global–regional nested aerosol and atmospheric chemistry model (IAP-AACM). The simulation for 2014 is evaluated against model datasets and a range of observational datasets. The results show that IAP-AACM is within the range of other models, and reproduces both spatial and seasonal variation of trace gases and aerosols over most areas well. In future, we recommend improving the model's ability to capture high spatial variation of PM2.5.
Zongbo Shi, Tuan Vu, Simone Kotthaus, Roy M. Harrison, Sue Grimmond, Siyao Yue, Tong Zhu, James Lee, Yiqun Han, Matthias Demuzere, Rachel E. Dunmore, Lujie Ren, Di Liu, Yuanlin Wang, Oliver Wild, James Allan, W. Joe Acton, Janet Barlow, Benjamin Barratt, David Beddows, William J. Bloss, Giulia Calzolai, David Carruthers, David C. Carslaw, Queenie Chan, Lia Chatzidiakou, Yang Chen, Leigh Crilley, Hugh Coe, Tie Dai, Ruth Doherty, Fengkui Duan, Pingqing Fu, Baozhu Ge, Maofa Ge, Daobo Guan, Jacqueline F. Hamilton, Kebin He, Mathew Heal, Dwayne Heard, C. Nicholas Hewitt, Michael Hollaway, Min Hu, Dongsheng Ji, Xujiang Jiang, Rod Jones, Markus Kalberer, Frank J. Kelly, Louisa Kramer, Ben Langford, Chun Lin, Alastair C. Lewis, Jie Li, Weijun Li, Huan Liu, Junfeng Liu, Miranda Loh, Keding Lu, Franco Lucarelli, Graham Mann, Gordon McFiggans, Mark R. Miller, Graham Mills, Paul Monk, Eiko Nemitz, Fionna O'Connor, Bin Ouyang, Paul I. Palmer, Carl Percival, Olalekan Popoola, Claire Reeves, Andrew R. Rickard, Longyi Shao, Guangyu Shi, Dominick Spracklen, David Stevenson, Yele Sun, Zhiwei Sun, Shu Tao, Shengrui Tong, Qingqing Wang, Wenhua Wang, Xinming Wang, Xuejun Wang, Zifang Wang, Lianfang Wei, Lisa Whalley, Xuefang Wu, Zhijun Wu, Pinhua Xie, Fumo Yang, Qiang Zhang, Yanli Zhang, Yuanhang Zhang, and Mei Zheng
Atmos. Chem. Phys., 19, 7519–7546, https://doi.org/10.5194/acp-19-7519-2019, https://doi.org/10.5194/acp-19-7519-2019, 2019
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APHH-Beijing is a collaborative international research programme to study the sources, processes and health effects of air pollution in Beijing. This introduction to the special issue provides an overview of (i) the APHH-Beijing programme, (ii) the measurement and modelling activities performed as part of it and (iii) the air quality and meteorological conditions during joint intensive field campaigns as a core activity within APHH-Beijing.
Linlin Wang, Junkai Liu, Zhiqiu Gao, Yubin Li, Meng Huang, Sihui Fan, Xiaoye Zhang, Yuanjian Yang, Shiguang Miao, Han Zou, Yele Sun, Yong Chen, and Ting Yang
Atmos. Chem. Phys., 19, 6949–6967, https://doi.org/10.5194/acp-19-6949-2019, https://doi.org/10.5194/acp-19-6949-2019, 2019
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Urban boundary layer (UBL) affects the physical and chemical processes of the pollutants, and UBL structure can also be altered by pollutants. This paper presents the interactions between air pollution and the UBL structure by using the field data mainly collected from a 325 m meteorology tower, as well as from a Doppler wind lidar, during a severe heavy pollution event that occurred during 1–4 December 2016 in Beijing.
Dantong Liu, Rutambhara Joshi, Junfeng Wang, Chenjie Yu, James D. Allan, Hugh Coe, Michael J. Flynn, Conghui Xie, James Lee, Freya Squires, Simone Kotthaus, Sue Grimmond, Xinlei Ge, Yele Sun, and Pingqing Fu
Atmos. Chem. Phys., 19, 6749–6769, https://doi.org/10.5194/acp-19-6749-2019, https://doi.org/10.5194/acp-19-6749-2019, 2019
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This study provides source attribution and characterization of BC in the Beijing urban environment in both winter and summer. For the first time, the physically and chemically based source apportionments are compared to evaluate the primary source contribution and secondary processing of BC-containing particles. A method is proposed to isolate the BC from the transportation sector and coal combustion sources.
Xionghui Qiu, Qi Ying, Shuxiao Wang, Lei Duan, Jian Zhao, Jia Xing, Dian Ding, Yele Sun, Baoxian Liu, Aijun Shi, Xiao Yan, Qingcheng Xu, and Jiming Hao
Atmos. Chem. Phys., 19, 6737–6747, https://doi.org/10.5194/acp-19-6737-2019, https://doi.org/10.5194/acp-19-6737-2019, 2019
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Current chemical transport models cannot capture the diurnal and nocturnal variation in atmospheric nitrate, which may be relative to the missing atmospheric chlorine chemistry. In this work, the Community Multiscale Air Quality (CMAQ) model with improved chlorine heterogeneous chemistry is applied to simulate the impact of chlorine chemistry on summer nitrate concentrations in Beijing. The results of this work can improve our understanding of nitrate formation.
Jialin Li, Meigen Zhang, Guiqian Tang, Yele Sun, Fangkun Wu, and Yongfu Xu
Atmos. Chem. Phys., 19, 6481–6495, https://doi.org/10.5194/acp-19-6481-2019, https://doi.org/10.5194/acp-19-6481-2019, 2019
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There are large uncertainties in the sources of secondary organic aerosol (SOA). Simulations of SOA concentrations in China with aqueous SOA formation pathway updated and glyoxal simulation improved reveal that dicarbonyl-derived SOA (AAQ) can explain a significant fraction of the unaccounted SOA sources. The mean AAQ can contribute 60.6 % and 64.5 % to the total concentration of SOA in summer and fall, respectively.
Lei Zhu, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Xuan Wang, Tomás Sherwen, Mat J. Evans, Qianjie Chen, Becky Alexander, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Michael Le Breton, Thomas J. Bannan, and Carl J. Percival
Atmos. Chem. Phys., 19, 6497–6507, https://doi.org/10.5194/acp-19-6497-2019, https://doi.org/10.5194/acp-19-6497-2019, 2019
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We quantify the effect of sea salt aerosol on tropospheric bromine chemistry with a new mechanistic description of the halogen chemistry in a global atmospheric chemistry model. For the first time, we are able to reproduce the observed levels of bromide activation from the sea salt aerosol in a manner consistent with bromine oxide radical measured from various platforms. Sea salt aerosol plays a far more complex role in global tropospheric chemistry than previously recognized.
Xiaofei Qin, Xiaohao Wang, Yijie Shi, Guangyuan Yu, Na Zhao, Yanfen Lin, Qingyan Fu, Dongfang Wang, Zhouqing Xie, Congrui Deng, and Kan Huang
Atmos. Chem. Phys., 19, 5923–5940, https://doi.org/10.5194/acp-19-5923-2019, https://doi.org/10.5194/acp-19-5923-2019, 2019
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The seasonal pattern of atmospheric mercury species over a regional transport intersection zone in east China indicated impacts from both natural re-emissions and anthropogenic emissions. Quasi-local sources were more important than long-range transport for mercury, opposite from particles. Shipping activities were especially outstanding emissions. Abnormally high GOM was ascribed to the high oxidant levels. The gas–particle partition inhibited the formation of GOM under high particle levels.
Yuqing Ye, Zhouqing Xie, Ming Zhu, and Xinming Wang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-410, https://doi.org/10.5194/acp-2019-410, 2019
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Aerosol samples from the Arctic Ocean and Antarctic atmosphere were analysed by ultrahigh resolution mass spectrometry coupled with negative ion mode electrospray ionization. Hundreds of organic compounds, including organosulfates, nitrooxy-organosulfates, organonitrates and oxygenated hydrocarbons, were detected. Our study presents the first overview of OSs and ONs in the polar regions and promotes the understanding of their characteristics and sources.
Zhenying Xu, Mingxu Liu, Minsi Zhang, Yu Song, Shuxiao Wang, Lin Zhang, Tingting Xu, Tiantian Wang, Caiqing Yan, Tian Zhou, Yele Sun, Yuepeng Pan, Min Hu, Mei Zheng, and Tong Zhu
Atmos. Chem. Phys., 19, 5605–5613, https://doi.org/10.5194/acp-19-5605-2019, https://doi.org/10.5194/acp-19-5605-2019, 2019
Xuan Wang, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Lei Zhu, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mathew J. Evans, Ben H. Lee, Jessica D. Haskins, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Gregory L. Huey, and Hong Liao
Atmos. Chem. Phys., 19, 3981–4003, https://doi.org/10.5194/acp-19-3981-2019, https://doi.org/10.5194/acp-19-3981-2019, 2019
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Chlorine radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a comprehensive simulation of tropospheric chlorine in a global 3-D model, which includes explicit accounting of chloride mobilization from sea salt aerosol. We find the chlorine chemistry contributes 1.0 % of the global oxidation of methane and decreases global burdens of tropospheric ozone by 7 % and OH by 3 % through the associated bromine radical chemistry.
Junting Zhong, Xiaoye Zhang, Yaqiang Wang, Jizhi Wang, Xiaojing Shen, Hongsheng Zhang, Tijian Wang, Zhouqing Xie, Cheng Liu, Hengde Zhang, Tianliang Zhao, Junying Sun, Shaojia Fan, Zhiqiu Gao, Yubin Li, and Linlin Wang
Atmos. Chem. Phys., 19, 3287–3306, https://doi.org/10.5194/acp-19-3287-2019, https://doi.org/10.5194/acp-19-3287-2019, 2019
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In various haze regions in China, including the Guanzhong Plain, the middle and lower reaches of the Yangtze River, the Pearl River Delta, the Sichuan Basin, and the Northeast China Plain, heavy aerosol pollution episodes include inter-/trans-regional transport stages and cumulative stages (CSs). During CSs a two-way feedback mechanism exists between unfavorable meteorological conditions and cumulative aerosol pollution. This two-way feedback is further quantified and its magnitude is compared.
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.
Kate R. Smith, Peter M. Edwards, Peter D. Ivatt, James D. Lee, Freya Squires, Chengliang Dai, Richard E. Peltier, Mat J. Evans, Yele Sun, and Alastair C. Lewis
Atmos. Meas. Tech., 12, 1325–1336, https://doi.org/10.5194/amt-12-1325-2019, https://doi.org/10.5194/amt-12-1325-2019, 2019
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Clusters of low-cost, low-power atmospheric gas sensors were built into a sensor instrument to monitor NO2 and O3 in Beijing, alongside reference instruments, aiming to improve the reliability of sensor measurements. Clustering identical sensors and using the median sensor signal was used to minimize drift over short and medium timescales. Three different machine learning techniques were used for all the sensor data in an attempt to correct for cross-interferences, which worked to some degree.
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.
Shaojie Song, Meng Gao, Weiqi Xu, Yele Sun, Douglas R. Worsnop, John T. Jayne, Yuzhong Zhang, Lei Zhu, Mei Li, Zhen Zhou, Chunlei Cheng, Yibing Lv, Ying Wang, Wei Peng, Xiaobin Xu, Nan Lin, Yuxuan Wang, Shuxiao Wang, J. William Munger, Daniel J. Jacob, and Michael B. McElroy
Atmos. Chem. Phys., 19, 1357–1371, https://doi.org/10.5194/acp-19-1357-2019, https://doi.org/10.5194/acp-19-1357-2019, 2019
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Chemistry responsible for sulfate production in northern China winter haze remains mysterious. We propose a potentially key pathway through the reaction of formaldehyde and sulfur dioxide that has not been accounted for in previous studies. The special atmospheric conditions favor the formation and existence of their complex, hydroxymethanesulfonate (HMS).
Jun Chen, Zhanqing Li, Min Lv, Yuying Wang, Wei Wang, Yingjie Zhang, Haofei Wang, Xing Yan, Yele Sun, and Maureen Cribb
Atmos. Chem. Phys., 19, 1327–1342, https://doi.org/10.5194/acp-19-1327-2019, https://doi.org/10.5194/acp-19-1327-2019, 2019
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The hygroscopic growth function of aerosol particles is derived from Raman lidar, whose dependence on aerosol chemical composition is investigated using data from an aerosol chemical speciation monitor (ACSM) and a hygroscopic tandem differential mobility analyzer (H-TDMA) deployed in China. Two distinct cases were chosen with marked differences in their hygroscopic growth, which was fitted by the Kasten model. The differences were attributed to different amounts of chemical species.
Junfeng Wang, Dantong Liu, Xinlei Ge, Yangzhou Wu, Fuzhen Shen, Mindong Chen, Jian Zhao, Conghui Xie, Qingqing Wang, Weiqi Xu, Jie Zhang, Jianlin Hu, James Allan, Rutambhara Joshi, Pingqing Fu, Hugh Coe, and Yele Sun
Atmos. Chem. Phys., 19, 447–458, https://doi.org/10.5194/acp-19-447-2019, https://doi.org/10.5194/acp-19-447-2019, 2019
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This work is part of the UK-China APHH campaign. We used a laser-only Aerodyne soot particle aerosol mass spectrometer, for the first time, to investigate the concentrations, size distributions and chemical compositions for those ambient submicron aerosol particles only with black carbon as cores. Our findings are valuable to understand the BC properties and processes in the densely populated megacities.
Qiang Huang, Jiubin Chen, Weilin Huang, John R. Reinfelder, Pingqing Fu, Shengliu Yuan, Zhongwei Wang, Wei Yuan, Hongming Cai, Hong Ren, Yele Sun, and Li He
Atmos. Chem. Phys., 19, 315–325, https://doi.org/10.5194/acp-19-315-2019, https://doi.org/10.5194/acp-19-315-2019, 2019
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Although the specific reactions and mechanisms in fine aerosols could not be explicitly determined from this field study, our results provide isotopic evidence that local daily photochemical reduction of divalent Hg is of critical importance to the fate of PM2.5-Hg in urban atmospheres and that, in addition to variation in sources, photochemical reduction appears to be an important process that affects both the particle mass-specific abundance and isotopic composition of PM2.5-Hg.
Conghui Xie, Weiqi Xu, Junfeng Wang, Qingqing Wang, Dantong Liu, Guiqian Tang, Ping Chen, Wei Du, Jian Zhao, Yingjie Zhang, Wei Zhou, Tingting Han, Qingyun Bian, Jie Li, Pingqing Fu, Zifa Wang, Xinlei Ge, James Allan, Hugh Coe, and Yele Sun
Atmos. Chem. Phys., 19, 165–179, https://doi.org/10.5194/acp-19-165-2019, https://doi.org/10.5194/acp-19-165-2019, 2019
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We present the first simultaneous real-time online measurements of aerosol optical properties at ground level and at 260 m on a meteorological tower in urban Beijing in winter. The vertical similarities and differences in scattering and absorption coefficients were characterized. The increases in MAC of BC were mainly associated with the coating materials on rBC. Coal combustion was the dominant source contribution of brown carbon followed by biomass burning and SOA in winter in Beijing.
Mingxu Liu, Xin Huang, Yu Song, Tingting Xu, Shuxiao Wang, Zhijun Wu, Min Hu, Lin Zhang, Qiang Zhang, Yuepeng Pan, Xuejun Liu, and Tong Zhu
Atmos. Chem. Phys., 18, 17933–17943, https://doi.org/10.5194/acp-18-17933-2018, https://doi.org/10.5194/acp-18-17933-2018, 2018
Lu Shen, Daniel J. Jacob, Loretta J. Mickley, Yuxuan Wang, and Qiang Zhang
Atmos. Chem. Phys., 18, 17489–17496, https://doi.org/10.5194/acp-18-17489-2018, https://doi.org/10.5194/acp-18-17489-2018, 2018
Eloise A. Marais, Daniel J. Jacob, Sungyeon Choi, Joanna Joiner, Maria Belmonte-Rivas, Ronald C. Cohen, Steffen Beirle, Lee T. Murray, Luke D. Schiferl, Viral Shah, and Lyatt Jaeglé
Atmos. Chem. Phys., 18, 17017–17027, https://doi.org/10.5194/acp-18-17017-2018, https://doi.org/10.5194/acp-18-17017-2018, 2018
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We intercompare two new products of global upper tropospheric nitrogen dioxide (NO2) retrieved from the Ozone Monitoring Instrument (OMI). We evaluate these products with aircraft observations from NASA DC8 aircraft campaigns and interpret the useful information these products can provide about nitrogen oxides (NOx) in the global upper troposphere using the GEOS-Chem chemical transport model.
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.
Yangyang Zhang, Aohan Tang, Dandan Wang, Qingqing Wang, Katie Benedict, Lin Zhang, Duanyang Liu, Yi Li, Jeffrey L. Collett Jr., Yele Sun, and Xuejun Liu
Atmos. Chem. Phys., 18, 16385–16398, https://doi.org/10.5194/acp-18-16385-2018, https://doi.org/10.5194/acp-18-16385-2018, 2018
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Our study is the first to continually monitor the vertical concentration profile of NH3 in urban Beijing. Weekly concentrations averaged 13.3 ± 4.8 μg m−3. The highest NH3 concentrations were always observed between 32 and 63 m, decreasing toward the surface and toward higher altitudes. Our results demonstrate a NH3 rich atmosphere in urban Beijing, from the ground to at least 320 m. Regional transport from the south (intensive agricultural regions) contributed high NH3 concentrations in Beijing.
Jiayue Huang, Lyatt Jaeglé, and Viral Shah
Atmos. Chem. Phys., 18, 16253–16269, https://doi.org/10.5194/acp-18-16253-2018, https://doi.org/10.5194/acp-18-16253-2018, 2018
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The contribution of blowing snow and frost flower as sources of sea salt aerosols (SSA) over polar regions remains uncertain, despite its potentially important role in polar climate and chemistry. Using chemical transport models and satellite observations, we find that blowing snow emissions are the dominant source of SSA over sea ice during the cold season. We infer a monthly snow salinity on first-year sea ice that decreases from fall–spring, minimizing the model discrepancy to within 10 %.
Archana Dayalu, J. William Munger, Steven C. Wofsy, Yuxuan Wang, Thomas Nehrkorn, Yu Zhao, Michael B. McElroy, Chris P. Nielsen, and Kristina Luus
Biogeosciences, 15, 6713–6729, https://doi.org/10.5194/bg-15-6713-2018, https://doi.org/10.5194/bg-15-6713-2018, 2018
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Accounting for the vegetation signal is critical for comprehensive CO2 budget assessment in China. We model and evaluate hourly vegetation carbon dioxide (CO2) exchange (mass per unit area per unit time) in northern China from 2005 to 2009. The model is driven by satellite and meteorological data, is linked to ground-level ecosystem observations, and is applicable to other time periods. We find vegetation uptake of CO2 in summer is comparable to emissions from fossil fuels in northern China.
Shaojie Song, Hélène Angot, Noelle E. Selin, Hubert Gallée, Francesca Sprovieri, Nicola Pirrone, Detlev Helmig, Joël Savarino, Olivier Magand, and Aurélien Dommergue
Atmos. Chem. Phys., 18, 15825–15840, https://doi.org/10.5194/acp-18-15825-2018, https://doi.org/10.5194/acp-18-15825-2018, 2018
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Mercury is a trace metal with adverse health effects on human and wildlife. Its unique property makes it undergo long-range transport, and even remote Antarctica receives significant inputs. This paper presents the first model that aims to understand mercury behavior over the Antarctic Plateau. We find that mercury is quickly cycled between snow and air in the sunlit period, likely driven by bromine chemistry, and that several uncertain processes contribute to its behavior in the dark period.
Hansen Cao, Tzung-May Fu, Lin Zhang, Daven K. Henze, Christopher Chan Miller, Christophe Lerot, Gonzalo González Abad, Isabelle De Smedt, Qiang Zhang, Michel van Roozendael, François Hendrick, Kelly Chance, Jie Li, Junyu Zheng, and Yuanhong Zhao
Atmos. Chem. Phys., 18, 15017–15046, https://doi.org/10.5194/acp-18-15017-2018, https://doi.org/10.5194/acp-18-15017-2018, 2018
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Our top-down estimates for annual total Chinese NMVOC emissions was 30.7 to 49.5 Tg y−1, including 16.4 to 23.6 Tg y−1 from anthropogenic sources, 12.2 to 22.8 Tg y−1 from biogenic sources, and 2.08 to 3.13 Tg y−1 from biomass burning. Our four inversions consistently showed that the emissions of Chinese anthropogenic NMVOC precursors of glyoxal were larger than the a priori estimates. The glyoxal and formaldehyde constraints helped distinguish the NMVOC species from different sources.
Yingjie Zhang, Wei Du, Yuying Wang, Qingqing Wang, Haofei Wang, Haitao Zheng, Fang Zhang, Hongrong Shi, Yuxuan Bian, Yongxiang Han, Pingqing Fu, Francesco Canonaco, André S. H. Prévôt, Tong Zhu, Pucai Wang, Zhanqing Li, and Yele Sun
Atmos. Chem. Phys., 18, 14637–14651, https://doi.org/10.5194/acp-18-14637-2018, https://doi.org/10.5194/acp-18-14637-2018, 2018
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We have a comprehensive characterization of aerosol chemistry and particle growth events at a downwind site of a highly polluted city in the North China Plain. Aerosol particles at the urban downwind site were highly aged and mainly from secondary formation. New particle growth events were also frequently observed on both clean and polluted days. While both sulfate and SOA played important roles in particle growth during clean periods, SOA was more important than sulfate during polluted events.
Lei Liu, Jian Zhang, Liang Xu, Qi Yuan, Dao Huang, Jianmin Chen, Zongbo Shi, Yele Sun, Pingqing Fu, Zifa Wang, Daizhou Zhang, and Weijun Li
Atmos. Chem. Phys., 18, 14681–14693, https://doi.org/10.5194/acp-18-14681-2018, https://doi.org/10.5194/acp-18-14681-2018, 2018
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Using transmission electron microscopy, we studied individual cloud droplet residual and interstitial particles collected in cloud events at Mt. Tai in the polluted North China region. We found that individual cloud droplets were an extremely complicated mixture containing abundant refractory soot (i.e., black carbon), fly ash, and metals. The complicated cloud droplets have not been reported in clean continental or marine air before.
Pengzhen He, Zhouqing Xie, Xiyuan Chi, Xiawei Yu, Shidong Fan, Hui Kang, Cheng Liu, and Haicong Zhan
Atmos. Chem. Phys., 18, 14465–14476, https://doi.org/10.5194/acp-18-14465-2018, https://doi.org/10.5194/acp-18-14465-2018, 2018
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We present the first observations of the oxygen-17 excess of atmospheric nitrate (Δ17O(NO−3)) collected in Beijing haze to reveal the relative importance of different nitrate formation pathways. We found that nocturnal pathways (N2O5 + H2O/Cl– and NO3 + HC) dominated nitrate production during polluted days (PM2.5 ≥ 75 μg m–3), with a mean possible fraction of 56–97 %.
Mingjie Kang, Pingqing Fu, Kimitaka Kawamura, Fan Yang, Hongliang Zhang, Zhengchen Zang, Hong Ren, Lujie Ren, Ye Zhao, Yele Sun, and Zifa Wang
Atmos. Chem. Phys., 18, 13947–13967, https://doi.org/10.5194/acp-18-13947-2018, https://doi.org/10.5194/acp-18-13947-2018, 2018
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Molecular characterization and spatial distribution of biogenic primary organic aerosol (POA) and secondary organic aerosol (SOA) in the marine atmosphere are not well known. Here, we analysed the organic molecular composition of marine aerosols collected during a marine cruise in the East China Sea during May–June 2014. Our results suggest that the Asian continent can be a natural emitter of biogenic POA and SOA, which can be transported to the downwind marine atmosphere.
Qianjie Chen, Tomás Sherwen, Mathew Evans, and Becky Alexander
Atmos. Chem. Phys., 18, 13617–13637, https://doi.org/10.5194/acp-18-13617-2018, https://doi.org/10.5194/acp-18-13617-2018, 2018
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Uncertainty in the natural tropospheric sulfur cycle represents the largest source of uncertainty in radiative forcing estimates of sulfate aerosol. This study investigates the natural sulfur cycle in the marine troposphere using the GEOS-Chem model. We found that BrO is important for DMS oxidation and multiphase chemistry is important for MSA production and loss, which have implications for the yield of SO2 and MSA from DMS oxidation and the radiative effect of DMS-derived sulfate aerosol.
Yuying Wang, Zhanqing Li, Yingjie Zhang, Wei Du, Fang Zhang, Haobo Tan, Hanbing Xu, Tianyi Fan, Xiaoai Jin, Xinxin Fan, Zipeng Dong, Qiuyan Wang, and Yele Sun
Atmos. Chem. Phys., 18, 11739–11752, https://doi.org/10.5194/acp-18-11739-2018, https://doi.org/10.5194/acp-18-11739-2018, 2018
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Very different aerosol hygroscopicities and mixing states were found at these sites in the North China Plain. The PDF for 40–200 nm particles showed the particles were highly aged and internally mixed at Xingtai because of high pollution and strong photochemical reactions. A good proxy for the chemical comical composition (kappa = 0.31) in calculating CCN concentration was found. Importantly, our study investigated the influence of industrial emissions on the aerosol properties.
Wei Zhou, Jian Zhao, Bin Ouyang, Archit Mehra, Weiqi Xu, Yuying Wang, Thomas J. Bannan, Stephen D. Worrall, Michael Priestley, Asan Bacak, Qi Chen, Conghui Xie, Qingqing Wang, Junfeng Wang, Wei Du, Yingjie Zhang, Xinlei Ge, Penglin Ye, James D. Lee, Pingqing Fu, Zifa Wang, Douglas Worsnop, Roderic Jones, Carl J. Percival, Hugh Coe, and Yele Sun
Atmos. Chem. Phys., 18, 11581–11597, https://doi.org/10.5194/acp-18-11581-2018, https://doi.org/10.5194/acp-18-11581-2018, 2018
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We present measurements of gas-phase N2O5 and ClNO2 by ToF-CIMS during summer in urban Beijing as part of the APHH campaign. High reactivity of N2O5 indicative of active nocturnal chemistry was observed. The lifetime of N2O5 as a function of aerosol surface area and relative humidity was characterized, and N2O5 uptake coefficients were estimated. We also found that the N2O5 loss in this study is mainly attributed to its indirect loss via reactions of NO3 with VOCs and NO.
Prasad Kasibhatla, Tomás Sherwen, Mathew J. Evans, Lucy J. Carpenter, Chris Reed, Becky Alexander, Qianjie Chen, Melissa P. Sulprizio, James D. Lee, Katie A. Read, William Bloss, Leigh R. Crilley, William C. Keene, Alexander A. P. Pszenny, and Alma Hodzic
Atmos. Chem. Phys., 18, 11185–11203, https://doi.org/10.5194/acp-18-11185-2018, https://doi.org/10.5194/acp-18-11185-2018, 2018
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Recent measurements of NOx and HONO suggest that photolysis of particulate nitrate in sea-salt aerosols is important in terms of marine boundary layer oxidant chemistry. We present the first global-scale assessment of the significance of this new chemical pathway for NOx, O3, and OH in the marine boundary layer. We also present a preliminary assessment of the potential impact of photolysis of particulate nitrate associated with other aerosol types on continental boundary layer chemistry.
Wen Xu, Lei Liu, Miaomiao Cheng, Yuanhong Zhao, Lin Zhang, Yuepeng Pan, Xiuming Zhang, Baojing Gu, Yi Li, Xiuying Zhang, Jianlin Shen, Li Lu, Xiaosheng Luo, Yu Zhao, Zhaozhong Feng, Jeffrey L. Collett Jr., Fusuo Zhang, and Xuejun Liu
Atmos. Chem. Phys., 18, 10931–10954, https://doi.org/10.5194/acp-18-10931-2018, https://doi.org/10.5194/acp-18-10931-2018, 2018
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Our main results demonstrate that atmospheric Nr pollution in eastern China is more serious in the northern region than in the southern region. Any effects of current emission controls are not yet apparent in Nr pollution. NH3 emissions from fertilizer use were the largest contributor (36 %) to total inorganic Nr deposition. Our results provide useful information for policy-makers that mitigation of NH3 emissions should be a priority to tackle serious N deposition.
Yele Sun, Weiqi Xu, Qi Zhang, Qi Jiang, Francesco Canonaco, André S. H. Prévôt, Pingqing Fu, Jie Li, John Jayne, Douglas R. Worsnop, and Zifa Wang
Atmos. Chem. Phys., 18, 8469–8489, https://doi.org/10.5194/acp-18-8469-2018, https://doi.org/10.5194/acp-18-8469-2018, 2018
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We present a 2–year analysis of organic aerosol (OA) from highly time–resolved measurements by an aerosol chemical speciation monitor in the megacity of Beijing. The sources of OA were analyzed with the advanced factor analysis of a multilinear engine (ME-2). Our results showed very different seasonal patterns, relative humidity and temperature dependence, and sources regions among different OA factors. The sources and processes of OA factors, and their roles in haze pollution are elucidated.
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
Jie Zhang, Sara Lance, Jeffrey M. Freedman, Yele Sun, Brian A. Crandall, Xiuli Wei, and James J. Schwab
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-529, https://doi.org/10.5194/acp-2018-529, 2018
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The impact of fireworks (FW) events on air quality was studied using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and collocated instruments during the Independence Day (July 4) holiday. The Independence Day FW events resulted in significant increases in both organic and inorganic (potassium, sulfate, chloride) chemical components, and the contribution from different aerosol sources was discussed.
Shaojie Song, Meng Gao, Weiqi Xu, Jingyuan Shao, Guoliang Shi, Shuxiao Wang, Yuxuan Wang, Yele Sun, and Michael B. McElroy
Atmos. Chem. Phys., 18, 7423–7438, https://doi.org/10.5194/acp-18-7423-2018, https://doi.org/10.5194/acp-18-7423-2018, 2018
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Severe haze events occur frequently over northern China, especially in winter. Acidity plays a critical role in the formation of secondary PM2.5 and its toxicity. Using field measurements of gases and particles to critically evaluate two thermodynamic models routinely employed to determine particle acidity, we found that China's winter haze particles are generally within a moderately acidic range (pH 4–5) and not highly acidic (0) or neutral (7) as has been previously reported in the literature.
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.
Jingye Ren, Fang Zhang, Yuying Wang, Don Collins, Xinxin Fan, Xiaoai Jin, Weiqi Xu, Yele Sun, Maureen Cribb, and Zhanqing Li
Atmos. Chem. Phys., 18, 6907–6921, https://doi.org/10.5194/acp-18-6907-2018, https://doi.org/10.5194/acp-18-6907-2018, 2018
Qianqian Hong, Cheng Liu, Ka Lok Chan, Qihou Hu, Zhouqing Xie, Haoran Liu, Fuqi Si, and Jianguo Liu
Atmos. Chem. Phys., 18, 5931–5951, https://doi.org/10.5194/acp-18-5931-2018, https://doi.org/10.5194/acp-18-5931-2018, 2018
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We presented ship-based MAX-DOAS measurements of tropospheric trace gases' distribution along the eastern part of the Yangtze River during winter 2015. Tropospheric VCDs of NO2, SO2, and HCHO were retrieved from MAX-DOAS measurement spectra. Enhanced tropospheric NO2 and SO2 VCDs were detected over downwind areas of industrial zones over the Yangtze River. Our results indicate that different pollution control strategies should be applied in different provinces.
Pengzhen He, Becky Alexander, Lei Geng, Xiyuan Chi, Shidong Fan, Haicong Zhan, Hui Kang, Guangjie Zheng, Yafang Cheng, Hang Su, Cheng Liu, and Zhouqing Xie
Atmos. Chem. Phys., 18, 5515–5528, https://doi.org/10.5194/acp-18-5515-2018, https://doi.org/10.5194/acp-18-5515-2018, 2018
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We use observations of the oxygen isotopic composition of sulfate aerosol as a fingerprint to quantify various sulfate formation mechanisms during pollution events in Beijing, China. We found that heterogeneous reactions on aerosols dominated sulfate production in general; however, in-cloud reactions would dominate haze sulfate production when cloud liquid water content was high. The findings also suggest the heterogeneity of aerosol acidity should be parameterized in models.
Jennifer Kaiser, Daniel J. Jacob, Lei Zhu, Katherine R. Travis, Jenny A. Fisher, Gonzalo González Abad, Lin Zhang, Xuesong Zhang, Alan Fried, John D. Crounse, Jason M. St. Clair, and Armin Wisthaler
Atmos. Chem. Phys., 18, 5483–5497, https://doi.org/10.5194/acp-18-5483-2018, https://doi.org/10.5194/acp-18-5483-2018, 2018
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Isoprene emissions from vegetation have a large effect on atmospheric chemistry and air quality. Here we use the adjoint of GEOS-Chem in an inversion of OMI formaldehyde observations to produce top-down estimates of isoprene emissions in the southeast US during the summer of 2013. We find that MEGAN v2.1 is biased high on average by 40 %. Our downward correction of isoprene emissions leads to a small reduction in modeled surface O3 and decreases the contribution of isoprene to organic aerosol.
Wei Zhou, Qingqing Wang, Xiujuan Zhao, Weiqi Xu, Chen Chen, Wei Du, Jian Zhao, Francesco Canonaco, André S. H. Prévôt, Pingqing Fu, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Chem. Phys., 18, 3951–3968, https://doi.org/10.5194/acp-18-3951-2018, https://doi.org/10.5194/acp-18-3951-2018, 2018
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We present a 3-month analysis of submicron aerosols that were measured at 260 m on a meteorological tower in Beijing, China. The sources of organic aerosol (OA) were analyzed by using a multi-linear engine (ME-2). Our results showed significant changes in both primary and secondary OA composition from the non-heating season to the heating season. We also observed a considerable contribution (10–13%) of cooking OA at 260 m and very different OA composition between ground level and 260 m.
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.
Xiao Lu, Lin Zhang, Xiong Liu, Meng Gao, Yuanhong Zhao, and Jingyuan Shao
Atmos. Chem. Phys., 18, 3101–3118, https://doi.org/10.5194/acp-18-3101-2018, https://doi.org/10.5194/acp-18-3101-2018, 2018
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Deteriorating tropospheric ozone pollution over India may not only affect local human health and vegetation but also perturb global ozone distribution. This study analyzes the processes controlling lower tropospheric ozone over India using OMI satellite observations (2006–2014) and model simulations (1990–2010). We show that the South Asian monsoon largely controls the seasonal cycle and interannual variability of Indian lower tropospheric ozone via changes in ozone production and transport.
Wanyu Zhao, Kimitaka Kawamura, Siyao Yue, Lianfang Wei, Hong Ren, Yu Yan, Mingjie Kang, Linjie Li, Lujie Ren, Senchao Lai, Jie Li, Yele Sun, Zifa Wang, and Pingqing Fu
Atmos. Chem. Phys., 18, 2749–2767, https://doi.org/10.5194/acp-18-2749-2018, https://doi.org/10.5194/acp-18-2749-2018, 2018
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In this paper, we investigate the seasonal trends in concentrations and compound-specific stable carbon isotope ratios of low molecular weight dicarboxylic acids (C2–C12) and related compounds in fine aerosols (PM2.5) in Beijing. Our study demonstrates that, in addition to the production via photo-oxidation, high abundances of diacids and related compounds in Beijing are largely associated with anthropogenic primary emissions such as biomass burning, fossil fuel combustion and plastic burning.
Qingqing Wang, Yele Sun, Weiqi Xu, Wei Du, Libo Zhou, Guiqian Tang, Chen Chen, Xueling Cheng, Xiujuan Zhao, Dongsheng Ji, Tingting Han, Zhe Wang, Jie Li, and Zifa Wang
Atmos. Chem. Phys., 18, 2495–2509, https://doi.org/10.5194/acp-18-2495-2018, https://doi.org/10.5194/acp-18-2495-2018, 2018
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We conducted the first real-time continuous vertical measurements of particle extinction, NO2, and BC from ground level to 260 m during two severe winter haze episodes in urban Beijing, China. Our results show very complex and dynamic vertical profiles that interact closely with boundary layer and meteorological conditions. Further analysis demonstrate that vertical convection, temperature inversion, and local emissions are three major factors affecting the changes in vertical profiles.
Lin Zhang, Youfan Chen, Yuanhong Zhao, Daven K. Henze, Liye Zhu, Yu Song, Fabien Paulot, Xuejun Liu, Yuepeng Pan, Yi Lin, and Binxiang Huang
Atmos. Chem. Phys., 18, 339–355, https://doi.org/10.5194/acp-18-339-2018, https://doi.org/10.5194/acp-18-339-2018, 2018
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Substantial differences exist in current estimates of agricultural ammonia emissions in China, hindering understanding of their environmental consequences. This study applies both bottom-up and top-down methods to better quantify agricultural ammonia sources in China using observations from satellite and surface networks interpreted by a chemical transport model. Our estimate of annual Chinese anthropogenic ammonia emission is 11.7 tg (teragram) for 2008 with a strong seasonality peak in summer.
Zheng Fang, Wei Deng, Yanli Zhang, Xiang Ding, Mingjin Tang, Tengyu Liu, Qihou Hu, Ming Zhu, Zhaoyi Wang, Weiqiang Yang, Zhonghui Huang, Wei Song, Xinhui Bi, Jianmin Chen, Yele Sun, Christian George, and Xinming Wang
Atmos. Chem. Phys., 17, 14821–14839, https://doi.org/10.5194/acp-17-14821-2017, https://doi.org/10.5194/acp-17-14821-2017, 2017
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Primary emissions and aging of open straw burning plumes were characterized in ambient dilution conditions in a chamber. Rich in alkenes, the plumes have high O3 formation potential. The emissions of specific particulate and gaseous compounds were less when the straws were fully burned. Organic aerosol (OA) mass increased by a factor of 2–8 with 3–9 h photo-oxidation, yet > 70 % of the mass cannot be explained by the known precursors. OA gained more O- and N-containing compounds during aging.
Yunjiang Zhang, Lili Tang, Philip L. Croteau, Olivier Favez, Yele Sun, Manjula R. Canagaratna, Zhuang Wang, Florian Couvidat, Alexandre Albinet, Hongliang Zhang, Jean Sciare, André S. H. Prévôt, John T. Jayne, and Douglas R. Worsnop
Atmos. Chem. Phys., 17, 14501–14517, https://doi.org/10.5194/acp-17-14501-2017, https://doi.org/10.5194/acp-17-14501-2017, 2017
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We conducted the first field measurements of non-refractory fine aerosols (NR-PM2.5) in a megacity of eastern China using a PM2.5-ACSM along with a PM1-ACSM measurement. Inter-comparisons demonstrated that the NR-PM2.5 components can be characterized. Substantial mass fractions of aerosol species were observed in the size range of 1–2.5 μm, with sulfate and SOA being the two largest contributors. The impacts of aerosol water driven by secondary inorganic aerosols on SOA formation were explored.
Chengzhi Xing, Cheng Liu, Shanshan Wang, Ka Lok Chan, Yang Gao, Xin Huang, Wenjing Su, Chengxin Zhang, Yunsheng Dong, Guangqiang Fan, Tianshu Zhang, Zhenyi Chen, Qihou Hu, Hang Su, Zhouqing Xie, and Jianguo Liu
Atmos. Chem. Phys., 17, 14275–14289, https://doi.org/10.5194/acp-17-14275-2017, https://doi.org/10.5194/acp-17-14275-2017, 2017
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Vertical profiles of the aerosol extinction coefficient and NO2 and HCHO concentrations were retrieved from MAX-DOAS measurement, while vertical distribution of O3 was obtained using ozone lidar. The measured O3 vertical distribution indicates that the ozone production not only occurs at surface level but also at higher altitudes (about 1.1 km), which are not directly related to horizontal and vertical transportation but are mainly influenced by the abundance of VOCs in the lower troposphere.
Yuxuan Wang, Yuanyu Xie, Wenhao Dong, Yi Ming, Jun Wang, and Lu Shen
Atmos. Chem. Phys., 17, 12827–12843, https://doi.org/10.5194/acp-17-12827-2017, https://doi.org/10.5194/acp-17-12827-2017, 2017
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Besides the well-known large impact on agriculture and water resources, drought is associated with significant adverse effects on air quality. Drought-induced degradation of air quality is largely due to natural processes, offsetting the effort of anthropogenic emission reduction during the past decades. Such adverse impacts should be included in modeling processes under current and future climate for mitigation policy.
Yue Zhao, Jeremy K. Chan, Felipe D. Lopez-Hilfiker, Megan A. McKeown, Emma L. D'Ambro, Jay G. Slowik, Jeffrey A. Riffell, and Joel A. Thornton
Atmos. Meas. Tech., 10, 3609–3625, https://doi.org/10.5194/amt-10-3609-2017, https://doi.org/10.5194/amt-10-3609-2017, 2017
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We present a novel atmospheric pressure electrospray chemical ionization (ESCI) source that can generate intense and stable currents of several specific reagent ions using a range of salt solutions prepared in methanol. We couple the ESCI source to a high-resolution time-of-flight mass spectrometer (HRToF-MS) and assess instrument performance through calibrations using different gas standards and measurements of organic mixtures formed by ozonolysis of α-pinene.
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.
Yuanhong Zhao, Lin Zhang, Amos P. K. Tai, Youfan Chen, and Yuepeng Pan
Atmos. Chem. Phys., 17, 9781–9796, https://doi.org/10.5194/acp-17-9781-2017, https://doi.org/10.5194/acp-17-9781-2017, 2017
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Human activities have substantially enhanced atmospheric deposition of reactive nitrogen, inducing complex environmental consequences. This study presents a first quantitative investigation of how anthropogenic nitrogen deposition could impact surface ozone air quality through surface–atmosphere exchange processes. We find important surface ozone changes driven by nitrogen deposition, which can be comparable with those due to historical climate and land use changes.
Viral Shah and Lyatt Jaeglé
Atmos. Chem. Phys., 17, 8999–9017, https://doi.org/10.5194/acp-17-8999-2017, https://doi.org/10.5194/acp-17-8999-2017, 2017
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We use a model of mercury chemistry and transport in the atmosphere, along with ground- and aircraft-based mercury observations, to learn that oxidized mercury chemically produced in the free troposphere descends in the subtropical anticyclones and makes up much of the mercury depositing to the Earth's surface. Our findings imply that mercury chemistry in the free troposphere and transport in the subtropics are important links between global emissions and surface deposition of mercury.
Johannes Bieser, Franz Slemr, Jesse Ambrose, Carl Brenninkmeijer, Steve Brooks, Ashu Dastoor, Francesco DeSimone, Ralf Ebinghaus, Christian N. Gencarelli, Beate Geyer, Lynne E. Gratz, Ian M. Hedgecock, Daniel Jaffe, Paul Kelley, Che-Jen Lin, Lyatt Jaegle, Volker Matthias, Andrei Ryjkov, Noelle E. Selin, Shaojie Song, Oleg Travnikov, Andreas Weigelt, Winston Luke, Xinrong Ren, Andreas Zahn, Xin Yang, Yun Zhu, and Nicola Pirrone
Atmos. Chem. Phys., 17, 6925–6955, https://doi.org/10.5194/acp-17-6925-2017, https://doi.org/10.5194/acp-17-6925-2017, 2017
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We conducted a multi model study to investigate our ability to reproduce the vertical distribution of mercury in the atmosphere. For this, we used observational data from over 40 aircraft flights in EU and US. We compared observations to the results of seven chemistry transport models and found that the models are able to reproduce vertical gradients of total and elemental Hg. Finally, we found that different chemical reactions seem responsible for the oxidation of Hg depending on altitude.
Wei Du, Jian Zhao, Yuying Wang, Yingjie Zhang, Qingqing Wang, Weiqi Xu, Chen Chen, Tingting Han, Fang Zhang, Zhanqing Li, Pingqing Fu, Jie Li, Zifa Wang, and Yele Sun
Atmos. Chem. Phys., 17, 6797–6811, https://doi.org/10.5194/acp-17-6797-2017, https://doi.org/10.5194/acp-17-6797-2017, 2017
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We conducted the first simultaneous measurements of size-resolved particle number concentrations at ground level and 260 m in urban Beijing. The vertical differences strongly depend on particle sizes, with accumulation-mode particles being highly correlated at the two heights. We further demonstrated that regional emission controls have a dominant impact on accumulation-mode particles, while the influences on Aitken particles were much smaller due to the enhanced NPF events.
Ting Yang, Zifa Wang, Wei Zhang, Alex Gbaguidi, Nobuo Sugimoto, Xiquan Wang, Ichiro Matsui, and Yele Sun
Atmos. Chem. Phys., 17, 6215–6225, https://doi.org/10.5194/acp-17-6215-2017, https://doi.org/10.5194/acp-17-6215-2017, 2017
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Predicting air pollution events over megacities requires, notably, continuous and accurate determination of the boundary layer height (BLH). Based on gravity wave theory, a new approach (CRGM) is developed to overcome existing algorithms' weakness in order to accurately reproduce the fluctuations of the BLH under various atmospheric pollution conditions from lidar observation. Comprehensive evaluation highlights strong effectiveness of this new method.
Oleg Travnikov, Hélène Angot, Paulo Artaxo, Mariantonia Bencardino, Johannes Bieser, Francesco D'Amore, Ashu Dastoor, Francesco De Simone, María del Carmen Diéguez, Aurélien Dommergue, Ralf Ebinghaus, Xin Bin Feng, Christian N. Gencarelli, Ian M. Hedgecock, Olivier Magand, Lynwill Martin, Volker Matthias, Nikolay Mashyanov, Nicola Pirrone, Ramesh Ramachandran, Katie Alana Read, Andrei Ryjkov, Noelle E. Selin, Fabrizio Sena, Shaojie Song, Francesca Sprovieri, Dennis Wip, Ingvar Wängberg, and Xin Yang
Atmos. Chem. Phys., 17, 5271–5295, https://doi.org/10.5194/acp-17-5271-2017, https://doi.org/10.5194/acp-17-5271-2017, 2017
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The study provides a complex analysis of processes governing Hg fate in the atmosphere involving both measurement data and simulation results of chemical transport models. Evaluation of the model simulations and numerical experiments against observations allows explaining spatial and temporal variations of Hg concentration in the near-surface atmospheric layer and shows possibility of multiple pathways of Hg oxidation occurring concurrently in various parts of the atmosphere.
Yuying Wang, Fang Zhang, Zhanqing Li, Haobo Tan, Hanbing Xu, Jingye Ren, Jian Zhao, Wei Du, and Yele Sun
Atmos. Chem. Phys., 17, 5239–5251, https://doi.org/10.5194/acp-17-5239-2017, https://doi.org/10.5194/acp-17-5239-2017, 2017
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A series of strict emission control measures were implemented in Beijing and the surrounding seven provinces to ensure good air quality during the 2015 China Victory Day parade, rendering a unique opportunity to investigate anthropogenic impact of aerosol properties. Submicron aerosol hygroscopicity and volatility were measured during and after the control period. By comparison we found aerosol particles became more hydrophobic and volatile due to the emission control measures.
Yue Zhao, Michelle C. Fairhurst, Lisa M. Wingen, Véronique Perraud, Michael J. Ezell, and Barbara J. Finlayson-Pitts
Atmos. Meas. Tech., 10, 1373–1386, https://doi.org/10.5194/amt-10-1373-2017, https://doi.org/10.5194/amt-10-1373-2017, 2017
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Two model systems are studied: dicarboxylic acid particles with gaseous amines and α-cedrene ozonolysis particles. Measurements by direct analysis in real-time mass spectrometry and high-resolution time-of-flight aerosol mass spectrometry
show that the reaction of the amines with the acid particles is restricted to the surface layer, with an odd–even alternating pattern. Furthermore, in the α-cedrene study, DART-MS is able to differentiate isomers based on their volatility.
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.
Jian Zhao, Wei Du, Yingjie Zhang, Qingqing Wang, Chen Chen, Weiqi Xu, Tingting Han, Yuying Wang, Pingqing Fu, Zifa Wang, Zhanqing Li, and Yele Sun
Atmos. Chem. Phys., 17, 3215–3232, https://doi.org/10.5194/acp-17-3215-2017, https://doi.org/10.5194/acp-17-3215-2017, 2017
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We conducted aerosol particle composition measurements at ground level and 260 m with two aerosol mass spectrometers in Beijing during the 2015 China Victory Day parade. Our results showed a stronger impact of emission controls on inorganic aerosol than OA. A larger decrease in more oxidized SOA than the less oxidized one during the control period was also observed. Our results indicate that emission controls and the changes in meteorological conditions have affected SOA formation mechanisms.
Shurui Chen, Liang Xu, Yinxiao Zhang, Bing Chen, Xinfeng Wang, Xiaoye Zhang, Mei Zheng, Jianmin Chen, Wenxing Wang, Yele Sun, Pingqing Fu, Zifa Wang, and Weijun Li
Atmos. Chem. Phys., 17, 1259–1270, https://doi.org/10.5194/acp-17-1259-2017, https://doi.org/10.5194/acp-17-1259-2017, 2017
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Many studies have focused on the unusually severe hazes instead of the more frequent light and moderate hazes (22–63 %) in winter in the North China Plain (NCP). The morphology, mixing state, and size of organic aerosols in the L & M hazes were characterized. We conclude that the direct emissions from residential coal stoves without any pollution controls in rural and urban outskirts contribute large amounts of primary OM particles to the regional L & M hazes in winter in the NCP.
Wen Xu, Wei Song, Yangyang Zhang, Xuejun Liu, Lin Zhang, Yuanhong Zhao, Duanyang Liu, Aohan Tang, Daowei Yang, Dandan Wang, Zhang Wen, Yuepeng Pan, David Fowler, Jeffrey L. Collett Jr., Jan Willem Erisman, Keith Goulding, Yi Li, and Fusuo Zhang
Atmos. Chem. Phys., 17, 31–46, https://doi.org/10.5194/acp-17-31-2017, https://doi.org/10.5194/acp-17-31-2017, 2017
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This paper evaluates the effectiveness of emission control measures implemented in Beijing during the Parade Blue period by integrating our own results, official-released data and modeling data. We demonstrate that emission control measures make a major contribution to air quality improvement in Beijing and surrounding regions. We conclude a joint local and regional control of secondary aerosol precursors to be key to curbing air pollution in Beijing.
Yuxuan Wang, Beixi Jia, Sing-Chun Wang, Mark Estes, Lu Shen, and Yuanyu Xie
Atmos. Chem. Phys., 16, 15265–15276, https://doi.org/10.5194/acp-16-15265-2016, https://doi.org/10.5194/acp-16-15265-2016, 2016
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This paper provides empirical evidence that the year-to-year variability of summertime ozone over Houston is linked to the Bermuda High (BH) large-scale circulation patterns. It identifies two BH indices that can explain up to 70 % of the interannual variability of summertime ozone in Houston and illustrates the mechanism underlying the BH and ozone linkage. Such a mechanism is tested for applicability to other coastal urban regions along the US Gulf Coast.
Xiao Lu, Lin Zhang, Xu Yue, Jiachen Zhang, Daniel A. Jaffe, Andreas Stohl, Yuanhong Zhao, and Jingyuan Shao
Atmos. Chem. Phys., 16, 14687–14702, https://doi.org/10.5194/acp-16-14687-2016, https://doi.org/10.5194/acp-16-14687-2016, 2016
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Increasing wildfire activities in the mountainous western US may present a challenge for the region to attain a recently revised ozone air quality standard in summer. We quantify the wildfire influence on the ozone variability, trends, and number of high ozone days over this region in summers 1989–2010 using a Lagrangian dispersion model and statistical regression models.
Biwu Chu, Xiao Zhang, Yongchun Liu, Hong He, Yele Sun, Jingkun Jiang, Junhua Li, and Jiming Hao
Atmos. Chem. Phys., 16, 14219–14230, https://doi.org/10.5194/acp-16-14219-2016, https://doi.org/10.5194/acp-16-14219-2016, 2016
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The interactive effects between inorganic and organic species under highly complex pollution conditions remain uncertain and were studied in a smog chamber. This study indicated that the synergistic formation of secondary inorganic and organic aerosol might increase the secondary aerosol load in the atmosphere and contribute haze pollution in eastern China. These synergistic effects were related to the heterogeneous process on aerosol surface and need to be considered in air quality models.
Maria Zatko, Joseph Erbland, Joel Savarino, Lei Geng, Lauren Easley, Andrew Schauer, Timothy Bates, Patricia K. Quinn, Bonnie Light, David Morison, Hans D. Osthoff, Seth Lyman, William Neff, Bin Yuan, and Becky Alexander
Atmos. Chem. Phys., 16, 13837–13851, https://doi.org/10.5194/acp-16-13837-2016, https://doi.org/10.5194/acp-16-13837-2016, 2016
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This manuscript presents chemical and optical observations collected in the air and snow during UBWOS2014 in eastern Utah. These observations are used to calculate fluxes of reactive nitrogen associated with snow nitrate photolysis. Snow-sourced reactive nitrogen fluxes are compared to reactive nitrogen emission inventories to find that snow-sourced reactive nitrogen is a minor contributor to the reactive nitrogen budget, and thus wintertime ground-level ozone formation, in the Uintah Basin.
Qianqian Hong, Zhouqing Xie, Cheng Liu, Feiyue Wang, Pinhua Xie, Hui Kang, Jin Xu, Jiancheng Wang, Fengcheng Wu, Pengzhen He, Fusheng Mou, Shidong Fan, Yunsheng Dong, Haicong Zhan, Xiawei Yu, Xiyuan Chi, and Jianguo Liu
Atmos. Chem. Phys., 16, 13807–13821, https://doi.org/10.5194/acp-16-13807-2016, https://doi.org/10.5194/acp-16-13807-2016, 2016
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It is known that rapid industrialization in developing countries has led to an increase in air pollution. Here we firstly report the speciated atmospheric mercury during haze days based upon 1-year synchronous observations in an inland city in China. The findings provide direct evidence to understand the biogeochemical cycles of atmospheric mercury related to air pollution and an opportunity to evaluate the potential health risks of atmospheric mercury.
Qianjie Chen, Lei Geng, Johan A. Schmidt, Zhouqing Xie, Hui Kang, Jordi Dachs, Jihong Cole-Dai, Andrew J. Schauer, Madeline G. Camp, and Becky Alexander
Atmos. Chem. Phys., 16, 11433–11450, https://doi.org/10.5194/acp-16-11433-2016, https://doi.org/10.5194/acp-16-11433-2016, 2016
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The formation mechanisms of sulfate in the marine boundary layer are not well understood, which could result in large uncertainties in aerosol radiative forcing. We measure the oxygen isotopic composition (Δ17O) of sulfate collected in the MBL and analyze with a global transport model. Our results suggest that 33–50 % of MBL sulfate is formed via oxidation of S(IV) by hypohalous acids HOBr / HOCl in the aqueous phase, and the daily-mean HOBr/HOCl concentrations are on the order of 0.01–0.1 ppt.
Xiawei Yu, Zhibin Wang, Minghui Zhang, Uwe Kuhn, Zhouqing Xie, Yafang Cheng, Ulrich Pöschl, and Hang Su
Atmos. Chem. Phys., 16, 11337–11348, https://doi.org/10.5194/acp-16-11337-2016, https://doi.org/10.5194/acp-16-11337-2016, 2016
Hélène Angot, Ashu Dastoor, Francesco De Simone, Katarina Gårdfeldt, Christian N. Gencarelli, Ian M. Hedgecock, Sarka Langer, Olivier Magand, Michelle N. Mastromonaco, Claus Nordstrøm, Katrine A. Pfaffhuber, Nicola Pirrone, Andrei Ryjkov, Noelle E. Selin, Henrik Skov, Shaojie Song, Francesca Sprovieri, Alexandra Steffen, Kenjiro Toyota, Oleg Travnikov, Xin Yang, and Aurélien Dommergue
Atmos. Chem. Phys., 16, 10735–10763, https://doi.org/10.5194/acp-16-10735-2016, https://doi.org/10.5194/acp-16-10735-2016, 2016
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This is a synthesis of the atmospheric mercury (Hg) monitoring data available in recent years (2011–2015) in the Arctic and in Antarctica along with a comparison of these observations with numerical simulations using four cutting-edge global models. Based on this comparison, we discuss whether the processes that affect atmospheric Hg seasonality and interannual variability are appropriately represented in the models, and identify remaining research gaps.
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.
Junfeng Wang, Xinlei Ge, Yanfang Chen, Yafei Shen, Qi Zhang, Yele Sun, Jianzhong Xu, Shun Ge, Huan Yu, and Mindong Chen
Atmos. Chem. Phys., 16, 9109–9127, https://doi.org/10.5194/acp-16-9109-2016, https://doi.org/10.5194/acp-16-9109-2016, 2016
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Highly time- and chemically resolved submicron aerosol properties were characterized online for the first time during springtime in Nanjing by using the Aerodyne SP-AMS. Both chemical and size information of black carbon together with other aerosol species were simultaneously determined. An in-depth analysis of the data elucidates the sources and evolution processes of the fine aerosols in the YRD region. Our findings are valuable for air quality remediation in the densely populated regions.
Yele Sun, Wei Du, Pingqing Fu, Qingqing Wang, Jie Li, Xinlei Ge, Qi Zhang, Chunmao Zhu, Lujie Ren, Weiqi Xu, Jian Zhao, Tingting Han, Douglas R. Worsnop, and Zifa Wang
Atmos. Chem. Phys., 16, 8309–8329, https://doi.org/10.5194/acp-16-8309-2016, https://doi.org/10.5194/acp-16-8309-2016, 2016
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We have a comprehensive characterization of the sources, variations and processes of submicron aerosols in Beijing in winter using HR-AMS and GC/MS measurements. The primary sources including traffic, cooking, biomass burning and coal combustion emissions, and secondary components were separated and quantified with PMF. Our results elucidated the important roles of primary emissions, particularly coal combustion, and aqueous-phase processing in the formation of severe air pollution in winter.
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.
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.
Fang Zhang, Zhanqing Li, Yanan Li, Yele Sun, Zhenzhu Wang, Ping Li, Li Sun, Pucai Wang, Maureen Cribb, Chuanfeng Zhao, Tianyi Fan, Xin Yang, and Qingqing Wang
Atmos. Chem. Phys., 16, 5413–5425, https://doi.org/10.5194/acp-16-5413-2016, https://doi.org/10.5194/acp-16-5413-2016, 2016
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.
Yue Zhao, Lisa M. Wingen, Véronique Perraud, and Barbara J. Finlayson-Pitts
Atmos. Chem. Phys., 16, 3245–3264, https://doi.org/10.5194/acp-16-3245-2016, https://doi.org/10.5194/acp-16-3245-2016, 2016
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A significant fraction of airborne particles, which have significant impacts on human health, visibility, and climate, are formed from the oxidation of gaseous precursors to generate low-volatility products. We show here that a sesquiterpene, α-cedrene, efficiently forms high-viscosity semisolid particles with complex composition via mechanisms that involve the highly reactive Criegee intermediate and that high molecular weight products play an important role in new particle formation.
Maria Zatko, Lei Geng, Becky Alexander, Eric Sofen, and Katarina Klein
Atmos. Chem. Phys., 16, 2819–2842, https://doi.org/10.5194/acp-16-2819-2016, https://doi.org/10.5194/acp-16-2819-2016, 2016
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We have incorporated an idealized snowpack with a nitrate photolysis parameterization into a global chemical transport model (GEOS-Chem) to examine the implications of snow nitrate photolysis for boundary layer chemistry, the recycling and redistribution of reactive nitrogen, and the preservation of ice-core nitrate in ice cores across Antarctica and Greenland. We also examine the sensitivity of these processes to meteorological parameters and chemical, optical, and physical snow properties.
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.
Wei Deng, Qihou Hu, Tengyu Liu, Xinming Wang, Yanli Zhang, Xiang Ding, Yele Sun, Xinhui Bi, Jianzhen Yu, Weiqiang Yang, Xinyu Huang, Zhou Zhang, Zhonghui Huang, Quanfu He, A. Mellouki, and Christian George
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2016-50, https://doi.org/10.5194/acp-2016-50, 2016
Revised manuscript not accepted
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.
V. Shah, L. Jaeglé, L. E. Gratz, J. L. Ambrose, D. A. Jaffe, N. E. Selin, S. Song, T. L. Campos, F. M. Flocke, M. Reeves, D. Stechman, M. Stell, J. Festa, J. Stutz, A. J. Weinheimer, D. J. Knapp, D. D. Montzka, G. S. Tyndall, E. C. Apel, R. S. Hornbrook, A. J. Hills, D. D. Riemer, N. J. Blake, C. A. Cantrell, and R. L. Mauldin III
Atmos. Chem. Phys., 16, 1511–1530, https://doi.org/10.5194/acp-16-1511-2016, https://doi.org/10.5194/acp-16-1511-2016, 2016
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We present airborne observations of mercury over the southeastern USA during summer. Higher concentrations of oxidized mercury were observed in clean, dry air masses descending in the subtropical anti-cyclones. We used an atmospheric model to simulate the chemistry and transport of mercury. We found reasonable agreement with the observations when the modeled oxidation of elemental mercury was increased, suggesting fast cycling between elemental and oxidized mercury.
T. Liu, X. Wang, Q. Hu, W. Deng, Y. Zhang, X. Ding, X. Fu, F. Bernard, Z. Zhang, S. Lü, Q. He, X. Bi, J. Chen, Y. Sun, J. Yu, P. Peng, G. Sheng, and J. Fu
Atmos. Chem. Phys., 16, 675–689, https://doi.org/10.5194/acp-16-675-2016, https://doi.org/10.5194/acp-16-675-2016, 2016
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The formation of SOA and sulfate aerosols from the photooxidation of gasoline vehicle exhaust (GVE) when mixing with SO2 was investigated in a smog chamber. We found that the presence of GVE enhanced the conversion of SO2 to sulfate predominantly through reactions with stabilized Criegee intermediates. On the other hand, the elevated particle acidity enhanced the SOA production from GVE. This study indicated that SO2 and GVE could enhance each other in forming secondary aerosols.
S. Walter, A. Kock, T. Steinhoff, B. Fiedler, P. Fietzek, J. Kaiser, M. Krol, M. E. Popa, Q. Chen, T. Tanhua, and T. Röckmann
Biogeosciences, 13, 323–340, https://doi.org/10.5194/bg-13-323-2016, https://doi.org/10.5194/bg-13-323-2016, 2016
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Oceans are a source of H2, an indirect greenhouse gas. Measurements constraining the temporal and spatial patterns of oceanic H2 emissions are sparse and although H2 is assumed to be produced mainly biologically, direct evidence for biogenic marine production was lacking. By analyzing the H2 isotopic composition (δD) we were able to constrain the global H2 budget in more detail, verify biogenic production and point to additional sources. We also showed that current models are reasonably working.
W. Q. Xu, Y. L. Sun, C. Chen, W. Du, T. T. Han, Q. Q. Wang, P. Q. Fu, Z. F. Wang, X. J. Zhao, L. B. Zhou, D. S. Ji, P. C. Wang, and D. R. Worsnop
Atmos. Chem. Phys., 15, 13681–13698, https://doi.org/10.5194/acp-15-13681-2015, https://doi.org/10.5194/acp-15-13681-2015, 2015
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We have investigated the response of aerosol composition, size distributions, and oxidation properties to emission controls during the 2014 Asia- Pacific Economic Cooperation (APEC) summit in Beijing. Our results showed substantial changes of aerosol bulk composition during APEC with the most reductions in secondary aerosols in large accumulation modes, demonstrating that that emission controls over regional scales can substantially reduce secondary particulates.
W. J. Li, S. R. Chen, Y. S. Xu, X. C. Guo, Y. L. Sun, X. Y. Yang, Z. F. Wang, X. D. Zhao, J. M. Chen, and W. X. Wang
Atmos. Chem. Phys., 15, 13365–13376, https://doi.org/10.5194/acp-15-13365-2015, https://doi.org/10.5194/acp-15-13365-2015, 2015
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We found that anthropogenic soot, fly ash, and visible organic particles likely adhere to the surface of secondary inorganic particles larger than 200nm due to coagulation. Biomass burning and coal combustion both constantly contribute to anthropogenic particles in the Qinghai-Tibet Plateau (QTP) background atmosphere. Organic coating and soot on the surface of the aged particles could have different impacts on their hygroscopic and optical properties in the QTP compared to the urban aerosols.
J.-W. Xu, R. V. Martin, A. van Donkelaar, J. Kim, M. Choi, Q. Zhang, G. Geng, Y. Liu, Z. Ma, L. Huang, Y. Wang, H. Chen, H. Che, P. Lin, and N. Lin
Atmos. Chem. Phys., 15, 13133–13144, https://doi.org/10.5194/acp-15-13133-2015, https://doi.org/10.5194/acp-15-13133-2015, 2015
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1. GOCI (Geostationary Ocean Color Imager) retrieval of AOD is consistent with AERONET AOD (RMSE=0.08-0.1)
2. GOCI-derived PM2.5 is in significant agreement with in situ observations (r2=0.66, rRMSE=18.3%)
3. Population-weighted GOCI-derived PM2.5 over eastern China for 2013 is 53.8 μg/m3, threatening the health of its more than 400 million residents
4. Secondary inorganics (SO42-, NO3-, NH4+) & organic matter are the most significant components of GOCI-derived PM2.5.
Q. Chen, M. E. Popa, A. M. Batenburg, and T. Röckmann
Atmos. Chem. Phys., 15, 13003–13021, https://doi.org/10.5194/acp-15-13003-2015, https://doi.org/10.5194/acp-15-13003-2015, 2015
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We investigated soil production and uptake of H2 and associated isotope effects. Uptake and emission of H2 occurred simultaneously at all sampling sites, with strongest emission where N2 fixing legume was present. The fractionation constant during soil uptake was about 0.945 and it did not show positive correlation with deposition velocity. The isotopic composition of H2 emitted from soil with legume was about -530‰, which is less deuterium-depleted than isotope equilibrium between H2O and H2.
C. Chen, Y. L. Sun, W. Q. Xu, W. Du, L. B. Zhou, T. T. Han, Q. Q. Wang, P. Q. Fu, Z. F. Wang, Z. Q. Gao, Q. Zhang, and D. R. Worsnop
Atmos. Chem. Phys., 15, 12879–12895, https://doi.org/10.5194/acp-15-12879-2015, https://doi.org/10.5194/acp-15-12879-2015, 2015
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A comprehensive characterization of submicron aerosol composition and sources at 260m in urban Beijing during APEC 2014 is presented. Aerosol species were shown to decrease substantially by 40–80% during APEC, whereas the bulk composition was relatively similar to the result of synergetic controls of secondary precursors. Our results elucidated that the good air quality during APEC was the combined result of emission controls and meteorological effects, with the former playing the dominant role.
W. Xu, X. S. Luo, Y. P. Pan, L. Zhang, A. H. Tang, J. L. Shen, Y. Zhang, K. H. Li, Q. H. Wu, D. W. Yang, Y. Y. Zhang, J. Xue, W. Q. Li, Q. Q. Li, L. Tang, S. H. Lu, T. Liang, Y. A. Tong, P. Liu, Q. Zhang, Z. Q. Xiong, X. J. Shi, L. H. Wu, W. Q. Shi, K. Tian, X. H. Zhong, K. Shi, Q. Y. Tang, L. J. Zhang, J. L. Huang, C. E. He, F. H. Kuang, B. Zhu, H. Liu, X. Jin, Y. J. Xin, X. K. Shi, E. Z. Du, A. J. Dore, S. Tang, J. L. Collett Jr., K. Goulding, Y. X. Sun, J. Ren, F. S. Zhang, and X. J. Liu
Atmos. Chem. Phys., 15, 12345–12360, https://doi.org/10.5194/acp-15-12345-2015, https://doi.org/10.5194/acp-15-12345-2015, 2015
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The annual average concentrations (1.3-47.0µg N m-3) and dry plus wet/bulk deposition fluxes (2.9-83.3kg N ha-1 yr-1) of inorganic Nr species ranked by land use as urban > rural > background sites and by regions as north China > southeast China > southwest China > northeast China > northwest China > Tibetan Plateau, reflecting the impact of anthropogenic Nr emission. Average dry and wet/bulk N deposition fluxes were 20.6 ± 11.2 and 19.3 ± 9.2kg kg N ha-1 yr-1 across China, respectively.
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.
Y. Zhao, L. Zhang, Y. Pan, Y. Wang, F. Paulot, and D. K. Henze
Atmos. Chem. Phys., 15, 10905–10924, https://doi.org/10.5194/acp-15-10905-2015, https://doi.org/10.5194/acp-15-10905-2015, 2015
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Rapid Asian industrialization has led to increased atmospheric nitrogen deposition downwind. This work analyzes the sources and processes controlling atmospheric nitrogen deposition to the northwestern Pacific. Both nitrogen emissions and meteorology, largely controlled by the East Asian Monsoon, determine the seasonality of nitrogen deposition. Ascribing deposition over the marginal seas to nitrogen sources from different regions and sectors shows important contribution from fertilizer use.
W. Du, Y. L. Sun, Y. S. Xu, Q. Jiang, Q. Q. Wang, W. Yang, F. Wang, Z. P. Bai, X. D. Zhao, and Y. C. Yang
Atmos. Chem. Phys., 15, 10811–10824, https://doi.org/10.5194/acp-15-10811-2015, https://doi.org/10.5194/acp-15-10811-2015, 2015
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A fall field campaign was conducted at a national background site (3295m a.s.l.) over the Tibetan Plateau. The submicron aerosol was dominated by organics (43%) and sulfate (28%). Secondary organic aerosol (SOA) dominated OA (85%), 17% of which being aged biomass burning OA. New particle formation and growth events were frequently observed, with an average particle growth rate of 2.0nm per hour. The important role of organics in particle growth in the Tibetan Plateau was also demonstrated.
Y. L. Sun, Z. F. Wang, W. Du, Q. Zhang, Q. Q. Wang, P. Q. Fu, X. L. Pan, J. Li, J. Jayne, and D. R. Worsnop
Atmos. Chem. Phys., 15, 10149–10165, https://doi.org/10.5194/acp-15-10149-2015, https://doi.org/10.5194/acp-15-10149-2015, 2015
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We conducted the first long-term real-time measurement of submicron aerosol composition in Beijing using an ACSM for 1 year. The seasonal variations of mass concentrations and chemical composition of submicron aerosol were investigated in detail, and the meteorological effects on aerosol chemistry, particularly temperature and relative humidity, were elucidated. Finally, the potential source areas of aerosol species during four seasons were identified.
W. Tao, J. Liu, G. A. Ban-Weiss, D. A. Hauglustaine, L. Zhang, Q. Zhang, Y. Cheng, Y. Yu, and S. Tao
Atmos. Chem. Phys., 15, 8597–8614, https://doi.org/10.5194/acp-15-8597-2015, https://doi.org/10.5194/acp-15-8597-2015, 2015
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We examine the responses of a range of meteorological and air quality indicators to the expansion of urban land using WRF/Chem. Sensitivity studies indicate that the responses of pollutant concentrations to the spatial extent of urbanization are linear near the surface but nonlinear at higher altitudes. The results of process analysis demonstrate that urban heat island circulation and a deeper boundary layer with stronger turbulent intensities play a significant role in relocating pollutants.
Y. R. Yang, X. G. Liu, Y. Qu, J. L. An, R. Jiang, Y. H. Zhang, Y. L. Sun, Z. J. Wu, F. Zhang, W. Q. Xu, and Q. X. Ma
Atmos. Chem. Phys., 15, 8165–8178, https://doi.org/10.5194/acp-15-8165-2015, https://doi.org/10.5194/acp-15-8165-2015, 2015
P. Achakulwisut, L. J. Mickley, L. T. Murray, A. P. K. Tai, J. O. Kaplan, and B. Alexander
Atmos. Chem. Phys., 15, 7977–7998, https://doi.org/10.5194/acp-15-7977-2015, https://doi.org/10.5194/acp-15-7977-2015, 2015
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The atmosphere’s oxidative capacity determines the lifetime of many trace gases important to climate, chemistry, and human health. Yet uncertainties remain about its past variations, its controlling factors, and the radiative forcing of short-lived species it influences. To reduce these uncertainties, we must better quantify the natural emissions and chemical reaction mechanisms of organic compounds in the atmosphere, which play a role in governing the oxidative capacity.
S. Song, N. E. Selin, A. L. Soerensen, H. Angot, R. Artz, S. Brooks, E.-G. Brunke, G. Conley, A. Dommergue, R. Ebinghaus, T. M. Holsen, D. A. Jaffe, S. Kang, P. Kelley, W. T. Luke, O. Magand, K. Marumoto, K. A. Pfaffhuber, X. Ren, G.-R. Sheu, F. Slemr, T. Warneke, A. Weigelt, P. Weiss-Penzias, D. C. Wip, and Q. Zhang
Atmos. Chem. Phys., 15, 7103–7125, https://doi.org/10.5194/acp-15-7103-2015, https://doi.org/10.5194/acp-15-7103-2015, 2015
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A better knowledge of mercury (Hg) emission fluxes into the global atmosphere is important for assessing its human health impacts and evaluating the effectiveness of corresponding policy actions. We for the first time apply a top-down approach at a global scale to quantitatively estimate present-day mercury emission sources as well as key parameters in a chemical transport model, in order to better constrain the global biogeochemical cycle of mercury.
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.
Q. Jiang, Y. L. Sun, Z. Wang, and Y. Yin
Atmos. Chem. Phys., 15, 6023–6034, https://doi.org/10.5194/acp-15-6023-2015, https://doi.org/10.5194/acp-15-6023-2015, 2015
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Aerosol composition and sources during the Chinese spring festival are characterized in detail. The roles of fireworks and secondary aerosol in fine particle pollution were elucidated. We observed large reductions of primary species, whereas changes of secondary aerosol during the holiday period were minor. This has significant implications; reducing primary emissions on a local scale during severe haze episodes might have a limited effect on improving air quality in megacities.
Y. J. Zhang, L. L. Tang, Z. Wang, H. X. Yu, Y. L. Sun, D. Liu, W. Qin, F. Canonaco, A. S. H. Prévôt, H. L. Zhang, and H. C. Zhou
Atmos. Chem. Phys., 15, 1331–1349, https://doi.org/10.5194/acp-15-1331-2015, https://doi.org/10.5194/acp-15-1331-2015, 2015
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The chemical composition, sources, and evolution processes of PM1 were investigated with an Aerodyne ACSM during harvest seasons in the Yangtze River delta, China. Two biomass burning organic aerosol (BBOA) factors derived from PMF model were assessed. The oxidized BBOA contributes ~80% of the total BBOA loadings in the BB plumes. Evidence that BBOA may be oxidized to more aged and less volatile organics during the aging process was suggested.
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.
L. Geng, J. Cole-Dai, B. Alexander, J. Erbland, J. Savarino, A. J. Schauer, E. J. Steig, P. Lin, Q. Fu, and M. C. Zatko
Atmos. Chem. Phys., 14, 13361–13376, https://doi.org/10.5194/acp-14-13361-2014, https://doi.org/10.5194/acp-14-13361-2014, 2014
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Examinations on snowpit and firn core results from Summit, Greenland suggest that there are two mechanisms leading to the observed double nitrate peaks in some years in the industrial era: 1) long-rang transport of nitrate and 2) enhanced local photochemical production of nitrate. Both of these mechanisms are related to pollution transport, as the additional nitrate from either direct transport or enhanced local photochemistry requires enhanced nitrogen sources from anthropogenic 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. 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
E. D. Sofen, B. Alexander, E. J. Steig, M. H. Thiemens, S. A. Kunasek, H. M. Amos, A. J. Schauer, M. G. Hastings, J. Bautista, T. L. Jackson, L. E. Vogel, J. R. McConnell, D. R. Pasteris, and E. S. Saltzman
Atmos. Chem. Phys., 14, 5749–5769, https://doi.org/10.5194/acp-14-5749-2014, https://doi.org/10.5194/acp-14-5749-2014, 2014
L. Zhang, D. J. Jacob, X. Yue, N. V. Downey, D. A. Wood, and D. Blewitt
Atmos. Chem. Phys., 14, 5295–5309, https://doi.org/10.5194/acp-14-5295-2014, https://doi.org/10.5194/acp-14-5295-2014, 2014
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
L. T. Murray, L. J. Mickley, J. O. Kaplan, E. D. Sofen, M. Pfeiffer, and B. Alexander
Atmos. Chem. Phys., 14, 3589–3622, https://doi.org/10.5194/acp-14-3589-2014, https://doi.org/10.5194/acp-14-3589-2014, 2014
C. A. McLinden, V. Fioletov, K. F. Boersma, S. K. Kharol, N. Krotkov, L. Lamsal, P. A. Makar, R. V. Martin, J. P. Veefkind, and K. Yang
Atmos. Chem. Phys., 14, 3637–3656, https://doi.org/10.5194/acp-14-3637-2014, https://doi.org/10.5194/acp-14-3637-2014, 2014
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
G. C. M. Vinken, K. F. Boersma, A. van Donkelaar, and L. Zhang
Atmos. Chem. Phys., 14, 1353–1369, https://doi.org/10.5194/acp-14-1353-2014, https://doi.org/10.5194/acp-14-1353-2014, 2014
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
R. A. Ellis, D. J. Jacob, M. P. Sulprizio, L. Zhang, C. D. Holmes, B. A. Schichtel, T. Blett, E. Porter, L. H. Pardo, and J. A. Lynch
Atmos. Chem. Phys., 13, 9083–9095, https://doi.org/10.5194/acp-13-9083-2013, https://doi.org/10.5194/acp-13-9083-2013, 2013
Y. L. Sun, Z. F. Wang, P. Q. Fu, T. Yang, Q. Jiang, H. B. Dong, J. Li, and J. J. Jia
Atmos. Chem. Phys., 13, 4577–4592, https://doi.org/10.5194/acp-13-4577-2013, https://doi.org/10.5194/acp-13-4577-2013, 2013
Y. Wang, Q. Q. Zhang, K. He, Q. Zhang, and L. Chai
Atmos. Chem. Phys., 13, 2635–2652, https://doi.org/10.5194/acp-13-2635-2013, https://doi.org/10.5194/acp-13-2635-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Modeling the drivers of fine PM pollution over Central Europe: impacts and contributions of emissions from different sources
Reaction of SO3 with H2SO4 and its implications for aerosol particle formation in the gas phase and at the air–water interface
Weakened aerosol–radiation interaction exacerbating ozone pollution in eastern China since China's clean air actions
Uncertainties from biomass burning aerosols in air quality models obscure public health impacts in Southeast Asia
Oxidative potential apportionment of atmospheric PM1: a new approach combining high-sensitive online analysers for chemical composition and offline OP measurement technique
Aqueous-phase chemistry of glyoxal with multifunctional reduced nitrogen compounds: a potential missing route for secondary brown carbon
An updated modeling framework to simulate Los Angeles air quality – Part 1: Model development, evaluation, and source apportionment
Frequent haze events associated with transport and stagnation over the corridor between the North China Plain and Yangtze River Delta
Evaluation of WRF-Chem-simulated meteorology and aerosols over northern India during the severe pollution episode of 2016
How well are aerosol–cloud interactions represented in climate models? – Part 1: Understanding the sulfate aerosol production from the 2014–15 Holuhraun eruption
pH regulates the formation of organosulfates and inorganic sulfate from organic peroxide reaction with dissolved SO2 in aquatic media
Technical note: Accurate, reliable, and high-resolution air quality predictions by improving the Copernicus Atmosphere Monitoring Service using a novel statistical post-processing method
Contribution of intermediate-volatility organic compounds from on-road transport to secondary organic aerosol levels in Europe
Secondary Organic Aerosols Derived from Intermediate Volatility n-Alkanes Adopt Low Viscous Phase State
Development of an integrated model framework for multi-air-pollutant exposure assessments in high-density cities
Observation-Constrained Kinetic Modelling of Isoprene SOA Formation in the Atmosphere
CAMx–UNIPAR simulation of secondary organic aerosol mass formed from multiphase reactions of hydrocarbons under the Central Valley urban atmospheres of California
Impact of urbanization on fine particulate matter concentrations over central Europe
Measurement report: Assessing the impacts of emission uncertainty on aerosol optical properties and radiative forcing from biomass burning in peninsular Southeast Asia
Significant impact of urban-tree biogenic emissions on air quality estimated by a bottom-up inventory and chemistry-transport modeling
The Emissions Model Intercomparison Project (Emissions-MIP): quantifying model sensitivity to emission characteristics
Dynamics-based estimates of decline trend with fine temporal variations in China's PM2.5 emissions
Modeling atmospheric brown carbon in the GISS ModelE Earth system model
Dual roles of inorganic aqueous phase on SOA growth from benzene and phenol
Effects of simulated secondary organic aerosol water on PM1 levels and composition over the US
Reactive organic carbon air emissions from mobile sources in the United States
Development and evaluation of processes affecting simulation of diel fine particulate matter variation in the GEOS-Chem model
Substantially positive contributions of new particle formation to cloud condensation nuclei under low supersaturation in China based on numerical model improvements
Evolution of atmospheric age of particles and its implications for the formation of a severe haze event in eastern China
A multimodel evaluation of the potential impact of shipping on particle species in the Mediterranean Sea
Investigating the contribution of grown new particles to cloud condensation nuclei with largely varying pre-existing particles – Part 2: Modeling chemical drivers and 3-D NPF occurrence
How does tropospheric VOC chemistry affect climate? An investigation of preindustrial control simulations using the Community Earth System Model version 2
Anthropogenic amplification of biogenic secondary organic aerosol production
A dynamic parameterization of sulfuric acid–dimethylamine nucleation and its application in three-dimensional modeling
Modeling dust mineralogical composition: sensitivity to soil mineralogy atlases and their expected climate impacts
Assessment of the impacts of cloud chemistry on surface SO2 and sulfate levels in typical regions of China
Impact of Landes forest fires on air quality in France during the 2022 summer
Global nitrogen and sulfur deposition mapping using a measurement–model fusion approach
Comprehensive simulations of new particle formation events in Beijing with a cluster dynamics–multicomponent sectional model
Implications of differences between recent anthropogenic aerosol emission inventories for diagnosed AOD and radiative forcing from 1990 to 2019
Unbalanced emission reductions of different species and sectors in China during COVID-19 lockdown derived by multi-species surface observation assimilation
Simulating organic aerosol in Delhi with WRF-Chem using the volatility-basis-set approach: exploring model uncertainty with a Gaussian process emulator
Modelling wintertime sea-spray aerosols under Arctic haze conditions
Impact of solar geoengineering on wildfires in the 21st century in CESM2/WACCM6
Linking gas, particulate, and toxic endpoints to air emissions in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM)
Contribution of regional aerosol nucleation to low-level CCN in an Amazonian deep convective environment: results from a regionally nested global model
Coarse particulate matter air quality in East Asia: implications for fine particulate nitrate
Foreign emissions exacerbate PM2.5 pollution in China through nitrate chemistry
Analysis of new particle formation events and comparisons to simulations of particle number concentrations based on GEOS-Chem–advanced particle microphysics in Beijing, China
Simulation of organic aerosol, its precursors, and related oxidants in the Landes pine forest in southwestern France: accounting for domain-specific land use and physical conditions
Lukáš Bartík, Peter Huszár, Jan Karlický, Ondřej Vlček, and Kryštof Eben
Atmos. Chem. Phys., 24, 4347–4387, https://doi.org/10.5194/acp-24-4347-2024, https://doi.org/10.5194/acp-24-4347-2024, 2024
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The presented study deals with the attribution of fine particulate matter (PM2.5) concentrations to anthropogenic emissions over Central Europe using regional-scale models. It calculates the present-day contributions of different emissions sectors to concentrations of PM2.5 and its secondary components. Moreover, the study investigates the effect of chemical nonlinearities by using multiple source attribution methods and secondary organic aerosol calculation methods.
Rui Wang, Yang Cheng, Shasha Chen, Rongrong Li, Yue Hu, Xiaokai Guo, Tianlei Zhang, Fengmin Song, and Hao Li
Atmos. Chem. Phys., 24, 4029–4046, https://doi.org/10.5194/acp-24-4029-2024, https://doi.org/10.5194/acp-24-4029-2024, 2024
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We used quantum chemical calculations, Born–Oppenheimer molecular dynamics simulations, and the ACDC kinetic model to characterize SO3–H2SO4 interaction in the gas phase and at the air–water interface and to study the effect of H2S2O7 on H2SO4–NH3-based clusters. The work expands our understanding of new pathways for the loss of SO3 in acidic polluted areas and helps reveal some missing sources of NPF in metropolitan industrial regions and understand the atmospheric organic–sulfur cycle better.
Hao Yang, Lei Chen, Hong Liao, Jia Zhu, Wenjie Wang, and Xin Li
Atmos. Chem. Phys., 24, 4001–4015, https://doi.org/10.5194/acp-24-4001-2024, https://doi.org/10.5194/acp-24-4001-2024, 2024
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The present study quantifies the response of aerosol–radiation interaction (ARI) to anthropogenic emission reduction from 2013 to 2017, with the main focus on the contribution to changed O3 concentrations over eastern China both in summer and winter using the WRF-Chem model. The weakened ARI due to decreased anthropogenic emission aggravates the summer (winter) O3 pollution by +0.81 ppb (+0.63 ppb), averaged over eastern China.
Margaret R. Marvin, Paul I. Palmer, Fei Yao, Mohd Talib Latif, and Md Firoz Khan
Atmos. Chem. Phys., 24, 3699–3715, https://doi.org/10.5194/acp-24-3699-2024, https://doi.org/10.5194/acp-24-3699-2024, 2024
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We use an atmospheric chemistry model to investigate aerosols emitted from fire activity across Southeast Asia. We find that the limited nature of measurements in this region leads to large uncertainties that significantly hinder the model representation of these aerosols and their impacts on air quality. As a result, the number of monthly attributable deaths is underestimated by as many as 4500, particularly in March at the peak of the mainland burning season.
Julie Camman, Benjamin Chazeau, Nicolas Marchand, Amandine Durand, Grégory Gille, Ludovic Lanzi, Jean-Luc Jaffrezo, Henri Wortham, and Gaëlle Uzu
Atmos. Chem. Phys., 24, 3257–3278, https://doi.org/10.5194/acp-24-3257-2024, https://doi.org/10.5194/acp-24-3257-2024, 2024
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Fine particle (PM1) pollution is a major health issue in the city of Marseille, which is subject to numerous pollution sources. Sampling carried out during the summer enabled a fine characterization of the PM1 sources and their oxidative potential, a promising new metric as a proxy for health impact. PM1 came mainly from combustion sources, secondary ammonium sulfate, and organic nitrate, while the oxidative potential of PM1 came from these sources and from resuspended dust in the atmosphere.
Yuemeng Ji, Zhang Shi, Wenjian Li, Jiaxin Wang, Qiuju Shi, Yixin Li, Lei Gao, Ruize Ma, Weijun Lu, Lulu Xu, Yanpeng Gao, Guiying Li, and Taicheng An
Atmos. Chem. Phys., 24, 3079–3091, https://doi.org/10.5194/acp-24-3079-2024, https://doi.org/10.5194/acp-24-3079-2024, 2024
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The formation mechanisms for secondary brown carbon (SBrC) contributed by multifunctional reduced nitrogen compounds (RNCs) remain unclear. Hence, from combined laboratory experiments and quantum chemical calculations, we investigated the heterogeneous reactions of glyoxal (GL) with multifunctional RNCs, which are driven by four-step indirect nucleophilic addition reactions. Our results show a possible missing source for SBrC formation on urban, regional, and global scales.
Elyse A. Pennington, Yuan Wang, Benjamin C. Schulze, Karl M. Seltzer, Jiani Yang, Bin Zhao, Zhe Jiang, Hongru Shi, Melissa Venecek, Daniel Chau, Benjamin N. Murphy, Christopher M. Kenseth, Ryan X. Ward, Havala O. T. Pye, and John H. Seinfeld
Atmos. Chem. Phys., 24, 2345–2363, https://doi.org/10.5194/acp-24-2345-2024, https://doi.org/10.5194/acp-24-2345-2024, 2024
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To assess the air quality in Los Angeles (LA), we improved the CMAQ model by using dynamic traffic emissions and new secondary organic aerosol schemes to represent volatile chemical products. Source apportionment demonstrates that the urban areas of the LA Basin and vicinity are NOx-saturated, with the largest sensitivity of O3 to changes in volatile organic compounds in the urban core. The improvement and remaining issues shed light on the future direction of the model development.
Feifan Yan, Hang Su, Yafang Cheng, Rujin Huang, Hong Liao, Ting Yang, Yuanyuan Zhu, Shaoqing Zhang, Lifang Sheng, Wenbin Kou, Xinran Zeng, Shengnan Xiang, Xiaohong Yao, Huiwang Gao, and Yang Gao
Atmos. Chem. Phys., 24, 2365–2376, https://doi.org/10.5194/acp-24-2365-2024, https://doi.org/10.5194/acp-24-2365-2024, 2024
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PM2.5 pollution is a major air quality issue deteriorating human health, and previous studies mostly focus on regions like the North China Plain and Yangtze River Delta. However, the characteristics of PM2.5 concentrations between these two regions are studied less often. Focusing on the transport corridor region, we identify an interesting seesaw transport phenomenon with stagnant weather conditions, conducive to PM2.5 accumulation over this region, resulting in large health effects.
Prerita Agarwal, David S. Stevenson, and Mathew R. Heal
Atmos. Chem. Phys., 24, 2239–2266, https://doi.org/10.5194/acp-24-2239-2024, https://doi.org/10.5194/acp-24-2239-2024, 2024
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Air pollution levels across northern India are amongst some of the worst in the world, with episodic and hazardous haze events. Here, the ability of the WRF-Chem model to predict air quality over northern India is assessed against several datasets. Whilst surface wind speed and particle pollution peaks are over- and underestimated, respectively, meteorology and aerosol trends are adequately captured, and we conclude it is suitable for investigating severe particle pollution events.
George Jordan, Florent Malavelle, Ying Chen, Amy Peace, Eliza Duncan, Daniel G. Partridge, Paul Kim, Duncan Watson-Parris, Toshihiko Takemura, David Neubauer, Gunnar Myhre, Ragnhild Skeie, Anton Laakso, and James Haywood
Atmos. Chem. Phys., 24, 1939–1960, https://doi.org/10.5194/acp-24-1939-2024, https://doi.org/10.5194/acp-24-1939-2024, 2024
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The 2014–15 Holuhraun eruption caused a huge aerosol plume in an otherwise unpolluted region, providing a chance to study how aerosol alters cloud properties. This two-part study uses observations and models to quantify this relationship’s impact on the Earth’s energy budget. Part 1 suggests the models capture the observed spatial and chemical evolution of the plume, yet no model plume is exact. Understanding these differences is key for Part 2, where changes to cloud properties are explored.
Lin Du, Xiaofan Lv, Makroni Lily, Kun Li, and Narcisse Tsona Tchinda
Atmos. Chem. Phys., 24, 1841–1853, https://doi.org/10.5194/acp-24-1841-2024, https://doi.org/10.5194/acp-24-1841-2024, 2024
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This study explores the pH effect on the reaction of dissolved SO2 with selected organic peroxides. Results show that the formation of organic and/or inorganic sulfate from these peroxides strongly depends on their electronic structures, and these processes are likely to alter the chemical composition of dissolved organic matter in different ways. The rate constants of these reactions exhibit positive pH and temperature dependencies within pH 1–10 and 240–340 K ranges.
Angelo Riccio and Elena Chianese
Atmos. Chem. Phys., 24, 1673–1689, https://doi.org/10.5194/acp-24-1673-2024, https://doi.org/10.5194/acp-24-1673-2024, 2024
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Starting from the Copernicus Atmosphere Monitoring Service (CAMS), we provided a novel ensemble statistical post-processing approach to improve their air quality predictions. Our approach is able to provide reliable short-term forecasts of pollutant concentrations, which is a key challenge in supporting national authorities in their tasks related to EU Air Quality Directives, such as planning and reporting the state of air quality to the citizens.
Stella E. I. Manavi and Spyros N. Pandis
Atmos. Chem. Phys., 24, 891–909, https://doi.org/10.5194/acp-24-891-2024, https://doi.org/10.5194/acp-24-891-2024, 2024
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Organic vapors of intermediate volatility have often been neglected as sources of atmospheric organic aerosol. In this work we use a new approach for their simulation and quantify the contribution of these compounds emitted by transportation sources (gasoline and diesel vehicles) to particulate matter over Europe. The estimated secondary organic aerosol levels are on average 60 % higher than predicted by previous approaches. However, these estimates are probably lower limits.
Tommaso Galeazzo, Bernard Aumont, Marie Camredon, Richard Valorso, Yong B. Lim, Paul J. Ziemann, and Manabu Shiraiwa
EGUsphere, https://doi.org/10.5194/egusphere-2024-51, https://doi.org/10.5194/egusphere-2024-51, 2024
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SOA derived from n-alkanes is a major component of anthropogenic particulate matter. We provide a comprehensive analysis of n-alkane SOA by explicit chemistry modeling, machine learning, and laboratory experiments, showing that n-alkane SOA adopt low viscous semisolid or liquid states. Our results indicate little kinetic limitations of mass accommodation in SOA formation, supporting the application of equilibrium partitioning for simulating n-alkane SOA in large-scale atmospheric models.
Zhiyuan Li, Kin-Fai Ho, Harry Fung Lee, and Steve Hung Lam Yim
Atmos. Chem. Phys., 24, 649–661, https://doi.org/10.5194/acp-24-649-2024, https://doi.org/10.5194/acp-24-649-2024, 2024
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This study developed an integrated model framework for accurate multi-air-pollutant exposure assessments in high-density and high-rise cities. Following the proposed integrated model framework, we established multi-air-pollutant exposure models for four major PM10 chemical species as well as four criteria air pollutants with R2 values ranging from 0.73 to 0.93. The proposed framework serves as an important tool for combined exposure assessment in epidemiological studies.
Chuanyang Shen, Xiaoyan Yang, Joel Thornton, John Shilling, Chenyang Bi, Gabriel Isaacman-VanWertz, and Haofei Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2024-97, https://doi.org/10.5194/egusphere-2024-97, 2024
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In this work, a multiphase condensed isoprene oxidation mechanism was developed to simulate isoprene SOA formation from chamber and field studies. Our results show that the measured isoprene SOA mass can be reasonably reproduced using the new mechanism. The simulation results indicate that multifunctional low-volatility products contribute significantly to total isoprene SOA. Our findings emphasize that the pathways to produce these low-volatility species should be considered in models.
Yujin Jo, Myoseon Jang, Sanghee Han, Azad Madhu, Bonyoung Koo, Yiqin Jia, Zechen Yu, Soontae Kim, and Jinsoo Park
Atmos. Chem. Phys., 24, 487–508, https://doi.org/10.5194/acp-24-487-2024, https://doi.org/10.5194/acp-24-487-2024, 2024
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The CAMx–UNIPAR model simulated the SOA budget formed via multiphase reactions of hydrocarbons and the impact of emissions and climate on SOA characteristics under California’s urban environments during winter 2018. SOA growth was dominated by daytime oxidation of long-chain alkanes and nighttime terpene oxidation with O3 and NO−3 radicals. The spatial distributions of anthropogenic SOA were affected by the northwesterly wind, whereas those of biogenic SOA were insensitive to wind directions.
Peter Huszar, Alvaro Patricio Prieto Perez, Lukáš Bartík, Jan Karlický, and Anahi Villalba-Pradas
Atmos. Chem. Phys., 24, 397–425, https://doi.org/10.5194/acp-24-397-2024, https://doi.org/10.5194/acp-24-397-2024, 2024
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Urbanization transforms rural land into artificial land, while due to human activities, it also introduces a great quantity of emissions. We quantify the impact of urbanization on the final particulate matter pollutant levels by looking not only at these emissions, but also at the way urban land cover influences meteorological conditions, how the removal of pollutants changes due to urban land cover, and how biogenic emissions from vegetation change due to less vegetation in urban areas.
Yinbao Jin, Yiming Liu, Xiao Lu, Xiaoyang Chen, Ao Shen, Haofan Wang, Yinping Cui, Yifei Xu, Siting Li, Jian Liu, Ming Zhang, Yingying Ma, and Qi Fan
Atmos. Chem. Phys., 24, 367–395, https://doi.org/10.5194/acp-24-367-2024, https://doi.org/10.5194/acp-24-367-2024, 2024
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This study aims to address these issues by evaluating eight independent biomass burning (BB) emission inventories (GFED, FINN1.5, FINN2.5 MOS, FINN2.5 MOSVIS, GFAS, FEER, QFED, and IS4FIRES) using the WRF-Chem model and analyzing their impact on aerosol optical properties (AOPs) and direct radiative forcing (DRF) during wildfire events in peninsular Southeast Asia (PSEA) that occurred in March 2019.
Alice Maison, Lya Lugon, Soo-Jin Park, Alexia Baudic, Christopher Cantrell, Florian Couvidat, Barbara D'Anna, Claudia Di Biagio, Aline Gratien, Valérie Gros, Carmen Kalalian, Julien Kammer, Vincent Michoud, Jean-Eudes Petit, Marwa Shahin, Leila Simon, Myrto Valari, Jérémy Vigneron, Andrée Tuzet, and Karine Sartelet
EGUsphere, https://doi.org/10.5194/egusphere-2023-2786, https://doi.org/10.5194/egusphere-2023-2786, 2023
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This study presents the development of a bottom-up inventory of urban-tree biogenic emissions. Emissions are computed for each tree based on their location and characteristics and are integrated in the regional air-quality model WRF-CHIMERE. The impact of these biogenic emissions on air quality is quantified for June–July 2022. Over Paris city, urban trees increase the concentrations of particulate organic matter by 4.6 %, of PM2.5 by 0.6 % and of ozone by 1.0 % on average over the two months.
Hamza Ahsan, Hailong Wang, Jingbo Wu, Mingxuan Wu, Steven J. Smith, Susanne Bauer, Harrison Suchyta, Dirk Olivié, Gunnar Myhre, Hitoshi Matsui, Huisheng Bian, Jean-François Lamarque, Ken Carslaw, Larry Horowitz, Leighton Regayre, Mian Chin, Michael Schulz, Ragnhild Bieltvedt Skeie, Toshihiko Takemura, and Vaishali Naik
Atmos. Chem. Phys., 23, 14779–14799, https://doi.org/10.5194/acp-23-14779-2023, https://doi.org/10.5194/acp-23-14779-2023, 2023
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We examine the impact of the assumed effective height of SO2 injection, SO2 and BC emission seasonality, and the assumed fraction of SO2 emissions injected as SO4 on climate and chemistry model results. We find that the SO2 injection height has a large impact on surface SO2 concentrations and, in some models, radiative flux. These assumptions are a
hiddensource of inter-model variability and may be leading to bias in some climate model results.
Zhen Peng, Lili Lei, Zhe-Min Tan, Meigen Zhang, Aijun Ding, and Xingxia Kou
Atmos. Chem. Phys., 23, 14505–14520, https://doi.org/10.5194/acp-23-14505-2023, https://doi.org/10.5194/acp-23-14505-2023, 2023
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Annual PM2.5 emissions in China consistently decreased by about 3% to 5% from 2017 to 2020 with spatial variations and seasonal dependencies. High-temporal-resolution and dynamics-based PM2.5 emission estimates provide quantitative diurnal variations for each season. Significant reductions in PM2.5 emissions in the North China Plain and northeast of China in 2020 were caused by COVID-19.
Maegan A. DeLessio, Kostas Tsigaridis, Susanne E. Bauer, Jacek Chowdhary, and Gregory L. Schuster
EGUsphere, https://doi.org/10.5194/egusphere-2023-2472, https://doi.org/10.5194/egusphere-2023-2472, 2023
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This study presents the first explicit representation of brown carbon aerosols in the GISS ModelE Earth system model (ESM). Model sensitivity to a range of brown carbon parameters, as well as model performance compared to AERONET and MODIS retrievals of total aerosol properties, was assessed. General recommendations for incorporating brown carbon into ESMs are also included.
Jiwon Choi, Myoseon Jang, and Spencer Blau
EGUsphere, https://doi.org/10.5194/egusphere-2023-2461, https://doi.org/10.5194/egusphere-2023-2461, 2023
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A persistent phenoxy radical (PPR) effectively forms via a heterogeneous reaction of phenol and phenol-related products in the presence of wet-inorganic aerosol. These PPR can catalytically consume ozone during a NOx cycle and negatively influence SOA formation. SOA formation from phenol or benzene is simulated using the UNIPAR model which predicted SOA formation via multiphase reactions of hydrocarbons and compared with chamber data obtained under varying NOx levels, humidity, and seed types.
Stylianos Kakavas, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 13555–13564, https://doi.org/10.5194/acp-23-13555-2023, https://doi.org/10.5194/acp-23-13555-2023, 2023
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Water uptake from organic species in aerosol can affect the partitioning of semi-volatile inorganic compounds but are not considered in global and chemical transport models. We address this with a version of the PM-CAMx model that considers such organic water effects and use it to carry out 1-year aerosol simulations over the continental US. We show that such organic water impacts can increase dry PM1 levels by up to 2 μg m-3 when RH levels and PM1 concentrations are high.
Benjamin N. Murphy, Darrell Sonntag, Karl M. Seltzer, Havala O. T. Pye, Christine Allen, Evan Murray, Claudia Toro, Drew R. Gentner, Cheng Huang, Shantanu Jathar, Li Li, Andrew A. May, and Allen L. Robinson
Atmos. Chem. Phys., 23, 13469–13483, https://doi.org/10.5194/acp-23-13469-2023, https://doi.org/10.5194/acp-23-13469-2023, 2023
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We update methods for calculating organic particle and vapor emissions from mobile sources in the USA. Conventionally, particulate matter (PM) and volatile organic carbon (VOC) are speciated without consideration of primary semivolatile emissions. Our methods integrate state-of-the-science speciation profiles and correct for common artifacts when sampling emissions in a laboratory. We quantify impacts of the emission updates on ambient pollution with the Community Multiscale Air Quality model.
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.
Chupeng Zhang, Shangfei Hai, Yang Gao, Yuhang Wang, Shaoqing Zhang, Lifang Sheng, Bin Zhao, Shuxiao Wang, Jingkun Jiang, Xin Huang, Xiaojing Shen, Junying Sun, Aura Lupascu, Manish Shrivastava, Jerome D. Fast, Wenxuan Cheng, Xiuwen Guo, Ming Chu, Nan Ma, Juan Hong, Qiaoqiao Wang, Xiaohong Yao, and Huiwang Gao
Atmos. Chem. Phys., 23, 10713–10730, https://doi.org/10.5194/acp-23-10713-2023, https://doi.org/10.5194/acp-23-10713-2023, 2023
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New particle formation is an important source of atmospheric particles, exerting critical influences on global climate. Numerical models are vital tools to understanding atmospheric particle evolution, which, however, suffer from large biases in simulating particle numbers. Here we improve the model chemical processes governing particle sizes and compositions. The improved model reveals substantial contributions of newly formed particles to climate through effects on cloud condensation nuclei.
Xiaodong Xie, Jianlin Hu, Momei Qin, Song Guo, Min Hu, Dongsheng Ji, Hongli Wang, Shengrong Lou, Cheng Huang, Chong Liu, Hongliang Zhang, Qi Ying, Hong Liao, and Yuanhang Zhang
Atmos. Chem. Phys., 23, 10563–10578, https://doi.org/10.5194/acp-23-10563-2023, https://doi.org/10.5194/acp-23-10563-2023, 2023
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The atmospheric age of particles reflects how long particles have been formed and suspended in the atmosphere, which is closely associated with the evolution processes of particles. An analysis of the atmospheric age of PM2.5 provides a unique perspective on the evolution processes of different PM2.5 components. The results also shed lights on how to design effective emission control actions under unfavorable meteorological conditions.
Lea Fink, Matthias Karl, Volker Matthias, Sonia Oppo, Richard Kranenburg, Jeroen Kuenen, Sara Jutterström, Jana Moldanova, Elisa Majamäki, and Jukka-Pekka Jalkanen
Atmos. Chem. Phys., 23, 10163–10189, https://doi.org/10.5194/acp-23-10163-2023, https://doi.org/10.5194/acp-23-10163-2023, 2023
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The Mediterranean Sea is a heavily trafficked shipping area, and air quality monitoring stations in numerous cities along the Mediterranean coast have detected high levels of air pollutants originating from shipping emissions. The current study investigates how existing restrictions on shipping-related emissions to the atmosphere ensure compliance with legislation. Focus was laid on fine particles and particle species, which were simulated with five different chemical transport models.
Ming Chu, Xing Wei, Shangfei Hai, Yang Gao, Huiwang Gao, Yujiao Zhu, Biwu Chu, Nan Ma, Juan Hong, Yele Sun, and Xiaohong Yao
EGUsphere, https://doi.org/10.5194/egusphere-2023-540, https://doi.org/10.5194/egusphere-2023-540, 2023
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We used a 20-bin WRF-Chem model to simulate NPF events in the NCP during a three-week observational period in the summer of 2019. The model was able to reproduce the observations during June 29–July 6, which was characterized by a high frequency of NPF occurrence.
Noah A. Stanton and Neil F. Tandon
Atmos. Chem. Phys., 23, 9191–9216, https://doi.org/10.5194/acp-23-9191-2023, https://doi.org/10.5194/acp-23-9191-2023, 2023
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Chemistry in Earth’s atmosphere has a potentially strong but very uncertain impact on climate. Past attempts to fully model chemistry in Earth’s troposphere (the lowest layer of the atmosphere) typically simplified the representation of Earth’s surface, which in turn limited the ability to simulate changes in climate. The cutting-edge model that we use in this study does not require such simplification, and we use it to examine the climate effects of chemical interactions in the troposphere.
Yiqi Zheng, Larry W. Horowitz, Raymond Menzel, David J. Paynter, Vaishali Naik, Jingyi Li, and Jingqiu Mao
Atmos. Chem. Phys., 23, 8993–9007, https://doi.org/10.5194/acp-23-8993-2023, https://doi.org/10.5194/acp-23-8993-2023, 2023
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Biogenic secondary organic aerosols (SOAs) account for a large fraction of fine aerosol at the global scale. Using long-term measurements and a climate model, we investigate anthropogenic impacts on biogenic SOA at both decadal and centennial timescales. Results show that despite reductions in biogenic precursor emissions, SOA has been strongly amplified by anthropogenic emissions since the preindustrial era and exerts a cooling radiative forcing.
Yuyang Li, Jiewen Shen, Bin Zhao, Runlong Cai, Shuxiao Wang, Yang Gao, Manish Shrivastava, Da Gao, Jun Zheng, Markku Kulmala, and Jingkun Jiang
Atmos. Chem. Phys., 23, 8789–8804, https://doi.org/10.5194/acp-23-8789-2023, https://doi.org/10.5194/acp-23-8789-2023, 2023
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We set up a new parameterization for 1.4 nm particle formation rates from sulfuric acid–dimethylamine (SA–DMA) nucleation, fully including the effects of coagulation scavenging and cluster stability. Incorporating the new parameterization into 3-D chemical transport models, we achieved better consistencies between simulation results and observation data. This new parameterization provides new insights into atmospheric nucleation simulations and its effects on atmospheric pollution or health.
María Gonçalves Ageitos, Vincenzo Obiso, Ron L. Miller, Oriol Jorba, Martina Klose, Matt Dawson, Yves Balkanski, Jan Perlwitz, Sara Basart, Enza Di Tomaso, Jerónimo Escribano, Francesca Macchia, Gilbert Montané, Natalie M. Mahowald, Robert O. Green, David R. Thompson, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 23, 8623–8657, https://doi.org/10.5194/acp-23-8623-2023, https://doi.org/10.5194/acp-23-8623-2023, 2023
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Dust aerosols affect our climate differently depending on their mineral composition. We include dust mineralogy in an atmospheric model considering two existing soil maps, which still have large associated uncertainties. The soil data and the distribution of the minerals in different aerosol sizes are key to our model performance. We find significant regional variations in climate-relevant variables, which supports including mineralogy in our current models and the need for improved soil maps.
Jianyan Lu, Sunling Gong, Jian Zhang, Jianmin Chen, Lei Zhang, and Chunhong Zhou
Atmos. Chem. Phys., 23, 8021–8037, https://doi.org/10.5194/acp-23-8021-2023, https://doi.org/10.5194/acp-23-8021-2023, 2023
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WRF/CUACE was used to assess the cloud chemistry contribution in China. Firstly, the CUACE cloud chemistry scheme was found to reproduce well the cloud processing and consumption of H2O2, O3, and SO2, as well as the increase of sulfate. Secondly, during cloud availability in December under a heavy pollution episode, sulfate production increased 60–95 % and SO2 was reduced by over 80 %. This study provides a way to analyze the phenomenon of overestimation of SO2 in many chemical transport models.
Laurent Menut, Arineh Cholakian, Guillaume Siour, Rémy Lapere, Romain Pennel, Sylvain Mailler, and Bertrand Bessagnet
Atmos. Chem. Phys., 23, 7281–7296, https://doi.org/10.5194/acp-23-7281-2023, https://doi.org/10.5194/acp-23-7281-2023, 2023
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This study is about the wildfires occurring in France during the summer 2022. We study the forest fires that took place in the Landes during the summer of 2022. We show the direct impact of these fires on the air quality, especially downstream of the smoke plume towards the Paris region. We quantify the impact of these fires on the pollutants peak concentrations and the possible exceedance of thresholds.
Hannah J. Rubin, Joshua S. Fu, Frank Dentener, Rui Li, Kan Huang, and Hongbo Fu
Atmos. Chem. Phys., 23, 7091–7102, https://doi.org/10.5194/acp-23-7091-2023, https://doi.org/10.5194/acp-23-7091-2023, 2023
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We update the 2010 global deposition budget for nitrogen (N) and sulfur (S) with new regional wet deposition measurements, improving the ensemble results of 11 global chemistry transport models from HTAP II. Our study demonstrates that a global measurement–model fusion approach can substantially improve N and S deposition model estimates at a regional scale and represents a step forward toward the WMO goal of global fusion products for accurately mapping harmful air pollution.
Chenxi Li, Yuyang Li, Xiaoxiao Li, Runlong Cai, Yaxin Fan, Xiaohui Qiao, Rujing Yin, Chao Yan, Yishuo Guo, Yongchun Liu, Jun Zheng, Veli-Matti Kerminen, Markku Kulmala, Huayun Xiao, and Jingkun Jiang
Atmos. Chem. Phys., 23, 6879–6896, https://doi.org/10.5194/acp-23-6879-2023, https://doi.org/10.5194/acp-23-6879-2023, 2023
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New particle formation and growth in polluted environments are not fully understood despite intensive research. We applied a cluster dynamics–multicomponent sectional model to simulate the new particle formation events observed in Beijing, China. The simulation approximately captures how the events evolve. Further diagnosis shows that the oxygenated organic molecules may have been under-detected, and modulating their abundance leads to significantly improved simulation–observation agreement.
Marianne Tronstad Lund, Gunnar Myhre, Ragnhild Bieltvedt Skeie, Bjørn Hallvard Samset, and Zbigniew Klimont
Atmos. Chem. Phys., 23, 6647–6662, https://doi.org/10.5194/acp-23-6647-2023, https://doi.org/10.5194/acp-23-6647-2023, 2023
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Here we show that differences, in magnitude and trend, between recent global anthropogenic emission inventories have a notable influence on simulated regional abundances of anthropogenic aerosol over the 1990–2019 period. This, in turn, affects estimates of radiative forcing. Our findings form a basis for comparing existing and upcoming studies on anthropogenic aerosols using different emission inventories.
Lei Kong, Xiao Tang, Jiang Zhu, Zifa Wang, Yele Sun, Pingqing Fu, Meng Gao, Huangjian Wu, Miaomiao Lu, Qian Wu, Shuyuan Huang, Wenxuan Sui, Jie Li, Xiaole Pan, Lin Wu, Hajime Akimoto, and Gregory R. Carmichael
Atmos. Chem. Phys., 23, 6217–6240, https://doi.org/10.5194/acp-23-6217-2023, https://doi.org/10.5194/acp-23-6217-2023, 2023
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A multi-air-pollutant inversion system has been developed in this study to estimate emission changes in China during COVID-19 lockdown. The results demonstrate that the lockdown is largely a nationwide road traffic control measure with NOx emissions decreasing by ~40 %. Emissions of other species only decreased by ~10 % due to smaller effects of lockdown on other sectors. Assessment results further indicate that the lockdown only had limited effects on the control of PM2.5 and O3 in China.
Ernesto Reyes-Villegas, Douglas Lowe, Jill S. Johnson, Kenneth S. Carslaw, Eoghan Darbyshire, Michael Flynn, James D. Allan, Hugh Coe, Ying Chen, Oliver Wild, Scott Archer-Nicholls, Alex Archibald, Siddhartha Singh, Manish Shrivastava, Rahul A. Zaveri, Vikas Singh, Gufran Beig, Ranjeet Sokhi, and Gordon McFiggans
Atmos. Chem. Phys., 23, 5763–5782, https://doi.org/10.5194/acp-23-5763-2023, https://doi.org/10.5194/acp-23-5763-2023, 2023
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Organic aerosols (OAs), their sources and their processes remain poorly understood. The volatility basis set (VBS) approach, implemented in air quality models such as WRF-Chem, can be a useful tool to describe primary OA (POA) production and aging. However, the main disadvantage is its complexity. We used a Gaussian process simulator to reproduce model results and to estimate the sources of model uncertainty. We do this by comparing the outputs with OA observations made at Delhi, India, in 2018.
Eleftherios Ioannidis, Kathy S. Law, Jean-Christophe Raut, Louis Marelle, Tatsuo Onishi, Rachel M. Kirpes, Lucia M. Upchurch, Thomas Tuch, Alfred Wiedensohler, Andreas Massling, Henrik Skov, Patricia K. Quinn, and Kerri A. Pratt
Atmos. Chem. Phys., 23, 5641–5678, https://doi.org/10.5194/acp-23-5641-2023, https://doi.org/10.5194/acp-23-5641-2023, 2023
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Remote and local anthropogenic emissions contribute to wintertime Arctic haze, with enhanced aerosol concentrations, but natural sources, which also contribute, are less well studied. Here, modelled wintertime sea-spray aerosols are improved in WRF-Chem over the wider Arctic by including updated wind speed and temperature-dependent treatments. As a result, anthropogenic nitrate aerosols are also improved. Open leads are confirmed to be the main source of sea-spray aerosols over northern Alaska.
Wenfu Tang, Simone Tilmes, David M. Lawrence, Fang Li, Cenlin He, Louisa K. Emmons, Rebecca R. Buchholz, and Lili Xia
Atmos. Chem. Phys., 23, 5467–5486, https://doi.org/10.5194/acp-23-5467-2023, https://doi.org/10.5194/acp-23-5467-2023, 2023
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Globally, total wildfire burned area is projected to increase over the 21st century under scenarios without geoengineering and decrease under the two geoengineering scenarios. Geoengineering reduces fire by decreasing surface temperature and wind speed and increasing relative humidity and soil water. However, geoengineering also yields reductions in precipitation, which offset some of the fire reduction.
Havala O. T. Pye, Bryan K. Place, Benjamin N. Murphy, Karl M. Seltzer, Emma L. D'Ambro, Christine Allen, Ivan R. Piletic, Sara Farrell, Rebecca H. Schwantes, Matthew M. Coggon, Emily Saunders, Lu Xu, Golam Sarwar, William T. Hutzell, Kristen M. Foley, George Pouliot, Jesse Bash, and William R. Stockwell
Atmos. Chem. Phys., 23, 5043–5099, https://doi.org/10.5194/acp-23-5043-2023, https://doi.org/10.5194/acp-23-5043-2023, 2023
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Chemical mechanisms describe how emissions from vehicles, vegetation, and other sources are chemically transformed in the atmosphere to secondary products including criteria and hazardous air pollutants. The Community Regional Atmospheric Chemistry Multiphase Mechanism integrates gas-phase radical chemistry with pathways to fine-particle mass. New species were implemented, resulting in a bottom-up representation of organic aerosol, which is required for accurate source attribution of pollutants.
Xuemei Wang, Hamish Gordon, Daniel P. Grosvenor, Meinrat O. Andreae, and Ken S. Carslaw
Atmos. Chem. Phys., 23, 4431–4461, https://doi.org/10.5194/acp-23-4431-2023, https://doi.org/10.5194/acp-23-4431-2023, 2023
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New particle formation in the upper troposphere is important for the global boundary layer aerosol population, and they can be transported downward in Amazonia. We use a global and a regional model to quantify the number of aerosols that are formed at high altitude and transported downward in a 1000 km region. We find that the majority of the aerosols are from outside the region. This suggests that the 1000 km region is unlikely to be a
closed loopfor aerosol formation, transport and growth.
Shixian Zhai, Daniel J. Jacob, Drew C. Pendergrass, Nadia K. Colombi, Viral Shah, Laura Hyesung Yang, Qiang Zhang, Shuxiao Wang, Hwajin Kim, Yele Sun, Jin-Soo Choi, Jin-Soo Park, Gan Luo, Fangqun Yu, Jung-Hun Woo, Younha Kim, Jack E. Dibb, Taehyoung Lee, Jin-Seok Han, Bruce E. Anderson, Ke Li, and Hong Liao
Atmos. Chem. Phys., 23, 4271–4281, https://doi.org/10.5194/acp-23-4271-2023, https://doi.org/10.5194/acp-23-4271-2023, 2023
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Anthropogenic fugitive dust in East Asia not only causes severe coarse particulate matter air pollution problems, but also affects fine particulate nitrate. Due to emission control efforts, coarse PM decreased steadily. We find that the decrease of coarse PM is a major driver for a lack of decrease of fine particulate nitrate, as it allows more nitric acid to form fine particulate nitrate. The continuing decrease of coarse PM requires more stringent ammonia and nitrogen oxides emission controls.
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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Research on the sources of Chinese PM2.5 pollution has focused on the contributions of China’s domestic emissions. However, the impact of foreign anthropogenic emissions has typically been simplified or neglected. Here we find that foreign anthropogenic emissions play an important role in Chinese PM2.5 pollution through chemical interactions between foreign-transported pollutants and China’s local emissions. Thus, foreign emission reductions are essential for improving Chinese air quality.
Kun Wang, Xiaoyan Ma, Rong Tian, and Fangqun Yu
Atmos. Chem. Phys., 23, 4091–4104, https://doi.org/10.5194/acp-23-4091-2023, https://doi.org/10.5194/acp-23-4091-2023, 2023
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From 12 March to 6 April 2016 in Beijing, there were 11 typical new particle formation days, 13 non-event days, and 2 undefined days. We first analyzed the favorable background of new particle formation in Beijing and then conducted the simulations using four nucleation schemes based on a global chemistry transport model (GEOS-Chem) to understand the nucleation mechanism.
Arineh Cholakian, Matthias Beekmann, Guillaume Siour, Isabelle Coll, Manuela Cirtog, Elena Ormeño, Pierre-Marie Flaud, Emilie Perraudin, and Eric Villenave
Atmos. Chem. Phys., 23, 3679–3706, https://doi.org/10.5194/acp-23-3679-2023, https://doi.org/10.5194/acp-23-3679-2023, 2023
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This article revolves around the simulation of biogenic secondary organic aerosols in the Landes forest (southwestern France). Several sensitivity cases involving biogenic emission factors, land cover data, anthropogenic emissions, and physical or meteorological parameters were performed and each compared to measurements both in the forest canopy and around the forest. The chemistry behind the formation of these aerosols and their production and transport in the forest canopy is discussed.
Cited articles
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Short summary
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.
Sulfate is a key species contributing to particle formation and growth during wintertime Chinese...
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