Articles | Volume 20, issue 3
Atmos. Chem. Phys., 20, 1483–1495, 2020
https://doi.org/10.5194/acp-20-1483-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Atmos. Chem. Phys., 20, 1483–1495, 2020
https://doi.org/10.5194/acp-20-1483-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article 07 Feb 2020
Research article | 07 Feb 2020
Effect of changing NOx lifetime on the seasonality and long-term trends of satellite-observed tropospheric NO2 columns over China
Viral Shah et al.
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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.
Jingyuan Shao, Qianjie Chen, Yuxuan Wang, Xiao Lu, Pengzhen He, Yele Sun, Viral Shah, Randall V. Martin, Sajeev Philip, Shaojie Song, Yue Zhao, Zhouqing Xie, Lin Zhang, and Becky Alexander
Atmos. Chem. Phys., 19, 6107–6123, https://doi.org/10.5194/acp-19-6107-2019, https://doi.org/10.5194/acp-19-6107-2019, 2019
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Sulfate is a key species contributing to particle formation and growth during wintertime Chinese haze events. This study combines observations and modeling of oxygen isotope signatures in sulfate aerosol to investigate its formation mechanisms, with a focus on heterogeneous production on aerosol surface via H2O2, O3, and NO2 and trace metal catalyzed oxidation. Contributions from different formation pathways are presented.
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.
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 %.
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.
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.
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 %.
Haipeng Lin, Daniel J. Jacob, Elizabeth W. Lundgren, Melissa P. Sulprizio, Christoph A. Keller, Thibaud M. Fritz, Sebastian D. Eastham, Louisa K. Emmons, Patrick C. Campbell, Barry Baker, Rick D. Saylor, and Raffaele Montuoro
Geosci. Model Dev., 14, 5487–5506, https://doi.org/10.5194/gmd-14-5487-2021, https://doi.org/10.5194/gmd-14-5487-2021, 2021
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Emissions are a central component of atmospheric chemistry models. The Harmonized Emissions Component (HEMCO) is a software component for computing emissions from a user-selected ensemble of emission inventories and algorithms. It allows users to select, add, and scale emissions from different sources through a configuration file with no change to the model source code. We demonstrate the implementation of HEMCO in several models, all sharing the same HEMCO core code and database library.
Yi Yin, Frederic Chevallier, Philippe Ciais, Philippe Bousquet, Marielle Saunois, Bo Zheng, John Worden, A. Anthony Bloom, Robert J. Parker, Daniel J. Jacob, Edward J. Dlugokencky, and Christian Frankenberg
Atmos. Chem. Phys., 21, 12631–12647, https://doi.org/10.5194/acp-21-12631-2021, https://doi.org/10.5194/acp-21-12631-2021, 2021
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The growth of methane, the second-most important anthropogenic greenhouse gas after carbon dioxide, has been accelerating in recent years. Using an ensemble of multi-tracer atmospheric inversions constrained by surface or satellite observations, we show that global methane emissions increased by nearly 1 % per year from 2010–2017, with leading contributions from the tropics and East Asia.
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, and Claudia A. Octaviano Villasana
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-671, https://doi.org/10.5194/acp-2021-671, 2021
Preprint under review for ACP
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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 peaks in 2014, in contrast to the report of steady decreasing trend over 2010–2017 from US EPA.
Hannah Nesser, Daniel J. Jacob, Joannes D. Maasakkers, Tia R. Scarpelli, Melissa P. Sulprizio, Yuzhong Zhang, and Chris H. Rycroft
Atmos. Meas. Tech., 14, 5521–5534, https://doi.org/10.5194/amt-14-5521-2021, https://doi.org/10.5194/amt-14-5521-2021, 2021
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Analytical inversions of satellite observations of atmospheric composition can improve emissions estimates and quantify errors but are computationally expensive at high resolutions. We propose two methods to decrease this cost. The methods reproduce a high-resolution inversion at a quarter of the cost. The reduced-dimension method creates a multiscale grid. The reduced-rank method solves the inversion where information content is highest.
Gongda Lu, Eloise A. Marais, Tuan V. Vu, Jingsha Xu, Zongbo Shi, James D. Lee, Qiang Zhang, Lu Shen, Gan Luo, and Fangqun Yu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-428, https://doi.org/10.5194/acp-2021-428, 2021
Preprint under review for ACP
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Emission controls were imposed in Beijing-Tianjin-Hebei in northern China in autumn-winter 2017. We find that regional PM2.5 targets (15 % decrease relative to previous year) were exceeded. Our analysis shows that decline in precursor emissions only leads to less than half (43 %) the improved air quality. Most of the change (57 %) is due to interannual variability in meteorology. Stricter emission controls may be necessary in years with unfavourable meteorology.
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.
Benjamin A. Nault, Duseong S. Jo, Brian C. McDonald, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Jason C. Schroder, James Allan, Donald R. Blake, Manjula R. Canagaratna, Hugh Coe, Matthew M. Coggon, Peter F. DeCarlo, Glenn S. Diskin, Rachel Dunmore, Frank Flocke, Alan Fried, Jessica B. Gilman, Georgios Gkatzelis, Jacqui F. Hamilton, Thomas F. Hanisco, Patrick L. Hayes, Daven K. Henze, Alma Hodzic, James Hopkins, Min Hu, L. Greggory Huey, B. Thomas Jobson, William C. Kuster, Alastair Lewis, Meng Li, Jin Liao, M. Omar Nawaz, Ilana B. Pollack, Jeffrey Peischl, Bernhard Rappenglück, Claire E. Reeves, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Min Shao, Jacob M. Sommers, James Walega, Carsten Warneke, Petter Weibring, Glenn M. Wolfe, Dominique E. Young, Bin Yuan, Qiang Zhang, Joost A. de Gouw, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 11201–11224, https://doi.org/10.5194/acp-21-11201-2021, https://doi.org/10.5194/acp-21-11201-2021, 2021
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Secondary organic aerosol (SOA) is an important aspect of poor air quality for urban regions around the world, where a large fraction of the population lives. However, there is still large uncertainty in predicting SOA in urban regions. Here, we used data from 11 urban campaigns and show that the variability in SOA production in these regions is predictable and is explained by key emissions. These results are used to estimate the premature mortality associated with SOA in urban regions.
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. Discuss., https://doi.org/10.5194/acp-2021-413, https://doi.org/10.5194/acp-2021-413, 2021
Revised manuscript under review for ACP
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Geostationary satellite aerosol optical depth (AOD) has tremendous potential for monitoring surface fine particulate matter (PM2.5). We integrated data from surface networks, aircraft, and satellites with the GEOS-Chem atmospheric chemistry model to enhance our ability to relate AOD to PM2.5. We attributed 550 nm AOD mainly to secondary aerosols in the planetary boundary layer (PBL) and explained the opposite seasonality between AOD and PM2.5 by seasonality in PBL heights and relative humidity.
Yuan Cheng, Qin-qin Yu, Jiu-meng Liu, Xu-bing Cao, Ying-jie Zhong, Zhen-yu Du, Lin-lin Liang, Guan-nan Geng, Wan-li Ma, Hong Qi, Qiang Zhang, and Ke-bin He
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-522, https://doi.org/10.5194/acp-2021-522, 2021
Revised manuscript accepted for ACP
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Open burning policies in Heilongjiang Province experienced a rapid transition during 2018 to 2020. This study evaluated the responses of PM2.5 pollution to this transition, and suggested neither of the policies could be considered successful. In addition, heterogeneous reactions were found to be at play in secondary aerosol formation, even in the frigid atmosphere in Heilongjiang. The unique haze in Northeast China deserves more attention.
Kelvin Bates, Daniel Jacob, Ke Li, Peter Ivatt, Mat Evans, Yingying Yan, and Jintai Lin
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-605, https://doi.org/10.5194/acp-2021-605, 2021
Preprint under review for ACP
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Simple aromatic compounds (benzene, toluene, xylene) have complex gas-phase chemistry that is inconsistently represented in atmospheric models. We compile recent experimental and theoretical insights to develop a new mechanism for gas-phase aromatic oxidation that is sufficiently compact for use in multiscale models. We compare our new mechanism to chamber experiments and other mechanisms, and implement it in a global model to quantify the impacts of aromatic oxidation on tropospheric chemistry.
Xu Feng, Haipeng Lin, Tzung-May Fu, Melissa P. Sulprizio, Jiawei Zhuang, Daniel J. Jacob, Heng Tian, Yaping Ma, Lijuan Zhang, Xiaolin Wang, Qi Chen, and Zhiwei Han
Geosci. Model Dev., 14, 3741–3768, https://doi.org/10.5194/gmd-14-3741-2021, https://doi.org/10.5194/gmd-14-3741-2021, 2021
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WRF-GC is an online coupling of the WRF meteorological model and GEOS-Chem chemical transport model for regional atmospheric chemistry and air quality modeling. In WRF-GC v2.0, we implemented the aerosol–radiation interactions and aerosol–cloud interactions, as well as the capability to nest multiple domains for high-resolution simulations based on the modular framework of WRF-GC v1.0. This allows the GEOS-Chem users to investigate the meteorology–atmospheric chemistry interactions.
Qingyang Xiao, Yixuan Zheng, Guannan Geng, Cuihong Chen, Xiaomeng Huang, Huizheng Che, Xiaoye Zhang, Kebin He, and Qiang Zhang
Atmos. Chem. Phys., 21, 9475–9496, https://doi.org/10.5194/acp-21-9475-2021, https://doi.org/10.5194/acp-21-9475-2021, 2021
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We used both statistical methods and a chemical transport model to assess the contribution of meteorology and emissions to PM2.5 during 2000–2018. Both methods revealed that emissions dominated the long-term PM2.5 trend with notable meteorological effects ranged up to 37.9 % of regional annual average PM2.5. The meteorological contribution became more beneficial to PM2.5 control in southern China but more unfavorable in northern China during the studied period.
Yulu Qiu, Zhiqiang Ma, Ke Li, Mengyu Huang, Jiujiang Sheng, Ping Tian, Jia Zhu, Weiwei Pu, Yingxiao Tang, Tingting Han, Huaigang Zhou, and Hong Liao
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-359, https://doi.org/10.5194/acp-2021-359, 2021
Revised manuscript under review for ACP
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Photochemical pollution over the North China Plain (NCP) are attracting much concern. Our observations at a rural site in the NCP identified high peroxyacetyl nitrate (PAN) concentrations even during cold days. Increased acetaldehyde concentration and hydroxyl radical production rate drive fast PAN formation. Moreover, our study emphasizes the importance of formaldehyde photolysis in PAN formation, and calls for implementing strict volatile organic compound controls out of summer over the NCP.
Bo Zheng, Qiang Zhang, Guannan Geng, Cuihong Chen, Qinren Shi, Mengshi Cui, Yu Lei, and Kebin He
Earth Syst. Sci. Data, 13, 2895–2907, https://doi.org/10.5194/essd-13-2895-2021, https://doi.org/10.5194/essd-13-2895-2021, 2021
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Here we report the monthly anthropogenic pollutant emissions in China during the COVID-19 pandemic by using a bottom-up approach based on near-real-time data. The COVID lockdowns were estimated to have reduced China's emissions substantially between January and March in 2020, with the largest reduction in February. With the spread of coronavirus controlled, China's anthropogenic emissions rebounded in April and since then returned to levels comparable to those of 2019 through December 2020.
Yuqiang Zhang, Drew Shindell, Karl Seltzer, Lu Shen, Jean-Francois Lamarque, Qiang Zhang, Bo Zheng, Jia Xing, Zhe Jiang, and Lei Zhang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-385, https://doi.org/10.5194/acp-2021-385, 2021
Revised manuscript under review for ACP
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In this study, we use global chemical transport model to simulate the effects on global air quality and human health due to emission changes in China from 2010 to 2017. By performing sensitivity analysis, we found that the air pollution control policies not only decrease the air pollutants concentration, but also bring significant co-benefits on air quality in downwind regions. The benefits for the improved air pollution are dominated by PM2.5.
David R. Lyon, Benjamin Hmiel, Ritesh Gautam, Mark Omara, Katherine A. Roberts, Zachary R. Barkley, Kenneth J. Davis, Natasha L. Miles, Vanessa C. Monteiro, Scott J. Richardson, Stephen Conley, Mackenzie L. Smith, Daniel J. Jacob, Lu Shen, Daniel J. Varon, Aijun Deng, Xander Rudelis, Nikhil Sharma, Kyle T. Story, Adam R. Brandt, Mary Kang, Eric A. Kort, Anthony J. Marchese, and Steven P. Hamburg
Atmos. Chem. Phys., 21, 6605–6626, https://doi.org/10.5194/acp-21-6605-2021, https://doi.org/10.5194/acp-21-6605-2021, 2021
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The Permian Basin (USA) is the world’s largest oil field. We use tower- and aircraft-based approaches to measure how methane emissions in the Permian Basin changed throughout 2020. In early 2020, 3.3 % of the region’s gas was emitted; then in spring 2020, the loss rate temporarily dropped to 1.9 % as oil price crashed. We find this short-term reduction to be a result of reduced well development, less gas flaring, and fewer abnormal events despite minimal reductions in oil and gas production.
Daniel J. Varon, Dylan Jervis, Jason McKeever, Ian Spence, David Gains, and Daniel J. Jacob
Atmos. Meas. Tech., 14, 2771–2785, https://doi.org/10.5194/amt-14-2771-2021, https://doi.org/10.5194/amt-14-2771-2021, 2021
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Satellites can detect methane emissions by measuring sunlight reflected from the Earth's surface and atmosphere. Here we show that the European Space Agency's Sentinel-2 twin satellites can be used to monitor anomalously large methane point sources around the world, with global coverage every 2–5 days and 20 m spatial resolution. We demonstrate this previously unreported capability through high-frequency Sentinel-2 monitoring of two strong methane point sources in Algeria and Turkmenistan.
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.
Yingying Yan, Yue Zhou, Shaofei Kong, Jintai Lin, Jian Wu, Huang Zheng, Zexuan Zhang, Aili Song, Yongqing Bai, Zhang Ling, Dantong Liu, and Tianliang Zhao
Atmos. Chem. Phys., 21, 3143–3162, https://doi.org/10.5194/acp-21-3143-2021, https://doi.org/10.5194/acp-21-3143-2021, 2021
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We analyze the effectiveness of emission reduction for local and upwind regions during winter haze episodes controlled by the main potential synoptic patterns over central China, a regional pollutant transport hub with sub-basin topography. Our results provide an opportunity to effectively mitigate haze pollution via local emission control actions in coordination with regional collaborative actions according to different synoptic patterns.
Lu Shen, Daniel J. Jacob, Mauricio Santillana, Kelvin Bates, Jiawei Zhuang, and Wei Chen
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2020-425, https://doi.org/10.5194/gmd-2020-425, 2021
Revised manuscript under review for GMD
Jun Liu, Dan Tong, Yixuan Zheng, Jing Cheng, Xinying Qin, Qinren Shi, Liu Yan, Yu Lei, and Qiang Zhang
Atmos. Chem. Phys., 21, 1627–1647, https://doi.org/10.5194/acp-21-1627-2021, https://doi.org/10.5194/acp-21-1627-2021, 2021
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In this study, we investigated the decadal changes in carbon dioxide and air pollutant emissions in China's cement industry for the period 1990–2015 based on intensive unit-based information. We found that from 1990 to 2015, accompanied by a 10.3-fold increase in cement production, CO2, SO2, and NOx emissions from China's cement industry increased by 627 %, 56 %, and 659 %, whereas CO, PM2.5, and PM10 emissions decreased by 9 %, 63 %, and 59 %, respectively.
Susan S. Kulawik, John R. Worden, Vivienne H. Payne, Dejian Fu, Steven C. Wofsy, Kathryn McKain, Colm Sweeney, Bruce C. Daube Jr., Alan Lipton, Igor Polonsky, Yuguang He, Karen E. Cady-Pereira, Edward J. Dlugokencky, Daniel J. Jacob, and Yi Yin
Atmos. Meas. Tech., 14, 335–354, https://doi.org/10.5194/amt-14-335-2021, https://doi.org/10.5194/amt-14-335-2021, 2021
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This paper shows comparisons of a new single-footprint methane product from the AIRS satellite to aircraft-based observations. We show that this AIRS methane product provides useful information to study seasonal and global methane trends of this important greenhouse gas.
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.
Sabour Baray, Daniel J. Jacob, Joannes D. Massakkers, Jian-Xiong Sheng, Melissa P. Sulprizio, Dylan B. A. Jones, A. Anthony Bloom, and Robert McLaren
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1195, https://doi.org/10.5194/acp-2020-1195, 2021
Revised manuscript under review for ACP
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We use 2010–2015 surface and satellite observations to disentangle methane from anthropogenic and natural sources in Canada. Using a chemical transport model (GEOS-Chem), the mismatch between modelled and observed methane concentrations can be used to infer emissions according to Bayesian statistics. Compared to prior knowledge, we show higher anthropogenic emissions attributed to energy and/or agriculture in Western Canada, and lower natural emissions from Boreal wetlands.
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, Steven Pawson, and Daniel J. Jacob
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2020-398, https://doi.org/10.5194/gmd-2020-398, 2020
Revised manuscript accepted for GMD
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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, so 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.
Yarong Peng, Hongli Wang, Qian Wang, Shengao Jing, Jingyu An, Yaqin Gao, Cheng Huang, Rusha Yan, Haixia Dai, Tiantao Cheng, Qiang Zhang, Meng Li, Li Li, Shengrong Lou, Shikang Tao, Qinyao Hu, Jun Lu, and Changhong Chen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1108, https://doi.org/10.5194/acp-2020-1108, 2020
Revised manuscript not accepted
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The evolution of NMHCs emissions and the effectiveness of control measures were investigated based on long term measurements in a megacity of China. Discrepancies between measurements and emission inventories emphasized the need for emission validation both in speciation and sources. Varied trends of NMHCs speciation and sources suggested the differential effect of the past control measures, which provided new insights into future clean air policies in polluted region including China.
W. Joe F. Acton, Zhonghui Huang, Brian Davison, Will S. Drysdale, Pingqing Fu, Michael Hollaway, Ben Langford, James Lee, Yanhui Liu, Stefan Metzger, Neil Mullinger, Eiko Nemitz, Claire E. Reeves, Freya A. Squires, Adam R. Vaughan, Xinming Wang, Zhaoyi Wang, Oliver Wild, Qiang Zhang, Yanli Zhang, and C. Nicholas Hewitt
Atmos. Chem. Phys., 20, 15101–15125, https://doi.org/10.5194/acp-20-15101-2020, https://doi.org/10.5194/acp-20-15101-2020, 2020
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Air quality in Beijing is of concern to both policy makers and the general public. In order to address concerns about air quality it is vital that the sources of atmospheric pollutants are understood. This work presents the first top-down measurement of volatile organic compound (VOC) emissions in Beijing. These measurements are used to evaluate the emissions inventory and assess the impact of VOC emission from the city centre on atmospheric chemistry.
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.
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.
Wei Tao, Hang Su, Guangjie Zheng, Jiandong Wang, Chao Wei, Lixia Liu, Nan Ma, Meng Li, Qiang Zhang, Ulrich Pöschl, and Yafang Cheng
Atmos. Chem. Phys., 20, 11729–11746, https://doi.org/10.5194/acp-20-11729-2020, https://doi.org/10.5194/acp-20-11729-2020, 2020
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We simulated the thermodynamic and multiphase reactions in aerosol water during a wintertime haze event over the North China Plain. It was found that aerosol pH exhibited a strong spatiotemporal variability, and multiple oxidation pathways were predominant for particulate sulfate formation in different locations. Sensitivity tests further showed that ammonia, crustal particles, and dissolved transition metal ions were important factors for multiphase chemistry during haze episodes.
Pengfei Han, Ning Zeng, Tom Oda, Xiaohui Lin, Monica Crippa, Dabo Guan, Greet Janssens-Maenhout, Xiaolin Ma, Zhu Liu, Yuli Shan, Shu Tao, Haikun Wang, Rong Wang, Lin Wu, Xiao Yun, Qiang Zhang, Fang Zhao, and Bo Zheng
Atmos. Chem. Phys., 20, 11371–11385, https://doi.org/10.5194/acp-20-11371-2020, https://doi.org/10.5194/acp-20-11371-2020, 2020
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An accurate estimation of China’s fossil-fuel CO2 emissions (FFCO2) is significant for quantification of carbon budget and emissions reductions towards the Paris Agreement goals. Here we assessed 9 global and regional inventories. Our findings highlight the significance of using locally measured coal emission factors. We call on the enhancement of physical measurements for validation and provide comprehensive information for inventory, monitoring, modeling, assimilation, and reducing emissions.
Ke Li, Daniel J. Jacob, Lu Shen, Xiao Lu, Isabelle De Smedt, and Hong Liao
Atmos. Chem. Phys., 20, 11423–11433, https://doi.org/10.5194/acp-20-11423-2020, https://doi.org/10.5194/acp-20-11423-2020, 2020
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Surface summer ozone increased in China from 2013 to 2019 despite new governmental efforts targeting ozone pollution. We find that the ozone increase is mostly due to anthropogenic drivers, although meteorology also plays a role. Further analysis for the North China Plain shows that PM2.5 continued to decrease through 2019, while emissions of volatile organic compounds (VOCs) stayed flat. This could explain the anthropogenic increase in ozone, as PM2.5 scavenges the radical precursors of ozone.
Xiao Lu, Lin Zhang, Tongwen Wu, Michael S. Long, Jun Wang, Daniel J. Jacob, Fang Zhang, Jie Zhang, Sebastian D. Eastham, Lu Hu, Lei Zhu, Xiong Liu, and Min Wei
Geosci. Model Dev., 13, 3817–3838, https://doi.org/10.5194/gmd-13-3817-2020, https://doi.org/10.5194/gmd-13-3817-2020, 2020
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This study presents the development and evaluation of a new climate chemistry model, BCC-GEOS-Chem v1.0, which couples the GEOS-Chem chemical transport model as an atmospheric chemistry component in the Beijing Climate Center atmospheric general circulation model. A 3-year (2012–2014) simulation of BCC-GEOS-Chem v1.0 shows that the model captures well the spatiotemporal distributions of tropospheric ozone, other gaseous pollutants, and aerosols.
Amir H. Souri, Caroline R. Nowlan, Gonzalo González Abad, Lei Zhu, Donald R. Blake, Alan Fried, Andrew J. Weinheimer, Armin Wisthaler, Jung-Hun Woo, Qiang Zhang, Christopher E. Chan Miller, Xiong Liu, and Kelly Chance
Atmos. Chem. Phys., 20, 9837–9854, https://doi.org/10.5194/acp-20-9837-2020, https://doi.org/10.5194/acp-20-9837-2020, 2020
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For the first time, we provide a joint nonlinear optimal estimate of NOx and NMVOC emissions during the KORUS-AQ campaign by simultaneously incorporating SAO's new product of HCHO columns from OMPS and OMI tropospheric NO2 columns into a regional model. Results demonstrate a promising improvement in the performance of the model in terms of HCHO and NO2 concentrations, which in turn enables us to quantify the impact of the emission changes on different pathways of ozone formation and loss.
Mengyao Liu, Jintai Lin, Hao Kong, K. Folkert Boersma, Henk Eskes, Yugo Kanaya, Qin He, Xin Tian, Kai Qin, Pinhua Xie, Robert Spurr, Ruijing Ni, Yingying Yan, Hongjian Weng, and Jingxu Wang
Atmos. Meas. Tech., 13, 4247–4259, https://doi.org/10.5194/amt-13-4247-2020, https://doi.org/10.5194/amt-13-4247-2020, 2020
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Nitrogen oxides (NOx = NO + NO2) are important air pollutants in the troposphere and play crucial roles in the formation of ozone and particulate matter. The recently launched TROPOspheric Monitoring Instrument (TROPOMI) provides an opportunity to retrieve tropospheric concentrations of nitrogen dioxide (NO2) at an unprecedented high horizontal resolution. This work presents a new NO2 retrieval product over East Asia and further quantifies key factors affecting the retrieval, including aerosol.
Yang Chen, Jing Cai, Zhichao Wang, Chao Peng, Xiaojiang Yao, Mi Tian, Yiqun Han, Guangming Shi, Zongbo Shi, Yue Liu, Xi Yang, Mei Zheng, Tong Zhu, Kebin He, Qiang Zhang, and Fumo Yang
Atmos. Chem. Phys., 20, 9231–9247, https://doi.org/10.5194/acp-20-9231-2020, https://doi.org/10.5194/acp-20-9231-2020, 2020
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Patterns of particle transport, accumulation, and evolution in both urban and rural areas of Beijing are investigated. The two sites shared 17 common particle types in different stages of atmospheric processing.
Yang Chen, Guangming Shi, Jing Cai, Zongbo Shi, Zhichao Wang, Xiaojiang Yao, Mi Tian, Chao Peng, Yiqun Han, Tong Zhu, Yue Liu, Xi Yang, Mei Zheng, Fumo Yang, Qiang Zhang, and Kebin He
Atmos. Chem. Phys., 20, 9249–9263, https://doi.org/10.5194/acp-20-9249-2020, https://doi.org/10.5194/acp-20-9249-2020, 2020
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Individual particles were observed in two field studies during winter 2016 in the urban and rural areas of Beijing. An online single-particle chemical composition analysis was used as a tracing system to investigate the impact of heating activities and the formation of haze events. During the pollution events, a pattern of transport and accumulation was found with evidence of single particles. The transport from Pinggu to Peking University was significant but PKU to PG occurred occasionally.
Freya A. Squires, Eiko Nemitz, Ben Langford, Oliver Wild, Will S. Drysdale, W. Joe F. Acton, Pingqing Fu, C. Sue B. Grimmond, Jacqueline F. Hamilton, C. Nicholas Hewitt, Michael Hollaway, Simone Kotthaus, James Lee, Stefan Metzger, Natchaya Pingintha-Durden, Marvin Shaw, Adam R. Vaughan, Xinming Wang, Ruili Wu, Qiang Zhang, and Yanli Zhang
Atmos. Chem. Phys., 20, 8737–8761, https://doi.org/10.5194/acp-20-8737-2020, https://doi.org/10.5194/acp-20-8737-2020, 2020
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Significant air quality problems exist in megacities like Beijing, China. To manage air pollution, legislators need a clear understanding of pollutant emissions. However, emissions inventories have large uncertainties, and reliable field measurements of pollutant emissions are required to constrain them. This work presents the first measurements of traffic-dominated emissions in Beijing which suggest that inventories overestimate these emissions in the region during both winter and summer.
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.
Jun Liu, Yixuan Zheng, Guannan Geng, Chaopeng Hong, Meng Li, Xin Li, Fei Liu, Dan Tong, Ruili Wu, Bo Zheng, Kebin He, and Qiang Zhang
Atmos. Chem. Phys., 20, 7783–7799, https://doi.org/10.5194/acp-20-7783-2020, https://doi.org/10.5194/acp-20-7783-2020, 2020
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Ambient PM2.5 pollution contributed substantially to premature mortality in China. The contributions of various sectors to anthropogenic PM2.5-related premature mortality have changed substantially during 1990–2015. In 1990, the residential sector was the leading source, followed by industry, power, agriculture, and transportation, whereas in 2015, the industrial sector became the largest contributor, followed by the residential sector, agriculture, transportation, and power.
Lu Shen, Daniel J. Jacob, Mauricio Santillana, Xuan Wang, and Wei Chen
Geosci. Model Dev., 13, 2475–2486, https://doi.org/10.5194/gmd-13-2475-2020, https://doi.org/10.5194/gmd-13-2475-2020, 2020
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Chemical mechanisms in air quality models tend to get more complicated with time, reflecting both increasing knowledge and the need for greater scope. This objectively improves the models but increases the computational burden. In this work, we present an approach that can reduce the computational cost of chemical integration by 30–40 % while maintaining an accuracy better than 1 %. It retains the complexity of the full mechanism where it is needed and preserves full diagnostic information.
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.
Dan Tong, Jing Cheng, Yang Liu, Sha Yu, Liu Yan, Chaopeng Hong, Yu Qin, Hongyan Zhao, Yixuan Zheng, Guannan Geng, Meng Li, Fei Liu, Yuxuan Zhang, Bo Zheng, Leon Clarke, and Qiang Zhang
Atmos. Chem. Phys., 20, 5729–5757, https://doi.org/10.5194/acp-20-5729-2020, https://doi.org/10.5194/acp-20-5729-2020, 2020
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Future trends in air pollution and greenhouse gas emissions in China are of great concern to the community. Here we developed a sophisticated dynamic projection model to understand 2015–2050 emission pathways under a range of socio-economic, climate policy, and pollution control scenarios. By coupling strong low-carbon transitions and clean air policy, emissions of major air pollutants in China will be reduced by 58–87 % during 2015–2050. This work can support future co-governance policy design.
Haixu Zhang, Chunrong Chen, Weijia Yan, Nana Wu, Yu Bo, Qiang Zhang, and Kebin He
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-280, https://doi.org/10.5194/acp-2020-280, 2020
Revised manuscript not accepted
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In this work, we provide first-hand information on VOC characters in a central Chinese city. Although benzenoids has the largest SOA formation potential, their weight decline with the aggravation of pollution, while the role of VOCs as oxidant producers of SOA formation is critical, especially in hazy periods. Furthermore, solvent evaporation is estimated as the top source for SOA formation considering the above dual roles of VOCs, which would assist to mitigate pollution in China.
Tia R. Scarpelli, Daniel J. Jacob, Joannes D. Maasakkers, Melissa P. Sulprizio, Jian-Xiong Sheng, Kelly Rose, Lucy Romeo, John R. Worden, and Greet Janssens-Maenhout
Earth Syst. Sci. Data, 12, 563–575, https://doi.org/10.5194/essd-12-563-2020, https://doi.org/10.5194/essd-12-563-2020, 2020
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Methane, a potent greenhouse gas, is emitted through the exploitation of oil, gas, and coal resources, and many efforts to reduce emissions have targeted these sources. We have created a global inventory of oil, gas, and coal methane emissions based on country reporting to the United Nations. The inventory can be used along with satellite observations of methane to better understand the contribution of these sources to global emissions and to identify potential biases in emissions reporting.
Qiuyan Du, Chun Zhao, Mingshuai Zhang, Xue Dong, Yu Chen, Zhen Liu, Zhiyuan Hu, Qiang Zhang, Yubin Li, Renmin Yuan, and Shiguang Miao
Atmos. Chem. Phys., 20, 2839–2863, https://doi.org/10.5194/acp-20-2839-2020, https://doi.org/10.5194/acp-20-2839-2020, 2020
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Simulated diurnal PM2.5 with WRF-Chem is primarily controlled by planetary boundary layer (PBL) mixing and emission variations. Modeling bias is likely primarily due to inefficient PBL mixing of primary PM2.5 during the night. The increase in PBL mixing strength during the night can significantly reduce biases. This study underscores that more effort is needed to improve the boundary mixing processes of pollutants in models with observations of PBL structure and mixing fluxes besides PBL height.
Marios Panagi, Zoë L. Fleming, Paul S. Monks, Matthew J. Ashfold, Oliver Wild, Michael Hollaway, Qiang Zhang, Freya A. Squires, and Joshua D. Vande Hey
Atmos. Chem. Phys., 20, 2825–2838, https://doi.org/10.5194/acp-20-2825-2020, https://doi.org/10.5194/acp-20-2825-2020, 2020
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In this paper, using dispersion modelling with emission inventories it was determined that on average 45 % of the total CO pollution that affects Beijing is transported from other areas. About half of the CO comes from beyond the immediate surrounding areas. Finally three classification types of pollution were identified and used to analyse the APHH winter campaign. The results can inform targeted control measures to be implemented in Beijing and the other regions to tackle air quality problems.
Michael Biggart, Jenny Stocker, Ruth M. Doherty, Oliver Wild, Michael Hollaway, David Carruthers, Jie Li, Qiang Zhang, Ruili Wu, Simone Kotthaus, Sue Grimmond, Freya A. Squires, James Lee, and Zongbo Shi
Atmos. Chem. Phys., 20, 2755–2780, https://doi.org/10.5194/acp-20-2755-2020, https://doi.org/10.5194/acp-20-2755-2020, 2020
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Ambient air pollution is a major cause of premature death in China. We examine the street-scale variation of pollutant levels in Beijing using air pollution dispersion and chemistry model ADMS-Urban. Campaign measurements are compared with simulated pollutant levels, providing a valuable means of evaluating the impact of key processes on urban air quality. Air quality modelling at such fine scales is essential for human exposure studies and for informing choices on future emission controls.
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.
Meng Gao, Zhiwei Han, Zhining Tao, Jiawei Li, Jeong-Eon Kang, Kan Huang, Xinyi Dong, Bingliang Zhuang, Shu Li, Baozhu Ge, Qizhong Wu, Hyo-Jung Lee, Cheol-Hee Kim, Joshua S. Fu, Tijian Wang, Mian Chin, Meng Li, Jung-Hun Woo, Qiang Zhang, Yafang Cheng, Zifa Wang, and Gregory R. Carmichael
Atmos. Chem. Phys., 20, 1147–1161, https://doi.org/10.5194/acp-20-1147-2020, https://doi.org/10.5194/acp-20-1147-2020, 2020
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Topic 3 of the Model Inter-Comparison Study for Asia (MICS-Asia) Phase III examines how online coupled air quality models perform in simulating high aerosol pollution in the North China Plain region during wintertime haze events and evaluates the importance of aerosol radiative feedbacks. This paper discusses the estimates of aerosol radiative forcing, aerosol feedbacks, and possible causes for the differences among the models.
Daniel H. Cusworth, Daniel J. Jacob, Daniel J. Varon, Christopher Chan Miller, Xiong Liu, Kelly Chance, Andrew K. Thorpe, Riley M. Duren, Charles E. Miller, David R. Thompson, Christian Frankenberg, Luis Guanter, and Cynthia A. Randles
Atmos. Meas. Tech., 12, 5655–5668, https://doi.org/10.5194/amt-12-5655-2019, https://doi.org/10.5194/amt-12-5655-2019, 2019
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We examine the potential for global detection of methane plumes from individual point sources with the new generation of spaceborne imaging spectrometers scheduled for launch in 2019–2025. We perform methane retrievals on simulated scenes with varying surfaces and atmospheric methane concentrations. Our results suggest that imaging spectrometers in space could play a transformative role in the future for quantifying methane emissions from point sources on a global scale.
Hao Kong, Jintai Lin, Ruixiong Zhang, Mengyao Liu, Hongjian Weng, Ruijing Ni, Lulu Chen, Jingxu Wang, Yingying Yan, and Qiang Zhang
Atmos. Chem. Phys., 19, 12835–12856, https://doi.org/10.5194/acp-19-12835-2019, https://doi.org/10.5194/acp-19-12835-2019, 2019
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We develop a computationally efficient space-based top-down method to inverting NOx emissions in major urban areas at high resolution. The inversion method uses long-term OMI NO2 data to enhance the horizontal resolution, and it accounts for the nonlinear effects of horizontal transport, chemical loss, and deposition on NOx. The inversion results reveal fine-scale spatial information of emissions which is hardly captured by bottom-up inventories.
Haiyan Li, Jing Cheng, Qiang Zhang, Bo Zheng, Yuxuan Zhang, Guangjie Zheng, and Kebin He
Atmos. Chem. Phys., 19, 11485–11499, https://doi.org/10.5194/acp-19-11485-2019, https://doi.org/10.5194/acp-19-11485-2019, 2019
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We combined the online observations of aerosol components and a regional chemical transport model to investigate the response of aerosol chemistry to the stringent clean air actions in Beijing. We found a rapid transition in winter aerosol composition from 2014 to 2017 with decreased sulfate contribution and increased nitrate fraction and evaluated the underlying drivers. The anthropogenic emission reductions in Beijing and its surrounding regions are identified to play a major role.
Tuan V. Vu, Zongbo Shi, Jing Cheng, Qiang Zhang, Kebin He, Shuxiao Wang, and Roy M. Harrison
Atmos. Chem. Phys., 19, 11303–11314, https://doi.org/10.5194/acp-19-11303-2019, https://doi.org/10.5194/acp-19-11303-2019, 2019
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A 5-year Clean Air Action Plan was implemented in 2013 to improve ambient air quality in Beijing. Here, we applied a novel machine-learning-based model to determine the real trend in air quality from 2013 to 2017 in Beijing to assess the efficacy of the plan. We showed that the action plan led to a major reduction in primary emissions and significant improvement in air quality. The marked decrease in PM2.5 and SO2 is largely attributable to a reduction in coal combustion.
Shixian Zhai, Daniel J. Jacob, Xuan Wang, Lu Shen, Ke Li, Yuzhong Zhang, Ke Gui, Tianliang Zhao, and Hong Liao
Atmos. Chem. Phys., 19, 11031–11041, https://doi.org/10.5194/acp-19-11031-2019, https://doi.org/10.5194/acp-19-11031-2019, 2019
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Observed annual mean PM2.5 decreased by 30–50 % in China from 2013–2018. However, meteorologically PM2.5 variability complicates trend attribution. We used a stepwise multiple linear regression model to quantitatively separate contributions from anthropogenic emissions and meteorology. Results show that 88 % of the PM2.5 decrease across China is attributable to anthropogenic emission changes, and 12 % is attributable to meteorology.
Katherine R. Travis and Daniel J. Jacob
Geosci. Model Dev., 12, 3641–3648, https://doi.org/10.5194/gmd-12-3641-2019, https://doi.org/10.5194/gmd-12-3641-2019, 2019
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Models of ozone air pollution are often evaluated with the policy metric set by the EPA of the maximum daily 8 h average ozone concentration. These models may be used in policy settings to evaluate air quality regulations. However, most models have difficulty simulating how ozone varies over the course of the day, and thus the use of this metric in model evaluation is problematic. Improved representation of mixed layer dynamics and ozone loss to the surface is needed to resolve this issue.
Yuxuan Zhang, Meng Li, Yafang Cheng, Guannan Geng, Chaopeng Hong, Haiyan Li, Xin Li, Dan Tong, Nana Wu, Xin Zhang, Bo Zheng, Yixuan Zheng, Yu Bo, Hang Su, and Qiang Zhang
Atmos. Chem. Phys., 19, 9663–9680, https://doi.org/10.5194/acp-19-9663-2019, https://doi.org/10.5194/acp-19-9663-2019, 2019
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In this work, we developed a new approach to simulate BC mixing state based on an emissions inventory and back-trajectory analysis. The model tracks the evolution of BC aging degree during atmospheric transport. Our simulations identified the important roles of extensive emission regions in the BC aging process during atmospheric transport, which provided more clues for improving air pollution and climate change.
Kelvin H. Bates and Daniel J. Jacob
Atmos. Chem. Phys., 19, 9613–9640, https://doi.org/10.5194/acp-19-9613-2019, https://doi.org/10.5194/acp-19-9613-2019, 2019
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Isoprene is a highly reactive chemical released to the atmosphere by plants. Its gas-phase reactions and interactions with chemicals released by human activity have far-reaching atmospheric consequences, contributing to ozone and particulate pollution and prolonging the lifetime of methane, a potent greenhouse gas. We use global simulations with a new isoprene reaction scheme to quantify those effects and to show how recently discovered aspects of isoprene chemistry play out on a global scale.
Rachel F. Silvern, Daniel J. Jacob, Loretta J. Mickley, Melissa P. Sulprizio, Katherine R. Travis, Eloise A. Marais, Ronald C. Cohen, Joshua L. Laughner, Sungyeon Choi, Joanna Joiner, and Lok N. Lamsal
Atmos. Chem. Phys., 19, 8863–8878, https://doi.org/10.5194/acp-19-8863-2019, https://doi.org/10.5194/acp-19-8863-2019, 2019
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The US EPA reports a steady decrease in nitrogen oxide (NOx) emissions from fuel combustion over the 2005–2017 period, while satellite observations show a leveling off after 2009, suggesting emission reductions and related air quality gains have halted. We show the sustained decrease in NOx emissions is in fact consistent with observed trends in surface NO2 and ozone concentrations and that the flattening of the satellite trend reflects a growing influence from the non-anthropogenic background.
Meng Li, Qiang Zhang, Bo Zheng, Dan Tong, Yu Lei, Fei Liu, Chaopeng Hong, Sicong Kang, Liu Yan, Yuxuan Zhang, Yu Bo, Hang Su, Yafang Cheng, and Kebin He
Atmos. Chem. Phys., 19, 8897–8913, https://doi.org/10.5194/acp-19-8897-2019, https://doi.org/10.5194/acp-19-8897-2019, 2019
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A long-term non-methane volatile organic compound (NMVOC) emission inventory is crucial for air quality management but still absent in China. We estimated China’s NMVOCs during 1990–2017 with speciation based on updated databases and investigated the trend of ozone formation potential (OFP) for the same period. Persistent growth of emissions and OFP highlights the need of control measures for solvent use and industrial sources and the importance of designing multi-pollutant control strategies.
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.
Joannes D. Maasakkers, Daniel J. Jacob, Melissa P. Sulprizio, Tia R. Scarpelli, Hannah Nesser, Jian-Xiong Sheng, Yuzhong Zhang, Monica Hersher, A. Anthony Bloom, Kevin W. Bowman, John R. Worden, Greet Janssens-Maenhout, and Robert J. Parker
Atmos. Chem. Phys., 19, 7859–7881, https://doi.org/10.5194/acp-19-7859-2019, https://doi.org/10.5194/acp-19-7859-2019, 2019
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We use 2010–2015 satellite observations of atmospheric methane to improve estimates of methane emissions and their trends, as well as the concentration and trend of tropospheric OH (hydroxyl radical, methane's main sink). We find overestimates of Chinese coal and Middle East oil/gas emissions in the prior estimate. The 2010–2015 growth in methane is attributed to an increase in emissions from India, China, and areas with large tropical wetlands. The contribution from OH is small in comparison.
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.
Yue Liu, Mei Zheng, Mingyuan Yu, Xuhui Cai, Huiyun Du, Jie Li, Tian Zhou, Caiqing Yan, Xuesong Wang, Zongbo Shi, Roy M. Harrison, Qiang Zhang, and Kebin He
Atmos. Chem. Phys., 19, 6595–6609, https://doi.org/10.5194/acp-19-6595-2019, https://doi.org/10.5194/acp-19-6595-2019, 2019
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This study is part of the UK–China APHH campaign. To identify both source types and source regions at the same time, this study developed a combined method including receptor model, footprint model, and air quality model for the first time to investigate sources of PM2.5 during haze episodes in Beijing. It is an expansion of the application of the receptor model and is helpful for formulating effective control strategies to improve air quality in this region.
Lu Shen, Daniel J. Jacob, Xiong Liu, Guanyu Huang, Ke Li, Hong Liao, and Tao Wang
Atmos. Chem. Phys., 19, 6551–6560, https://doi.org/10.5194/acp-19-6551-2019, https://doi.org/10.5194/acp-19-6551-2019, 2019
Lei Zhu, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Xuan Wang, Tomás Sherwen, Mat J. Evans, Qianjie Chen, Becky Alexander, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Michael Le Breton, Thomas J. Bannan, and Carl J. Percival
Atmos. Chem. Phys., 19, 6497–6507, https://doi.org/10.5194/acp-19-6497-2019, https://doi.org/10.5194/acp-19-6497-2019, 2019
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We quantify the effect of sea salt aerosol on tropospheric bromine chemistry with a new mechanistic description of the halogen chemistry in a global atmospheric chemistry model. For the first time, we are able to reproduce the observed levels of bromide activation from the sea salt aerosol in a manner consistent with bromine oxide radical measured from various platforms. Sea salt aerosol plays a far more complex role in global tropospheric chemistry than previously recognized.
Jing Cheng, Jingping Su, Tong Cui, Xiang Li, Xin Dong, Feng Sun, Yanyan Yang, Dan Tong, Yixuan Zheng, Yanshun Li, Jinxiang Li, Qiang Zhang, and Kebin He
Atmos. Chem. Phys., 19, 6125–6146, https://doi.org/10.5194/acp-19-6125-2019, https://doi.org/10.5194/acp-19-6125-2019, 2019
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We attribute Beijing’s PM2.5 abatement in 2017 (compared to 2013) to the following factors: meteorology changes (3.8 μg m−3, 12.1 % of total), regional emission reduction (7.1 μg m−3, 22.5 %), and seven specific categories of control measures in Beijing (20.6 μg m−3, 65.4 %). Our study confirms the effectiveness of clean air actions in Beijing and its surrounding regions and reveals a new generation of control measures, and strengthened regional joint protection measures should be implemented.
Jingyuan Shao, Qianjie Chen, Yuxuan Wang, Xiao Lu, Pengzhen He, Yele Sun, Viral Shah, Randall V. Martin, Sajeev Philip, Shaojie Song, Yue Zhao, Zhouqing Xie, Lin Zhang, and Becky Alexander
Atmos. Chem. Phys., 19, 6107–6123, https://doi.org/10.5194/acp-19-6107-2019, https://doi.org/10.5194/acp-19-6107-2019, 2019
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Sulfate is a key species contributing to particle formation and growth during wintertime Chinese haze events. This study combines observations and modeling of oxygen isotope signatures in sulfate aerosol to investigate its formation mechanisms, with a focus on heterogeneous production on aerosol surface via H2O2, O3, and NO2 and trace metal catalyzed oxidation. Contributions from different formation pathways are presented.
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.
Lei Sun, Likun Xue, Yuhang Wang, Longlei Li, Jintai Lin, Ruijing Ni, Yingying Yan, Lulu Chen, Juan Li, Qingzhu Zhang, and Wenxing Wang
Atmos. Chem. Phys., 19, 1455–1469, https://doi.org/10.5194/acp-19-1455-2019, https://doi.org/10.5194/acp-19-1455-2019, 2019
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We quantified the detailed impacts of meteorology and anthropogenic emissions on surface O3 increase in central eastern China between 2003 and 2015 using GEOS-Chem. The emission change plays a more important role than the meteorological change, while the regions with a larger O3 increase are more sensitive to meteorology. NMVOC emission change dominated the O3 increase in eastern CEC, while NOx emission change led to an O3 increase in western and central CEC and O3 decrease in urban areas.
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).
Yingying Yan, David Cabrera-Perez, Jintai Lin, Andrea Pozzer, Lu Hu, Dylan B. Millet, William C. Porter, and Jos Lelieveld
Geosci. Model Dev., 12, 111–130, https://doi.org/10.5194/gmd-12-111-2019, https://doi.org/10.5194/gmd-12-111-2019, 2019
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The GEOS-Chem model has been updated with the SAPRC-11 aromatics chemical mechanism to evaluate global and regional effects of aromatics on tropospheric oxidation capacity. Our results reveal relatively slight changes in ozone, hydroxyl radical, and nitrogen oxides on a global mean basis (1–4 %), although remarkable regional differences (5–20 %) exist near the source regions. Improved representation of aromatics is important to simulate the tropospheric oxidation.
Mengyao Liu, Jintai Lin, K. Folkert Boersma, Gaia Pinardi, Yang Wang, Julien Chimot, Thomas Wagner, Pinhua Xie, Henk Eskes, Michel Van Roozendael, François Hendrick, Pucai Wang, Ting Wang, Yingying Yan, Lulu Chen, and Ruijing Ni
Atmos. Meas. Tech., 12, 1–21, https://doi.org/10.5194/amt-12-1-2019, https://doi.org/10.5194/amt-12-1-2019, 2019
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China has become the world’s largest emitter of NOx, which mainly comes from vehicle exhaust, power plants, etc. However, there are no official ground-based measurements before 2013, so satellites have been widely used to monitor and analyze NOx pollution here. Aerosol is the key factor influencing the accuracy of the satellite NOx product. Our study provides a more accurate way to account for aerosol's influence compared to current widely used products.
Ting Wang, Pucai Wang, Nicolas Theys, Dan Tong, François Hendrick, Qiang Zhang, and Michel Van Roozendael
Atmos. Chem. Phys., 18, 18063–18078, https://doi.org/10.5194/acp-18-18063-2018, https://doi.org/10.5194/acp-18-18063-2018, 2018
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In the last decade, four temporal regimes of SO2 in China have been identified. After an initial rise, SO2 undergoes two sharp drops in 2007–2008 and 2014–2016, during which 5-year rebounding is sustained. Different mechanisms are tied to North and South China. The industrial emission is responsible for SO2 variation in North China, while in South China the meteorological conditions make a large contribution. The result is crucial to the understanding of SO2 changes and future polices.
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.
Jian-Xiong Sheng, Daniel J. Jacob, Joannes D. Maasakkers, Yuzhong Zhang, and Melissa P. Sulprizio
Atmos. Meas. Tech., 11, 6379–6388, https://doi.org/10.5194/amt-11-6379-2018, https://doi.org/10.5194/amt-11-6379-2018, 2018
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We conduct Observing System Simulation Experiments to compare the ability of future satellite measurements of atmospheric methane columns for constraining methane emissions at the 25 km scale. We find that the geostationary instruments can do much better than TROPOMI and are less sensitive to cloud cover. GeoCARB observing twice a day would provide 70 % of the information from the nominal GEO-CAPE mission considered by NASA in response to the Decadal Survey of the US National Research Council.
Daniel H. Cusworth, Daniel J. Jacob, Jian-Xiong Sheng, Joshua Benmergui, Alexander J. Turner, Jeremy Brandman, Laurent White, and Cynthia A. Randles
Atmos. Chem. Phys., 18, 16885–16896, https://doi.org/10.5194/acp-18-16885-2018, https://doi.org/10.5194/acp-18-16885-2018, 2018
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Methane emissions from oil/gas fields originate from a large number of small and densely clustered point sources. We examine the potential of recently launched or planned satellites to locate these high-mode emitters through measurements of atmospheric methane. We find that the recently launched TROPOMI and the planned GeoCARB instruments are successful at locating high-emitting sources for fields of 20-50 emitters within the 50 × 50 km2 geographic domain but are unsuccessful for denser fields.
Jiayue Huang, Lyatt Jaeglé, and Viral Shah
Atmos. Chem. Phys., 18, 16253–16269, https://doi.org/10.5194/acp-18-16253-2018, https://doi.org/10.5194/acp-18-16253-2018, 2018
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The contribution of blowing snow and frost flower as sources of sea salt aerosols (SSA) over polar regions remains uncertain, despite its potentially important role in polar climate and chemistry. Using chemical transport models and satellite observations, we find that blowing snow emissions are the dominant source of SSA over sea ice during the cold season. We infer a monthly snow salinity on first-year sea ice that decreases from fall–spring, minimizing the model discrepancy to within 10 %.
Lu Hu, Christoph A. Keller, Michael S. Long, Tomás Sherwen, Benjamin Auer, Arlindo Da Silva, Jon E. Nielsen, Steven Pawson, Matthew A. Thompson, Atanas L. Trayanov, Katherine R. Travis, Stuart K. Grange, Mat J. Evans, and Daniel J. Jacob
Geosci. Model Dev., 11, 4603–4620, https://doi.org/10.5194/gmd-11-4603-2018, https://doi.org/10.5194/gmd-11-4603-2018, 2018
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We present a full-year online global simulation of tropospheric chemistry at 12.5 km resolution. To the best of our knowledge, such a resolution in a state-of-the-science global simulation of tropospheric chemistry is unprecedented. This simulation will serve as the Nature Run for observing system simulation experiments to support the future geostationary satellite constellation for tropospheric chemistry, and can also be used for various air quality applications.
Yuzhong Zhang, Daniel J. Jacob, Joannes D. Maasakkers, Melissa P. Sulprizio, Jian-Xiong Sheng, Ritesh Gautam, and John Worden
Atmos. Chem. Phys., 18, 15959–15973, https://doi.org/10.5194/acp-18-15959-2018, https://doi.org/10.5194/acp-18-15959-2018, 2018
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We assess the potential of using satellite observations of atmospheric methane to monitor global mean tropospheric OH concentration, a key parameter for the oxidizing power of the atmosphere.
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.
Daniel J. Varon, Daniel J. Jacob, Jason McKeever, Dylan Jervis, Berke O. A. Durak, Yan Xia, and Yi Huang
Atmos. Meas. Tech., 11, 5673–5686, https://doi.org/10.5194/amt-11-5673-2018, https://doi.org/10.5194/amt-11-5673-2018, 2018
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Methane is a powerful greenhouse gas emitted from numerous human activities. Space-based observation of point sources would be a cost-effective monitoring solution, but the resolution of most current and planned methane-observing satellites is too coarse to resolve individual emitters. We simulate fine-resolution (50 m) satellite observations of methane plumes as would be measured by GHGSat (to be launched in 2019) and show that such data can usefully quantify large methane point sources.
Bo Zheng, Dan Tong, Meng Li, Fei Liu, Chaopeng Hong, Guannan Geng, Haiyan Li, Xin Li, Liqun Peng, Ji Qi, Liu Yan, Yuxuan Zhang, Hongyan Zhao, Yixuan Zheng, Kebin He, and Qiang Zhang
Atmos. Chem. Phys., 18, 14095–14111, https://doi.org/10.5194/acp-18-14095-2018, https://doi.org/10.5194/acp-18-14095-2018, 2018
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To tackle the problem of severe air pollution, China has implemented active clean air policies in recent years. We quantified China’s anthropogenic emissions during 2010–2017 and identified the major driving forces of these trends by using a combination of bottom-up emission inventory and index decomposition analysis (IDA) approaches. The major air pollutants have reduced their emissions by 17–62 % during 2010–2017. The IDA results suggest that emission control measures are the main drivers.
Mengyao Liu, Jintai Lin, Yuchen Wang, Yang Sun, Bo Zheng, Jingyuan Shao, Lulu Chen, Yixuan Zheng, Jinxuan Chen, Tzung-May Fu, Yingying Yan, Qiang Zhang, and Zhaohua Wu
Atmos. Chem. Phys., 18, 12933–12952, https://doi.org/10.5194/acp-18-12933-2018, https://doi.org/10.5194/acp-18-12933-2018, 2018
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Eastern China is heavily polluted by NO2, PM2.5, and other air pollutants. Our study uses EOF–EEMD to analyze the spatiotemporal variability of ground-level NO2, PM2.5, and their associations with meteorological processes. Their regular diurnal cycles are mainly affected by human activities, while irregular day-to-day variations are dominated by weather processes representing synchronous variation or north–south opposing changes over Eastern China.
Jian-Xiong Sheng, Daniel J. Jacob, Alexander J. Turner, Joannes D. Maasakkers, Joshua Benmergui, A. Anthony Bloom, Claudia Arndt, Ritesh Gautam, Daniel Zavala-Araiza, Hartmut Boesch, and Robert J. Parker
Atmos. Chem. Phys., 18, 12257–12267, https://doi.org/10.5194/acp-18-12257-2018, https://doi.org/10.5194/acp-18-12257-2018, 2018
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Analysis of 7 years (2010–2016) of GOSAT methane trends over Canada, the contiguous US, and Mexico suggests that US methane emissions increased by 2.5 ± 1.4 % a−1 over the 7-year period, with contributions from both oil–gas systems and livestock in the Midwest. Mexican emissions show a decrease that can be attributed to a decreasing cattle population. Canadian emissions show year-to-year variability driven by wetland emissions and correlated with wetland areal extent.
Ruijing Ni, Jintai Lin, Yingying Yan, and Weili Lin
Atmos. Chem. Phys., 18, 11447–11469, https://doi.org/10.5194/acp-18-11447-2018, https://doi.org/10.5194/acp-18-11447-2018, 2018
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By integrating several modeling methods, we find considerable contributions of foreign anthropogenic emissions to surface ozone over China (2–11 ppb). For anthropogenic ozone over China, the foreign contribution is 40–50 % below 2 km and 85 % in the upper troposphere. For total foreign anthropogenic ozone over China, the portion of transboundary ozone produced within foreign emission source regions is less than 50 %, with the rest produced by precursors transported out of those source regions.
Sebastian D. Eastham, Michael S. Long, Christoph A. Keller, Elizabeth Lundgren, Robert M. Yantosca, Jiawei Zhuang, Chi Li, Colin J. Lee, Matthew Yannetti, Benjamin M. Auer, Thomas L. Clune, Jules Kouatchou, William M. Putman, Matthew A. Thompson, Atanas L. Trayanov, Andrea M. Molod, Randall V. Martin, and Daniel J. Jacob
Geosci. Model Dev., 11, 2941–2953, https://doi.org/10.5194/gmd-11-2941-2018, https://doi.org/10.5194/gmd-11-2941-2018, 2018
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Global atmospheric chemical transport models are crucial tools in atmospheric science, used to address problems ranging from climate change to acid rain. GEOS-Chem High Performance (GCHP) is a new implementation of the widely used GEOS-Chem model, designed for massively parallel architectures. GCHP v11-02c is shown to be highly scalable from 6 to over 500 cores, enabling the routine simulation of global atmospheric chemistry from the surface to the stratopause at resolutions of ~50 km or finer.
Yuxuan Zhang, Xin Li, Meng Li, Yixuan Zheng, Guannan Geng, Chaopeng Hong, Haiyan Li, Dan Tong, Xin Zhang, Yafang Cheng, Hang Su, Kebin He, and Qiang Zhang
Atmos. Chem. Phys., 18, 10275–10287, https://doi.org/10.5194/acp-18-10275-2018, https://doi.org/10.5194/acp-18-10275-2018, 2018
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When emission controls were implemented during APEC, we found that the reduction in BC light absorption was driven by simultaneously reducing the mass concentration and light-absorption capability of BC. The weakening of BC light-absorption capability could be attributed to less coating material on BC surfaces due to the decreased chemical production of secondary aerosols. Our results imply that a synergetic reduction in multiple-pollutant emissions could benefit both air quality and climate.
Yuxuan Zhang, Qiang Zhang, Yafang Cheng, Hang Su, Haiyan Li, Meng Li, Xin Zhang, Aijun Ding, and Kebin He
Atmos. Chem. Phys., 18, 9879–9896, https://doi.org/10.5194/acp-18-9879-2018, https://doi.org/10.5194/acp-18-9879-2018, 2018
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The light absorption of BC-containing particles strongly depends on their aging process in the atmosphere. Whether and how the aging degree and light absorption capability of BC-containing particles will change with air pollution development is still unclear. Our results reveal that under a more polluted environment, the BC-containing particles are characterized not only by higher BC mass concentrations but also by more coating materials on BC surfaces and thus higher light absorption capacity.
Alexander J. Turner, Daniel J. Jacob, Joshua Benmergui, Jeremy Brandman, Laurent White, and Cynthia A. Randles
Atmos. Chem. Phys., 18, 8265–8278, https://doi.org/10.5194/acp-18-8265-2018, https://doi.org/10.5194/acp-18-8265-2018, 2018
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We conduct a 1-week WRF-STILT simulation to generate methane column footprints at 1.3 km spatial resolution and hourly temporal resolution over the Barnett Shale. We find that a week of TROPOMI observations should provide regional (~30 km) information on temporally invariant sources and GeoCARB should provide information on temporally invariant sources at 2–7 km spatial resolution. An instrument precision better than 6 ppb is an important threshold for achieving fine resolution of emissions.
Nan Li, Qingyang He, Jim Greenberg, Alex Guenther, Jingyi Li, Junji Cao, Jun Wang, Hong Liao, Qiyuan Wang, and Qiang Zhang
Atmos. Chem. Phys., 18, 7489–7507, https://doi.org/10.5194/acp-18-7489-2018, https://doi.org/10.5194/acp-18-7489-2018, 2018
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O3 pollution has been increasing in most Chinese cities in recent years. Our study reveals that the synergistic impact of individual source contributions to O3 formation should be considered in the formation of air pollution control strategies, especially for big cities in the vicinity of forests.
Jian-Xiong Sheng, Daniel J. Jacob, Alexander J. Turner, Joannes D. Maasakkers, Melissa P. Sulprizio, A. Anthony Bloom, Arlyn E. Andrews, and Debra Wunch
Atmos. Chem. Phys., 18, 6483–6491, https://doi.org/10.5194/acp-18-6483-2018, https://doi.org/10.5194/acp-18-6483-2018, 2018
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We use observations of boundary layer methane from the SEAC4RS aircraft campaign over the Southeast US to estimate methane emissions in that region. Our results suggest that the EPA inventory is regionally unbiased but there are large local biases, suggesting variable emission factors. Our results also suggest that the choice of landcover map is the dominant source of error for wetland emission estimates.
Shixian Zhai, Xingqin An, Tianliang Zhao, Zhaobin Sun, Wei Wang, Qing Hou, Zengyuan Guo, and Chao Wang
Atmos. Chem. Phys., 18, 6241–6258, https://doi.org/10.5194/acp-18-6241-2018, https://doi.org/10.5194/acp-18-6241-2018, 2018
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The GRAPES–CUACE aerosol adjoint model was developed and applied in detecting PM2.5 sources for haze events in eastern China (EC). The response time of Beijing PM2.5 pollution peaks to local and surrounding emissions is quantized for regional transport of air pollution over the EC. The adjoint results agreed well with the Models-3/CMAQ assessments. The adjoint method is powerful in simulating the receptor–source relationship and can be utilized in dynamic air quality control scheme design.
Jiawei Zhuang, Daniel J. Jacob, and Sebastian D. Eastham
Atmos. Chem. Phys., 18, 6039–6055, https://doi.org/10.5194/acp-18-6039-2018, https://doi.org/10.5194/acp-18-6039-2018, 2018
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Our work explains why current model simulations are unable to capture the intercontinental influences of pollution plumes that are often observed over some regions like California. Due to inadequate vertical grid resolution in these models, the plumes get diffused too rapidly during intercontinental transport. Increasing the vertical grid resolution greatly improves the simulation of plumes and considerably increases the estimate of local surface pollution influence.
Yingying Yan, Andrea Pozzer, Narendra Ojha, Jintai Lin, and Jos Lelieveld
Atmos. Chem. Phys., 18, 5589–5605, https://doi.org/10.5194/acp-18-5589-2018, https://doi.org/10.5194/acp-18-5589-2018, 2018
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Surface-based measurements from the EMEP network and EMAC model simulations are used to estimate the European surface ozone changes over 1995–2014. It shows a significantly decreasing trend in the 95th percentile ozone concentrations, while increasing in the 5th percentile ozone. Sensitivity simulations and statistical analysis show that a decrease in European anthropogenic emissions had contrasting effects on surface ozone trends between the 95th and 5th percentile levels.
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.
Haiyan Li, Qiang Zhang, Bo Zheng, Chunrong Chen, Nana Wu, Hongyu Guo, Yuxuan Zhang, Yixuan Zheng, Xin Li, and Kebin He
Atmos. Chem. Phys., 18, 5293–5306, https://doi.org/10.5194/acp-18-5293-2018, https://doi.org/10.5194/acp-18-5293-2018, 2018
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This study revealed the driving role of nitrate in urban haze development in the North China Plain (NCP) during summertime. Several factors favoring the rapid nitrate formation were investigated in detail. The higher concentration and, in particular, the higher contribution of nitrate in PM1 suggest an urgent need to initiate ammonia emission control measures and further reduce NOx emissions over the NCP region.
Meng Gao, Zhiwei Han, Zirui Liu, Meng Li, Jinyuan Xin, Zhining Tao, Jiawei Li, Jeong-Eon Kang, Kan Huang, Xinyi Dong, Bingliang Zhuang, Shu Li, Baozhu Ge, Qizhong Wu, Yafang Cheng, Yuesi Wang, Hyo-Jung Lee, Cheol-Hee Kim, Joshua S. Fu, Tijian Wang, Mian Chin, Jung-Hun Woo, Qiang Zhang, Zifa Wang, and Gregory R. Carmichael
Atmos. Chem. Phys., 18, 4859–4884, https://doi.org/10.5194/acp-18-4859-2018, https://doi.org/10.5194/acp-18-4859-2018, 2018
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Topic 3 of the Model Inter-Comparison Study for Asia (MICS-Asia) Phase III examines how online coupled air quality models perform in simulating high aerosol pollution in the North China Plain region during wintertime haze events and evaluates the importance of aerosol radiative and microphysical feedbacks. A comprehensive overview of the MICS-ASIA III Topic 3 study design is presented.
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.
Tianyi Fan, Xiaohong Liu, Po-Lun Ma, Qiang Zhang, Zhanqing Li, Yiquan Jiang, Fang Zhang, Chuanfeng Zhao, Xin Yang, Fang Wu, and Yuying Wang
Atmos. Chem. Phys., 18, 1395–1417, https://doi.org/10.5194/acp-18-1395-2018, https://doi.org/10.5194/acp-18-1395-2018, 2018
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We found that 22–28 % of the low AOD bias in eastern China simulated by the Community Atmosphere Model version 5 can be improved by using a new emission inventory. The concentrations of primary aerosols are closely related to the emission, while the seasonal variations of secondary aerosols depend more on atmospheric processes. This study highlights the importance of improving both the emission and atmospheric processes in modeling the atmospheric aerosols and their radiative effects.
Yingying Yan, Jintai Lin, and Cenlin He
Atmos. Chem. Phys., 18, 1185–1202, https://doi.org/10.5194/acp-18-1185-2018, https://doi.org/10.5194/acp-18-1185-2018, 2018
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Examining observed and simulated ozone at about 1000 sites during 1990–2014, we find a clear diurnal cycle both in the magnitude of ozone trends and in the relative importance of climate variability versus anthropogenic emissions to ozone changes, which has policy implications to mitigate ozone at night and other non-peak hours.
Rachel M. Hoesly, Steven J. Smith, Leyang Feng, Zbigniew Klimont, Greet Janssens-Maenhout, Tyler Pitkanen, Jonathan J. Seibert, Linh Vu, Robert J. Andres, Ryan M. Bolt, Tami C. Bond, Laura Dawidowski, Nazar Kholod, June-ichi Kurokawa, Meng Li, Liang Liu, Zifeng Lu, Maria Cecilia P. Moura, Patrick R. O'Rourke, and Qiang Zhang
Geosci. Model Dev., 11, 369–408, https://doi.org/10.5194/gmd-11-369-2018, https://doi.org/10.5194/gmd-11-369-2018, 2018
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Historical emission trends are key inputs to Earth systems and atmospheric chemistry models. We present a new data set of historical (1750–2014) anthropogenic gases (CO, CH4, NH3, NOx, SO2, NMVOCs, BC, OC, and CO2) developed with the Community Emissions Data System (CEDS). This improves on existing inventories as it uses consistent methods and data across emissions species, has annual resolution for a longer and more recent time series, and is designed to be transparent and reproducible.
Karen Yu, Christoph A. Keller, Daniel J. Jacob, Andrea M. Molod, Sebastian D. Eastham, and Michael S. Long
Geosci. Model Dev., 11, 305–319, https://doi.org/10.5194/gmd-11-305-2018, https://doi.org/10.5194/gmd-11-305-2018, 2018
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Global simulations of atmospheric chemistry are generally conducted with off-line chemical transport models (CTMs) driven by archived meteorological data from general circulation models (GCMs). The off-line approach has the advantages of simplicity and expediency, but it is unable to reproduce the GCM transport exactly. We investigate the cascade of errors associated with the off-line approach using the GEOS-5 GCM and GEOS-Chem CTM and discuss improvements in the use of archived meteorology.
Theodore K. Koenig, Rainer Volkamer, Sunil Baidar, Barbara Dix, Siyuan Wang, Daniel C. Anderson, Ross J. Salawitch, Pamela A. Wales, Carlos A. Cuevas, Rafael P. Fernandez, Alfonso Saiz-Lopez, Mathew J. Evans, Tomás Sherwen, Daniel J. Jacob, Johan Schmidt, Douglas Kinnison, Jean-François Lamarque, Eric C. Apel, James C. Bresch, Teresa Campos, Frank M. Flocke, Samuel R. Hall, Shawn B. Honomichl, Rebecca Hornbrook, Jørgen B. Jensen, Richard Lueb, Denise D. Montzka, Laura L. Pan, J. Michael Reeves, Sue M. Schauffler, Kirk Ullmann, Andrew J. Weinheimer, Elliot L. Atlas, Valeria Donets, Maria A. Navarro, Daniel Riemer, Nicola J. Blake, Dexian Chen, L. Gregory Huey, David J. Tanner, Thomas F. Hanisco, and Glenn M. Wolfe
Atmos. Chem. Phys., 17, 15245–15270, https://doi.org/10.5194/acp-17-15245-2017, https://doi.org/10.5194/acp-17-15245-2017, 2017
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Tropospheric inorganic bromine (BrO and Bry) shows a C-shaped profile over the tropical western Pacific Ocean, and supports previous speculation that marine convection is a source for inorganic bromine from sea salt to the upper troposphere. The Bry profile in the tropical tropopause layer (TTL) is complex, suggesting that the total Bry budget in the TTL is not closed without considering aerosol bromide. The implications for atmospheric composition and bromine sources are discussed.
Jianlin Hu, Xun Li, Lin Huang, Qi Ying, Qiang Zhang, Bin Zhao, Shuxiao Wang, and Hongliang Zhang
Atmos. Chem. Phys., 17, 13103–13118, https://doi.org/10.5194/acp-17-13103-2017, https://doi.org/10.5194/acp-17-13103-2017, 2017
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The model performance of CMAQ with WRF using four different emission inventories in China was validated and compared to obtain the best air pollutants prediction for health effect studies of severe air pollution. The differences in performance of chemical transport model were analyzed for different months and regions in the vast part of China and ensemble predictions were firstly obtained from different inventories for health analysis with minimized errors for pollutants including PM2.5 and O3.
Huan Liu, Hanyang Man, Hongyang Cui, Yanjun Wang, Fanyuan Deng, Yue Wang, Xiaofan Yang, Qian Xiao, Qiang Zhang, Yan Ding, and Kebin He
Atmos. Chem. Phys., 17, 12709–12724, https://doi.org/10.5194/acp-17-12709-2017, https://doi.org/10.5194/acp-17-12709-2017, 2017
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The VOC emission inventory has large uncertainties. An updated VOC emission inventory of vehicles in China was developed based on a set of state-of-the-art methods and big data. Exhausts and evaporation were taken into account. Our results narrowed the gap between inventories and the real emissions. Detailed speciation reveals the chemical characteristics of emissions, which has the potential to improve the understanding of atmospheric chemical processes in polluted regions.
Qing Mu, Gerhard Lammel, Christian N. Gencarelli, Ian M. Hedgecock, Ying Chen, Petra Přibylová, Monique Teich, Yuxuan Zhang, Guangjie Zheng, Dominik van Pinxteren, Qiang Zhang, Hartmut Herrmann, Manabu Shiraiwa, Peter Spichtinger, Hang Su, Ulrich Pöschl, and Yafang Cheng
Atmos. Chem. Phys., 17, 12253–12267, https://doi.org/10.5194/acp-17-12253-2017, https://doi.org/10.5194/acp-17-12253-2017, 2017
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Polycyclic aromatic hydrocarbons (PAHs) are hazardous pollutants with the largest emissions in East Asia. The regional WRF-Chem-PAH model has been developed to reflect the state-of-the-art understanding of current PAHs studies with several new or updated features. It is able to reasonably well simulate the concentration levels and particulate mass fractions of PAHs near the sources and at a remote outflow region of East Asia, in high spatial and temporal resolutions.
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.
Jieying Ding, Kazuyuki Miyazaki, Ronald Johannes van der A, Bas Mijling, Jun-ichi Kurokawa, SeogYeon Cho, Greet Janssens-Maenhout, Qiang Zhang, Fei Liu, and Pieternel Felicitas Levelt
Atmos. Chem. Phys., 17, 10125–10141, https://doi.org/10.5194/acp-17-10125-2017, https://doi.org/10.5194/acp-17-10125-2017, 2017
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To evaluate the quality of the satellite-derived NOx emissions, we compare nine emission inventories of nitrogen oxides including four satellite-derived NOx inventories and bottom-up inventories for East Asia. The temporal and spatial distribution of NOx emissions over East Asia are evaluated. We analyse the differences in satellite-derived emissions from two different inversion methods. The paper ends with recommendations for future improvements of emission estimates.
Li Zhang, Qinyi Li, Tao Wang, Ravan Ahmadov, Qiang Zhang, Meng Li, and Mengyao Lv
Atmos. Chem. Phys., 17, 9733–9750, https://doi.org/10.5194/acp-17-9733-2017, https://doi.org/10.5194/acp-17-9733-2017, 2017
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Little is known of the integrated impacts of HONO and ClNO2 on lower-tropospheric ozone so far. In this study, we updated WRF-Chem with the CBMZ_ReNOM module, which considers both the sources and chemistry of HONO and ClNO2. The revised model revealed that the two reactive nitrogen compounds significantly affected the oxidation capacity and ozone formation at the surface and within the lower troposphere over polluted regions and noticeably improved summertime O3 predictions over China.
Fei Liu, Steffen Beirle, Qiang Zhang, Ronald J. van der A, Bo Zheng, Dan Tong, and Kebin He
Atmos. Chem. Phys., 17, 9261–9275, https://doi.org/10.5194/acp-17-9261-2017, https://doi.org/10.5194/acp-17-9261-2017, 2017
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We assess NOx emission trends over Chinese cities based on satellite NO2 observations using a method independent of chemical transport models. NOx emissions over 48 Chinese cities have decreased significantly since 2011. Cities with different dominant emission sources (i.e. power, industrial, and transportation sectors) showed variable emission decline timelines that corresponded to the schedules for emission control in different sectors.
Katherine R. Travis, Daniel J. Jacob, Christoph A. Keller, Shi Kuang, Jintai Lin, Michael J. Newchurch, and Anne M. Thompson
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-596, https://doi.org/10.5194/acp-2017-596, 2017
Preprint retracted
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Models severely overestimate surface ozone in the Southeast US during summertime which has implications for the design of air quality regulations. We use a model (GEOS-Chem) to interpret ozone observations from a suite of observations taken during August–September 2013. The model is unbiased relative to observations below 1 km but is biased high at the surface. We attribute this bias to model representation error, an underestimate in low-cloud, and insufficient treatment of vertical mixing.
Guannan Geng, Qiang Zhang, Dan Tong, Meng Li, Yixuan Zheng, Siwen Wang, and Kebin He
Atmos. Chem. Phys., 17, 9187–9203, https://doi.org/10.5194/acp-17-9187-2017, https://doi.org/10.5194/acp-17-9187-2017, 2017
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We presented the characteristics of PM2.5 chemical composition over China during 2005–2012 by synthesis of in situ measurement data and satellite-based estimates. We also investigated the driving forces behind the changes by examining the changes in precursor emissions. We found that the decrease in sulfate is partly offset by the increase in nitrate. The results indicate that the synchronized abatement of emissions for multipollutants is necessary for reducing ambient PM2.5 over China.
Viral Shah and Lyatt Jaeglé
Atmos. Chem. Phys., 17, 8999–9017, https://doi.org/10.5194/acp-17-8999-2017, https://doi.org/10.5194/acp-17-8999-2017, 2017
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We use a model of mercury chemistry and transport in the atmosphere, along with ground- and aircraft-based mercury observations, to learn that oxidized mercury chemically produced in the free troposphere descends in the subtropical anticyclones and makes up much of the mercury depositing to the Earth's surface. Our findings imply that mercury chemistry in the free troposphere and transport in the subtropics are important links between global emissions and surface deposition of mercury.
Christopher Chan Miller, Daniel J. Jacob, Eloise A. Marais, Karen Yu, Katherine R. Travis, Patrick S. Kim, Jenny A. Fisher, Lei Zhu, Glenn M. Wolfe, Thomas F. Hanisco, Frank N. Keutsch, Jennifer Kaiser, Kyung-Eun Min, Steven S. Brown, Rebecca A. Washenfelder, Gonzalo González Abad, and Kelly Chance
Atmos. Chem. Phys., 17, 8725–8738, https://doi.org/10.5194/acp-17-8725-2017, https://doi.org/10.5194/acp-17-8725-2017, 2017
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The use of satellite glyoxal observations for estimating isoprene emissions has been limited by knowledge of the glyoxal yield from isoprene. We use SENEX aircraft observations over the southeast US to evaluate glyoxal yields from isoprene in a 3-D atmospheric model. The SENEX observations support a pathway for glyoxal formation in pristine regions that we propose here, which may have implications for improving isoprene emissions estimates from upcoming high-resolution geostationary satellites.
Chaopeng Hong, Qiang Zhang, Yang Zhang, Youhua Tang, Daniel Tong, and Kebin He
Geosci. Model Dev., 10, 2447–2470, https://doi.org/10.5194/gmd-10-2447-2017, https://doi.org/10.5194/gmd-10-2447-2017, 2017
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A regional coupled climate–chemistry modeling system using the dynamical downscaling technique was established and evaluated. The modeling system performed well for both the climatological and the short-term air quality applications over east Asia. Regional models outperformed global models in regional climate and air quality predictions. The coupled modeling system improved the model performance, although some biases remained in the aerosol–cloud–radiation variables.
A. Anthony Bloom, Kevin W. Bowman, Meemong Lee, Alexander J. Turner, Ronny Schroeder, John R. Worden, Richard Weidner, Kyle C. McDonald, and Daniel J. Jacob
Geosci. Model Dev., 10, 2141–2156, https://doi.org/10.5194/gmd-10-2141-2017, https://doi.org/10.5194/gmd-10-2141-2017, 2017
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Wetland emissions are a principal source of uncertainty in the global atmospheric methane budget due to poor knowledge of wetland processes. We construct a wetland methane emission and uncertainty dataset for use in global atmospheric methane models. Our wetland model ensemble is based on static wetland maps, satellite-derived inundation and carbon cycle models. The ensemble performs favourably against regional flux estimates and atmospheric methane measurements relative to previous studies.
Eri Saikawa, Hankyul Kim, Min Zhong, Alexander Avramov, Yu Zhao, Greet Janssens-Maenhout, Jun-ichi Kurokawa, Zbigniew Klimont, Fabian Wagner, Vaishali Naik, Larry W. Horowitz, and Qiang Zhang
Atmos. Chem. Phys., 17, 6393–6421, https://doi.org/10.5194/acp-17-6393-2017, https://doi.org/10.5194/acp-17-6393-2017, 2017
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We analyze differences in existing air pollutant emission estimates to better understand the magnitude of emissions as well as the source regions and sectors of air pollution in China. We find large disagreements among the inventories, and we show that these differences have a significant impact on regional air quality simulations. Better understanding of air pollutant emissions at more disaggregated levels is essential for air pollution mitigation in China.
Hannah M. Horowitz, Daniel J. Jacob, Yanxu Zhang, Theodore S. Dibble, Franz Slemr, Helen M. Amos, Johan A. Schmidt, Elizabeth S. Corbitt, Eloïse A. Marais, and Elsie M. Sunderland
Atmos. Chem. Phys., 17, 6353–6371, https://doi.org/10.5194/acp-17-6353-2017, https://doi.org/10.5194/acp-17-6353-2017, 2017
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Mercury is a toxic, global pollutant released to the air from human activities like coal burning. Chemical reactions in air determine how far mercury is transported before it is deposited to the environment, where it may be converted to a form that accumulates in fish. We use a 3-D atmospheric model to evaluate a new set of chemical reactions and its effects on mercury deposition. We find it is consistent with observations and leads to increased deposition to oceans, especially in the tropics.
Rachel F. Silvern, Daniel J. Jacob, Patrick S. Kim, Eloise A. Marais, Jay R. Turner, Pedro Campuzano-Jost, and Jose L. Jimenez
Atmos. Chem. Phys., 17, 5107–5118, https://doi.org/10.5194/acp-17-5107-2017, https://doi.org/10.5194/acp-17-5107-2017, 2017
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We identify a fundamental discrepancy between thermodynamic equilibrium theory and observations of inorganic aerosol composition in the eastern US in summer that shows low ammonium sulfate aerosol ratios. In addition, from 2003 to 2013, while SO2 emissions have declined due to US emission controls, aerosols have become more acidic in the southeastern US. To explain these observations, we suggest that the large and increasing source of organic aerosol may be affecting thermodynamic equilibrium.
Yuxuan Zhang, Hang Su, Simonas Kecorius, Zhibin Wang, Min Hu, Tong Zhu, Kebin He, Alfred Wiedensohler, Qiang Zhang, and Yafang Cheng
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-222, https://doi.org/10.5194/acp-2017-222, 2017
Revised manuscript not accepted
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The light absorption of black carbon (BC) strongly depends on their mixing state. By now, the BC mixing state in the atmosphere is still unclear. In this work, we have investigated the comprehensive characterization of BC mixing state at a polluted regional background site of the North China Plain (NCP) based on in site measurements. we found that BC aerosols of the NCP were fully aged, suggesting a strong optical and climate effect of BC on the regional scale in northern China.
Haiyan Li, Qi Zhang, Qiang Zhang, Chunrong Chen, Litao Wang, Zhe Wei, Shan Zhou, Caroline Parworth, Bo Zheng, Francesco Canonaco, André S. H. Prévôt, Ping Chen, Hongliang Zhang, Timothy J. Wallington, and Kebin He
Atmos. Chem. Phys., 17, 4751–4768, https://doi.org/10.5194/acp-17-4751-2017, https://doi.org/10.5194/acp-17-4751-2017, 2017
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The sources and aerosol evolution processes of severe pollution episodes were investigated in Handan during wintertime using real-time measurements. An in-depth analysis of the data uncovered that primary emissions from coal combustion and biomass burning together with secondary formation of sulfate (mainly from SO2 emitted by coal combustion) are important driving factors for haze evolution. Our findings provide useful insights into air pollution control in heavily polluted regions.
Guannan Geng, Qiang Zhang, Randall V. Martin, Jintai Lin, Hong Huo, Bo Zheng, Siwen Wang, and Kebin He
Atmos. Chem. Phys., 17, 4131–4145, https://doi.org/10.5194/acp-17-4131-2017, https://doi.org/10.5194/acp-17-4131-2017, 2017
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We investigated the impact of spatial proxies on the representation of gridded emissions by comparing six gridded NOx emission datasets over China developed from the same magnitude of emissions and different spatial proxies. GEOS-Chem-modeled NO2 columns from the six gridded emissions are compared with satellite-based columns from OMI. Results show that differences between modeled and satellite-based NO2 columns are sensitive to the spatial proxies used in the gridded emission inventories.
Alba Lorente, K. Folkert Boersma, Huan Yu, Steffen Dörner, Andreas Hilboll, Andreas Richter, Mengyao Liu, Lok N. Lamsal, Michael Barkley, Isabelle De Smedt, Michel Van Roozendael, Yang Wang, Thomas Wagner, Steffen Beirle, Jin-Tai Lin, Nickolay Krotkov, Piet Stammes, Ping Wang, Henk J. Eskes, and Maarten Krol
Atmos. Meas. Tech., 10, 759–782, https://doi.org/10.5194/amt-10-759-2017, https://doi.org/10.5194/amt-10-759-2017, 2017
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Choices and assumptions made to represent the state of the atmosphere introduce an uncertainty of 42 % in the air mass factor calculation in trace gas satellite retrievals in polluted regions. The AMF strongly depends on the choice of a priori trace gas profile, surface albedo data set and the correction method to account for clouds and aerosols. We call for well-designed validation exercises focusing on situations when AMF structural uncertainty has the highest impact on satellite retrievals.
Guohui Li, Naifang Bei, Junji Cao, Rujin Huang, Jiarui Wu, Tian Feng, Yichen Wang, Suixin Liu, Qiang Zhang, Xuexi Tie, and Luisa T. Molina
Atmos. Chem. Phys., 17, 3301–3316, https://doi.org/10.5194/acp-17-3301-2017, https://doi.org/10.5194/acp-17-3301-2017, 2017
Sebastian D. Eastham and Daniel J. Jacob
Atmos. Chem. Phys., 17, 2543–2553, https://doi.org/10.5194/acp-17-2543-2017, https://doi.org/10.5194/acp-17-2543-2017, 2017
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Intercontinental atmospheric transport can disrupt local chemistry and cause air quality issues thousands of kilometers from the source, complicating correct attribution of air quality exceedances. This transport occurs in long, thin plumes which current-generation models consistently fail to reproduce. Our study investigates the cause of this failure, finding that greater vertical resolution than is currently available is required to reliably resolve the plumes and their effects.
Jiarui Wu, Guohui Li, Junji Cao, Naifang Bei, Yichen Wang, Tian Feng, Rujin Huang, Suixin Liu, Qiang Zhang, and Xuexi Tie
Atmos. Chem. Phys., 17, 2035–2051, https://doi.org/10.5194/acp-17-2035-2017, https://doi.org/10.5194/acp-17-2035-2017, 2017
Chaopeng Hong, Qiang Zhang, Kebin He, Dabo Guan, Meng Li, Fei Liu, and Bo Zheng
Atmos. Chem. Phys., 17, 1227–1239, https://doi.org/10.5194/acp-17-1227-2017, https://doi.org/10.5194/acp-17-1227-2017, 2017
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We found that the apparent uncertainties in China’s energy consumption increased from 2004 to 2012. SO2 emissions are most sensitive to energy uncertainties because of the high contributions from industrial coal combustion. The energy-induced emission uncertainties for some species are comparable to total uncertainties of emissions as estimated by previous studies, indicating variations in energy consumption could be an important source of China’s emission uncertainties.
Meng Li, Qiang Zhang, Jun-ichi Kurokawa, Jung-Hun Woo, Kebin He, Zifeng Lu, Toshimasa Ohara, Yu Song, David G. Streets, Gregory R. Carmichael, Yafang Cheng, Chaopeng Hong, Hong Huo, Xujia Jiang, Sicong Kang, Fei Liu, Hang Su, and Bo Zheng
Atmos. Chem. Phys., 17, 935–963, https://doi.org/10.5194/acp-17-935-2017, https://doi.org/10.5194/acp-17-935-2017, 2017
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An anthropogenic emission inventory for Asia is developed for the years 2008 and 2010 to support the Model Inter-Comparison Study for Asia (MICS-Asia) and the Task Force on Hemispheric Transport of Air Pollution (TF HTAP) projects by a mosaic of up-to-date regional emission inventories. The total Asian emissions in 2010 are estimated as follows: 51.3 Tg SO2, 52.1 Tg NOx, 336.5 Tg CO, 67.0 Tg NMVOC, 28.7 Tg NH3, 31.7 Tg PM10, 22.7 Tg PM2.5, 3.5 Tg BC, 8.3 Tg OC, and 17.3 Pg CO2.
Bo Zheng, Qiang Zhang, Dan Tong, Chuchu Chen, Chaopeng Hong, Meng Li, Guannan Geng, Yu Lei, Hong Huo, and Kebin He
Atmos. Chem. Phys., 17, 921–933, https://doi.org/10.5194/acp-17-921-2017, https://doi.org/10.5194/acp-17-921-2017, 2017
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The resolution dependence of uncertainties in proxy-based gridded inventories can be explained by the decoupling of emission facility locations from spatial proxies on fine scales. We conclude that proxy-based inventories are of sufficient quality to support regional and global models (larger than 0.25° in this case study); however, to support urban-scale models with accurate emission inputs, bottom-up inventories incorporating exact locations of emitting facilities have to be developed instead.
Yaduan Zhou, Yu Zhao, Pan Mao, Qiang Zhang, Jie Zhang, Liping Qiu, and Yang Yang
Atmos. Chem. Phys., 17, 211–233, https://doi.org/10.5194/acp-17-211-2017, https://doi.org/10.5194/acp-17-211-2017, 2017
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A high-resolution emission inventory was developed for Jiangsu, China, using the bottom-up approach. Through comparisons with other national and regional inventories, the best agreement between available ground observation and air quality simulation was found when the provincial inventory was applied. The result implied the advantage of improved emission inventory at local scale for high-resolution air quality modeling.
Qinyi Li, Li Zhang, Tao Wang, Yee Jun Tham, Ravan Ahmadov, Likun Xue, Qiang Zhang, and Junyu Zheng
Atmos. Chem. Phys., 16, 14875–14890, https://doi.org/10.5194/acp-16-14875-2016, https://doi.org/10.5194/acp-16-14875-2016, 2016
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The regional distributions and impacts of N2O5 and ClNO2 remain poorly understood. To address the problem, we developed a chemical transport model further and conducted the first high-resolution simulation of the distributions of the two species. Our research demonstrated the significant impacts of the two gases on the lifetime of nitrogen oxides, secondary nitrate production and ozone formation in southern China and highlighted the necessity of considering this chemistry in air quality models.
Daniel J. Jacob, Alexander J. Turner, Joannes D. Maasakkers, Jianxiong Sheng, Kang Sun, Xiong Liu, Kelly Chance, Ilse Aben, Jason McKeever, and Christian Frankenberg
Atmos. Chem. Phys., 16, 14371–14396, https://doi.org/10.5194/acp-16-14371-2016, https://doi.org/10.5194/acp-16-14371-2016, 2016
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Methane is a greenhouse gas emitted by a range of natural and anthropogenic sources. Atmospheric methane has been measured continuously from space since 2003, and new instruments are planned to launch in the near future that will greatly expand the capabilities of space-based observations. We review the value of current, future, and proposed satellite observations to better quantify methane emissions from the global scale down to the scale of point sources.
Lei Zhu, Daniel J. Jacob, Patrick S. Kim, Jenny A. Fisher, Karen Yu, Katherine R. Travis, Loretta J. Mickley, Robert M. Yantosca, Melissa P. Sulprizio, Isabelle De Smedt, Gonzalo González Abad, Kelly Chance, Can Li, Richard Ferrare, Alan Fried, Johnathan W. Hair, Thomas F. Hanisco, Dirk Richter, Amy Jo Scarino, James Walega, Petter Weibring, and Glenn M. Wolfe
Atmos. Chem. Phys., 16, 13477–13490, https://doi.org/10.5194/acp-16-13477-2016, https://doi.org/10.5194/acp-16-13477-2016, 2016
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HCHO column data are widely used as a proxy for VOCs emissions, but validation of the data has been extremely limited. We use accurate aircraft observations to validate and intercompare 6 HCHO retrievals with GEOS-Chem as the intercomparison platform. Retrievals are interconsistent in spatial variability over the SE US and in daily variability, but are biased low by 20–51 %. Our work supports the use of HCHO column as a quantitative proxy for isoprene emission after correction of the low bias.
Katherine R. Travis, Daniel J. Jacob, Jenny A. Fisher, Patrick S. Kim, Eloise A. Marais, Lei Zhu, Karen Yu, Christopher C. Miller, Robert M. Yantosca, Melissa P. Sulprizio, Anne M. Thompson, Paul O. Wennberg, John D. Crounse, Jason M. St. Clair, Ronald C. Cohen, Joshua L. Laughner, Jack E. Dibb, Samuel R. Hall, Kirk Ullmann, Glenn M. Wolfe, Illana B. Pollack, Jeff Peischl, Jonathan A. Neuman, and Xianliang Zhou
Atmos. Chem. Phys., 16, 13561–13577, https://doi.org/10.5194/acp-16-13561-2016, https://doi.org/10.5194/acp-16-13561-2016, 2016
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Ground-level ozone pollution in the Southeast US involves complex chemistry driven by anthropogenic emissions of nitrogen oxides (NOx) and biogenic emissions of isoprene. We find that US NOx emissions are overestimated nationally by as much as 50 % and that reducing model emissions by this amount results in good agreement with SEAC4RS aircraft measurements in August and September 2013. Observations of nitrate wet deposition fluxes and satellite NO2 columns further support this result.
Tomás Sherwen, Johan A. Schmidt, Mat J. Evans, Lucy J. Carpenter, Katja Großmann, Sebastian D. Eastham, Daniel J. Jacob, Barbara Dix, Theodore K. Koenig, Roman Sinreich, Ivan Ortega, Rainer Volkamer, Alfonso Saiz-Lopez, Cristina Prados-Roman, Anoop S. Mahajan, and Carlos Ordóñez
Atmos. Chem. Phys., 16, 12239–12271, https://doi.org/10.5194/acp-16-12239-2016, https://doi.org/10.5194/acp-16-12239-2016, 2016
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We present a simulation of tropospheric Cl, Br, I chemistry within the GEOS-Chem CTM. We find a decrease in tropospheric ozone burden of 18.6 % and a 8.2 % decrease in global mean OH concentrations. Cl oxidation of some VOCs range from 15 to 27 % of the total loss. Bromine plays a small role in oxidising oVOCs. Surface ozone, ozone sondes, and methane lifetime are in general improved by the inclusion of halogens. We argue that simulated bromine and chlorine represent a lower limit.
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.
Xing Qin An, Shi Xian Zhai, Min Jin, Sunling Gong, and Yu Wang
Geosci. Model Dev., 9, 2153–2165, https://doi.org/10.5194/gmd-9-2153-2016, https://doi.org/10.5194/gmd-9-2153-2016, 2016
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The aerosol adjoint module of the atmospheric chemical modeling system GRAPES–CUACE was developed, tested for its correctness, and used in a receptor–source sensitivity test. The results showed that controlling critical emission sources during critical time intervals on the basis of adjoint sensitivity analysis is much more efficient than controlling administrative specified regions during an experiential time period.
Yuanzheng Cui, Jintai Lin, Chunqiao Song, Mengyao Liu, Yingying Yan, Yuan Xu, and Bo Huang
Atmos. Chem. Phys., 16, 6207–6221, https://doi.org/10.5194/acp-16-6207-2016, https://doi.org/10.5194/acp-16-6207-2016, 2016
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We find rapid NO2 growth over Western China over 2005–2013 at a rate which exceeds the rates over the well-known polluted regions in the east. A nested GEOS-Chem simulation and Chinese official emission data confirm that anthropogenic emissions are the main driver of NO2 variations. Additional socioeconomic analysis suggests that this rapid NO2 growth is likely related to the fast industrialization and urbanization along with the "Go West" movement as well as relatively weak emission controls.
Jenny A. Fisher, Daniel J. Jacob, Katherine R. Travis, Patrick S. Kim, Eloise A. Marais, Christopher Chan Miller, Karen Yu, Lei Zhu, Robert M. Yantosca, Melissa P. Sulprizio, Jingqiu Mao, Paul O. Wennberg, John D. Crounse, Alex P. Teng, Tran B. Nguyen, Jason M. St. Clair, Ronald C. Cohen, Paul Romer, Benjamin A. Nault, Paul J. Wooldridge, Jose L. Jimenez, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Paul B. Shepson, Fulizi Xiong, Donald R. Blake, Allen H. Goldstein, Pawel K. Misztal, Thomas F. Hanisco, Glenn M. Wolfe, Thomas B. Ryerson, Armin Wisthaler, and Tomas Mikoviny
Atmos. Chem. Phys., 16, 5969–5991, https://doi.org/10.5194/acp-16-5969-2016, https://doi.org/10.5194/acp-16-5969-2016, 2016
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We use new airborne and ground-based observations from two summer 2013 campaigns in the southeastern US, interpreted with a chemical transport model, to understand the impact of isoprene and monoterpene chemistry on the atmospheric NOx budget via production of organic nitrates (RONO2). We find that a diversity of species contribute to observed RONO2. Our work implies that the NOx sink to RONO2 production is only sensitive to NOx emissions in regions where they are already low.
Fei Liu, Steffen Beirle, Qiang Zhang, Steffen Dörner, Kebin He, and Thomas Wagner
Atmos. Chem. Phys., 16, 5283–5298, https://doi.org/10.5194/acp-16-5283-2016, https://doi.org/10.5194/acp-16-5283-2016, 2016
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We present a new method to quantify NOx emissions and corresponding atmospheric lifetimes from OMI NO2 observations together with ECMWF wind fields without further model input for sources located in polluted background. The derived NOx emissions show generally good agreement with bottom-up inventories for power plants and cities. Global inventory significantly underestimated NOx emissions in Chinese cities, most likely due to uncertainties associated with downscaling approaches.
Yuxuan Zhang, Qiang Zhang, Yafang Cheng, Hang Su, Simonas Kecorius, Zhibin Wang, Zhijun Wu, Min Hu, Tong Zhu, Alfred Wiedensohler, and Kebin He
Atmos. Meas. Tech., 9, 1833–1843, https://doi.org/10.5194/amt-9-1833-2016, https://doi.org/10.5194/amt-9-1833-2016, 2016
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We develop a novel method in this work for in situ measurements of the morphology and effective density of ambient In-BC cores using a volatility tandem differential mobility analyzer and a single-particle soot photometer. We find that In-BC cores hardly transform the morphology of BC into a void-free sphere. Taking the morphology and density of ambient In-BC cores into account, our work provides a new insight into the enhancement of light absorption for In-BC particles in the atmosphere.
Christopher Chan Miller, Daniel J. Jacob, Gonzalo González Abad, and Kelly Chance
Atmos. Chem. Phys., 16, 4631–4639, https://doi.org/10.5194/acp-16-4631-2016, https://doi.org/10.5194/acp-16-4631-2016, 2016
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Volatile organic compounds (VOCs) are important precursors for photochemical smog.
Glyoxal is an organic compound produced in the atmosphere from reactions of larger VOCs. OMI satellite observations of glyoxal show a large hotspot over the Pearl River delta. The hotspot can be explained by industrial paint and solvent emissions of aromatic VOCs. Our work shows OMI observations are consistent with current VOC emissions estimates, whereas previous work has suggested large underestimates.
Karen Yu, Daniel J. Jacob, Jenny A. Fisher, Patrick S. Kim, Eloise A. Marais, Christopher C. Miller, Katherine R. Travis, Lei Zhu, Robert M. Yantosca, Melissa P. Sulprizio, Ron C. Cohen, Jack E. Dibb, Alan Fried, Tomas Mikoviny, Thomas B. Ryerson, Paul O. Wennberg, and Armin Wisthaler
Atmos. Chem. Phys., 16, 4369–4378, https://doi.org/10.5194/acp-16-4369-2016, https://doi.org/10.5194/acp-16-4369-2016, 2016
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Increasing the spatial resolution of a chemical transport model may improve simulations but can be computationally expensive. Using observations from the SEAC4RS aircraft campaign, we find that at higher spatial resolutions, models are better able to simulate the chemical pathways of ozone precursors, but the overall effect on regional mean concentrations is small. This implies that for continental boundary layer applications, coarse resolution models are adequate.
Xuekun Fang, Min Shao, Andreas Stohl, Qiang Zhang, Junyu Zheng, Hai Guo, Chen Wang, Ming Wang, Jiamin Ou, Rona L. Thompson, and Ronald G. Prinn
Atmos. Chem. Phys., 16, 3369–3382, https://doi.org/10.5194/acp-16-3369-2016, https://doi.org/10.5194/acp-16-3369-2016, 2016
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This is the first study reporting top-down estimates of benzene and toluene emissions in southern China using atmospheric measurement data from a rural site in the area, an atmospheric transport model and an inverse modeling method. This study shows in detail the temporal and spatial differences between the inversion estimate and four different bottom-up emission inventories (RCP, REAS, MEIC; Yin et al., 2015). We propose that more observations are urgently needed in future.
Yuli Shan, Dabo Guan, Jianghua Liu, Zhu Liu, Jingru Liu, Heike Schroeder, Yang Chen, Shuai Shao, Zhifu Mi, and Qiang Zhang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2016-176, https://doi.org/10.5194/acp-2016-176, 2016
Revised manuscript not accepted
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Cities contribute 85 % of the total CO2 emissions in China and thus are considered the key areas for implementing policies designed for climate change adaption and CO2 emission mitigation. This study presents a method for constructing a CO2 emissions inventory for Chinese cities in terms of the definition provided by the IPCC territorial emission accounting approach. We apply this method to compile CO2 emissions inventories for 20 Chinese cities and analyse their emission characteristic.
Yingying Yan, Jintai Lin, Jinxuan Chen, and Lu Hu
Atmos. Chem. Phys., 16, 2381–2400, https://doi.org/10.5194/acp-16-2381-2016, https://doi.org/10.5194/acp-16-2381-2016, 2016
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We use a newly built two-way coupling system of the GEOS-Chem CTM to simulate the global tropospheric O3 in 2009. It significantly improves the simulation upon the global model by comparisons with a suite of ground, aircraft, and satellite measurements, also reduces the global OH by 5 % with enhancements by 5 % in the lifetimes of MCF and methane. Therefore, improving model representations of small-scale processes is a critical step forward to understanding the global tropospheric chemistry.
Yaning Kang, Mingxu Liu, Yu Song, Xin Huang, Huan Yao, Xuhui Cai, Hongsheng Zhang, Ling Kang, Xuejun Liu, Xiaoyuan Yan, Hong He, Qiang Zhang, Min Shao, and Tong Zhu
Atmos. Chem. Phys., 16, 2043–2058, https://doi.org/10.5194/acp-16-2043-2016, https://doi.org/10.5194/acp-16-2043-2016, 2016
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The multi-year (1980–2012) comprehensive ammonia emissions inventories were compiled for China on 1 km × 1 km grid.
Various realistic parameters (ambient temperature, wind speed, soil acidity, synthetic fertilizer types, etc.) were considered in these inventories to synthetically refine the emission factors of ammonia volatilization according to local agricultural practice.
This paper shows the interannual trend and spatial distribution of ammonia emissions in details over recent decades.
E. A. Marais, D. J. Jacob, J. L. Jimenez, P. Campuzano-Jost, D. A. Day, W. Hu, J. Krechmer, L. Zhu, P. S. Kim, C. C. Miller, J. A. Fisher, K. Travis, K. Yu, T. F. Hanisco, G. M. Wolfe, H. L. Arkinson, H. O. T. Pye, K. D. Froyd, J. Liao, and V. F. McNeill
Atmos. Chem. Phys., 16, 1603–1618, https://doi.org/10.5194/acp-16-1603-2016, https://doi.org/10.5194/acp-16-1603-2016, 2016
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Isoprene secondary organic aerosol (SOA) is a dominant aerosol component in the southeast US, but models routinely underestimate isoprene SOA with traditional schemes based on chamber studies operated under conditions not representative of isoprene-emitting forests. We develop a new irreversible uptake mechanism to reproduce isoprene SOA yields (3.3 %) and composition, and find a factor of 2 co-benefit of SO2 emission controls on reducing sulfate and organic aerosol in the southeast US.
V. Shah, L. Jaeglé, L. E. Gratz, J. L. Ambrose, D. A. Jaffe, N. E. Selin, S. Song, T. L. Campos, F. M. Flocke, M. Reeves, D. Stechman, M. Stell, J. Festa, J. Stutz, A. J. Weinheimer, D. J. Knapp, D. D. Montzka, G. S. Tyndall, E. C. Apel, R. S. Hornbrook, A. J. Hills, D. D. Riemer, N. J. Blake, C. A. Cantrell, and R. L. Mauldin III
Atmos. Chem. Phys., 16, 1511–1530, https://doi.org/10.5194/acp-16-1511-2016, https://doi.org/10.5194/acp-16-1511-2016, 2016
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We present airborne observations of mercury over the southeastern USA during summer. Higher concentrations of oxidized mercury were observed in clean, dry air masses descending in the subtropical anti-cyclones. We used an atmospheric model to simulate the chemistry and transport of mercury. We found reasonable agreement with the observations when the modeled oxidation of elemental mercury was increased, suggesting fast cycling between elemental and oxidized mercury.
H.-M. Lee, F. Paulot, D. K. Henze, K. Travis, D. J. Jacob, L. H. Pardo, and B. A. Schichtel
Atmos. Chem. Phys., 16, 525–540, https://doi.org/10.5194/acp-16-525-2016, https://doi.org/10.5194/acp-16-525-2016, 2016
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Sources of nitrogen deposition (Ndep) in Federal Class I areas in the US are investigated, identifying unique features in contributions from different species, sectors and locations. Ndep in many parks is impacted by emissions several hundred km away; the role of oxidized vs reduced sources varies regionally. Emissions reductions in the western US most effectively reduce the extent of areas in critical load exceedance, while reductions in the east most effectively reduce exceedance magnitudes.
F. Liu, Q. Zhang, D. Tong, B. Zheng, M. Li, H. Huo, and K. B. He
Atmos. Chem. Phys., 15, 13299–13317, https://doi.org/10.5194/acp-15-13299-2015, https://doi.org/10.5194/acp-15-13299-2015, 2015
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This is the first study in which emissions from China’s coal-fired power plants were estimated at unit level for a 20-year period. This new emission inventory is constructed from a unit-based database compiled in this work, named the China coal-fired Power plant Emissions Database (CPED), which includes detailed information on the technologies, activity data, operation situation, emission factors, and locations of individual units.
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.
Y. Zhao, L. P. Qiu, R. Y. Xu, F. J. Xie, Q. Zhang, Y. Y. Yu, C. P. Nielsen, H. X. Qin, H. K. Wang, X. C. Wu, W. Q. Li, and J. Zhang
Atmos. Chem. Phys., 15, 12623–12644, https://doi.org/10.5194/acp-15-12623-2015, https://doi.org/10.5194/acp-15-12623-2015, 2015
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A high-resolution emission inventory of air pollutants and CO2 for Nanjing, a typical city in eastern China, is developed, incorporating the best available local information from on-site surveys. The temporal and spatial distribution of the emissions and the correlation between specific species of the inventory are assessed by comparisons with observations and other inventories at larger spatial scale. The emission inventory provides a basis to consider the quality of instrumental observations.
G. Janssens-Maenhout, M. Crippa, D. Guizzardi, F. Dentener, M. Muntean, G. Pouliot, T. Keating, Q. Zhang, J. Kurokawa, R. Wankmüller, H. Denier van der Gon, J. J. P. Kuenen, Z. Klimont, G. Frost, S. Darras, B. Koffi, and M. Li
Atmos. Chem. Phys., 15, 11411–11432, https://doi.org/10.5194/acp-15-11411-2015, https://doi.org/10.5194/acp-15-11411-2015, 2015
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This paper provides monthly emission grid maps at 0.1deg x 0.1deg resolution with global coverage for air pollutants and aerosols anthropogenic emissions in 2008 and 2010.
Countries are consistently inter-compared with sector-specific implied emission factors, per capita emissions and emissions per unit of GDP.
The emission grid maps compose the reference emissions data set for the community modelling hemispheric transport of air pollution (HTAP).
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.
P. S. Kim, D. J. Jacob, J. A. Fisher, K. Travis, K. Yu, L. Zhu, R. M. Yantosca, M. P. Sulprizio, J. L. Jimenez, P. Campuzano-Jost, K. D. Froyd, J. Liao, J. W. Hair, M. A. Fenn, C. F. Butler, N. L. Wagner, T. D. Gordon, A. Welti, P. O. Wennberg, J. D. Crounse, J. M. St. Clair, A. P. Teng, D. B. Millet, J. P. Schwarz, M. Z. Markovic, and A. E. Perring
Atmos. Chem. Phys., 15, 10411–10433, https://doi.org/10.5194/acp-15-10411-2015, https://doi.org/10.5194/acp-15-10411-2015, 2015
L. Zhang, D. K. Henze, G. A. Grell, G. R. Carmichael, N. Bousserez, Q. Zhang, O. Torres, C. Ahn, Z. Lu, J. Cao, and Y. Mao
Atmos. Chem. Phys., 15, 10281–10308, https://doi.org/10.5194/acp-15-10281-2015, https://doi.org/10.5194/acp-15-10281-2015, 2015
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We attempt to reduce uncertainties in BC emissions and improve BC model simulations by developing top-down, spatially resolved, estimates of BC emissions through assimilation of OMI observations of aerosol absorption optical depth (AAOD) with the GEOS-Chem model and its adjoint for April and October of 2006. Despite the limitations and uncertainties, using OMI AAOD to constrain BC sources we are able to improve model representation of BC distributions, particularly over China.
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.
J. Kaiser, G. M. Wolfe, K. E. Min, S. S. Brown, C. C. Miller, D. J. Jacob, J. A. deGouw, M. Graus, T. F. Hanisco, J. Holloway, J. Peischl, I. B. Pollack, T. B. Ryerson, C. Warneke, R. A. Washenfelder, and F. N. Keutsch
Atmos. Chem. Phys., 15, 7571–7583, https://doi.org/10.5194/acp-15-7571-2015, https://doi.org/10.5194/acp-15-7571-2015, 2015
A. J. Turner and D. J. Jacob
Atmos. Chem. Phys., 15, 7039–7048, https://doi.org/10.5194/acp-15-7039-2015, https://doi.org/10.5194/acp-15-7039-2015, 2015
A. J. Turner, D. J. Jacob, K. J. Wecht, J. D. Maasakkers, E. Lundgren, A. E. Andrews, S. C. Biraud, H. Boesch, K. W. Bowman, N. M. Deutscher, M. K. Dubey, D. W. T. Griffith, F. Hase, A. Kuze, J. Notholt, H. Ohyama, R. Parker, V. H. Payne, R. Sussmann, C. Sweeney, V. A. Velazco, T. Warneke, P. O. Wennberg, and D. Wunch
Atmos. Chem. Phys., 15, 7049–7069, https://doi.org/10.5194/acp-15-7049-2015, https://doi.org/10.5194/acp-15-7049-2015, 2015
H. Y. Zhao, Q. Zhang, D. B. Guan, S. J. Davis, Z. Liu, H. Huo, J. T. Lin, W. D. Liu, and K. B. He
Atmos. Chem. Phys., 15, 5443–5456, https://doi.org/10.5194/acp-15-5443-2015, https://doi.org/10.5194/acp-15-5443-2015, 2015
G. J. Zheng, F. K. Duan, H. Su, Y. L. Ma, Y. Cheng, B. Zheng, Q. Zhang, T. Huang, T. Kimoto, D. Chang, U. Pöschl, Y. F. Cheng, and K. B. He
Atmos. Chem. Phys., 15, 2969–2983, https://doi.org/10.5194/acp-15-2969-2015, https://doi.org/10.5194/acp-15-2969-2015, 2015
M. S. Long, R. Yantosca, J. E. Nielsen, C. A. Keller, A. da Silva, M. P. Sulprizio, S. Pawson, and D. J. Jacob
Geosci. Model Dev., 8, 595–602, https://doi.org/10.5194/gmd-8-595-2015, https://doi.org/10.5194/gmd-8-595-2015, 2015
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This paper presents results from the modularization of the GEOS-Chem chemical transport model, and its coupling as the chemical operator within the NASA-GMAO GEOS-5 Earth system model (ESM). The key findings are that chemistry within the modular GEOS-Chem system shows consistent, high strong-scaling properties across the range of distributed processors, transport is the limiting component prohibiting efficient scalability, and GEOS-Chem is able to generate suitable chemical results in an ESM.
B. Zheng, Q. Zhang, Y. Zhang, K. B. He, K. Wang, G. J. Zheng, F. K. Duan, Y. L. Ma, and T. Kimoto
Atmos. Chem. Phys., 15, 2031–2049, https://doi.org/10.5194/acp-15-2031-2015, https://doi.org/10.5194/acp-15-2031-2015, 2015
M. Wang, M. Shao, W. Chen, S. Lu, Y. Liu, B. Yuan, Q. Zhang, Q. Zhang, C.-C. Chang, B. Wang, L. Zeng, M. Hu, Y. Yang, and Y. Li
Atmos. Chem. Phys., 15, 1489–1502, https://doi.org/10.5194/acp-15-1489-2015, https://doi.org/10.5194/acp-15-1489-2015, 2015
G. Snider, C. L. Weagle, R. V. Martin, A. van Donkelaar, K. Conrad, D. Cunningham, C. Gordon, M. Zwicker, C. Akoshile, P. Artaxo, N. X. Anh, J. Brook, J. Dong, R. M. Garland, R. Greenwald, D. Griffith, K. He, B. N. Holben, R. Kahn, I. Koren, N. Lagrosas, P. Lestari, Z. Ma, J. Vanderlei Martins, E. J. Quel, Y. Rudich, A. Salam, S. N. Tripathi, C. Yu, Q. Zhang, Y. Zhang, M. Brauer, A. Cohen, M. D. Gibson, and Y. Liu
Atmos. Meas. Tech., 8, 505–521, https://doi.org/10.5194/amt-8-505-2015, https://doi.org/10.5194/amt-8-505-2015, 2015
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We have initiated a global network of ground-level monitoring stations to measure concentrations of fine aerosols in urban environments. Our findings include major ions species, total mass, and total scatter at three wavelengths. Results will be used to further evaluate and enhance satellite remote sensing estimates.
Z. Jiang, J. R. Worden, D. B. A. Jones, J.-T. Lin, W. W. Verstraeten, and D. K. Henze
Atmos. Chem. Phys., 15, 99–112, https://doi.org/10.5194/acp-15-99-2015, https://doi.org/10.5194/acp-15-99-2015, 2015
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We use satellite measurements of O3, CO and NO2 from TES, MOPITT and OMI to quantify O3 precursor emissions for 2006 and their impact on free tropospheric O3 over northeastern Asia. Using the adjoint of GEOS-Chem, we found that Chinese emissions have the largest influence on the free tropospheric O3. The contributions from lightning NOx in summer and India and southeastern Asia emissions in winter are sizable, comparable with Chinese emissions.
Y.-Y. Yan, J.-T. Lin, Y. Kuang, D. Yang, and L. Zhang
Atmos. Chem. Phys., 14, 12649–12663, https://doi.org/10.5194/acp-14-12649-2014, https://doi.org/10.5194/acp-14-12649-2014, 2014
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Limited by coarse resolutions, global chemical transport models cannot well capture small-scale nonlinear processes. To alleviate the problem, we develop a two-way coupled system to integrate the global GEOS-Chem model and its three high-resolution nested models covering Asia, Europe and North America. Confirmed by comparisons with observations, the coupled system improves upon the global model with a 10% increase in global tropospheric CO, a 4% decrease in OH and a 4% increase in MCF lifetime.
S. Nordmann, Y. F. Cheng, G. R. Carmichael, M. Yu, H. A. C. Denier van der Gon, Q. Zhang, P. E. Saide, U. Pöschl, H. Su, W. Birmili, and A. Wiedensohler
Atmos. Chem. Phys., 14, 12683–12699, https://doi.org/10.5194/acp-14-12683-2014, https://doi.org/10.5194/acp-14-12683-2014, 2014
C. Chan Miller, G. Gonzalez Abad, H. Wang, X. Liu, T. Kurosu, D. J. Jacob, and K. Chance
Atmos. Meas. Tech., 7, 3891–3907, https://doi.org/10.5194/amt-7-3891-2014, https://doi.org/10.5194/amt-7-3891-2014, 2014
B. Zheng, H. Huo, Q. Zhang, Z. L. Yao, X. T. Wang, X. F. Yang, H. Liu, and K. B. He
Atmos. Chem. Phys., 14, 9787–9805, https://doi.org/10.5194/acp-14-9787-2014, https://doi.org/10.5194/acp-14-9787-2014, 2014
K. J. Wecht, D. J. Jacob, M. P. Sulprizio, G. W. Santoni, S. C. Wofsy, R. Parker, H. Bösch, and J. Worden
Atmos. Chem. Phys., 14, 8173–8184, https://doi.org/10.5194/acp-14-8173-2014, https://doi.org/10.5194/acp-14-8173-2014, 2014
C. A. Keller, M. S. Long, R. M. Yantosca, A. M. Da Silva, S. Pawson, and D. J. Jacob
Geosci. Model Dev., 7, 1409–1417, https://doi.org/10.5194/gmd-7-1409-2014, https://doi.org/10.5194/gmd-7-1409-2014, 2014
C. He, Q. B. Li, K. N. Liou, J. Zhang, L. Qi, Y. Mao, M. Gao, Z. Lu, D. G. Streets, Q. Zhang, M. M. Sarin, and K. Ram
Atmos. Chem. Phys., 14, 7091–7112, https://doi.org/10.5194/acp-14-7091-2014, https://doi.org/10.5194/acp-14-7091-2014, 2014
P. Zoogman, D. J. Jacob, K. Chance, X. Liu, M. Lin, A. Fiore, and K. Travis
Atmos. Chem. Phys., 14, 6261–6271, https://doi.org/10.5194/acp-14-6261-2014, https://doi.org/10.5194/acp-14-6261-2014, 2014
M. Wang, M. Shao, W. Chen, B. Yuan, S. Lu, Q. Zhang, L. Zeng, and Q. Wang
Atmos. Chem. Phys., 14, 5871–5891, https://doi.org/10.5194/acp-14-5871-2014, https://doi.org/10.5194/acp-14-5871-2014, 2014
M. Li, Q. Zhang, D. G. Streets, K. B. He, Y. F. Cheng, L. K. Emmons, H. Huo, S. C. Kang, Z. Lu, M. Shao, H. Su, X. Yu, and Y. Zhang
Atmos. Chem. Phys., 14, 5617–5638, https://doi.org/10.5194/acp-14-5617-2014, https://doi.org/10.5194/acp-14-5617-2014, 2014
L. Zhang, D. J. Jacob, X. Yue, N. V. Downey, D. A. Wood, and D. Blewitt
Atmos. Chem. Phys., 14, 5295–5309, https://doi.org/10.5194/acp-14-5295-2014, https://doi.org/10.5194/acp-14-5295-2014, 2014
L. T. Wang, Z. Wei, J. Yang, Y. Zhang, F. F. Zhang, J. Su, C. C. Meng, and Q. Zhang
Atmos. Chem. Phys., 14, 3151–3173, https://doi.org/10.5194/acp-14-3151-2014, https://doi.org/10.5194/acp-14-3151-2014, 2014
E. V. Fischer, D. J. Jacob, R. M. Yantosca, M. P. Sulprizio, D. B. Millet, J. Mao, F. Paulot, H. B. Singh, A. Roiger, L. Ries, R.W. Talbot, K. Dzepina, and S. Pandey Deolal
Atmos. Chem. Phys., 14, 2679–2698, https://doi.org/10.5194/acp-14-2679-2014, https://doi.org/10.5194/acp-14-2679-2014, 2014
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
B. Mijling, R. J. van der A, and Q. Zhang
Atmos. Chem. Phys., 13, 12003–12012, https://doi.org/10.5194/acp-13-12003-2013, https://doi.org/10.5194/acp-13-12003-2013, 2013
P. S. Kim, D. J. Jacob, X. Liu, J. X. Warner, K. Yang, K. Chance, V. Thouret, and P. Nedelec
Atmos. Chem. Phys., 13, 9321–9335, https://doi.org/10.5194/acp-13-9321-2013, https://doi.org/10.5194/acp-13-9321-2013, 2013
T. Stavrakou, J.-F. Müller, K. F. Boersma, R. J. van der A, J. Kurokawa, T. Ohara, and Q. Zhang
Atmos. Chem. Phys., 13, 9057–9082, https://doi.org/10.5194/acp-13-9057-2013, https://doi.org/10.5194/acp-13-9057-2013, 2013
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
J. Mao, S. Fan, D. J. Jacob, and K. R. Travis
Atmos. Chem. Phys., 13, 509–519, https://doi.org/10.5194/acp-13-509-2013, https://doi.org/10.5194/acp-13-509-2013, 2013
J.-T. Lin, Z. Liu, Q. Zhang, H. Liu, J. Mao, and G. Zhuang
Atmos. Chem. Phys., 12, 12255–12275, https://doi.org/10.5194/acp-12-12255-2012, https://doi.org/10.5194/acp-12-12255-2012, 2012
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Global tropospheric halogen (Cl, Br, I) chemistry and its impact on oxidants
The role of emission reductions and the meteorological situation for air quality improvements during the COVID-19 lockdown period in central Europe
Heterogeneity and chemical reactivity of the remote troposphere defined by aircraft measurements
A mass-balance-based emission inventory of non-methane volatile organic compounds (NMVOCs) for solvent use in China
Opinion: The germicidal effect of ambient air (open-air factor) revisited
Impact of Athabasca oil sands operations on mercury levels in air and deposition
Study of different Carbon Bond 6 (CB6) mechanisms by using a concentration sensitivity analysis
Accelerating methane growth rate from 2010 to 2017: leading contributions from the tropics and East Asia
Observation and modelling of ozone-destructive halogen chemistry in a passively degassing volcanic plume
Modeling study of the impact of SO2 volcanic passive emissions on the tropospheric sulfur budget
The impact of organic pollutants from Indonesian peatland fires on the tropospheric and lower stratospheric composition
Comprehensive evaluations of diurnal NO2 measurements during DISCOVER-AQ 2011: effects of resolution-dependent representation of NOx emissions
Downscaling system for modeling of atmospheric composition on regional, urban and street scales
Satellite soil moisture data assimilation impacts on modeling weather variables and ozone in the southeastern US – Part 1: An overview
Development of ozone reactivity scales for volatile organic compounds in a Chinese megacity
Measured and modelled air quality trends in Italy over the period 2003–2010
Large and increasing methane emissions from eastern Amazonia derived from satellite data, 2010–2018
Contrasting chemical environments in summertime for atmospheric ozone across major Chinese industrial regions: the effectiveness of emission control strategies
Unexpected enhancement of ozone exposure and health risks during National Day in China
Role of oceanic ozone deposition in explaining temporal variability in surface ozone at High Arctic sites
Technical note: Quality assessment of ozone reanalysis products over subarctic Europe for biome modeling and ozone risk mapping
Oxidation of low-molecular-weight organic compounds in cloud droplets: global impact on tropospheric oxidants
Bias-correcting carbon fluxes derived from land-surface satellite data for retrospective and near-real-time assimilation systems
Characterizing model errors in chemical transport modeling of methane: using GOSAT XCH4 data with weak-constraint four-dimensional variational data assimilation
Estimation of fire-induced carbon emissions from Equatorial Asia in 2015 using in situ aircraft and ship observations
Influence of weather situation on non-CO2 aviation climate effects: the REACT4C climate change functions
Impact of international shipping emissions on ozone and PM2.5 in East Asia during summer: the important role of HONO and ClNO2
Modelling the impacts of iodine chemistry on the northern Indian Ocean marine boundary layer
Time-dependent 3D simulations of tropospheric ozone depletion events in the Arctic spring using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem)
Assessing and improving cloud-height-based parameterisations of global lightning flash rate, and their impact on lightning-produced NOx and tropospheric composition in a chemistry–climate model
Impact of regional Northern Hemisphere mid-latitude anthropogenic sulfur dioxide emissions on local and remote tropospheric oxidants
Impact of organic molecular structure on the estimation of atmospherically relevant physicochemical parameters
Spatial and temporal variability in the hydroxyl (OH) radical: understanding the role of large-scale climate features and their influence on OH through its dynamical and photochemical drivers
Analysis of atmospheric ammonia over South and East Asia based on the MOZART-4 model and its comparison with satellite and surface observations
Air quality and health benefits from ultra-low emission control policy indicated by continuous emission monitoring: a case study in the Yangtze River Delta region, China
Background conditions for an urban greenhouse gas network in the Washington, DC, and Baltimore metropolitan region
Explicit modeling of isoprene chemical processing in polluted air masses in suburban areas of the Yangtze River Delta region: radical cycling and formation of ozone and formaldehyde
Evaluating consistency between total column CO2 retrievals from OCO-2 and the in-situ network over North America: Implications for carbon flux estimation
Evaluation of the LOTOS-EUROS NO2 simulations using ground-based measurements and S5P/TROPOMI observations over Greece
Reactive organic carbon emissions from volatile chemical products
A three-dimensional-model inversion of methyl chloroform to constrain the atmospheric oxidative capacity
Technical note: On comparing greenhouse gas emission metrics
Late-spring and summertime tropospheric ozone and NO2 in western Siberia and the Russian Arctic: regional model evaluation and sensitivities
10-year satellite-constrained fluxes of ammonia improve performance of chemistry transport models
Revealing the sulfur dioxide emission reductions in China by assimilating surface observations in WRF-Chem
Tropospheric ozone in CMIP6 simulations
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 %.
Volker Matthias, Markus Quante, Jan A. Arndt, Ronny Badeke, Lea Fink, Ronny Petrik, Josefine Feldner, Daniel Schwarzkopf, Eliza-Maria Link, Martin O. P. Ramacher, and Ralf Wedemann
Atmos. Chem. Phys., 21, 13931–13971, https://doi.org/10.5194/acp-21-13931-2021, https://doi.org/10.5194/acp-21-13931-2021, 2021
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COVID-19 lockdown measures in spring 2020 led to cleaner air in central Europe. Densely populated areas benefitted mainly from largely reduced NO2 concentrations, while rural areas experienced lower reductions in NO2 but also lower ozone concentrations. Very low particulate matter (PM) concentrations in parts of Europe were not an effect of lockdown measures. Model simulations show that modified weather conditions are more significant for ozone and PM than severe traffic emission reductions.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven Wofsy
Atmos. Chem. Phys., 21, 13729–13746, https://doi.org/10.5194/acp-21-13729-2021, https://doi.org/10.5194/acp-21-13729-2021, 2021
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The NASA Atmospheric Tomography (ATom) mission built a climatology of the chemical composition of tropospheric air parcels throughout the middle of the Pacific and Atlantic oceans. The level of detail allows us to reconstruct the photochemical budgets of O3 and CH4 over these vast, remote regions. We find that most of the chemical heterogeneity is captured at the resolution used in current global chemistry models and that the majority of reactivity occurs in the
hottest20 % of parcels.
Ziwei Mo, Ru Cui, Bin Yuan, Huihua Cai, Brian C. McDonald, Meng Li, Junyu Zheng, and Min Shao
Atmos. Chem. Phys., 21, 13655–13666, https://doi.org/10.5194/acp-21-13655-2021, https://doi.org/10.5194/acp-21-13655-2021, 2021
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There is a lack of detailed understanding of NMVOC emissions from the use of volatile chemical products (VCPs) in China. This study used a mass balance method to compile a long-term emission inventory for solvent use (including coatings, adhesives, inks, pesticides, cleaners and personal care products) in China during 2000–2017. The striking growth and recent trend of solvent use NMVOC emissions can give important implications for air quality modeling and NMVOC control strategies in China.
R. Anthony Cox, Markus Ammann, John N. Crowley, Paul T. Griffiths, Hartmut Herrmann, Erik H. Hoffmann, Michael E. Jenkin, V. Faye McNeill, Abdelwahid Mellouki, Christopher J. Penkett, Andreas Tilgner, and Timothy J. Wallington
Atmos. Chem. Phys., 21, 13011–13018, https://doi.org/10.5194/acp-21-13011-2021, https://doi.org/10.5194/acp-21-13011-2021, 2021
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The term open-air factor was coined in the 1960s, establishing that rural air had powerful germicidal properties possibly resulting from immediate products of the reaction of ozone with alkenes, unsaturated compounds ubiquitously present in natural and polluted environments. We have re-evaluated those early experiments, applying the recently substantially improved knowledge, and put them into the context of the lifetime of aerosol-borne pathogens that are so important in the Covid-19 pandemic.
Ashu Dastoor, Andrei Ryjkov, Gregor Kos, Junhua Zhang, Jane Kirk, Matthew Parsons, and Alexandra Steffen
Atmos. Chem. Phys., 21, 12783–12807, https://doi.org/10.5194/acp-21-12783-2021, https://doi.org/10.5194/acp-21-12783-2021, 2021
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An assessment of mercury levels in air and deposition in the Athabasca oil sands region (AOSR) in Northern Alberta, Canada, was conducted to investigate the contribution of Hg emitted from oil sands activities to the surrounding landscape using a 3D process-based Hg model in 2012–2015. Oil sands Hg emissions are found to be important sources of Hg contamination to the local landscape in proximity to the processing activities, particularly in wintertime.
Le Cao, Simeng Li, and Luhang Sun
Atmos. Chem. Phys., 21, 12687–12714, https://doi.org/10.5194/acp-21-12687-2021, https://doi.org/10.5194/acp-21-12687-2021, 2021
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Gas-phase chemical reaction mechanisms, e.g., CB6 mechanism, are essential parts of the atmospheric transport model. In order to better understand the changes caused by the updates between different versions of the CB6 mechanism, in this study, the behavior of three different CB6 mechanisms in simulating ozone, nitrogen oxides and formaldehyde under two different emission conditions was analyzed using a concentration sensitivity analysis, and the reasons causing the deviations were figured out.
Yi Yin, Frederic Chevallier, Philippe Ciais, Philippe Bousquet, Marielle Saunois, Bo Zheng, John Worden, A. Anthony Bloom, Robert J. Parker, Daniel J. Jacob, Edward J. Dlugokencky, and Christian Frankenberg
Atmos. Chem. Phys., 21, 12631–12647, https://doi.org/10.5194/acp-21-12631-2021, https://doi.org/10.5194/acp-21-12631-2021, 2021
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The growth of methane, the second-most important anthropogenic greenhouse gas after carbon dioxide, has been accelerating in recent years. Using an ensemble of multi-tracer atmospheric inversions constrained by surface or satellite observations, we show that global methane emissions increased by nearly 1 % per year from 2010–2017, with leading contributions from the tropics and East Asia.
Luke Surl, Tjarda Roberts, and Slimane Bekki
Atmos. Chem. Phys., 21, 12413–12441, https://doi.org/10.5194/acp-21-12413-2021, https://doi.org/10.5194/acp-21-12413-2021, 2021
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Many different chemical reactions happen when the gases from a volcano mix with air, but what effects do they have? We present aircraft measurements which show that there is less ozone within the plume of Etna than outside it. We have also made a computer model of this chemistry. This model can reproduce the effects seen when halogens (bromine and chlorine) are included in the volcanic emissions.
We look closely at the simulation to discover how complicated halogen reactions cause ozone loss.
Claire Lamotte, Jonathan Guth, Virginie Marécal, Martin Cussac, Paul David Hamer, Nicolas Theys, and Philipp Schneider
Atmos. Chem. Phys., 21, 11379–11404, https://doi.org/10.5194/acp-21-11379-2021, https://doi.org/10.5194/acp-21-11379-2021, 2021
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Improvements are made in a global chemical transfer model by considering a new volcanic SO2 emissions inventory, with more volcanoes referenced and more information on the altitude of injection. Better constraining volcanic emissions with this inventory improves the global, but mostly local, tropospheric sulfur composition. The tropospheric sulfur budget shows a nonlinearity to the volcanic contribution, especially to the sulfate aerosol burden and sulfur wet deposition.
Simon Rosanka, Bruno Franco, Lieven Clarisse, Pierre-François Coheur, Andrea Pozzer, Andreas Wahner, and Domenico Taraborrelli
Atmos. Chem. Phys., 21, 11257–11288, https://doi.org/10.5194/acp-21-11257-2021, https://doi.org/10.5194/acp-21-11257-2021, 2021
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The strong El Niño in 2015 led to a particular dry season in Indonesia and favoured severe peatland fires. The smouldering conditions of these fires and the high carbon content of peat resulted in high volatile organic compound (VOC) emissions. By using a comprehensive atmospheric model, we show that these emissions have a significant impact on the tropospheric composition and oxidation capacity. These emissions are transported into to the lower stratosphere, resulting in a depletion of ozone.
Jianfeng Li, Yuhang Wang, Ruixiong Zhang, Charles Smeltzer, Andrew Weinheimer, Jay Herman, K. Folkert Boersma, Edward A. Celarier, Russell W. Long, James J. Szykman, Ruben Delgado, Anne M. Thompson, Travis N. Knepp, Lok N. Lamsal, Scott J. Janz, Matthew G. Kowalewski, Xiong Liu, and Caroline R. Nowlan
Atmos. Chem. Phys., 21, 11133–11160, https://doi.org/10.5194/acp-21-11133-2021, https://doi.org/10.5194/acp-21-11133-2021, 2021
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Comprehensive evaluations of simulated diurnal cycles of NO2 and NOy concentrations, vertical profiles, and tropospheric vertical column densities at two different resolutions with various measurements during the DISCOVER-AQ 2011 campaign show potential distribution biases of NOx emissions in the National Emissions Inventory 2011 at both 36 and 4 km resolutions, providing another possible explanation for the overestimation of model results.
Roman Nuterman, Alexander Mahura, Alexander Baklanov, Bjarne Amstrup, and Ashraf Zakey
Atmos. Chem. Phys., 21, 11099–11112, https://doi.org/10.5194/acp-21-11099-2021, https://doi.org/10.5194/acp-21-11099-2021, 2021
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The street air pollution is usually higher than the pollution at regional and urban scales. It mostly associated with both local emission sources and urban weather conditions. We present the downscaling system for regional, subregional-urban and street scales and evaluate it for acute air-pollution episode. Its evaluation showed a good prediction score across various spatiotemporal scales as well as feasibility of deterministic modelling approach for the operational street scale forecasting.
Min Huang, James H. Crawford, Joshua P. DiGangi, Gregory R. Carmichael, Kevin W. Bowman, Sujay V. Kumar, and Xiwu Zhan
Atmos. Chem. Phys., 21, 11013–11040, https://doi.org/10.5194/acp-21-11013-2021, https://doi.org/10.5194/acp-21-11013-2021, 2021
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This study evaluates the impact of satellite soil moisture data assimilation on modeled weather and ozone fields at various altitudes above the southeastern US during the summer. It emphasizes the importance of soil moisture in the understanding of surface ozone pollution and upper tropospheric chemistry, as well as air pollutants’ source–receptor relationships between the US and its downwind areas.
Yingnan Zhang, Likun Xue, William P. L. Carter, Chenglei Pei, Tianshu Chen, Jiangshan Mu, Yujun Wang, Qingzhu Zhang, and Wenxing Wang
Atmos. Chem. Phys., 21, 11053–11068, https://doi.org/10.5194/acp-21-11053-2021, https://doi.org/10.5194/acp-21-11053-2021, 2021
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We developed the localized incremental reactivity (IR) for VOCs in a Chinese megacity and elucidated their applications in calculating the ozone formation potential (OFP). The IR scales showed a strong dependence on chemical mechanisms. Both emission- and observation-based inputs are suitable for the MIR calculation but not the case under mixed-limited or NOx-limited O3 formation regimes. We provide suggestions for the application of IR and OFP scales to aid in VOC control in China.
Ilaria D'Elia, Gino Briganti, Lina Vitali, Antonio Piersanti, Gaia Righini, Massimo D'Isidoro, Andrea Cappelletti, Mihaela Mircea, Mario Adani, Gabriele Zanini, and Luisella Ciancarella
Atmos. Chem. Phys., 21, 10825–10849, https://doi.org/10.5194/acp-21-10825-2021, https://doi.org/10.5194/acp-21-10825-2021, 2021
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We present an analysis of modelled trends of PM10, NO2, and O3 airborne concentrations over the Italian territory in 2003–2010. Our analysis shows a general downward simulated trend for all pollutants, with good agreement between observed and modelled values and the model widening both coverage and significance of air concentration trends. Due to the complex atmospheric dynamics, emission reductions do not always result in decreasing concentrations, especially for secondary pollutants.
Chris Wilson, Martyn P. Chipperfield, Manuel Gloor, Robert J. Parker, Hartmut Boesch, Joey McNorton, Luciana V. Gatti, John B. Miller, Luana S. Basso, and Sarah A. Monks
Atmos. Chem. Phys., 21, 10643–10669, https://doi.org/10.5194/acp-21-10643-2021, https://doi.org/10.5194/acp-21-10643-2021, 2021
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Methane (CH4) is an important greenhouse gas emitted from wetlands like those found in the basin of the Amazon River. Using an atmospheric model and observations from GOSAT, we quantified CH4 emissions from Amazonia during the previous decade. We found that the largest emissions came from a region in the eastern basin and that emissions there were rising faster than in other areas of South America. This finding was supported by CH4 observations made on aircraft within the basin.
Zhenze Liu, Ruth M. Doherty, Oliver Wild, Michael Hollaway, and Fiona M. O’Connor
Atmos. Chem. Phys., 21, 10689–10706, https://doi.org/10.5194/acp-21-10689-2021, https://doi.org/10.5194/acp-21-10689-2021, 2021
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Surface ozone (O3) has become the main cause of atmospheric pollution in the summertime in China since 2013. We find that 70 % reductions in NOx emissions are required to reduce O3 pollution in most of industrial regions of China, and controls in VOC emissions are very important. The new chemical scheme developed for a global chemistry–climate model not only captures the regional air pollution but also benefits the future studies of regional air-quality–climate interactions.
Peng Wang, Juanyong Shen, Men Xia, Shida Sun, Yanli Zhang, Hongliang Zhang, and Xinming Wang
Atmos. Chem. Phys., 21, 10347–10356, https://doi.org/10.5194/acp-21-10347-2021, https://doi.org/10.5194/acp-21-10347-2021, 2021
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Ozone (O3) pollution has received extensive attention due to worsening air quality and rising health risks. The Chinese National Day holiday (CNDH), which is associated with intensive commercial and tourist activities, serves as a valuable experiment to evaluate the O3 response during the holiday. We find sharply increasing trends of observed O3 concentrations throughout China during the CNDH, leading to 33 % additional total daily deaths.
Johannes G. M. Barten, Laurens N. Ganzeveld, Gert-Jan Steeneveld, and Maarten C. Krol
Atmos. Chem. Phys., 21, 10229–10248, https://doi.org/10.5194/acp-21-10229-2021, https://doi.org/10.5194/acp-21-10229-2021, 2021
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We present an evaluation of ocean and snow/ice O3 deposition in explaining observed hourly surface O3 at 25 pan-Arctic sites using an atmospheric meteorology/chemistry model. The model includes a mechanistic representation of ocean O3 deposition as a function of ocean biogeochemical and mixing conditions. The mechanistic representation agrees better with O3 observations in terms of magnitude and temporal variability especially in the High Arctic (> 70° N).
Stefanie Falk, Ane Victoria Vollsnes, Aud Eriksen, Frode Stordal, and Terje Koren Berntsen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-527, https://doi.org/10.5194/acp-2021-527, 2021
Revised manuscript accepted for ACP
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We evaluate regional and global models for ozone modeling and damage risk mapping of vegetation over subarctic Europe. Our analysis suggests that low-resolution global models do not reproduce the observed ozone seasonal cycle at ground level underestimating ozone by 30–50 %. High-resolution regional models capture the seasonal cycle well still underestimating ozone by up to 20 %. Our proposed gap-filling method for site observations shows a 78 % accuracy compared to the regional model (73 %).
Simon Rosanka, Rolf Sander, Bruno Franco, Catherine Wespes, Andreas Wahner, and Domenico Taraborrelli
Atmos. Chem. Phys., 21, 9909–9930, https://doi.org/10.5194/acp-21-9909-2021, https://doi.org/10.5194/acp-21-9909-2021, 2021
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In-cloud destruction of ozone depends on hydroperoxyl radicals in cloud droplets, where they are produced by oxygenated volatile organic compound (OVOC) oxygenation. Only rudimentary representations of these processes, if any, are currently available in global atmospheric models. By using a comprehensive atmospheric model that includes a complex in-cloud OVOC oxidation scheme, we show that atmospheric oxidants are reduced and models ignoring this process will underpredict clouds as ozone sinks.
Brad Weir, Lesley E. Ott, George J. Collatz, Stephan R. Kawa, Benjamin Poulter, Abhishek Chatterjee, Tomohiro Oda, and Steven Pawson
Atmos. Chem. Phys., 21, 9609–9628, https://doi.org/10.5194/acp-21-9609-2021, https://doi.org/10.5194/acp-21-9609-2021, 2021
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We present a collection of carbon surface fluxes, the Low-order Flux Inversion (LoFI), derived from satellite observations of the Earth's surface and calibrated to match long-term inventories and atmospheric and oceanic records. Simulations using LoFI reproduce background atmospheric carbon dioxide measurements with comparable skill to the leading surface flux products. Available both retrospectively and as a forecast, LoFI enables the study of the carbon cycle as it occurs.
Ilya Stanevich, Dylan B. A. Jones, Kimberly Strong, Martin Keller, Daven K. Henze, Robert J. Parker, Hartmut Boesch, Debra Wunch, Justus Notholt, Christof Petri, Thorsten Warneke, Ralf Sussmann, Matthias Schneider, Frank Hase, Rigel Kivi, Nicholas M. Deutscher, Voltaire A. Velazco, Kaley A. Walker, and Feng Deng
Atmos. Chem. Phys., 21, 9545–9572, https://doi.org/10.5194/acp-21-9545-2021, https://doi.org/10.5194/acp-21-9545-2021, 2021
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We explore the utility of a weak-constraint (WC) four-dimensional variational (4D-Var) data assimilation scheme for mitigating systematic errors in methane simulation in the GEOS-Chem model. We use data from the Greenhouse Gases Observing Satellite (GOSAT) and show that, compared to the traditional 4D-Var approach, the WC scheme improves the agreement between the model and independent observations. We find that the WC corrections to the model provide insight into the source of the errors.
Yosuke Niwa, Yousuke Sawa, Hideki Nara, Toshinobu Machida, Hidekazu Matsueda, Taku Umezawa, Akihiko Ito, Shin-Ichiro Nakaoka, Hiroshi Tanimoto, and Yasunori Tohjima
Atmos. Chem. Phys., 21, 9455–9473, https://doi.org/10.5194/acp-21-9455-2021, https://doi.org/10.5194/acp-21-9455-2021, 2021
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Fires in Equatorial Asia release a large amount of carbon into the atmosphere. Extensively using high-precision atmospheric carbon dioxide (CO2) data from a commercial aircraft observation project, we estimated fire carbon emissions in Equatorial Asia induced by the big El Niño event in 2015. Additional shipboard measurement data elucidated the validity of the analysis and the best estimate indicated 273 Tg C for fire emissions during September–October 2015.
Christine Frömming, Volker Grewe, Sabine Brinkop, Patrick Jöckel, Amund S. Haslerud, Simon Rosanka, Jesper van Manen, and Sigrun Matthes
Atmos. Chem. Phys., 21, 9151–9172, https://doi.org/10.5194/acp-21-9151-2021, https://doi.org/10.5194/acp-21-9151-2021, 2021
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The influence of weather situations on non-CO2 aviation climate impact is investigated to identify systematic weather-related sensitivities. If aircraft avoid the most sensitive areas, climate impact might be reduced. Enhanced significance is found for emission in relation to high-pressure systems, jet stream, polar night, and tropopause altitude. The results represent a comprehensive data set for studies aiming at weather-dependent flight trajectory optimization to reduce total climate impact.
Jianing Dai and Tao Wang
Atmos. Chem. Phys., 21, 8747–8759, https://doi.org/10.5194/acp-21-8747-2021, https://doi.org/10.5194/acp-21-8747-2021, 2021
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We used the WRF–Chem model with the latest HONO and ClNO2 processes to investigate their effects on the concentrations of ROx radicals, O3, and PM2.5 in Asia during summer. The results show that the ship-derived HONO and ClNO2 increased the ROx radical concentration by 2–3 times and subsequently increased the O3 and PM2.5 concentrations in marine areas. These findings indicate the importance of these nitrogen processes in the evaluation of the impact of ship emissions on air quality.
Anoop S. Mahajan, Qinyi Li, Swaleha Inamdar, Kirpa Ram, Alba Badia, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 21, 8437–8454, https://doi.org/10.5194/acp-21-8437-2021, https://doi.org/10.5194/acp-21-8437-2021, 2021
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Using a regional model, we show that iodine-catalysed reactions cause large regional changes in the chemical composition in the northern Indian Ocean, with peak changes of up to 25 % in O3, 50 % in nitrogen oxides (NO and NO2), 15 % in hydroxyl radicals (OH), 25 % in hydroperoxyl radicals (HO2), and up to a 50 % change in the nitrate radical (NO3). These results show the importance of including iodine chemistry in modelling the atmosphere in this region.
Maximilian Herrmann, Holger Sihler, Udo Frieß, Thomas Wagner, Ulrich Platt, and Eva Gutheil
Atmos. Chem. Phys., 21, 7611–7638, https://doi.org/10.5194/acp-21-7611-2021, https://doi.org/10.5194/acp-21-7611-2021, 2021
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Time-dependent 3D numerical simulations of tropospheric bromine release and ozone depletion events (ODEs) in the Arctic polar spring of 2009 are compared to observations. Simulation results agree well with the observations at both Utqiaġvik, Alaska, and at Summit, Greenland. In a parameter study, different settings for the bromine release mechanism are evaluated. An enhancement of the bromine release mechanism improves the agreement regarding the occurrence of ODEs with the observations.
Ashok K. Luhar, Ian E. Galbally, Matthew T. Woodhouse, and Nathan Luke Abraham
Atmos. Chem. Phys., 21, 7053–7082, https://doi.org/10.5194/acp-21-7053-2021, https://doi.org/10.5194/acp-21-7053-2021, 2021
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Lightning-generated nitrogen oxides (LNOx) greatly influence tropospheric photochemistry. The most common parameterisation of lightning flash rate used to calculate LNOx in global composition models underestimates measurements over the ocean by a factor of 20–25. We formulate and validate an alternative parameterisation to remedy this problem. The new scheme causes an increase in the ozone burden by 8.5 % and the hydroxyl radical by 13 %, and these have implications for climate and air quality.
Daniel M. Westervelt, Arlene M. Fiore, Colleen B. Baublitz, and Gustavo Correa
Atmos. Chem. Phys., 21, 6799–6810, https://doi.org/10.5194/acp-21-6799-2021, https://doi.org/10.5194/acp-21-6799-2021, 2021
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Particulate air pollution in the atmosphere can impact the availability of gas-phase chemical constituents, which can then have feedbacks on gas-phase air pollutants. We use a chemistry–climate computer model to simulate the impact of particulate pollution from three major world regions on gas-phase chemical constituents. We find that surface-level ozone air pollution decreases by up to 5 ppbv over China in response to Chinese particulate air pollution, which has implications for policy.
Gabriel Isaacman-VanWertz and Bernard Aumont
Atmos. Chem. Phys., 21, 6541–6563, https://doi.org/10.5194/acp-21-6541-2021, https://doi.org/10.5194/acp-21-6541-2021, 2021
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There are tens of thousands of different chemical compounds in the atmosphere. To tackle this complexity, there are a wide range of different methods to estimate their physical and chemical properties. We use these methods to understand how much the detailed structure of a molecule impacts its properties, and the extent to which properties can be estimated without knowing this level of detail. We find that structure matters, but methods lacking that level of detail still perform reasonably well.
Daniel C. Anderson, Bryan N. Duncan, Arlene M. Fiore, Colleen B. Baublitz, Melanie B. Follette-Cook, Julie M. Nicely, and Glenn M. Wolfe
Atmos. Chem. Phys., 21, 6481–6508, https://doi.org/10.5194/acp-21-6481-2021, https://doi.org/10.5194/acp-21-6481-2021, 2021
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We demonstrate that large-scale climate features are the primary driver of year-to-year variability in simulated values of the hydroxyl radical, the primary atmospheric oxidant, over 1980–2018. The El Niño–Southern Oscillation is the dominant mode of hydroxyl variability, resulting in large-scale global decreases in OH during El Niño events. Other climate modes, such as the Australian monsoon and the North Atlantic Oscillation, have impacts of similar magnitude but on on more localized scales.
Pooja V. Pawar, Sachin D. Ghude, Chinmay Jena, Andrea Móring, Mark A. Sutton, Santosh Kulkarni, Deen Mani Lal, Divya Surendran, Martin Van Damme, Lieven Clarisse, Pierre-François Coheur, Xuejun Liu, Gaurav Govardhan, Wen Xu, Jize Jiang, and Tapan Kumar Adhya
Atmos. Chem. Phys., 21, 6389–6409, https://doi.org/10.5194/acp-21-6389-2021, https://doi.org/10.5194/acp-21-6389-2021, 2021
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In this study, simulations of atmospheric ammonia (NH3) with MOZART-4 and HTAP-v2 are compared with satellite (IASI) and ground-based measurements to understand the spatial and temporal variability of NH3 over two emission hotspot regions of Asia, the IGP and the NCP. Our simulations indicate that the formation of ammonium aerosols is quicker over the NCP than the IGP, leading to smaller NH3 columns over the higher NH3-emitting NCP compared to the IGP region for comparable emissions.
Yan Zhang, Yu Zhao, Meng Gao, Xin Bo, and Chris P. Nielsen
Atmos. Chem. Phys., 21, 6411–6430, https://doi.org/10.5194/acp-21-6411-2021, https://doi.org/10.5194/acp-21-6411-2021, 2021
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We combined air quality and exposure response models to analyze the benefits for air quality and human health of China’s ultra-low emission policy in one of its most developed regions. Atmospheric observations and the air quality model were also used to demonstrate improvement of emission inventories incorporating online emission monitoring data. With implementation of the policy in both power and industrial sectors, the attributable deaths due to PM2.5 exposure are estimated to decrease 5.5 %.
Anna Karion, Israel Lopez-Coto, Sharon M. Gourdji, Kimberly Mueller, Subhomoy Ghosh, William Callahan, Michael Stock, Elizabeth DiGangi, Steve Prinzivalli, and James Whetstone
Atmos. Chem. Phys., 21, 6257–6273, https://doi.org/10.5194/acp-21-6257-2021, https://doi.org/10.5194/acp-21-6257-2021, 2021
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Estimating city emissions based on atmospheric observations requires that the portion of observed greenhouse gases that originated in the city be separated from the portion that originated outside the city, also known as the background concentration. Here, we investigate different methods to determine background concentrations for the Washington, DC, and Baltimore, MD, region and evaluate how well those methods work and the uncertainties they involve.
Kun Zhang, Ling Huang, Qing Li, Juntao Huo, Yusen Duan, Yuhang Wang, Elly Yaluk, Yangjun Wang, Qingyan Fu, and Li Li
Atmos. Chem. Phys., 21, 5905–5917, https://doi.org/10.5194/acp-21-5905-2021, https://doi.org/10.5194/acp-21-5905-2021, 2021
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Recently, high O3 concentrations were frequently observed in rural areas of the Yangtze River Delta (YRD) region under stagnant conditions. Using an online measurement and observation-based model, we investigated the budget of ROx radicals and the influence of isoprene chemistry on O3 formation. Our results underline that isoprene chemistry in the rural atmosphere becomes important with the participation of anthropogenic NOx.
Bharat Rastogi, John B. Miller, Micheal Trudeau, Arlyn E. Andrews, Lei Hu, Marikate Mountain, Thomas Nehrkorn, John Mund, Kaiyu Guan, and Caroline B. Alden
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-299, https://doi.org/10.5194/acp-2021-299, 2021
Revised manuscript accepted for ACP
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Predicting Earth's climate is difficult partly due to uncertainty in forecasting how much CO2 can be removed by oceans and plants, because we cannot measure these exchanges directly on large scales. Satellites such as NASA's OCO-2 can provide part of the needed information, but data need to be highly precise and accurate. We evaluate these data and find small biases in certain months that are similar to the signals of interest. We argue that continued improvement in these data is necessary.
Ioanna Skoulidou, Maria-Elissavet Koukouli, Astrid Manders, Arjo Segers, Dimitris Karagkiozidis, Myrto Gratsea, Dimitris Balis, Alkiviadis Bais, Evangelos Gerasopoulos, Trisevgeni Stavrakou, Jos van Geffen, Henk Eskes, and Andreas Richter
Atmos. Chem. Phys., 21, 5269–5288, https://doi.org/10.5194/acp-21-5269-2021, https://doi.org/10.5194/acp-21-5269-2021, 2021
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The performance of LOTOS-EUROS v2.2.001 regional chemical transport model NO2 simulations is investigated over Greece from June to December 2018. Comparison with in situ NO2 measurements shows a spatial correlation coefficient of 0.86, while the model underestimates the concentrations mostly during daytime (12 to 15:00 local time). Further, the simulated tropospheric NO2 columns are evaluated against ground-based MAX-DOAS NO2 measurements and S5P/TROPOMI observations for July and December 2018.
Karl M. Seltzer, Elyse Pennington, Venkatesh Rao, Benjamin N. Murphy, Madeleine Strum, Kristin K. Isaacs, and Havala O. T. Pye
Atmos. Chem. Phys., 21, 5079–5100, https://doi.org/10.5194/acp-21-5079-2021, https://doi.org/10.5194/acp-21-5079-2021, 2021
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Volatile chemical products (VCPs) are an increasingly important source of anthropogenic reactive organic carbon emissions. Here, we develop VCPy, a new framework to model organic emissions from VCPs throughout the United States. At the national-level, VCPy emissions are broadly consistent with the US EPA’s 2017 National Emission Inventory, however county-level and categorical estimates can differ substantially. An observational evaluation indicates high fidelity in the methods employed here.
Stijn Naus, Stephen A. Montzka, Prabir K. Patra, and Maarten C. Krol
Atmos. Chem. Phys., 21, 4809–4824, https://doi.org/10.5194/acp-21-4809-2021, https://doi.org/10.5194/acp-21-4809-2021, 2021
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Following up on previous box model studies, we employ a 3D transport model to estimate variations in the hydroxyl radical (OH) from observations of methyl chloroform (MCF). We derive small interannual OH variations that are consistent with variations in the El Niño–Southern Oscillation. We also find evidence for the release of MCF from oceans in atmospheric gradients of MCF. Both findings highlight the added value of a 3D transport model since box model studies did not identify these effects.
Ian Enting and Nathan Clisby
Atmos. Chem. Phys., 21, 4699–4708, https://doi.org/10.5194/acp-21-4699-2021, https://doi.org/10.5194/acp-21-4699-2021, 2021
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We provide a new framework for comparing short-lived greenhouse gases to long-lived greenhouse gases such as carbon dioxide using methane as an example. This can clarify the differences between various proposals that have been introduced in order to overcome the use of global warming potentials as a measure of greenhouse gas equivalence.
Thomas Thorp, Stephen R. Arnold, Richard J. Pope, Dominick V. Spracklen, Luke Conibear, Christoph Knote, Mikhail Arshinov, Boris Belan, Eija Asmi, Tuomas Laurila, Andrei I. Skorokhod, Tuomo Nieminen, and Tuukka Petäjä
Atmos. Chem. Phys., 21, 4677–4697, https://doi.org/10.5194/acp-21-4677-2021, https://doi.org/10.5194/acp-21-4677-2021, 2021
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We compare modelled near-surface pollutants with surface and satellite observations to better understand the controls on the regional concentrations of pollution in western Siberia for late spring and summer in 2011. We find two commonly used emission inventories underestimate human emissions when compared to observations. Transport emissions are the main source of pollutants within the region during this period, whilst fire emissions peak during June and are only significant south of 60° N.
Nikolaos Evangeliou, Yves Balkanski, Sabine Eckhardt, Anne Cozic, Martin Van Damme, Pierre-François Coheur, Lieven Clarisse, Mark W. Shephard, Karen E. Cady-Pereira, and Didier Hauglustaine
Atmos. Chem. Phys., 21, 4431–4451, https://doi.org/10.5194/acp-21-4431-2021, https://doi.org/10.5194/acp-21-4431-2021, 2021
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Ammonia, a substance that has played a key role in sustaining life, has been increasing in the atmosphere, affecting climate and humans. Understanding the reasons for this increase is important for the beneficial use of ammonia. The evolution of satellite products gives us the opportunity to calculate ammonia emissions easier. We calculated global ammonia emissions over the last 10 years, incorporated them into a chemistry model and recorded notable improvement in reproducing observations.
Tie Dai, Yueming Cheng, Daisuke Goto, Yingruo Li, Xiao Tang, Guangyu Shi, and Teruyuki Nakajima
Atmos. Chem. Phys., 21, 4357–4379, https://doi.org/10.5194/acp-21-4357-2021, https://doi.org/10.5194/acp-21-4357-2021, 2021
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The anthropogenic emission of sulfur dioxide (SO2) over China has significantly declined as a consequence of the clean air actions. We have developed a new emission inversion system to dynamically update the SO2 emission grid by grid over China by assimilating ground-based SO2 observations. The inverted SO2 emission over China in November 2016 on average had declined by 49.4 % since 2010, which is well in agreement with the bottom-up estimation of 48.0 %.
Paul T. Griffiths, Lee T. Murray, Guang Zeng, Youngsub Matthew Shin, N. Luke Abraham, Alexander T. Archibald, Makoto Deushi, Louisa K. Emmons, Ian E. Galbally, Birgit Hassler, Larry W. Horowitz, James Keeble, Jane Liu, Omid Moeini, Vaishali Naik, Fiona M. O'Connor, Naga Oshima, David Tarasick, Simone Tilmes, Steven T. Turnock, Oliver Wild, Paul J. Young, and Prodromos Zanis
Atmos. Chem. Phys., 21, 4187–4218, https://doi.org/10.5194/acp-21-4187-2021, https://doi.org/10.5194/acp-21-4187-2021, 2021
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We analyse the CMIP6 Historical and future simulations for tropospheric ozone, a species which is important for many aspects of atmospheric chemistry. We show that the current generation of models agrees well with observations, being particularly successful in capturing trends in surface ozone and its vertical distribution in the troposphere. We analyse the factors that control ozone and show that they evolve over the period of the CMIP6 experiments.