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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Qingyang Xiao, Guannan Geng, Shigan Liu, Jiajun Liu, Xia Meng, and Qiang Zhang
EGUsphere, https://doi.org/10.48550/arXiv.2203.07591, https://doi.org/10.48550/arXiv.2203.07591, 2022
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We provided complete coverage PM2.5 concentration at a 1-km resolution from 2000 to the present that carefully considered the significant changes in land-use characteristics in China. This high-resolution PM2.5 data sucessfully revealed the local scale PM2.5 variations. We noticed changes in PM2.5 spatial patterns in association with the clean air policies that the pollution hotspots have transferred from urban centers to rural regions with limited air quality monitoring.
John R. Worden, Daniel H. Cusworth, Zhen Qu, Yi Yin, Yuzhong Zhang, A. Anthony Bloom, Shuang Ma, Brendan K. Byrne, Tia Scarpelli, Joannes D. Maasakkers, David Crisp, Riley Duren, and Daniel J. Jacob
Atmos. Chem. Phys., 22, 6811–6841, https://doi.org/10.5194/acp-22-6811-2022, https://doi.org/10.5194/acp-22-6811-2022, 2022
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This paper is intended to accomplish two goals: 1) describe a new algorithm by which remotely sensed measurements of methane or other tracers can be used to not just quantify methane fluxes, but also attribute these fluxes to specific sources and regions and characterize their uncertainties, and 2) use this new algorithm to provide methane emissions by sector and country in support of the global stock take.
Thibaud M. Fritz, Sebastian D. Eastham, Louisa K. Emmons, Haipeng Lin, Elizabeth W. Lundgren, Steve Goldhaber, Steven R. H. Barrett, and Daniel J. Jacob
EGUsphere, https://doi.org/10.5194/egusphere-2022-226, https://doi.org/10.5194/egusphere-2022-226, 2022
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We bring the state-of-the-science chemistry module GEOS-Chem into the Community Earth System Model (CESM). We show that some known differences between results from GEOS-Chem and CESM’s CAM-chem chemistry module may be due to the configuration of model meteorology rather than inherent differences in the model chemistry. This is a significant step towards a truly modular ESM and allows two strong but currently separate research communities to benefit from each other’s advances.
Tia R. Scarpelli, Daniel J. Jacob, Shayna Grossman, Xiao Lu, Zhen Qu, Melissa P. Sulprizio, Yuzhong Zhang, Frances Reuland, Deborah Gordon, and John R. Worden
Atmos. Chem. Phys., 22, 3235–3249, https://doi.org/10.5194/acp-22-3235-2022, https://doi.org/10.5194/acp-22-3235-2022, 2022
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Drew C. Pendergrass, Shixian Zhai, Jhoon Kim, Ja-Ho Koo, Seoyoung Lee, Minah Bae, Soontae Kim, Hong Liao, and Daniel J. Jacob
Atmos. Meas. Tech., 15, 1075–1091, https://doi.org/10.5194/amt-15-1075-2022, https://doi.org/10.5194/amt-15-1075-2022, 2022
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This paper uses a machine learning algorithm to infer high-resolution maps of particulate air quality in eastern China, Japan, and the Korean peninsula, using data from a geostationary satellite along with meteorology. We then perform an extensive evaluation of this inferred air quality and use it to diagnose trends in the region. We hope this paper and the associated data will be valuable to other scientists interested in epidemiology, air quality, remote sensing, and machine learning.
Lu Shen, Daniel J. Jacob, Mauricio Santillana, Kelvin Bates, Jiawei Zhuang, and Wei Chen
Geosci. Model Dev., 15, 1677–1687, https://doi.org/10.5194/gmd-15-1677-2022, https://doi.org/10.5194/gmd-15-1677-2022, 2022
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The high computational cost of chemical integration is a long-standing limitation in global atmospheric chemistry models. Here we present an adaptive and efficient algorithm that can reduce the computational time of atmospheric chemistry by 50 % and maintain the error below 2 % for important species, inspired by machine learning clustering techniques and traditional asymptotic analysis ideas.
Randall V. Martin, Sebastian D. Eastham, Liam Bindle, Elizabeth W. Lundgren, Thomas L. Clune, Christoph A. Keller, William Downs, Dandan Zhang, Robert A. Lucchesi, Melissa P. Sulprizio, Robert M. Yantosca, Yanshun Li, Lucas Estrada, William M. Putman, Benjamin M. Auer, Atanas L. Trayanov, Steven Pawson, and Daniel J. Jacob
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2022-42, https://doi.org/10.5194/gmd-2022-42, 2022
Preprint under review for GMD
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Atmospheric chemistry models must be able to operate both online as components of Earth system models and offline as stand-alone models. The widely-used GEOS-Chem model operates both online and offline, but the classic offline version is not suitable for massively parallel simulations. We describe a new generation of the off-line high-performance GEOS-Chem (GCHP) that enables high-resolution simulations on thousands of cores including on the cloud with improved access, performance, and accuracy.
Xiao Lu, Daniel J. Jacob, Haolin Wang, Joannes D. Maasakkers, Yuzhong Zhang, Tia R. Scarpelli, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Hannah Nesser, A. Anthony Bloom, Shuang Ma, John R. Worden, Shaojia Fan, Robert J. Parker, Hartmut Boesch, Ritesh Gautam, Deborah Gordon, Michael D. Moran, Frances Reuland, Claudia A. Octaviano Villasana, and Arlyn Andrews
Atmos. Chem. Phys., 22, 395–418, https://doi.org/10.5194/acp-22-395-2022, https://doi.org/10.5194/acp-22-395-2022, 2022
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We evaluate methane emissions and trends for 2010–2017 in the gridded national emission inventories for the United States, Canada, and Mexico by inversion of in situ and satellite methane observations. We find that anthropogenic methane emissions for all three countries are underestimated in the national inventories, largely driven by oil emissions. Anthropogenic methane emissions in the US peak in 2014, in contrast to the report of a steadily decreasing trend over 2010–2017 from the US EPA.
Kelvin H. Bates, Daniel J. Jacob, Ke Li, Peter D. Ivatt, Mat J. Evans, Yingying Yan, and Jintai Lin
Atmos. Chem. Phys., 21, 18351–18374, https://doi.org/10.5194/acp-21-18351-2021, https://doi.org/10.5194/acp-21-18351-2021, 2021
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Simple aromatic compounds (benzene, toluene, xylene) have complex gas-phase chemistry that is inconsistently represented in atmospheric models. We compile recent experimental and theoretical insights to develop a new mechanism for gas-phase aromatic oxidation that is sufficiently compact for use in multiscale models. We compare our new mechanism to chamber experiments and other mechanisms, and implement it in a global model to quantify the impacts of aromatic oxidation on tropospheric chemistry.
Sabour Baray, Daniel J. Jacob, Joannes D. Maasakkers, Jian-Xiong Sheng, Melissa P. Sulprizio, Dylan B. A. Jones, A. Anthony Bloom, and Robert McLaren
Atmos. Chem. Phys., 21, 18101–18121, https://doi.org/10.5194/acp-21-18101-2021, https://doi.org/10.5194/acp-21-18101-2021, 2021
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We use 2010–2015 surface and satellite observations to disentangle methane from anthropogenic and natural sources in Canada. Using a chemical transport model (GEOS-Chem), the mismatch between modelled and observed methane concentrations can be used to infer emissions according to Bayesian statistics. Compared to prior knowledge, we show higher anthropogenic emissions attributed to energy and/or agriculture in Western Canada and lower natural emissions from Boreal wetlands.
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., 21, 17995–18010, https://doi.org/10.5194/acp-21-17995-2021, https://doi.org/10.5194/acp-21-17995-2021, 2021
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Photochemical pollution over the North China Plain (NCP) is attracting much concern. Our observations at a rural site in the NCP identified high peroxyacetyl nitrate (PAN) concentrations, even on cold days. Increased acetaldehyde concentration and hydroxyl radical production rates 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 after summer over the NCP.
Shixian Zhai, Daniel J. Jacob, Jared F. Brewer, Ke Li, Jonathan M. Moch, Jhoon Kim, Seoyoung Lee, Hyunkwang Lim, Hyun Chul Lee, Su Keun Kuk, Rokjin J. Park, Jaein I. Jeong, Xuan Wang, Pengfei Liu, Gan Luo, Fangqun Yu, Jun Meng, Randall V. Martin, Katherine R. Travis, Johnathan W. Hair, Bruce E. Anderson, Jack E. Dibb, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jung-Hun Woo, Younha Kim, Qiang Zhang, and Hong Liao
Atmos. Chem. Phys., 21, 16775–16791, https://doi.org/10.5194/acp-21-16775-2021, https://doi.org/10.5194/acp-21-16775-2021, 2021
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Geostationary satellite aerosol optical depth (AOD) has tremendous potential for monitoring surface fine particulate matter (PM2.5). Our study explored the physical relationship between AOD and PM2.5 by integrating data from surface networks, aircraft, and satellites with the GEOS-Chem chemical transport model. We quantitatively showed that accurate simulation of aerosol size distributions, boundary layer depths, relative humidity, coarse particles, and diurnal variations in PM2.5 are essential.
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., 21, 16051–16065, https://doi.org/10.5194/acp-21-16051-2021, https://doi.org/10.5194/acp-21-16051-2021, 2021
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In this study, we use a 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 pollutant concentration but also bring significant co-benefits in air quality to downwind regions. The benefits for the improved air pollution are dominated by PM2.5.
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., 21, 15199–15211, https://doi.org/10.5194/acp-21-15199-2021, https://doi.org/10.5194/acp-21-15199-2021, 2021
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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 that 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.
Liam Bindle, Randall V. Martin, Matthew J. Cooper, Elizabeth W. Lundgren, Sebastian D. Eastham, Benjamin M. Auer, Thomas L. Clune, Hongjian Weng, Jintai Lin, Lee T. Murray, Jun Meng, Christoph A. Keller, William M. Putman, Steven Pawson, and Daniel J. Jacob
Geosci. Model Dev., 14, 5977–5997, https://doi.org/10.5194/gmd-14-5977-2021, https://doi.org/10.5194/gmd-14-5977-2021, 2021
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Atmospheric chemistry models like GEOS-Chem are versatile tools widely used in air pollution and climate studies. The simulations used in such studies can be very computationally demanding, and thus it is useful if the model can simulate a specific geographic region at a higher resolution than the rest of the globe. Here, we implement, test, and demonstrate a new variable-resolution capability in GEOS-Chem that is suitable for simulations conducted on supercomputers.
Zhen Qu, Daniel J. Jacob, Lu Shen, Xiao Lu, Yuzhong Zhang, Tia R. Scarpelli, Hannah Nesser, Melissa P. Sulprizio, Joannes D. Maasakkers, A. Anthony Bloom, John R. Worden, Robert J. Parker, and Alba L. Delgado
Atmos. Chem. Phys., 21, 14159–14175, https://doi.org/10.5194/acp-21-14159-2021, https://doi.org/10.5194/acp-21-14159-2021, 2021
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The recent launch of TROPOMI offers an unprecedented opportunity to quantify the methane budget from a top-down perspective. We use TROPOMI and the more mature GOSAT methane observations to estimate methane emissions and get consistent global budgets. However, TROPOMI shows biases over regions where surface albedo is small and provides less information for the coarse-resolution inversion due to the larger error correlations and spatial variations in the number of observations.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Haipeng Lin, Daniel J. Jacob, Elizabeth W. Lundgren, Melissa P. Sulprizio, Christoph A. Keller, Thibaud M. Fritz, Sebastian D. Eastham, Louisa K. Emmons, Patrick C. Campbell, Barry Baker, Rick D. Saylor, and Raffaele Montuoro
Geosci. Model Dev., 14, 5487–5506, https://doi.org/10.5194/gmd-14-5487-2021, https://doi.org/10.5194/gmd-14-5487-2021, 2021
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Emissions are a central component of atmospheric chemistry models. The Harmonized Emissions Component (HEMCO) is a software component for computing emissions from a user-selected ensemble of emission inventories and algorithms. It allows users to select, add, and scale emissions from different sources through a configuration file with no change to the model source code. We demonstrate the implementation of HEMCO in several models, all sharing the same HEMCO core code and database library.
Yi Yin, Frederic Chevallier, Philippe Ciais, Philippe Bousquet, Marielle Saunois, Bo Zheng, John Worden, A. Anthony Bloom, Robert J. Parker, Daniel J. Jacob, Edward J. Dlugokencky, and Christian Frankenberg
Atmos. Chem. Phys., 21, 12631–12647, https://doi.org/10.5194/acp-21-12631-2021, https://doi.org/10.5194/acp-21-12631-2021, 2021
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The growth of methane, the second-most important anthropogenic greenhouse gas after carbon dioxide, has been accelerating in recent years. Using an ensemble of multi-tracer atmospheric inversions constrained by surface or satellite observations, we show that global methane emissions increased by nearly 1 % per year from 2010–2017, with leading contributions from the tropics and East Asia.
Hannah Nesser, Daniel J. Jacob, Joannes D. Maasakkers, Tia R. Scarpelli, Melissa P. Sulprizio, Yuzhong Zhang, and Chris H. Rycroft
Atmos. Meas. Tech., 14, 5521–5534, https://doi.org/10.5194/amt-14-5521-2021, https://doi.org/10.5194/amt-14-5521-2021, 2021
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Analytical inversions of satellite observations of atmospheric composition can improve emissions estimates and quantify errors but are computationally expensive at high resolutions. We propose two methods to decrease this cost. The methods reproduce a high-resolution inversion at a quarter of the cost. The reduced-dimension method creates a multiscale grid. The reduced-rank method solves the inversion where information content is highest.
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
Revised manuscript not accepted
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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.
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.
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.
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.
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.
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)
Long-term regional trends of nitrogen and sulfur deposition in the United States from 2002 to 2017
Impact of urbanization on gas-phase pollutant concentrations: a regional-scale, model-based analysis of the contributing factors
Correcting ozone biases in a global chemistry–climate model: implications for future ozone
Evaluating the contribution of the unexplored photochemistry of aldehydes on the tropospheric levels of molecular hydrogen (H2)
The ozone–climate penalty over South America and Africa by 2100
An improved representation of fire non-methane organic gases (NMOGs) in models: emissions to reactivity
Impact of present and future aircraft NOx and aerosol emissions on atmospheric composition and associated direct radiative forcing of climate
Attribution of surface ozone to NOx and volatile organic compound sources during two different high ozone events
Model output statistics (MOS) applied to Copernicus Atmospheric Monitoring Service (CAMS) O3 forecasts: trade-offs between continuous and categorical skill scores
Bayesian assessment of chlorofluorocarbon (CFC), hydrochlorofluorocarbon (HCFC) and halon banks suggest large reservoirs still present in old equipment
Global and regional carbon budget for 2015–2020 inferred from OCO-2 based on an ensemble Kalman filter coupled with GEOS-Chem
Impact of a subtropical high and a typhoon on a severe ozone pollution episode in the Pearl River Delta, China
A renewed rise in global HCFC-141b emissions between 2017–2021
A model for simultaneous evaluation of NO2, O3, and PM10 pollution in urban and rural areas: handling incomplete data sets with multivariate curve resolution analysis
Technical note: Entrainment-limited kinetics of bimolecular reactions in clouds
Improving NOx emission estimates in Beijing using network observations and a perturbed emissions ensemble
Global tropospheric ozone trends, attributions, and radiative impacts in 1995–2017: an integrated analysis using aircraft (IAGOS) observations, ozonesonde, and multi-decadal chemical model simulations
Modelling the growth of atmospheric nitrous oxide using a global hierarchical inversion
Observation-based analysis of ozone production sensitivity for two persistent ozone episodes in Guangdong, China
A machine learning approach to quantify meteorological drivers of ozone pollution in China from 2015 to 2019
Discrepancy in assimilated atmospheric CO over East Asia in 2015–2020 by assimilating satellite and surface CO measurements
Potential environmental impact of bromoform from Asparagopsis farming in Australia
Satellite soil moisture data assimilation impacts on modeling weather variables and ozone in the southeastern US – Part 2: Sensitivity to dry-deposition parameterizations
The impacts of marine-emitted halogens on OH radicals in East Asia during summer
Sarah E. Benish, Jesse O. Bash, Kristen M. Foley, K. Wyat Appel, Christian Hogrefe, Robert Gilliam, and George Pouliot
Atmos. Chem. Phys., 22, 12749–12767, https://doi.org/10.5194/acp-22-12749-2022, https://doi.org/10.5194/acp-22-12749-2022, 2022
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We assess Community Multiscale Air Quality (CMAQ) model simulations of nitrogen and sulfur deposition over US climate regions to evaluate the model ability to reproduce long-term deposition trends and total deposition budgets. A measurement–model fusion technique is found to improve estimates of wet deposition. Emission controls set by the Clean Air Act successfully decreased oxidized nitrogen deposition across the US; we find increasing amounts of reduced nitrogen to the total nitrogen budget.
Peter Huszar, Jan Karlický, Lukáš Bartík, Marina Liaskoni, Alvaro Patricio Prieto Perez, and Kateřina Šindelářová
Atmos. Chem. Phys., 22, 12647–12674, https://doi.org/10.5194/acp-22-12647-2022, https://doi.org/10.5194/acp-22-12647-2022, 2022
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Urbanization turns rural land cover into artificial land cover, while due to human activities, it introduces a great quantity of emissions. We attempt to quantify the impact of urbanization on the final air pollutant levels by looking not only at these emissions, but also the way urban land cover influences meteorological conditions, how the removal of pollutants changes due to urban land cover, and how biogenic emissions from vegetation change due to less vegetation in urban areas.
Zhenze Liu, Ruth M. Doherty, Oliver Wild, Fiona M. O'Connor, and Steven T. Turnock
Atmos. Chem. Phys., 22, 12543–12557, https://doi.org/10.5194/acp-22-12543-2022, https://doi.org/10.5194/acp-22-12543-2022, 2022
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Weaknesses in process representation in chemistry–climate models lead to biases in simulating surface ozone and to uncertainty in projections of future ozone change. We develop a deep learning model to demonstrate the feasibility of ozone bias correction and show its capability in providing improved assessments of the impacts of climate and emission changes on future air quality, along with valuable information to guide future model development.
Maria Paula Pérez-Peña, Jenny A. Fisher, Dylan B. Millet, Hisashi Yashiro, Ray L. Langenfelds, Paul B. Krummel, and Scott H. Kable
Atmos. Chem. Phys., 22, 12367–12386, https://doi.org/10.5194/acp-22-12367-2022, https://doi.org/10.5194/acp-22-12367-2022, 2022
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We used two atmospheric models to test the implications of previously unexplored aldehyde photochemistry on the atmospheric levels of molecular hydrogen (H2). We showed that the new photochemistry from aldehydes produces more H2 over densely forested areas. Compared to the rest of the world, it is over these forested regions where the produced H2 is more likely to be removed. The results highlight that other processes that contribute to atmospheric H2 levels should be studied further.
Flossie Brown, Gerd A. Folberth, Stephen Sitch, Susanne Bauer, Marijn Bauters, Pascal Boeckx, Alexander W. Cheesman, Makoto Deushi, Inês Dos Santos Vieira, Corinne Galy-Lacaux, James Haywood, James Keeble, Lina M. Mercado, Fiona M. O'Connor, Naga Oshima, Kostas Tsigaridis, and Hans Verbeeck
Atmos. Chem. Phys., 22, 12331–12352, https://doi.org/10.5194/acp-22-12331-2022, https://doi.org/10.5194/acp-22-12331-2022, 2022
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Surface ozone can decrease plant productivity and impair human health. In this study, we evaluate the change in surface ozone due to climate change over South America and Africa using Earth system models. We find that if the climate were to change according to the worst-case scenario used here, models predict that forested areas in biomass burning locations and urban populations will be at increasing risk of ozone exposure, but other areas will experience a climate benefit.
Therese S. Carter, Colette L. Heald, Jesse H. Kroll, Eric C. Apel, Donald Blake, Matthew Coggon, Achim Edtbauer, Georgios Gkatzelis, Rebecca S. Hornbrook, Jeff Peischl, Eva Y. Pfannerstill, Felix Piel, Nina G. Reijrink, Akima Ringsdorf, Carsten Warneke, Jonathan Williams, Armin Wisthaler, and Lu Xu
Atmos. Chem. Phys., 22, 12093–12111, https://doi.org/10.5194/acp-22-12093-2022, https://doi.org/10.5194/acp-22-12093-2022, 2022
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Fires emit many gases which can contribute to smog and air pollution. However, the amount and properties of these chemicals are not well understood, so this work updates and expands their representation in a global atmospheric model, including by adding new chemicals. We confirm that this updated representation generally matches measurements taken in several fire regions. We then show that fires provide ~15 % of atmospheric reactivity globally and more than 75 % over fire source regions.
Etienne Terrenoire, Didier A. Hauglustaine, Yann Cohen, Anne Cozic, Richard Valorso, Franck Lefèvre, and Sigrun Matthes
Atmos. Chem. Phys., 22, 11987–12023, https://doi.org/10.5194/acp-22-11987-2022, https://doi.org/10.5194/acp-22-11987-2022, 2022
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Aviation NOx emissions not only have an impact on global climate by changing ozone and methane levels in the atmosphere, but also contribute to the deterioration of local air quality. The LMDZ-INCA global model is applied to re-evaluate the impact of aircraft NOx and aerosol emissions on climate. We investigate the impact of present-day and future (2050) aircraft emissions on atmospheric composition and the associated radiative forcings of climate for ozone, methane and aerosol direct forcings.
Aurelia Lupaşcu, Noelia Otero, Andrea Minkos, and Tim Butler
Atmos. Chem. Phys., 22, 11675–11699, https://doi.org/10.5194/acp-22-11675-2022, https://doi.org/10.5194/acp-22-11675-2022, 2022
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Ground-level ozone is an important air pollutant that affects human health, ecosystems, and climate. Ozone is not emitted directly but rather formed in the atmosphere through chemical reactions involving two distinct precursors. Our results provide detailed information about the origin of ozone in Germany during two peak ozone events that took place in 2015 and 2018, thus improving our understanding of ground-level ozone.
Hervé Petetin, Dene Bowdalo, Pierre-Antoine Bretonnière, Marc Guevara, Oriol Jorba, Jan Mateu Armengol, Margarida Samso Cabre, Kim Serradell, Albert Soret, and Carlos Pérez Garcia-Pando
Atmos. Chem. Phys., 22, 11603–11630, https://doi.org/10.5194/acp-22-11603-2022, https://doi.org/10.5194/acp-22-11603-2022, 2022
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This study investigates the extent to which ozone forecasts provided by the Copernicus Atmospheric Monitoring Service (CAMS) can be improved using surface observations and state-of-the-art statistical methods. Through a case study over the Iberian Peninsula in 2018–2019, it unambiguously demonstrates the value of these methods for improving the raw CAMS O3 forecasts while at the same time highlighting the complexity of improving the detection of the highest O3 concentrations.
Megan Jeramaz Lickley, John S. Daniel, Eric L. Fleming, Stefan Reimann, and Susan Solomon
Atmos. Chem. Phys., 22, 11125–11136, https://doi.org/10.5194/acp-22-11125-2022, https://doi.org/10.5194/acp-22-11125-2022, 2022
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Halocarbons contained in equipment continue to be emitted after production has ceased. These
banksmust be carefully accounted for in evaluating compliance with the Montreal Protocol. We extend a Bayesian model to the suite of regulated chemicals subject to banking. We find that banks are substantially larger than previous estimates, and we identify banks by chemical and equipment type whose future emissions will contribute to global warming and delay ozone-hole recovery if left unrecovered.
Yawen Kong, Bo Zheng, Qiang Zhang, and Kebin He
Atmos. Chem. Phys., 22, 10769–10788, https://doi.org/10.5194/acp-22-10769-2022, https://doi.org/10.5194/acp-22-10769-2022, 2022
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We developed a Bayesian atmospheric inversion system based on the 4D local ensemble transform Kalman filter (4D-LETKF) algorithm coupled with GEOS-Chem from the latest Orbiting Carbon Observatory-2 (OCO-2) V10r XCO2 retrievals. This is the first adaptation of 4D-LETKF to an OCO-2-based global carbon inversion system. We inferred global gridded carbon fluxes and investigated their magnitudes, variations, and partitioning schemes to understand the global and regional carbon budgets for 2015–2020.
Shanshan Ouyang, Tao Deng, Run Liu, Jingyang Chen, Guowen He, Jeremy Cheuk-Hin Leung, Nan Wang, and Shaw Chen Liu
Atmos. Chem. Phys., 22, 10751–10767, https://doi.org/10.5194/acp-22-10751-2022, https://doi.org/10.5194/acp-22-10751-2022, 2022
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A record-breaking severe O3 pollution episode occurred under the influence of a Pacific subtropical high followed by Typhoon Mitag in the Pearl River Delta (PRD) in early Autumn 2019. Through WRF-CMAQ model simulations, we propose that the enhanced photochemical production of O3 during the episode is a major cause of the most severe O3 pollution year since the official O3 observation started in the PRD in 2006.
Luke M. Western, Alison L. Redington, Alistair J. Manning, Cathy M. Trudinger, Lei Hu, Stephan Henne, Xuekun Fang, Lambert J. M. Kuijpers, Christina Theodoridi, David S. Godwin, Jgor Arduini, Bronwyn Dunse, Andreas Engel, Paul J. Fraser, Christina M. Harth, Paul B. Krummel, Michela Maione, Jens Mühle, Simon O'Doherty, Hyeri Park, Sunyoung Park, Stefan Reimann, Peter K. Salameh, Daniel Say, Roland Schmidt, Tanja Schuck, Carolina Siso, Kieran M. Stanley, Isaac Vimont, Martin K. Vollmer, Dickon Young, Ronald G. Prinn, Ray F. Weiss, Stephen A. Montzka, and Matthew Rigby
Atmos. Chem. Phys., 22, 9601–9616, https://doi.org/10.5194/acp-22-9601-2022, https://doi.org/10.5194/acp-22-9601-2022, 2022
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The production of ozone-destroying gases is being phased out. Even though production of one of the main ozone-depleting gases, called HCFC-141b, has been declining for many years, the amount that is being released to the atmosphere has been increasing since 2017. We do not know for sure why this is. A possible explanation is that HCFC-141b that was used to make insulating foams many years ago is only now escaping to the atmosphere, or a large part of its production is not being reported.
Eva Gorrochategui, Isabel Hernandez, and Romà Tauler
Atmos. Chem. Phys., 22, 9111–9127, https://doi.org/10.5194/acp-22-9111-2022, https://doi.org/10.5194/acp-22-9111-2022, 2022
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A multiway methodology is proposed to handle complex and incomplete atmospheric data sets, providing concise and easily interpretable results. Changes in air quality by NO2, O3 and PM10 in 8 sampling stations located in Catalonia during the COVID-19 lockdown with respect to previous years (2018 and 2019) are investigated. Simultaneous analysis of the 3 contaminants among the 8 stations and for the 3 years allows the evaluation of correlations among the pollutants, even when having missing data.
Christopher D. Holmes
Atmos. Chem. Phys., 22, 9011–9015, https://doi.org/10.5194/acp-22-9011-2022, https://doi.org/10.5194/acp-22-9011-2022, 2022
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Cloud water and ice enable reactions that lead to acid rain and alter atmospheric oxidants, among other impacts. This work develops and evaluates an efficient method of simulating cloud chemistry within global and regional atmospheric models in order to better understand the role of clouds in atmospheric chemistry.
Le Yuan, Olalekan A. M. Popoola, Christina Hood, David Carruthers, Roderic L. Jones, Haitong Zhe Sun, Huan Liu, Qiang Zhang, and Alexander T. Archibald
Atmos. Chem. Phys., 22, 8617–8637, https://doi.org/10.5194/acp-22-8617-2022, https://doi.org/10.5194/acp-22-8617-2022, 2022
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Emission estimates represent a major source of uncertainty in air quality modelling. We developed a novel approach to improve emission estimates from existing inventories using air quality models and routine in situ observations. Using this approach, we derived improved estimates of NOx emissions from the transport sector in Beijing in 2016. This approach has great potential in deriving timely updates of emissions for other pollutants, particularly in regions undergoing rapid emission changes.
Haolin Wang, Xiao Lu, Daniel J. Jacob, Owen R. Cooper, Kai-Lan Chang, Ke Li, Meng Gao, Yiming Liu, Bosi Sheng, Kai Wu, Tongwen Wu, Jie Zhang, Bastien Sauvage, Philippe Nédélec, Romain Blot, and Shaojia Fan
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-381, https://doi.org/10.5194/acp-2022-381, 2022
Revised manuscript accepted for ACP
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We report significant global tropospheric ozone increases in 1995–2017 based on extensive aircraft and ozonesonde observations. Using GEOS-Chem multi-decadal global simulations, we find that changes in global anthropogenic emissions, in particular the rapid increases in aircraft emissions, contribute significantly to the increases in tropospheric ozone and resulting radiative impact.
Angharad C. Stell, Michael Bertolacci, Andrew Zammit-Mangion, Matthew Rigby, Paul J. Fraser, Christina M. Harth, Paul B. Krummel, Xin Lan, Manfredi Manizza, Jens Mühle, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, Dickon Young, and Anita L. Ganesan
EGUsphere, https://doi.org/10.5194/egusphere-2022-513, https://doi.org/10.5194/egusphere-2022-513, 2022
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Nitrous oxide is a potent greenhouse gas and ozone depleting substance, whose atmospheric abundance has risen throughout the contemporary record. In this work, we carry out the first global hierarchical Bayesian inversion to solve for nitrous oxide emissions. We derive increasing global nitrous oxide emissions, which are mainly driven by emissions between 0° and 30° N, with the highest emissions recorded in 2020.
Kaixiang Song, Run Liu, Yu Wang, Tao Liu, Liyan Wei, Yanxing Wu, Junyu Zheng, Boguang Wang, and Shaw Chen Liu
Atmos. Chem. Phys., 22, 8403–8416, https://doi.org/10.5194/acp-22-8403-2022, https://doi.org/10.5194/acp-22-8403-2022, 2022
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We developed an observation-based method to investigate the sensitivity of ozone formation to precursors during two elevated ozone episodes observed at 77 stations in Guangdong, China. We found approximately 67 % of the station days exhibit ozone formation sensitivity to NOx, 20 % of the station days are in the transitional regime sensitive to both NOx and volatile organic compounds (VOCs), and only 13 % of the station days are sensitive to VOCs.
Xiang Weng, Grant L. Forster, and Peer Nowack
Atmos. Chem. Phys., 22, 8385–8402, https://doi.org/10.5194/acp-22-8385-2022, https://doi.org/10.5194/acp-22-8385-2022, 2022
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We use machine learning to quantify the meteorological drivers behind surface ozone variations in China between 2015 and 2019. Our novel approaches show improved performance when compared to previous analysis methods. We highlight that nonlinearity in driver relationships and the impacts of large-scale meteorological phenomena are key to understanding ozone pollution. Moreover, we find that almost half of the observed ozone trend between 2015 and 2019 might have been driven by meteorology.
Zhaojun Tang, Jiaqi Chen, and Zhe Jiang
Atmos. Chem. Phys., 22, 7815–7826, https://doi.org/10.5194/acp-22-7815-2022, https://doi.org/10.5194/acp-22-7815-2022, 2022
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We provide a comparative analysis to explore the effects of satellite and surface measurements on atmospheric CO in data assimilations in 2015–2020 over East Asia. We find possible overestimated enhancements of atmospheric CO by assimilating surface CO measurements due to model representation errors, and a large discrepancy in the derived trends of CO columns due to different vertical sensitivities of satellite and surface observations to lower and free troposphere.
Yue Jia, Birgit Quack, Robert D. Kinley, Ignacio Pisso, and Susann Tegtmeier
Atmos. Chem. Phys., 22, 7631–7646, https://doi.org/10.5194/acp-22-7631-2022, https://doi.org/10.5194/acp-22-7631-2022, 2022
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In this study, we assessed the potential risks of bromoform released from Asparagopsis farming near Australia for the stratospheric ozone layer by analyzing different cultivation scenarios. We conclude that the intended operation of Asparagopsis seaweed cultivation farms with an annual yield to meet the needs of 50 % of feedlots and cattle in either open-ocean or terrestrial cultures in Australia will not impact the ozone layer under normal operating conditions.
Min Huang, James H. Crawford, Gregory R. Carmichael, Kevin W. Bowman, Sujay V. Kumar, and Colm Sweeney
Atmos. Chem. Phys., 22, 7461–7487, https://doi.org/10.5194/acp-22-7461-2022, https://doi.org/10.5194/acp-22-7461-2022, 2022
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This study demonstrates that ozone dry-deposition modeling can be improved by revising the model's dry-deposition parameterizations to better represent the effects of environmental conditions including the soil moisture fields. Applying satellite soil moisture data assimilation is shown to also have added value. Such advancements in coupled modeling and data assimilation can benefit the assessments of ozone impacts on human and vegetation health.
Shidong Fan and Ying Li
Atmos. Chem. Phys., 22, 7331–7351, https://doi.org/10.5194/acp-22-7331-2022, https://doi.org/10.5194/acp-22-7331-2022, 2022
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We investigated the mechanisms by which marine-emitted halogens influence the OH radical, which is not considered in air quality forecasting model systems. The atmospheric OH radical has a complicated response to halogen emissions by species through both physical and chemical processes. Over ocean, inorganic iodine is the controlling species and chemistry is more important. Over land, the physics of sea salt aerosols are more important. The mechanism is applicable to other circumstances.