Articles | Volume 20, issue 11
https://doi.org/10.5194/acp-20-6651-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-20-6651-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
05 Jun 2020
Research article |
| 05 Jun 2020
| 05 Jun 2020
Inverse modeling of SO2 and NOx emissions over China using multisensor satellite data – Part 2: Downscaling techniques for air quality analysis and forecasts
Yi Wang
CORRESPONDING AUTHOR
Interdisciplinary Graduate Program in Informatics, The University of Iowa, Iowa City, IA 52242, USA
Interdisciplinary Graduate Program in Informatics, The University of Iowa, Iowa City, IA 52242, USA
Department of Chemical and Biochemical Engineering, and Center for
Global and Regional Environmental Research, The University of Iowa, Iowa
City, IA 52242, USA
Meng Zhou
Interdisciplinary Graduate Program in Informatics, The University of Iowa, Iowa City, IA 52242, USA
Daven K. Henze
Department of Mechanical Engineering, University of Colorado, Boulder, CO 80309, USA
Cui Ge
Department of Chemical and Biochemical Engineering, and Center for
Global and Regional Environmental Research, The University of Iowa, Iowa
City, IA 52242, USA
South Coast Air Quality Management District, Diamond Bar, CA 91765,
USA
Wei Wang
China National Environmental Monitoring Center, Beijing 100012, China
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Jing Wei, Zhanqing Li, Rachel T. Pinker, Jun Wang, Lin Sun, Wenhao Xue, Runze Li, and Maureen Cribb
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Zichong Chen, Junjie Liu, Daven K. Henze, Deborah N. Huntzinger, Kelley C. Wells, Stephen Sitch, Pierre Friedlingstein, Emilie Joetzjer, Vladislav Bastrikov, Daniel S. Goll, Vanessa Haverd, Atul K. Jain, Etsushi Kato, Sebastian Lienert, Danica L. Lombardozzi, Patrick C. McGuire, Joe R. Melton, Julia E. M. S. Nabel, Benjamin Poulter, Hanqin Tian, Andrew J. Wiltshire, Sönke Zaehle, and Scot M. Miller
Atmos. Chem. Phys., 21, 6663–6680, https://doi.org/10.5194/acp-21-6663-2021, https://doi.org/10.5194/acp-21-6663-2021, 2021
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Lei Kong, Xiao Tang, Jiang Zhu, Zifa Wang, Jianjun Li, Huangjian Wu, Qizhong Wu, Huansheng Chen, Lili Zhu, Wei Wang, Bing Liu, Qian Wang, Duohong Chen, Yuepeng Pan, Tao Song, Fei Li, Haitao Zheng, Guanglin Jia, Miaomiao Lu, Lin Wu, and Gregory R. Carmichael
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Yilin Chen, Huizhong Shen, Jennifer Kaiser, Yongtao Hu, Shannon L. Capps, Shunliu Zhao, Amir Hakami, Jhih-Shyang Shih, Gertrude K. Pavur, Matthew D. Turner, Daven K. Henze, Jaroslav Resler, Athanasios Nenes, Sergey L. Napelenok, Jesse O. Bash, Kathleen M. Fahey, Gregory R. Carmichael, Tianfeng Chai, Lieven Clarisse, Pierre-François Coheur, Martin Van Damme, and Armistead G. Russell
Atmos. Chem. Phys., 21, 2067–2082, https://doi.org/10.5194/acp-21-2067-2021, https://doi.org/10.5194/acp-21-2067-2021, 2021
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Xueying Yu, Dylan B. Millet, Kelley C. Wells, Daven K. Henze, Hansen Cao, Timothy J. Griffis, Eric A. Kort, Genevieve Plant, Malte J. Deventer, Randall K. Kolka, D. Tyler Roman, Kenneth J. Davis, Ankur R. Desai, Bianca C. Baier, Kathryn McKain, Alan C. Czarnetzki, and A. Anthony Bloom
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This study aims to address a challenge in biosphere–atmosphere interactions: to what extent can biogenic organic aerosol (OA) be modified through human activities? From three surface network observations, we show OA is weakly dependent on sulfate and aerosol acidity in the summer southeast US, on both long-term trends and monthly variability. The results are in strong contrast to a global model, GEOS-Chem, suggesting the need to revisit the representation of aqueous-phase secondary OA formation.
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.
Tong Sha, Xiaoyan Ma, Jun Wang, Rong Tian, Jianqi Zhao, Fang Cao, and Yan-Lin Zhang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-760, https://doi.org/10.5194/acp-2020-760, 2020
Preprint withdrawn
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Most numerical models perform poorly on simulating the inorganic chemical components in PM2.5 (sulfate, nitrate, and ammonium (SNA)), generally underestimate sulfate but overestimate nitrate concentrations in haze events. Our work aims at investigating the role of cloud water in simulating SNA. We find that the uncertainties of cloud water can lead to model bias in simulating SNA, and can be reduced by constraining the modeled cloud water with MODIS satellite observations.
Shunliu Zhao, Matthew G. Russell, Amir Hakami, Shannon L. Capps, Matthew D. Turner, Daven K. Henze, Peter B. Percell, Jaroslav Resler, Huizhong Shen, Armistead G. Russell, Athanasios Nenes, Amanda J. Pappin, Sergey L. Napelenok, Jesse O. Bash, Kathleen M. Fahey, Gregory R. Carmichael, Charles O. Stanier, and Tianfeng Chai
Geosci. Model Dev., 13, 2925–2944, https://doi.org/10.5194/gmd-13-2925-2020, https://doi.org/10.5194/gmd-13-2925-2020, 2020
Matthew J. Cooper, Randall V. Martin, Daven K. Henze, and Dylan B. A. Jones
Atmos. Chem. Phys., 20, 7231–7241, https://doi.org/10.5194/acp-20-7231-2020, https://doi.org/10.5194/acp-20-7231-2020, 2020
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Comparisons between satellite-retrieved and model-simulated NO2 columns are affected by differences between the model vertical profile and the assumed profile used in the retrieval process. We examine how such differences impact NOx emission estimates from satellite observations. Larger differences between the simulated and assumed profile shape correspond to larger emission errors. This reveals the importance of using consistent profile information when comparing satellite columns to models.
Yi Wang, Jun Wang, Xiaoguang Xu, Daven K. Henze, Zhen Qu, and Kai Yang
Atmos. Chem. Phys., 20, 6631–6650, https://doi.org/10.5194/acp-20-6631-2020, https://doi.org/10.5194/acp-20-6631-2020, 2020
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The use of OMPS satellite observations to inverse-model SO2 and NO2 emissions is presented through the GEOS-Chem adjoint modeling framework. The work is illustrated over China. The robustness of the results is studied through separate and joint inversions of SO2 and NO2 and the consideration of NH3 uncertainty. Independent validation is performed with OMI SO2 and NO2 data. It is shown that simultaneous inversion of NO2 and SO2 from OMPS provides an effective way to rapidly update emissions.
Sojin Lee, Chul Han Song, Kyung Man Han, Daven K. Henze, Kyunghwa Lee, Jinhyeok Yu, Jung-Hun Woo, Jia Jung, Yunsoo Choi, Pablo E. Saide, and Gregory R. Carmichael
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2020-116, https://doi.org/10.5194/gmd-2020-116, 2020
Revised manuscript not accepted
Tongwen Wu, Fang Zhang, Jie Zhang, Weihua Jie, Yanwu Zhang, Fanghua Wu, Laurent Li, Jinghui Yan, Xiaohong Liu, Xiao Lu, Haiyue Tan, Lin Zhang, Jun Wang, and Aixue Hu
Geosci. Model Dev., 13, 977–1005, https://doi.org/10.5194/gmd-13-977-2020, https://doi.org/10.5194/gmd-13-977-2020, 2020
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This paper describes the first version of the Beijing Climate Center (BCC) fully coupled Earth System Model with interactive atmospheric chemistry and aerosols (BCC-ESM1). It is one of the models at the BCC for the Coupled Model Intercomparison Project Phase 6 (CMIP6). The CMIP6 Aerosol Chemistry Model Intercomparison Project (AerChemMIP) experiment using BCC-ESM1 has been finished. The evaluations show an overall good agreement between BCC-ESM1 simulations and observations in the 20th century.
Xiaohua Pan, Charles Ichoku, Mian Chin, Huisheng Bian, Anton Darmenov, Peter Colarco, Luke Ellison, Tom Kucsera, Arlindo da Silva, Jun Wang, Tomohiro Oda, and Ge Cui
Atmos. Chem. Phys., 20, 969–994, https://doi.org/10.5194/acp-20-969-2020, https://doi.org/10.5194/acp-20-969-2020, 2020
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The differences between these six BB emission datasets are large. Our study found that (1) most current biomass burning (BB) aerosol emission datasets derived from satellite observations lead to the underestimation of aerosol optical depth (AOD) in this model in the biomass-burning-dominated regions and (2) it is important to accurately estimate both the magnitudes and spatial patterns of regional BB emissions in order for a model using these emissions to reproduce observed AOD levels.
Jun Zhu, Xiangao Xia, Huizheng Che, Jun Wang, Zhiyuan Cong, Tianliang Zhao, Shichang Kang, Xuelei Zhang, Xingna Yu, and Yanlin Zhang
Atmos. Chem. Phys., 19, 14637–14656, https://doi.org/10.5194/acp-19-14637-2019, https://doi.org/10.5194/acp-19-14637-2019, 2019
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The long-term temporal–spatial variations of the aerosol optical properties over the Tibetan Plateau (TP) based on the multiple ground-based sun photometer sites and the MODIS product are presented. Besides, the aerosol pollution and aerosol transport processes over the TP are also analyzed by the observations and models. The results in this region could help reduce the assessment uncertainties of aerosol radiative forcing and provide more information on aerosol transportation.
Cheng Chen, Oleg Dubovik, Daven K. Henze, Mian Chin, Tatyana Lapyonok, Gregory L. Schuster, Fabrice Ducos, David Fuertes, Pavel Litvinov, Lei Li, Anton Lopatin, Qiaoyun Hu, and Benjamin Torres
Atmos. Chem. Phys., 19, 14585–14606, https://doi.org/10.5194/acp-19-14585-2019, https://doi.org/10.5194/acp-19-14585-2019, 2019
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Global BC, OC and DD aerosol emissions are inverted from POLDER/PARASOL observations for the year 2010 based on the GEOS-Chem inverse modeling framework. The retrieved emissions are 18.4 Tg yr−1 BC, 109.9 Tg yr−1 OC and 731.6 Tg yr−1 DD, which indicate an increase of 166.7 % for BC and 184.0 % for OC, while a decrease of 42.4 % for DD with respect to GEOS-Chem a priori emission inventories is seen. Global annul mean AOD and AAOD resulting from retrieved emissions are 0.119 and 0.0071 at 550 nm.
Sajeev Philip, Matthew S. Johnson, Christopher Potter, Vanessa Genovesse, David F. Baker, Katherine D. Haynes, Daven K. Henze, Junjie Liu, and Benjamin Poulter
Atmos. Chem. Phys., 19, 13267–13287, https://doi.org/10.5194/acp-19-13267-2019, https://doi.org/10.5194/acp-19-13267-2019, 2019
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This research was conducted to quantify the impact of different prior global biosphere models on the estimate of terrestrial CO2 fluxes when assimilating Orbiting Carbon Observatory-2 (OCO-2) satellite observations. To determine the prior model impact, we apply observing system simulation experiments (OSSEs). Even with the substantial spatiotemporal coverage of OCO-2 data, residual differences in posterior CO2 flux estimates remain due to the choice of prior flux mean and uncertainties.
Steven D. Miller, Louie D. Grasso, Qijing Bian, Sonia M. Kreidenweis, Jack F. Dostalek, Jeremy E. Solbrig, Jennifer Bukowski, Susan C. van den Heever, Yi Wang, Xiaoguang Xu, Jun Wang, Annette L. Walker, Ting-Chi Wu, Milija Zupanski, Christine Chiu, and Jeffrey S. Reid
Atmos. Meas. Tech., 12, 5101–5118, https://doi.org/10.5194/amt-12-5101-2019, https://doi.org/10.5194/amt-12-5101-2019, 2019
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Satellite–based detection of lofted mineral via infrared–window channels, well established in the literature, faces significant challenges in the presence of atmospheric moisture. Here, we consider a case featuring the juxtaposition of two dust plumes embedded within dry and moist air masses. The case is considered from the vantage points of numerical modeling, multi–sensor observations, and radiative transfer theory arriving at a new method for mitigating the water vapor masking effect.
Stephen M. Saleeby, Susan C. van den Heever, Jennie Bukowski, Annette L. Walker, Jeremy E. Solbrig, Samuel A. Atwood, Qijing Bian, Sonia M. Kreidenweis, Yi Wang, Jun Wang, and Steven D. Miller
Atmos. Chem. Phys., 19, 10279–10301, https://doi.org/10.5194/acp-19-10279-2019, https://doi.org/10.5194/acp-19-10279-2019, 2019
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This study seeks to understand how intense dust storms impact the heating and cooling of the land surface and atmosphere. Dust storms that are intense enough to substantially impact visibility can also alter how much sunlight reaches the surface during the day and how much heat is trapped in the atmosphere at night. These radiation changes can impact the temperature of the atmosphere and impact the weather in the vicinity.
Jiarui Wu, Naifang Bei, Bo Hu, Suixin Liu, Meng Zhou, Qiyuan Wang, Xia Li, Lang Liu, Tian Feng, Zirui Liu, Yichen Wang, Junji Cao, Xuexi Tie, Jun Wang, Luisa T. Molina, and Guohui Li
Atmos. Chem. Phys., 19, 8703–8719, https://doi.org/10.5194/acp-19-8703-2019, https://doi.org/10.5194/acp-19-8703-2019, 2019
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In the present study, simulations during a persistent and heavy haze pollution episode from 5 December 2015 to 4 January 2016 in the North China Plain (NCP) were performed using the WRF-Chem model to comprehensively quantify contributions of the aerosol shortwave radiative feedback (ARF) to near-surface PM2.5 mass concentrations. During the episode, the ARF deteriorates the haze pollution, increasing the near-surface PM2.5 concentration in the NCP by 10.2 μg m−3 (7.8 %) on average.
Jiarui Wu, Naifang Bei, Bo Hu, Suixin Liu, Meng Zhou, Qiyuan Wang, Xia Li, Lang Liu, Tian Feng, Zirui Liu, Yichen Wang, Junji Cao, Xuexi Tie, Jun Wang, Luisa T. Molina, and Guohui Li
Atmos. Chem. Phys., 19, 8721–8739, https://doi.org/10.5194/acp-19-8721-2019, https://doi.org/10.5194/acp-19-8721-2019, 2019
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The near-surface PM2.5 contribution of the ALW total effect is 17.5 % in NCP, indicating that ALW plays an important role in the PM2.5 formation during the wintertime haze pollution. Moreover, the ALW-HET overwhelmingly dominates the PM2.5 enhancement due to the ALW. The ALW does not consistently enhance near-surface [PM2.5] with increasing RH. When the RH exceeds 80 %, the contribution of the ALW begins to decrease, which is caused by the high occurrence frequencies of precipitation.
Ying Wei, Xueshun Chen, Huansheng Chen, Jie Li, Zifa Wang, Wenyi Yang, Baozhu Ge, Huiyun Du, Jianqi Hao, Wei Wang, Jianjun Li, Yele Sun, and Huili Huang
Atmos. Chem. Phys., 19, 8269–8296, https://doi.org/10.5194/acp-19-8269-2019, https://doi.org/10.5194/acp-19-8269-2019, 2019
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This study presents a full description and evaluation of a global–regional nested aerosol and atmospheric chemistry model (IAP-AACM). The simulation for 2014 is evaluated against model datasets and a range of observational datasets. The results show that IAP-AACM is within the range of other models, and reproduces both spatial and seasonal variation of trace gases and aerosols over most areas well. In future, we recommend improving the model's ability to capture high spatial variation of PM2.5.
Xiaoguang Xu, Jun Wang, Yi Wang, Jing Zeng, Omar Torres, Jeffrey S. Reid, Steven D. Miller, J. Vanderlei Martins, and Lorraine A. Remer
Atmos. Meas. Tech., 12, 3269–3288, https://doi.org/10.5194/amt-12-3269-2019, https://doi.org/10.5194/amt-12-3269-2019, 2019
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Detecting aerosol layer height from space is challenging. The traditional method relies on active sensors such as lidar that provide the detailed vertical structure of the aerosol profile but is costly with limited spatial coverage (more than 1 year is needed for global coverage). Here we developed a passive remote sensing technique that uses backscattered sunlight to retrieve smoke aerosol layer height over both water and vegetated surfaces from a sensor 1.5 million kilometers from the Earth.
Zainab Q. Hakim, Scott Archer-Nicholls, Gufran Beig, Gerd A. Folberth, Kengo Sudo, Nathan Luke Abraham, Sachin Ghude, Daven K. Henze, and Alexander T. Archibald
Atmos. Chem. Phys., 19, 6437–6458, https://doi.org/10.5194/acp-19-6437-2019, https://doi.org/10.5194/acp-19-6437-2019, 2019
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Surface ozone is an important air pollutant and recent work has calculated that large numbers of people die prematurely because of exposure to high levels of surface ozone in India. However, these calculations require model simulations of ozone as key inputs.
Here we perform the most thorough evaluation of global model surface ozone over India to date. These analyses of model simulations and observations highlight some successes and shortcomings and the need for further process-based studies.
Huanxin Zhang, Jun Wang, Lorena Castro García, Jing Zeng, Connor Dennhardt, Yang Liu, and Nickolay A. Krotkov
Atmos. Chem. Phys., 19, 2165–2181, https://doi.org/10.5194/acp-19-2165-2019, https://doi.org/10.5194/acp-19-2165-2019, 2019
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OMU-based surface erythemal UV irradiance is compared with ground observations in the United States from 2005 to 2017. We reveal that the assumption of constant atmospheric conditions between OMI overpass time and local solar noon time may not fully represent the real atmosphere and the peaks of surface UV are not always at local solar noon because of cloud effects. Future geostationary satellites (e.g., TEMPO) would reduce sampling bias and improve trend analysis of surface UV estimate.
Milija Zupanski, Anton Kliewer, Ting-Chi Wu, Karina Apodaca, Qijing Bian, Sam Atwood, Yi Wang, Jun Wang, and Steven D. Miller
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-2, https://doi.org/10.5194/acp-2019-2, 2019
Revised manuscript not accepted
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The problem of under-observed aerosol observations and in particular the vertical distribution of aerosols is addressed using a strongly coupled atmosphere-aerosol data assimilation system. In the strongly coupled system the atmospheric observations, which are more numerous in general, can impact the aerosol initial conditions. In an application over a coastal zone, results indicate that atmospheric observations have a positive impact on aerosols.
Ting-Chi Wu, Milija Zupanski, Stephen Saleeby, Anton Kliewer, Lewis Grasso, Qijing Bian, Samuel A. Atwood, Yi Wang, and Jun Wang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-1249, https://doi.org/10.5194/acp-2018-1249, 2018
Revised manuscript not accepted
Anton Kliewer, Milija Zupanski, Qijing Bian, Sam Atwood, Yi Wang, and Jun Wang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-1156, https://doi.org/10.5194/acp-2018-1156, 2018
Revised manuscript not accepted
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This research is focused on improving numerical weather prediction by including data regarding aerosols in the atmosphere. Using weather prediction models along with data assimilation (the process of marrying observations with a model prediction), a better representation of the atmosphere can be described. As no model or observational platform is ever perfect, the aerosol observations have to be de-biased (adjusting for systematic error). Here we look at two such methods.
Xinyi Dong, Joshua S. Fu, Qingzhao Zhu, Jian Sun, Jiani Tan, Terry Keating, Takashi Sekiya, Kengo Sudo, Louisa Emmons, Simone Tilmes, Jan Eiof Jonson, Michael Schulz, Huisheng Bian, Mian Chin, Yanko Davila, Daven Henze, Toshihiko Takemura, Anna Maria Katarina Benedictow, and Kan Huang
Atmos. Chem. Phys., 18, 15581–15600, https://doi.org/10.5194/acp-18-15581-2018, https://doi.org/10.5194/acp-18-15581-2018, 2018
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We have applied the HTAP phase II multi-model data to investigate the long-range transport impacts on surface concentration and column density of PM from Europe and Russia, Belarus, and Ukraine to eastern Asia, with a special focus on the long-range transport contribution during haze episodes in China. We found that long-range transport plays a more important role in elevating the background concentration of surface PM during the haze days.
Elizabeth M. Lennartson, Jun Wang, Juping Gu, Lorena Castro Garcia, Cui Ge, Meng Gao, Myungje Choi, Pablo E. Saide, Gregory R. Carmichael, Jhoon Kim, and Scott J. Janz
Atmos. Chem. Phys., 18, 15125–15144, https://doi.org/10.5194/acp-18-15125-2018, https://doi.org/10.5194/acp-18-15125-2018, 2018
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This paper is among the first to study the diurnal variations of AOD, PM2.5, and their relationships in South Korea. We show that the PM2.5–AOD relationship has strong diurnal variations, and, hence, using AOD data retrieved from geostationary satellite can improve the monitoring of surface PM2.5 air quality on a daily basis as well as constrain the diurnal variation of aerosol emission.
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.
Jan Eiof Jonson, Michael Schulz, Louisa Emmons, Johannes Flemming, Daven Henze, Kengo Sudo, Marianne Tronstad Lund, Meiyun Lin, Anna Benedictow, Brigitte Koffi, Frank Dentener, Terry Keating, Rigel Kivi, and Yanko Davila
Atmos. Chem. Phys., 18, 13655–13672, https://doi.org/10.5194/acp-18-13655-2018, https://doi.org/10.5194/acp-18-13655-2018, 2018
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Focusing on Europe, this HTAP 2 study computes ozone in several global models when reducing anthropogenic emissions by 20 % in different world regions. The differences in model results are explored
by use of a novel stepwise approach combining a tracer, CO and ozone. For ozone the contributions from the rest of the world are larger than from Europe, with the largest contributions from North America and eastern Asia. Contributions do, however, depend on the choice of ozone metric.
Cheng Chen, Oleg Dubovik, Daven K. Henze, Tatyana Lapyonak, Mian Chin, Fabrice Ducos, Pavel Litvinov, Xin Huang, and Lei Li
Atmos. Chem. Phys., 18, 12551–12580, https://doi.org/10.5194/acp-18-12551-2018, https://doi.org/10.5194/acp-18-12551-2018, 2018
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This paper introduces a method to use satellite-observed spectral AOD and AAOD to derive three types of aerosol emission sources simultaneously based on inverse modelling at a high spatial and temporal resolution. This study shows it is possible to estimate aerosol emissions and improve the atmospheric aerosol simulation using detailed aerosol optical and microphysical information from satellite observations.
Ciao-Kai Liang, J. Jason West, Raquel A. Silva, Huisheng Bian, Mian Chin, Yanko Davila, Frank J. Dentener, Louisa Emmons, Johannes Flemming, Gerd Folberth, Daven Henze, Ulas Im, Jan Eiof Jonson, Terry J. Keating, Tom Kucsera, Allen Lenzen, Meiyun Lin, Marianne Tronstad Lund, Xiaohua Pan, Rokjin J. Park, R. Bradley Pierce, Takashi Sekiya, Kengo Sudo, and Toshihiko Takemura
Atmos. Chem. Phys., 18, 10497–10520, https://doi.org/10.5194/acp-18-10497-2018, https://doi.org/10.5194/acp-18-10497-2018, 2018
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Emissions from one continent affect air quality and health elsewhere. Here we quantify the effects of intercontinental PM2.5 and ozone transport on human health using a new multi-model ensemble, evaluating the health effects of emissions from six world regions and three emission source sectors. Emissions from one region have significant health impacts outside of that source region; similarly, foreign emissions contribute significantly to air-pollution-related deaths in several world regions.
Steven T. Turnock, Oliver Wild, Frank J. Dentener, Yanko Davila, Louisa K. Emmons, Johannes Flemming, Gerd A. Folberth, Daven K. Henze, Jan E. Jonson, Terry J. Keating, Sudo Kengo, Meiyun Lin, Marianne Lund, Simone Tilmes, and Fiona M. O'Connor
Atmos. Chem. Phys., 18, 8953–8978, https://doi.org/10.5194/acp-18-8953-2018, https://doi.org/10.5194/acp-18-8953-2018, 2018
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A simple parameterisation was developed in this study to provide a rapid assessment of the impacts and uncertainties associated with future emission control strategies by predicting changes to surface ozone air quality and near-term climate forcing of ozone. Future emissions scenarios based on currently implemented legislation are shown to worsen surface ozone air quality and enhance near-term climate warming, with changes in methane becoming increasingly important in the future.
Stefano Galmarini, Ioannis Kioutsioukis, Efisio Solazzo, Ummugulsum Alyuz, Alessandra Balzarini, Roberto Bellasio, Anna M. K. Benedictow, Roberto Bianconi, Johannes Bieser, Joergen Brandt, Jesper H. Christensen, Augustin Colette, Gabriele Curci, Yanko Davila, Xinyi Dong, Johannes Flemming, Xavier Francis, Andrea Fraser, Joshua Fu, Daven K. Henze, Christian Hogrefe, Ulas Im, Marta Garcia Vivanco, Pedro Jiménez-Guerrero, Jan Eiof Jonson, Nutthida Kitwiroon, Astrid Manders, Rohit Mathur, Laura Palacios-Peña, Guido Pirovano, Luca Pozzoli, Marie Prank, Martin Schultz, Rajeet S. Sokhi, Kengo Sudo, Paolo Tuccella, Toshihiko Takemura, Takashi Sekiya, and Alper Unal
Atmos. Chem. Phys., 18, 8727–8744, https://doi.org/10.5194/acp-18-8727-2018, https://doi.org/10.5194/acp-18-8727-2018, 2018
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An ensemble of model results relating to ozone concentrations in Europe in 2010 has been produced and studied. The novelty consists in the fact that the ensemble is made of results of models working at two different scales (regional and global), therefore contributing in detail two different parts of the atmospheric spectrum. The ensemble defined as a hybrid has been studied in detail and shown to bring additional value to the assessment of air quality.
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.
Jiani Tan, Joshua S. Fu, Frank Dentener, Jian Sun, Louisa Emmons, Simone Tilmes, Kengo Sudo, Johannes Flemming, Jan Eiof Jonson, Sylvie Gravel, Huisheng Bian, Yanko Davila, Daven K. Henze, Marianne T. Lund, Tom Kucsera, Toshihiko Takemura, and Terry Keating
Atmos. Chem. Phys., 18, 6847–6866, https://doi.org/10.5194/acp-18-6847-2018, https://doi.org/10.5194/acp-18-6847-2018, 2018
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We study the distributions of sulfur and nitrogen deposition, which are associated with current environmental issues such as formation of acid rain and ecosystem eutrophication and result in widespread problems such as loss of environmental diversity, harming the crop yield and even food insecurity. According to our study, both the amount and distribution of sulfate and nitrogen deposition have changed significantly in the last decade, particularly in East Asia, South Asia and Southeast Asia.
Kira Sadighi, Evan Coffey, Andrea Polidori, Brandon Feenstra, Qin Lv, Daven K. Henze, and Michael Hannigan
Atmos. Meas. Tech., 11, 1777–1792, https://doi.org/10.5194/amt-11-1777-2018, https://doi.org/10.5194/amt-11-1777-2018, 2018
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Ground-level ozone has negative human health impacts. In the summer of 2015, 13 low-cost sensor monitors were deployed to several neighborhoods around Riverside, California. There were significant spatial differences between monitors. This is important because it means that ozone in certain places may be higher than what EPA monitors report for an area, which is pertinent for residents of those communities. This research helps inform the limitations and advantages of low-cost sensor networks.
Kelley C. Wells, Dylan B. Millet, Nicolas Bousserez, Daven K. Henze, Timothy J. Griffis, Sreelekha Chaliyakunnel, Edward J. Dlugokencky, Eri Saikawa, Gao Xiang, Ronald G. Prinn, Simon O'Doherty, Dickon Young, Ray F. Weiss, Geoff S. Dutton, James W. Elkins, Paul B. Krummel, Ray Langenfelds, and L. Paul Steele
Atmos. Chem. Phys., 18, 735–756, https://doi.org/10.5194/acp-18-735-2018, https://doi.org/10.5194/acp-18-735-2018, 2018
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This paper uses three different frameworks to derive nitrous oxide (N2O) emissions based on global surface observations. One of these frameworks employs a new approach that allows for fast computation and explores a larger solution space than other methods. Our results point to a few conclusions about the global N2O budget, including a larger contribution from tropical sources, an overestimate of natural soil emissions, and an underestimate of agricultural sources particularly in springtime.
Lin Zhang, Youfan Chen, Yuanhong Zhao, Daven K. Henze, Liye Zhu, Yu Song, Fabien Paulot, Xuejun Liu, Yuepeng Pan, Yi Lin, and Binxiang Huang
Atmos. Chem. Phys., 18, 339–355, https://doi.org/10.5194/acp-18-339-2018, https://doi.org/10.5194/acp-18-339-2018, 2018
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Substantial differences exist in current estimates of agricultural ammonia emissions in China, hindering understanding of their environmental consequences. This study applies both bottom-up and top-down methods to better quantify agricultural ammonia sources in China using observations from satellite and surface networks interpreted by a chemical transport model. Our estimate of annual Chinese anthropogenic ammonia emission is 11.7 tg (teragram) for 2008 with a strong seasonality peak in summer.
Yuxuan Wang, Yuanyu Xie, Wenhao Dong, Yi Ming, Jun Wang, and Lu Shen
Atmos. Chem. Phys., 17, 12827–12843, https://doi.org/10.5194/acp-17-12827-2017, https://doi.org/10.5194/acp-17-12827-2017, 2017
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Besides the well-known large impact on agriculture and water resources, drought is associated with significant adverse effects on air quality. Drought-induced degradation of air quality is largely due to natural processes, offsetting the effort of anthropogenic emission reduction during the past decades. Such adverse impacts should be included in modeling processes under current and future climate for mitigation policy.
Jun-Wei Xu, Randall V. Martin, Andrew Morrow, Sangeeta Sharma, Lin Huang, W. Richard Leaitch, Julia Burkart, Hannes Schulz, Marco Zanatta, Megan D. Willis, Daven K. Henze, Colin J. Lee, Andreas B. Herber, and Jonathan P. D. Abbatt
Atmos. Chem. Phys., 17, 11971–11989, https://doi.org/10.5194/acp-17-11971-2017, https://doi.org/10.5194/acp-17-11971-2017, 2017
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We interpret a series of recent airborne and ground-based measurements with the GEOS-Chem model and its adjoint to attribute the sources of Arctic BC. Anthropogenic emissions in eastern and southern Asia make the largest contribution to Arctic BC. Gas flaring emissions from oilfields in western Siberia and from the Tarim oilfield in western China could have striking impacts on Arctic BC loadings.
Ling Qi, Qinbin Li, Daven K. Henze, Hsien-Liang Tseng, and Cenlin He
Atmos. Chem. Phys., 17, 9697–9716, https://doi.org/10.5194/acp-17-9697-2017, https://doi.org/10.5194/acp-17-9697-2017, 2017
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We find that Asian anthropogenic sources are the largest contributors (~ 40 %) to surface BC in spring in the Arctic, inconsistent with previous studies which repeatedly identified sources of surface BC as anthropogenic emissions from Europe and Russia. It takes 12–17 days for Asian anthropogenic emissions to be transported to the Arctic surface. Additionally, a large fraction (40–65 %) of Asian contribution is in the form of chronic pollution on 1- to 2-month timescales.
Jonathan J. Guerrette and Daven K. Henze
Atmos. Chem. Phys., 17, 7605–7633, https://doi.org/10.5194/acp-17-7605-2017, https://doi.org/10.5194/acp-17-7605-2017, 2017
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This work describes the implementation and application of a new advanced tool, WRFDA-Chem, for top-down constraints of regional atmospheric chemical emissions. Aircraft and surface observations of black carbon are traced to anthropogenic and biomass burning sources in California during ARCTAS-CARB. The information content of the observations is quantified through variance reduction and degrees of freedom of signal, which can be used to assess observing strategies and emission inventories.
Zhe Jiang, Helen Worden, John R. Worden, Daven K. Henze, Dylan B. A. Jones, Avelino F. Arellano, Emily V. Fischer, Liye Zhu, Kazuyuki Miyazaki, K. Folkert Boersma, and Vivienne H. Payne
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-382, https://doi.org/10.5194/acp-2017-382, 2017
Preprint withdrawn
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We investigated the variation of US tropospheric NO2 in the past decade. We demonstrated significant divergence between the time variation in tropospheric NO2 columns from OMI retrievals and surface measurements. Our analysis suggests limited contributions from local effects such as fossil fuel emissions, lightning, or instrument artifacts, and indicates possible important contributions from long-range transport of Asian emissions that are modulated by ENSO.
Min Huang, Gregory R. Carmichael, R. Bradley Pierce, Duseong S. Jo, Rokjin J. Park, Johannes Flemming, Louisa K. Emmons, Kevin W. Bowman, Daven K. Henze, Yanko Davila, Kengo Sudo, Jan Eiof Jonson, Marianne Tronstad Lund, Greet Janssens-Maenhout, Frank J. Dentener, Terry J. Keating, Hilke Oetjen, and Vivienne H. Payne
Atmos. Chem. Phys., 17, 5721–5750, https://doi.org/10.5194/acp-17-5721-2017, https://doi.org/10.5194/acp-17-5721-2017, 2017
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In support of the HTAP phase 2 experiment, we conducted a number of regional-scale Sulfur Transport and dEposition Model base and sensitivity simulations over North America during May–June 2010. The STEM chemical boundary conditions were downscaled from three (GEOS-Chem, RAQMS, and ECMWF C-IFS) global chemical transport models' simulations. Analyses were performed on large spatial–temporal scales relative to HTAP1 and also on subcontinental and event scales including the use of satellite data.
Zhe Jiang, John R. Worden, Helen Worden, Merritt Deeter, Dylan B. A. Jones, Avelino F. Arellano, and Daven K. Henze
Atmos. Chem. Phys., 17, 4565–4583, https://doi.org/10.5194/acp-17-4565-2017, https://doi.org/10.5194/acp-17-4565-2017, 2017
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We constrain the long-term variation in global CO emissions for 2001–2015. Our results confirm that the decreasing trend of tropospheric CO in the Northern Hemisphere is due to decreasing CO emissions from anthropogenic and biomass burning sources. In particular, we find decreasing CO emissions from the United States and China in the past 15 years, unchanged anthropogenic CO emissions from Europe since 2008, and likely a positive trend from India and southeast Asia.
Chantelle R. Lonsdale, Jennifer D. Hegarty, Karen E. Cady-Pereira, Matthew J. Alvarado, Daven K. Henze, Matthew D. Turner, Shannon L. Capps, John B. Nowak, J. Andy Neuman, Ann M. Middlebrook, Roya Bahreini, Jennifer G. Murphy, Milos Z. Markovic, Trevor C. VandenBoer, Lynn M. Russell, and Amy Jo Scarino
Atmos. Chem. Phys., 17, 2721–2739, https://doi.org/10.5194/acp-17-2721-2017, https://doi.org/10.5194/acp-17-2721-2017, 2017
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This study takes advantage of the high-resolution observations of NH3(g) made by the TES satellite instrument over Bakersfield during the CalNex campaign, along with campaign measurements, to compare CMAQ model results in the San Joaquin Valley, California. Additionally we evaluate the CMAQ bi-directional ammonia flux results using the CARB emissions inventory against these satellite and campaign measurements, not previously explored in combination.
Camilla Weum Stjern, Bjørn Hallvard Samset, Gunnar Myhre, Huisheng Bian, Mian Chin, Yanko Davila, Frank Dentener, Louisa Emmons, Johannes Flemming, Amund Søvde Haslerud, Daven Henze, Jan Eiof Jonson, Tom Kucsera, Marianne Tronstad Lund, Michael Schulz, Kengo Sudo, Toshihiko Takemura, and Simone Tilmes
Atmos. Chem. Phys., 16, 13579–13599, https://doi.org/10.5194/acp-16-13579-2016, https://doi.org/10.5194/acp-16-13579-2016, 2016
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Air pollution can reach distant regions through intercontinental transport. Here we first present results from the Hemispheric Transport of Air Pollution Phase 2 exercise, where many models performed the same set of coordinated emission-reduction experiments. We find that mitigations have considerable extra-regional effects, and show that this is particularly true for black carbon emissions, as long-range transport elevates aerosols to higher levels where their radiative influence is stronger.
Zeli Tan, Qianlai Zhuang, Daven K. Henze, Christian Frankenberg, Ed Dlugokencky, Colm Sweeney, Alexander J. Turner, Motoki Sasakawa, and Toshinobu Machida
Atmos. Chem. Phys., 16, 12649–12666, https://doi.org/10.5194/acp-16-12649-2016, https://doi.org/10.5194/acp-16-12649-2016, 2016
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Methane emissions from the pan-Arctic could be important in understanding the global carbon cycle but are still poorly constrained to date. This study demonstrated that satellite retrievals can be used to reduce the uncertainty of the estimates of these emissions. We also provided additional evidence for the existence of large methane emissions from pan-Arctic lakes in the Siberian yedoma permafrost region. We found that biogeochemical models should be improved for better estimates.
Zhe Jiang, Kazuyuki Miyazaki, John R. Worden, Jane J. Liu, Dylan B. A. Jones, and Daven K. Henze
Atmos. Chem. Phys., 16, 6537–6546, https://doi.org/10.5194/acp-16-6537-2016, https://doi.org/10.5194/acp-16-6537-2016, 2016
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We quantify the impacts of anthropogenic and natural sources on free tropospheric ozone over the Middle East, using the adjoint of the GEOS-Chem model with updated NOx emissions estimates from an ensemble Kalman filter. We show that the global total contribution of lightning NOx on free tropospheric O3 over the Middle East is about 2 times larger than that from global anthropogenic sources. The summertime free tropospheric O3 enhancement is primarily due to Asian NOx emissions.
Nicolas Bousserez, Daven K. Henze, Brigitte Rooney, Andre Perkins, Kevin J. Wecht, Alexander J. Turner, Vijay Natraj, and John R. Worden
Atmos. Chem. Phys., 16, 6175–6190, https://doi.org/10.5194/acp-16-6175-2016, https://doi.org/10.5194/acp-16-6175-2016, 2016
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This work provides new insight into the observational constraints provided by current low-Earth orbit (LEO) and future potential geostationary (GEO) satellite missions on methane emissions in North America. Using efficient numerical tools, the information content (error reductions, spatial resolution of the constraints) of methane inversions using different instrument configurations (TIR, SWIR and multi-spectral) was estimated at model grid-scale resolution (0.5° × 0.7°).
Shouguo Ding, Jun Wang, and Xiaoguang Xu
Atmos. Meas. Tech., 9, 2077–2092, https://doi.org/10.5194/amt-9-2077-2016, https://doi.org/10.5194/amt-9-2077-2016, 2016
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Knowledge on the vertical distribution of aerosols in the atmospheric is important for studying aerosol impacts on air quality and climate change. The polarization measurements in O2 A and B bands is shown here theoretically to have rich information for characterizing aerosol vertical profile over land. This paper presents a passive remote sensing technique supplementary to the existing technique to retrieve aerosol vertical distribution over land from space.
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.
M. W. Shephard, C. A. McLinden, K. E. Cady-Pereira, M. Luo, S. G. Moussa, A. Leithead, J. Liggio, R. M. Staebler, A. Akingunola, P. Makar, P. Lehr, J. Zhang, D. K. Henze, D. B. Millet, J. O. Bash, L. Zhu, K. C. Wells, S. L. Capps, S. Chaliyakunnel, M. Gordon, K. Hayden, J. R. Brook, M. Wolde, and S.-M. Li
Atmos. Meas. Tech., 8, 5189–5211, https://doi.org/10.5194/amt-8-5189-2015, https://doi.org/10.5194/amt-8-5189-2015, 2015
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This study provides direct validations of Tropospheric Emission Spectrometer (TES) satellite retrieved profiles against coincident aircraft profiles of carbon monoxide, ammonia, methanol, and formic acid, all of which are of interest for air quality. The comparisons are performed over the Canadian oil sands region during an intensive field campaign in support of the Joint Canada-Alberta Implementation Plan for the Oil Sands Monitoring (JOSM). Initial model evaluations are also provided.
L. Zhu, D. Henze, J. Bash, G.-R. Jeong, K. Cady-Pereira, M. Shephard, M. Luo, F. Paulot, and S. Capps
Atmos. Chem. Phys., 15, 12823–12843, https://doi.org/10.5194/acp-15-12823-2015, https://doi.org/10.5194/acp-15-12823-2015, 2015
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We implement new diurnal variation scheme for ammonia livestock emissions and bidirectional exchange scheme and its adjoint in the GEOS-Chem global chemical transport model. Updated diurnal variability improves modeled-to-hourly in situ measurements comparison. The ammonium soil pool in the bidirectional exchange model largely extends the ammonia lifetime in the atmosphere. Large model biases remain as livestock emissions are still underestimated.
F. Deng, D. B. A. Jones, T. W. Walker, M. Keller, K. W. Bowman, D. K. Henze, R. Nassar, E. A. Kort, S. C. Wofsy, K. A. Walker, A. E. Bourassa, and D. A. Degenstein
Atmos. Chem. Phys., 15, 11773–11788, https://doi.org/10.5194/acp-15-11773-2015, https://doi.org/10.5194/acp-15-11773-2015, 2015
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The upper troposphere and lower stratosphere (UTLS) is characterized by strong gradients in the distribution of long-lived tracers, which are sensitive to discrepancies in transport in models. We found that our model overestimates CO2 in the polar UTLS through comparison of modeled CO2 with aircraft observations. We then corrected the modeled CO2 and quantified the impact of the correction on the flux estimates using an atmospheric model together with atmospheric CO2 measured from a satellite.
K. C. Wells, D. B. Millet, N. Bousserez, D. K. Henze, S. Chaliyakunnel, T. J. Griffis, Y. Luan, E. J. Dlugokencky, R. G. Prinn, S. O'Doherty, R. F. Weiss, G. S. Dutton, J. W. Elkins, P. B. Krummel, R. Langenfelds, L. P. Steele, E. A. Kort, S. C. Wofsy, and T. Umezawa
Geosci. Model Dev., 8, 3179–3198, https://doi.org/10.5194/gmd-8-3179-2015, https://doi.org/10.5194/gmd-8-3179-2015, 2015
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This paper introduces a new inversion framework for N2O using GEOS-Chem and its adjoint, which we employed in a series of observing system simulation experiments to evaluate the source and sink constraints provided by surface and aircraft-based N2O measurements. We also applied a new approach for estimating a posteriori uncertainty for high-dimensional inversions, and used it to quantify the spatial and temporal resolution of N2O emission constraints achieved with the current observing network.
Y. Zhao, L. Zhang, Y. Pan, Y. Wang, F. Paulot, and D. K. Henze
Atmos. Chem. Phys., 15, 10905–10924, https://doi.org/10.5194/acp-15-10905-2015, https://doi.org/10.5194/acp-15-10905-2015, 2015
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Rapid Asian industrialization has led to increased atmospheric nitrogen deposition downwind. This work analyzes the sources and processes controlling atmospheric nitrogen deposition to the northwestern Pacific. Both nitrogen emissions and meteorology, largely controlled by the East Asian Monsoon, determine the seasonality of nitrogen deposition. Ascribing deposition over the marginal seas to nitrogen sources from different regions and sectors shows important contribution from fertilizer use.
P. D. Hamer, K. W. Bowman, D. K. Henze, J.-L. Attié, and V. Marécal
Atmos. Chem. Phys., 15, 10645–10667, https://doi.org/10.5194/acp-15-10645-2015, https://doi.org/10.5194/acp-15-10645-2015, 2015
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Using a simplified air quality forecasting model, we explore how characteristics of air quality observations affect our ability to understand and predict ozone air pollution. We show that the photochemical conditions can strongly influence the observing priorities for ozone prediction, such as which species are observed and how well, when, and how frequently. High-freqency observations of ozone, NOx and HCHO in combination during the morning and afternoon are particularly advantageous.
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.
Y. H. Mao, Q. B. Li, D. K. Henze, Z. Jiang, D. B. A. Jones, M. Kopacz, C. He, L. Qi, M. Gao, W.-M. Hao, and K.-N. Liou
Atmos. Chem. Phys., 15, 7685–7702, https://doi.org/10.5194/acp-15-7685-2015, https://doi.org/10.5194/acp-15-7685-2015, 2015
J. J. Guerrette and D. K. Henze
Geosci. Model Dev., 8, 1857–1876, https://doi.org/10.5194/gmd-8-1857-2015, https://doi.org/10.5194/gmd-8-1857-2015, 2015
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WRFPLUS-Chem is a coupled meteorology-chemistry adjoint and tangent linear model, with applications in sensitivity analysis and four-dimensional variational data assimilation. The linearized models are verified against finite difference approximations from the nonlinear forward model, WRF-Chem. A new checkpointing scheme enables data assimilation beyond 6h. New capabilities are demonstrated in an emission sensitivity study.
Z. Jiang, D. B. A. Jones, J. Worden, H. M. Worden, D. K. Henze, and Y. X. Wang
Atmos. Chem. Phys., 15, 6801–6814, https://doi.org/10.5194/acp-15-6801-2015, https://doi.org/10.5194/acp-15-6801-2015, 2015
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We present a high-resolution (0.5 x 0.667) regional CO inversion over North America in the period of June 2004–May 2005, using a combination of GEOS-Chem model and MOPITT CO observations. With optimized lateral boundary conditions, we show that regional inversion analyses can reduce the sensitivity of the CO source estimates to errors in long-range transport and in the distributions of the hydroxyl radical (OH), and consequently, provide better quantification on regional CO source estimates.
Z. Jiang, D. B. A. Jones, H. M. Worden, and D. K. Henze
Atmos. Chem. Phys., 15, 1521–1537, https://doi.org/10.5194/acp-15-1521-2015, https://doi.org/10.5194/acp-15-1521-2015, 2015
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Using MOPITT (version 5) tropospheric profile and surface layer retrievals, we constrain global CO emissions in the period of June 2004 – May 2005. The inversions suggest a reduction in CO emission in the tropics and an increase in emissions at middle and high latitudes. The results demonstrate that the use of the surface layer retrievals from MOPITT can significantly mitigate the potential impacts of model bias in OH and long-range transport on CO emission 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.
Q. Zhu, Q. Zhuang, D. Henze, K. Bowman, M. Chen, Y. Liu, Y. He, H. Matsueda, T. Machida, Y. Sawa, and W. Oechel
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-14-22587-2014, https://doi.org/10.5194/acpd-14-22587-2014, 2014
Revised manuscript not accepted
Z. Shen, J. Liu, L. W. Horowitz, D. K. Henze, S. Fan, Levy II H., D. L. Mauzerall, J.-T. Lin, and S. Tao
Atmos. Chem. Phys., 14, 6315–6327, https://doi.org/10.5194/acp-14-6315-2014, https://doi.org/10.5194/acp-14-6315-2014, 2014
F. Deng, D. B. A. Jones, D. K. Henze, N. Bousserez, K. W. Bowman, J. B. Fisher, R. Nassar, C. O'Dell, D. Wunch, P. O. Wennberg, E. A. Kort, S. C. Wofsy, T. Blumenstock, N. M. Deutscher, D. W. T. Griffith, F. Hase, P. Heikkinen, V. Sherlock, K. Strong, R. Sussmann, and T. Warneke
Atmos. Chem. Phys., 14, 3703–3727, https://doi.org/10.5194/acp-14-3703-2014, https://doi.org/10.5194/acp-14-3703-2014, 2014
K. C. Wells, D. B. Millet, K. E. Cady-Pereira, M. W. Shephard, D. K. Henze, N. Bousserez, E. C. Apel, J. de Gouw, C. Warneke, and H. B. Singh
Atmos. Chem. Phys., 14, 2555–2570, https://doi.org/10.5194/acp-14-2555-2014, https://doi.org/10.5194/acp-14-2555-2014, 2014
C. Ge, J. Wang, and J. S. Reid
Atmos. Chem. Phys., 14, 159–174, https://doi.org/10.5194/acp-14-159-2014, https://doi.org/10.5194/acp-14-159-2014, 2014
B. S. Meland, X. Xu, D. K. Henze, and J. Wang
Atmos. Meas. Tech., 6, 3441–3457, https://doi.org/10.5194/amt-6-3441-2013, https://doi.org/10.5194/amt-6-3441-2013, 2013
J. Wang, S. Park, J. Zeng, C. Ge, K. Yang, S. Carn, N. Krotkov, and A. H. Omar
Atmos. Chem. Phys., 13, 1895–1912, https://doi.org/10.5194/acp-13-1895-2013, https://doi.org/10.5194/acp-13-1895-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Anthropogenic emission controls reduce summertime ozone–temperature sensitivity in the United States
Investigating the response of China's surface ozone concentration to the future changes of multiple factors
Assessing the relative impacts of satellite ozone and its precursor observations to improve global tropospheric ozone analysis using multiple chemical reanalysis systems
Evaluating present-day and future impacts of agricultural ammonia emissions on atmospheric chemistry and climate
Air-pollution-satellite-based CO2 emission inversion: system evaluation, sensitivity analysis, and future research direction
Insights into ozone pollution control in urban areas by decoupling meteorological factors based on machine learning
Quantification of regional net CO2 flux errors in the Orbiting Carbon Observatory-2 (OCO-2) v10 model intercomparison project (MIP) ensemble using airborne measurements
Reactive nitrogen in and around the northeastern and mid-Atlantic US: sources, sinks, and connections with ozone
Preindustrial-to-present-day changes in atmospheric carbon monoxide: agreement and gaps between ice archives and global model reconstructions
Investigating processes influencing simulation of local Arctic wintertime anthropogenic pollution in Fairbanks, Alaska, during ALPACA-2022
Urban ozone formation and sensitivities to volatile chemical products, cooking emissions, and NOx upwind of and within two Los Angeles Basin cities
Causes of growing middle-to-upper tropospheric ozone over the northwest Pacific region
Impact of introducing electric vehicles on ground-level O3 and PM2.5 in the Greater Tokyo Area: yearly trends and the importance of changes in the urban heat island effect
A CO2–Δ14CO2 inversion setup for estimating European fossil CO2 emissions
Maximum ozone concentrations in the southwestern US and Texas: implications of the growing predominance of the background contribution
Derivation of atmospheric reaction mechanisms for volatile organic compounds by the SAPRC mechanism generation system (MechGen)
Seasonal, regional, and vertical characteristics of high-carbon-monoxide plumes along with their associated ozone anomalies, as seen by IAGOS between 2002 and 2019
The potential of drone observations to improve air quality predictions by 4D-Var
Process analysis of elevated concentrations of organic acids at Whiteface Mountain, New York
Ozone source attribution in polluted European areas during summer 2017 as simulated with MECO(n)
Opinion: Challenges and needs of tropospheric chemical mechanism development
The atmospheric oxidizing capacity in China – Part 2: Sensitivity to emissions of primary pollutants
Role of chemical production and depositional losses on formaldehyde in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM)
Review of source analyses of ambient volatile organic compounds considering reactive losses: methods of reducing loss effects, impacts of losses, and sources
Interpreting summertime hourly variation of NO2 columns with implications for geostationary satellite applications
An investigation into atmospheric nitrous acid (HONO) processes in South Korea
Performance evaluation of UKESM1 for surface ozone across the pan-tropics
Constraining light dependency in modeled emissions through comparison to observed biogenic volatile organic compound (BVOC) concentrations in a southeastern US forest
A global re-analysis of regionally resolved emissions and atmospheric mole fractions of SF6 for the period 2005–2021
Monoterpene oxidation pathways initiated by acyl peroxy radical addition
Tropospheric ozone precursors: global and regional distributions, trends, and variability
Sensitivity of climate effects of hydrogen to leakage size, location, and chemical background
The contribution of transport emissions to ozone mixing ratios and methane lifetime in 2015 and 2050 in the Shared Socioeconomic Pathways (SSPs)
Local and transboundary contributions to nitrogen loadings across East Asia using CMAQ-ISAM and GEMS-informed emissions inventory during the winter-spring transition
Ether and ester formation from peroxy radical recombination: a qualitative reaction channel analysis
ACEIC: a comprehensive anthropogenic chlorine emission inventory for China
Impact of methane and other precursor emission reductions on surface ozone in Europe: scenario analysis using the European Monitoring and Evaluation Programme (EMEP) Meteorological Synthesizing Centre – West (MSC-W) model
Chemistry-climate feedback of atmospheric methane in a methane emission flux driven chemistry-climate model
Natural emissions of VOC and NOx over Africa constrained by TROPOMI HCHO and NO2 data using the MAGRITTEv1.1 model
Verifying national inventory-based combustion emissions of CO2 across the UK and mainland Europe using satellite observations of atmospheric CO and CO2
Revisiting the high tropospheric ozone over Southern Africa: overestimated biomass burning and underestimated anthropogenic emissions
Enhanced understanding of atmospheric blocking modulation on ozone dynamics within a high-resolution Earth system model
Estimating the variability of NOx emissions from Wuhan with TROPOMI NO2 data during 2018 to 2023
An improved estimate of inorganic iodine emissions from the ocean using a coupled surface microlayer box model
Technical note: A comparative study of chemistry schemes for volcanic sulfur dioxide in Lagrangian transport simulations: a case study of the 2019 Raikoke eruption
Evaluating tropospheric nitrogen dioxide in UKCA using OMI satellite retrievals over South and East Asia
Impact of improved representation of volatile organic compound emissions and production of NOx reservoirs on modeled urban ozone production
The effect of different climate and air quality policies in China on in situ ozone production in Beijing
Enhancing long-term trend simulation of the global tropospheric hydroxyl (TOH) and its drivers from 2005 to 2019: a synergistic integration of model simulations and satellite observations
Intercomparison of GEOS-Chem and CAM-chem tropospheric oxidant chemistry within the Community Earth System Model version 2 (CESM2)
Shuai Li, Haolin Wang, and Xiao Lu
Atmos. Chem. Phys., 25, 2725–2743, https://doi.org/10.5194/acp-25-2725-2025, https://doi.org/10.5194/acp-25-2725-2025, 2025
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Summertime ozone–temperature sensitivity has decreased by 50 % from 3.0 ppbv per K in 1990 to 1.5 ppb per K in 2021 in the US. GEOS-Chem simulations show that anthropogenic nitrogen oxide emission reduction is the dominant driver of ozone–temperature sensitivity decline by influencing both temperature direct and temperature indirect processes. Reduced ozone–temperature sensitivity has decreased ozone enhancement from low to high temperatures by an average of 6.8 ppbv across the US.
Jinya Yang, Yutong Wang, Lei Zhang, and Yu Zhao
Atmos. Chem. Phys., 25, 2649–2666, https://doi.org/10.5194/acp-25-2649-2025, https://doi.org/10.5194/acp-25-2649-2025, 2025
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We develop a modeling framework to predict future ozone concentrations (till the 2060s) in China following an IPCC scenario. We evaluate the contributions of climatic, anthropogenic, and biogenic factors by season and region. We find persistent emission controls will alter the nonlinear response of ozone to its precursors and dominate the declining ozone level. The outcomes highlight the importance of human actions, even with a climate penalty on air quality.
Takashi Sekiya, Emanuele Emili, Kazuyuki Miyazaki, Antje Inness, Zhen Qu, R. Bradley Pierce, Dylan Jones, Helen Worden, William Y. Y. Cheng, Vincent Huijnen, and Gerbrand Koren
Atmos. Chem. Phys., 25, 2243–2268, https://doi.org/10.5194/acp-25-2243-2025, https://doi.org/10.5194/acp-25-2243-2025, 2025
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Five global chemical reanalysis datasets were used to assess the relative impacts of assimilating satellite ozone and its precursor measurements on tropospheric ozone analyses for 2010. The multiple reanalysis system comparison allows an evaluation of the dependency of the impacts on different reanalysis systems. The results suggested the importance of satellite ozone and its precursor measurements for improving ozone analysis in the whole troposphere, with varying magnitudes among the systems.
Maureen Beaudor, Didier Hauglustaine, Juliette Lathière, Martin Van Damme, Lieven Clarisse, and Nicolas Vuichard
Atmos. Chem. Phys., 25, 2017–2046, https://doi.org/10.5194/acp-25-2017-2025, https://doi.org/10.5194/acp-25-2017-2025, 2025
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Agriculture is the biggest ammonia (NH3) source, impacting air quality, climate, and ecosystems. Because of food demand, NH3 emissions are projected to rise by 2100. Using a global model, we analyzed the impact of present and future NH3 emissions generated from a land model. Our results show improved ammonia patterns compared to a reference inventory. Future scenarios predict up to 70 % increase in global NH3 burden, with significant changes in radiative forcing that can greatly elevate N2O.
Hui Li, Jiaxin Qiu, and Bo Zheng
Atmos. Chem. Phys., 25, 1949–1963, https://doi.org/10.5194/acp-25-1949-2025, https://doi.org/10.5194/acp-25-1949-2025, 2025
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We conduct a sensitivity analysis with 31 tests on various factors including prior emissions, model resolution, satellite constraint, and other system configurations to assess the vulnerability of emission estimates across temporal, sectoral, and regional dimensions. This reveals the robustness of emissions estimated by this air-pollution-satellite-based CO2 emission inversion system, with relative change between tests and base inversion below 4.0 % for national annual NOx and CO2 emissions.
Yuqing Qiu, Xin Li, Wenxuan Chai, Yi Liu, Mengdi Song, Xudong Tian, Qiaoli Zou, Wenjun Lou, Wangyao Zhang, Juan Li, and Yuanhang Zhang
Atmos. Chem. Phys., 25, 1749–1763, https://doi.org/10.5194/acp-25-1749-2025, https://doi.org/10.5194/acp-25-1749-2025, 2025
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The chemical reactions of ozone (O3) formation are related to meteorology and local emissions. Here, a random forest approach was used to eliminate the effects of meteorological factors (dispersion or transport) on O3 and its precursors. Variations in the sensitivity of O3 formation and the apportionment of emission sources were revealed after meteorological normalization. Our results suggest that meteorological variations should be considered when diagnosing O3 formation.
Jeongmin Yun, Junjie Liu, Brendan Byrne, Brad Weir, Lesley E. Ott, Kathryn McKain, Bianca C. Baier, Luciana V. Gatti, and Sebastien C. Biraud
Atmos. Chem. Phys., 25, 1725–1748, https://doi.org/10.5194/acp-25-1725-2025, https://doi.org/10.5194/acp-25-1725-2025, 2025
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This study quantifies errors in regional net surface–atmosphere CO2 flux estimates from an inverse model ensemble using airborne CO2 measurements. Our results show that flux error estimates based on observations significantly exceed those computed from the ensemble spread of flux estimates in regions with high fossil fuel emissions. This finding suggests the presence of systematic biases in the inversion estimates, associated with errors in the fossil fuel emissions common to all models.
Min Huang, Gregory R. Carmichael, Kevin W. Bowman, Isabelle De Smedt, Andreas Colliander, Michael H. Cosh, Sujay V. Kumar, Alex B. Guenther, Scott J. Janz, Ryan M. Stauffer, Anne M. Thompson, Niko M. Fedkin, Robert J. Swap, John D. Bolten, and Alicia T. Joseph
Atmos. Chem. Phys., 25, 1449–1476, https://doi.org/10.5194/acp-25-1449-2025, https://doi.org/10.5194/acp-25-1449-2025, 2025
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We use model simulations along with multiplatform, multidisciplinary observations and a range of analysis methods to estimate and understand the distributions, temporal changes, and impacts of reactive nitrogen and ozone over the most populous US region that has undergone significant environmental changes. Deposition, biogenic emissions, and extra-regional sources have been playing increasingly important roles in controlling pollutant budgets in this area as local anthropogenic emissions drop.
Xavier Faïn, Sophie Szopa, Vaishali Naïk, Patricia Martinerie, David M. Etheridge, Rachael H. Rhodes, Cathy M. Trudinger, Vasilii V. Petrenko, Kévin Fourteau, and Philip Place
Atmos. Chem. Phys., 25, 1105–1119, https://doi.org/10.5194/acp-25-1105-2025, https://doi.org/10.5194/acp-25-1105-2025, 2025
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Carbon monoxide (CO) plays a crucial role in the atmosphere's oxidizing capacity. In this study, we analyse how historical (1850–2014) [CO] outputs from state-of-the-art global chemistry–climate models over Greenland and Antarctica are able to capture both absolute values and trends recorded in multi-site ice archives. A disparity in [CO] growth rates emerges in the Northern Hemisphere between models and observations from 1920–1975 CE, possibly linked to uncertainties in CO emission factors.
Natalie Brett, Kathy S. Law, Steve R. Arnold, Javier G. Fochesatto, Jean-Christophe Raut, Tatsuo Onishi, Robert Gilliam, Kathleen Fahey, Deanna Huff, George Pouliot, Brice Barret, Elsa Dieudonné, Roman Pohorsky, Julia Schmale, Andrea Baccarini, Slimane Bekki, Gianluca Pappaccogli, Federico Scoto, Stefano Decesari, Antonio Donateo, Meeta Cesler-Maloney, William Simpson, Patrice Medina, Barbara D'Anna, Brice Temime-Roussel, Joel Savarino, Sarah Albertin, Jingqiu Mao, Becky Alexander, Allison Moon, Peter F. DeCarlo, Vanessa Selimovic, Robert Yokelson, and Ellis S. Robinson
Atmos. Chem. Phys., 25, 1063–1104, https://doi.org/10.5194/acp-25-1063-2025, https://doi.org/10.5194/acp-25-1063-2025, 2025
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Processes influencing dispersion of local anthropogenic pollution in Arctic wintertime are investigated with Lagrangian dispersion modelling. Simulated power plant plume rise that considers temperature inversion layers improves results compared to observations (interior Alaska). Modelled surface concentrations are improved by representation of vertical mixing and emission estimates. Large increases in diesel vehicle emissions at temperatures reaching −35°C are required to reproduce observed NOx.
Chelsea E. Stockwell, Matthew M. Coggon, Rebecca H. Schwantes, Colin Harkins, Bert Verreyken, Congmeng Lyu, Qindan Zhu, Lu Xu, Jessica B. Gilman, Aaron Lamplugh, Jeff Peischl, Michael A. Robinson, Patrick R. Veres, Meng Li, Andrew W. Rollins, Kristen Zuraski, Sunil Baidar, Shang Liu, Toshihiro Kuwayama, Steven S. Brown, Brian C. McDonald, and Carsten Warneke
Atmos. Chem. Phys., 25, 1121–1143, https://doi.org/10.5194/acp-25-1121-2025, https://doi.org/10.5194/acp-25-1121-2025, 2025
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In urban areas, emissions from everyday products like paints, cleaners, and personal care products, along with non-traditional sources such as cooking, are increasingly important and impact air quality. This study uses a box model to evaluate how these emissions impact ozone in the Los Angeles Basin and quantifies the impact of gaseous cooking emissions. Accurate representation of these and other anthropogenic sources in inventories is crucial for informing effective air quality policies.
Xiaodan Ma, Jianping Huang, Michaela I. Hegglin, Patrick Jöckel, and Tianliang Zhao
Atmos. Chem. Phys., 25, 943–958, https://doi.org/10.5194/acp-25-943-2025, https://doi.org/10.5194/acp-25-943-2025, 2025
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Our research explored changes in ozone levels in the northwest Pacific region over 30 years, revealing a significant increase in the middle-to-upper troposphere, especially during spring and summer. This rise is influenced by both stratospheric and tropospheric sources, which affect climate and air quality in East Asia. This work underscores the need for continued study to understand underlying mechanisms.
Hiroo Hata, Norifumi Mizushima, and Tomohiko Ihara
Atmos. Chem. Phys., 25, 1037–1061, https://doi.org/10.5194/acp-25-1037-2025, https://doi.org/10.5194/acp-25-1037-2025, 2025
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The introduction of battery electric vehicles (BEVs) is expected to reduce the primary air pollutants from vehicular exhaust and evaporative emissions while reducing the anthropogenic heat produced by vehicles, ultimately mitigating the urban heat island (UHI) effect. This study revealed the impact of introducing BEVs on the decrease in the UHI effect and the impact of BEVs on the formation of tropospheric ozone and fine particulate matter in the Greater Tokyo Area of Japan.
Carlos Gómez-Ortiz, Guillaume Monteil, Sourish Basu, and Marko Scholze
Atmos. Chem. Phys., 25, 397–424, https://doi.org/10.5194/acp-25-397-2025, https://doi.org/10.5194/acp-25-397-2025, 2025
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In this paper, we test new implementations of our inverse modeling tool to estimate the weekly and regional CO2 emissions from fossil fuels in Europe. We use synthetic atmospheric observations of CO2 and radiocarbon (14CO2) to trace emissions to their sources, while separating the natural and fossil CO2. Our tool accurately estimates fossil CO2 emissions in densely monitored regions like western/central Europe. This approach aids in developing strategies for reducing CO2 emissions.
David D. Parrish, Ian C. Faloona, and Richard G. Derwent
Atmos. Chem. Phys., 25, 263–289, https://doi.org/10.5194/acp-25-263-2025, https://doi.org/10.5194/acp-25-263-2025, 2025
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Observation-based estimates of contributions to maximum ozone (O3) concentrations show that background O3 can exceed the air quality standard of 70 ppb in the southwestern US, precluding standard attainment. Over the past 4 decades, US anthropogenic O3 has decreased by a factor of ~ 6.3, while wildfire contributions have increased, so that the background now dominates maximum concentrations, even in Los Angeles, and the occurrence of maximum O3 has shifted from the eastern to the western US.
William P. L. Carter, Jia Jiang, John J. Orlando, and Kelley C. Barsanti
Atmos. Chem. Phys., 25, 199–242, https://doi.org/10.5194/acp-25-199-2025, https://doi.org/10.5194/acp-25-199-2025, 2025
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This paper describes the scientific basis for gas-phase atmospheric chemical mechanisms derived using the SAPRC mechanism generation system, MechGen. It can derive mechanisms for most organic compounds with C, H, O, or N atoms, including initial reactions of organics with OH, O3, NO3, and O3P or by photolysis, as well as the reactions of the various types of intermediates that are formed. The paper includes a description of areas of uncertainty where additional research and updates are needed.
Thibaut Lebourgeois, Bastien Sauvage, Pawel Wolff, Béatrice Josse, Virginie Marécal, Yasmine Bennouna, Romain Blot, Damien Boulanger, Hannah Clark, Jean-Marc Cousin, Philippe Nedelec, and Valérie Thouret
Atmos. Chem. Phys., 24, 13975–14004, https://doi.org/10.5194/acp-24-13975-2024, https://doi.org/10.5194/acp-24-13975-2024, 2024
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Our study examines intense-carbon-monoxide (CO) pollution events measured by commercial aircraft from the In-service Aircraft for a Global Observing System (IAGOS) research infrastructure. We combine these measurements with the SOFT-IO model to trace the origin of the observed CO. A comprehensive analysis of the geographical origin, source type, seasonal variation, and ozone levels of these pollution events is provided.
Hassnae Erraji, Philipp Franke, Astrid Lampert, Tobias Schuldt, Ralf Tillmann, Andreas Wahner, and Anne Caroline Lange
Atmos. Chem. Phys., 24, 13913–13934, https://doi.org/10.5194/acp-24-13913-2024, https://doi.org/10.5194/acp-24-13913-2024, 2024
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Four-dimensional variational data assimilation allows for the simultaneous optimisation of initial values and emission rates by using trace-gas profiles from drone observations in a regional air quality model. Assimilated profiles positively impact the representation of air pollutants in the model by improving their vertical distribution and ground-level concentrations. This case study highlights the potential of drone data to enhance air quality analyses including local emission evaluation.
Christopher Lawrence, Mary Barth, John Orlando, Paul Casson, Richard Brandt, Daniel Kelting, Elizabeth Yerger, and Sara Lance
Atmos. Chem. Phys., 24, 13693–13713, https://doi.org/10.5194/acp-24-13693-2024, https://doi.org/10.5194/acp-24-13693-2024, 2024
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This work uses chemical transport and box modeling to study the gas- and aqueous-phase production of organic acid concentrations measured in cloud water at the summit of Whiteface Mountain on 1 July 2018. Isoprene was the major source of formic, acetic, and oxalic acid. Gas-phase chemistry greatly underestimated formic and acetic acid, indicating missing sources, while cloud chemistry was a key source of oxalic acid. More studies of organic acids are required to better constrain their sources.
Markus Kilian, Volker Grewe, Patrick Jöckel, Astrid Kerkweg, Mariano Mertens, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 24, 13503–13523, https://doi.org/10.5194/acp-24-13503-2024, https://doi.org/10.5194/acp-24-13503-2024, 2024
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Anthropogenic emissions are a major source of precursors of tropospheric ozone. As ozone formation is highly non-linear, we apply a global–regional chemistry–climate model with a source attribution method (tagging) to quantify the contribution of anthropogenic emissions to ozone. Our analysis shows that the contribution of European anthropogenic emissions largely increases during large ozone periods, indicating that emissions from these sectors drive ozone values.
Barbara Ervens, Andrew Rickard, Bernard Aumont, William P. L. Carter, Max McGillen, Abdelwahid Mellouki, John Orlando, Bénédicte Picquet-Varrault, Paul Seakins, William R. Stockwell, Luc Vereecken, and Timothy J. Wallington
Atmos. Chem. Phys., 24, 13317–13339, https://doi.org/10.5194/acp-24-13317-2024, https://doi.org/10.5194/acp-24-13317-2024, 2024
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Chemical mechanisms describe the chemical processes in atmospheric models that are used to describe the changes in the atmospheric composition. Therefore, accurate chemical mechanisms are necessary to predict the evolution of air pollution and climate change. The article describes all steps that are needed to build chemical mechanisms and discusses the advances and needs of experimental and theoretical research activities needed to build reliable chemical mechanisms.
Jianing Dai, Guy P. Brasseur, Mihalis Vrekoussis, Maria Kanakidou, Kun Qu, Yijuan Zhang, Hongliang Zhang, and Tao Wang
Atmos. Chem. Phys., 24, 12943–12962, https://doi.org/10.5194/acp-24-12943-2024, https://doi.org/10.5194/acp-24-12943-2024, 2024
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This paper employs a regional chemical transport model to quantify the sensitivity of air pollutants and photochemical parameters to specified emission reductions in China for representative winter and summer conditions. The study provides insights into further air quality control in China with reduced primary emissions.
T. Nash Skipper, Emma L. D'Ambro, Forwood C. Wiser, V. Faye McNeill, Rebecca H. Schwantes, Barron H. Henderson, Ivan R. Piletic, Colleen B. Baublitz, Jesse O. Bash, Andrew R. Whitehill, Lukas C. Valin, Asher P. Mouat, Jennifer Kaiser, Glenn M. Wolfe, Jason M. St. Clair, Thomas F. Hanisco, Alan Fried, Bryan K. Place, and Havala O.T. Pye
Atmos. Chem. Phys., 24, 12903–12924, https://doi.org/10.5194/acp-24-12903-2024, https://doi.org/10.5194/acp-24-12903-2024, 2024
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We develop the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM) version 2 to improve predictions of formaldehyde in ambient air compared to satellite-, aircraft-, and ground-based observations. With the updated chemistry, we estimate the cancer risk from inhalation exposure to ambient formaldehyde across the contiguous USA and predict that 40 % of this risk is controllable through reductions in anthropogenic emissions of nitrogen oxides and reactive organic carbon.
Baoshuang Liu, Yao Gu, Yutong Wu, Qili Dai, Shaojie Song, Yinchang Feng, and Philip K. Hopke
Atmos. Chem. Phys., 24, 12861–12879, https://doi.org/10.5194/acp-24-12861-2024, https://doi.org/10.5194/acp-24-12861-2024, 2024
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Reactive loss of volatile organic compounds (VOCs) is a long-term issue yet to be resolved in VOC source analyses. We assess common methods of, and existing issues in, reducing losses, impacts of losses, and sources in current source analyses. We offer a potential supporting role for solving issues of VOC conversion. Source analyses of consumed VOCs that reacted to produce ozone and secondary organic aerosols can play an important role in the effective control of secondary pollution in air.
Deepangsu Chatterjee, Randall V. Martin, Chi Li, Dandan Zhang, Haihui Zhu, Daven K. Henze, James H. Crawford, Ronald C. Cohen, Lok N. Lamsal, and Alexander M. Cede
Atmos. Chem. Phys., 24, 12687–12706, https://doi.org/10.5194/acp-24-12687-2024, https://doi.org/10.5194/acp-24-12687-2024, 2024
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We investigate the hourly variation of NO2 columns and surface concentrations by applying the GEOS-Chem model to interpret aircraft and ground-based measurements over the US and Pandora sun photometer measurements over the US, Europe, and Asia. Corrections to the Pandora columns and finer model resolution improve the modeled representation of the summertime hourly variation of total NO2 columns to explain the weaker hourly variation in NO2 columns than at the surface.
Kiyeon Kim, Kyung Man Han, Chul Han Song, Hyojun Lee, Ross Beardsley, Jinhyeok Yu, Greg Yarwood, Bonyoung Koo, Jasper Madalipay, Jung-Hun Woo, and Seogju Cho
Atmos. Chem. Phys., 24, 12575–12593, https://doi.org/10.5194/acp-24-12575-2024, https://doi.org/10.5194/acp-24-12575-2024, 2024
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We incorporated each HONO process into the current CMAQ modeling framework to enhance the accuracy of HONO mixing ratio predictions. These results expand our understanding of HONO photochemistry and identify crucial sources of HONO that impact the total HONO budget in Seoul, South Korea. Through this investigation, we contribute to resolving discrepancies in understanding chemical transport models, with implications for better air quality management and environmental protection in the region.
Flossie Brown, Gerd Folberth, Stephen Sitch, Paulo Artaxo, Marijn Bauters, Pascal Boeckx, Alexander W. Cheesman, Matteo Detto, Ninong Komala, Luciana Rizzo, Nestor Rojas, Ines dos Santos Vieira, Steven Turnock, Hans Verbeeck, and Alfonso Zambrano
Atmos. Chem. Phys., 24, 12537–12555, https://doi.org/10.5194/acp-24-12537-2024, https://doi.org/10.5194/acp-24-12537-2024, 2024
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Ozone is a pollutant that is detrimental to human and plant health. Ozone monitoring sites in the tropics are limited, so models are often used to understand ozone exposure. We use measurements from the tropics to evaluate ozone from the UK Earth system model, UKESM1. UKESM1 is able to capture the pattern of ozone in the tropics, except in southeast Asia, although it systematically overestimates it at all sites. This work highlights that UKESM1 can capture seasonal and hourly variability.
Namrata Shanmukh Panji, Deborah F. McGlynn, Laura E. R. Barry, Todd M. Scanlon, Manuel T. Lerdau, Sally E. Pusede, and Gabriel Isaacman-VanWertz
Atmos. Chem. Phys., 24, 12495–12507, https://doi.org/10.5194/acp-24-12495-2024, https://doi.org/10.5194/acp-24-12495-2024, 2024
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Climate change will bring about changes in parameters that are currently used in global-scale models to calculate biogenic emissions. This study seeks to understand the factors driving these models by comparing long-term datasets of biogenic compounds to modeled emissions. We note that the light-dependent fractions currently used in models do not accurately represent regional observations. We provide evidence for the time-dependent variation in this parameter for future modifications to models.
Martin Vojta, Andreas Plach, Saurabh Annadate, Sunyoung Park, Gawon Lee, Pallav Purohit, Florian Lindl, Xin Lan, Jens Mühle, Rona L. Thompson, and Andreas Stohl
Atmos. Chem. Phys., 24, 12465–12493, https://doi.org/10.5194/acp-24-12465-2024, https://doi.org/10.5194/acp-24-12465-2024, 2024
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We constrain the global emissions of the very potent greenhouse gas sulfur hexafluoride (SF6) between 2005 and 2021. We show that SF6 emissions are decreasing in the USA and in the EU, while they are substantially growing in China, leading overall to an increasing global emission trend. The national reports for the USA, EU, and China all underestimated their SF6 emissions. However, stringent mitigation measures can successfully reduce SF6 emissions, as can be seen in the EU emission trend.
Dominika Pasik, Thomas Golin Almeida, Emelda Ahongshangbam, Siddharth Iyer, and Nanna Myllys
EGUsphere, https://doi.org/10.5194/egusphere-2024-3464, https://doi.org/10.5194/egusphere-2024-3464, 2024
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We used quantum chemistry methods to investigate the oxidation mechanisms of acyl peroxy radicals (APRs) with various monoterpenes. Our findings reveal unique oxidation pathways for different monoterpenes, leading to either chain-terminating products or highly reactive intermediates that can contribute to particle formation in the atmosphere. This research highlights APRs as potentially significant but underexplored atmospheric oxidants, which may influence future approaches to modeling climate.
Yasin Elshorbany, Jerald R. Ziemke, Sarah Strode, Hervé Petetin, Kazuyuki Miyazaki, Isabelle De Smedt, Kenneth Pickering, Rodrigo J. Seguel, Helen Worden, Tamara Emmerichs, Domenico Taraborrelli, Maria Cazorla, Suvarna Fadnavis, Rebecca R. Buchholz, Benjamin Gaubert, Néstor Y. Rojas, Thiago Nogueira, Thérèse Salameh, and Min Huang
Atmos. Chem. Phys., 24, 12225–12257, https://doi.org/10.5194/acp-24-12225-2024, https://doi.org/10.5194/acp-24-12225-2024, 2024
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We investigated tropospheric ozone spatial variability and trends from 2005 to 2019 and related those to ozone precursors on global and regional scales. We also investigate the spatiotemporal characteristics of the ozone formation regime in relation to ozone chemical sources and sinks. Our analysis is based on remote sensing products of the tropospheric column of ozone and its precursors, nitrogen dioxide, formaldehyde, and total column CO, as well as ozonesonde data and model simulations.
Ragnhild Bieltvedt Skeie, Marit Sandstad, Srinath Krishnan, Gunnar Myhre, and Maria Sand
EGUsphere, https://doi.org/10.5194/egusphere-2024-3079, https://doi.org/10.5194/egusphere-2024-3079, 2024
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Hydrogen leakages can alter the amount of climate gases in the atmosphere and hence have a climate impact. In this study we investigate, using an atmospheric chemistry model, how this indirect climate effect differs for different amounts of leakages, where the hydrogen leaks and if this effect changes in the future. The effect is largest for emissions far from areas where hydrogen is removed from the atmosphere by the soil, but these are not relevant locations for a future hydrogen economy.
Mariano Mertens, Sabine Brinkop, Phoebe Graf, Volker Grewe, Johannes Hendricks, Patrick Jöckel, Anna Lanteri, Sigrun Matthes, Vanessa S. Rieger, Mattia Righi, and Robin N. Thor
Atmos. Chem. Phys., 24, 12079–12106, https://doi.org/10.5194/acp-24-12079-2024, https://doi.org/10.5194/acp-24-12079-2024, 2024
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We quantified the contributions of land transport, shipping, and aviation emissions to tropospheric ozone; its radiative forcing; and the reductions of the methane lifetime using chemistry-climate model simulations. The contributions were analysed for the conditions of 2015 and for three projections for the year 2050. The results highlight the challenges of mitigating ozone formed by emissions of the transport sector, caused by the non-linearitiy of the ozone chemistry and the long lifetime.
Jincheol Park, Yunsoo Choi, and Sagun Kayastha
EGUsphere, https://doi.org/10.5194/egusphere-2024-3312, https://doi.org/10.5194/egusphere-2024-3312, 2024
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We investigated NOx emissions’ contributions to nitrogen loadings across five regions of East Asia during the 2022 winter-spring transition through chemical transport modeling informed by satellite data. As seasons progress, local contributions within each region to its NOy budget decreased from 32 %–43 % to 23 %–30 %, while transboundary contributions increased from 16 %–33 % to 27 %–37 %, driven by a shift in synoptic settings that allowed pollutants to spread more broadly across the regions.
Lauri Franzon, Marie Camredon, Richard Valorso, Bernard Aumont, and Theo Kurtén
Atmos. Chem. Phys., 24, 11679–11699, https://doi.org/10.5194/acp-24-11679-2024, https://doi.org/10.5194/acp-24-11679-2024, 2024
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In this article we investigate the formation of large, sticky molecules from various organic compounds entering the atmosphere as primary emissions and the degree to which these processes may contribute to organic aerosol particle mass. More specifically, we qualitatively investigate a recently discovered chemical reaction channel for one of the most important short-lived radical compounds, peroxy radicals, and discover which of these reactions are most atmospherically important.
Siting Li, Yiming Liu, Yuqi Zhu, Yinbao Jin, Yingying Hong, Ao Shen, Yifei Xu, Haofan Wang, Haichao Wang, Xiao Lu, Shaojia Fan, and Qi Fan
Atmos. Chem. Phys., 24, 11521–11544, https://doi.org/10.5194/acp-24-11521-2024, https://doi.org/10.5194/acp-24-11521-2024, 2024
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This study establishes an inventory of anthropogenic chlorine emissions in China in 2019 with expanded species (HCl, Cl-, Cl2, HOCl) and sources (41 specific sources). The inventory is validated by a modeling study against the observations. This study enhances the understanding of anthropogenic chlorine emissions in the atmosphere, identifies key sources, and provides scientific support for pollution control and climate change.
Willem E. van Caspel, Zbigniew Klimont, Chris Heyes, and Hilde Fagerli
Atmos. Chem. Phys., 24, 11545–11563, https://doi.org/10.5194/acp-24-11545-2024, https://doi.org/10.5194/acp-24-11545-2024, 2024
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Methane in the atmosphere contributes to the production of ozone gas – an air pollutant and greenhouse gas. Our results highlight that simultaneous reductions in methane emissions help avoid offsetting the air pollution benefits already achieved by the already-approved precursor emission reductions by 2050 in the European Monitoring and Evaluation Programme region, while also playing an important role in bringing air pollution further down towards World Health Organization guideline limits.
Laura Stecher, Franziska Winterstein, Patrick Jöckel, Michael Ponater, Mariano Mertens, and Martin Dameris
EGUsphere, https://doi.org/10.5194/egusphere-2024-2938, https://doi.org/10.5194/egusphere-2024-2938, 2024
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Methane, the second most important anthropogenic greenhouse gas, is chemically decomposed in the atmosphere. The chemical sink of atmospheric methane is not constant, but depends on the temperature and on the abundance of its reaction partners. In this study, we use a global chemistry-climate model to assess the feedback of atmospheric methane induced by changes of the chemical sink in a warming climate, and its implications for the chemical composition and the surface air temperature change.
Beata Opacka, Trissevgeni Stavrakou, Jean-François Müller, Isabelle De Smedt, Jos van Geffen, Eloise A. Marais, Rebekah P. Horner, Dylan B. Millet, Kelly C. Wells, and Alex B. Guenther
EGUsphere, https://doi.org/10.5194/egusphere-2024-2912, https://doi.org/10.5194/egusphere-2024-2912, 2024
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Vegetation releases biogenic volatile organic compounds, while soils and lightning contribute to the natural emissions of nitrogen oxides into the atmosphere. These gases interact in complex ways. Using satellite data and models, we developed a new method to simultaneously optimise these natural emissions over Africa in 2019. Our approach led to an increase in natural emissions that is supported by independent data showing that current estimates are underestimated.
Tia R. Scarpelli, Paul I. Palmer, Mark Lunt, Ingrid Super, and Arjan Droste
Atmos. Chem. Phys., 24, 10773–10791, https://doi.org/10.5194/acp-24-10773-2024, https://doi.org/10.5194/acp-24-10773-2024, 2024
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Under the Paris Agreement, countries must track their anthropogenic greenhouse gas emissions. This study describes a method to determine self-consistent estimates for combustion emissions and natural fluxes of CO2 from atmospheric data. We report consistent estimates inferred using this approach from satellite data and ground-based data over Europe, suggesting that satellite data can be used to determine national anthropogenic CO2 emissions for countries where ground-based CO2 data are absent.
Yufen Wang, Ke Li, Xi Chen, Zhenjiang Yang, Minglong Tang, Pascoal M. D. Campos, Yang Yang, Xu Yue, and Hong Liao
EGUsphere, https://doi.org/10.5194/egusphere-2024-2576, https://doi.org/10.5194/egusphere-2024-2576, 2024
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The impact of biomass burning and anthropogenic emissions on high tropospheric ozone was not well studied in Southern Africa. We combined the model simulation with recent observations at the surface and from space to quantify tropospheric ozone and its main drivers in Southern Africa. Our work focuses on the impact of emissions from different sources at different spatial scales, contributing to a comprehensive understanding of air pollution drivers and their uncertainties in Southern Africa.
Wenbin Kou, Yang Gao, Dan Tong, Xiaojie Guo, Xiadong An, Wenyu Liu, Mengshi Cui, Xiuwen Guo, Shaoqing Zhang, Huiwang Gao, and Lixin Wu
EGUsphere, https://doi.org/10.5194/egusphere-2024-2500, https://doi.org/10.5194/egusphere-2024-2500, 2024
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Unlike traditional numerical studies, we apply a high-resolution Earth system model, improving simulations of ozone and large-scale circulations such as atmospheric blocking. In addition to local heatwave effects, we quantify the impact of atmospheric blocking on downstream ozone concentrations, which is closely associated with the blocking position. We identify three major pathways of Rossby wave propagation, stressing the critical role of large-scale circulation play in regional air quality.
Qianqian Zhang, K. Folkert Boersma, Chiel van der Laan, Alba Mols, Bin Zhao, Shengyue Li, and Yuepeng Pan
EGUsphere, https://doi.org/10.5194/egusphere-2024-2641, https://doi.org/10.5194/egusphere-2024-2641, 2024
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Accurate NOx emission estimates are required to better understand air pollution. This study investigates and demonstrates the ability of the superposition column model in combination with TROPOMI tropospheric NO2 column data to estimate city-scale NOx emissions and lifetimes and their variabilities. The results of this work nevertheless confirm the strength of the superposition column model in estimating urban NOx emissions with reasonable accuracy.
Ryan J. Pound, Lucy V. Brown, Mat J. Evans, and Lucy J. Carpenter
Atmos. Chem. Phys., 24, 9899–9921, https://doi.org/10.5194/acp-24-9899-2024, https://doi.org/10.5194/acp-24-9899-2024, 2024
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Iodine-mediated loss of ozone to the ocean surface and the subsequent emission of iodine species has a large effect on the troposphere. Here we combine recent experimental insights to develop a box model of the process, which we then parameterize and incorporate into the GEOS-Chem transport model. We find that these new insights have a small impact on the total emission of iodine but significantly change its distribution.
Mingzhao Liu, Lars Hoffmann, Jens-Uwe Grooß, Zhongyin Cai, Sabine Grießbach, and Yi Heng
EGUsphere, https://doi.org/10.5194/egusphere-2024-2596, https://doi.org/10.5194/egusphere-2024-2596, 2024
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We studied the transport and chemical decomposition of volcanic SO2, focusing on the 2019 Raikoke event. By comparing two different chemistry modeling schemes, we found that including complex chemical reactions leads to a more accurate prediction of how long SO2 stays in the atmosphere. This research helps improve our understanding of volcanic pollution and its impact on air quality and climate, providing better tools for scientists to track and predict the movement of these pollutants.
Alok K. Pandey, David S. Stevenson, Alcide Zhao, Richard J. Pope, Ryan Hossaini, Krishan Kumar, and Marytn P. Chipperfield
EGUsphere, https://doi.org/10.5194/egusphere-2024-2686, https://doi.org/10.5194/egusphere-2024-2686, 2024
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Nitrogen dioxide is an air pollutant largely controlled by human activity that affects ozone, methane and aerosols. Satellite instruments can quantify column NO2, and by carefully matching the time and location of measurements, enable evaluation of model simulations. NO2 over SE Asia is assessed, showing that the model captures many features of the measurements, but also important differences that suggest model deficiencies in representing several aspects of the atmospheric chemistry of NO2.
Katherine R. Travis, Benjamin A. Nault, James H. Crawford, Kelvin H. Bates, Donald R. Blake, Ronald C. Cohen, Alan Fried, Samuel R. Hall, L. Gregory Huey, Young Ro Lee, Simone Meinardi, Kyung-Eun Min, Isobel J. Simpson, and Kirk Ullman
Atmos. Chem. Phys., 24, 9555–9572, https://doi.org/10.5194/acp-24-9555-2024, https://doi.org/10.5194/acp-24-9555-2024, 2024
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Human activities result in the emission of volatile organic compounds (VOCs) that contribute to air pollution. Detailed VOC measurements were taken during a field study in South Korea. When compared to VOC inventories, large discrepancies showed underestimates from chemical products, liquefied petroleum gas, and long-range transport. Improved emissions and chemistry of these VOCs better described urban pollution. The new chemical scheme is relevant to urban areas and other VOC sources.
Beth S. Nelson, Zhenze Liu, Freya A. Squires, Marvin Shaw, James R. Hopkins, Jacqueline F. Hamilton, Andrew R. Rickard, Alastair C. Lewis, Zongbo Shi, and James D. Lee
Atmos. Chem. Phys., 24, 9031–9044, https://doi.org/10.5194/acp-24-9031-2024, https://doi.org/10.5194/acp-24-9031-2024, 2024
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The impact of combined air quality and carbon neutrality policies on O3 formation in Beijing was investigated. Emissions inventory data were used to estimate future pollutant mixing ratios relative to ground-level observations. O3 production was found to be most sensitive to changes in alkenes, but large reductions in less reactive compounds led to larger reductions in future O3 production. This study highlights the importance of understanding the emissions of organic pollutants.
Amir H. Souri, Bryan N. Duncan, Sarah A. Strode, Daniel C. Anderson, Michael E. Manyin, Junhua Liu, Luke D. Oman, Zhen Zhang, and Brad Weir
Atmos. Chem. Phys., 24, 8677–8701, https://doi.org/10.5194/acp-24-8677-2024, https://doi.org/10.5194/acp-24-8677-2024, 2024
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We explore a new method of using the wealth of information obtained from satellite observations of Aura OMI NO2, HCHO, and MERRA-2 reanalysis in NASA’s GEOS model equipped with an efficient tropospheric OH (TOH) estimator to enhance the representation of TOH spatial distribution and its long-term trends. This new framework helps us pinpoint regional inaccuracies in TOH and differentiate between established prior knowledge and newly acquired information from satellites on TOH trends.
Haipeng Lin, Louisa K. Emmons, Elizabeth W. Lundgren, Laura Hyesung Yang, Xu Feng, Ruijun Dang, Shixian Zhai, Yunxiao Tang, Makoto M. Kelp, Nadia K. Colombi, Sebastian D. Eastham, Thibaud M. Fritz, and Daniel J. Jacob
Atmos. Chem. Phys., 24, 8607–8624, https://doi.org/10.5194/acp-24-8607-2024, https://doi.org/10.5194/acp-24-8607-2024, 2024
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Tropospheric ozone is a major air pollutant, a greenhouse gas, and a major indicator of model skill. Global atmospheric chemistry models show large differences in simulations of tropospheric ozone, but isolating sources of differences is complicated by different model environments. By implementing the GEOS-Chem model side by side to CAM-chem within a common Earth system model, we identify and evaluate specific differences between the two models and their impacts on key chemical species.
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Xu, X., Wang, J., Henze, D. K., Qu, W., and Kopacz, M.: Constraints on
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Short summary
We developed four different methods to downscale SO2 and NO2 emissions derived from OMPS satellite observations (in Part 1) for regional air quality modeling at a spatial resolution that is finer than satellite observations. The VIIRS (city lights), TROPOMI, and OMI satellite data as well as surface data are used to evaluate the model. The method of using the top-down emissions from the past month for the air quality forecast in the present month is also shown to have practical merit.
We developed four different methods to downscale SO2 and NO2 emissions derived from OMPS...
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