Articles | Volume 21, issue 11
Atmos. Chem. Phys., 21, 8747–8759, 2021
https://doi.org/10.5194/acp-21-8747-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Atmos. Chem. Phys., 21, 8747–8759, 2021
https://doi.org/10.5194/acp-21-8747-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article 10 Jun 2021
Research article | 10 Jun 2021
Impact of international shipping emissions on ozone and PM2.5 in East Asia during summer: the important role of HONO and ClNO2
Jianing Dai and Tao Wang
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Yuting Wang, Yong-Feng Ma, Domingo Muñoz-Esparza, Cathy W. Y. Li, Mary Barth, Tao Wang, and Guy P. Brasseur
Atmos. Chem. Phys., 21, 3531–3553, https://doi.org/10.5194/acp-21-3531-2021, https://doi.org/10.5194/acp-21-3531-2021, 2021
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Large-eddy simulations (LESs) were performed in the mountainous region of the island of Hong Kong to investigate the degree to which the rates of chemical reactions between two reactive species are reduced due to the segregation of species within the convective boundary layer. We show that the inhomogeneity in emissions plays an important role in the segregation effect. Topography also has a significant influence on the segregation locally.
Men Xia, Xiang Peng, Weihao Wang, Chuan Yu, Zhe Wang, Yee Jun Tham, Jianmin Chen, Hui Chen, Yujing Mu, Chenglong Zhang, Pengfei Liu, Likun Xue, Xinfeng Wang, Jian Gao, Hong Li, and Tao Wang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-104, https://doi.org/10.5194/acp-2021-104, 2021
Revised manuscript under review for ACP
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ClNO2 is an important precursor of chlorine radical that affects photochemistry. However, its production and impact are not well understood. Our study presents field observations of ClNO2 at three sites in northern China. These observations provide new insights into nighttime processes that produce ClNO2, and the significant impact of ClNO2 on secondary pollutions during daytime. The results improve the understanding of photochemical pollution in the lower part of the atmosphere.
Yujiao Zhu, Likun Xue, Jian Gao, Jianmin Chen, Hongyong Li, Yong Zhao, Zhaoxin Guo, Tianshu Chen, Liang Wen, Penggang Zheng, Ye Shan, Xinfeng Wang, Tao Wang, Xiaohong Yao, and Wenxing Wang
Atmos. Chem. Phys., 21, 1305–1323, https://doi.org/10.5194/acp-21-1305-2021, https://doi.org/10.5194/acp-21-1305-2021, 2021
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This work investigates the long-term changes in new particle formation (NPF) events under reduced SO2 emissions at the summit of Mt. Tai during seven campaigns from 2007 to 2018. We found the NPF intensity increased 2- to 3-fold in 2018 compared to 2007. In contrast, the probability of new particles growing to CCN size largely decreased. Changes to biogenic VOCs and anthropogenic emissions are proposed to explain the distinct NPF characteristics.
Thierno Doumbia, Claire Granier, Nellie Elguindi, Idir Bouarar, Sabine Darras, Guy Brasseur, Benjamin Gaubert, Yiming Liu, Xiaoqin Shi, Trissevgeni Stavrakou, Simone Tilmes, Forrest Lacey, Adrien Deroubaix, and Tao Wang
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2020-348, https://doi.org/10.5194/essd-2020-348, 2021
Preprint under review for ESSD
Zhenhao Ling, Qianqian Xie, Min Shao, Zhe Wang, Tao Wang, Hai Guo, and Xuemei Wang
Atmos. Chem. Phys., 20, 11451–11467, https://doi.org/10.5194/acp-20-11451-2020, https://doi.org/10.5194/acp-20-11451-2020, 2020
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The observation data from a receptor site in the Pearl River Delta region were analyzed by a photochemical box model with near-explicit chemical mechanisms (i.e., the Master Chemical Mechanism, MCM), improvements with reversible and irreversible heterogeneous processes of glyoxal and methylglyoxal, and the gas-particle partitioning of oxidation products in the present study.
Wei Pu, Zhouxing Zou, Weihao Wang, David Tanner, Zhe Wang, and Tao Wang
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2020-252, https://doi.org/10.5194/amt-2020-252, 2020
Revised manuscript not accepted
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The hydroxyl radical (OH) is responsible for the degradation of trace gases and plays key roles in major environmental issues such as photochemical pollution. However, the measurement of atmospheric OH radical is a huge challenge due to its high reactivity. Our study provides systematic optimization of a chemical ionization mass spectrometer (CIMS) for OH measurement as a reference for other CIMS users. The ambient result demonstrates the capability of the CIMS for ambient OH measurement.
Yiming Liu and Tao Wang
Atmos. Chem. Phys., 20, 6305–6321, https://doi.org/10.5194/acp-20-6305-2020, https://doi.org/10.5194/acp-20-6305-2020, 2020
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This study revealed the effects of changes in meteorology and anthropogenic emissions on the summer ozone variations from 2013 to 2017 across China by conducting numerical experiments. We highlighted the important but varying roles of meteorology in ozone variations attributed to the synergistic or counteracting effects from individual meteorological factors. Developing future ozone pollution mitigation policies should consider the counteracting impact of meteorological changes.
Yiming Liu and Tao Wang
Atmos. Chem. Phys., 20, 6323–6337, https://doi.org/10.5194/acp-20-6323-2020, https://doi.org/10.5194/acp-20-6323-2020, 2020
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Surface ozone levels in urban areas of China were increasing despite the implementation of stringent emission control measures since 2013. Our modeling results show that the decrease in NOx, SO2, and PM emissions and increase in VOC emissions contributed to the urban ozone increases due to the nonlinear ozone chemistry and complex aerosol affects. VOC reduction measures should be implemented in the current and future policies to achieve the goal of improving the overall air quality.
Men Xia, Xiang Peng, Weihao Wang, Chuan Yu, Peng Sun, Yuanyuan Li, Yuliang Liu, Zhengning Xu, Zhe Wang, Zheng Xu, Wei Nie, Aijun Ding, and Tao Wang
Atmos. Chem. Phys., 20, 6147–6158, https://doi.org/10.5194/acp-20-6147-2020, https://doi.org/10.5194/acp-20-6147-2020, 2020
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ClNO2 and Cl2 can be photolyzed by sunlight to produce a highly reactive Cl atom which affects air quality and climate. We observed high ClNO2 and Cl2 concentrations during a recent field study in east China. We analyzed the data and proposed a new hypothesis on the Cl2 production mechanism. Yields of ClNO2 and Cl2 from N2O2 uptake were parameterized using observational constraints, and they can be used in air quality models to improve simulations of atmospheric photochemistry and air quality.
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, https://doi.org/10.5194/acp-20-4809-2020, 2020
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Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
Chuan Yu, Zhe Wang, Men Xia, Xiao Fu, Weihao Wang, Yee Jun Tham, Tianshu Chen, Penggang Zheng, Hongyong Li, Ye Shan, Xinfeng Wang, Likun Xue, Yan Zhou, Dingli Yue, Yubo Ou, Jian Gao, Keding Lu, Steven S. Brown, Yuanhang Zhang, and Tao Wang
Atmos. Chem. Phys., 20, 4367–4378, https://doi.org/10.5194/acp-20-4367-2020, https://doi.org/10.5194/acp-20-4367-2020, 2020
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This study provides a holistic picture of N2O5 heterogeneous uptake on ambient aerosols and the influencing factors under various climatic and chemical conditions in China, and it proposes an observation-based empirical parameterization. The empirical parameterization can be used in air quality models to improve the prediction of PM2.5 and photochemical pollution in China and similar polluted regions of the world.
Tao Li, Zhe Wang, Yaru Wang, Chen Wu, Yiheng Liang, Men Xia, Chuan Yu, Hui Yun, Weihao Wang, Yan Wang, Jia Guo, Hartmut Herrmann, and Tao Wang
Atmos. Chem. Phys., 20, 391–407, https://doi.org/10.5194/acp-20-391-2020, https://doi.org/10.5194/acp-20-391-2020, 2020
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This work presents a field study of cloud water chemistry and interactions of cloud, gas, and aerosols in the polluted coastal boundary layer in southern China. Substantial dissolved organic matter in the acidic cloud water was observed, and the gas- and aqueous-phase partitioning of carbonyl compounds was investigated. The results demonstrated the significant role of cloud processing in altering aerosol properties, especially in producing aqueous organics and droplet-mode aerosols.
Lu Shen, Daniel J. Jacob, Xiong Liu, Guanyu Huang, Ke Li, Hong Liao, and Tao Wang
Atmos. Chem. Phys., 19, 6551–6560, https://doi.org/10.5194/acp-19-6551-2019, https://doi.org/10.5194/acp-19-6551-2019, 2019
Xiao Fu, Tao Wang, Li Zhang, Qinyi Li, Zhe Wang, Men Xia, Hui Yun, Weihao Wang, Chuan Yu, Dingli Yue, Yan Zhou, Junyun Zheng, and Rui Han
Atmos. Chem. Phys., 19, 1–14, https://doi.org/10.5194/acp-19-1-2019, https://doi.org/10.5194/acp-19-1-2019, 2019
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This study has identified the major contributors to the observed high HONO levels during a severe winter pollution episode and highlighted the importance of HONO chemistry in the combined photochemical and haze pollution in a subtropical region. It also highlighted the critical need to include and update HONO sources in regional air quality models in order to predict ozone and other secondary pollutants better during heavy pollution events in southern China and similar regions.
Hui Yun, Weihao Wang, Tao Wang, Men Xia, Chuan Yu, Zhe Wang, Steven C. N. Poon, Dingli Yue, and Yan Zhou
Atmos. Chem. Phys., 18, 17515–17527, https://doi.org/10.5194/acp-18-17515-2018, https://doi.org/10.5194/acp-18-17515-2018, 2018
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Based on the data analysis of simultaneous measurement of N2O5 and ClNO2 in a severe winter haze in the Pearl River Delta, this study underscores the importance of N2O5 heterogeneous reactions in nitrate formation and calls for better parameterization of N2O5 heterogeneous chemistry in order to predict haze pollution in China.
Weihao Wang, Zhe Wang, Chuan Yu, Men Xia, Xiang Peng, Yan Zhou, Dingli Yue, Yubo Ou, and Tao Wang
Atmos. Meas. Tech., 11, 5643–5655, https://doi.org/10.5194/amt-11-5643-2018, https://doi.org/10.5194/amt-11-5643-2018, 2018
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This study introduces an in situ experimental approach to direct measurement of N2O5 heterogeneous reactivity in polluted environments. Laboratory tests, model simulations, and field deployment of the method at a polluted site in south China demonstrated its applicability in accurately measuring N2O5 uptake coefficient with high ambient pollutants levels and air mass changes. The introduced method is also applicable to in situ measurement of reactivity of other trace gases on ambient aerosols.
Yee Jun Tham, Zhe Wang, Qinyi Li, Weihao Wang, Xinfeng Wang, Keding Lu, Nan Ma, Chao Yan, Simonas Kecorius, Alfred Wiedensohler, Yuanhang Zhang, and Tao Wang
Atmos. Chem. Phys., 18, 13155–13171, https://doi.org/10.5194/acp-18-13155-2018, https://doi.org/10.5194/acp-18-13155-2018, 2018
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This study addresses the limited understanding of heterogeneous N2O5 uptake and ClNO2 production in the polluted environment of China. The results showed that N2O5 uptake and ClNO2 yield cannot be well explained by previous parameterizations and were largely influenced by factors like aerosol water content and biomass burning emission. Our findings illuminate the need to realistically parameterize these heterogeneous processes for better simulation of photochemical and haze pollution in China.
Michael Le Breton, Åsa M. Hallquist, Ravi Kant Pathak, David Simpson, Yujue Wang, John Johansson, Jing Zheng, Yudong Yang, Dongjie Shang, Haichao Wang, Qianyun Liu, Chak Chan, Tao Wang, Thomas J. Bannan, Michael Priestley, Carl J. Percival, Dudley E. Shallcross, Keding Lu, Song Guo, Min Hu, and Mattias Hallquist
Atmos. Chem. Phys., 18, 13013–13030, https://doi.org/10.5194/acp-18-13013-2018, https://doi.org/10.5194/acp-18-13013-2018, 2018
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We apply state-of-the-art chemical characterization to determine the chloride radical production in Beijing via measurement of inorganic halogens at a semi-rural site. The high concentration of inorganic halogens, namely nitryl chloride, enables the production of chlorinated volatile organic compounds which are measured in both the gas and particle phases simultaneously. This enables the secondary production of aerosols via chlorine oxidation to be directly observed in ambient air.
Liang Wen, Likun Xue, Xinfeng Wang, Caihong Xu, Tianshu Chen, Lingxiao Yang, Tao Wang, Qingzhu Zhang, and Wenxing Wang
Atmos. Chem. Phys., 18, 11261–11275, https://doi.org/10.5194/acp-18-11261-2018, https://doi.org/10.5194/acp-18-11261-2018, 2018
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We present the first piece of observational evidence of the increasing trend of fine nitrate aerosol in the North China Plain (NCP) during 2005–2015. The summertime nitrate formation mechanism is dissected with a multiphase chemical box model based on observations at three different sites. The nitrate formation is most sensitive to NO2 and to a lesser extent to O3. NH3 plays a significant role in prompting the nitrate formation, but it is usually in excess in summer in the NCP region.
Liwei Wang, Xinfeng Wang, Rongrong Gu, Hao Wang, Lan Yao, Liang Wen, Fanping Zhu, Weihao Wang, Likun Xue, Lingxiao Yang, Keding Lu, Jianmin Chen, Tao Wang, Yuanghang Zhang, and Wenxing Wang
Atmos. Chem. Phys., 18, 4349–4359, https://doi.org/10.5194/acp-18-4349-2018, https://doi.org/10.5194/acp-18-4349-2018, 2018
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This study presents concentrations, variation characteristics, sources and secondary formations of nitrated phenols, a major component of brown carbon, in typical seasons at four sites in northern China. The results highlight the strong influences and contributions of anthropogenic activities, in particular coal combustion and the aging processes, to the atmospheric nitrated phenols in this region.
Zhe Wang, Weihao Wang, Yee Jun Tham, Qinyi Li, Hao Wang, Liang Wen, Xinfeng Wang, and Tao Wang
Atmos. Chem. Phys., 17, 12361–12378, https://doi.org/10.5194/acp-17-12361-2017, https://doi.org/10.5194/acp-17-12361-2017, 2017
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This work addresses unclear roles of heterogeneous N2O5 reactions and chlorine activation processes in the polluted residual layer from a mountaintop measurement in northern China. The results revealed efficient ClNO2 production in the coal-fired plumes in this region, having large impacts on next-morning photochemistry. Fast heterogeneous N2O5 reactions dominate the nocturnal NOx loss and contribute to substantial nitrate formation, which may boost the haze pollution in northern China.
Li Zhang, Qinyi Li, Tao Wang, Ravan Ahmadov, Qiang Zhang, Meng Li, and Mengyao Lv
Atmos. Chem. Phys., 17, 9733–9750, https://doi.org/10.5194/acp-17-9733-2017, https://doi.org/10.5194/acp-17-9733-2017, 2017
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Little is known of the integrated impacts of HONO and ClNO2 on lower-tropospheric ozone so far. In this study, we updated WRF-Chem with the CBMZ_ReNOM module, which considers both the sources and chemistry of HONO and ClNO2. The revised model revealed that the two reactive nitrogen compounds significantly affected the oxidation capacity and ozone formation at the surface and within the lower troposphere over polluted regions and noticeably improved summertime O3 predictions over China.
Jiaping Wang, Aki Virkkula, Yuan Gao, Shuncheng Lee, Yicheng Shen, Xuguang Chi, Wei Nie, Qiang Liu, Zheng Xu, Xin Huang, Tao Wang, Long Cui, and Aijun Ding
Atmos. Chem. Phys., 17, 2653–2671, https://doi.org/10.5194/acp-17-2653-2017, https://doi.org/10.5194/acp-17-2653-2017, 2017
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Multi-year observations at a coastal station in Hong Kong reveals that aerosol optical properties showed clear temporal variations according to the dominant sources of aerosols. LPDM modeling and correlation analysis gave similar signals about the freshness of aerosols during different seasons. Fresh emissions of particles from nearby cities and ship exhausts affected light optical properties and particle size in summer and aged air mass in winter caused larger variability of light extinction.
Yee Jun Tham, Zhe Wang, Qinyi Li, Hui Yun, Weihao Wang, Xinfeng Wang, Likun Xue, Keding Lu, Nan Ma, Birger Bohn, Xin Li, Simonas Kecorius, Johannes Größ, Min Shao, Alfred Wiedensohler, Yuanhang Zhang, and Tao Wang
Atmos. Chem. Phys., 16, 14959–14977, https://doi.org/10.5194/acp-16-14959-2016, https://doi.org/10.5194/acp-16-14959-2016, 2016
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This work addresses the unclear global significance of chlorine activation processes in the troposphere. The first high-quality measurement data set of ClNO2 in northern China revealed strong ClNO2 production in the residual layers, and demonstrated its significant effects on radical budget and ozone production. Our findings imply the widespread effects of ClNO2 over the polluted regions of northern China, which may increase photochemical and haze pollution.
Qinyi Li, Li Zhang, Tao Wang, Yee Jun Tham, Ravan Ahmadov, Likun Xue, Qiang Zhang, and Junyu Zheng
Atmos. Chem. Phys., 16, 14875–14890, https://doi.org/10.5194/acp-16-14875-2016, https://doi.org/10.5194/acp-16-14875-2016, 2016
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The regional distributions and impacts of N2O5 and ClNO2 remain poorly understood. To address the problem, we developed a chemical transport model further and conducted the first high-resolution simulation of the distributions of the two species. Our research demonstrated the significant impacts of the two gases on the lifetime of nitrogen oxides, secondary nitrate production and ozone formation in southern China and highlighted the necessity of considering this chemistry in air quality models.
Lei Sun, Likun Xue, Tao Wang, Jian Gao, Aijun Ding, Owen R. Cooper, Meiyun Lin, Pengju Xu, Zhe Wang, Xinfeng Wang, Liang Wen, Yanhong Zhu, Tianshu Chen, Lingxiao Yang, Yan Wang, Jianmin Chen, and Wenxing Wang
Atmos. Chem. Phys., 16, 10637–10650, https://doi.org/10.5194/acp-16-10637-2016, https://doi.org/10.5194/acp-16-10637-2016, 2016
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We compiled the available observations of surface O3 at Mt. Tai – the highest mountain in the North China Plain, and found a significant increase of O3 concenrations from 2003 to 2015. The observed O3 increase was mainly due to the increase of O3 precursors, especially VOCs. Our analysis shows that controlling NOx alone, in the absence of VOC controls, is not sufficient to reduce regional O3 levels in North China in a short period.
Likun Xue, Rongrong Gu, Tao Wang, Xinfeng Wang, Sandra Saunders, Donald Blake, Peter K. K. Louie, Connie W. Y. Luk, Isobel Simpson, Zheng Xu, Zhe Wang, Yuan Gao, Shuncheng Lee, Abdelwahid Mellouki, and Wenxing Wang
Atmos. Chem. Phys., 16, 9891–9903, https://doi.org/10.5194/acp-16-9891-2016, https://doi.org/10.5194/acp-16-9891-2016, 2016
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The chemical budgets and principal sources of ROx and NO3 radicals during a multi-day photochemical smog episode in Hong Kong are elucidated by an observation-constrained MCM model. NO3 was shown to be an important oxidant even during daytime in a pollution case when high aerosol loading attenuated the solar irradiation. This study suggests the potential important role of daytime NO3 chemistry in polluted atmospheres under conditions with the co-existence of abundant O3, NO2, VOCs, and aerosols.
L. K. Xue, S. M. Saunders, T. Wang, R. Gao, X. F. Wang, Q. Z. Zhang, and W. X. Wang
Geosci. Model Dev., 8, 3151–3162, https://doi.org/10.5194/gmd-8-3151-2015, https://doi.org/10.5194/gmd-8-3151-2015, 2015
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A detailed chemical mechanism including 205 reactions is developed for use in the Master Chemical Mechanism. With this new chlorine mechanism, it was found that the nocturnal formation of ClNO2 has high potential to perturb the next day's atmospheric photochemistry, by enhancing the radical production and cycling, VOC oxidation and O3 formation, in the polluted coastal environments.
T. Li, Y. Wang, W. J. Li, J. M. Chen, T. Wang, and W. X. Wang
Atmos. Chem. Phys., 15, 8987–9002, https://doi.org/10.5194/acp-15-8987-2015, https://doi.org/10.5194/acp-15-8987-2015, 2015
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Twelve trace elements in fine particles and clouds at a mountain site in southern China were investigated.
Long-range transport contributed the most to element concentrations, whereas the YRD and the area around Mt. Lushan exhibited the highest element solubility.
We demonstrated that cloud processing can enhance aerosol element solubility and increase sulfate concentration correspondingly, by irreversibly altering the morphology of metal particles in cloud droplet residues.
L. K. Xue, T. Wang, J. Gao, A. J. Ding, X. H. Zhou, D. R. Blake, X. F. Wang, S. M. Saunders, S. J. Fan, H. C. Zuo, Q. Z. Zhang, and W. X. Wang
Atmos. Chem. Phys., 14, 13175–13188, https://doi.org/10.5194/acp-14-13175-2014, https://doi.org/10.5194/acp-14-13175-2014, 2014
X. Wang, T. Wang, C. Yan, Y. J. Tham, L. Xue, Z. Xu, and Q. Zha
Atmos. Meas. Tech., 7, 1–12, https://doi.org/10.5194/amt-7-1-2014, https://doi.org/10.5194/amt-7-1-2014, 2014
L. K. Xue, T. Wang, J. Gao, A. J. Ding, X. H. Zhou, D. R. Blake, X. F. Wang, S. M. Saunders, S. J. Fan, H. C. Zuo, Q. Z. Zhang, and W. X. Wang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-13-27243-2013, https://doi.org/10.5194/acpd-13-27243-2013, 2013
Revised manuscript not accepted
L. K. Xue, T. Wang, H. Guo, D. R. Blake, J. Tang, X. C. Zhang, S. M. Saunders, and W. X. Wang
Atmos. Chem. Phys., 13, 8551–8567, https://doi.org/10.5194/acp-13-8551-2013, https://doi.org/10.5194/acp-13-8551-2013, 2013
W. Nie, T. Wang, L. K. Xue, A. J. Ding, X. F. Wang, X. M. Gao, Z. Xu, Y. C. Yu, C. Yuan, Z. S. Zhou, R. Gao, X. H. Liu, Y. Wang, S. J. Fan, S. Poon, Q. Z. Zhang, and W. X. Wang
Atmos. Chem. Phys., 12, 11985–11995, https://doi.org/10.5194/acp-12-11985-2012, https://doi.org/10.5194/acp-12-11985-2012, 2012
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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Simon Rosanka, Bruno Franco, Lieven Clarisse, Pierre-François Coheur, Andrea Pozzer, Andreas Wahner, and Domenico Taraborrelli
Atmos. Chem. Phys., 21, 11257–11288, https://doi.org/10.5194/acp-21-11257-2021, https://doi.org/10.5194/acp-21-11257-2021, 2021
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The strong El Niño in 2015 led to a particular dry season in Indonesia and favoured severe peatland fires. The smouldering conditions of these fires and the high carbon content of peat resulted in high volatile organic compound (VOC) emissions. By using a comprehensive atmospheric model, we show that these emissions have a significant impact on the tropospheric composition and oxidation capacity. These emissions are transported into to the lower stratosphere, resulting in a depletion of ozone.
Jianfeng Li, Yuhang Wang, Ruixiong Zhang, Charles Smeltzer, Andrew Weinheimer, Jay Herman, K. Folkert Boersma, Edward A. Celarier, Russell W. Long, James J. Szykman, Ruben Delgado, Anne M. Thompson, Travis N. Knepp, Lok N. Lamsal, Scott J. Janz, Matthew G. Kowalewski, Xiong Liu, and Caroline R. Nowlan
Atmos. Chem. Phys., 21, 11133–11160, https://doi.org/10.5194/acp-21-11133-2021, https://doi.org/10.5194/acp-21-11133-2021, 2021
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Comprehensive evaluations of simulated diurnal cycles of NO2 and NOy concentrations, vertical profiles, and tropospheric vertical column densities at two different resolutions with various measurements during the DISCOVER-AQ 2011 campaign show potential distribution biases of NOx emissions in the National Emissions Inventory 2011 at both 36 and 4 km resolutions, providing another possible explanation for the overestimation of model results.
Roman Nuterman, Alexander Mahura, Alexander Baklanov, Bjarne Amstrup, and Ashraf Zakey
Atmos. Chem. Phys., 21, 11099–11112, https://doi.org/10.5194/acp-21-11099-2021, https://doi.org/10.5194/acp-21-11099-2021, 2021
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The street air pollution is usually higher than the pollution at regional and urban scales. It mostly associated with both local emission sources and urban weather conditions. We present the downscaling system for regional, subregional-urban and street scales and evaluate it for acute air-pollution episode. Its evaluation showed a good prediction score across various spatiotemporal scales as well as feasibility of deterministic modelling approach for the operational street scale forecasting.
Min Huang, James H. Crawford, Joshua P. DiGangi, Gregory R. Carmichael, Kevin W. Bowman, Sujay V. Kumar, and Xiwu Zhan
Atmos. Chem. Phys., 21, 11013–11040, https://doi.org/10.5194/acp-21-11013-2021, https://doi.org/10.5194/acp-21-11013-2021, 2021
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This study evaluates the impact of satellite soil moisture data assimilation on modeled weather and ozone fields at various altitudes above the southeastern US during the summer. It emphasizes the importance of soil moisture in the understanding of surface ozone pollution and upper tropospheric chemistry, as well as air pollutants’ source–receptor relationships between the US and its downwind areas.
Yingnan Zhang, Likun Xue, William P. L. Carter, Chenglei Pei, Tianshu Chen, Jiangshan Mu, Yujun Wang, Qingzhu Zhang, and Wenxing Wang
Atmos. Chem. Phys., 21, 11053–11068, https://doi.org/10.5194/acp-21-11053-2021, https://doi.org/10.5194/acp-21-11053-2021, 2021
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We developed the localized incremental reactivity (IR) for VOCs in a Chinese megacity and elucidated their applications in calculating the ozone formation potential (OFP). The IR scales showed a strong dependence on chemical mechanisms. Both emission- and observation-based inputs are suitable for the MIR calculation but not the case under mixed-limited or NOx-limited O3 formation regimes. We provide suggestions for the application of IR and OFP scales to aid in VOC control in China.
Ilaria D'Elia, Gino Briganti, Lina Vitali, Antonio Piersanti, Gaia Righini, Massimo D'Isidoro, Andrea Cappelletti, Mihaela Mircea, Mario Adani, Gabriele Zanini, and Luisella Ciancarella
Atmos. Chem. Phys., 21, 10825–10849, https://doi.org/10.5194/acp-21-10825-2021, https://doi.org/10.5194/acp-21-10825-2021, 2021
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We present an analysis of modelled trends of PM10, NO2, and O3 airborne concentrations over the Italian territory in 2003–2010. Our analysis shows a general downward simulated trend for all pollutants, with good agreement between observed and modelled values and the model widening both coverage and significance of air concentration trends. Due to the complex atmospheric dynamics, emission reductions do not always result in decreasing concentrations, especially for secondary pollutants.
Chris Wilson, Martyn P. Chipperfield, Manuel Gloor, Robert J. Parker, Hartmut Boesch, Joey McNorton, Luciana V. Gatti, John B. Miller, Luana S. Basso, and Sarah A. Monks
Atmos. Chem. Phys., 21, 10643–10669, https://doi.org/10.5194/acp-21-10643-2021, https://doi.org/10.5194/acp-21-10643-2021, 2021
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Methane (CH4) is an important greenhouse gas emitted from wetlands like those found in the basin of the Amazon River. Using an atmospheric model and observations from GOSAT, we quantified CH4 emissions from Amazonia during the previous decade. We found that the largest emissions came from a region in the eastern basin and that emissions there were rising faster than in other areas of South America. This finding was supported by CH4 observations made on aircraft within the basin.
Zhenze Liu, Ruth M. Doherty, Oliver Wild, Michael Hollaway, and Fiona M. O’Connor
Atmos. Chem. Phys., 21, 10689–10706, https://doi.org/10.5194/acp-21-10689-2021, https://doi.org/10.5194/acp-21-10689-2021, 2021
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Surface ozone (O3) has become the main cause of atmospheric pollution in the summertime in China since 2013. We find that 70 % reductions in NOx emissions are required to reduce O3 pollution in most of industrial regions of China, and controls in VOC emissions are very important. The new chemical scheme developed for a global chemistry–climate model not only captures the regional air pollution but also benefits the future studies of regional air-quality–climate interactions.
Peng Wang, Juanyong Shen, Men Xia, Shida Sun, Yanli Zhang, Hongliang Zhang, and Xinming Wang
Atmos. Chem. Phys., 21, 10347–10356, https://doi.org/10.5194/acp-21-10347-2021, https://doi.org/10.5194/acp-21-10347-2021, 2021
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Ozone (O3) pollution has received extensive attention due to worsening air quality and rising health risks. The Chinese National Day holiday (CNDH), which is associated with intensive commercial and tourist activities, serves as a valuable experiment to evaluate the O3 response during the holiday. We find sharply increasing trends of observed O3 concentrations throughout China during the CNDH, leading to 33 % additional total daily deaths.
Johannes G. M. Barten, Laurens N. Ganzeveld, Gert-Jan Steeneveld, and Maarten C. Krol
Atmos. Chem. Phys., 21, 10229–10248, https://doi.org/10.5194/acp-21-10229-2021, https://doi.org/10.5194/acp-21-10229-2021, 2021
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We present an evaluation of ocean and snow/ice O3 deposition in explaining observed hourly surface O3 at 25 pan-Arctic sites using an atmospheric meteorology/chemistry model. The model includes a mechanistic representation of ocean O3 deposition as a function of ocean biogeochemical and mixing conditions. The mechanistic representation agrees better with O3 observations in terms of magnitude and temporal variability especially in the High Arctic (> 70° N).
Simon Rosanka, Rolf Sander, Bruno Franco, Catherine Wespes, Andreas Wahner, and Domenico Taraborrelli
Atmos. Chem. Phys., 21, 9909–9930, https://doi.org/10.5194/acp-21-9909-2021, https://doi.org/10.5194/acp-21-9909-2021, 2021
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In-cloud destruction of ozone depends on hydroperoxyl radicals in cloud droplets, where they are produced by oxygenated volatile organic compound (OVOC) oxygenation. Only rudimentary representations of these processes, if any, are currently available in global atmospheric models. By using a comprehensive atmospheric model that includes a complex in-cloud OVOC oxidation scheme, we show that atmospheric oxidants are reduced and models ignoring this process will underpredict clouds as ozone sinks.
Brad Weir, Lesley E. Ott, George J. Collatz, Stephan R. Kawa, Benjamin Poulter, Abhishek Chatterjee, Tomohiro Oda, and Steven Pawson
Atmos. Chem. Phys., 21, 9609–9628, https://doi.org/10.5194/acp-21-9609-2021, https://doi.org/10.5194/acp-21-9609-2021, 2021
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We present a collection of carbon surface fluxes, the Low-order Flux Inversion (LoFI), derived from satellite observations of the Earth's surface and calibrated to match long-term inventories and atmospheric and oceanic records. Simulations using LoFI reproduce background atmospheric carbon dioxide measurements with comparable skill to the leading surface flux products. Available both retrospectively and as a forecast, LoFI enables the study of the carbon cycle as it occurs.
Ilya Stanevich, Dylan B. A. Jones, Kimberly Strong, Martin Keller, Daven K. Henze, Robert J. Parker, Hartmut Boesch, Debra Wunch, Justus Notholt, Christof Petri, Thorsten Warneke, Ralf Sussmann, Matthias Schneider, Frank Hase, Rigel Kivi, Nicholas M. Deutscher, Voltaire A. Velazco, Kaley A. Walker, and Feng Deng
Atmos. Chem. Phys., 21, 9545–9572, https://doi.org/10.5194/acp-21-9545-2021, https://doi.org/10.5194/acp-21-9545-2021, 2021
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We explore the utility of a weak-constraint (WC) four-dimensional variational (4D-Var) data assimilation scheme for mitigating systematic errors in methane simulation in the GEOS-Chem model. We use data from the Greenhouse Gases Observing Satellite (GOSAT) and show that, compared to the traditional 4D-Var approach, the WC scheme improves the agreement between the model and independent observations. We find that the WC corrections to the model provide insight into the source of the errors.
Yosuke Niwa, Yousuke Sawa, Hideki Nara, Toshinobu Machida, Hidekazu Matsueda, Taku Umezawa, Akihiko Ito, Shin-Ichiro Nakaoka, Hiroshi Tanimoto, and Yasunori Tohjima
Atmos. Chem. Phys., 21, 9455–9473, https://doi.org/10.5194/acp-21-9455-2021, https://doi.org/10.5194/acp-21-9455-2021, 2021
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Fires in Equatorial Asia release a large amount of carbon into the atmosphere. Extensively using high-precision atmospheric carbon dioxide (CO2) data from a commercial aircraft observation project, we estimated fire carbon emissions in Equatorial Asia induced by the big El Niño event in 2015. Additional shipboard measurement data elucidated the validity of the analysis and the best estimate indicated 273 Tg C for fire emissions during September–October 2015.
Christine Frömming, Volker Grewe, Sabine Brinkop, Patrick Jöckel, Amund S. Haslerud, Simon Rosanka, Jesper van Manen, and Sigrun Matthes
Atmos. Chem. Phys., 21, 9151–9172, https://doi.org/10.5194/acp-21-9151-2021, https://doi.org/10.5194/acp-21-9151-2021, 2021
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The influence of weather situations on non-CO2 aviation climate impact is investigated to identify systematic weather-related sensitivities. If aircraft avoid the most sensitive areas, climate impact might be reduced. Enhanced significance is found for emission in relation to high-pressure systems, jet stream, polar night, and tropopause altitude. The results represent a comprehensive data set for studies aiming at weather-dependent flight trajectory optimization to reduce total climate impact.
Anoop S. Mahajan, Qinyi Li, Swaleha Inamdar, Kirpa Ram, Alba Badia, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 21, 8437–8454, https://doi.org/10.5194/acp-21-8437-2021, https://doi.org/10.5194/acp-21-8437-2021, 2021
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Using a regional model, we show that iodine-catalysed reactions cause large regional changes in the chemical composition in the northern Indian Ocean, with peak changes of up to 25 % in O3, 50 % in nitrogen oxides (NO and NO2), 15 % in hydroxyl radicals (OH), 25 % in hydroperoxyl radicals (HO2), and up to a 50 % change in the nitrate radical (NO3). These results show the importance of including iodine chemistry in modelling the atmosphere in this region.
Maximilian Herrmann, Holger Sihler, Udo Frieß, Thomas Wagner, Ulrich Platt, and Eva Gutheil
Atmos. Chem. Phys., 21, 7611–7638, https://doi.org/10.5194/acp-21-7611-2021, https://doi.org/10.5194/acp-21-7611-2021, 2021
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Time-dependent 3D numerical simulations of tropospheric bromine release and ozone depletion events (ODEs) in the Arctic polar spring of 2009 are compared to observations. Simulation results agree well with the observations at both Utqiaġvik, Alaska, and at Summit, Greenland. In a parameter study, different settings for the bromine release mechanism are evaluated. An enhancement of the bromine release mechanism improves the agreement regarding the occurrence of ODEs with the observations.
Ashok K. Luhar, Ian E. Galbally, Matthew T. Woodhouse, and Nathan Luke Abraham
Atmos. Chem. Phys., 21, 7053–7082, https://doi.org/10.5194/acp-21-7053-2021, https://doi.org/10.5194/acp-21-7053-2021, 2021
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Lightning-generated nitrogen oxides (LNOx) greatly influence tropospheric photochemistry. The most common parameterisation of lightning flash rate used to calculate LNOx in global composition models underestimates measurements over the ocean by a factor of 20–25. We formulate and validate an alternative parameterisation to remedy this problem. The new scheme causes an increase in the ozone burden by 8.5 % and the hydroxyl radical by 13 %, and these have implications for climate and air quality.
Daniel M. Westervelt, Arlene M. Fiore, Colleen B. Baublitz, and Gustavo Correa
Atmos. Chem. Phys., 21, 6799–6810, https://doi.org/10.5194/acp-21-6799-2021, https://doi.org/10.5194/acp-21-6799-2021, 2021
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Particulate air pollution in the atmosphere can impact the availability of gas-phase chemical constituents, which can then have feedbacks on gas-phase air pollutants. We use a chemistry–climate computer model to simulate the impact of particulate pollution from three major world regions on gas-phase chemical constituents. We find that surface-level ozone air pollution decreases by up to 5 ppbv over China in response to Chinese particulate air pollution, which has implications for policy.
Ashu Dastoor, Andrei Ryjkov, Gregor Kos, Junhua Zhang, Jane Kirk, Matthew Parsons, and Alexandra Steffen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-296, https://doi.org/10.5194/acp-2021-296, 2021
Revised manuscript accepted for ACP
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An assessment of mercury levels in air and deposition in the Athabasca oil sands region (AOSR) in Northern Alberta, Canada, was conducted to investigate the contribution of Hg emitted from oil sands activities on the surrounding landscape using a 3D process-based Hg model in 2012–2015. Oil sands Hg emissions are found to be important sources of Hg contamination to the local landscape in proximity of the processing activities, particularly in wintertime.
Gabriel Isaacman-VanWertz and Bernard Aumont
Atmos. Chem. Phys., 21, 6541–6563, https://doi.org/10.5194/acp-21-6541-2021, https://doi.org/10.5194/acp-21-6541-2021, 2021
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There are tens of thousands of different chemical compounds in the atmosphere. To tackle this complexity, there are a wide range of different methods to estimate their physical and chemical properties. We use these methods to understand how much the detailed structure of a molecule impacts its properties, and the extent to which properties can be estimated without knowing this level of detail. We find that structure matters, but methods lacking that level of detail still perform reasonably well.
Daniel C. Anderson, Bryan N. Duncan, Arlene M. Fiore, Colleen B. Baublitz, Melanie B. Follette-Cook, Julie M. Nicely, and Glenn M. Wolfe
Atmos. Chem. Phys., 21, 6481–6508, https://doi.org/10.5194/acp-21-6481-2021, https://doi.org/10.5194/acp-21-6481-2021, 2021
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We demonstrate that large-scale climate features are the primary driver of year-to-year variability in simulated values of the hydroxyl radical, the primary atmospheric oxidant, over 1980–2018. The El Niño–Southern Oscillation is the dominant mode of hydroxyl variability, resulting in large-scale global decreases in OH during El Niño events. Other climate modes, such as the Australian monsoon and the North Atlantic Oscillation, have impacts of similar magnitude but on on more localized scales.
Pooja V. Pawar, Sachin D. Ghude, Chinmay Jena, Andrea Móring, Mark A. Sutton, Santosh Kulkarni, Deen Mani Lal, Divya Surendran, Martin Van Damme, Lieven Clarisse, Pierre-François Coheur, Xuejun Liu, Gaurav Govardhan, Wen Xu, Jize Jiang, and Tapan Kumar Adhya
Atmos. Chem. Phys., 21, 6389–6409, https://doi.org/10.5194/acp-21-6389-2021, https://doi.org/10.5194/acp-21-6389-2021, 2021
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In this study, simulations of atmospheric ammonia (NH3) with MOZART-4 and HTAP-v2 are compared with satellite (IASI) and ground-based measurements to understand the spatial and temporal variability of NH3 over two emission hotspot regions of Asia, the IGP and the NCP. Our simulations indicate that the formation of ammonium aerosols is quicker over the NCP than the IGP, leading to smaller NH3 columns over the higher NH3-emitting NCP compared to the IGP region for comparable emissions.
Yan Zhang, Yu Zhao, Meng Gao, Xin Bo, and Chris P. Nielsen
Atmos. Chem. Phys., 21, 6411–6430, https://doi.org/10.5194/acp-21-6411-2021, https://doi.org/10.5194/acp-21-6411-2021, 2021
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We combined air quality and exposure response models to analyze the benefits for air quality and human health of China’s ultra-low emission policy in one of its most developed regions. Atmospheric observations and the air quality model were also used to demonstrate improvement of emission inventories incorporating online emission monitoring data. With implementation of the policy in both power and industrial sectors, the attributable deaths due to PM2.5 exposure are estimated to decrease 5.5 %.
Anna Karion, Israel Lopez-Coto, Sharon M. Gourdji, Kimberly Mueller, Subhomoy Ghosh, William Callahan, Michael Stock, Elizabeth DiGangi, Steve Prinzivalli, and James Whetstone
Atmos. Chem. Phys., 21, 6257–6273, https://doi.org/10.5194/acp-21-6257-2021, https://doi.org/10.5194/acp-21-6257-2021, 2021
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Estimating city emissions based on atmospheric observations requires that the portion of observed greenhouse gases that originated in the city be separated from the portion that originated outside the city, also known as the background concentration. Here, we investigate different methods to determine background concentrations for the Washington, DC, and Baltimore, MD, region and evaluate how well those methods work and the uncertainties they involve.
Kun Zhang, Ling Huang, Qing Li, Juntao Huo, Yusen Duan, Yuhang Wang, Elly Yaluk, Yangjun Wang, Qingyan Fu, and Li Li
Atmos. Chem. Phys., 21, 5905–5917, https://doi.org/10.5194/acp-21-5905-2021, https://doi.org/10.5194/acp-21-5905-2021, 2021
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Recently, high O3 concentrations were frequently observed in rural areas of the Yangtze River Delta (YRD) region under stagnant conditions. Using an online measurement and observation-based model, we investigated the budget of ROx radicals and the influence of isoprene chemistry on O3 formation. Our results underline that isoprene chemistry in the rural atmosphere becomes important with the participation of anthropogenic NOx.
Ioanna Skoulidou, Maria-Elissavet Koukouli, Astrid Manders, Arjo Segers, Dimitris Karagkiozidis, Myrto Gratsea, Dimitris Balis, Alkiviadis Bais, Evangelos Gerasopoulos, Trisevgeni Stavrakou, Jos van Geffen, Henk Eskes, and Andreas Richter
Atmos. Chem. Phys., 21, 5269–5288, https://doi.org/10.5194/acp-21-5269-2021, https://doi.org/10.5194/acp-21-5269-2021, 2021
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The performance of LOTOS-EUROS v2.2.001 regional chemical transport model NO2 simulations is investigated over Greece from June to December 2018. Comparison with in situ NO2 measurements shows a spatial correlation coefficient of 0.86, while the model underestimates the concentrations mostly during daytime (12 to 15:00 local time). Further, the simulated tropospheric NO2 columns are evaluated against ground-based MAX-DOAS NO2 measurements and S5P/TROPOMI observations for July and December 2018.
Karl M. Seltzer, Elyse Pennington, Venkatesh Rao, Benjamin N. Murphy, Madeleine Strum, Kristin K. Isaacs, and Havala O. T. Pye
Atmos. Chem. Phys., 21, 5079–5100, https://doi.org/10.5194/acp-21-5079-2021, https://doi.org/10.5194/acp-21-5079-2021, 2021
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Volatile chemical products (VCPs) are an increasingly important source of anthropogenic reactive organic carbon emissions. Here, we develop VCPy, a new framework to model organic emissions from VCPs throughout the United States. At the national-level, VCPy emissions are broadly consistent with the US EPA’s 2017 National Emission Inventory, however county-level and categorical estimates can differ substantially. An observational evaluation indicates high fidelity in the methods employed here.
Stijn Naus, Stephen A. Montzka, Prabir K. Patra, and Maarten C. Krol
Atmos. Chem. Phys., 21, 4809–4824, https://doi.org/10.5194/acp-21-4809-2021, https://doi.org/10.5194/acp-21-4809-2021, 2021
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Following up on previous box model studies, we employ a 3D transport model to estimate variations in the hydroxyl radical (OH) from observations of methyl chloroform (MCF). We derive small interannual OH variations that are consistent with variations in the El Niño–Southern Oscillation. We also find evidence for the release of MCF from oceans in atmospheric gradients of MCF. Both findings highlight the added value of a 3D transport model since box model studies did not identify these effects.
Ian Enting and Nathan Clisby
Atmos. Chem. Phys., 21, 4699–4708, https://doi.org/10.5194/acp-21-4699-2021, https://doi.org/10.5194/acp-21-4699-2021, 2021
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We provide a new framework for comparing short-lived greenhouse gases to long-lived greenhouse gases such as carbon dioxide using methane as an example. This can clarify the differences between various proposals that have been introduced in order to overcome the use of global warming potentials as a measure of greenhouse gas equivalence.
Thomas Thorp, Stephen R. Arnold, Richard J. Pope, Dominick V. Spracklen, Luke Conibear, Christoph Knote, Mikhail Arshinov, Boris Belan, Eija Asmi, Tuomas Laurila, Andrei I. Skorokhod, Tuomo Nieminen, and Tuukka Petäjä
Atmos. Chem. Phys., 21, 4677–4697, https://doi.org/10.5194/acp-21-4677-2021, https://doi.org/10.5194/acp-21-4677-2021, 2021
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We compare modelled near-surface pollutants with surface and satellite observations to better understand the controls on the regional concentrations of pollution in western Siberia for late spring and summer in 2011. We find two commonly used emission inventories underestimate human emissions when compared to observations. Transport emissions are the main source of pollutants within the region during this period, whilst fire emissions peak during June and are only significant south of 60° N.
Nikolaos Evangeliou, Yves Balkanski, Sabine Eckhardt, Anne Cozic, Martin Van Damme, Pierre-François Coheur, Lieven Clarisse, Mark W. Shephard, Karen E. Cady-Pereira, and Didier Hauglustaine
Atmos. Chem. Phys., 21, 4431–4451, https://doi.org/10.5194/acp-21-4431-2021, https://doi.org/10.5194/acp-21-4431-2021, 2021
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Ammonia, a substance that has played a key role in sustaining life, has been increasing in the atmosphere, affecting climate and humans. Understanding the reasons for this increase is important for the beneficial use of ammonia. The evolution of satellite products gives us the opportunity to calculate ammonia emissions easier. We calculated global ammonia emissions over the last 10 years, incorporated them into a chemistry model and recorded notable improvement in reproducing observations.
Tie Dai, Yueming Cheng, Daisuke Goto, Yingruo Li, Xiao Tang, Guangyu Shi, and Teruyuki Nakajima
Atmos. Chem. Phys., 21, 4357–4379, https://doi.org/10.5194/acp-21-4357-2021, https://doi.org/10.5194/acp-21-4357-2021, 2021
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The anthropogenic emission of sulfur dioxide (SO2) over China has significantly declined as a consequence of the clean air actions. We have developed a new emission inversion system to dynamically update the SO2 emission grid by grid over China by assimilating ground-based SO2 observations. The inverted SO2 emission over China in November 2016 on average had declined by 49.4 % since 2010, which is well in agreement with the bottom-up estimation of 48.0 %.
Paul T. Griffiths, Lee T. Murray, Guang Zeng, Youngsub Matthew Shin, N. Luke Abraham, Alexander T. Archibald, Makoto Deushi, Louisa K. Emmons, Ian E. Galbally, Birgit Hassler, Larry W. Horowitz, James Keeble, Jane Liu, Omid Moeini, Vaishali Naik, Fiona M. O'Connor, Naga Oshima, David Tarasick, Simone Tilmes, Steven T. Turnock, Oliver Wild, Paul J. Young, and Prodromos Zanis
Atmos. Chem. Phys., 21, 4187–4218, https://doi.org/10.5194/acp-21-4187-2021, https://doi.org/10.5194/acp-21-4187-2021, 2021
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We analyse the CMIP6 Historical and future simulations for tropospheric ozone, a species which is important for many aspects of atmospheric chemistry. We show that the current generation of models agrees well with observations, being particularly successful in capturing trends in surface ozone and its vertical distribution in the troposphere. We analyse the factors that control ozone and show that they evolve over the period of the CMIP6 experiments.
Luke Surl, Tjarda Roberts, and Slimane Bekki
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-145, https://doi.org/10.5194/acp-2021-145, 2021
Revised manuscript accepted for ACP
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Many different chemical reactions happen when the gases from a volcano mix with air, but what effects do they have? We present aircraft measurements which show that there is less ozone within the plume of Etna than outside it. We have also made a computer model of this chemistry. This model can reproduce the effects seen when halogens (bromine and chlorine) are included in the volcanic emissions.
We look closely at the simulation to discover how complicated halogen reactions cause ozone loss.
Annika Vogel and Hendrik Elbern
Atmos. Chem. Phys., 21, 4039–4057, https://doi.org/10.5194/acp-21-4039-2021, https://doi.org/10.5194/acp-21-4039-2021, 2021
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Forecasts of biogenic trace gases highly depend on the model setup and input fields. This study identifies sources of related forecast uncertainties for biogenic gases. Exceptionally high differences in both biogenic emissions and pollutant transport in the Po Valley are identified to be caused by the representation of the land surface and boundary layer dynamics. Consequently, changes in the model configuration are shown to induce significantly different local concentrations of biogenic gases.
Mengyuan Zhang, Arpit Katiyar, Shengqiang Zhu, Juanyong Shen, Men Xia, Jinlong Ma, Sri Harsha Kota, Peng Wang, and Hongliang Zhang
Atmos. Chem. Phys., 21, 4025–4037, https://doi.org/10.5194/acp-21-4025-2021, https://doi.org/10.5194/acp-21-4025-2021, 2021
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We studied changes in air quality in India induced by the COVID-19 lockdown through both surface observations and the CMAQ model. Our results show that emission reductions improved the air quality across India during the lockdown. On average, the levels of PM2.5 and O3 decreased by 28 % and 15 %, indicating positive effects of lockdown measures. We suggest that more stringent and localized emission control strategies should be implemented in India to mitigate air pollutions.
Elena Macdonald, Noelia Otero, and Tim Butler
Atmos. Chem. Phys., 21, 4007–4023, https://doi.org/10.5194/acp-21-4007-2021, https://doi.org/10.5194/acp-21-4007-2021, 2021
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NO2 limit values are still regularly exceeded in many European cities despite decreasing emissions. Measurements of NOx concentrations from stations across Europe were systematically analysed to assess long-term changes observed in urban areas. We compared trends in concentration increments to trends in total and traffic emissions to find potential discrepancies. The results can help in evaluating inaccuracies in emission inventories and in improving spatial imbalances in data availability.
Yuzhong Zhang, Daniel J. Jacob, Xiao Lu, Joannes D. Maasakkers, Tia R. Scarpelli, Jian-Xiong Sheng, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Jinfeng Chang, A. Anthony Bloom, Shuang Ma, John Worden, Robert J. Parker, and Hartmut Boesch
Atmos. Chem. Phys., 21, 3643–3666, https://doi.org/10.5194/acp-21-3643-2021, https://doi.org/10.5194/acp-21-3643-2021, 2021
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We use 2010–2018 satellite observations of atmospheric methane to interpret the factors controlling atmospheric methane and its accelerating increase during the period. The 2010–2018 increase in global methane emissions is driven by tropical and boreal wetlands and tropical livestock (South Asia, Africa, Brazil), with an insignificant positive trend in emissions from the fossil fuel sector. The peak methane growth rates in 2014–2015 are also contributed by low OH and high fire emissions.
Christoph A. Keller, Mathew J. Evans, K. Emma Knowland, Christa A. Hasenkopf, Sruti Modekurty, Robert A. Lucchesi, Tomohiro Oda, Bruno B. Franca, Felipe C. Mandarino, M. Valeria Díaz Suárez, Robert G. Ryan, Luke H. Fakes, and Steven Pawson
Atmos. Chem. Phys., 21, 3555–3592, https://doi.org/10.5194/acp-21-3555-2021, https://doi.org/10.5194/acp-21-3555-2021, 2021
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This study combines surface observations and model simulations to quantify the impact of COVID-19 restrictions on air quality across the world. The presented methodology removes the confounding impacts of meteorology on air pollution. Our results indicate that surface concentrations of nitrogen dioxide, an important air pollutant emitted during the combustion of fossil fuels, declined by up to 60 % following the implementation of COVID-19 containment measures.
Yuting Wang, Yong-Feng Ma, Domingo Muñoz-Esparza, Cathy W. Y. Li, Mary Barth, Tao Wang, and Guy P. Brasseur
Atmos. Chem. Phys., 21, 3531–3553, https://doi.org/10.5194/acp-21-3531-2021, https://doi.org/10.5194/acp-21-3531-2021, 2021
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Large-eddy simulations (LESs) were performed in the mountainous region of the island of Hong Kong to investigate the degree to which the rates of chemical reactions between two reactive species are reduced due to the segregation of species within the convective boundary layer. We show that the inhomogeneity in emissions plays an important role in the segregation effect. Topography also has a significant influence on the segregation locally.
Jin Ma, Linda M. J. Kooijmans, Ara Cho, Stephen A. Montzka, Norbert Glatthor, John R. Worden, Le Kuai, Elliot L. Atlas, and Maarten C. Krol
Atmos. Chem. Phys., 21, 3507–3529, https://doi.org/10.5194/acp-21-3507-2021, https://doi.org/10.5194/acp-21-3507-2021, 2021
Short summary
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Carbonyl sulfide is an important trace gas in the atmosphere and useful to estimating gross primary productivity in ecosystems, but its sources and sinks remain highly uncertain. Therefore, we applied inverse model system TM5-4DVAR to better constrain the global budget. Our finding is in line with earlier studies, pointing to missing sources in the tropics and more uptake in high latitudes. We also stress the necessity of more ground-based observations and satellite data assimilation in future.
Domenico Taraborrelli, David Cabrera-Perez, Sara Bacer, Sergey Gromov, Jos Lelieveld, Rolf Sander, and Andrea Pozzer
Atmos. Chem. Phys., 21, 2615–2636, https://doi.org/10.5194/acp-21-2615-2021, https://doi.org/10.5194/acp-21-2615-2021, 2021
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Atmospheric pollutants from anthropogenic activities and biomass burning are usually regarded as ozone precursors. Monocyclic aromatics are no exception. Calculations with a comprehensive atmospheric model are consistent with this view but only for air masses close to pollution source regions. However, the same model predicts that aromatics, when transported to remote areas, may effectively destroy ozone. This loss of tropospheric ozone rivals the one attributed to bromine.
Jingyu An, Yiwei Huang, Cheng Huang, Xin Wang, Rusha Yan, Qian Wang, Hongli Wang, Sheng'ao Jing, Yan Zhang, Yiming Liu, Yuan Chen, Chang Xu, Liping Qiao, Min Zhou, Shuhui Zhu, Qingyao Hu, Jun Lu, and Changhong Chen
Atmos. Chem. Phys., 21, 2003–2025, https://doi.org/10.5194/acp-21-2003-2021, https://doi.org/10.5194/acp-21-2003-2021, 2021
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This study established a 4 km × 4 km anthropogenic emission inventory in the Yangtze River Delta region, China, for 2017 based on locally measured emission factors and source profiles. There are high-intensity NOx and NMVOC species emissions in the eastern areas of the region. Toluene, 1,2,4-trimethylbenzene, m,p-xylene, propylene, ethylene, o-xylene, and OVOCs from industry and mobile sources have the highest comprehensive potentials for ozone and secondary organic aerosol formation.
Margaret R. Marvin, Paul I. Palmer, Barry G. Latter, Richard Siddans, Brian J. Kerridge, Mohd Talib Latif, and Md Firoz Khan
Atmos. Chem. Phys., 21, 1917–1935, https://doi.org/10.5194/acp-21-1917-2021, https://doi.org/10.5194/acp-21-1917-2021, 2021
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We use an atmospheric chemistry model in combination with satellite and surface observations to investigate how biomass burning affects tropospheric ozone over Southeast Asia during its fire seasons. We find that nitrogen oxides from biomass burning were responsible for about 30 % of the regional ozone formation potential, and we estimate that ozone from biomass burning caused more than 400 excess premature deaths in Southeast Asia during the peak burning months of March and September 2014.
Angharad C. Stell, Luke M. Western, Tomás Sherwen, and Matthew Rigby
Atmos. Chem. Phys., 21, 1717–1736, https://doi.org/10.5194/acp-21-1717-2021, https://doi.org/10.5194/acp-21-1717-2021, 2021
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Although it is the second-most important greenhouse gas, our understanding of the atmospheric-methane budget is limited. The uncertainty highlights the need for new tools to investigate sources and sinks. Here, we use a Gaussian process emulator to efficiently approximate the response of atmospheric-methane observations to changes in the most uncertain emission or loss processes. With this new method, we rigorously quantify the sensitivity of atmospheric observations to budget uncertainties.
Jun Liu, Dan Tong, Yixuan Zheng, Jing Cheng, Xinying Qin, Qinren Shi, Liu Yan, Yu Lei, and Qiang Zhang
Atmos. Chem. Phys., 21, 1627–1647, https://doi.org/10.5194/acp-21-1627-2021, https://doi.org/10.5194/acp-21-1627-2021, 2021
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In this study, we investigated the decadal changes in carbon dioxide and air pollutant emissions in China's cement industry for the period 1990–2015 based on intensive unit-based information. We found that from 1990 to 2015, accompanied by a 10.3-fold increase in cement production, CO2, SO2, and NOx emissions from China's cement industry increased by 627 %, 56 %, and 659 %, whereas CO, PM2.5, and PM10 emissions decreased by 9 %, 63 %, and 59 %, respectively.
Fiona M. O'Connor, N. Luke Abraham, Mohit Dalvi, Gerd A. Folberth, Paul T. Griffiths, Catherine Hardacre, Ben T. Johnson, Ron Kahana, James Keeble, Byeonghyeon Kim, Olaf Morgenstern, Jane P. Mulcahy, Mark Richardson, Eddy Robertson, Jeongbyn Seo, Sungbo Shim, João C. Teixeira, Steven T. Turnock, Jonny Williams, Andrew J. Wiltshire, Stephanie Woodward, and Guang Zeng
Atmos. Chem. Phys., 21, 1211–1243, https://doi.org/10.5194/acp-21-1211-2021, https://doi.org/10.5194/acp-21-1211-2021, 2021
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This paper calculates how changes in emissions and/or concentrations of different atmospheric constituents since the pre-industrial era have altered the Earth's energy budget at the present day using a metric called effective radiative forcing. The impact of land use change is also assessed. We find that individual contributions do not add linearly, and different Earth system interactions can affect the magnitude of the calculated effective radiative forcing.
Shamil Maksyutov, Tomohiro Oda, Makoto Saito, Rajesh Janardanan, Dmitry Belikov, Johannes W. Kaiser, Ruslan Zhuravlev, Alexander Ganshin, Vinu K. Valsala, Arlyn Andrews, Lukasz Chmura, Edward Dlugokencky, László Haszpra, Ray L. Langenfelds, Toshinobu Machida, Takakiyo Nakazawa, Michel Ramonet, Colm Sweeney, and Douglas Worthy
Atmos. Chem. Phys., 21, 1245–1266, https://doi.org/10.5194/acp-21-1245-2021, https://doi.org/10.5194/acp-21-1245-2021, 2021
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In order to improve the top-down estimation of the anthropogenic greenhouse gas emissions, a high-resolution inverse modelling technique was developed for applications to global transport modelling of carbon dioxide and other greenhouse gases. A coupled Eulerian–Lagrangian transport model and its adjoint are combined with surface fluxes at 0.1° resolution to provide high-resolution forward simulation and inverse modelling of surface fluxes accounting for signals from emission hot spots.
Yang Yang, Yu Zhao, Lei Zhang, Jie Zhang, Xin Huang, Xuefen Zhao, Yan Zhang, Mengxiao Xi, and Yi Lu
Atmos. Chem. Phys., 21, 1191–1209, https://doi.org/10.5194/acp-21-1191-2021, https://doi.org/10.5194/acp-21-1191-2021, 2021
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We conducted new NOx emission estimation based on the satellite-derived NO2 column constraint and found reduced emissions compared to previous estimates for a developed region in east China. The subsequent improvement in air quality modeling was demonstrated based on available ground observations. With multiple emission reduction cases for various pollutants, we explored the effective control approaches for ozone and inorganic aerosol pollution.
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Short summary
We used the WRF–Chem model with the latest HONO and ClNO2 processes to investigate their effects on the concentrations of ROx radicals, O3, and PM2.5 in Asia during summer. The results show that the ship-derived HONO and ClNO2 increased the ROx radical concentration by 2–3 times and subsequently increased the O3 and PM2.5 concentrations in marine areas. These findings indicate the importance of these nitrogen processes in the evaluation of the impact of ship emissions on air quality.
We used the WRF–Chem model with the latest HONO and ClNO2 processes to investigate their...
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