Articles | Volume 20, issue 22
Atmos. Chem. Phys., 20, 14347–14359, 2020
https://doi.org/10.5194/acp-20-14347-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Atmos. Chem. Phys., 20, 14347–14359, 2020
https://doi.org/10.5194/acp-20-14347-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article 25 Nov 2020
Research article | 25 Nov 2020
Quantifying the emission changes and associated air quality impacts during the COVID-19 pandemic on the North China Plain: a response modeling study
Jia Xing et al.
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Six heterogeneous HONO chemistry updates in CMAQ significantly improve HONO concentration. HONO production is primarily controlled by the heterogeneous reactions on ground and aerosol surfaces during haze. Additional HONO chemistry updates increase OH and production of secondary aerosols: sulfate, nitrate, and SOA.
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Accurate estimation of emissions is a prerequisite for effectively controlling air pollution, but current methods lack either sufficient data or a representation of nonlinearity. Here, we proposed a novel deep learning method to model the dual relationship between emissions and pollutant concentrations. Emissions can be updated by back-propagating the gradient of the loss function measuring the deviation between simulations and observations, resulting in better model performance.
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In this study, we use global chemical transport model to simulate the effects on global air quality and human health due to emission changes in China from 2010 to 2017. By performing sensitivity analysis, we found that the air pollution control policies not only decrease the air pollutants concentration, but also bring significant co-benefits on air quality in downwind regions. The benefits for the improved air pollution are dominated by PM2.5.
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The present work aims at identifying and quantifying the relative contributions of the key factors in driving a rapid increase in summertime surface O3 over the North China Plain during 2013–2019. In addition to anthropogenic emission reduction and meteorological variabilities, our study highlights the importance of inclusion of aerosol absorption and scattering properties rather than aerosol abundance only in accurate assessment of aerosol radiative effect on surface O3 formation and change.
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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.
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J. Xing, R. Mathur, J. Pleim, C. Hogrefe, C.-M. Gan, D. C. Wong, C. Wei, R. Gilliam, and G. Pouliot
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C.-M. Gan, J. Pleim, R. Mathur, C. Hogrefe, C. N. Long, J. Xing, S. Roselle, and C. Wei
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Six heterogeneous HONO chemistry updates in CMAQ significantly improve HONO concentration. HONO production is primarily controlled by the heterogeneous reactions on ground and aerosol surfaces during haze. Additional HONO chemistry updates increase OH and production of secondary aerosols: sulfate, nitrate, and SOA.
Lin Huang, Song Liu, Zeyuan Yang, Jia Xing, Jia Zhang, Jiang Bian, Siwei Li, Shovan Kumar Sahu, Shuxiao Wang, and Tie-Yan Liu
Geosci. Model Dev., 14, 4641–4654, https://doi.org/10.5194/gmd-14-4641-2021, https://doi.org/10.5194/gmd-14-4641-2021, 2021
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Accurate estimation of emissions is a prerequisite for effectively controlling air pollution, but current methods lack either sufficient data or a representation of nonlinearity. Here, we proposed a novel deep learning method to model the dual relationship between emissions and pollutant concentrations. Emissions can be updated by back-propagating the gradient of the loss function measuring the deviation between simulations and observations, resulting in better model performance.
Yuqiang Zhang, Drew Shindell, Karl Seltzer, Lu Shen, Jean-Francois Lamarque, Qiang Zhang, Bo Zheng, Jia Xing, Zhe Jiang, and Lei Zhang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-385, https://doi.org/10.5194/acp-2021-385, 2021
Revised manuscript accepted for ACP
Short summary
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In this study, we use global chemical transport model to simulate the effects on global air quality and human health due to emission changes in China from 2010 to 2017. By performing sensitivity analysis, we found that the air pollution control policies not only decrease the air pollutants concentration, but also bring significant co-benefits on air quality in downwind regions. The benefits for the improved air pollution are dominated by PM2.5.
Xiaomeng Wu, Daoyuan Yang, Jiajun Gu, Yifan Wen, Shaojun Zhang, Rui Wu, Renjie Wang, Honglei Xu, K. Max Zhang, Ye Wu, and Jiming Hao
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-281, https://doi.org/10.5194/acp-2021-281, 2021
Revised manuscript under review for ACP
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Our work pioneered land-use machine learning methods for developing link-level emission inventories, utilizing hourly traffic profiles including volume, speed and fleet mix obtained from the governmental intercity highway monitoring network in the "capital circles" of China. This research provides a platform to realize the near real-time process of establishing high-resolution vehicle emission inventories for policy makers to engage in sophisticated traffic management.
Sunling Gong, Hongli Liu, Bihui Zhang, Jianjun He, Hengde Zhang, Yaqiang Wang, Shuxiao Wang, Lei Zhang, and Jie Wang
Atmos. Chem. Phys., 21, 2999–3013, https://doi.org/10.5194/acp-21-2999-2021, https://doi.org/10.5194/acp-21-2999-2021, 2021
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Surface concentrations of PM2.5 in China have had a declining trend since 2013 across the country. This research found that the control measures of emission reduction are the dominant factors in the PM2.5 declining trends in various regions. The contribution by the meteorology to the surface PM2.5 concentrations from 2013 to 2019 was not found to show a consistent trend, fluctuating positively or negatively by about 5% on the annual average and 10–20% for the fall–winter heavy-pollution seasons.
Runlong Cai, Chao Yan, Dongsen Yang, Rujing Yin, Yiqun Lu, Chenjuan Deng, Yueyun Fu, Jiaxin Ruan, Xiaoxiao Li, Jenni Kontkanen, Qiang Zhang, Juha Kangasluoma, Yan Ma, Jiming Hao, Douglas R. Worsnop, Federico Bianchi, Pauli Paasonen, Veli-Matti Kerminen, Yongchun Liu, Lin Wang, Jun Zheng, Markku Kulmala, and Jingkun Jiang
Atmos. Chem. Phys., 21, 2457–2468, https://doi.org/10.5194/acp-21-2457-2021, https://doi.org/10.5194/acp-21-2457-2021, 2021
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Based on long-term measurements, we discovered that the collision of H2SO4–amine clusters is the governing mechanism that initializes fast new particle formation in the polluted atmospheric environment of urban Beijing. The mechanism and the governing factors for H2SO4–amine nucleation in the polluted atmosphere are quantitatively investigated in this study.
Xiaodan Ma, Jianping Huang, Tianliang Zhao, Cheng Liu, Kaihui Zhao, Jia Xing, and Wei Xiao
Atmos. Chem. Phys., 21, 1–16, https://doi.org/10.5194/acp-21-1-2021, https://doi.org/10.5194/acp-21-1-2021, 2021
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The present work aims at identifying and quantifying the relative contributions of the key factors in driving a rapid increase in summertime surface O3 over the North China Plain during 2013–2019. In addition to anthropogenic emission reduction and meteorological variabilities, our study highlights the importance of inclusion of aerosol absorption and scattering properties rather than aerosol abundance only in accurate assessment of aerosol radiative effect on surface O3 formation and change.
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, https://doi.org/10.5194/acp-20-4809-2020, 2020
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Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
Meng Gao, Zirui Liu, Bo Zheng, Dongsheng Ji, Peter Sherman, Shaojie Song, Jinyuan Xin, Cheng Liu, Yuesi Wang, Qiang Zhang, Jia Xing, Jingkun Jiang, Zifa Wang, Gregory R. Carmichael, and Michael B. McElroy
Atmos. Chem. Phys., 20, 1497–1505, https://doi.org/10.5194/acp-20-1497-2020, https://doi.org/10.5194/acp-20-1497-2020, 2020
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Short summary
We quantified the relative influences of anthropogenic emissions and meteorological conditions on PM2.5 concentrations in Beijing over the winters of 2002–2016. Meteorological conditions over the study period would have led to an increase of haze in Beijing, but the strict emission control measures have suppressed the unfavorable influences of the recent climate.
Jia Xing, Dian Ding, Shuxiao Wang, Zhaoxin Dong, James T. Kelly, Carey Jang, Yun Zhu, and Jiming Hao
Atmos. Chem. Phys., 19, 13627–13646, https://doi.org/10.5194/acp-19-13627-2019, https://doi.org/10.5194/acp-19-13627-2019, 2019
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The study aims at addressing the challenge in efficient quantification of the nonlinear response of air pollution to precursor emission perturbations. The newly developed observable response indicators can be easily calculated by a combination of ambient concentrations of certain species. Their capability in representing the spatial and temporal variation in PM2.5 and O3 chemistry has also been well evaluated and applied in China.
Mingchen Ma, Yang Gao, Yuhang Wang, Shaoqing Zhang, L. Ruby Leung, Cheng Liu, Shuxiao Wang, Bin Zhao, Xing Chang, Hang Su, Tianqi Zhang, Lifang Sheng, Xiaohong Yao, and Huiwang Gao
Atmos. Chem. Phys., 19, 12195–12207, https://doi.org/10.5194/acp-19-12195-2019, https://doi.org/10.5194/acp-19-12195-2019, 2019
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Ozone pollution has become severe in China, and extremely high ozone episodes occurred in summer 2017 over the North China Plain. While meteorology impacts are clear, we find that enhanced biogenic emissions, previously ignored by the community, driven by high vapor pressure deficit, land cover change and urban landscape contribute substantially to ozone formation. This study has significant implications for ozone pollution control with more frequent heat waves and urbanization growth in future.
Xiaoxiao Li, Shaojie Song, Wei Zhou, Jiming Hao, Douglas R. Worsnop, and Jingkun Jiang
Atmos. Chem. Phys., 19, 12163–12174, https://doi.org/10.5194/acp-19-12163-2019, https://doi.org/10.5194/acp-19-12163-2019, 2019
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Aerosol liquid water is ubiquitous in ambient aerosol. Using long-term aerosol chemical composition to model the aerosol water in Beijing, we found that water absorbed by organics contributes a significant fraction to the total aerosol water. We emphasize the hygroscopicity of organics is highly variable and should be taken into consideration in modelling. A positive feedback loop between organic hygroscopicity and aerosol water was found as one of the driving factors of severe haze in Beijing.
Ling Qi and Shuxiao Wang
Atmos. Chem. Phys., 19, 11545–11557, https://doi.org/10.5194/acp-19-11545-2019, https://doi.org/10.5194/acp-19-11545-2019, 2019
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Black carbon (BC) contributes two-thirds of the climate impact of carbon dioxide, pushing methane into third place of the human contributors to global warming. This study shows that contributions from biomass burning (producing marginal lensing effect) have a strong spatial variation, from 20 % in Europe to 60 % in Africa. Thus, the inclusion of strong lensing-related absorption enhancement to all BC particles in previous estimates may lead to overestimating their positive radiative forcing.
Tuan V. Vu, Zongbo Shi, Jing Cheng, Qiang Zhang, Kebin He, Shuxiao Wang, and Roy M. Harrison
Atmos. Chem. Phys., 19, 11303–11314, https://doi.org/10.5194/acp-19-11303-2019, https://doi.org/10.5194/acp-19-11303-2019, 2019
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A 5-year Clean Air Action Plan was implemented in 2013 to improve ambient air quality in Beijing. Here, we applied a novel machine-learning-based model to determine the real trend in air quality from 2013 to 2017 in Beijing to assess the efficacy of the plan. We showed that the action plan led to a major reduction in primary emissions and significant improvement in air quality. The marked decrease in PM2.5 and SO2 is largely attributable to a reduction in coal combustion.
Xionghui Qiu, Qi Ying, Shuxiao Wang, Lei Duan, Jian Zhao, Jia Xing, Dian Ding, Yele Sun, Baoxian Liu, Aijun Shi, Xiao Yan, Qingcheng Xu, and Jiming Hao
Atmos. Chem. Phys., 19, 6737–6747, https://doi.org/10.5194/acp-19-6737-2019, https://doi.org/10.5194/acp-19-6737-2019, 2019
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Current chemical transport models cannot capture the diurnal and nocturnal variation in atmospheric nitrate, which may be relative to the missing atmospheric chlorine chemistry. In this work, the Community Multiscale Air Quality (CMAQ) model with improved chlorine heterogeneous chemistry is applied to simulate the impact of chlorine chemistry on summer nitrate concentrations in Beijing. The results of this work can improve our understanding of nitrate formation.
Junlan Feng, Yan Zhang, Shanshan Li, Jingbo Mao, Allison P. Patton, Yuyan Zhou, Weichun Ma, Cong Liu, Haidong Kan, Cheng Huang, Jingyu An, Li Li, Yin Shen, Qingyan Fu, Xinning Wang, Juan Liu, Shuxiao Wang, Dian Ding, Jie Cheng, Wangqi Ge, Hong Zhu, and Katherine Walker
Atmos. Chem. Phys., 19, 6167–6183, https://doi.org/10.5194/acp-19-6167-2019, https://doi.org/10.5194/acp-19-6167-2019, 2019
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This study aims to estimate the emissions, air quality and population exposure impacts of shipping in 2015, prior to the implementation of the DECAs. It shows that ship emissions within 12 NM of the shore could account for over 55 % of the shipping impact on air pollution in the YRD in summer. Ships entering the Yangtze River and other inland waterways of Shanghai contribute 40–80 % of the ship-related air pollution and population exposure，which both have important implications regarding policy.
Zhenying Xu, Mingxu Liu, Minsi Zhang, Yu Song, Shuxiao Wang, Lin Zhang, Tingting Xu, Tiantian Wang, Caiqing Yan, Tian Zhou, Yele Sun, Yuepeng Pan, Min Hu, Mei Zheng, and Tong Zhu
Atmos. Chem. Phys., 19, 5605–5613, https://doi.org/10.5194/acp-19-5605-2019, https://doi.org/10.5194/acp-19-5605-2019, 2019
Haotian Zheng, Siyi Cai, Shuxiao Wang, Bin Zhao, Xing Chang, and Jiming Hao
Atmos. Chem. Phys., 19, 3447–3462, https://doi.org/10.5194/acp-19-3447-2019, https://doi.org/10.5194/acp-19-3447-2019, 2019
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The heavy air pollution in the Beijing-Tianjin-Hebei (BTH) region is a global hot topic. We established a unit-based industrial emission inventory for the BTH region. The inventory significantly improved air quality modeling results; this improvement subsequently contributes to an accurate source apportionment of haze pollution and more precisely targeted decision making.
Shaojie Song, Meng Gao, Weiqi Xu, Yele Sun, Douglas R. Worsnop, John T. Jayne, Yuzhong Zhang, Lei Zhu, Mei Li, Zhen Zhou, Chunlei Cheng, Yibing Lv, Ying Wang, Wei Peng, Xiaobin Xu, Nan Lin, Yuxuan Wang, Shuxiao Wang, J. William Munger, Daniel J. Jacob, and Michael B. McElroy
Atmos. Chem. Phys., 19, 1357–1371, https://doi.org/10.5194/acp-19-1357-2019, https://doi.org/10.5194/acp-19-1357-2019, 2019
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Chemistry responsible for sulfate production in northern China winter haze remains mysterious. We propose a potentially key pathway through the reaction of formaldehyde and sulfur dioxide that has not been accounted for in previous studies. The special atmospheric conditions favor the formation and existence of their complex, hydroxymethanesulfonate (HMS).
Ge Zhang, Yang Gao, Wenju Cai, L. Ruby Leung, Shuxiao Wang, Bin Zhao, Minghuai Wang, Huayao Shan, Xiaohong Yao, and Huiwang Gao
Atmos. Chem. Phys., 19, 565–576, https://doi.org/10.5194/acp-19-565-2019, https://doi.org/10.5194/acp-19-565-2019, 2019
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Based on observed data, this study reveals a distinct seesaw feature of abnormally high and low PM2.5 concentrations in December 2015 and January 2016 over North China. The mechanism of the seesaw pattern was found to be linked to a super El Niño and the Arctic Oscillation (AO). During the mature phase of El Niño in December 2015, the weakened East Asian winter monsoon favors strong haze formation; however, the circulation pattern was reversed in the next month due to the phase change of the AO.
Mingxu Liu, Xin Huang, Yu Song, Tingting Xu, Shuxiao Wang, Zhijun Wu, Min Hu, Lin Zhang, Qiang Zhang, Yuepeng Pan, Xuejun Liu, and Tong Zhu
Atmos. Chem. Phys., 18, 17933–17943, https://doi.org/10.5194/acp-18-17933-2018, https://doi.org/10.5194/acp-18-17933-2018, 2018
Runlong Cai, Indra Chandra, Dongsen Yang, Lei Yao, Yueyun Fu, Xiaoxiao Li, Yiqun Lu, Lun Luo, Jiming Hao, Yan Ma, Lin Wang, Jun Zheng, Takafumi Seto, and Jingkun Jiang
Atmos. Chem. Phys., 18, 16587–16599, https://doi.org/10.5194/acp-18-16587-2018, https://doi.org/10.5194/acp-18-16587-2018, 2018
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Significant influences of transport on measured aerosol size distributions are commonly observed. We propose a method for estimating the contributions of transport to nanoparticles during new particle formation events. This method was used to analyze new particle formation events in Southeast Tibet, Fukue Island, and urban Beijing. The changes in the contributions of transport have a good correlation with the changes in wind speed and direction, indicating the feasibility of the method.
Runlong Cai, Dongsen Yang, Lauri R. Ahonen, Linlin Shi, Frans Korhonen, Yan Ma, Jiming Hao, Tuukka Petäjä, Jun Zheng, Juha Kangasluoma, and Jingkun Jiang
Atmos. Meas. Tech., 11, 4477–4491, https://doi.org/10.5194/amt-11-4477-2018, https://doi.org/10.5194/amt-11-4477-2018, 2018
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We tested the performance of four inversion methods to recover sub-3 nm aerosol size distributions using the particle size magnifier (PSM). The PSM is widely used in new particle formation study; however, the inversion methods used in previous studies may report false particle concentrations. Due to the results, we suggest using the expectation–maximization algorithm to address the PSM inversion problem. We also gave practical suggestions on PSM operation based on the inversion analysis.
Yuqiang Zhang, Rohit Mathur, Jesse O. Bash, Christian Hogrefe, Jia Xing, and Shawn J. Roselle
Atmos. Chem. Phys., 18, 9091–9106, https://doi.org/10.5194/acp-18-9091-2018, https://doi.org/10.5194/acp-18-9091-2018, 2018
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For this study, we evaluated the WRF–CMAQ coupled model's ability to simulate the long-term trends of wet deposition of nitrogen and sulfur from 1990 to 2010 by comparing the model results with long-term observation datasets in the US. The model generally underestimates the wet deposition of both nitrogen and sulfur but captured well the decreasing trends for the deposition. Then we estimated the deposition budget in the US, including wet deposition and dry deposition from model simulations.
Yi Tang, Shuxiao Wang, Qingru Wu, Kaiyun Liu, Long Wang, Shu Li, Wei Gao, Lei Zhang, Haotian Zheng, Zhijian Li, and Jiming Hao
Atmos. Chem. Phys., 18, 8279–8291, https://doi.org/10.5194/acp-18-8279-2018, https://doi.org/10.5194/acp-18-8279-2018, 2018
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In this study, 3-year measurements of atmospheric Hg were carried out at a rural site in East China. A significant downward trend was observed during the sampling period. This study used a new approach that considers both cluster frequency and the Hg concentration associated with each cluster, and we calculated that atmospheric Hg from the whole region of China has caused a 70 % decline of GEM concentration at the Chongming monitoring site due to strict air pollution control policies in China.
Chandra Venkataraman, Michael Brauer, Kushal Tibrewal, Pankaj Sadavarte, Qiao Ma, Aaron Cohen, Sreelekha Chaliyakunnel, Joseph Frostad, Zbigniew Klimont, Randall V. Martin, Dylan B. Millet, Sajeev Philip, Katherine Walker, and Shuxiao Wang
Atmos. Chem. Phys., 18, 8017–8039, https://doi.org/10.5194/acp-18-8017-2018, https://doi.org/10.5194/acp-18-8017-2018, 2018
Jia Xing, Dian Ding, Shuxiao Wang, Bin Zhao, Carey Jang, Wenjing Wu, Fenfen Zhang, Yun Zhu, and Jiming Hao
Atmos. Chem. Phys., 18, 7799–7814, https://doi.org/10.5194/acp-18-7799-2018, https://doi.org/10.5194/acp-18-7799-2018, 2018
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NOx is the common precursor for both PM2.5 and O3 pollution, while the effectiveness of NOx controls for reducing PM2.5 and O3 are largely influenced by the ambient levels of NH3 and VOCs. This study developed a new method to quantify the nonlinear effectiveness of emission controls for reducing PM2.5 and O3. The new method not only substantially reduces the computational burden but also provides a series of quantitative indicators to quantify the nonlinear control effectiveness.
Shaojie Song, Meng Gao, Weiqi Xu, Jingyuan Shao, Guoliang Shi, Shuxiao Wang, Yuxuan Wang, Yele Sun, and Michael B. McElroy
Atmos. Chem. Phys., 18, 7423–7438, https://doi.org/10.5194/acp-18-7423-2018, https://doi.org/10.5194/acp-18-7423-2018, 2018
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Severe haze events occur frequently over northern China, especially in winter. Acidity plays a critical role in the formation of secondary PM2.5 and its toxicity. Using field measurements of gases and particles to critically evaluate two thermodynamic models routinely employed to determine particle acidity, we found that China's winter haze particles are generally within a moderately acidic range (pH 4–5) and not highly acidic (0) or neutral (7) as has been previously reported in the literature.
Xing Chang, Shuxiao Wang, Bin Zhao, Siyi Cai, and Jiming Hao
Atmos. Chem. Phys., 18, 4843–4858, https://doi.org/10.5194/acp-18-4843-2018, https://doi.org/10.5194/acp-18-4843-2018, 2018
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The Beijing–Tianjin–Hebei region in China has been suffering from a severe particulate matter pollution, and the inter-city transport of the pollutant plays an important role. The current research quantitatively assesses the transport process. We identify three transport pathways. The southwest–northwest one happens in both winter and summer. The transport is stronger at 300–1000 m, or 1–2 days before a pollution peak. The result may guide the joint emission control along the transport pathway.
Qian Yu, Yao Luo, Shuxiao Wang, Zhiqi Wang, Jiming Hao, and Lei Duan
Atmos. Chem. Phys., 18, 495–509, https://doi.org/10.5194/acp-18-495-2018, https://doi.org/10.5194/acp-18-495-2018, 2018
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This study provides high-quality direct observation data of a clean and a contaminated site in subtropical south China and quantifies the natural forest Hg emission. We find that clean and contaminated forests present a net GEM source with annual average values of 6.67 and 0.30 ng m-2 h-1, respectively; daily variations of GEM fluxes showed a source in the daytime with a peak at 13:00, and as a sink or balance at night; and higher atmospheric GEM concentration restricted the forest GEM emission.
Rohit Mathur, Jia Xing, Robert Gilliam, Golam Sarwar, Christian Hogrefe, Jonathan Pleim, George Pouliot, Shawn Roselle, Tanya L. Spero, David C. Wong, and Jeffrey Young
Atmos. Chem. Phys., 17, 12449–12474, https://doi.org/10.5194/acp-17-12449-2017, https://doi.org/10.5194/acp-17-12449-2017, 2017
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We extend CMAQ's applicability to the entire Northern Hemisphere to enable consistent examination of interactions between atmospheric processes occurring on various spatial and temporal scales. Improvements were made in model process representation, structure, and input data sets that enable a range of model applications including episodic intercontinental pollutant transport, long-term trends in air pollution across the Northern Hemisphere, and air pollution–climate interactions.
Runlong Cai, Dongsen Yang, Yueyun Fu, Xing Wang, Xiaoxiao Li, Yan Ma, Jiming Hao, Jun Zheng, and Jingkun Jiang
Atmos. Chem. Phys., 17, 12327–12340, https://doi.org/10.5194/acp-17-12327-2017, https://doi.org/10.5194/acp-17-12327-2017, 2017
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The governing factors for new particle formation (NPF) events in Beijing were analyzed. The roles of gaseous precursors and aerosol surface area were illustrated. It appears that the abundance of gaseous precursors in Beijing is high enough to have nucleation; however, it is aerosol surface area that determines the occurrence of NPF events in Beijing. Aerosol loading thresholds (in the form of aerosol surface area and PM2.5 concentration) for predicting NPF days in Beijing were suggested.
Bin Zhao, Wenjing Wu, Shuxiao Wang, Jia Xing, Xing Chang, Kuo-Nan Liou, Jonathan H. Jiang, Yu Gu, Carey Jang, Joshua S. Fu, Yun Zhu, Jiandong Wang, Yan Lin, and Jiming Hao
Atmos. Chem. Phys., 17, 12031–12050, https://doi.org/10.5194/acp-17-12031-2017, https://doi.org/10.5194/acp-17-12031-2017, 2017
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Using over 1000 chemical transport model simulations in the Beijing–Tianjin–Hebei region, we find that the emissions of primary inorganic PM2.5 make the largest contribution to PM2.5 concentrations and thus should be prioritized in PM2.5 control strategies. Among the precursors, PM2.5 concentrations are primarily sensitive to the emissions of NH3, NMVOC+IVOC, and POA, and the sensitivities increase substantially for NH3 and NHx with the increase in emission reduction ratio.
Qingru Wu, Wei Gao, Shuxiao Wang, and Jiming Hao
Atmos. Chem. Phys., 17, 10423–10433, https://doi.org/10.5194/acp-17-10423-2017, https://doi.org/10.5194/acp-17-10423-2017, 2017
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Iron and steel production (ISP) is one of the most significant atmospheric Hg emission sources in China. Atmospheric Hg emissions from ISP increased from 11.5 t in 2000 to 32.75 t in 2015 with a peak of 35.65 t in 2013. In the coming years, emissions from ISP are expected to decrease. Although sinter/pellet plants and blast furnaces were the largest two emission processes, emissions from roasting plants and coke ovens accounted for 22 %–34 % of ISP’s emissions.
Jia Xing, Jiandong Wang, Rohit Mathur, Shuxiao Wang, Golam Sarwar, Jonathan Pleim, Christian Hogrefe, Yuqiang Zhang, Jingkun Jiang, David C. Wong, and Jiming Hao
Atmos. Chem. Phys., 17, 9869–9883, https://doi.org/10.5194/acp-17-9869-2017, https://doi.org/10.5194/acp-17-9869-2017, 2017
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The assessment of the impacts of aerosol direct effects (ADE) is important for understanding emission reduction strategies that seek co-benefits associated with reductions in both particulate matter and ozone. This study quantifies the ADE impacts on tropospheric ozone by using a two-way coupled meteorology and atmospheric chemistry model. Results suggest that reducing ADE may have the potential risk of increasing ozone in winter, but it will benefit the reduction of maxima ozone in summer.
Leiming Zhang, Seth Lyman, Huiting Mao, Che-Jen Lin, David A. Gay, Shuxiao Wang, Mae Sexauer Gustin, Xinbin Feng, and Frank Wania
Atmos. Chem. Phys., 17, 9133–9144, https://doi.org/10.5194/acp-17-9133-2017, https://doi.org/10.5194/acp-17-9133-2017, 2017
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Future research needs are proposed for improving the understanding of atmospheric mercury cycling. These include refinement of mercury emission estimations, quantification of dry deposition and air–surface exchange, improvement of the treatment of chemical mechanisms in chemical transport models, increase in the accuracy of oxidized mercury measurements, better interpretation of atmospheric mercury chemistry data, and harmonization of network operation.
Johannes Bieser, Franz Slemr, Jesse Ambrose, Carl Brenninkmeijer, Steve Brooks, Ashu Dastoor, Francesco DeSimone, Ralf Ebinghaus, Christian N. Gencarelli, Beate Geyer, Lynne E. Gratz, Ian M. Hedgecock, Daniel Jaffe, Paul Kelley, Che-Jen Lin, Lyatt Jaegle, Volker Matthias, Andrei Ryjkov, Noelle E. Selin, Shaojie Song, Oleg Travnikov, Andreas Weigelt, Winston Luke, Xinrong Ren, Andreas Zahn, Xin Yang, Yun Zhu, and Nicola Pirrone
Atmos. Chem. Phys., 17, 6925–6955, https://doi.org/10.5194/acp-17-6925-2017, https://doi.org/10.5194/acp-17-6925-2017, 2017
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We conducted a multi model study to investigate our ability to reproduce the vertical distribution of mercury in the atmosphere. For this, we used observational data from over 40 aircraft flights in EU and US. We compared observations to the results of seven chemistry transport models and found that the models are able to reproduce vertical gradients of total and elemental Hg. Finally, we found that different chemical reactions seem responsible for the oxidation of Hg depending on altitude.
Qiao Ma, Siyi Cai, Shuxiao Wang, Bin Zhao, Randall V. Martin, Michael Brauer, Aaron Cohen, Jingkun Jiang, Wei Zhou, Jiming Hao, Joseph Frostad, Mohammad H. Forouzanfar, and Richard T. Burnett
Atmos. Chem. Phys., 17, 4477–4491, https://doi.org/10.5194/acp-17-4477-2017, https://doi.org/10.5194/acp-17-4477-2017, 2017
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In order to quantitatively identify the contributions of coal combustion to airborne fine particles, we developed an emission inventory using up-to-date information and conducted simulations using an atmospheric model. Results show that coal combustion contributes 40 % of the airborne fine-particle concentration on national average in China. Among the subsectors of coal combustion, industrial coal burning is the dominant contributor, which should be prioritized when policies are applied.
Jianlin Hu, Peng Wang, Qi Ying, Hongliang Zhang, Jianjun Chen, Xinlei Ge, Xinghua Li, Jingkun Jiang, Shuxiao Wang, Jie Zhang, Yu Zhao, and Yingyi Zhang
Atmos. Chem. Phys., 17, 77–92, https://doi.org/10.5194/acp-17-77-2017, https://doi.org/10.5194/acp-17-77-2017, 2017
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An annual simulation of secondary organic aerosol (SOA) concentrations in China with updated SOA formation pathways reveals that SOA can be a significant contributor to PM2.5 in major urban areas. Summer SOA is dominated by emissions from biogenic sources, while winter SOA is dominated by anthropogenic emissions such as alkanes and aromatic compounds. Reactive surface uptake of dicarbonyls throughout the year and isoprene epoxides in summer is the most important contributor.
Yang Hua, Shuxiao Wang, Jiandong Wang, Jingkun Jiang, Tianshu Zhang, Yu Song, Ling Kang, Wei Zhou, Runlong Cai, Di Wu, Siwei Fan, Tong Wang, Xiaoqing Tang, Qiang Wei, Feng Sun, and Zhimei Xiao
Atmos. Chem. Phys., 16, 15451–15460, https://doi.org/10.5194/acp-16-15451-2016, https://doi.org/10.5194/acp-16-15451-2016, 2016
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The characteristics of three PM2.5 pollution episodes were analyzed during the APEC Summit at a rural site outside of Beijing. It was found that meteorological conditions on the ground could not explain the pollution process, while vertical parameters helped improve the understanding of heavy pollution processes. Our research suggests that regional transport of air pollutants contributes significantly to severe secondary particle pollution, even when local emission is controlled effectively.
Biwu Chu, Xiao Zhang, Yongchun Liu, Hong He, Yele Sun, Jingkun Jiang, Junhua Li, and Jiming Hao
Atmos. Chem. Phys., 16, 14219–14230, https://doi.org/10.5194/acp-16-14219-2016, https://doi.org/10.5194/acp-16-14219-2016, 2016
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The interactive effects between inorganic and organic species under highly complex pollution conditions remain uncertain and were studied in a smog chamber. This study indicated that the synergistic formation of secondary inorganic and organic aerosol might increase the secondary aerosol load in the atmosphere and contribute haze pollution in eastern China. These synergistic effects were related to the heterogeneous process on aerosol surface and need to be considered in air quality models.
Jia Xing, Rohit Mathur, Jonathan Pleim, Christian Hogrefe, Jiandong Wang, Chuen-Meei Gan, Golam Sarwar, David C. Wong, and Stuart McKeen
Atmos. Chem. Phys., 16, 10865–10877, https://doi.org/10.5194/acp-16-10865-2016, https://doi.org/10.5194/acp-16-10865-2016, 2016
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Downward transport of ozone from the stratosphere has large impacts on surface concentration and needs to be properly represented in regional models. This study developed a seasonally and spatially varying PV-based function from an investigation of the relationship between PV and O3. The implementation of the new function significantly improves the model's performance in O3 simulation, which enables a more accurate simulation of the vertical distribution of O3 across the Northern Hemisphere.
Shaojun Zhang, Ye Wu, Ruikun Huang, Jiandong Wang, Han Yan, Yali Zheng, and Jiming Hao
Atmos. Chem. Phys., 16, 9965–9981, https://doi.org/10.5194/acp-16-9965-2016, https://doi.org/10.5194/acp-16-9965-2016, 2016
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For highly populated cities in eastern Asian, traffic management has played an increasingly important role in mitigating local emissions from vehicles. Therefore, high-resolution vehicle emission inventory is an irreplaceable assessment tool. This study selected Macau, the most populated city in the world, to demonstrate a high-resolution simulation of vehicular pollution by coupling detailed local data collected and interdisciplinary models.
Bin Zhao, Kuo-Nan Liou, Yu Gu, Cenlin He, Wee-Liang Lee, Xing Chang, Qinbin Li, Shuxiao Wang, Hsien-Liang R. Tseng, Lai-Yung R. Leung, and Jiming Hao
Atmos. Chem. Phys., 16, 5841–5852, https://doi.org/10.5194/acp-16-5841-2016, https://doi.org/10.5194/acp-16-5841-2016, 2016
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We examine the impact of buildings on surface solar fluxes in Beijing by accounting for their 3-D structures. We find that inclusion of buildings changes surface solar fluxes by within ±1 W m−2, ±1–10 W m−2, and up to ±100 W m−2 at grid resolutions of 4 km, 800 m, and 90 m, respectively. We can resolve pairs of positive-negative flux deviations on different sides of buildings at ≤ 800 m resolutions. We should treat building-effect on solar fluxes differently in models with different resolutions.
Lei Zhang, Shuxiao Wang, Qingru Wu, Fengyang Wang, Che-Jen Lin, Leiming Zhang, Mulin Hui, Mei Yang, Haitao Su, and Jiming Hao
Atmos. Chem. Phys., 16, 2417–2433, https://doi.org/10.5194/acp-16-2417-2016, https://doi.org/10.5194/acp-16-2417-2016, 2016
C.-M. Gan, J. Pleim, R. Mathur, C. Hogrefe, C. N. Long, J. Xing, D. Wong, R. Gilliam, and C. Wei
Atmos. Chem. Phys., 15, 12193–12209, https://doi.org/10.5194/acp-15-12193-2015, https://doi.org/10.5194/acp-15-12193-2015, 2015
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This study attempts to determine the consequences of the changes in tropospheric aerosol burden arising from substantial reductions in emissions of SO2 and NOx associated with control measures under the Clean Air Act especially on trends in solar radiation. Comparisons of model results with observations of aerosol optical depth, aerosol concentration, and radiation demonstrate that the coupled WRF-CMAQ model is capable of replicating the trends well even though it tends to underestimate the AOD.
A. Stohl, B. Aamaas, M. Amann, L. H. Baker, N. Bellouin, T. K. Berntsen, O. Boucher, R. Cherian, W. Collins, N. Daskalakis, M. Dusinska, S. Eckhardt, J. S. Fuglestvedt, M. Harju, C. Heyes, Ø. Hodnebrog, J. Hao, U. Im, M. Kanakidou, Z. Klimont, K. Kupiainen, K. S. Law, M. T. Lund, R. Maas, C. R. MacIntosh, G. Myhre, S. Myriokefalitakis, D. Olivié, J. Quaas, B. Quennehen, J.-C. Raut, S. T. Rumbold, B. H. Samset, M. Schulz, Ø. Seland, K. P. Shine, R. B. Skeie, S. Wang, K. E. Yttri, and T. Zhu
Atmos. Chem. Phys., 15, 10529–10566, https://doi.org/10.5194/acp-15-10529-2015, https://doi.org/10.5194/acp-15-10529-2015, 2015
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This paper presents a summary of the findings of the ECLIPSE EU project. The project has investigated the climate and air quality impacts of short-lived climate pollutants (especially methane, ozone, aerosols) and has designed a global mitigation strategy that maximizes co-benefits between air quality and climate policy. Transient climate model simulations allowed quantifying the impacts on temperature (e.g., reduction in global warming by 0.22K for the decade 2041-2050) and precipitation.
H. Z. Tian, C. Y. Zhu, J. J. Gao, K. Cheng, J. M. Hao, K. Wang, S. B. Hua, Y. Wang, and J. R. Zhou
Atmos. Chem. Phys., 15, 10127–10147, https://doi.org/10.5194/acp-15-10127-2015, https://doi.org/10.5194/acp-15-10127-2015, 2015
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For the first time, with S-shaped curves, the best available representation of time-varying emission factors of 12 heavy metals (Hg, As, Se, Pb, Cd, Cr, Ni, Sb, Mn, Co, Cu and Zn) from primary anthropogenic sources of China are determined on account of economic transitions and pollution control technology improvement. The temporal and spatial variation characteristics of these heavy metals emissions during the period of 1949−2012 are calculated and evaluated with uncertainty analysis.
J. Xing, R. Mathur, J. Pleim, C. Hogrefe, C.-M. Gan, D. C. Wong, and C. Wei
Atmos. Chem. Phys., 15, 9997–10018, https://doi.org/10.5194/acp-15-9997-2015, https://doi.org/10.5194/acp-15-9997-2015, 2015
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The ability of a coupled meteorology-chemistry model (WRF-CMAQ) to reproduce the historical trend in AOD and clear-sky SWR over the N. Hemisphere has been evaluated through a comparison of 21-year simulated results with observation-derived records from 1990 to 2010. Questions of how well the model represents the regional and temporal variability of aerosol burden and DRE, and whether the model is able to capture past trends in aerosol loading and associated radiation effects, will be addressed.
X. Fu, S. X. Wang, L. M. Ran, J. E. Pleim, E. Cooter, J. O. Bash, V. Benson, and J. M. Hao
Atmos. Chem. Phys., 15, 6637–6649, https://doi.org/10.5194/acp-15-6637-2015, https://doi.org/10.5194/acp-15-6637-2015, 2015
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In this study, we estimate, for the first time, the NH3 emission from the agricultural fertilizer application in China online using the bi-directional CMAQ model coupled to an agro-ecosystem model. Compared with previous researches, this method considers more influencing factors, such as meteorological fields, soil and the fertilizer application, and provides improved NH3 emission with higher spatial and temporal resolution.
J. Xing, R. Mathur, J. Pleim, C. Hogrefe, C.-M. Gan, D. C. Wong, C. Wei, R. Gilliam, and G. Pouliot
Atmos. Chem. Phys., 15, 2723–2747, https://doi.org/10.5194/acp-15-2723-2015, https://doi.org/10.5194/acp-15-2723-2015, 2015
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Model-simulated air quality trends over the past 2 decades largely agree with those derived from observations. In the relative amounts of VOC and NOx emission controls in different regions across the northern hemisphere have led to significantly different trends in tropospheric O3. Differences in the historical changes in the relative amounts of NH3, NOx and SO2 emissions also impact the trends in inorganic particulate matter amounts and composition in China, the U.S. and Europe.
B. Zhao, S. X. Wang, J. Xing, K. Fu, J. S. Fu, C. Jang, Y. Zhu, X. Y. Dong, Y. Gao, W. J. Wu, J. D. Wang, and J. M. Hao
Geosci. Model Dev., 8, 115–128, https://doi.org/10.5194/gmd-8-115-2015, https://doi.org/10.5194/gmd-8-115-2015, 2015
S. X. Wang, B. Zhao, S. Y. Cai, Z. Klimont, C. P. Nielsen, T. Morikawa, J. H. Woo, Y. Kim, X. Fu, J. Y. Xu, J. M. Hao, and K. B. He
Atmos. Chem. Phys., 14, 6571–6603, https://doi.org/10.5194/acp-14-6571-2014, https://doi.org/10.5194/acp-14-6571-2014, 2014
Z. Cheng, S. Wang, X. Fu, J. G. Watson, J. Jiang, Q. Fu, C. Chen, B. Xu, J. Yu, J. C. Chow, and J. Hao
Atmos. Chem. Phys., 14, 4573–4585, https://doi.org/10.5194/acp-14-4573-2014, https://doi.org/10.5194/acp-14-4573-2014, 2014
C.-M. Gan, J. Pleim, R. Mathur, C. Hogrefe, C. N. Long, J. Xing, S. Roselle, and C. Wei
Atmos. Chem. Phys., 14, 1701–1715, https://doi.org/10.5194/acp-14-1701-2014, https://doi.org/10.5194/acp-14-1701-2014, 2014
X. Fu, S. X. Wang, Z. Cheng, J. Xing, B. Zhao, J. D. Wang, and J. M. Hao
Atmos. Chem. Phys., 14, 1239–1254, https://doi.org/10.5194/acp-14-1239-2014, https://doi.org/10.5194/acp-14-1239-2014, 2014
L. Zhang, S. X. Wang, L. Wang, and J. M. Hao
Atmos. Chem. Phys., 13, 10505–10516, https://doi.org/10.5194/acp-13-10505-2013, https://doi.org/10.5194/acp-13-10505-2013, 2013
B. Zhao, S. X. Wang, H. Liu, J. Y. Xu, K. Fu, Z. Klimont, J. M. Hao, K. B. He, J. Cofala, and M. Amann
Atmos. Chem. Phys., 13, 9869–9897, https://doi.org/10.5194/acp-13-9869-2013, https://doi.org/10.5194/acp-13-9869-2013, 2013
J. Xing, J. Pleim, R. Mathur, G. Pouliot, C. Hogrefe, C.-M. Gan, and C. Wei
Atmos. Chem. Phys., 13, 7531–7549, https://doi.org/10.5194/acp-13-7531-2013, https://doi.org/10.5194/acp-13-7531-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Technical note: Quality assessment of ozone reanalysis products and gap-filling over subarctic Europe for vegetation risk mapping
Evolution of OH reactivity in NO-free volatile organic compound photooxidation investigated by the fully explicit GECKO-A model
Impact of pyruvic acid photolysis on acetaldehyde and peroxy radical formation in the boreal forest: theoretical calculations and model results
Evaluating consistency between total column CO2 retrievals from OCO-2 and the in situ network over North America: implications for carbon flux estimation
Global tropospheric halogen (Cl, Br, I) chemistry and its impact on oxidants
The role of emission reductions and the meteorological situation for air quality improvements during the COVID-19 lockdown period in central Europe
Heterogeneity and chemical reactivity of the remote troposphere defined by aircraft measurements
A mass-balance-based emission inventory of non-methane volatile organic compounds (NMVOCs) for solvent use in China
Opinion: The germicidal effect of ambient air (open-air factor) revisited
Impact of Athabasca oil sands operations on mercury levels in air and deposition
Study of different Carbon Bond 6 (CB6) mechanisms by using a concentration sensitivity analysis
Accelerating methane growth rate from 2010 to 2017: leading contributions from the tropics and East Asia
Observation and modelling of ozone-destructive halogen chemistry in a passively degassing volcanic plume
Modeling study of the impact of SO2 volcanic passive emissions on the tropospheric sulfur budget
The impact of organic pollutants from Indonesian peatland fires on the tropospheric and lower stratospheric composition
Comprehensive evaluations of diurnal NO2 measurements during DISCOVER-AQ 2011: effects of resolution-dependent representation of NOx emissions
Downscaling system for modeling of atmospheric composition on regional, urban and street scales
Satellite soil moisture data assimilation impacts on modeling weather variables and ozone in the southeastern US – Part 1: An overview
Development of ozone reactivity scales for volatile organic compounds in a Chinese megacity
Measured and modelled air quality trends in Italy over the period 2003–2010
Large and increasing methane emissions from eastern Amazonia derived from satellite data, 2010–2018
Contrasting chemical environments in summertime for atmospheric ozone across major Chinese industrial regions: the effectiveness of emission control strategies
Unexpected enhancement of ozone exposure and health risks during National Day in China
Role of oceanic ozone deposition in explaining temporal variability in surface ozone at High Arctic sites
Atmospheric observations consistent with reported decline in the UK's methane emissions, 2013–2020
Oxidation of low-molecular-weight organic compounds in cloud droplets: global impact on tropospheric oxidants
Bias-correcting carbon fluxes derived from land-surface satellite data for retrospective and near-real-time assimilation systems
Characterizing model errors in chemical transport modeling of methane: using GOSAT XCH4 data with weak-constraint four-dimensional variational data assimilation
Estimation of fire-induced carbon emissions from Equatorial Asia in 2015 using in situ aircraft and ship observations
Influence of weather situation on non-CO2 aviation climate effects: the REACT4C climate change functions
Influence of atmospheric in-cloud aqueous-phase chemistry on global simulation of SO2 in CESM2
Impact of international shipping emissions on ozone and PM2.5 in East Asia during summer: the important role of HONO and ClNO2
Modelling the impacts of iodine chemistry on the northern Indian Ocean marine boundary layer
Time-dependent 3D simulations of tropospheric ozone depletion events in the Arctic spring using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem)
Assessing and improving cloud-height-based parameterisations of global lightning flash rate, and their impact on lightning-produced NOx and tropospheric composition in a chemistry–climate model
Impact of regional Northern Hemisphere mid-latitude anthropogenic sulfur dioxide emissions on local and remote tropospheric oxidants
Impact of organic molecular structure on the estimation of atmospherically relevant physicochemical parameters
Spatial and temporal variability in the hydroxyl (OH) radical: understanding the role of large-scale climate features and their influence on OH through its dynamical and photochemical drivers
Analysis of atmospheric ammonia over South and East Asia based on the MOZART-4 model and its comparison with satellite and surface observations
Air quality and health benefits from ultra-low emission control policy indicated by continuous emission monitoring: a case study in the Yangtze River Delta region, China
Background conditions for an urban greenhouse gas network in the Washington, DC, and Baltimore metropolitan region
Explicit modeling of isoprene chemical processing in polluted air masses in suburban areas of the Yangtze River Delta region: radical cycling and formation of ozone and formaldehyde
Evaluation of the LOTOS-EUROS NO2 simulations using ground-based measurements and S5P/TROPOMI observations over Greece
Reactive organic carbon emissions from volatile chemical products
A three-dimensional-model inversion of methyl chloroform to constrain the atmospheric oxidative capacity
Technical note: On comparing greenhouse gas emission metrics
Late-spring and summertime tropospheric ozone and NO2 in western Siberia and the Russian Arctic: regional model evaluation and sensitivities
10-year satellite-constrained fluxes of ammonia improve performance of chemistry transport models
Revealing the sulfur dioxide emission reductions in China by assimilating surface observations in WRF-Chem
Tropospheric ozone in CMIP6 simulations
Stefanie Falk, Ane V. Vollsnes, Aud B. Eriksen, Frode Stordal, and Terje Koren Berntsen
Atmos. Chem. Phys., 21, 15647–15661, https://doi.org/10.5194/acp-21-15647-2021, https://doi.org/10.5194/acp-21-15647-2021, 2021
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We evaluate regional and global models for ozone modeling and damage risk mapping of vegetation over subarctic Europe. Our analysis suggests that low-resolution global models do not reproduce the observed ozone seasonal cycle at ground level, underestimating ozone by 30–50 %. High-resolution regional models capture the seasonal cycle well, still underestimating ozone by up to 20 %. Our proposed gap-filling method for site observations shows a 76 % accuracy compared to the regional model (80 %).
Zhe Peng, Julia Lee-Taylor, Harald Stark, John J. Orlando, Bernard Aumont, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 14649–14669, https://doi.org/10.5194/acp-21-14649-2021, https://doi.org/10.5194/acp-21-14649-2021, 2021
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We use the fully explicit GECKO-A model to study the OH reactivity (OHR) evolution in the NO-free photooxidation of several volatile organic compounds. Oxidation progressively produces more saturated and functionalized species, then breaks them into small species. OHR per C atom evolution is similar for different precursors once saturated multifunctional species are formed. We also find that partitioning of these species to chamber walls leads to large deviations in chambers from the atmosphere.
Philipp G. Eger, Luc Vereecken, Rolf Sander, Jan Schuladen, Nicolas Sobanski, Horst Fischer, Einar Karu, Jonathan Williams, Ville Vakkari, Tuukka Petäjä, Jos Lelieveld, Andrea Pozzer, and John N. Crowley
Atmos. Chem. Phys., 21, 14333–14349, https://doi.org/10.5194/acp-21-14333-2021, https://doi.org/10.5194/acp-21-14333-2021, 2021
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We determine the impact of pyruvic acid photolysis on the formation of acetaldehyde and peroxy radicals during summer and autumn in the Finnish boreal forest using a data-constrained box model. Our results are dependent on the chosen scenario in which the overall quantum yield and the photolysis products are varied. We highlight that pyruvic acid photolysis can be an important contributor to acetaldehyde and peroxy radical formation in remote, forested regions.
Bharat Rastogi, John B. Miller, Micheal Trudeau, Arlyn E. Andrews, Lei Hu, Marikate Mountain, Thomas Nehrkorn, Bianca Baier, Kathryn McKain, John Mund, Kaiyu Guan, and Caroline B. Alden
Atmos. Chem. Phys., 21, 14385–14401, https://doi.org/10.5194/acp-21-14385-2021, https://doi.org/10.5194/acp-21-14385-2021, 2021
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Predicting Earth's climate is difficult, partly due to uncertainty in forecasting how much CO2 can be removed by oceans and plants, because we cannot measure these exchanges directly on large scales. Satellites such as NASA's OCO-2 can provide part of the needed information, but data need to be highly precise and accurate. We evaluate these data and find small biases in certain months that are similar to the signals of interest. We argue that continued improvement of these data is necessary.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Volker Matthias, Markus Quante, Jan A. Arndt, Ronny Badeke, Lea Fink, Ronny Petrik, Josefine Feldner, Daniel Schwarzkopf, Eliza-Maria Link, Martin O. P. Ramacher, and Ralf Wedemann
Atmos. Chem. Phys., 21, 13931–13971, https://doi.org/10.5194/acp-21-13931-2021, https://doi.org/10.5194/acp-21-13931-2021, 2021
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COVID-19 lockdown measures in spring 2020 led to cleaner air in central Europe. Densely populated areas benefitted mainly from largely reduced NO2 concentrations, while rural areas experienced lower reductions in NO2 but also lower ozone concentrations. Very low particulate matter (PM) concentrations in parts of Europe were not an effect of lockdown measures. Model simulations show that modified weather conditions are more significant for ozone and PM than severe traffic emission reductions.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven Wofsy
Atmos. Chem. Phys., 21, 13729–13746, https://doi.org/10.5194/acp-21-13729-2021, https://doi.org/10.5194/acp-21-13729-2021, 2021
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The NASA Atmospheric Tomography (ATom) mission built a climatology of the chemical composition of tropospheric air parcels throughout the middle of the Pacific and Atlantic oceans. The level of detail allows us to reconstruct the photochemical budgets of O3 and CH4 over these vast, remote regions. We find that most of the chemical heterogeneity is captured at the resolution used in current global chemistry models and that the majority of reactivity occurs in the
hottest20 % of parcels.
Ziwei Mo, Ru Cui, Bin Yuan, Huihua Cai, Brian C. McDonald, Meng Li, Junyu Zheng, and Min Shao
Atmos. Chem. Phys., 21, 13655–13666, https://doi.org/10.5194/acp-21-13655-2021, https://doi.org/10.5194/acp-21-13655-2021, 2021
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There is a lack of detailed understanding of NMVOC emissions from the use of volatile chemical products (VCPs) in China. This study used a mass balance method to compile a long-term emission inventory for solvent use (including coatings, adhesives, inks, pesticides, cleaners and personal care products) in China during 2000–2017. The striking growth and recent trend of solvent use NMVOC emissions can give important implications for air quality modeling and NMVOC control strategies in China.
R. Anthony Cox, Markus Ammann, John N. Crowley, Paul T. Griffiths, Hartmut Herrmann, Erik H. Hoffmann, Michael E. Jenkin, V. Faye McNeill, Abdelwahid Mellouki, Christopher J. Penkett, Andreas Tilgner, and Timothy J. Wallington
Atmos. Chem. Phys., 21, 13011–13018, https://doi.org/10.5194/acp-21-13011-2021, https://doi.org/10.5194/acp-21-13011-2021, 2021
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The term open-air factor was coined in the 1960s, establishing that rural air had powerful germicidal properties possibly resulting from immediate products of the reaction of ozone with alkenes, unsaturated compounds ubiquitously present in natural and polluted environments. We have re-evaluated those early experiments, applying the recently substantially improved knowledge, and put them into the context of the lifetime of aerosol-borne pathogens that are so important in the Covid-19 pandemic.
Ashu Dastoor, Andrei Ryjkov, Gregor Kos, Junhua Zhang, Jane Kirk, Matthew Parsons, and Alexandra Steffen
Atmos. Chem. Phys., 21, 12783–12807, https://doi.org/10.5194/acp-21-12783-2021, https://doi.org/10.5194/acp-21-12783-2021, 2021
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An assessment of mercury levels in air and deposition in the Athabasca oil sands region (AOSR) in Northern Alberta, Canada, was conducted to investigate the contribution of Hg emitted from oil sands activities to the surrounding landscape using a 3D process-based Hg model in 2012–2015. Oil sands Hg emissions are found to be important sources of Hg contamination to the local landscape in proximity to the processing activities, particularly in wintertime.
Le Cao, Simeng Li, and Luhang Sun
Atmos. Chem. Phys., 21, 12687–12714, https://doi.org/10.5194/acp-21-12687-2021, https://doi.org/10.5194/acp-21-12687-2021, 2021
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Gas-phase chemical reaction mechanisms, e.g., CB6 mechanism, are essential parts of the atmospheric transport model. In order to better understand the changes caused by the updates between different versions of the CB6 mechanism, in this study, the behavior of three different CB6 mechanisms in simulating ozone, nitrogen oxides and formaldehyde under two different emission conditions was analyzed using a concentration sensitivity analysis, and the reasons causing the deviations were figured out.
Yi Yin, Frederic Chevallier, Philippe Ciais, Philippe Bousquet, Marielle Saunois, Bo Zheng, John Worden, A. Anthony Bloom, Robert J. Parker, Daniel J. Jacob, Edward J. Dlugokencky, and Christian Frankenberg
Atmos. Chem. Phys., 21, 12631–12647, https://doi.org/10.5194/acp-21-12631-2021, https://doi.org/10.5194/acp-21-12631-2021, 2021
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The growth of methane, the second-most important anthropogenic greenhouse gas after carbon dioxide, has been accelerating in recent years. Using an ensemble of multi-tracer atmospheric inversions constrained by surface or satellite observations, we show that global methane emissions increased by nearly 1 % per year from 2010–2017, with leading contributions from the tropics and East Asia.
Luke Surl, Tjarda Roberts, and Slimane Bekki
Atmos. Chem. Phys., 21, 12413–12441, https://doi.org/10.5194/acp-21-12413-2021, https://doi.org/10.5194/acp-21-12413-2021, 2021
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Many different chemical reactions happen when the gases from a volcano mix with air, but what effects do they have? We present aircraft measurements which show that there is less ozone within the plume of Etna than outside it. We have also made a computer model of this chemistry. This model can reproduce the effects seen when halogens (bromine and chlorine) are included in the volcanic emissions.
We look closely at the simulation to discover how complicated halogen reactions cause ozone loss.
Claire Lamotte, Jonathan Guth, Virginie Marécal, Martin Cussac, Paul David Hamer, Nicolas Theys, and Philipp Schneider
Atmos. Chem. Phys., 21, 11379–11404, https://doi.org/10.5194/acp-21-11379-2021, https://doi.org/10.5194/acp-21-11379-2021, 2021
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Improvements are made in a global chemical transfer model by considering a new volcanic SO2 emissions inventory, with more volcanoes referenced and more information on the altitude of injection. Better constraining volcanic emissions with this inventory improves the global, but mostly local, tropospheric sulfur composition. The tropospheric sulfur budget shows a nonlinearity to the volcanic contribution, especially to the sulfate aerosol burden and sulfur wet deposition.
Simon Rosanka, Bruno Franco, Lieven Clarisse, Pierre-François Coheur, Andrea Pozzer, Andreas Wahner, and Domenico Taraborrelli
Atmos. Chem. Phys., 21, 11257–11288, https://doi.org/10.5194/acp-21-11257-2021, https://doi.org/10.5194/acp-21-11257-2021, 2021
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The strong El Niño in 2015 led to a particular dry season in Indonesia and favoured severe peatland fires. The smouldering conditions of these fires and the high carbon content of peat resulted in high volatile organic compound (VOC) emissions. By using a comprehensive atmospheric model, we show that these emissions have a significant impact on the tropospheric composition and oxidation capacity. These emissions are transported into to the lower stratosphere, resulting in a depletion of ozone.
Jianfeng Li, Yuhang Wang, Ruixiong Zhang, Charles Smeltzer, Andrew Weinheimer, Jay Herman, K. Folkert Boersma, Edward A. Celarier, Russell W. Long, James J. Szykman, Ruben Delgado, Anne M. Thompson, Travis N. Knepp, Lok N. Lamsal, Scott J. Janz, Matthew G. Kowalewski, Xiong Liu, and Caroline R. Nowlan
Atmos. Chem. Phys., 21, 11133–11160, https://doi.org/10.5194/acp-21-11133-2021, https://doi.org/10.5194/acp-21-11133-2021, 2021
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Comprehensive evaluations of simulated diurnal cycles of NO2 and NOy concentrations, vertical profiles, and tropospheric vertical column densities at two different resolutions with various measurements during the DISCOVER-AQ 2011 campaign show potential distribution biases of NOx emissions in the National Emissions Inventory 2011 at both 36 and 4 km resolutions, providing another possible explanation for the overestimation of model results.
Roman Nuterman, Alexander Mahura, Alexander Baklanov, Bjarne Amstrup, and Ashraf Zakey
Atmos. Chem. Phys., 21, 11099–11112, https://doi.org/10.5194/acp-21-11099-2021, https://doi.org/10.5194/acp-21-11099-2021, 2021
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The street air pollution is usually higher than the pollution at regional and urban scales. It mostly associated with both local emission sources and urban weather conditions. We present the downscaling system for regional, subregional-urban and street scales and evaluate it for acute air-pollution episode. Its evaluation showed a good prediction score across various spatiotemporal scales as well as feasibility of deterministic modelling approach for the operational street scale forecasting.
Min Huang, James H. Crawford, Joshua P. DiGangi, Gregory R. Carmichael, Kevin W. Bowman, Sujay V. Kumar, and Xiwu Zhan
Atmos. Chem. Phys., 21, 11013–11040, https://doi.org/10.5194/acp-21-11013-2021, https://doi.org/10.5194/acp-21-11013-2021, 2021
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This study evaluates the impact of satellite soil moisture data assimilation on modeled weather and ozone fields at various altitudes above the southeastern US during the summer. It emphasizes the importance of soil moisture in the understanding of surface ozone pollution and upper tropospheric chemistry, as well as air pollutants’ source–receptor relationships between the US and its downwind areas.
Yingnan Zhang, Likun Xue, William P. L. Carter, Chenglei Pei, Tianshu Chen, Jiangshan Mu, Yujun Wang, Qingzhu Zhang, and Wenxing Wang
Atmos. Chem. Phys., 21, 11053–11068, https://doi.org/10.5194/acp-21-11053-2021, https://doi.org/10.5194/acp-21-11053-2021, 2021
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We developed the localized incremental reactivity (IR) for VOCs in a Chinese megacity and elucidated their applications in calculating the ozone formation potential (OFP). The IR scales showed a strong dependence on chemical mechanisms. Both emission- and observation-based inputs are suitable for the MIR calculation but not the case under mixed-limited or NOx-limited O3 formation regimes. We provide suggestions for the application of IR and OFP scales to aid in VOC control in China.
Ilaria D'Elia, Gino Briganti, Lina Vitali, Antonio Piersanti, Gaia Righini, Massimo D'Isidoro, Andrea Cappelletti, Mihaela Mircea, Mario Adani, Gabriele Zanini, and Luisella Ciancarella
Atmos. Chem. Phys., 21, 10825–10849, https://doi.org/10.5194/acp-21-10825-2021, https://doi.org/10.5194/acp-21-10825-2021, 2021
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We present an analysis of modelled trends of PM10, NO2, and O3 airborne concentrations over the Italian territory in 2003–2010. Our analysis shows a general downward simulated trend for all pollutants, with good agreement between observed and modelled values and the model widening both coverage and significance of air concentration trends. Due to the complex atmospheric dynamics, emission reductions do not always result in decreasing concentrations, especially for secondary pollutants.
Chris Wilson, Martyn P. Chipperfield, Manuel Gloor, Robert J. Parker, Hartmut Boesch, Joey McNorton, Luciana V. Gatti, John B. Miller, Luana S. Basso, and Sarah A. Monks
Atmos. Chem. Phys., 21, 10643–10669, https://doi.org/10.5194/acp-21-10643-2021, https://doi.org/10.5194/acp-21-10643-2021, 2021
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Methane (CH4) is an important greenhouse gas emitted from wetlands like those found in the basin of the Amazon River. Using an atmospheric model and observations from GOSAT, we quantified CH4 emissions from Amazonia during the previous decade. We found that the largest emissions came from a region in the eastern basin and that emissions there were rising faster than in other areas of South America. This finding was supported by CH4 observations made on aircraft within the basin.
Zhenze Liu, Ruth M. Doherty, Oliver Wild, Michael Hollaway, and Fiona M. O’Connor
Atmos. Chem. Phys., 21, 10689–10706, https://doi.org/10.5194/acp-21-10689-2021, https://doi.org/10.5194/acp-21-10689-2021, 2021
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Surface ozone (O3) has become the main cause of atmospheric pollution in the summertime in China since 2013. We find that 70 % reductions in NOx emissions are required to reduce O3 pollution in most of industrial regions of China, and controls in VOC emissions are very important. The new chemical scheme developed for a global chemistry–climate model not only captures the regional air pollution but also benefits the future studies of regional air-quality–climate interactions.
Peng Wang, Juanyong Shen, Men Xia, Shida Sun, Yanli Zhang, Hongliang Zhang, and Xinming Wang
Atmos. Chem. Phys., 21, 10347–10356, https://doi.org/10.5194/acp-21-10347-2021, https://doi.org/10.5194/acp-21-10347-2021, 2021
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Ozone (O3) pollution has received extensive attention due to worsening air quality and rising health risks. The Chinese National Day holiday (CNDH), which is associated with intensive commercial and tourist activities, serves as a valuable experiment to evaluate the O3 response during the holiday. We find sharply increasing trends of observed O3 concentrations throughout China during the CNDH, leading to 33 % additional total daily deaths.
Johannes G. M. Barten, Laurens N. Ganzeveld, Gert-Jan Steeneveld, and Maarten C. Krol
Atmos. Chem. Phys., 21, 10229–10248, https://doi.org/10.5194/acp-21-10229-2021, https://doi.org/10.5194/acp-21-10229-2021, 2021
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We present an evaluation of ocean and snow/ice O3 deposition in explaining observed hourly surface O3 at 25 pan-Arctic sites using an atmospheric meteorology/chemistry model. The model includes a mechanistic representation of ocean O3 deposition as a function of ocean biogeochemical and mixing conditions. The mechanistic representation agrees better with O3 observations in terms of magnitude and temporal variability especially in the High Arctic (> 70° N).
Mark Lunt, Alistair Manning, Grant Allen, Tim Arnold, Stéphane Bauguitte, Hartmut Boesch, Anita Ganesan, Aoife Grant, Carole Helfter, Eiko Nemitz, Simon O'Doherty, Paul Palmer, Joseph Pitt, Chris Rennick, Daniel Say, Kieran Stanley, Ann Stavert, Dickon Young, and Matt Rigby
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-548, https://doi.org/10.5194/acp-2021-548, 2021
Revised manuscript accepted for ACP
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We present an evaluation of the UK's methane emissions between 2013 and 2020 using a network of tall tower measurement sites. We find emissions that are consistent in both magnitude and trend with the UK's reported emissions with a declining trend driven by a decrease in emissions from England. The impact of various components of the modelling setup on these findings are explored through a number of sensitivity studies.
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.
Wendong Ge, Junfeng Liu, Kan Yi, Jiayu Xu, Yizhou Zhang, Xiurong Hu, Jianmin Ma, Xuejun Wang, Yi Wan, Jianying Hu, Zhaobin Zhang, Xilong Wang, and Shu Tao
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-406, https://doi.org/10.5194/acp-2021-406, 2021
Revised manuscript accepted for ACP
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Compared with the observations, the results incorporating detailed aqueous-phase chemistry greatly reduced SO2 overestimation. The biases in annual simulated SO2 concentrations decreased by 46 %, 41 %, and 22 % in Europe, the United States and China, respectively. Fe-chemistry and HOx-chemistry contributed more to SO2 oxidation than N-chemistry. Higher concentrations of soluble Fe and higher pH values could further enhance the oxidation capacity.
Jianing Dai and Tao Wang
Atmos. Chem. Phys., 21, 8747–8759, https://doi.org/10.5194/acp-21-8747-2021, https://doi.org/10.5194/acp-21-8747-2021, 2021
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We used the WRF–Chem model with the latest HONO and ClNO2 processes to investigate their effects on the concentrations of ROx radicals, O3, and PM2.5 in Asia during summer. The results show that the ship-derived HONO and ClNO2 increased the ROx radical concentration by 2–3 times and subsequently increased the O3 and PM2.5 concentrations in marine areas. These findings indicate the importance of these nitrogen processes in the evaluation of the impact of ship emissions on air quality.
Anoop S. Mahajan, Qinyi Li, Swaleha Inamdar, Kirpa Ram, Alba Badia, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 21, 8437–8454, https://doi.org/10.5194/acp-21-8437-2021, https://doi.org/10.5194/acp-21-8437-2021, 2021
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Using a regional model, we show that iodine-catalysed reactions cause large regional changes in the chemical composition in the northern Indian Ocean, with peak changes of up to 25 % in O3, 50 % in nitrogen oxides (NO and NO2), 15 % in hydroxyl radicals (OH), 25 % in hydroperoxyl radicals (HO2), and up to a 50 % change in the nitrate radical (NO3). These results show the importance of including iodine chemistry in modelling the atmosphere in this region.
Maximilian Herrmann, Holger Sihler, Udo Frieß, Thomas Wagner, Ulrich Platt, and Eva Gutheil
Atmos. Chem. Phys., 21, 7611–7638, https://doi.org/10.5194/acp-21-7611-2021, https://doi.org/10.5194/acp-21-7611-2021, 2021
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Time-dependent 3D numerical simulations of tropospheric bromine release and ozone depletion events (ODEs) in the Arctic polar spring of 2009 are compared to observations. Simulation results agree well with the observations at both Utqiaġvik, Alaska, and at Summit, Greenland. In a parameter study, different settings for the bromine release mechanism are evaluated. An enhancement of the bromine release mechanism improves the agreement regarding the occurrence of ODEs with the observations.
Ashok K. Luhar, Ian E. Galbally, Matthew T. Woodhouse, and Nathan Luke Abraham
Atmos. Chem. Phys., 21, 7053–7082, https://doi.org/10.5194/acp-21-7053-2021, https://doi.org/10.5194/acp-21-7053-2021, 2021
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Lightning-generated nitrogen oxides (LNOx) greatly influence tropospheric photochemistry. The most common parameterisation of lightning flash rate used to calculate LNOx in global composition models underestimates measurements over the ocean by a factor of 20–25. We formulate and validate an alternative parameterisation to remedy this problem. The new scheme causes an increase in the ozone burden by 8.5 % and the hydroxyl radical by 13 %, and these have implications for climate and air quality.
Daniel M. Westervelt, Arlene M. Fiore, Colleen B. Baublitz, and Gustavo Correa
Atmos. Chem. Phys., 21, 6799–6810, https://doi.org/10.5194/acp-21-6799-2021, https://doi.org/10.5194/acp-21-6799-2021, 2021
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Particulate air pollution in the atmosphere can impact the availability of gas-phase chemical constituents, which can then have feedbacks on gas-phase air pollutants. We use a chemistry–climate computer model to simulate the impact of particulate pollution from three major world regions on gas-phase chemical constituents. We find that surface-level ozone air pollution decreases by up to 5 ppbv over China in response to Chinese particulate air pollution, which has implications for policy.
Gabriel Isaacman-VanWertz and Bernard Aumont
Atmos. Chem. Phys., 21, 6541–6563, https://doi.org/10.5194/acp-21-6541-2021, https://doi.org/10.5194/acp-21-6541-2021, 2021
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There are tens of thousands of different chemical compounds in the atmosphere. To tackle this complexity, there are a wide range of different methods to estimate their physical and chemical properties. We use these methods to understand how much the detailed structure of a molecule impacts its properties, and the extent to which properties can be estimated without knowing this level of detail. We find that structure matters, but methods lacking that level of detail still perform reasonably well.
Daniel C. Anderson, Bryan N. Duncan, Arlene M. Fiore, Colleen B. Baublitz, Melanie B. Follette-Cook, Julie M. Nicely, and Glenn M. Wolfe
Atmos. Chem. Phys., 21, 6481–6508, https://doi.org/10.5194/acp-21-6481-2021, https://doi.org/10.5194/acp-21-6481-2021, 2021
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We demonstrate that large-scale climate features are the primary driver of year-to-year variability in simulated values of the hydroxyl radical, the primary atmospheric oxidant, over 1980–2018. The El Niño–Southern Oscillation is the dominant mode of hydroxyl variability, resulting in large-scale global decreases in OH during El Niño events. Other climate modes, such as the Australian monsoon and the North Atlantic Oscillation, have impacts of similar magnitude but on on more localized scales.
Pooja V. Pawar, Sachin D. Ghude, Chinmay Jena, Andrea Móring, Mark A. Sutton, Santosh Kulkarni, Deen Mani Lal, Divya Surendran, Martin Van Damme, Lieven Clarisse, Pierre-François Coheur, Xuejun Liu, Gaurav Govardhan, Wen Xu, Jize Jiang, and Tapan Kumar Adhya
Atmos. Chem. Phys., 21, 6389–6409, https://doi.org/10.5194/acp-21-6389-2021, https://doi.org/10.5194/acp-21-6389-2021, 2021
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In this study, simulations of atmospheric ammonia (NH3) with MOZART-4 and HTAP-v2 are compared with satellite (IASI) and ground-based measurements to understand the spatial and temporal variability of NH3 over two emission hotspot regions of Asia, the IGP and the NCP. Our simulations indicate that the formation of ammonium aerosols is quicker over the NCP than the IGP, leading to smaller NH3 columns over the higher NH3-emitting NCP compared to the IGP region for comparable emissions.
Yan Zhang, Yu Zhao, Meng Gao, Xin Bo, and Chris P. Nielsen
Atmos. Chem. Phys., 21, 6411–6430, https://doi.org/10.5194/acp-21-6411-2021, https://doi.org/10.5194/acp-21-6411-2021, 2021
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We combined air quality and exposure response models to analyze the benefits for air quality and human health of China’s ultra-low emission policy in one of its most developed regions. Atmospheric observations and the air quality model were also used to demonstrate improvement of emission inventories incorporating online emission monitoring data. With implementation of the policy in both power and industrial sectors, the attributable deaths due to PM2.5 exposure are estimated to decrease 5.5 %.
Anna Karion, Israel Lopez-Coto, Sharon M. Gourdji, Kimberly Mueller, Subhomoy Ghosh, William Callahan, Michael Stock, Elizabeth DiGangi, Steve Prinzivalli, and James Whetstone
Atmos. Chem. Phys., 21, 6257–6273, https://doi.org/10.5194/acp-21-6257-2021, https://doi.org/10.5194/acp-21-6257-2021, 2021
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Estimating city emissions based on atmospheric observations requires that the portion of observed greenhouse gases that originated in the city be separated from the portion that originated outside the city, also known as the background concentration. Here, we investigate different methods to determine background concentrations for the Washington, DC, and Baltimore, MD, region and evaluate how well those methods work and the uncertainties they involve.
Kun Zhang, Ling Huang, Qing Li, Juntao Huo, Yusen Duan, Yuhang Wang, Elly Yaluk, Yangjun Wang, Qingyan Fu, and Li Li
Atmos. Chem. Phys., 21, 5905–5917, https://doi.org/10.5194/acp-21-5905-2021, https://doi.org/10.5194/acp-21-5905-2021, 2021
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Recently, high O3 concentrations were frequently observed in rural areas of the Yangtze River Delta (YRD) region under stagnant conditions. Using an online measurement and observation-based model, we investigated the budget of ROx radicals and the influence of isoprene chemistry on O3 formation. Our results underline that isoprene chemistry in the rural atmosphere becomes important with the participation of anthropogenic NOx.
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.
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Short summary
Quantifying emission changes is a prerequisite for assessment of control effectiveness in improving air quality. However, traditional bottom-up methods usually take months to perform and limit timely assessments. A novel method was developed by using a response model that provides real-time estimation of emission changes based on air quality observations. It was successfully applied to quantify emission changes on the North China Plain due to the COVID-19 pandemic shutdown.
Quantifying emission changes is a prerequisite for assessment of control effectiveness in...
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