Research article
30 Jan 2018
Research article
| 30 Jan 2018
Ozone trends over the United States at different times of day
Yingying Yan et al.
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Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2022-154, https://doi.org/10.5194/essd-2022-154, 2022
Preprint under review for ESSD
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We present an emission inventory from 2000 to 2018 with a high spatial-temporal resolution for five missing sources that are related to people’s daily life. The emission factors of carbonaceous aerosol were tested in our laboratory, and activity data were obtained from the combination of multiple proxy data.
Kelvin H. Bates, Daniel J. Jacob, Ke Li, Peter D. Ivatt, Mat J. Evans, Yingying Yan, and Jintai Lin
Atmos. Chem. Phys., 21, 18351–18374, https://doi.org/10.5194/acp-21-18351-2021, https://doi.org/10.5194/acp-21-18351-2021, 2021
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Simple aromatic compounds (benzene, toluene, xylene) have complex gas-phase chemistry that is inconsistently represented in atmospheric models. We compile recent experimental and theoretical insights to develop a new mechanism for gas-phase aromatic oxidation that is sufficiently compact for use in multiscale models. We compare our new mechanism to chamber experiments and other mechanisms, and implement it in a global model to quantify the impacts of aromatic oxidation on tropospheric chemistry.
Yingying Yan, Yue Zhou, Shaofei Kong, Jintai Lin, Jian Wu, Huang Zheng, Zexuan Zhang, Aili Song, Yongqing Bai, Zhang Ling, Dantong Liu, and Tianliang Zhao
Atmos. Chem. Phys., 21, 3143–3162, https://doi.org/10.5194/acp-21-3143-2021, https://doi.org/10.5194/acp-21-3143-2021, 2021
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We analyze the effectiveness of emission reduction for local and upwind regions during winter haze episodes controlled by the main potential synoptic patterns over central China, a regional pollutant transport hub with sub-basin topography. Our results provide an opportunity to effectively mitigate haze pollution via local emission control actions in coordination with regional collaborative actions according to different synoptic patterns.
Mengyao Liu, Jintai Lin, Hao Kong, K. Folkert Boersma, Henk Eskes, Yugo Kanaya, Qin He, Xin Tian, Kai Qin, Pinhua Xie, Robert Spurr, Ruijing Ni, Yingying Yan, Hongjian Weng, and Jingxu Wang
Atmos. Meas. Tech., 13, 4247–4259, https://doi.org/10.5194/amt-13-4247-2020, https://doi.org/10.5194/amt-13-4247-2020, 2020
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Nitrogen oxides (NOx = NO + NO2) are important air pollutants in the troposphere and play crucial roles in the formation of ozone and particulate matter. The recently launched TROPOspheric Monitoring Instrument (TROPOMI) provides an opportunity to retrieve tropospheric concentrations of nitrogen dioxide (NO2) at an unprecedented high horizontal resolution. This work presents a new NO2 retrieval product over East Asia and further quantifies key factors affecting the retrieval, including aerosol.
Hao Kong, Jintai Lin, Ruixiong Zhang, Mengyao Liu, Hongjian Weng, Ruijing Ni, Lulu Chen, Jingxu Wang, Yingying Yan, and Qiang Zhang
Atmos. Chem. Phys., 19, 12835–12856, https://doi.org/10.5194/acp-19-12835-2019, https://doi.org/10.5194/acp-19-12835-2019, 2019
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We develop a computationally efficient space-based top-down method to inverting NOx emissions in major urban areas at high resolution. The inversion method uses long-term OMI NO2 data to enhance the horizontal resolution, and it accounts for the nonlinear effects of horizontal transport, chemical loss, and deposition on NOx. The inversion results reveal fine-scale spatial information of emissions which is hardly captured by bottom-up inventories.
Huang Zheng, Shaofei Kong, Fangqi Wu, Yi Cheng, Zhenzhen Niu, Shurui Zheng, Guowei Yang, Liquan Yao, Qin Yan, Jian Wu, Mingming Zheng, Nan Chen, Ke Xu, Yingying Yan, Dantong Liu, Delong Zhao, Tianliang Zhao, Yongqing Bai, Shuanglin Li, and Shihua Qi
Atmos. Chem. Phys., 19, 4499–4516, https://doi.org/10.5194/acp-19-4499-2019, https://doi.org/10.5194/acp-19-4499-2019, 2019
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This study simultaneously observed black carbon (BC) at five sites in central China and on the south edge of North China Plain, which have the most serious air pollution issues in China. The differences in BC properties between different air quality conditions and the property changes during transportation were studied. The main findings of this study were that during the downwind transportation of air, the BC mass concentration increased, whereas the absorption Ångström exponent decreased.
Lei Sun, Likun Xue, Yuhang Wang, Longlei Li, Jintai Lin, Ruijing Ni, Yingying Yan, Lulu Chen, Juan Li, Qingzhu Zhang, and Wenxing Wang
Atmos. Chem. Phys., 19, 1455–1469, https://doi.org/10.5194/acp-19-1455-2019, https://doi.org/10.5194/acp-19-1455-2019, 2019
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We quantified the detailed impacts of meteorology and anthropogenic emissions on surface O3 increase in central eastern China between 2003 and 2015 using GEOS-Chem. The emission change plays a more important role than the meteorological change, while the regions with a larger O3 increase are more sensitive to meteorology. NMVOC emission change dominated the O3 increase in eastern CEC, while NOx emission change led to an O3 increase in western and central CEC and O3 decrease in urban areas.
Yingying Yan, David Cabrera-Perez, Jintai Lin, Andrea Pozzer, Lu Hu, Dylan B. Millet, William C. Porter, and Jos Lelieveld
Geosci. Model Dev., 12, 111–130, https://doi.org/10.5194/gmd-12-111-2019, https://doi.org/10.5194/gmd-12-111-2019, 2019
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The GEOS-Chem model has been updated with the SAPRC-11 aromatics chemical mechanism to evaluate global and regional effects of aromatics on tropospheric oxidation capacity. Our results reveal relatively slight changes in ozone, hydroxyl radical, and nitrogen oxides on a global mean basis (1–4 %), although remarkable regional differences (5–20 %) exist near the source regions. Improved representation of aromatics is important to simulate the tropospheric oxidation.
Mengyao Liu, Jintai Lin, K. Folkert Boersma, Gaia Pinardi, Yang Wang, Julien Chimot, Thomas Wagner, Pinhua Xie, Henk Eskes, Michel Van Roozendael, François Hendrick, Pucai Wang, Ting Wang, Yingying Yan, Lulu Chen, and Ruijing Ni
Atmos. Meas. Tech., 12, 1–21, https://doi.org/10.5194/amt-12-1-2019, https://doi.org/10.5194/amt-12-1-2019, 2019
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China has become the world’s largest emitter of NOx, which mainly comes from vehicle exhaust, power plants, etc. However, there are no official ground-based measurements before 2013, so satellites have been widely used to monitor and analyze NOx pollution here. Aerosol is the key factor influencing the accuracy of the satellite NOx product. Our study provides a more accurate way to account for aerosol's influence compared to current widely used products.
Mengyao Liu, Jintai Lin, Yuchen Wang, Yang Sun, Bo Zheng, Jingyuan Shao, Lulu Chen, Yixuan Zheng, Jinxuan Chen, Tzung-May Fu, Yingying Yan, Qiang Zhang, and Zhaohua Wu
Atmos. Chem. Phys., 18, 12933–12952, https://doi.org/10.5194/acp-18-12933-2018, https://doi.org/10.5194/acp-18-12933-2018, 2018
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Eastern China is heavily polluted by NO2, PM2.5, and other air pollutants. Our study uses EOF–EEMD to analyze the spatiotemporal variability of ground-level NO2, PM2.5, and their associations with meteorological processes. Their regular diurnal cycles are mainly affected by human activities, while irregular day-to-day variations are dominated by weather processes representing synchronous variation or north–south opposing changes over Eastern China.
Ruijing Ni, Jintai Lin, Yingying Yan, and Weili Lin
Atmos. Chem. Phys., 18, 11447–11469, https://doi.org/10.5194/acp-18-11447-2018, https://doi.org/10.5194/acp-18-11447-2018, 2018
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By integrating several modeling methods, we find considerable contributions of foreign anthropogenic emissions to surface ozone over China (2–11 ppb). For anthropogenic ozone over China, the foreign contribution is 40–50 % below 2 km and 85 % in the upper troposphere. For total foreign anthropogenic ozone over China, the portion of transboundary ozone produced within foreign emission source regions is less than 50 %, with the rest produced by precursors transported out of those source regions.
Yingying Yan, Andrea Pozzer, Narendra Ojha, Jintai Lin, and Jos Lelieveld
Atmos. Chem. Phys., 18, 5589–5605, https://doi.org/10.5194/acp-18-5589-2018, https://doi.org/10.5194/acp-18-5589-2018, 2018
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Surface-based measurements from the EMEP network and EMAC model simulations are used to estimate the European surface ozone changes over 1995–2014. It shows a significantly decreasing trend in the 95th percentile ozone concentrations, while increasing in the 5th percentile ozone. Sensitivity simulations and statistical analysis show that a decrease in European anthropogenic emissions had contrasting effects on surface ozone trends between the 95th and 5th percentile levels.
Yuanzheng Cui, Jintai Lin, Chunqiao Song, Mengyao Liu, Yingying Yan, Yuan Xu, and Bo Huang
Atmos. Chem. Phys., 16, 6207–6221, https://doi.org/10.5194/acp-16-6207-2016, https://doi.org/10.5194/acp-16-6207-2016, 2016
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We find rapid NO2 growth over Western China over 2005–2013 at a rate which exceeds the rates over the well-known polluted regions in the east. A nested GEOS-Chem simulation and Chinese official emission data confirm that anthropogenic emissions are the main driver of NO2 variations. Additional socioeconomic analysis suggests that this rapid NO2 growth is likely related to the fast industrialization and urbanization along with the "Go West" movement as well as relatively weak emission controls.
Yingying Yan, Jintai Lin, Jinxuan Chen, and Lu Hu
Atmos. Chem. Phys., 16, 2381–2400, https://doi.org/10.5194/acp-16-2381-2016, https://doi.org/10.5194/acp-16-2381-2016, 2016
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We use a newly built two-way coupling system of the GEOS-Chem CTM to simulate the global tropospheric O3 in 2009. It significantly improves the simulation upon the global model by comparisons with a suite of ground, aircraft, and satellite measurements, also reduces the global OH by 5 % with enhancements by 5 % in the lifetimes of MCF and methane. Therefore, improving model representations of small-scale processes is a critical step forward to understanding the global tropospheric chemistry.
Y.-Y. Yan, J.-T. Lin, Y. Kuang, D. Yang, and L. Zhang
Atmos. Chem. Phys., 14, 12649–12663, https://doi.org/10.5194/acp-14-12649-2014, https://doi.org/10.5194/acp-14-12649-2014, 2014
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Limited by coarse resolutions, global chemical transport models cannot well capture small-scale nonlinear processes. To alleviate the problem, we develop a two-way coupled system to integrate the global GEOS-Chem model and its three high-resolution nested models covering Asia, Europe and North America. Confirmed by comparisons with observations, the coupled system improves upon the global model with a 10% increase in global tropospheric CO, a 4% decrease in OH and a 4% increase in MCF lifetime.
Chaman Gul, Shichang Kang, Siva Praveen Puppala, Xiaokang Wu, Cenlin He, Yangyang Xu, Inka Koch, Sher Muhammad, Rajesh Kumar, and Getachew Dubache
Atmos. Chem. Phys., 22, 8725–8737, https://doi.org/10.5194/acp-22-8725-2022, https://doi.org/10.5194/acp-22-8725-2022, 2022
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This work aims to understand concentrations, spatial variability, and potential source regions of light-absorbing impurities (black carbon aerosols, dust particles, and organic carbon) in the surface snow of central and western Himalayan glaciers and their impact on snow albedo and radiative forcing.
Huilin Huang, Yun Qian, Ye Liu, Cenlin He, Jianyu Zheng, Zhibo Zhang, and Antonis Gkikas
EGUsphere, https://doi.org/10.5194/egusphere-2022-588, https://doi.org/10.5194/egusphere-2022-588, 2022
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Using a clustering method developed in the field of artificial neural networks, we identify four typical dust transport patterns across the Sierra Nevada, associated with the mesoscale and regional scale wind circulations. Our results highlight the connection between dust transport and dominant weather patterns, which can be used to understand dust transport in a changing climate.
Yi Cheng, Shaofei Kong, Liquan Yao, Huang Zheng, Jian Wu, Qin Yan, Shurui Zheng, Yao Hu, Zhenzhen Niu, Yingying Yan, Zhenxing Shen, Guofeng Shen, Dantong Liu, Shuxiao Wang, and Shihua Qi
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2022-154, https://doi.org/10.5194/essd-2022-154, 2022
Preprint under review for ESSD
Short summary
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We present an emission inventory from 2000 to 2018 with a high spatial-temporal resolution for five missing sources that are related to people’s daily life. The emission factors of carbonaceous aerosol were tested in our laboratory, and activity data were obtained from the combination of multiple proxy data.
Dalei Hao, Gautam Bisht, Cenlin He, Edward Bair, Huilin Huang, Cheng Dang, Karl Rittger, Yu Gu, Hailong Wang, Yun Qian, and L. Ruby Leung
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2022-67, https://doi.org/10.5194/gmd-2022-67, 2022
Preprint under review for GMD
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Snow with the highest albedo of land surface plays a vital role in Earth’s surface energy and water cycles. Our study demonstrates that snow grain shape and mixing state of light absorbing particle-snow play an important role in snow processes, surface energy balance and water cycle. This study offers guidance for improving snow simulations and surface radiative forcing estimates in Earth system models under future climate.
Mark G. Flanner, Julian B. Arnheim, Joseph M. Cook, Cheng Dang, Cenlin He, Xianglei Huang, Deepak Singh, S. McKenzie Skiles, Chloe A. Whicker, and Charles S. Zender
Geosci. Model Dev., 14, 7673–7704, https://doi.org/10.5194/gmd-14-7673-2021, https://doi.org/10.5194/gmd-14-7673-2021, 2021
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We present the technical formulation and evaluation of a publicly available code and web-based model to simulate the spectral albedo of snow. Our model accounts for numerous features of the snow state and ambient conditions, including the the presence of light-absorbing matter like black and brown carbon, mineral dust, volcanic ash, and snow algae. Carbon dioxide snow, found on Mars, is also represented. The model accurately reproduces spectral measurements of clean and contaminated snow.
Kelvin H. Bates, Daniel J. Jacob, Ke Li, Peter D. Ivatt, Mat J. Evans, Yingying Yan, and Jintai Lin
Atmos. Chem. Phys., 21, 18351–18374, https://doi.org/10.5194/acp-21-18351-2021, https://doi.org/10.5194/acp-21-18351-2021, 2021
Short summary
Short summary
Simple aromatic compounds (benzene, toluene, xylene) have complex gas-phase chemistry that is inconsistently represented in atmospheric models. We compile recent experimental and theoretical insights to develop a new mechanism for gas-phase aromatic oxidation that is sufficiently compact for use in multiscale models. We compare our new mechanism to chamber experiments and other mechanisms, and implement it in a global model to quantify the impacts of aromatic oxidation on tropospheric chemistry.
Liam Bindle, Randall V. Martin, Matthew J. Cooper, Elizabeth W. Lundgren, Sebastian D. Eastham, Benjamin M. Auer, Thomas L. Clune, Hongjian Weng, Jintai Lin, Lee T. Murray, Jun Meng, Christoph A. Keller, William M. Putman, Steven Pawson, and Daniel J. Jacob
Geosci. Model Dev., 14, 5977–5997, https://doi.org/10.5194/gmd-14-5977-2021, https://doi.org/10.5194/gmd-14-5977-2021, 2021
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Atmospheric chemistry models like GEOS-Chem are versatile tools widely used in air pollution and climate studies. The simulations used in such studies can be very computationally demanding, and thus it is useful if the model can simulate a specific geographic region at a higher resolution than the rest of the globe. Here, we implement, test, and demonstrate a new variable-resolution capability in GEOS-Chem that is suitable for simulations conducted on supercomputers.
Yingying Yan, Yue Zhou, Shaofei Kong, Jintai Lin, Jian Wu, Huang Zheng, Zexuan Zhang, Aili Song, Yongqing Bai, Zhang Ling, Dantong Liu, and Tianliang Zhao
Atmos. Chem. Phys., 21, 3143–3162, https://doi.org/10.5194/acp-21-3143-2021, https://doi.org/10.5194/acp-21-3143-2021, 2021
Short summary
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We analyze the effectiveness of emission reduction for local and upwind regions during winter haze episodes controlled by the main potential synoptic patterns over central China, a regional pollutant transport hub with sub-basin topography. Our results provide an opportunity to effectively mitigate haze pollution via local emission control actions in coordination with regional collaborative actions according to different synoptic patterns.
Julián Gelman Constantin, Lucas Ruiz, Gustavo Villarosa, Valeria Outes, Facundo N. Bajano, Cenlin He, Hector Bajano, and Laura Dawidowski
The Cryosphere, 14, 4581–4601, https://doi.org/10.5194/tc-14-4581-2020, https://doi.org/10.5194/tc-14-4581-2020, 2020
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We present the results of two field campaigns and modeling activities on the impact of atmospheric particles on Alerce Glacier (Argentinean Andes). We found that volcanic ash remains at different snow layers several years after eruption, increasing light absorption on the glacier surface (with a minor contribution of soot). This leads to 36 % higher annual glacier melting. We find remarkably that volcano eruptions in 2011 and 2015 have a relevant effect on the glacier even in 2016 and 2017.
Wenfu Tang, Benjamin Gaubert, Louisa Emmons, Yonghoon Choi, Joshua P. DiGangi, Glenn S. Diskin, Xiaomei Xu, Cenlin He, Helen Worden, Simone Tilmes, Rebecca Buchholz, Hannah S. Halliday, and Avelino F. Arellano
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-864, https://doi.org/10.5194/acp-2020-864, 2020
Revised manuscript not accepted
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A specific demonstration of the potential use of correlative information from carbon monoxide to refine estimates of regional carbon dioxide emissions from fossil fuel combustion.
Mengyao Liu, Jintai Lin, Hao Kong, K. Folkert Boersma, Henk Eskes, Yugo Kanaya, Qin He, Xin Tian, Kai Qin, Pinhua Xie, Robert Spurr, Ruijing Ni, Yingying Yan, Hongjian Weng, and Jingxu Wang
Atmos. Meas. Tech., 13, 4247–4259, https://doi.org/10.5194/amt-13-4247-2020, https://doi.org/10.5194/amt-13-4247-2020, 2020
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Nitrogen oxides (NOx = NO + NO2) are important air pollutants in the troposphere and play crucial roles in the formation of ozone and particulate matter. The recently launched TROPOspheric Monitoring Instrument (TROPOMI) provides an opportunity to retrieve tropospheric concentrations of nitrogen dioxide (NO2) at an unprecedented high horizontal resolution. This work presents a new NO2 retrieval product over East Asia and further quantifies key factors affecting the retrieval, including aerosol.
Viral Shah, Daniel J. Jacob, Ke Li, Rachel F. Silvern, Shixian Zhai, Mengyao Liu, Jintai Lin, and Qiang Zhang
Atmos. Chem. Phys., 20, 1483–1495, https://doi.org/10.5194/acp-20-1483-2020, https://doi.org/10.5194/acp-20-1483-2020, 2020
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We analyze 15 years of satellite observations of nitrogen dioxide (NO2) and use an atmospheric chemistry model to understand the seasonal changes and trends in nitrogen oxides (NOx) over China. We show that the seasonal changes in NO2 occur due to changes in the NOx oxidation lifetime. We find that Chinese NOx emissions peaked in 2011 and had decreased by about 25 % by 2018. But the decrease in NO2 in winter was larger, likely because of a simultaneous decrease in the NOx oxidation lifetime.
Hao Kong, Jintai Lin, Ruixiong Zhang, Mengyao Liu, Hongjian Weng, Ruijing Ni, Lulu Chen, Jingxu Wang, Yingying Yan, and Qiang Zhang
Atmos. Chem. Phys., 19, 12835–12856, https://doi.org/10.5194/acp-19-12835-2019, https://doi.org/10.5194/acp-19-12835-2019, 2019
Short summary
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We develop a computationally efficient space-based top-down method to inverting NOx emissions in major urban areas at high resolution. The inversion method uses long-term OMI NO2 data to enhance the horizontal resolution, and it accounts for the nonlinear effects of horizontal transport, chemical loss, and deposition on NOx. The inversion results reveal fine-scale spatial information of emissions which is hardly captured by bottom-up inventories.
Wei Pu, Jiecan Cui, Tenglong Shi, Xuelei Zhang, Cenlin He, and Xin Wang
Atmos. Chem. Phys., 19, 9949–9968, https://doi.org/10.5194/acp-19-9949-2019, https://doi.org/10.5194/acp-19-9949-2019, 2019
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LAPs (light-absorbing particles) deposited on snow can decrease snow albedo and increase the absorption of solar radiation. Radiative forcing by LAPs will affect the regional hydrological cycle and climate. We use MODIS observations to retrieve the radiative forcing by LAPs in snow across northeastern China (NEC). The results of radiative forcing present distinct spatial variability. We find that the biases are negatively correlated with LAP concentrations and range from
~ 5 % to ~ 350 %.
Xiao Lu, Lin Zhang, Youfan Chen, Mi Zhou, Bo Zheng, Ke Li, Yiming Liu, Jintai Lin, Tzung-May Fu, and Qiang Zhang
Atmos. Chem. Phys., 19, 8339–8361, https://doi.org/10.5194/acp-19-8339-2019, https://doi.org/10.5194/acp-19-8339-2019, 2019
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Severe and deteriorating surface ozone pollution over major Chinese cities has become an emerging environmental concern in China. This study assesses the source contributions (including anthropogenic, background, and individual natural sources) and meteorological influences of surface ozone over China in 2016–2017 using the GEOS-Chem chemical transport model at high horizontal resolution with the most up-to-date Chinese anthropogenic emission inventory.
Huang Zheng, Shaofei Kong, Fangqi Wu, Yi Cheng, Zhenzhen Niu, Shurui Zheng, Guowei Yang, Liquan Yao, Qin Yan, Jian Wu, Mingming Zheng, Nan Chen, Ke Xu, Yingying Yan, Dantong Liu, Delong Zhao, Tianliang Zhao, Yongqing Bai, Shuanglin Li, and Shihua Qi
Atmos. Chem. Phys., 19, 4499–4516, https://doi.org/10.5194/acp-19-4499-2019, https://doi.org/10.5194/acp-19-4499-2019, 2019
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This study simultaneously observed black carbon (BC) at five sites in central China and on the south edge of North China Plain, which have the most serious air pollution issues in China. The differences in BC properties between different air quality conditions and the property changes during transportation were studied. The main findings of this study were that during the downwind transportation of air, the BC mass concentration increased, whereas the absorption Ångström exponent decreased.
Lei Sun, Likun Xue, Yuhang Wang, Longlei Li, Jintai Lin, Ruijing Ni, Yingying Yan, Lulu Chen, Juan Li, Qingzhu Zhang, and Wenxing Wang
Atmos. Chem. Phys., 19, 1455–1469, https://doi.org/10.5194/acp-19-1455-2019, https://doi.org/10.5194/acp-19-1455-2019, 2019
Short summary
Short summary
We quantified the detailed impacts of meteorology and anthropogenic emissions on surface O3 increase in central eastern China between 2003 and 2015 using GEOS-Chem. The emission change plays a more important role than the meteorological change, while the regions with a larger O3 increase are more sensitive to meteorology. NMVOC emission change dominated the O3 increase in eastern CEC, while NOx emission change led to an O3 increase in western and central CEC and O3 decrease in urban areas.
Yingying Yan, David Cabrera-Perez, Jintai Lin, Andrea Pozzer, Lu Hu, Dylan B. Millet, William C. Porter, and Jos Lelieveld
Geosci. Model Dev., 12, 111–130, https://doi.org/10.5194/gmd-12-111-2019, https://doi.org/10.5194/gmd-12-111-2019, 2019
Short summary
Short summary
The GEOS-Chem model has been updated with the SAPRC-11 aromatics chemical mechanism to evaluate global and regional effects of aromatics on tropospheric oxidation capacity. Our results reveal relatively slight changes in ozone, hydroxyl radical, and nitrogen oxides on a global mean basis (1–4 %), although remarkable regional differences (5–20 %) exist near the source regions. Improved representation of aromatics is important to simulate the tropospheric oxidation.
Mengyao Liu, Jintai Lin, K. Folkert Boersma, Gaia Pinardi, Yang Wang, Julien Chimot, Thomas Wagner, Pinhua Xie, Henk Eskes, Michel Van Roozendael, François Hendrick, Pucai Wang, Ting Wang, Yingying Yan, Lulu Chen, and Ruijing Ni
Atmos. Meas. Tech., 12, 1–21, https://doi.org/10.5194/amt-12-1-2019, https://doi.org/10.5194/amt-12-1-2019, 2019
Short summary
Short summary
China has become the world’s largest emitter of NOx, which mainly comes from vehicle exhaust, power plants, etc. However, there are no official ground-based measurements before 2013, so satellites have been widely used to monitor and analyze NOx pollution here. Aerosol is the key factor influencing the accuracy of the satellite NOx product. Our study provides a more accurate way to account for aerosol's influence compared to current widely used products.
Mengyao Liu, Jintai Lin, Yuchen Wang, Yang Sun, Bo Zheng, Jingyuan Shao, Lulu Chen, Yixuan Zheng, Jinxuan Chen, Tzung-May Fu, Yingying Yan, Qiang Zhang, and Zhaohua Wu
Atmos. Chem. Phys., 18, 12933–12952, https://doi.org/10.5194/acp-18-12933-2018, https://doi.org/10.5194/acp-18-12933-2018, 2018
Short summary
Short summary
Eastern China is heavily polluted by NO2, PM2.5, and other air pollutants. Our study uses EOF–EEMD to analyze the spatiotemporal variability of ground-level NO2, PM2.5, and their associations with meteorological processes. Their regular diurnal cycles are mainly affected by human activities, while irregular day-to-day variations are dominated by weather processes representing synchronous variation or north–south opposing changes over Eastern China.
Ruijing Ni, Jintai Lin, Yingying Yan, and Weili Lin
Atmos. Chem. Phys., 18, 11447–11469, https://doi.org/10.5194/acp-18-11447-2018, https://doi.org/10.5194/acp-18-11447-2018, 2018
Short summary
Short summary
By integrating several modeling methods, we find considerable contributions of foreign anthropogenic emissions to surface ozone over China (2–11 ppb). For anthropogenic ozone over China, the foreign contribution is 40–50 % below 2 km and 85 % in the upper troposphere. For total foreign anthropogenic ozone over China, the portion of transboundary ozone produced within foreign emission source regions is less than 50 %, with the rest produced by precursors transported out of those source regions.
Cenlin He, Mark G. Flanner, Fei Chen, Michael Barlage, Kuo-Nan Liou, Shichang Kang, Jing Ming, and Yun Qian
Atmos. Chem. Phys., 18, 11507–11527, https://doi.org/10.5194/acp-18-11507-2018, https://doi.org/10.5194/acp-18-11507-2018, 2018
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Snow albedo plays a key role in the Earth and climate system. It can be affected by impurities and snow properties. This study implements new parameterizations into a widely used snow model to account for effects of snow shape and black carbon–snow mixing state on snow albedo reduction in the Tibetan Plateau. This study points toward an imperative need for extensive measurements and improved model characterization of snow grain shape and aerosol–snow mixing state in Tibet and elsewhere.
Yingying Yan, Andrea Pozzer, Narendra Ojha, Jintai Lin, and Jos Lelieveld
Atmos. Chem. Phys., 18, 5589–5605, https://doi.org/10.5194/acp-18-5589-2018, https://doi.org/10.5194/acp-18-5589-2018, 2018
Short summary
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Surface-based measurements from the EMEP network and EMAC model simulations are used to estimate the European surface ozone changes over 1995–2014. It shows a significantly decreasing trend in the 95th percentile ozone concentrations, while increasing in the 5th percentile ozone. Sensitivity simulations and statistical analysis show that a decrease in European anthropogenic emissions had contrasting effects on surface ozone trends between the 95th and 5th percentile levels.
Bin Zhao, Kuo-Nan Liou, Yu Gu, Jonathan H. Jiang, Qinbin Li, Rong Fu, Lei Huang, Xiaohong Liu, Xiangjun Shi, Hui Su, and Cenlin He
Atmos. Chem. Phys., 18, 1065–1078, https://doi.org/10.5194/acp-18-1065-2018, https://doi.org/10.5194/acp-18-1065-2018, 2018
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The interactions between aerosols and ice clouds represent one of the largest uncertainties among anthropogenic forcings on climate change. We find that the responses of ice crystal effective radius, a key parameter determining ice clouds' net radiative effect, to aerosol loadings are modulated by water vapor amount and vary from a significant negative correlation in moist conditions (consistent with the “Twomey effect” for liquid clouds) to a strong positive correlation in dry conditions.
Hongyan Zhao, Xin Li, Qiang Zhang, Xujia Jiang, Jintai Lin, Glen P. Peters, Meng Li, Guannan Geng, Bo Zheng, Hong Huo, Lin Zhang, Haikun Wang, Steven J. Davis, and Kebin He
Atmos. Chem. Phys., 17, 10367–10381, https://doi.org/10.5194/acp-17-10367-2017, https://doi.org/10.5194/acp-17-10367-2017, 2017
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Effective and efficient control of air pollution relies upon an understanding of the pollution sources. We conduct an interdisciplinary study and find that 33 % of China’s PM2.5-related premature mortality in 2010 were caused by production emission in other regions; 56 % of the mortality was related to consumption in other regions. Multilateral and multi-stage cooperation under a regional sustainable development framework is in urgent need to mitigate air pollution and related health impacts.
Ling Qi, Qinbin Li, Daven K. Henze, Hsien-Liang Tseng, and Cenlin He
Atmos. Chem. Phys., 17, 9697–9716, https://doi.org/10.5194/acp-17-9697-2017, https://doi.org/10.5194/acp-17-9697-2017, 2017
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We find that Asian anthropogenic sources are the largest contributors (~ 40 %) to surface BC in spring in the Arctic, inconsistent with previous studies which repeatedly identified sources of surface BC as anthropogenic emissions from Europe and Russia. It takes 12–17 days for Asian anthropogenic emissions to be transported to the Arctic surface. Additionally, a large fraction (40–65 %) of Asian contribution is in the form of chronic pollution on 1- to 2-month timescales.
Katherine R. Travis, Daniel J. Jacob, Christoph A. Keller, Shi Kuang, Jintai Lin, Michael J. Newchurch, and Anne M. Thompson
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-596, https://doi.org/10.5194/acp-2017-596, 2017
Preprint retracted
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Models severely overestimate surface ozone in the Southeast US during summertime which has implications for the design of air quality regulations. We use a model (GEOS-Chem) to interpret ozone observations from a suite of observations taken during August–September 2013. The model is unbiased relative to observations below 1 km but is biased high at the surface. We attribute this bias to model representation error, an underestimate in low-cloud, and insufficient treatment of vertical mixing.
Ling Qi, Qinbin Li, Cenlin He, Xin Wang, and Jianping Huang
Atmos. Chem. Phys., 17, 7459–7479, https://doi.org/10.5194/acp-17-7459-2017, https://doi.org/10.5194/acp-17-7459-2017, 2017
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Black carbon (BC) is the second only to CO2 in heating the planet, but the simulation of BC is associated with large uncertainties. BC burden is largely underestimated over land and overestimated over ocean. Our study finds that a missing process in current Wegener–Bergeron–Findeisen models largely explains the discrepancy in BC simulation over land. We call for more observations of BC in mixed-phase clouds to understand this process and improve the simulation of global BC.
Guannan Geng, Qiang Zhang, Randall V. Martin, Jintai Lin, Hong Huo, Bo Zheng, Siwen Wang, and Kebin He
Atmos. Chem. Phys., 17, 4131–4145, https://doi.org/10.5194/acp-17-4131-2017, https://doi.org/10.5194/acp-17-4131-2017, 2017
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We investigated the impact of spatial proxies on the representation of gridded emissions by comparing six gridded NOx emission datasets over China developed from the same magnitude of emissions and different spatial proxies. GEOS-Chem-modeled NO2 columns from the six gridded emissions are compared with satellite-based columns from OMI. Results show that differences between modeled and satellite-based NO2 columns are sensitive to the spatial proxies used in the gridded emission inventories.
Alba Lorente, K. Folkert Boersma, Huan Yu, Steffen Dörner, Andreas Hilboll, Andreas Richter, Mengyao Liu, Lok N. Lamsal, Michael Barkley, Isabelle De Smedt, Michel Van Roozendael, Yang Wang, Thomas Wagner, Steffen Beirle, Jin-Tai Lin, Nickolay Krotkov, Piet Stammes, Ping Wang, Henk J. Eskes, and Maarten Krol
Atmos. Meas. Tech., 10, 759–782, https://doi.org/10.5194/amt-10-759-2017, https://doi.org/10.5194/amt-10-759-2017, 2017
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Choices and assumptions made to represent the state of the atmosphere introduce an uncertainty of 42 % in the air mass factor calculation in trace gas satellite retrievals in polluted regions. The AMF strongly depends on the choice of a priori trace gas profile, surface albedo data set and the correction method to account for clouds and aerosols. We call for well-designed validation exercises focusing on situations when AMF structural uncertainty has the highest impact on satellite retrievals.
Ling Qi, Qinbin Li, Yinrui Li, and Cenlin He
Atmos. Chem. Phys., 17, 1037–1059, https://doi.org/10.5194/acp-17-1037-2017, https://doi.org/10.5194/acp-17-1037-2017, 2017
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The Arctic is the most vulnerable region for climate change. Black carbon (BC) in air and deposited on snow and ice warms the Arctic substantially, but simulations of BC climate effects are associated with large uncertainties. To reduce this uncertainty, it is imperative to improve the simulation of BC distribution in the Arctic. We evaluate the effects of controlling factors (emissions, dry and wet deposition) on BC distribution and call for more observations to constrain these processes.
Yuanzheng Cui, Jintai Lin, Chunqiao Song, Mengyao Liu, Yingying Yan, Yuan Xu, and Bo Huang
Atmos. Chem. Phys., 16, 6207–6221, https://doi.org/10.5194/acp-16-6207-2016, https://doi.org/10.5194/acp-16-6207-2016, 2016
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We find rapid NO2 growth over Western China over 2005–2013 at a rate which exceeds the rates over the well-known polluted regions in the east. A nested GEOS-Chem simulation and Chinese official emission data confirm that anthropogenic emissions are the main driver of NO2 variations. Additional socioeconomic analysis suggests that this rapid NO2 growth is likely related to the fast industrialization and urbanization along with the "Go West" movement as well as relatively weak emission controls.
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.
Cenlin He, Qinbin Li, Kuo-Nan Liou, Ling Qi, Shu Tao, and Joshua P. Schwarz
Atmos. Chem. Phys., 16, 3077–3098, https://doi.org/10.5194/acp-16-3077-2016, https://doi.org/10.5194/acp-16-3077-2016, 2016
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Blarck carbon aging significantly affects its global distribution and thus climatic effects. This study develops a microphysics-based BC aging scheme in a global model, which substantially improves model simulations of BC over the remote Pacific. The microphysical scheme shows fast aging over source regions and much slower aging in remote regions. The microphysical aging significantly reduces global BC burden and lifetime, showing important implications for the estimate of BC radiative effects.
Yingying Yan, Jintai Lin, Jinxuan Chen, and Lu Hu
Atmos. Chem. Phys., 16, 2381–2400, https://doi.org/10.5194/acp-16-2381-2016, https://doi.org/10.5194/acp-16-2381-2016, 2016
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We use a newly built two-way coupling system of the GEOS-Chem CTM to simulate the global tropospheric O3 in 2009. It significantly improves the simulation upon the global model by comparisons with a suite of ground, aircraft, and satellite measurements, also reduces the global OH by 5 % with enhancements by 5 % in the lifetimes of MCF and methane. Therefore, improving model representations of small-scale processes is a critical step forward to understanding the global tropospheric chemistry.
C. He, K.-N. Liou, Y. Takano, R. Zhang, M. Levy Zamora, P. Yang, Q. Li, and L. R. Leung
Atmos. Chem. Phys., 15, 11967–11980, https://doi.org/10.5194/acp-15-11967-2015, https://doi.org/10.5194/acp-15-11967-2015, 2015
J.-T. Lin, M.-Y. Liu, J.-Y. Xin, K. F. Boersma, R. Spurr, R. Martin, and Q. Zhang
Atmos. Chem. Phys., 15, 11217–11241, https://doi.org/10.5194/acp-15-11217-2015, https://doi.org/10.5194/acp-15-11217-2015, 2015
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We conduct an improved OMI-based retrieval of tropospheric NO2 VCDs (POMINO) over China by explicitly accounting for aerosol optical effects and surface reflectance anisotropy. Compared to the traditional implicit aerosol treatment, an explicit treatment greatly lowers NO2 VCDs and subsequently estimated NOx emissions over eastern China, but with large spatiotemporal dependence. An explicit treatment also better captures high-pollution days. Effects of surface reflectance treatments are smaller.
Y. H. Mao, Q. B. Li, D. K. Henze, Z. Jiang, D. B. A. Jones, M. Kopacz, C. He, L. Qi, M. Gao, W.-M. Hao, and K.-N. Liou
Atmos. Chem. Phys., 15, 7685–7702, https://doi.org/10.5194/acp-15-7685-2015, https://doi.org/10.5194/acp-15-7685-2015, 2015
Z. Jiang, J. R. Worden, D. B. A. Jones, J.-T. Lin, W. W. Verstraeten, and D. K. Henze
Atmos. Chem. Phys., 15, 99–112, https://doi.org/10.5194/acp-15-99-2015, https://doi.org/10.5194/acp-15-99-2015, 2015
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We use satellite measurements of O3, CO and NO2 from TES, MOPITT and OMI to quantify O3 precursor emissions for 2006 and their impact on free tropospheric O3 over northeastern Asia. Using the adjoint of GEOS-Chem, we found that Chinese emissions have the largest influence on the free tropospheric O3. The contributions from lightning NOx in summer and India and southeastern Asia emissions in winter are sizable, comparable with Chinese emissions.
Y.-Y. Yan, J.-T. Lin, Y. Kuang, D. Yang, and L. Zhang
Atmos. Chem. Phys., 14, 12649–12663, https://doi.org/10.5194/acp-14-12649-2014, https://doi.org/10.5194/acp-14-12649-2014, 2014
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Limited by coarse resolutions, global chemical transport models cannot well capture small-scale nonlinear processes. To alleviate the problem, we develop a two-way coupled system to integrate the global GEOS-Chem model and its three high-resolution nested models covering Asia, Europe and North America. Confirmed by comparisons with observations, the coupled system improves upon the global model with a 10% increase in global tropospheric CO, a 4% decrease in OH and a 4% increase in MCF lifetime.
C. He, Q. B. Li, K. N. Liou, J. Zhang, L. Qi, Y. Mao, M. Gao, Z. Lu, D. G. Streets, Q. Zhang, M. M. Sarin, and K. Ram
Atmos. Chem. Phys., 14, 7091–7112, https://doi.org/10.5194/acp-14-7091-2014, https://doi.org/10.5194/acp-14-7091-2014, 2014
J.-T. Lin, R. V. Martin, K. F. Boersma, M. Sneep, P. Stammes, R. Spurr, P. Wang, M. Van Roozendael, K. Clémer, and H. Irie
Atmos. Chem. Phys., 14, 1441–1461, https://doi.org/10.5194/acp-14-1441-2014, https://doi.org/10.5194/acp-14-1441-2014, 2014
J.-T. Lin, Z. Liu, Q. Zhang, H. Liu, J. Mao, and G. Zhuang
Atmos. Chem. Phys., 12, 12255–12275, https://doi.org/10.5194/acp-12-12255-2012, https://doi.org/10.5194/acp-12-12255-2012, 2012
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
A renewed rise in global HCFC-141b emissions between 2017–2021
A model for simultaneous evaluation of NO2, O3, and PM10 pollution in urban and rural areas: handling incomplete data sets with multivariate curve resolution analysis
Technical note: Entrainment-limited kinetics of bimolecular reactions in clouds
Improving NOx emission estimates in Beijing using network observations and a perturbed emissions ensemble
Observation-based analysis of ozone production sensitivity for two persistent ozone episodes in Guangdong, China
A machine learning approach to quantify meteorological drivers of ozone pollution in China from 2015 to 2019
Discrepancy in assimilated atmospheric CO over East Asia in 2015–2020 by assimilating satellite and surface CO measurements
Potential environmental impact of bromoform from Asparagopsis farming in Australia
Satellite soil moisture data assimilation impacts on modeling weather variables and ozone in the southeastern US – Part 2: Sensitivity to dry-deposition parameterizations
The impacts of marine-emitted halogens on OH radicals in East Asia during summer
Impact of eastern and central Pacific El Niño on lower tropospheric ozone in China
Contribution of Asian emissions to upper tropospheric CO over the remote Pacific
Impact of a subtropical high and a typhoon on a severe ozone pollution episode in the Pearl River Delta, China
An ensemble-variational inversion system for the estimation of ammonia emissions using CrIS satellite ammonia retrievals
A process-oriented evaluation of CAMS reanalysis ozone during tropopause folds over Europe for the period 2003–2018
Estimation of mechanistic parameters in the gas-phase reactions of ozone with alkenes for use in automated mechanism construction
Projections of hydrofluorocarbon (HFC) emissions and the resulting global warming based on recent trends in observed abundances and current policies
Quantification of methane emissions from hotspots and during COVID-19 using a global atmospheric inversion
Model evaluation of short-lived climate forcers for the Arctic Monitoring and Assessment Programme: a multi-species, multi-model study
Global simulations of monoterpene-derived peroxy radical fates and the distributions of highly oxygenated organic molecules (HOMs) and accretion products
Impact of present and future aircraft NOx and aerosol emissions on atmospheric composition and associated direct radiative forcing of climate
Influence of photochemical loss of volatile organic compounds on understanding ozone formation mechanism
North China Plain as a hot spot of ozone pollution exacerbated by extreme high temperatures
Bayesian assessment of chlorofluorocarbon (CFC), hydrochlorofluorocarbon (HCFC) and halon banks suggest large reservoirs still present in old equipment
Photochemical evolution of the 2013 California Rim Fire: synergistic impacts of reactive hydrocarbons and enhanced oxidants
Impact of biomass burning and stratospheric intrusions in the remote South Pacific Ocean troposphere
Global and regional carbon budget 2015–2020 inferred from OCO-2 based on an ensemble Kalman filter coupled with GEOS-Chem
Influence of total ozone column (TOC) on the occurrence of tropospheric ozone depletion events (ODEs) in the Antarctic
Changes in anthropogenic precursor emissions drive shifts in the ozone seasonal cycle throughout the northern midlatitude troposphere
Amplified role of potential HONO sources in O3 formation in North China Plain during autumn haze aggravating processes
Continental-scale contributions to the global CFC-11 emission increase between 2012 and 2017
Surface ozone impacts on major crop production in China from 2010 to 2017
Enhanced summertime ozone and SOA from biogenic volatile organic compound (BVOC) emissions due to vegetation biomass variability during 1981–2018 in China
Pyruvic acid, an efficient catalyst in SO3 hydrolysis and effective clustering agent in sulfuric-acid-based new particle formation
Tropospheric ozone changes and ozone sensitivity from the present day to the future under shared socio-economic pathways
An integrated analysis of contemporary methane emissions and concentration trends over China using in situ and satellite observations and model simulations
An assessment of the tropospherically accessible photo-initiated ground state chemistry of organic carbonyls
Methane emissions in the United States, Canada, and Mexico: evaluation of national methane emission inventories and 2010–2017 sectoral trends by inverse analysis of in situ (GLOBALVIEWplus CH4 ObsPack) and satellite (GOSAT) atmospheric observations
Evaluation of SO2, SO42− and an updated SO2 dry deposition parameterization in the United Kingdom Earth System Model
Development and evaluation of a new compact mechanism for aromatic oxidation in atmospheric models
Ozone deposition impact assessments for forest canopies require accurate ozone flux partitioning on diurnal timescales
Unraveling pathways of elevated ozone induced by the 2020 lockdown in Europe by an observationally constrained regional model using TROPOMI
Model Output Statistics (MOS) applied to CAMS O3 forecasts: trade-offs between continuous and categorical skill scores
Cloud-scale modelling of the impact of deep convection on the fate of oceanic bromoform in the troposphere: a case study over the west coast of Borneo
Improving predictability of high-ozone episodes through dynamic boundary conditions, emission refresh and chemical data assimilation during the Long Island Sound Tropospheric Ozone Study (LISTOS) field campaign
Atmospheric observations consistent with reported decline in the UK's methane emissions (2013–2020)
Influence of atmospheric in-cloud aqueous-phase chemistry on the global simulation of SO2 in CESM2
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
Luke M. Western, Alison L. Redington, Alistair J. Manning, Cathy M. Trudinger, Lei Hu, Stephan Henne, Xuekun Fang, Lambert J. M. Kuijpers, Christina Theodoridi, David S. Godwin, Jgor Arduini, Bronwyn Dunse, Andreas Engel, Paul J. Fraser, Christina M. Harth, Paul B. Krummel, Michela Maione, Jens Mühle, Simon O'Doherty, Hyeri Park, Sunyoung Park, Stefan Reimann, Peter K. Salameh, Daniel Say, Roland Schmidt, Tanja Schuck, Carolina Siso, Kieran M. Stanley, Isaac Vimont, Martin K. Vollmer, Dickon Young, Ronald G. Prinn, Ray F. Weiss, Stephen A. Montzka, and Matthew Rigby
Atmos. Chem. Phys., 22, 9601–9616, https://doi.org/10.5194/acp-22-9601-2022, https://doi.org/10.5194/acp-22-9601-2022, 2022
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The production of ozone-destroying gases is being phased out. Even though production of one of the main ozone-depleting gases, called HCFC-141b, has been declining for many years, the amount that is being released to the atmosphere has been increasing since 2017. We do not know for sure why this is. A possible explanation is that HCFC-141b that was used to make insulating foams many years ago is only now escaping to the atmosphere, or a large part of its production is not being reported.
Eva Gorrochategui, Isabel Hernandez, and Romà Tauler
Atmos. Chem. Phys., 22, 9111–9127, https://doi.org/10.5194/acp-22-9111-2022, https://doi.org/10.5194/acp-22-9111-2022, 2022
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A multiway methodology is proposed to handle complex and incomplete atmospheric data sets, providing concise and easily interpretable results. Changes in air quality by NO2, O3 and PM10 in 8 sampling stations located in Catalonia during the COVID-19 lockdown with respect to previous years (2018 and 2019) are investigated. Simultaneous analysis of the 3 contaminants among the 8 stations and for the 3 years allows the evaluation of correlations among the pollutants, even when having missing data.
Christopher D. Holmes
Atmos. Chem. Phys., 22, 9011–9015, https://doi.org/10.5194/acp-22-9011-2022, https://doi.org/10.5194/acp-22-9011-2022, 2022
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Cloud water and ice enable reactions that lead to acid rain and alter atmospheric oxidants, among other impacts. This work develops and evaluates an efficient method of simulating cloud chemistry within global and regional atmospheric models in order to better understand the role of clouds in atmospheric chemistry.
Le Yuan, Olalekan A. M. Popoola, Christina Hood, David Carruthers, Roderic L. Jones, Haitong Zhe Sun, Huan Liu, Qiang Zhang, and Alexander T. Archibald
Atmos. Chem. Phys., 22, 8617–8637, https://doi.org/10.5194/acp-22-8617-2022, https://doi.org/10.5194/acp-22-8617-2022, 2022
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Emission estimates represent a major source of uncertainty in air quality modelling. We developed a novel approach to improve emission estimates from existing inventories using air quality models and routine in situ observations. Using this approach, we derived improved estimates of NOx emissions from the transport sector in Beijing in 2016. This approach has great potential in deriving timely updates of emissions for other pollutants, particularly in regions undergoing rapid emission changes.
Kaixiang Song, Run Liu, Yu Wang, Tao Liu, Liyan Wei, Yanxing Wu, Junyu Zheng, Boguang Wang, and Shaw Chen Liu
Atmos. Chem. Phys., 22, 8403–8416, https://doi.org/10.5194/acp-22-8403-2022, https://doi.org/10.5194/acp-22-8403-2022, 2022
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We developed an observation-based method to investigate the sensitivity of ozone formation to precursors during two elevated ozone episodes observed at 77 stations in Guangdong, China. We found approximately 67 % of the station days exhibit ozone formation sensitivity to NOx, 20 % of the station days are in the transitional regime sensitive to both NOx and volatile organic compounds (VOCs), and only 13 % of the station days are sensitive to VOCs.
Xiang Weng, Grant L. Forster, and Peer Nowack
Atmos. Chem. Phys., 22, 8385–8402, https://doi.org/10.5194/acp-22-8385-2022, https://doi.org/10.5194/acp-22-8385-2022, 2022
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We use machine learning to quantify the meteorological drivers behind surface ozone variations in China between 2015 and 2019. Our novel approaches show improved performance when compared to previous analysis methods. We highlight that nonlinearity in driver relationships and the impacts of large-scale meteorological phenomena are key to understanding ozone pollution. Moreover, we find that almost half of the observed ozone trend between 2015 and 2019 might have been driven by meteorology.
Zhaojun Tang, Jiaqi Chen, and Zhe Jiang
Atmos. Chem. Phys., 22, 7815–7826, https://doi.org/10.5194/acp-22-7815-2022, https://doi.org/10.5194/acp-22-7815-2022, 2022
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We provide a comparative analysis to explore the effects of satellite and surface measurements on atmospheric CO in data assimilations in 2015–2020 over East Asia. We find possible overestimated enhancements of atmospheric CO by assimilating surface CO measurements due to model representation errors, and a large discrepancy in the derived trends of CO columns due to different vertical sensitivities of satellite and surface observations to lower and free troposphere.
Yue Jia, Birgit Quack, Robert D. Kinley, Ignacio Pisso, and Susann Tegtmeier
Atmos. Chem. Phys., 22, 7631–7646, https://doi.org/10.5194/acp-22-7631-2022, https://doi.org/10.5194/acp-22-7631-2022, 2022
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In this study, we assessed the potential risks of bromoform released from Asparagopsis farming near Australia for the stratospheric ozone layer by analyzing different cultivation scenarios. We conclude that the intended operation of Asparagopsis seaweed cultivation farms with an annual yield to meet the needs of 50 % of feedlots and cattle in either open-ocean or terrestrial cultures in Australia will not impact the ozone layer under normal operating conditions.
Min Huang, James H. Crawford, Gregory R. Carmichael, Kevin W. Bowman, Sujay V. Kumar, and Colm Sweeney
Atmos. Chem. Phys., 22, 7461–7487, https://doi.org/10.5194/acp-22-7461-2022, https://doi.org/10.5194/acp-22-7461-2022, 2022
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This study demonstrates that ozone dry-deposition modeling can be improved by revising the model's dry-deposition parameterizations to better represent the effects of environmental conditions including the soil moisture fields. Applying satellite soil moisture data assimilation is shown to also have added value. Such advancements in coupled modeling and data assimilation can benefit the assessments of ozone impacts on human and vegetation health.
Shidong Fan and Ying Li
Atmos. Chem. Phys., 22, 7331–7351, https://doi.org/10.5194/acp-22-7331-2022, https://doi.org/10.5194/acp-22-7331-2022, 2022
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We investigated the mechanisms by which marine-emitted halogens influence the OH radical, which is not considered in air quality forecasting model systems. The atmospheric OH radical has a complicated response to halogen emissions by species through both physical and chemical processes. Over ocean, inorganic iodine is the controlling species and chemistry is more important. Over land, the physics of sea salt aerosols are more important. The mechanism is applicable to other circumstances.
Zhongjing Jiang and Jing Li
Atmos. Chem. Phys., 22, 7273–7285, https://doi.org/10.5194/acp-22-7273-2022, https://doi.org/10.5194/acp-22-7273-2022, 2022
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This study investigates the changes of tropospheric ozone in China associated with EP and CP El Niño, using satellite observations and the GEOS-Chem model. We found that El Niño generally leads to lower tropospheric ozone (LTO) decrease over most parts of China; La Niña acts the opposite. The difference between LTO changes during EP and CP El Niño primarily lies in southern China. Regional transport and chemical processes play the leading and secondary roles in driving the LTO changes.
Linda Smoydzin and Peter Hoor
Atmos. Chem. Phys., 22, 7193–7206, https://doi.org/10.5194/acp-22-7193-2022, https://doi.org/10.5194/acp-22-7193-2022, 2022
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Our study presents a detailed analysis of the spatial and temporal distribution of elevated CO level in the upper troposphere over the Pacific using 20 years of MOPITT data. We create a climatology of severe pollution episodes and use trajectory calculations to link each particular pollution event detected in MOPITT satellite data with a distinct source region. Additionally, we analyse uplift mechanisms such as WCB-related upward transport.
Shanshan Ouyang, Tao Deng, Run Liu, Jingyang Chen, Guowen He, Jeremy Cheuk-Hin Leung, Nan Wang, and Shaw Chen Liu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-290, https://doi.org/10.5194/acp-2022-290, 2022
Revised manuscript accepted for ACP
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A record-breaking severe O3 pollution episode occurred under the influence of a Pacific subtropical high followed by Typhoon Mina in the Pearl River Delta (PRD) in early Autumn 2019. Through the WRF-CMAQ model simulations, we propose that the enhanced photochemical production of O3 during the episode is a major cause of the most severe O3 pollution year since the official O3 observation started in PRD in 2006.
Michael Sitwell, Mark W. Shephard, Yves Rochon, Karen Cady-Pereira, and Enrico Dammers
Atmos. Chem. Phys., 22, 6595–6624, https://doi.org/10.5194/acp-22-6595-2022, https://doi.org/10.5194/acp-22-6595-2022, 2022
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Observations of ammonia made using the satellite-borne CrIS instrument were used to improve the ammonia emissions used in the GEM-MACH model. These observations were used to refine estimates of the monthly mean ammonia emissions over North America for May to August 2016. The updated ammonia emissions reduced biases of GEM-MACH surface ammonia fields with surface observations and showed some improvements in the forecasting of species involved in inorganic particulate matter formation.
Dimitris Akritidis, Andrea Pozzer, Johannes Flemming, Antje Inness, Philippe Nédélec, and Prodromos Zanis
Atmos. Chem. Phys., 22, 6275–6289, https://doi.org/10.5194/acp-22-6275-2022, https://doi.org/10.5194/acp-22-6275-2022, 2022
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We perform a process-oriented evaluation of Copernicus Atmosphere Monitoring Service (CAMS) reanalysis (CAMSRA) O3 over Europe using WOUDC (World Ozone and Ultraviolet Radiation Data Centre) ozonesondes and IAGOS (In-service Aircraft for a Global Observing System) aircraft measurements. Chemical data assimilation assists CAMSRA to reproduce the observed O3 increases in the troposphere during the examined folding events, but it mostly results in O3 overestimation in the upper troposphere.
Mike J. Newland, Camille Mouchel-Vallon, Richard Valorso, Bernard Aumont, Luc Vereecken, Michael E. Jenkin, and Andrew R. Rickard
Atmos. Chem. Phys., 22, 6167–6195, https://doi.org/10.5194/acp-22-6167-2022, https://doi.org/10.5194/acp-22-6167-2022, 2022
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Alkene ozonolysis produces Criegee intermediates, which can act as oxidants or decompose to give a range of closed-shell and radical products, including OH. Therefore it is essential to accurately represent the chemistry of Criegee intermediates in atmospheric models in order to understand their impacts on atmospheric composition. Here we provide a mechanism construction protocol by which the central features of alkene ozonolysis chemistry can be included in an automatic mechanism generator.
Guus J. M. Velders, John S. Daniel, Stephen A. Montzka, Isaac Vimont, Matthew Rigby, Paul B. Krummel, Jens Muhle, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 22, 6087–6101, https://doi.org/10.5194/acp-22-6087-2022, https://doi.org/10.5194/acp-22-6087-2022, 2022
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The emissions of hydrofluorocarbons (HFCs) have increased significantly in the past as a result of the phasing out of ozone-depleting substances. Observations indicate that HFCs are used much less in certain refrigeration applications than previously projected. Current policies are projected to reduce emissions and the surface temperature contribution of HFCs from 0.28–0.44 °C to 0.14–0.31 °C in 2100. The Kigali Amendment is projected to reduce the contributions further to 0.04 °C in 2100.
Joe McNorton, Nicolas Bousserez, Anna Agustí-Panareda, Gianpaolo Balsamo, Luca Cantarello, Richard Engelen, Vincent Huijnen, Antje Inness, Zak Kipling, Mark Parrington, and Roberto Ribas
Atmos. Chem. Phys., 22, 5961–5981, https://doi.org/10.5194/acp-22-5961-2022, https://doi.org/10.5194/acp-22-5961-2022, 2022
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Concentrations of atmospheric methane continue to grow, in recent years at an increasing rate, for unknown reasons. Using newly available satellite observations and a state-of-the-art weather prediction model we perform global estimates of emissions from hotspots at high resolution. Results show that the system can accurately report on biases in national inventories and is used to conclude that the early COVID-19 slowdown period (March–June 2020) had little impact on global methane emissions.
Cynthia H. Whaley, Rashed Mahmood, Knut von Salzen, Barbara Winter, Sabine Eckhardt, Stephen Arnold, Stephen Beagley, Silvia Becagli, Rong-You Chien, Jesper Christensen, Sujay Manish Damani, Xinyi Dong, Konstantinos Eleftheriadis, Nikolaos Evangeliou, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Fabio Giardi, Wanmin Gong, Jens Liengaard Hjorth, Lin Huang, Ulas Im, Yugo Kanaya, Srinath Krishnan, Zbigniew Klimont, Thomas Kühn, Joakim Langner, Kathy S. Law, Louis Marelle, Andreas Massling, Dirk Olivié, Tatsuo Onishi, Naga Oshima, Yiran Peng, David A. Plummer, Olga Popovicheva, Luca Pozzoli, Jean-Christophe Raut, Maria Sand, Laura N. Saunders, Julia Schmale, Sangeeta Sharma, Ragnhild Bieltvedt Skeie, Henrik Skov, Fumikazu Taketani, Manu A. Thomas, Rita Traversi, Kostas Tsigaridis, Svetlana Tsyro, Steven Turnock, Vito Vitale, Kaley A. Walker, Minqi Wang, Duncan Watson-Parris, and Tahya Weiss-Gibbons
Atmos. Chem. Phys., 22, 5775–5828, https://doi.org/10.5194/acp-22-5775-2022, https://doi.org/10.5194/acp-22-5775-2022, 2022
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Air pollutants, like ozone and soot, play a role in both global warming and air quality. Atmospheric models are often used to provide information to policy makers about current and future conditions under different emissions scenarios. In order to have confidence in those simulations, in this study we compare simulated air pollution from 18 state-of-the-art atmospheric models to measured air pollution in order to assess how well the models perform.
Ruochong Xu, Joel A. Thornton, Ben H. Lee, Yanxu Zhang, Lyatt Jaeglé, Felipe D. Lopez-Hilfiker, Pekka Rantala, and Tuukka Petäjä
Atmos. Chem. Phys., 22, 5477–5494, https://doi.org/10.5194/acp-22-5477-2022, https://doi.org/10.5194/acp-22-5477-2022, 2022
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Monoterpenes are emitted into the atmosphere by vegetation and by the use of certain consumer products. Reactions of monoterpenes in the atmosphere lead to low-volatility products that condense to grow particulate matter or participate in new particle formation and, thus, affect air quality and climate. We use a model of atmospheric chemistry and transport to evaluate the global-scale importance of recent updates to our understanding of monoterpene chemistry in particle formation and growth.
Etienne Terrenoire, Didier Hauglustaine, Yann Cohen, Anne Cozic, Richard Valorso, Franck Lefèvre, and Sigrun Matthes
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-222, https://doi.org/10.5194/acp-2022-222, 2022
Revised manuscript accepted for ACP
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Aviation NOx emissions have not only an impact on global climate by changing ozone and methane levels in the atmosphere but also contribute to deteriorate local air quality. The LMDZ-INCA global model is applied to reevaluate the impact of aircraft NOx and aerosol emissions on climate. We investigate the impact of present-day and future (2050) aircraft emissions on atmospheric composition and the associated radiative forcings of climate of ozone, methane and the aerosol direct forcings.
Wei Ma, Zemin Feng, Junlei Zhan, Yongchun Liu, Pengfei Liu, Chengtang Liu, Qingxin Ma, Kang Yang, Yafei Wang, Hong He, Markku Kulmala, Yujing Mu, and Junfeng Liu
Atmos. Chem. Phys., 22, 4841–4851, https://doi.org/10.5194/acp-22-4841-2022, https://doi.org/10.5194/acp-22-4841-2022, 2022
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The influence of photochemical loss of volatile organic compounds (VOCS) on O3 formation is investigated using an observation-based model. The sensitivity regime of ozone formation might be misdiagnosed due to the photochemical loss of VOCs in the atmosphere. The contribution of local photochemistry is underestimated regarding O3 pollution when one does not consider the photochemical loss of VOCs.
Pinya Wang, Yang Yang, Huimin Li, Lei Chen, Ruijun Dang, Daokai Xue, Baojie Li, Jianping Tang, L. Ruby Leung, and Hong Liao
Atmos. Chem. Phys., 22, 4705–4719, https://doi.org/10.5194/acp-22-4705-2022, https://doi.org/10.5194/acp-22-4705-2022, 2022
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China is now suffering from both severe ozone (O3) pollution and heat events. We highlight that North China Plain is the hot spot of the co-occurrences of extremes in O3 and high temperatures in China. Such coupled extremes exhibit an increasing trend during 2014–2019 and will continue to increase until the middle of this century. And the coupled extremes impose more severe health impacts to human than O3 pollution occurring alone because of elevated O3 levels and temperatures.
Megan Jeramaz Lickley, John S. Daniel, Eric L. Fleming, Stefan Reimann, and Susan Solomon
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-240, https://doi.org/10.5194/acp-2022-240, 2022
Revised manuscript accepted for ACP
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Halocarbons contained in equipment continue to be emitted after production has ceased. These ‘banks’ must be carefully accounted for in evaluating compliance with the Montreal Protocol. We extend a Bayesian model to the suite of regulated chemicals subject to banking. We find banks are substantially larger than previous estimates, and we identify banks by chemical and equipment type whose future emissions will contribute to global warming and delay ozone hole recovery if left unrecovered.
Glenn M. Wolfe, Thomas F. Hanisco, Heather L. Arkinson, Donald R. Blake, Armin Wisthaler, Tomas Mikoviny, Thomas B. Ryerson, Ilana Pollack, Jeff Peischl, Paul O. Wennberg, John D. Crounse, Jason M. St. Clair, Alex Teng, L. Gregory Huey, Xiaoxi Liu, Alan Fried, Petter Weibring, Dirk Richter, James Walega, Samuel R. Hall, Kirk Ullmann, Jose L. Jimenez, Pedro Campuzano-Jost, T. Paul Bui, Glenn Diskin, James R. Podolske, Glen Sachse, and Ronald C. Cohen
Atmos. Chem. Phys., 22, 4253–4275, https://doi.org/10.5194/acp-22-4253-2022, https://doi.org/10.5194/acp-22-4253-2022, 2022
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Smoke plumes are chemically complex. This work combines airborne observations of smoke plume composition with a photochemical model to probe the production of ozone and the fate of reactive gases in the outflow of a large wildfire. Model–measurement comparisons illustrate how uncertain emissions and chemical processes propagate into simulated chemical evolution. Results provide insight into how this system responds to perturbations, which can help guide future observation and modeling efforts.
Nikos Daskalakis, Laura Gallardo, Maria Kanakidou, Johann Rasmus Nüß, Camilo Menares, Roberto Rondanelli, Anne M. Thompson, and Mihalis Vrekoussis
Atmos. Chem. Phys., 22, 4075–4099, https://doi.org/10.5194/acp-22-4075-2022, https://doi.org/10.5194/acp-22-4075-2022, 2022
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Forest fires emit carbon monoxide (CO) that can be transported into the atmosphere far from the sources and reacts to produce ozone (O3) that affects climate, ecosystems and health. O3 is also produced in the stratosphere and can be transported downwards. Using a global numerical model, we found that forest fires can affect CO and O3 even in the South Pacific, the most pristine region of the global ocean, but transport from the stratosphere is a more important O3 source than fires in the region.
Yawen Kong, Bo Zheng, Qiang Zhang, and Kebin He
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-183, https://doi.org/10.5194/acp-2022-183, 2022
Revised manuscript accepted for ACP
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We developed a Bayesian atmospheric inversion system based on the 4D-LETKF algorithm coupled with GEOS-Chem, constrained by OCO-2 XCO2. This work represents the first time the 4D-LETKF algorithm was adapted to a global carbon inversion system that assimilated OCO-2 data. We inferred global gridded carbon fluxes from the latest OCO-2 V10r retrievals and investigated their magnitudes, variations, and partitioning schemes to understand the global and regional carbon budgets between 2015 and 2020.
Le Cao, Linjie Fan, Simeng Li, and Shuangyan Yang
Atmos. Chem. Phys., 22, 3875–3890, https://doi.org/10.5194/acp-22-3875-2022, https://doi.org/10.5194/acp-22-3875-2022, 2022
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We analyzed the observational data and used models to discover the impact of the total ozone column (TOC) on the occurrence of tropospheric ozone depletion events (ODE) in the Antarctic. The results suggest that the decrease of TOC favors the occurrence of ODE. When TOC varies the rates of major ODE accelerating reactions are substantially altered but the rates of major ODE decelerating reactions remain unchanged. As a result, the occurrence of ODE negatively depends on the TOC.
Henry Bowman, Steven Turnock, Susanne E. Bauer, Kostas Tsigaridis, Makoto Deushi, Naga Oshima, Fiona M. O'Connor, Larry Horowitz, Tongwen Wu, Jie Zhang, Dagmar Kubistin, and David D. Parrish
Atmos. Chem. Phys., 22, 3507–3524, https://doi.org/10.5194/acp-22-3507-2022, https://doi.org/10.5194/acp-22-3507-2022, 2022
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A full understanding of ozone in the troposphere requires investigation of its temporal variability over all timescales. Model simulations show that the northern midlatitude ozone seasonal cycle shifted with industrial development (1850–2014), with an increasing magnitude and a later summer peak. That shift reached a maximum in the mid-1980s, followed by a reversal toward the preindustrial cycle. The few available observations, beginning in the 1970s, are consistent with the model simulations.
Jingwei Zhang, Chaofan Lian, Weigang Wang, Maofa Ge, Yitian Guo, Haiyan Ran, Yusheng Zhang, Feixue Zheng, Xiaolong Fan, Chao Yan, Kaspar R. Daellenbach, Yongchun Liu, Markku Kulmala, and Junling An
Atmos. Chem. Phys., 22, 3275–3302, https://doi.org/10.5194/acp-22-3275-2022, https://doi.org/10.5194/acp-22-3275-2022, 2022
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This study added six potential HONO sources to the WRF-Chem model, evaluated their impact on HONO and O3 concentrations, including surface and vertical concentrations. The simulations extend our knowledge on atmospheric HONO sources, especially for nitrate photolysis. The study also explains the HONO difference in O3 formation on clean and hazy days, and reveals key potential HONO sources to O3 enhancements in haze-aggravating processes with a co-occurrence of high PM2.5 and O3 concentrations.
Lei Hu, Stephen A. Montzka, Fred Moore, Eric Hintsa, Geoff Dutton, M. Carolina Siso, Kirk Thoning, Robert W. Portmann, Kathryn McKain, Colm Sweeney, Isaac Vimont, David Nance, Bradley Hall, and Steven Wofsy
Atmos. Chem. Phys., 22, 2891–2907, https://doi.org/10.5194/acp-22-2891-2022, https://doi.org/10.5194/acp-22-2891-2022, 2022
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The unexpected increase in CFC-11 emissions between 2012 and 2017 resulted in concerns about delaying the stratospheric ozone recovery. Although the subsequent decline of CFC-11 emissions indicated a mitigation in part to this problem, the regions fully responsible for these large emission changes were unclear. Here, our new estimate, based on atmospheric measurements from two global campaigns and from NOAA, suggests Asia primarily contributed to the global CFC-11 emission rise during 2012–2017.
Dianyi Li, Drew Shindell, Dian Ding, Xiao Lu, Lin Zhang, and Yuqiang Zhang
Atmos. Chem. Phys., 22, 2625–2638, https://doi.org/10.5194/acp-22-2625-2022, https://doi.org/10.5194/acp-22-2625-2022, 2022
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In this study, we applied chemical transport model simulation with the latest annual anthropogenic emission inventory to study the long-term trend of ozone-induced crop production losses from 2010 to 2017 in China. We find that overall the ozone-induced crop production loss in China is significant and the annual average economic losses for wheat, rice, maize, and soybean in China are USD 9.55 billion, USD 8.53 billion, USD 2.23 billion, and USD 1.16 billion respectively, over the 8 years.
Jing Cao, Shuping Situ, Yufang Hao, Shaodong Xie, and Lingyu Li
Atmos. Chem. Phys., 22, 2351–2364, https://doi.org/10.5194/acp-22-2351-2022, https://doi.org/10.5194/acp-22-2351-2022, 2022
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Based on localized emission factors and high-resolution vegetation data, we simulated the impacts of BVOC emissions on O3 and SOA during 1981–2018 in China. The interannual variation of BVOC emissions caused by increasing leaf biomass resulted in O3 and SOA concentrations increasing at average annual rates of 0.11 ppb and 0.008 μg m−3, respectively. The results show different variations which can be attributed to the different changing trends of leaf biomass by region and vegetation type.
Narcisse Tsona Tchinda, Lin Du, Ling Liu, and Xiuhui Zhang
Atmos. Chem. Phys., 22, 1951–1963, https://doi.org/10.5194/acp-22-1951-2022, https://doi.org/10.5194/acp-22-1951-2022, 2022
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This study explores the effect of pyruvic acid (PA) both in the SO3 hydrolysis and in sulfuric-acid-based aerosol formation. Results show that in dry and polluted areas, PA-catalyzed SO3 hydrolysis is about 2 orders of magnitude more efficient at forming sulfuric acid than the water-catalyzed reaction. Moreover, PA can effectively enhance the ternary SA-PA-NH3 particle formation rate by up to 4.7×102 relative to the binary SA-NH3 particle formation rate at cold temperatures.
Zhenze Liu, Ruth M. Doherty, Oliver Wild, Fiona M. O'Connor, and Steven T. Turnock
Atmos. Chem. Phys., 22, 1209–1227, https://doi.org/10.5194/acp-22-1209-2022, https://doi.org/10.5194/acp-22-1209-2022, 2022
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Tropospheric ozone is important to future air quality and climate, and changing emissions and climate influence ozone. We investigate the evolution of ozone and ozone sensitivity from the present day (2004–2014) to the future (2045–2055) and explore the main drivers of ozone changes from global and regional perspectives. This helps guide suitable emission control strategies to mitigate ozone pollution.
Haiyue Tan, Lin Zhang, Xiao Lu, Yuanhong Zhao, Bo Yao, Robert J. Parker, and Hartmut Boesch
Atmos. Chem. Phys., 22, 1229–1249, https://doi.org/10.5194/acp-22-1229-2022, https://doi.org/10.5194/acp-22-1229-2022, 2022
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Methane is the second most important anthropogenic greenhouse gas. Understanding methane emissions and concentration growth over China in the past decade is important to support its mitigation. This study analyzes the contributions of methane emissions from different regions and sources over the globe to methane changes over China in 2007–2018. Our results show strong international transport influences and emphasize the need of intensive methane measurements covering eastern China.
Keiran N. Rowell, Scott H. Kable, and Meredith J. T. Jordan
Atmos. Chem. Phys., 22, 929–949, https://doi.org/10.5194/acp-22-929-2022, https://doi.org/10.5194/acp-22-929-2022, 2022
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Sunlight drives chemical reactions in the atmosphere by breaking chemical bonds. Motivated by the knowledge that if we can better understand the fundamental chemistry, we will be better able to predict atmospheric composition and model any future changes, we use quantum chemistry to investigate new classes of atmospheric reactions. We identify several potentially important reaction classes that will have implications for the atmospheric production of organic acids and molecular hydrogen.
Xiao Lu, Daniel J. Jacob, Haolin Wang, Joannes D. Maasakkers, Yuzhong Zhang, Tia R. Scarpelli, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Hannah Nesser, A. Anthony Bloom, Shuang Ma, John R. Worden, Shaojia Fan, Robert J. Parker, Hartmut Boesch, Ritesh Gautam, Deborah Gordon, Michael D. Moran, Frances Reuland, Claudia A. Octaviano Villasana, and Arlyn Andrews
Atmos. Chem. Phys., 22, 395–418, https://doi.org/10.5194/acp-22-395-2022, https://doi.org/10.5194/acp-22-395-2022, 2022
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We evaluate methane emissions and trends for 2010–2017 in the gridded national emission inventories for the United States, Canada, and Mexico by inversion of in situ and satellite methane observations. We find that anthropogenic methane emissions for all three countries are underestimated in the national inventories, largely driven by oil emissions. Anthropogenic methane emissions in the US peak in 2014, in contrast to the report of a steadily decreasing trend over 2010–2017 from the US EPA.
Catherine Hardacre, Jane P. Mulcahy, Richard J. Pope, Colin G. Jones, Steven T. Rumbold, Can Li, Colin Johnson, and Steven T. Turnock
Atmos. Chem. Phys., 21, 18465–18497, https://doi.org/10.5194/acp-21-18465-2021, https://doi.org/10.5194/acp-21-18465-2021, 2021
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We investigate UKESM1's ability to represent the sulfur (S) cycle in the recent historical period. The S cycle is a key driver of historical radiative forcing. Earth system models such as UKESM1 should represent the S cycle well so that we can have confidence in their projections of future climate. We compare UKESM1 to observations of sulfur compounds, finding that the model generally performs well. We also identify areas for UKESM1’s development, focussing on how SO2 is removed from the air.
Kelvin H. Bates, Daniel J. Jacob, Ke Li, Peter D. Ivatt, Mat J. Evans, Yingying Yan, and Jintai Lin
Atmos. Chem. Phys., 21, 18351–18374, https://doi.org/10.5194/acp-21-18351-2021, https://doi.org/10.5194/acp-21-18351-2021, 2021
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Simple aromatic compounds (benzene, toluene, xylene) have complex gas-phase chemistry that is inconsistently represented in atmospheric models. We compile recent experimental and theoretical insights to develop a new mechanism for gas-phase aromatic oxidation that is sufficiently compact for use in multiscale models. We compare our new mechanism to chamber experiments and other mechanisms, and implement it in a global model to quantify the impacts of aromatic oxidation on tropospheric chemistry.
Auke J. Visser, Laurens N. Ganzeveld, Ignacio Goded, Maarten C. Krol, Ivan Mammarella, Giovanni Manca, and K. Folkert Boersma
Atmos. Chem. Phys., 21, 18393–18411, https://doi.org/10.5194/acp-21-18393-2021, https://doi.org/10.5194/acp-21-18393-2021, 2021
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Dry deposition is an important sink for tropospheric ozone that affects ecosystem carbon uptake, but process understanding remains incomplete. We apply a common deposition representation in atmospheric chemistry models and a multi-layer canopy model to multi-year ozone deposition observations. The multi-layer canopy model performs better on diurnal timescales compared to the common approach, leading to a substantially improved simulation of ozone deposition and vegetation ozone impact metrics.
Amir H. Souri, Kelly Chance, Juseon Bak, Caroline R. Nowlan, Gonzalo González Abad, Yeonjin Jung, David C. Wong, Jingqiu Mao, and Xiong Liu
Atmos. Chem. Phys., 21, 18227–18245, https://doi.org/10.5194/acp-21-18227-2021, https://doi.org/10.5194/acp-21-18227-2021, 2021
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The global pandemic is believed to have an impact on emissions of air pollutants such as nitrogen dioxide (NO2) and formaldehyde (HCHO). This study quantifies the changes in the amount of NOx and VOC emissions via state-of-the-art inverse modeling technique using satellite observations during the lockdown 2020 with respect to a baseline over Europe, which in turn, it permits unraveling atmospheric processes being responsible for ozone formation in a less cloudy month.
Hervé Petetin, Dene Bowdalo, Pierre-Antoine Bretonnière, Marc Guevara, Oriol Jorba, Jan Mateu Armengol, Margarida Samso Cabre, Kim Serradell, Albert Soret, and Carlos Pérez Garcia-Pando
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-864, https://doi.org/10.5194/acp-2021-864, 2021
Revised manuscript accepted for ACP
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This study investigates to which extent ozone forecasts provided by the Copernicus Atmospheric Monitoring Service (CAMS) can be improved using surface observations and state-of-the-art statistical methods. Through a case study over the Iberian Peninsula in 2018–2019, it unambiguously demonstrates the value of these methods for improving the raw CAMS O3 forecasts, while highlighting at the same time the complexity of improving the detection of highest O3 concentrations.
Paul D. Hamer, Virginie Marécal, Ryan Hossaini, Michel Pirre, Gisèle Krysztofiak, Franziska Ziska, Andreas Engel, Stephan Sala, Timo Keber, Harald Bönisch, Elliot Atlas, Kirstin Krüger, Martyn Chipperfield, Valery Catoire, Azizan A. Samah, Marcel Dorf, Phang Siew Moi, Hans Schlager, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 16955–16984, https://doi.org/10.5194/acp-21-16955-2021, https://doi.org/10.5194/acp-21-16955-2021, 2021
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Bromoform is a stratospheric ozone-depleting gas released by seaweed and plankton transported to the stratosphere via convection in the tropics. We study the chemical interactions of bromoform and its derivatives within convective clouds using a cloud-scale model and observations. Our findings are that soluble bromine gases are efficiently washed out and removed within the convective clouds and that most bromine is transported vertically to the upper troposphere in the form of bromoform.
Siqi Ma, Daniel Tong, Lok Lamsal, Julian Wang, Xuelei Zhang, Youhua Tang, Rick Saylor, Tianfeng Chai, Pius Lee, Patrick Campbell, Barry Baker, Shobha Kondragunta, Laura Judd, Timothy A. Berkoff, Scott J. Janz, and Ivanka Stajner
Atmos. Chem. Phys., 21, 16531–16553, https://doi.org/10.5194/acp-21-16531-2021, https://doi.org/10.5194/acp-21-16531-2021, 2021
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Predicting high ozone gets more challenging as urban emissions decrease. How can different techniques be used to foretell the quality of air to better protect human health? We tested four techniques with the CMAQ model against observations during a field campaign over New York City. The new system proves to better predict the magnitude and timing of high ozone. These approaches can be extended to other regions to improve the predictability of high-O3 episodes in contemporary urban environments.
Mark F. Lunt, Alistair J. Manning, Grant Allen, Tim Arnold, Stéphane J.-B. Bauguitte, Hartmut Boesch, Anita L. Ganesan, Aoife Grant, Carole Helfter, Eiko Nemitz, Simon J. O'Doherty, Paul I. Palmer, Joseph R. Pitt, Chris Rennick, Daniel Say, Kieran M. Stanley, Ann R. Stavert, Dickon Young, and Matt Rigby
Atmos. Chem. Phys., 21, 16257–16276, https://doi.org/10.5194/acp-21-16257-2021, https://doi.org/10.5194/acp-21-16257-2021, 2021
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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 set-up on these findings are explored through a number of sensitivity studies.
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., 21, 16093–16120, https://doi.org/10.5194/acp-21-16093-2021, https://doi.org/10.5194/acp-21-16093-2021, 2021
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Compared with the observations, the results incorporating detailed cloud aqueous-phase chemistry greatly reduced SO2 overestimation. The biases in annual simulated SO2 concentrations (or mixing ratios) decreased by 46 %, 41 %, and 22 % in Europe, the USA, 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.
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.
Cited articles
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Short summary
Examining observed and simulated ozone at about 1000 sites during 1990–2014, we find a clear diurnal cycle both in the magnitude of ozone trends and in the relative importance of climate variability versus anthropogenic emissions to ozone changes, which has policy implications to mitigate ozone at night and other non-peak hours.
Examining observed and simulated ozone at about 1000 sites during 1990–2014, we find a clear...
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