Articles | Volume 21, issue 13
https://doi.org/10.5194/acp-21-10065-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-21-10065-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Quantitative assessment of changes in surface particulate matter concentrations and precursor emissions over China during the COVID-19 pandemic and their implications for Chinese economic activity
Air Resources Laboratory, National Oceanic and Atmospheric Administration, College Park, MD, USA
Cooperative Institute for Satellite Earth System Studies, University of Maryland, College Park, MD, USA
Soontae Kim
CORRESPONDING AUTHOR
Department of Environmental and Safety Engineering, Ajou University, Suwon, South Korea
Mark Cohen
Air Resources Laboratory, National Oceanic and Atmospheric Administration, College Park, MD, USA
Changhan Bae
National Air Emission Inventory and Research Center, Sejong, South Korea
Dasom Lee
School of Earth Sciences and Environmental Engineering, Gwangju Institute of Science and Technology, Gwangju, South Korea
now at: Division of Climate & Environmental Research,
Seoul Institute of Technology, Seoul, South Korea
Rick Saylor
Air Resources Laboratory, National Oceanic and Atmospheric Administration, College Park, MD, USA
Minah Bae
Department of Environmental and Safety Engineering, Ajou University, Suwon, South Korea
Eunhye Kim
Department of Environmental and Safety Engineering, Ajou University, Suwon, South Korea
Byeong-Uk Kim
Georgia Environmental Protection Division, Atlanta, GA, USA
Jin-Ho Yoon
School of Earth Sciences and Environmental Engineering, Gwangju Institute of Science and Technology, Gwangju, South Korea
Ariel Stein
Air Resources Laboratory, National Oceanic and Atmospheric Administration, College Park, MD, USA
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Hyun Cheol Kim, Tianfeng Chai, Ariel Stein, and Shobha Kondragunta
Atmos. Chem. Phys., 20, 10259–10277, https://doi.org/10.5194/acp-20-10259-2020, https://doi.org/10.5194/acp-20-10259-2020, 2020
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Smoke forecasts have been challenged by high uncertainty in fire emission estimates. We develop an inverse modeling system, the HYSPLIT-based Emissions Inverse Modeling System for wildfires, that estimates wildfire emissions from the transport and dispersion of smoke plumes as measured by satellite observations. Using NOAA HYSPLIT and GOES Aerosol/Smoke Product (GASP), the system resolves smoke source strength as a function of time and vertical level and outperforms current operational system.
Li Pan, HyunCheol Kim, Pius Lee, Rick Saylor, YouHua Tang, Daniel Tong, Barry Baker, Shobha Kondragunta, Chuanyu Xu, Mark G. Ruminski, Weiwei Chen, Jeff Mcqueen, and Ivanka Stajner
Geosci. Model Dev., 13, 2169–2184, https://doi.org/10.5194/gmd-13-2169-2020, https://doi.org/10.5194/gmd-13-2169-2020, 2020
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Compared to anthropogenic emissions, emissions from wildfires are largely uncontrolled and unpredictable. Quantitatively describing wildfire emissions and their contributions to air pollution remains a substantial challenge for air quality forecasting efforts. In this study, we test the wildfire calculation algorithm used by the National Air Quality Forecasting Capability (NAQFC) by comparison with ground, satellite and flight measurements during the Southeast Nexus (SENEX) field experiment.
Youhua Tang, Mariusz Pagowski, Tianfeng Chai, Li Pan, Pius Lee, Barry Baker, Rajesh Kumar, Luca Delle Monache, Daniel Tong, and Hyun-Cheol Kim
Geosci. Model Dev., 10, 4743–4758, https://doi.org/10.5194/gmd-10-4743-2017, https://doi.org/10.5194/gmd-10-4743-2017, 2017
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In order to evaluate the data assimilation tools for regional real-time PM2.5 forecasts, we applied a 3D-Var assimilation tool to adjust the aerosol initial condition by assimilating satellite-retrieved aerosol optical depth and surface PM2.5 observations for a regional air quality model, which is compared to another assimilation method, optimal interpolation. We discuss the pros and cons of these two assimilation methods based on the comparison of their 1-month four-cycles-per-day runs.
Li Pan, Hyun Cheol Kim, Pius Lee, Rick Saylor, YouHua Tang, Daniel Tong, Barry Baker, Shobha Kondragunta, Chuanyu Xu, Mark G. Ruminski, Weiwei Chen, Jeff Mcqueen, and Ivanka Stajner
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2017-207, https://doi.org/10.5194/gmd-2017-207, 2017
Revised manuscript not accepted
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In this study, a system accounting for fire emissions in a chemical transport model is described. The focus of this work is to qualitatively evaluate the system's capability to capture fire signals identified by multiple observation data sets. We discuss how to use observational data correctly to filter out fire signals and synergistic use of multiple data sets together. We also address the limitations of each of the observation data sets and of the evaluation methods.
Hyun Cheol Kim, Eunhye Kim, Changhan Bae, Jeong Hoon Cho, Byeong-Uk Kim, and Soontae Kim
Atmos. Chem. Phys., 17, 10315–10332, https://doi.org/10.5194/acp-17-10315-2017, https://doi.org/10.5194/acp-17-10315-2017, 2017
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This study is intended to provide reference information regarding quantitative estimation of regional contributions and model uncertainty in meteorology simulations and emissions inventories. Simulated PM concentration is sensitive to meteorology, but estimated contributions are mostly robust. Regional contributions are also found to be sensitive to the choice of emissions inventories. The modeled results should be considered with caution when interpreted for emission regulation policy making.
Hyun Cheol Kim, Soontae Kim, Seok-Woo Son, Pius Lee, Chun-Sil Jin, Eunhye Kim, Byeong-Uk Kim, Fong Ngan, Changhan Bae, Chang-Keun Song, and Ariel Stein
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2016-673, https://doi.org/10.5194/acp-2016-673, 2016
Revised manuscript not accepted
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In recent years, frequent occurrence of severe haze events in East Asia is one of the most serious public concerns in this region. We demonstrate that daily pollutant transport patterns in East Asia are visible from satellite images when inspected with corresponding synoptic weather analyses. Our manuscript focuses on the possible role of meteorology, especially by the routine passages of synoptic systems, on the production and removal of regional pollution in East Asia.
Hyun Cheol Kim, Pius Lee, Laura Judd, Li Pan, and Barry Lefer
Geosci. Model Dev., 9, 1111–1123, https://doi.org/10.5194/gmd-9-1111-2016, https://doi.org/10.5194/gmd-9-1111-2016, 2016
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Fair comparison between satellite- and modeled urban NO2 column densities is important in emission inventory evaluation and regulation policy making. This study focuses on the impact of satellite footprint resolution geometry. Since OMI NO2 pixels are too coarse to resolve fine-scale urban plumes, it may cause 20–30 % bias over major cities. We introduce approaches to adjust spatial and vertical structure (downscaling & averaging kernel), and demonstrate improved agreement between sat. and model.
Xiangshang Li, Yunsoo Choi, Beata Czader, Anirban Roy, Hyuncheol Kim, Barry Lefer, and Shuai Pan
Atmos. Chem. Phys., 16, 3127–3144, https://doi.org/10.5194/acp-16-3127-2016, https://doi.org/10.5194/acp-16-3127-2016, 2016
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We performed a a month-long sensitivity study of obs-nudging on meteorology and ozone chemistry. Notable increases in temperature and wind performance were observed after obs-nudging with hourly nudging files. PBL height also matched better in the sensitivity case. The model ozone improved at ground level and aloft but to a lesser degree. An examination of a high ozone episode showed that the current nudging process does not perform consistently – quite well at times while poor at other times.
H. C. Kim, P. Lee, F. Ngan, Y. Tang, H. L. Yoo, and L. Pan
Geosci. Model Dev., 8, 2959–2965, https://doi.org/10.5194/gmd-8-2959-2015, https://doi.org/10.5194/gmd-8-2959-2015, 2015
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This study focuses on the evaluation of regional air quality model's performance based on the cloud information from satellites. While cloud information is crucial in photochemistry model, the definitions of cloud fraction from model and satellite are not physically consistent. We demonstrate that improper modeling of cloud fraction is correlated with surface ozone bias, and we also show that current model cloud field might be too bright, causing an overestimation of surface ozone level.
T. Chai, H.-C. Kim, P. Lee, D. Tong, L. Pan, Y. Tang, J. Huang, J. McQueen, M. Tsidulko, and I. Stajner
Geosci. Model Dev., 6, 1831–1850, https://doi.org/10.5194/gmd-6-1831-2013, https://doi.org/10.5194/gmd-6-1831-2013, 2013
Tianfeng Chai, Xinrong Ren, Fong Ngan, Mark Cohen, and Alice Crawford
EGUsphere, https://doi.org/10.5194/egusphere-2023-329, https://doi.org/10.5194/egusphere-2023-329, 2023
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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An ensemble of HYSPLIT dispersion simulations are carried out with 15 different heat release parameters in plume rise calculation. The SO2 emissions of the three power plant are estimated by minimizing a cost function which measures the difference between logarithmic predicted and observed mixing ratios. The emission estimates based on the highest correlation coefficient or the lowest RMSE between the predicted and observed mixing ratios are presented and they agree well with the CEMS data.
Yunyao Li, Daniel Tong, Siqi Ma, Saulo R. Freitas, Ravan Ahmadov, Mikhail Sofiev, Xiaoyang Zhang, Shobha Kondragunta, Ralph Kahn, Youhua Tang, Barry Baker, Patrick Campbell, Rick Saylor, Georg Grell, and Fangjun Li
Atmos. Chem. Phys., 23, 3083–3101, https://doi.org/10.5194/acp-23-3083-2023, https://doi.org/10.5194/acp-23-3083-2023, 2023
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Plume height is important in wildfire smoke dispersion and affects air quality and human health. We assess the impact of plume height on wildfire smoke dispersion and the exceedances of the National Ambient Air Quality Standards. A higher plume height predicts lower pollution near the source region, but higher pollution in downwind regions, due to the faster spread of the smoke once ejected, affects pollution exceedance forecasts and the early warning of extreme air pollution events.
Yujin Jo, Myoseon Jang, Sanghee Han, Azad Madhu, Bonyoung Koo, Yiqin Jia, Zechen Yu, Soontae Kim, and Jinsoo Park
EGUsphere, https://doi.org/10.5194/egusphere-2023-93, https://doi.org/10.5194/egusphere-2023-93, 2023
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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The CAMx-UNIPAR model simulated the SOA budget formed via multiphase reactions of hydrocarbons and the impact of emissions and climate on SOA characteristics under California’s urban environments during winter 2018. SOA growth was dominated by daytime oxidation of long-chain alkanes and nighttime terpene oxidation with O3 and NO3 radicals. The spatial distributions of anthropogenic SOA were affected by the northwesterly wind whereas those of biogenic SOA were insensitive to wind directions.
Bok H. Baek, Carlie Coats, Siqi Ma, Chi-Tsan Wang, Jia Xing, Daniel Tong, Soontae Kim, and Jung-Hun Woo
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2022-253, https://doi.org/10.5194/gmd-2022-253, 2023
Preprint under review for GMD
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To enable the direct feedback effects of aerosols and local meteorology in an air quality modeling system without any computational bottleneck, we have developed an “inline” meteorology-induce emissions coupler module within the US EPA’s CMAQ modeling system, called “Meteorologically-induced anthropogenic Emissions: CMAQ-MetEmis”, to dynamically model the complex MOVES onroad mobile emissions inline without a separate dedicated emissions processing model like SMOKE.
Nadia Kathryn Colombi, Daniel J. Jacob, Laura Hyesung Yang, Shixian Zhai, Viral Shah, Stuart K. Grange, Robert M. Yantosca, Soontae Kim, and Hong Liao
EGUsphere, https://doi.org/10.5194/egusphere-2022-1366, https://doi.org/10.5194/egusphere-2022-1366, 2022
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Surface ozone, detrimental to human and ecosystem health, is very high and increasing in South Korea. Using a global model of the atmosphere, we found that emissions from South Korea and China contribute equally to the high ozone observed. We found that in the absence of all anthropogenic emissions over East Asia, ozone is still very high, implying that the air quality standard in South Korea is not practically achievable unless this background external to East Asia can be decreased.
Youhua Tang, Patrick C. Campbell, Pius Lee, Rick Saylor, Fanglin Yang, Barry Baker, Daniel Tong, Ariel Stein, Jianping Huang, Ho-Chun Huang, Li Pan, Jeff McQueen, Ivanka Stajner, Jose Tirado-Delgado, Youngsun Jung, Melissa Yang, Ilann Bourgeois, Jeff Peischl, Tom Ryerson, Donald Blake, Joshua Schwarz, Jose-Luis Jimenez, James Crawford, Glenn Diskin, Richard Moore, Johnathan Hair, Greg Huey, Andrew Rollins, Jack Dibb, and Xiaoyang Zhang
Geosci. Model Dev., 15, 7977–7999, https://doi.org/10.5194/gmd-15-7977-2022, https://doi.org/10.5194/gmd-15-7977-2022, 2022
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This paper compares two meteorological datasets for driving a regional air quality model: a regional meteorological model using WRF (WRF-CMAQ) and direct interpolation from an operational global model (GFS-CMAQ). In the comparison with surface measurements and aircraft data in summer 2019, these two methods show mixed performance depending on the corresponding meteorological settings. Direct interpolation is found to be a viable method to drive air quality models.
Zechen Yu, Myoseon Jang, Soontae Kim, Kyuwon Son, Sanghee Han, Azad Madhu, and Jinsoo Park
Atmos. Chem. Phys., 22, 9083–9098, https://doi.org/10.5194/acp-22-9083-2022, https://doi.org/10.5194/acp-22-9083-2022, 2022
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The UNIPAR model was incorporated into CAMx to predict the ambient concentration of organic matter in urban atmospheres during the KORUS-AQ campaign. CAMx–UNIPAR significantly improved the simulation of SOA formation under the wet aerosol condition through the consideration of aqueous reactions of reactive organic species and gas–aqueous partitioning into the wet inorganic aerosol.
Kai Zhang, Wentao Zhang, Hui Wan, Philip J. Rasch, Steven J. Ghan, Richard C. Easter, Xiangjun Shi, Yong Wang, Hailong Wang, Po-Lun Ma, Shixuan Zhang, Jian Sun, Susannah M. Burrows, Manish Shrivastava, Balwinder Singh, Yun Qian, Xiaohong Liu, Jean-Christophe Golaz, Qi Tang, Xue Zheng, Shaocheng Xie, Wuyin Lin, Yan Feng, Minghuai Wang, Jin-Ho Yoon, and L. Ruby Leung
Atmos. Chem. Phys., 22, 9129–9160, https://doi.org/10.5194/acp-22-9129-2022, https://doi.org/10.5194/acp-22-9129-2022, 2022
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Here we analyze the effective aerosol forcing simulated by E3SM version 1 using both century-long free-running and short nudged simulations. The aerosol forcing in E3SMv1 is relatively large compared to other models, mainly due to the large indirect aerosol effect. Aerosol-induced changes in liquid and ice cloud properties in E3SMv1 have a strong correlation. The aerosol forcing estimates in E3SMv1 are sensitive to the parameterization changes in both liquid and ice cloud processes.
Li Zhang, Raffaele Montuoro, Stuart A. McKeen, Barry Baker, Partha S. Bhattacharjee, Georg A. Grell, Judy Henderson, Li Pan, Gregory J. Frost, Jeff McQueen, Rick Saylor, Haiqin Li, Ravan Ahmadov, Jun Wang, Ivanka Stajner, Shobha Kondragunta, Xiaoyang Zhang, and Fangjun Li
Geosci. Model Dev., 15, 5337–5369, https://doi.org/10.5194/gmd-15-5337-2022, https://doi.org/10.5194/gmd-15-5337-2022, 2022
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The NOAA’s air quality predictions contribute to protecting lives and health in the US, which requires sustainable development and improvement of forecast systems. GEFS-Aerosols v1 has been developed in a collaboration between the NOAA research laboratories for operational forecast since September 2020 in the NCEP. The predictions demonstrate substantial improvements for both composition and variability of aerosol distributions over those from the former operational system.
Patrick C. Campbell, Youhua Tang, Pius Lee, Barry Baker, Daniel Tong, Rick Saylor, Ariel Stein, Jianping Huang, Ho-Chun Huang, Edward Strobach, Jeff McQueen, Li Pan, Ivanka Stajner, Jamese Sims, Jose Tirado-Delgado, Youngsun Jung, Fanglin Yang, Tanya L. Spero, and Robert C. Gilliam
Geosci. Model Dev., 15, 3281–3313, https://doi.org/10.5194/gmd-15-3281-2022, https://doi.org/10.5194/gmd-15-3281-2022, 2022
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NOAA's National Air Quality Forecast Capability (NAQFC) continues to protect Americans from the harmful effects of air pollution, while saving billions of dollars per year. Here we describe and evaluate the development of the most advanced version of the NAQFC to date, which became operational at NOAA on 20 July 2021. The new NAQFC is based on a coupling of NOAA's operational Global Forecast System (GFS) version 16 with the Community Multiscale Air Quality (CMAQ) model version 5.3.1.
Po-Lun Ma, Bryce E. Harrop, Vincent E. Larson, Richard B. Neale, Andrew Gettelman, Hugh Morrison, Hailong Wang, Kai Zhang, Stephen A. Klein, Mark D. Zelinka, Yuying Zhang, Yun Qian, Jin-Ho Yoon, Christopher R. Jones, Meng Huang, Sheng-Lun Tai, Balwinder Singh, Peter A. Bogenschutz, Xue Zheng, Wuyin Lin, Johannes Quaas, Hélène Chepfer, Michael A. Brunke, Xubin Zeng, Johannes Mülmenstädt, Samson Hagos, Zhibo Zhang, Hua Song, Xiaohong Liu, Michael S. Pritchard, Hui Wan, Jingyu Wang, Qi Tang, Peter M. Caldwell, Jiwen Fan, Larry K. Berg, Jerome D. Fast, Mark A. Taylor, Jean-Christophe Golaz, Shaocheng Xie, Philip J. Rasch, and L. Ruby Leung
Geosci. Model Dev., 15, 2881–2916, https://doi.org/10.5194/gmd-15-2881-2022, https://doi.org/10.5194/gmd-15-2881-2022, 2022
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An alternative set of parameters for E3SM Atmospheric Model version 1 has been developed based on a tuning strategy that focuses on clouds. When clouds in every regime are improved, other aspects of the model are also improved, even though they are not the direct targets for calibration. The recalibrated model shows a lower sensitivity to anthropogenic aerosols and surface warming, suggesting potential improvements to the simulated climate in the past and future.
Drew C. Pendergrass, Shixian Zhai, Jhoon Kim, Ja-Ho Koo, Seoyoung Lee, Minah Bae, Soontae Kim, Hong Liao, and Daniel J. Jacob
Atmos. Meas. Tech., 15, 1075–1091, https://doi.org/10.5194/amt-15-1075-2022, https://doi.org/10.5194/amt-15-1075-2022, 2022
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This paper uses a machine learning algorithm to infer high-resolution maps of particulate air quality in eastern China, Japan, and the Korean peninsula, using data from a geostationary satellite along with meteorology. We then perform an extensive evaluation of this inferred air quality and use it to diagnose trends in the region. We hope this paper and the associated data will be valuable to other scientists interested in epidemiology, air quality, remote sensing, and machine learning.
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.
Haipeng Lin, Daniel J. Jacob, Elizabeth W. Lundgren, Melissa P. Sulprizio, Christoph A. Keller, Thibaud M. Fritz, Sebastian D. Eastham, Louisa K. Emmons, Patrick C. Campbell, Barry Baker, Rick D. Saylor, and Raffaele Montuoro
Geosci. Model Dev., 14, 5487–5506, https://doi.org/10.5194/gmd-14-5487-2021, https://doi.org/10.5194/gmd-14-5487-2021, 2021
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Emissions are a central component of atmospheric chemistry models. The Harmonized Emissions Component (HEMCO) is a software component for computing emissions from a user-selected ensemble of emission inventories and algorithms. It allows users to select, add, and scale emissions from different sources through a configuration file with no change to the model source code. We demonstrate the implementation of HEMCO in several models, all sharing the same HEMCO core code and database library.
Hyun Cheol Kim, Tianfeng Chai, Ariel Stein, and Shobha Kondragunta
Atmos. Chem. Phys., 20, 10259–10277, https://doi.org/10.5194/acp-20-10259-2020, https://doi.org/10.5194/acp-20-10259-2020, 2020
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Smoke forecasts have been challenged by high uncertainty in fire emission estimates. We develop an inverse modeling system, the HYSPLIT-based Emissions Inverse Modeling System for wildfires, that estimates wildfire emissions from the transport and dispersion of smoke plumes as measured by satellite observations. Using NOAA HYSPLIT and GOES Aerosol/Smoke Product (GASP), the system resolves smoke source strength as a function of time and vertical level and outperforms current operational system.
Li Pan, HyunCheol Kim, Pius Lee, Rick Saylor, YouHua Tang, Daniel Tong, Barry Baker, Shobha Kondragunta, Chuanyu Xu, Mark G. Ruminski, Weiwei Chen, Jeff Mcqueen, and Ivanka Stajner
Geosci. Model Dev., 13, 2169–2184, https://doi.org/10.5194/gmd-13-2169-2020, https://doi.org/10.5194/gmd-13-2169-2020, 2020
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Compared to anthropogenic emissions, emissions from wildfires are largely uncontrolled and unpredictable. Quantitatively describing wildfire emissions and their contributions to air pollution remains a substantial challenge for air quality forecasting efforts. In this study, we test the wildfire calculation algorithm used by the National Air Quality Forecasting Capability (NAQFC) by comparison with ground, satellite and flight measurements during the Southeast Nexus (SENEX) field experiment.
Doug M. Smith, James A. Screen, Clara Deser, Judah Cohen, John C. Fyfe, Javier García-Serrano, Thomas Jung, Vladimir Kattsov, Daniela Matei, Rym Msadek, Yannick Peings, Michael Sigmond, Jinro Ukita, Jin-Ho Yoon, and Xiangdong Zhang
Geosci. Model Dev., 12, 1139–1164, https://doi.org/10.5194/gmd-12-1139-2019, https://doi.org/10.5194/gmd-12-1139-2019, 2019
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The Polar Amplification Model Intercomparison Project (PAMIP) is an endorsed contribution to the sixth Coupled Model Intercomparison Project (CMIP6). It will investigate the causes and global consequences of polar amplification through coordinated multi-model numerical experiments. This paper documents the experimental protocol.
Anna Karion, Thomas Lauvaux, Israel Lopez Coto, Colm Sweeney, Kimberly Mueller, Sharon Gourdji, Wayne Angevine, Zachary Barkley, Aijun Deng, Arlyn Andrews, Ariel Stein, and James Whetstone
Atmos. Chem. Phys., 19, 2561–2576, https://doi.org/10.5194/acp-19-2561-2019, https://doi.org/10.5194/acp-19-2561-2019, 2019
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In this study, we use atmospheric methane concentration observations collected during an airborne campaign to compare different model-based emissions estimates from the Barnett Shale oil and natural gas production basin in Texas, USA. We find that the tracer dispersion model has a significant impact on the results because the models differ in their simulation of vertical dispersion. Additional work is needed to evaluate and improve vertical mixing in the tracer dispersion models.
Tianfeng Chai, Ariel Stein, and Fong Ngan
Geosci. Model Dev., 11, 5135–5148, https://doi.org/10.5194/gmd-11-5135-2018, https://doi.org/10.5194/gmd-11-5135-2018, 2018
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While model predictions depend on release parameters, model uncertainties in inverse modeling should also vary with the source terms. In this paper, model uncertainties that will change with the source terms are introduced in a weak-constraint inverse modeling system. Tests using HYSPLIT model and CAPTEX observations show that adding such model uncertainty terms improves release rate estimates. A cost function normalization scheme introduced to avoid spurious solutions proves to be effective.
Ben Kravitz, Philip J. Rasch, Hailong Wang, Alan Robock, Corey Gabriel, Olivier Boucher, Jason N. S. Cole, Jim Haywood, Duoying Ji, Andy Jones, Andrew Lenton, John C. Moore, Helene Muri, Ulrike Niemeier, Steven Phipps, Hauke Schmidt, Shingo Watanabe, Shuting Yang, and Jin-Ho Yoon
Atmos. Chem. Phys., 18, 13097–13113, https://doi.org/10.5194/acp-18-13097-2018, https://doi.org/10.5194/acp-18-13097-2018, 2018
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Marine cloud brightening has been proposed as a means of geoengineering/climate intervention, or deliberately altering the climate system to offset anthropogenic climate change. In idealized simulations that highlight contrasts between land and ocean, we find that the globe warms, including the ocean due to transport of heat from land. This study reinforces that no net energy input into the Earth system does not mean that temperature will necessarily remain unchanged.
Kai Zhang, Philip J. Rasch, Mark A. Taylor, Hui Wan, Ruby Leung, Po-Lun Ma, Jean-Christophe Golaz, Jon Wolfe, Wuyin Lin, Balwinder Singh, Susannah Burrows, Jin-Ho Yoon, Hailong Wang, Yun Qian, Qi Tang, Peter Caldwell, and Shaocheng Xie
Geosci. Model Dev., 11, 1971–1988, https://doi.org/10.5194/gmd-11-1971-2018, https://doi.org/10.5194/gmd-11-1971-2018, 2018
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The conservation of total water is an important numerical feature for global Earth system models. Even small conservation problems in the water budget can lead to systematic errors in century-long simulations for sea level rise projection. This study quantifies and reduces various sources of water conservation error in the atmosphere component of the Energy Exascale Earth System Model.
Youhua Tang, Mariusz Pagowski, Tianfeng Chai, Li Pan, Pius Lee, Barry Baker, Rajesh Kumar, Luca Delle Monache, Daniel Tong, and Hyun-Cheol Kim
Geosci. Model Dev., 10, 4743–4758, https://doi.org/10.5194/gmd-10-4743-2017, https://doi.org/10.5194/gmd-10-4743-2017, 2017
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In order to evaluate the data assimilation tools for regional real-time PM2.5 forecasts, we applied a 3D-Var assimilation tool to adjust the aerosol initial condition by assimilating satellite-retrieved aerosol optical depth and surface PM2.5 observations for a regional air quality model, which is compared to another assimilation method, optimal interpolation. We discuss the pros and cons of these two assimilation methods based on the comparison of their 1-month four-cycles-per-day runs.
Li Pan, Hyun Cheol Kim, Pius Lee, Rick Saylor, YouHua Tang, Daniel Tong, Barry Baker, Shobha Kondragunta, Chuanyu Xu, Mark G. Ruminski, Weiwei Chen, Jeff Mcqueen, and Ivanka Stajner
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2017-207, https://doi.org/10.5194/gmd-2017-207, 2017
Revised manuscript not accepted
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In this study, a system accounting for fire emissions in a chemical transport model is described. The focus of this work is to qualitatively evaluate the system's capability to capture fire signals identified by multiple observation data sets. We discuss how to use observational data correctly to filter out fire signals and synergistic use of multiple data sets together. We also address the limitations of each of the observation data sets and of the evaluation methods.
Hyun Cheol Kim, Eunhye Kim, Changhan Bae, Jeong Hoon Cho, Byeong-Uk Kim, and Soontae Kim
Atmos. Chem. Phys., 17, 10315–10332, https://doi.org/10.5194/acp-17-10315-2017, https://doi.org/10.5194/acp-17-10315-2017, 2017
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This study is intended to provide reference information regarding quantitative estimation of regional contributions and model uncertainty in meteorology simulations and emissions inventories. Simulated PM concentration is sensitive to meteorology, but estimated contributions are mostly robust. Regional contributions are also found to be sensitive to the choice of emissions inventories. The modeled results should be considered with caution when interpreted for emission regulation policy making.
Tianfeng Chai, Alice Crawford, Barbara Stunder, Michael J. Pavolonis, Roland Draxler, and Ariel Stein
Atmos. Chem. Phys., 17, 2865–2879, https://doi.org/10.5194/acp-17-2865-2017, https://doi.org/10.5194/acp-17-2865-2017, 2017
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An inverse system based on the HYSPLIT dispersion model has been built to estimate volcanic ash source strengths, vertical distribution, and temporal variations. Using MODIS retrievals from the 2008 Kasatochi volcanic ash clouds, three options for matching model results to satellite mass loadings are tested. They all show decent skill. It is also found that simultaneously assimilating observations at different times produces better hindcasts than only assimilating the most recent observations.
Wonbae Jeon, Yunsoo Choi, Peter Percell, Amir Hossein Souri, Chang-Keun Song, Soon-Tae Kim, and Jhoon Kim
Geosci. Model Dev., 9, 3671–3684, https://doi.org/10.5194/gmd-9-3671-2016, https://doi.org/10.5194/gmd-9-3671-2016, 2016
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This study suggests a new hybrid Lagrangian–Eulerian modeling tool (the Screening Trajectory Ozone Prediction System, STOPS) for an accurate/fast prediction of Asian dust events. The STOPS is a moving nest (Lagrangian approach) between the source and the receptor inside Eulerian model. We run STOPS, instead of running a time-consuming Eulerian model, using constrained PM concentration from remote sensing aerosol optical depth, reflecting real-time dust particles. STOPS is for unexpected events.
Hyun Cheol Kim, Soontae Kim, Seok-Woo Son, Pius Lee, Chun-Sil Jin, Eunhye Kim, Byeong-Uk Kim, Fong Ngan, Changhan Bae, Chang-Keun Song, and Ariel Stein
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2016-673, https://doi.org/10.5194/acp-2016-673, 2016
Revised manuscript not accepted
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In recent years, frequent occurrence of severe haze events in East Asia is one of the most serious public concerns in this region. We demonstrate that daily pollutant transport patterns in East Asia are visible from satellite images when inspected with corresponding synoptic weather analyses. Our manuscript focuses on the possible role of meteorology, especially by the routine passages of synoptic systems, on the production and removal of regional pollution in East Asia.
Yong-Seok Seo, Seung-Pyo Jeong, Thomas M. Holsen, Young-Ji Han, Eunhwa Choi, Eun Ha Park, Tae Young Kim, Hee-Sang Eum, Dae Gun Park, Eunhye Kim, Soontae Kim, Jeong-Hun Kim, Jaewon Choi, and Seung-Muk Yi
Atmos. Chem. Phys., 16, 10215–10228, https://doi.org/10.5194/acp-16-10215-2016, https://doi.org/10.5194/acp-16-10215-2016, 2016
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This study was performed to identify likely source directions and locations of total gaseous mercury (TGM) using CPF, CBPF and TPSCF. Previous studies showed the importance of long-range transport of TGM but not local sources. However, the results from various approaches suggested the importance of local sources near industrial areas including iron and manufacturing facilities, hazardous waste incinerators and the coastal areas relative to distant sources.
Hyun Cheol Kim, Pius Lee, Laura Judd, Li Pan, and Barry Lefer
Geosci. Model Dev., 9, 1111–1123, https://doi.org/10.5194/gmd-9-1111-2016, https://doi.org/10.5194/gmd-9-1111-2016, 2016
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Fair comparison between satellite- and modeled urban NO2 column densities is important in emission inventory evaluation and regulation policy making. This study focuses on the impact of satellite footprint resolution geometry. Since OMI NO2 pixels are too coarse to resolve fine-scale urban plumes, it may cause 20–30 % bias over major cities. We introduce approaches to adjust spatial and vertical structure (downscaling & averaging kernel), and demonstrate improved agreement between sat. and model.
Xiangshang Li, Yunsoo Choi, Beata Czader, Anirban Roy, Hyuncheol Kim, Barry Lefer, and Shuai Pan
Atmos. Chem. Phys., 16, 3127–3144, https://doi.org/10.5194/acp-16-3127-2016, https://doi.org/10.5194/acp-16-3127-2016, 2016
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We performed a a month-long sensitivity study of obs-nudging on meteorology and ozone chemistry. Notable increases in temperature and wind performance were observed after obs-nudging with hourly nudging files. PBL height also matched better in the sensitivity case. The model ozone improved at ground level and aloft but to a lesser degree. An examination of a high ozone episode showed that the current nudging process does not perform consistently – quite well at times while poor at other times.
H. C. Kim, P. Lee, F. Ngan, Y. Tang, H. L. Yoo, and L. Pan
Geosci. Model Dev., 8, 2959–2965, https://doi.org/10.5194/gmd-8-2959-2015, https://doi.org/10.5194/gmd-8-2959-2015, 2015
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This study focuses on the evaluation of regional air quality model's performance based on the cloud information from satellites. While cloud information is crucial in photochemistry model, the definitions of cloud fraction from model and satellite are not physically consistent. We demonstrate that improper modeling of cloud fraction is correlated with surface ozone bias, and we also show that current model cloud field might be too bright, causing an overestimation of surface ozone level.
H. Lei, D. J. Wuebbles, X.-Z. Liang, Z. Tao, S. Olsen, R. Artz, X. Ren, and M. Cohen
Atmos. Chem. Phys., 14, 783–795, https://doi.org/10.5194/acp-14-783-2014, https://doi.org/10.5194/acp-14-783-2014, 2014
T. Chai, H.-C. Kim, P. Lee, D. Tong, L. Pan, Y. Tang, J. Huang, J. McQueen, M. Tsidulko, and I. Stajner
Geosci. Model Dev., 6, 1831–1850, https://doi.org/10.5194/gmd-6-1831-2013, https://doi.org/10.5194/gmd-6-1831-2013, 2013
R. D. Saylor
Atmos. Chem. Phys., 13, 693–715, https://doi.org/10.5194/acp-13-693-2013, https://doi.org/10.5194/acp-13-693-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Impacts of estimated plume rise on PM2.5 exceedance prediction during extreme wildfire events: a comparison of three schemes (Briggs, Freitas, and Sofiev)
Strong particle production and condensational growth in the upper troposphere sustained by biogenic VOCs from the canopy of the Amazon Basin
Sources of organic aerosols in eastern China: a modeling study with high-resolution intermediate-volatility and semivolatile organic compound emissions
Modelling the European wind-blown dust emissions and their impact on PM concentrations
Composited analyses of the chemical and physical characteristics of co-polluted days by ozone and PM2.5 over 2013–2020 in the Beijing–Tianjin–Hebei region
Observation-based constraints on modeled aerosol surface area: implications for heterogeneous chemistry
Analysis of new particle nucleation events and comparisons to simulations of particle number concentrations based on GEOS-Chem/APM in Beijing, China
Oligomer formation from the gas-phase reactions of Criegee intermediates with hydroperoxide esters: mechanism and kinetics
Modelling SO2 conversion into sulfates in the mid-troposphere with a 3D chemistry transport model: the case of Mount Etna's eruption on 12 April 2012
Simulation of organic aerosol, its precursors and related oxidants in the Landes pine forest in south-western France: Need to account for domain specific land-use and physical conditions
Global distribution of Asian, Middle Eastern, and North African dust simulated by CESM1/CARMA
Opinion: Coordinated development of emission inventories for climate forcers and air pollutants
Linking gas, particulate, and toxic endpoints to air emissions in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM) version 1.0
Contribution of regional aerosol nucleation to low-level CCN in an Amazonian deep convective environment: Results from a regionally nested global model
Seasonal modeling analysis of nitrate formation pathways in Yangtze River Delta region, China
Foreign emissions exacerbate PM2.5 pollution in China through nitrate chemistry
Modeling radiative and climatic effects of brown carbon aerosols with the ARPEGE-Climat global climate model
Numerical simulation of the impact of COVID-19 lockdown on tropospheric composition and aerosol radiative forcing in Europe
Evaluation of the WRF and CHIMERE models for the simulation of PM2.5 in large East African urban conurbations
Impact of urban heat island on inorganic aerosol in the lower free troposphere: a case study in Hangzhou, China
Statistical and machine learning methods for evaluating trends in air quality under changing meteorological conditions
Simulating the radiative forcing of oceanic dimethylsulfide (DMS) in Asia based on machine learning estimates
Quantifying the effects of mixing state on aerosol optical properties
Secondary organic aerosol formation via multiphase reaction of hydrocarbons in urban atmospheres using CAMx integrated with the UNIPAR model
Contrasting source contributions of Arctic black carbon to atmospheric concentrations, deposition flux, and atmospheric and snow radiative effects
Effect of dust on rainfall over the Red Sea coast based on WRF-Chem model simulations
A new assessment of global and regional budgets, fluxes, and lifetimes of atmospheric reactive N and S gases and aerosols
Limitations in representation of physical processes prevent successful simulation of PM2.5 during KORUS-AQ
Eurodelta multi-model simulated and observed particulate matter trends in Europe in the period of 1990–2010
Elucidating the critical oligomeric steps in secondary organic aerosol and brown carbon formation
Fast climate responses to emission reductions in aerosol and ozone precursors in China during 2013–2017
Secondary PM2.5 decreases significantly less than NO2 emission reductions during COVID lockdown in Germany
Modelling wintertime Arctic Haze and sea-spray aerosols
Molecular-level nucleation mechanism of iodic acid and methanesulfonic acid
Estimation of secondary PM2.5 in China and the United States using a multi-tracer approach
Two-way coupled meteorology and air quality models in Asia: a systematic review and meta-analysis of impacts of aerosol feedbacks on meteorology and air quality
OCEANFILMS (Organic Compounds from Ecosystems to Aerosols: Natural Films and Interfaces via Langmuir Molecular Surfactants) sea spray organic aerosol emissions – implementation in a global climate model and impacts on clouds
The pathway of impacts of aerosol direct effects on secondary inorganic aerosol formation
The impact of molecular self-organisation on the atmospheric fate of a cooking aerosol proxy
The formation and mitigation of nitrate pollution: comparison between urban and suburban environments
Impacts of aerosol–photolysis interaction and aerosol–radiation feedback on surface-layer ozone in North China during multi-pollutant air pollution episodes
Reducing future air-pollution-related premature mortality over Europe by mitigating emissions from the energy sector: assessing an 80 % renewable energies scenario
The impact of chlorine chemistry combined with heterogeneous N2O5 reactions on air quality in China
OH-initiated atmospheric degradation of hydroxyalkyl hydroperoxides: mechanism, kinetics, and structure–activity relationship
A predictive viscosity model for aqueous electrolytes and mixed organic–inorganic aerosol phases
The role of organic acids in new particle formation from methanesulfonic acid and methylamine
The number fraction of iron-containing particles affects OH, HO2 and H2O2 budgets in the atmospheric aqueous phase
Source-resolved variability of fine particulate matter and human exposure in an urban area
The impact of atmospheric blocking on the compounding effect of ozone pollution and temperature: a copula-based approach
Exploring dimethyl sulfide (DMS) oxidation and implications for global aerosol radiative forcing
Yunyao Li, Daniel Tong, Siqi Ma, Saulo R. Freitas, Ravan Ahmadov, Mikhail Sofiev, Xiaoyang Zhang, Shobha Kondragunta, Ralph Kahn, Youhua Tang, Barry Baker, Patrick Campbell, Rick Saylor, Georg Grell, and Fangjun Li
Atmos. Chem. Phys., 23, 3083–3101, https://doi.org/10.5194/acp-23-3083-2023, https://doi.org/10.5194/acp-23-3083-2023, 2023
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Plume height is important in wildfire smoke dispersion and affects air quality and human health. We assess the impact of plume height on wildfire smoke dispersion and the exceedances of the National Ambient Air Quality Standards. A higher plume height predicts lower pollution near the source region, but higher pollution in downwind regions, due to the faster spread of the smoke once ejected, affects pollution exceedance forecasts and the early warning of extreme air pollution events.
Yunfan Liu, Hang Su, Siwen Wang, Chao Wei, Wei Tao, Mira L. Pöhlker, Christopher Pöhlker, Bruna A. Holanda, Ovid O. Krüger, Thorsten Hoffmann, Manfred Wendisch, Paulo Artaxo, Ulrich Pöschl, Meinrat O. Andreae, and Yafang Cheng
Atmos. Chem. Phys., 23, 251–272, https://doi.org/10.5194/acp-23-251-2023, https://doi.org/10.5194/acp-23-251-2023, 2023
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The origins of the abundant cloud condensation nuclei (CCN) in the upper troposphere (UT) of the Amazon remain unclear. With model developments of new secondary organic aerosol schemes and constrained by observation, we show that strong aerosol nucleation and condensation in the UT is triggered by biogenic organics, and organic condensation is key for UT CCN production. This UT CCN-producing mechanism may prevail over broader vegetation canopies and deserves emphasis in aerosol–climate feedback.
Jingyu An, Cheng Huang, Dandan Huang, Momei Qin, Huan Liu, Rusha Yan, Liping Qiao, Min Zhou, Yingjie Li, Shuhui Zhu, Qian Wang, and Hongli Wang
Atmos. Chem. Phys., 23, 323–344, https://doi.org/10.5194/acp-23-323-2023, https://doi.org/10.5194/acp-23-323-2023, 2023
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This paper aims to build up an approach to establish a high-resolution emission inventory of intermediate-volatility and semi-volatile organic compounds in city-scale and detailed source categories and incorporate it into the CMAQ model. We believe this approach can be widely applied to improve the simulation of secondary organic aerosol and its source contributions.
Marina Liaskoni, Peter Huszar, Lukáš Bartík, Alvaro Patricio Prieto Perez, Jan Karlický, and Ondřej Vlček
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-804, https://doi.org/10.5194/acp-2022-804, 2023
Revised manuscript accepted for ACP
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Wind-blown dust (WBD) emissions emitted from European soils are estimated for the 2007–2016 period and their impact on the total particulate matter (PM) concentration is calculated. We found considerable increase of PM concentrations due to such emissions, especially during selected days (rather than in seasonal average). We also found that WBD emissions are strongest over western Europe and the highest impacts on PM are calculated for this region.
Huibin Dai, Hong Liao, Ke Li, Xu Yue, Yang Yang, Jia Zhu, Jianbing Jin, Baojie Li, and Xingwen Jiang
Atmos. Chem. Phys., 23, 23–39, https://doi.org/10.5194/acp-23-23-2023, https://doi.org/10.5194/acp-23-23-2023, 2023
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We apply the 3-D global chemical transport model (GEOS-Chem) to simulate co-polluted days by O3 and PM2.5 (O3–PM2.5PDs) in Beijing–Tianjin–Hebei in 2013–2020 and investigate the chemical and physical characteristics of O3–PM2.5PDs by composited analyses of such days that are captured by both the observations and the model. We report for the first time the unique features in vertical distributions of aerosols during O3–PM2.5PDs and the physical and chemical characteristics of O3–PM2.5PDs.
Rachel A. Bergin, Monica Harkey, Alicia Hoffman, Richard H. Moore, Bruce Anderson, Andreas Beyersdorf, Luke Ziemba, Lee Thornhill, Edward Winstead, Tracey Holloway, and Timothy H. Bertram
Atmos. Chem. Phys., 22, 15449–15468, https://doi.org/10.5194/acp-22-15449-2022, https://doi.org/10.5194/acp-22-15449-2022, 2022
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Correctly predicting aerosol surface area concentrations is important for determining the rate of heterogeneous reactions in chemical transport models. Here, we compare aircraft measurements of aerosol surface area with a regional model. In polluted air masses, we show that the model underpredicts aerosol surface area by a factor of 2. Despite this disagreement, the representation of heterogeneous chemistry still dominates the overall uncertainty in the loss rate of molecules such as N2O5.
Kun Wang, Xiaoyan Ma, Rong Tian, and Fangqun Yu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-797, https://doi.org/10.5194/acp-2022-797, 2022
Revised manuscript accepted for ACP
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During March 12th to April 6th, 2016 in Beijing, there were 11 typical new particle formation days, 13 non-event days and 2 undefined days. We first analyzed the favorable background of new particle formation in Beijing, and then obtained the quantitative meteorological and solar radiation conditions of new particle formation. In addition, we conducted the simulations using four nucleation schemes based on a global chemistry transport model (GEOS-Chem) to understand the nucleation mechanism.
Long Chen, Yu Huang, Yonggang Xue, Zhihui Jia, and Wenliang Wang
Atmos. Chem. Phys., 22, 14529–14546, https://doi.org/10.5194/acp-22-14529-2022, https://doi.org/10.5194/acp-22-14529-2022, 2022
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Quantum chemical methods are applied to gain insight into the oligomerization reaction mechanisms and kinetics of distinct stabilized Criegee intermediate (SCI) reactions with hydroperoxide esters, where calculations show that SCI addition reactions with hydroperoxide esters proceed through the successive insertion of SCIs to form oligomers that involve SCIs as the repeating unit. The saturated vapor pressure of the formed oligomers decreases monotonically with the increasing number of SCIs.
Mathieu Lachatre, Sylvain Mailler, Laurent Menut, Arineh Cholakian, Pasquale Sellitto, Guillaume Siour, Henda Guermazi, Giuseppe Salerno, and Salvatore Giammanco
Atmos. Chem. Phys., 22, 13861–13879, https://doi.org/10.5194/acp-22-13861-2022, https://doi.org/10.5194/acp-22-13861-2022, 2022
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In this study, we have evaluated the predominance of various pathways of volcanic SO2 conversion to sulfates in the upper troposphere. We show that the main conversion pathway was gaseous oxidation by OH, although the liquid pathways were expected to be predominant. These results are interesting with respect to a better understanding of sulfate formation in the middle and upper troposphere and are an important component to help evaluate particulate matter radiative forcing.
Arineh Cholakian, Matthias Beekmann, Guillaume Siour, Isabelle Coll, Manuela Cirtog, Elena Ormeno, Pierre-Marie Flaud, Emilie Perraudin, and Eric Villenave
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-697, https://doi.org/10.5194/acp-2022-697, 2022
Revised manuscript accepted for ACP
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This article revolves around the simulation of biogenic secondary organic aerosols in the Landes forest (south-west France). In order to do so, several sensitivity cases involving biogenic emission factors, landcover data, anthropogenic emissions and physical parameters were performed and each compared to measurements both in the forest canopy and around the forest. The chemistry behind the formation of these aerosols and their production and transport in the forest canopy are discussed.
Siying Lian, Luxi Zhou, Daniel M. Murphy, Karl D. Froyd, Owen B. Toon, and Pengfei Yu
Atmos. Chem. Phys., 22, 13659–13676, https://doi.org/10.5194/acp-22-13659-2022, https://doi.org/10.5194/acp-22-13659-2022, 2022
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Parameterizations of dust lifting and microphysical properties of dust in climate models are still subject to large uncertainty. Here we use a sectional aerosol climate model to investigate the global vertical distributions of the dust. Constrained by a suite of observations, the model suggests that, although North African dust dominates global dust mass loading at the surface, the relative contribution of Asian dust increases with altitude and becomes dominant in the upper troposphere.
Steven J. Smith, Erin E. McDuffie, and Molly Charles
Atmos. Chem. Phys., 22, 13201–13218, https://doi.org/10.5194/acp-22-13201-2022, https://doi.org/10.5194/acp-22-13201-2022, 2022
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Emissions into the atmosphere of greenhouse gases (GHGs) and air pollutants, quantified in emission inventories, impact human health, ecosystems, and the climate. We review how air pollutant and GHG inventory activities have historically been structured and their different uses and requirements. We discuss the benefits of increasing coordination between air pollutant and GHG inventory development efforts, but also caution that there are differences in appropriate methodologies and applications.
Havala O. T. Pye, Bryan K. Place, Benjamin N. Murphy, Karl M. Seltzer, Emma L. D'Ambro, Christine Allen, Ivan R. Piletic, Sara Farrell, Rebecca H. Schwantes, Matthew M. Coggon, Emily Saunders, Lu Xu, Golam Sarwar, William T. Hutzell, Kristen M. Foley, George Pouliot, Jesse Bash, and William R. Stockwell
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-695, https://doi.org/10.5194/acp-2022-695, 2022
Revised manuscript accepted for ACP
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Chemical mechanisms describe how emissions from vehicles, chemical products, vegetation, and other sources are chemically transformed in the atmosphere to secondary products. The Community Regional Atmospheric Chemistry Multiphase Mechanism is a new mechanism that integrates radical chemistry leading to gas-phase endpoints with pathways to fine particle mass. In addition, some hazardous air pollutants are explicitly included to enable calculation of health risks from specific chemicals.
Xuemei Wang, Hamish Gordon, Daniel P. Grosvenor, Meinrat O. Andreae, and Ken S. Carslaw
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-705, https://doi.org/10.5194/acp-2022-705, 2022
Revised manuscript accepted for ACP
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New particle formation in the upper troposphere is important for the global boundary layer aerosol population and they can be transported downward in Amazonia. We use a global and a regional model to quantify the number of aerosols that are formed at high altitude and transported downward in a 1000 km region. We find that the majority of the aerosols are from outside the region. This suggests that the 1000 km region is unlikely to be a ‘closed loop’ for aerosol formation, transport and growth.
Jinjin Sun, Momei Qin, Xiaodong Xie, Wenxing Fu, Yang Qin, Li Sheng, Lin Li, Jingyi Li, Ishaq Dimeji Sulaymon, Lei Jiang, Lin Huang, Xingna Yu, and Jianlin Hu
Atmos. Chem. Phys., 22, 12629–12646, https://doi.org/10.5194/acp-22-12629-2022, https://doi.org/10.5194/acp-22-12629-2022, 2022
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NO3- has become the dominant and the least reduced chemical component of fine particulate matter in China. NO3- formation is mostly in the NH3-rich regime in the Yangtze River Delta (YRD). OH + NO2 contributes 60 %–83 % of the TNO3 production rates, and the N2O5 heterogeneous pathway contributes 10 %–36 %. The N2O5 heterogeneous pathway becomes more important in cold seasons. Local emissions and regional transportation contribute 50 %–62 % and 38 %–50 % to YRD NO3- concentrations, respectively.
Jun-Wei Xu, Jintai Lin, Gan Luo, Jamiu Adeniran, and Hao Kong
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-646, https://doi.org/10.5194/acp-2022-646, 2022
Revised manuscript accepted for ACP
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Research on the sources of Chinese PM2.5 pollution has focused on the contributions of China’s domestic emissions. However, the impact of foreign anthropogenic emissions has typically been simplified or neglected. Here we find that foreign anthropogenic emissions play an important role in Chinese PM2.5 pollution through chemical interactions between transported pollutants and China’s local emissions. Thus, foreign emission reductions are essential for improving Chinese air quality.
Thomas Drugé, Pierre Nabat, Marc Mallet, Martine Michou, Samuel Rémy, and Oleg Dubovik
Atmos. Chem. Phys., 22, 12167–12205, https://doi.org/10.5194/acp-22-12167-2022, https://doi.org/10.5194/acp-22-12167-2022, 2022
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This study presents the implementation of brown carbon in the atmospheric component of the CNRM global climate model and particularly in its aerosol scheme TACTIC. Several simulations were carried out with this climate model, over the period 2000–2014, to evaluate the model by comparison with different reference datasets (PARASOL-GRASP, OMI-OMAERUVd, MACv2, FMI_SAT, AERONET) and to analyze the brown carbon radiative and climatic effects.
Simon F. Reifenberg, Anna Martin, Matthias Kohl, Sara Bacer, Zaneta Hamryszczak, Ivan Tadic, Lenard Röder, Daniel J. Crowley, Horst Fischer, Katharina Kaiser, Johannes Schneider, Raphael Dörich, John N. Crowley, Laura Tomsche, Andreas Marsing, Christiane Voigt, Andreas Zahn, Christopher Pöhlker, Bruna A. Holanda, Ovid Krüger, Ulrich Pöschl, Mira Pöhlker, Patrick Jöckel, Marcel Dorf, Ulrich Schumann, Jonathan Williams, Birger Bohn, Joachim Curtius, Hardwig Harder, Hans Schlager, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 22, 10901–10917, https://doi.org/10.5194/acp-22-10901-2022, https://doi.org/10.5194/acp-22-10901-2022, 2022
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In this work we use a combination of observational data from an aircraft campaign and model results to investigate the effect of the European lockdown due to COVID-19 in spring 2020. Using model results, we show that the largest relative changes to the atmospheric composition caused by the reduced emissions are located in the upper troposphere around aircraft cruise altitude, while the largest absolute changes are present at the surface.
Andrea Mazzeo, Michael Burrow, Andrew Quinn, Eloise A. Marais, Ajit Singh, David Ng'ang'a, Michael J. Gatari, and Francis D. Pope
Atmos. Chem. Phys., 22, 10677–10701, https://doi.org/10.5194/acp-22-10677-2022, https://doi.org/10.5194/acp-22-10677-2022, 2022
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A modelling system for meteorology and chemistry transport processes, WRF–CHIMERE, has been tested and validated for three East African conurbations using the most up-to-date anthropogenic emissions available. Results show that the model is able to reproduce hourly and daily temporal variabilities in aerosol concentrations that are close to observations in both urban and rural environments, encouraging the adoption of numerical modelling as a tool for air quality management in East Africa.
Hanqing Kang, Bin Zhu, Gerrit de Leeuw, Bu Yu, Ronald J. van der A, and Wen Lu
Atmos. Chem. Phys., 22, 10623–10634, https://doi.org/10.5194/acp-22-10623-2022, https://doi.org/10.5194/acp-22-10623-2022, 2022
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This study quantified the contribution of each urban-induced meteorological effect (temperature, humidity, and circulation) to aerosol concentration. We found that the urban heat island (UHI) circulation dominates the UHI effects on aerosol. The UHI circulation transports aerosol and its precursor gases from the warmer lower boundary layer to the colder lower free troposphere and promotes the secondary formation of ammonium nitrate aerosol in the cold atmosphere.
Minghao Qiu, Corwin Zigler, and Noelle E. Selin
Atmos. Chem. Phys., 22, 10551–10566, https://doi.org/10.5194/acp-22-10551-2022, https://doi.org/10.5194/acp-22-10551-2022, 2022
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Evaluating impacts of emission changes on air quality requires accounting for meteorological variability. Many studies use simple regression methods to correct for meteorology, but little is known about their performance. Using cases in the US and China, we show that widely used regression models do not perform well and can lead to biased estimates of emission-driven trends. We propose a novel machine learning method with lower bias and provide recommendations to policymakers and researchers.
Junri Zhao, Weichun Ma, Kelsey R. Bilsback, Jeffrey R. Pierce, Shengqian Zhou, Ying Chen, Guipeng Yang, and Yan Zhang
Atmos. Chem. Phys., 22, 9583–9600, https://doi.org/10.5194/acp-22-9583-2022, https://doi.org/10.5194/acp-22-9583-2022, 2022
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Marine dimethylsulfide (DMS) emissions play important roles in atmospheric sulfur cycle and climate effects. In this study, DMS emissions were estimated by using the machine learning method and drove the global 3D chemical transport model to simulate their climate effects. To our knowledge, this is the first study in the Asian region that quantifies the combined impacts of DMS on sulfate, particle number concentration, and radiative forcings.
Yu Yao, Jeffrey H. Curtis, Joseph Ching, Zhonghua Zheng, and Nicole Riemer
Atmos. Chem. Phys., 22, 9265–9282, https://doi.org/10.5194/acp-22-9265-2022, https://doi.org/10.5194/acp-22-9265-2022, 2022
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Investigating the impacts of aerosol mixing state on aerosol optical properties has a long history from both the modeling and experimental perspective. In this study, we used particle-resolved simulations as a benchmark to determine the error in optical properties when using simplified aerosol representations. We found that errors in single scattering albedo due to the internal mixture assumptions can have substantial effects on calculating aerosol direct radiative forcing.
Zechen Yu, Myoseon Jang, Soontae Kim, Kyuwon Son, Sanghee Han, Azad Madhu, and Jinsoo Park
Atmos. Chem. Phys., 22, 9083–9098, https://doi.org/10.5194/acp-22-9083-2022, https://doi.org/10.5194/acp-22-9083-2022, 2022
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The UNIPAR model was incorporated into CAMx to predict the ambient concentration of organic matter in urban atmospheres during the KORUS-AQ campaign. CAMx–UNIPAR significantly improved the simulation of SOA formation under the wet aerosol condition through the consideration of aqueous reactions of reactive organic species and gas–aqueous partitioning into the wet inorganic aerosol.
Hitoshi Matsui, Tatsuhiro Mori, Sho Ohata, Nobuhiro Moteki, Naga Oshima, Kumiko Goto-Azuma, Makoto Koike, and Yutaka Kondo
Atmos. Chem. Phys., 22, 8989–9009, https://doi.org/10.5194/acp-22-8989-2022, https://doi.org/10.5194/acp-22-8989-2022, 2022
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Using a global aerosol model, we find that the source contributions to radiative effects of black carbon (BC) in the Arctic are quite different from those to mass concentrations and deposition flux of BC in the Arctic. This is because microphysical properties (e.g., mixing state), altitudes, and seasonal variations of BC in the atmosphere differ among emissions sources. These differences need to be considered for accurate simulations of Arctic BC and its source contributions and climate impacts.
Sagar P. Parajuli, Georgiy L. Stenchikov, Alexander Ukhov, Suleiman Mostamandi, Paul A. Kucera, Duncan Axisa, William I. Gustafson Jr., and Yannian Zhu
Atmos. Chem. Phys., 22, 8659–8682, https://doi.org/10.5194/acp-22-8659-2022, https://doi.org/10.5194/acp-22-8659-2022, 2022
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Rainfall affects the distribution of surface- and groundwater resources, which are constantly declining over the Middle East and North Africa (MENA) due to overexploitation. Here, we explored the effects of dust on rainfall using WRF-Chem model simulations. Although dust is considered a nuisance from an air quality perspective, our results highlight the positive fundamental role of dust particles in modulating rainfall formation and distribution, which has implications for cloud seeding.
Yao Ge, Massimo Vieno, David S. Stevenson, Peter Wind, and Mathew R. Heal
Atmos. Chem. Phys., 22, 8343–8368, https://doi.org/10.5194/acp-22-8343-2022, https://doi.org/10.5194/acp-22-8343-2022, 2022
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Reactive N and S gases and aerosols are critical determinants of air quality. We report a comprehensive analysis of the concentrations, wet and dry deposition, fluxes, and lifetimes of these species globally as well as for 10 world regions. We used the EMEP MSC-W model coupled with WRF meteorology and 2015 global emissions. Our work demonstrates the substantial regional variation in these quantities and the need for modelling to simulate atmospheric responses to precursor emissions.
Katherine R. Travis, James H. Crawford, Gao Chen, Carolyn E. Jordan, Benjamin A. Nault, Hwajin Kim, Jose L. Jimenez, Pedro Campuzano-Jost, Jack E. Dibb, Jung-Hun Woo, Younha Kim, Shixian Zhai, Xuan Wang, Erin E. McDuffie, Gan Luo, Fangqun Yu, Saewung Kim, Isobel J. Simpson, Donald R. Blake, Limseok Chang, and Michelle J. Kim
Atmos. Chem. Phys., 22, 7933–7958, https://doi.org/10.5194/acp-22-7933-2022, https://doi.org/10.5194/acp-22-7933-2022, 2022
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The 2016 Korea–United States Air Quality (KORUS-AQ) field campaign provided a unique set of observations to improve our understanding of PM2.5 pollution in South Korea. Models typically have errors in simulating PM2.5 in this region, which is of concern for the development of control measures. We use KORUS-AQ observations to improve our understanding of the mechanisms driving PM2.5 and the implications of model errors for determining PM2.5 that is attributable to local or foreign sources.
Svetlana Tsyro, Wenche Aas, Augustin Colette, Camilla Andersson, Bertrand Bessagnet, Giancarlo Ciarelli, Florian Couvidat, Kees Cuvelier, Astrid Manders, Kathleen Mar, Mihaela Mircea, Noelia Otero, Maria-Teresa Pay, Valentin Raffort, Yelva Roustan, Mark R. Theobald, Marta G. Vivanco, Hilde Fagerli, Peter Wind, Gino Briganti, Andrea Cappelletti, Massimo D'Isidoro, and Mario Adani
Atmos. Chem. Phys., 22, 7207–7257, https://doi.org/10.5194/acp-22-7207-2022, https://doi.org/10.5194/acp-22-7207-2022, 2022
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Particulate matter (PM) air pollution causes adverse health effects. In Europe, the emissions caused by anthropogenic activities have been reduced in the last decades. To assess the efficiency of emission reductions in improving air quality, we have studied the evolution of PM pollution in Europe. Simulations with six air quality models and observational data indicate a decrease in PM concentrations by 10 % to 30 % across Europe from 2000 to 2010, which is mainly a result of emission reductions.
Yuemeng Ji, Qiuju Shi, Xiaohui Ma, Lei Gao, Jiaxin Wang, Yixin Li, Yanpeng Gao, Guiying Li, Renyi Zhang, and Taicheng An
Atmos. Chem. Phys., 22, 7259–7271, https://doi.org/10.5194/acp-22-7259-2022, https://doi.org/10.5194/acp-22-7259-2022, 2022
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The formation mechanisms of secondary organic aerosol and brown carbon from small α-carbonyls are still unclear. Thus, the mechanisms and kinetics of aqueous-phase reactions of glyoxal were investigated using quantum chemical and kinetic rate calculations. Several essential isomeric processes were identified, including protonation to yield diol/tetrol and carbenium ions as well as nucleophilic addition of carbenium ions to diol/tetrol and free methylamine/ammonia.
Jiyuan Gao, Yang Yang, Hailong Wang, Pinya Wang, Huimin Li, Mengyun Li, Lili Ren, Xu Yue, and Hong Liao
Atmos. Chem. Phys., 22, 7131–7142, https://doi.org/10.5194/acp-22-7131-2022, https://doi.org/10.5194/acp-22-7131-2022, 2022
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China has been implementing a sequence of policies for clean air since the year 2013. The aerosol decline produced a 0.09 ± 0.10°C warming during 2013–2017 estimated in this study, and the increase in ozone in the lower troposphere during this time period accelerated the warming, leading to a total 0.16 ± 0.15°C temperature increase in eastern China. Residential emission reductions led to a cooling effect because of a substantial decrease in light-absorbing aerosols.
Vigneshkumar Balamurugan, Jia Chen, Zhen Qu, Xiao Bi, and Frank N. Keutsch
Atmos. Chem. Phys., 22, 7105–7129, https://doi.org/10.5194/acp-22-7105-2022, https://doi.org/10.5194/acp-22-7105-2022, 2022
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In this study, we investigated the response of secondary pollutants to changes in precursor emissions, focusing on the formation of secondary PM, during the COVID-19 lockdown period. We show that, due to the decrease in primary NOx emissions, atmospheric oxidizing capacity is increased. The nighttime increase in ozone, caused by less NO titration, results in higher NO3 radicals, which contribute significantly to the formation of PM nitrates. O3 should be limited in order to control PM pollution.
Eleftherios Ioannidis, Kathy S. Law, Jean-Christophe Raut, Louis Marelle, Tatsuo Onishi, Rachel M. Kirpes, Lucia Upchurch, Andreas Massling, Henrik Skov, Patricia K. Quinn, and Kerri A. Pratt
EGUsphere, https://doi.org/10.5194/egusphere-2022-310, https://doi.org/10.5194/egusphere-2022-310, 2022
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Enhanced concentrations of aerosols influence the Arctic region during wintertime and winter-spring transition, transported from mid-latitude source regions. However, there are also local anthropogenic and natural (sea-spray aerosols – SSA) sources. SSA are a major contributor to PM1.0/PM10 at remote coastal sites during wintertime, however, models tend to miss essential mechanisms for SSA production and local sources of marine organics in the Arctic. This study addresses these uncertainties.
An Ning, Ling Liu, Lin Ji, and Xiuhui Zhang
Atmos. Chem. Phys., 22, 6103–6114, https://doi.org/10.5194/acp-22-6103-2022, https://doi.org/10.5194/acp-22-6103-2022, 2022
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Iodic acid (IA) and methanesulfonic acid (MSA) were previously proved to be significant nucleation precursors in marine areas. However, the nucleation process involved in IA and MSA remains unclear. We show the enhancement of MSA on IA cluster formation and reveal the IAM-SA nucleating mechanism using a theoretical approach. This study helps to understand the clustering process in which marine sulfur- and iodine-containing species are jointly involved and its impact on new particle formation.
Haoran Zhang, Nan Li, Keqin Tang, Hong Liao, Chong Shi, Cheng Huang, Hongli Wang, Song Guo, Min Hu, Xinlei Ge, Mindong Chen, Zhenxin Liu, Huan Yu, and Jianlin Hu
Atmos. Chem. Phys., 22, 5495–5514, https://doi.org/10.5194/acp-22-5495-2022, https://doi.org/10.5194/acp-22-5495-2022, 2022
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We developed a new algorithm with low economic/technique costs to identify primary and secondary components of PM2.5. Our model was shown to be reliable by comparison with different observation datasets. We systematically explored the patterns and changes in the secondary PM2.5 pollution in China at large spatial and time scales. We believe that this method is a promising tool for efficiently estimating primary and secondary PM2.5, and has huge potential for future PM mitigation.
Chao Gao, Aijun Xiu, Xuelei Zhang, Qingqing Tong, Hongmei Zhao, Shichun Zhang, Guangyi Yang, and Mengduo Zhang
Atmos. Chem. Phys., 22, 5265–5329, https://doi.org/10.5194/acp-22-5265-2022, https://doi.org/10.5194/acp-22-5265-2022, 2022
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With ever-growing applications of two-way coupled meteorology and air quality models in Asia over the past decade, this paper summarizes the current status and research focuses, as well as how aerosol effects impact model performance, meteorology, and air quality. These models enable investigations of ARI and ACI effects induced by natural and anthropogenic aerosols in Asia, which has serious air pollution problems. The current gaps and perspectives are also presented and discussed.
Susannah M. Burrows, Richard C. Easter, Xiaohong Liu, Po-Lun Ma, Hailong Wang, Scott M. Elliott, Balwinder Singh, Kai Zhang, and Philip J. Rasch
Atmos. Chem. Phys., 22, 5223–5251, https://doi.org/10.5194/acp-22-5223-2022, https://doi.org/10.5194/acp-22-5223-2022, 2022
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Sea spray particles are composed of a mixture of salts and organic substances from oceanic microorganisms. In prior work, our team developed an approach connecting sea spray chemistry to ocean biology, called OCEANFILMS. Here we describe its implementation within an Earth system model, E3SM. We show that simulated sea spray chemistry is consistent with observed seasonal cycles and that sunlight reflected by simulated Southern Ocean clouds increases, consistent with analysis of satellite data.
Jiandong Wang, Jia Xing, Shuxiao Wang, Rohit Mathur, Jiaping Wang, Yuqiang Zhang, Chao Liu, Jonathan Pleim, Dian Ding, Xing Chang, Jingkun Jiang, Peng Zhao, Shovan Kumar Sahu, Yuzhi Jin, David C. Wong, and Jiming Hao
Atmos. Chem. Phys., 22, 5147–5156, https://doi.org/10.5194/acp-22-5147-2022, https://doi.org/10.5194/acp-22-5147-2022, 2022
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Aerosols reduce surface solar radiation and change the photolysis rate and planetary boundary layer stability. In this study, the online coupled meteorological and chemistry model was used to explore the detailed pathway of how aerosol direct effects affect secondary inorganic aerosol. The effects through the dynamics pathway act as an equally or even more important route compared with the photolysis pathway in affecting secondary aerosol concentration in both summer and winter.
Adam Milsom, Adam M. Squires, Andrew D. Ward, and Christian Pfrang
Atmos. Chem. Phys., 22, 4895–4907, https://doi.org/10.5194/acp-22-4895-2022, https://doi.org/10.5194/acp-22-4895-2022, 2022
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Cooking emissions can self-organise into nanostructured lamellar bilayers, and this can influence reaction kinetics. We developed a kinetic multi-layer model-based description of decay data we obtained from laboratory experiments of the ozonolysis of coated films of such a self-organised system, demonstrating a decreased diffusivity for both oleic acid and ozone. Nanostructure formation can thus increase the reactive half-life of oleic acid by days under typical indoor and outdoor conditions.
Suxia Yang, Bin Yuan, Yuwen Peng, Shan Huang, Wei Chen, Weiwei Hu, Chenglei Pei, Jun Zhou, David D. Parrish, Wenjie Wang, Xianjun He, Chunlei Cheng, Xiao-Bing Li, Xiaoyun Yang, Yu Song, Haichao Wang, Jipeng Qi, Baolin Wang, Chen Wang, Chaomin Wang, Zelong Wang, Tiange Li, E Zheng, Sihang Wang, Caihong Wu, Mingfu Cai, Chenshuo Ye, Wei Song, Peng Cheng, Duohong Chen, Xinming Wang, Zhanyi Zhang, Xuemei Wang, Junyu Zheng, and Min Shao
Atmos. Chem. Phys., 22, 4539–4556, https://doi.org/10.5194/acp-22-4539-2022, https://doi.org/10.5194/acp-22-4539-2022, 2022
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We use a model constrained using observations to study the formation of nitrate aerosol in and downwind of a representative megacity. We found different contributions of various chemical reactions to ground-level nitrate concentrations between urban and suburban regions. We also show that controlling VOC emissions are effective for decreasing nitrate formation in both urban and regional environments, although VOCs are not direct precursors of nitrate aerosol.
Hao Yang, Lei Chen, Hong Liao, Jia Zhu, Wenjie Wang, and Xin Li
Atmos. Chem. Phys., 22, 4101–4116, https://doi.org/10.5194/acp-22-4101-2022, https://doi.org/10.5194/acp-22-4101-2022, 2022
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Aerosols can influence O3 through aerosol–radiation interactions, including aerosol–photolysis interaction (API) and aerosol–radiation feedback (ARF). The weakened photolysis rates and changed meteorological conditions reduce surface-layer O3 concentrations by up to 9.3–11.4 ppb, with API and ARF contributing 74.6 %–90.0 % and 10.0 %–25.4 % of the O3 decrease in three episodes, respectively, which indicates that API is the dominant way for O3 reduction related to aerosol–radiation interactions.
Patricia Tarín-Carrasco, Ulas Im, Camilla Geels, Laura Palacios-Peña, and Pedro Jiménez-Guerrero
Atmos. Chem. Phys., 22, 3945–3965, https://doi.org/10.5194/acp-22-3945-2022, https://doi.org/10.5194/acp-22-3945-2022, 2022
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The evidence of the effects of atmospheric pollution (and particularly fine particulate matter, PM2.5) on human mortality is now unquestionable. Here, 895 000 annual premature deaths (PD) are estimated for the present (1991–2010), which increases to 1 540 000 in the year 2050 due to the ageing of the European population. The implementation of a mitigation scenario (80 % of the energy production in Europe from renewable sources) could lead to a decrease of over 60 000 annual PD for the year 2050.
Xiajie Yang, Qiaoqiao Wang, Nan Ma, Weiwei Hu, Yang Gao, Zhijiong Huang, Junyu Zheng, Bin Yuan, Ning Yang, Jiangchuan Tao, Juan Hong, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 22, 3743–3762, https://doi.org/10.5194/acp-22-3743-2022, https://doi.org/10.5194/acp-22-3743-2022, 2022
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We use the GEOS-Chem model with additional anthropogenic and biomass burning chlorine emissions combined with updated parameterizations for N2O5 + Cl chemistry to investigate the impacts of chlorine chemistry on air quality in China. Our study not only significantly improves the model's performance but also demonstrates the importance of non-sea-salt chlorine sources as well as an appropriate parameterization for N2O5 + Cl chemistry to the impact of chlorine chemistry in China.
Long Chen, Yu Huang, Yonggang Xue, Zhihui Jia, and Wenliang Wang
Atmos. Chem. Phys., 22, 3693–3711, https://doi.org/10.5194/acp-22-3693-2022, https://doi.org/10.5194/acp-22-3693-2022, 2022
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Quantum chemical methods are applied to gain insight into the detailed mechanisms of OH-initiated oxidation of distinct HHPs. The dominant pathway is H-abstraction from the -OOH group in the initiation reactions of the OH radical with HOCH2OOH and HOC(CH3)2OOH. H-abstraction from -CH group is competitive with that from the -OOH group in the reaction of the OH radical with HOCH(CH3)OOH. The barrier of H-abstraction from the -OOH group is slightly increased as the methyl group number increases.
Joseph Lilek and Andreas Zuend
Atmos. Chem. Phys., 22, 3203–3233, https://doi.org/10.5194/acp-22-3203-2022, https://doi.org/10.5194/acp-22-3203-2022, 2022
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Depending on temperature and chemical makeup, certain aerosols can be highly viscous or glassy, with atmospheric implications. We have therefore implemented two major upgrades to the predictive viscosity model AIOMFAC-VISC. First, we created a new viscosity model for aqueous electrolyte solutions containing an arbitrary number of ion species. Second, we integrated the electrolyte model within the existing AIOMFAC-VISC framework to enable viscosity predictions for organic–inorganic mixtures.
Rongjie Zhang, Jiewen Shen, Hong-Bin Xie, Jingwen Chen, and Jonas Elm
Atmos. Chem. Phys., 22, 2639–2650, https://doi.org/10.5194/acp-22-2639-2022, https://doi.org/10.5194/acp-22-2639-2022, 2022
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Formic acid is screened out as the species that can effectively catalyze the new particle formation (NPF) of the methanesulfonic acid (MSA)–methylamine system, indicating organic acids might be required to facilitate MSA-driven NPF in the atmosphere. The results are significant to comprehensively understand the MSA-driven NPF and expand current knowledge of the contribution of OAs to NPF.
Amina Khaled, Minghui Zhang, and Barbara Ervens
Atmos. Chem. Phys., 22, 1989–2009, https://doi.org/10.5194/acp-22-1989-2022, https://doi.org/10.5194/acp-22-1989-2022, 2022
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Chemical reactions with iron in clouds and aerosol form and cycle reactive oxygen species (ROS). Previous model studies assumed that all cloud droplets (particles) contain iron, while single-particle analyses showed otherwise. By means of a model, we explore the bias in predicted ROS budgets by distributing a given iron mass to either all or only a few droplets (particles). Implications for oxidation potential, radical loss and iron oxidation state are discussed.
Pablo Garcia Rivera, Brian T. Dinkelacker, Ioannis Kioutsioukis, Peter J. Adams, and Spyros N. Pandis
Atmos. Chem. Phys., 22, 2011–2027, https://doi.org/10.5194/acp-22-2011-2022, https://doi.org/10.5194/acp-22-2011-2022, 2022
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The contribution of various pollution sources to the variability of fine PM in an urban area was examined using as an example the city of Pittsburgh. Biomass burning aerosol shows the largest variability during the winter with local maxima within the city and in the suburbs. During both periods the largest contributing source to the average PM2.5 is particles from outside the modeling domain. The average population-weighted PM2.5 concentration does not change significantly with resolution.
Noelia Otero, Oscar E. Jurado, Tim Butler, and Henning W. Rust
Atmos. Chem. Phys., 22, 1905–1919, https://doi.org/10.5194/acp-22-1905-2022, https://doi.org/10.5194/acp-22-1905-2022, 2022
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Surface ozone and temperature are strongly dependent and their extremes might be exacerbated by underlying climatological drivers, such as atmospheric blocking. Using an observational data set, we measure the dependence structure between ozone and temperature under the influence of atmospheric blocking. Blocks enhanced the probability of occurrence of compound ozone and temperature extremes over northwestern and central Europe, leading to greater health risks.
Ka Ming Fung, Colette L. Heald, Jesse H. Kroll, Siyuan Wang, Duseong S. Jo, Andrew Gettelman, Zheng Lu, Xiaohong Liu, Rahul A. Zaveri, Eric C. Apel, Donald R. Blake, Jose-Luis Jimenez, Pedro Campuzano-Jost, Patrick R. Veres, Timothy S. Bates, John E. Shilling, and Maria Zawadowicz
Atmos. Chem. Phys., 22, 1549–1573, https://doi.org/10.5194/acp-22-1549-2022, https://doi.org/10.5194/acp-22-1549-2022, 2022
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Understanding the natural aerosol burden in the preindustrial era is crucial for us to assess how atmospheric aerosols affect the Earth's radiative budgets. Our study explores how a detailed description of dimethyl sulfide (DMS) oxidation (implemented in the Community Atmospheric Model version 6 with chemistry, CAM6-chem) could help us better estimate the present-day and preindustrial concentrations of sulfate and other relevant chemicals, as well as the resulting aerosol radiative impacts.
Cited articles
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Surface ozone response to satellite-constrained SO2 emission adjustments and its implications,
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Bae, C., Kim, H. C., Kim, B.-U., Kim, Y., Woo, J.-H., and Kim, S.:
Updating Chinese SO2 emissions with surface observations for regional air-quality modeling over East Asia,
Atmos. Environ.,
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Does lockdown reduce air pollution? Evidence from 44 cities in northern China,
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Short summary
Global outbreaks of COVID-19 offer rare opportunities of natural experiments in emission control and corresponding responses of tropospheric chemistry. This study's novel approach investigates (1) isolating the pandemic's impact from natural and anthropogenic variations, (2) emission adjustment to reproduce real-time emissions, and (3) brute-force modeling to investigate Chinese economic activities. Results provide characteristics of the region's chemistry and emissions.
Global outbreaks of COVID-19 offer rare opportunities of natural experiments in emission control...
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