Articles | Volume 21, issue 21
Atmos. Chem. Phys., 21, 16183–16201, 2021
https://doi.org/10.5194/acp-21-16183-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Atmos. Chem. Phys., 21, 16183–16201, 2021
https://doi.org/10.5194/acp-21-16183-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
04 Nov 2021
Research article
| 04 Nov 2021
Process-based and observation-constrained SOA simulations in China: the role of semivolatile and intermediate-volatility organic compounds and OH levels
Ruqian Miao et al.
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This work characterized the spatial variabilities of air pollutants in a megacity by advanced mobile measurements. The results show a large spatial heterogeneity in the distributions of PM2.5 composition and volatile organic compounds under non-haze conditions, and relatively uniform spatial distributions under haze conditions that may indicate a chemical homogeneity on an intracity scale. The findings improve our understanding of urban air pollution.
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In this study we evaluated the model performances for simulating secondary inorganic aerosol (SIA) and organic aerosol (OA) in PM2.5 in China against comprehensive datasets. The potential biases from factors related to meteorology, emission, chemistry, and atmospheric removal are systematically investigated. This study provides a comprehensive understanding of modeling PM2.5, which is important for studies on the effectiveness of emission control strategies.
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Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-426, https://doi.org/10.5194/acp-2022-426, 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 YRD. OH+NO2 pathway contributes to 60–83 % of the TNO3 production rates, and the N2O5 heterogeneous pathway contributes to 10–36 %. N2O5 heterogeneous pathway becomes more important in cold seasons. Local emissions and regional transportation contribute to YRD NO3- concentrations by 50–62 % and 38–50 %, respectively.
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Atmos. Chem. Phys., 22, 7389–7404, https://doi.org/10.5194/acp-22-7389-2022, https://doi.org/10.5194/acp-22-7389-2022, 2022
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This work characterized the spatial variabilities of air pollutants in a megacity by advanced mobile measurements. The results show a large spatial heterogeneity in the distributions of PM2.5 composition and volatile organic compounds under non-haze conditions, and relatively uniform spatial distributions under haze conditions that may indicate a chemical homogeneity on an intracity scale. The findings improve our understanding of urban air pollution.
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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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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 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 Ruby L. Leung
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Here we analyze effective aerosol forcing simulated by E3SMv1 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.
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Atmos. Chem. Phys., 21, 12005–12019, https://doi.org/10.5194/acp-21-12005-2021, https://doi.org/10.5194/acp-21-12005-2021, 2021
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In this study, we conducted laboratory studies to investigate the formation of gas-phase highly oxygenated organic molecules (HOMs). We provide a thorough analysis on the importance of multistep auto-oxidation and multigeneration OH reactions. We also give an intensive investigation on the roles of high-NO2 conditions that represent a wide range of anthropogenically influenced environments.
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Atmos. Chem. Phys., 21, 11531–11543, https://doi.org/10.5194/acp-21-11531-2021, https://doi.org/10.5194/acp-21-11531-2021, 2021
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Atmos. Chem. Phys., 21, 11405–11421, https://doi.org/10.5194/acp-21-11405-2021, https://doi.org/10.5194/acp-21-11405-2021, 2021
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Light absorption and radiative forcing of black carbon (BC) is influenced by both BC itself and its interactions with other aerosol chemical compositions. In this study, we used the online coupled WRF-Chem model to examine how emission control measures during the Asian-Pacific Economic Cooperation (APEC) conference affect the mixing state and light absorption of BC and the associated implications for BC-PBL interactions.
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WRF-GC is an online coupling of the WRF meteorological model and GEOS-Chem chemical transport model for regional atmospheric chemistry and air quality modeling. In WRF-GC v2.0, we implemented the aerosol–radiation interactions and aerosol–cloud interactions, as well as the capability to nest multiple domains for high-resolution simulations based on the modular framework of WRF-GC v1.0. This allows the GEOS-Chem users to investigate the meteorology–atmospheric chemistry interactions.
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Atmos. Chem. Phys., 21, 8003–8021, https://doi.org/10.5194/acp-21-8003-2021, https://doi.org/10.5194/acp-21-8003-2021, 2021
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Wei Yuan, Ru-Jin Huang, Lu Yang, Ting Wang, Jing Duan, Jie Guo, Haiyan Ni, Yang Chen, Qi Chen, Yongjie Li, Ulrike Dusek, Colin O'Dowd, and Thorsten Hoffmann
Atmos. Chem. Phys., 21, 3685–3697, https://doi.org/10.5194/acp-21-3685-2021, https://doi.org/10.5194/acp-21-3685-2021, 2021
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We characterized the seasonal variations in nitrated aromatic compounds (NACs) in composition, sources, and their light absorption contribution to brown carbon (BrC) aerosol in Xi'an, Northwest China. Our results show that secondary formation and vehicular emission were dominant sources in summer (~80 %), and biomass burning and coal combustion were major sources in winter (~75 %), and they indicate that the composition and sources of NACs have a profound impact on the light absorption of BrC
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This study demonstrates that the intensity of the western Pacific subtropical high (WPSH), a major synoptic pattern in the northern Pacific during summer, can induce a dipole change in surface ozone pollution over eastern China. Ozone concentration increases in the north and decreases in the south during the strong WPSH phase, and vice versa. The change in chemical processes associated with the WPSH change plays a decisive role, whereas the natural emission of ozone precursors accounts for ~ 30 %.
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Meteorological conditions play important roles in the formation of O3 and PM2.5 pollution in China. O3 is most sensitive to temperature and the sensitivity is dependent on the O3 chemistry formation or loss regime. PM2.5 is negatively sensitive to temperature, wind speed, and planetary boundary layer height and positively sensitive to humidity. The results imply that air quality in certain regions of China is sensitive to climate changes.
Lixia Liu, Yafang Cheng, Siwen Wang, Chao Wei, Mira L. Pöhlker, Christopher Pöhlker, Paulo Artaxo, Manish Shrivastava, Meinrat O. Andreae, Ulrich Pöschl, and Hang Su
Atmos. Chem. Phys., 20, 13283–13301, https://doi.org/10.5194/acp-20-13283-2020, https://doi.org/10.5194/acp-20-13283-2020, 2020
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This modeling paper reveals how aerosol–cloud interactions (ACIs) and aerosol–radiation interactions (ARIs) induced by biomass burning (BB) aerosols act oppositely on radiation, cloud, and precipitation in the Amazon during the dry season. The varying relative significance of ACIs and ARIs with BB aerosol concentration leads to a nonlinear dependence of the total climate response on BB aerosol loading and features the growing importance of ARIs at high aerosol loading.
Ruqian Miao, Qi Chen, Yan Zheng, Xi Cheng, Yele Sun, Paul I. Palmer, Manish Shrivastava, Jianping Guo, Qiang Zhang, Yuhan Liu, Zhaofeng Tan, Xuefei Ma, Shiyi Chen, Limin Zeng, Keding Lu, and Yuanhang Zhang
Atmos. Chem. Phys., 20, 12265–12284, https://doi.org/10.5194/acp-20-12265-2020, https://doi.org/10.5194/acp-20-12265-2020, 2020
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In this study we evaluated the model performances for simulating secondary inorganic aerosol (SIA) and organic aerosol (OA) in PM2.5 in China against comprehensive datasets. The potential biases from factors related to meteorology, emission, chemistry, and atmospheric removal are systematically investigated. This study provides a comprehensive understanding of modeling PM2.5, which is important for studies on the effectiveness of emission control strategies.
Xiao Lu, Lin Zhang, Tongwen Wu, Michael S. Long, Jun Wang, Daniel J. Jacob, Fang Zhang, Jie Zhang, Sebastian D. Eastham, Lu Hu, Lei Zhu, Xiong Liu, and Min Wei
Geosci. Model Dev., 13, 3817–3838, https://doi.org/10.5194/gmd-13-3817-2020, https://doi.org/10.5194/gmd-13-3817-2020, 2020
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This study presents the development and evaluation of a new climate chemistry model, BCC-GEOS-Chem v1.0, which couples the GEOS-Chem chemical transport model as an atmospheric chemistry component in the Beijing Climate Center atmospheric general circulation model. A 3-year (2012–2014) simulation of BCC-GEOS-Chem v1.0 shows that the model captures well the spatiotemporal distributions of tropospheric ozone, other gaseous pollutants, and aerosols.
Ru-Jin Huang, Yao He, Jing Duan, Yongjie Li, Qi Chen, Yan Zheng, Yang Chen, Weiwei Hu, Chunshui Lin, Haiyan Ni, Wenting Dai, Junji Cao, Yunfei Wu, Renjian Zhang, Wei Xu, Jurgita Ovadnevaite, Darius Ceburnis, Thorsten Hoffmann, and Colin D. O'Dowd
Atmos. Chem. Phys., 20, 9101–9114, https://doi.org/10.5194/acp-20-9101-2020, https://doi.org/10.5194/acp-20-9101-2020, 2020
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We systematically compared the submicron particle (PM1) processes in haze days with low and high relative humidity (RH) in wintertime Beijing. Nitrate had similar daytime growth rates in low-RH and high-RH pollution. OOA had a higher growth rate in low-RH pollution than in high-RH pollution. Sulfate had a decreasing trend in low-RH pollution, while it increased significantly in high-RH pollution. This distinction may be explained by the different processes affected by meteorological conditions.
Haipeng Lin, Xu Feng, Tzung-May Fu, Heng Tian, Yaping Ma, Lijuan Zhang, Daniel J. Jacob, Robert M. Yantosca, Melissa P. Sulprizio, Elizabeth W. Lundgren, Jiawei Zhuang, Qiang Zhang, Xiao Lu, Lin Zhang, Lu Shen, Jianping Guo, Sebastian D. Eastham, and Christoph A. Keller
Geosci. Model Dev., 13, 3241–3265, https://doi.org/10.5194/gmd-13-3241-2020, https://doi.org/10.5194/gmd-13-3241-2020, 2020
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Online coupling of meteorology and chemistry models often presents maintenance issues with hard-wired coding. We present WRF-GC, an one-way online coupling of the WRF meteorological model and GEOS-Chem atmospheric chemistry model for regional atmospheric chemistry and air quality modeling. Our coupling structure allows future versions of either parent model to be immediately integrated into WRF-GC. The WRF-GC model was able to well reproduce regional PM2.5 with greater computational efficiency.
Jingyi Li, Haowen Zhang, Qi Ying, Zhijun Wu, Yanli Zhang, Xinming Wang, Xinghua Li, Yele Sun, Min Hu, Yuanhang Zhang, and Jianlin Hu
Atmos. Chem. Phys., 20, 7291–7306, https://doi.org/10.5194/acp-20-7291-2020, https://doi.org/10.5194/acp-20-7291-2020, 2020
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Large gaps still exist in modeled and observed secondary organic aerosol (SOA) mass loading and properties. Here we investigated the impacts of water partitioning into organic aerosol and nonideality of the organic–water mixture on SOA over eastern China using a regional 3D model. SOA is increased more significantly in humid and hot environments. Increases in SOA further cause an enhancement of the cooling effects of aerosols. It is crucial to consider the above processes in modeling SOA.
Camille Mouchel-Vallon, Julia Lee-Taylor, Alma Hodzic, Paulo Artaxo, Bernard Aumont, Marie Camredon, David Gurarie, Jose-Luis Jimenez, Donald H. Lenschow, Scot T. Martin, Janaina Nascimento, John J. Orlando, Brett B. Palm, John E. Shilling, Manish Shrivastava, and Sasha Madronich
Atmos. Chem. Phys., 20, 5995–6014, https://doi.org/10.5194/acp-20-5995-2020, https://doi.org/10.5194/acp-20-5995-2020, 2020
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The GoAmazon 2014/5 field campaign took place near the city of Manaus, Brazil, isolated in the Amazon rainforest, to study the impacts of urban pollution on natural air masses. We simulated this campaign with an extremely detailed organic chemistry model to understand how the city would affect the growth and composition of natural aerosol particles. Discrepancies between the model and the measurements indicate that the chemistry of naturally emitted organic compounds is still poorly understood.
Yan Zheng, Xi Cheng, Keren Liao, Yaowei Li, Yong Jie Li, Ru-Jin Huang, Weiwei Hu, Ying Liu, Tong Zhu, Shiyi Chen, Limin Zeng, Douglas R. Worsnop, and Qi Chen
Atmos. Meas. Tech., 13, 2457–2472, https://doi.org/10.5194/amt-13-2457-2020, https://doi.org/10.5194/amt-13-2457-2020, 2020
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This paper provides important information to help researchers to understand the mass quantification and source apportionment by Aerodyne aerosol mass spectrometers.
Youwen Sun, Cheng Liu, Lin Zhang, Mathias Palm, Justus Notholt, Hao Yin, Corinne Vigouroux, Erik Lutsch, Wei Wang, Changong Shan, Thomas Blumenstock, Tomoo Nagahama, Isamu Morino, Emmanuel Mahieu, Kimberly Strong, Bavo Langerock, Martine De Mazière, Qihou Hu, Huifang Zhang, Christof Petri, and Jianguo Liu
Atmos. Chem. Phys., 20, 5437–5456, https://doi.org/10.5194/acp-20-5437-2020, https://doi.org/10.5194/acp-20-5437-2020, 2020
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We present multiyear time series of ground-based Fourier-transform infrared spectroscopy measurements of HCN in densely populated eastern China. The seasonality and interannual variability of tropospheric HCN columns were investigated. The potential sources that drive the observed HCN seasonality and interannual variability were determined using a GEOS-Chem tagged CO simulation, global fire maps, and potential source contribution function values calculated using HYSPLIT back trajectories.
Wei Yuan, Ru-Jin Huang, Lu Yang, Jie Guo, Ziyi Chen, Jing Duan, Ting Wang, Haiyan Ni, Yongming Han, Yongjie Li, Qi Chen, Yang Chen, Thorsten Hoffmann, and Colin O'Dowd
Atmos. Chem. Phys., 20, 5129–5144, https://doi.org/10.5194/acp-20-5129-2020, https://doi.org/10.5194/acp-20-5129-2020, 2020
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We characterized light-absorbing properties, chromophore composition and sources of brown carbon (BrC) in Xi'an; identified three groups of light-absorbing organics; and quantified their contribution to overall BrC absorption. Our results showed that vehicle emissions and secondary formation are major sources of BrC in spring, coal combustion and vehicle emissions are major sources in fall, biomass burning and coal combustion become major sources in winter, and secondary BrC dominates in summer.
Meng Gao, Jinhui Gao, Bin Zhu, Rajesh Kumar, Xiao Lu, Shaojie Song, Yuzhong Zhang, Beixi Jia, Peng Wang, Gufran Beig, Jianlin Hu, Qi Ying, Hongliang Zhang, Peter Sherman, and Michael B. McElroy
Atmos. Chem. Phys., 20, 4399–4414, https://doi.org/10.5194/acp-20-4399-2020, https://doi.org/10.5194/acp-20-4399-2020, 2020
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A regional fully coupled meteorology–chemistry model, Weather Research and Forecasting model with Chemistry (WRF-Chem), was employed to study the seasonality of ozone (O3) pollution and its sources in both China and India.
Jing Duan, Ru-Jin Huang, Yongjie Li, Qi Chen, Yan Zheng, Yang Chen, Chunshui Lin, Haiyan Ni, Meng Wang, Jurgita Ovadnevaite, Darius Ceburnis, Chunying Chen, Douglas R. Worsnop, Thorsten Hoffmann, Colin O'Dowd, and Junji Cao
Atmos. Chem. Phys., 20, 3793–3807, https://doi.org/10.5194/acp-20-3793-2020, https://doi.org/10.5194/acp-20-3793-2020, 2020
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We characterized secondary aerosol formation in Beijing. Our results showed that relative humidity (RH) and Ox have opposite effects on sulfate and nitrate formation in summer and winter. The wintertime more-oxidized OOA (MO-OOA) showed a good correlation with aerosol liquid water content (ALWC). Meanwhile, the dependence of less-oxidized OOA (LO-OOA) and the mass ratio of LO-OOA to MO-OOA in Ox both degraded when RH > 60 %, suggesting that RH or ALWC may also affect LO-OOA formation.
Yadong Lei, Xu Yue, Hong Liao, Cheng Gong, and Lin Zhang
Geosci. Model Dev., 13, 1137–1153, https://doi.org/10.5194/gmd-13-1137-2020, https://doi.org/10.5194/gmd-13-1137-2020, 2020
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We coupled a dynamic vegetation model YIBs with the chemical transport model GEOS-Chem to develop a new tool for studying interactions between atmospheric chemistry and biosphere. Within this framework, leaf area index and stomatal conductance are predicted for chemical simulations. In turn, surface ozone causes negative impacts to plant growth and the consequent dry deposition. Such interactions are important for air pollution prediction but ignored in most of current chemical models.
Tongwen Wu, Fang Zhang, Jie Zhang, Weihua Jie, Yanwu Zhang, Fanghua Wu, Laurent Li, Jinghui Yan, Xiaohong Liu, Xiao Lu, Haiyue Tan, Lin Zhang, Jun Wang, and Aixue Hu
Geosci. Model Dev., 13, 977–1005, https://doi.org/10.5194/gmd-13-977-2020, https://doi.org/10.5194/gmd-13-977-2020, 2020
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This paper describes the first version of the Beijing Climate Center (BCC) fully coupled Earth System Model with interactive atmospheric chemistry and aerosols (BCC-ESM1). It is one of the models at the BCC for the Coupled Model Intercomparison Project Phase 6 (CMIP6). The CMIP6 Aerosol Chemistry Model Intercomparison Project (AerChemMIP) experiment using BCC-ESM1 has been finished. The evaluations show an overall good agreement between BCC-ESM1 simulations and observations in the 20th century.
Xin Yu, Melissa Venecek, Anikender Kumar, Jianlin Hu, Saffet Tanrikulu, Su-Tzai Soon, Cuong Tran, David Fairley, and Michael J. Kleeman
Atmos. Chem. Phys., 19, 14677–14702, https://doi.org/10.5194/acp-19-14677-2019, https://doi.org/10.5194/acp-19-14677-2019, 2019
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Predictions and measurements of ultrafine particle number and mass concentrations were in overall good agreement at 14 sites across California in the years 2012, 2015, and 2016. On-road vehicles, food cooking, and aircraft were important sources of ultrafine particles as expected, but natural gas combustion was also a significant source at all locations across California. These results can be used to study the health effects of ultrafine particles.
Meng Wang, Ru-Jin Huang, Junji Cao, Wenting Dai, Jiamao Zhou, Chunshui Lin, Haiyan Ni, Jing Duan, Ting Wang, Yang Chen, Yongjie Li, Qi Chen, Imad El Haddad, and Thorsten Hoffmann
Atmos. Meas. Tech., 12, 4779–4789, https://doi.org/10.5194/amt-12-4779-2019, https://doi.org/10.5194/amt-12-4779-2019, 2019
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The analytical performances of SE-GC-MS and TD-GC-MS for the determination of n-alkanes, PAHs and hopanes were evaluated and compared. The two methods show a good agreement with a high correlation efficient (R2 > 0.98) and a slope close to unity. The concentrations of n-alkanes, PAHs and hopanes are found to be much higher in Beijing than those in Chengdu, Shanghai and Guangzhou, most likely due to emissions from coal combustion for wintertime heating in Beijing.
Jingwei Liu, Xin Li, Yiming Yang, Haichao Wang, Yusheng Wu, Xuewei Lu, Mindong Chen, Jianlin Hu, Xiaobo Fan, Limin Zeng, and Yuanhang Zhang
Atmos. Meas. Tech., 12, 4439–4453, https://doi.org/10.5194/amt-12-4439-2019, https://doi.org/10.5194/amt-12-4439-2019, 2019
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Incoherent broadband cavity-enhanced absorption spectroscopy (IBBCEAS) has been proven to be a reliable method for measuring glyoxal and methylglyoxal in the atmosphere. However, the commonly overlying strong spectral absorption of nitrogen dioxide hampers the accurate and sensitive resolve of the weak absorption features of glyoxal and methylglyoxal. Here, we report a custom-built IBBCEAS system that could overcome this problem by quantitatively removing nitrogen dioxide from the sample air.
Jing Duan, Ru-Jin Huang, Chunshui Lin, Wenting Dai, Meng Wang, Yifang Gu, Ying Wang, Haobin Zhong, Yan Zheng, Haiyan Ni, Uli Dusek, Yang Chen, Yongjie Li, Qi Chen, Douglas R. Worsnop, Colin D. O'Dowd, and Junji Cao
Atmos. Chem. Phys., 19, 10319–10334, https://doi.org/10.5194/acp-19-10319-2019, https://doi.org/10.5194/acp-19-10319-2019, 2019
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We present the seasonal distinction of secondary aerosol formation in urban Beijing. Both photochemical oxidation and aqueous-phase processing played important roles in SOA (secondary organic aerosol) formation during all three seasons; while for sulfate formation, gas-phase photochemical oxidation was the major pathway in late summer, aqueous-phase reactions were more responsible during early winter, and both processes had contributions during autumn.
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.
Jingyuan Shao, Qianjie Chen, Yuxuan Wang, Xiao Lu, Pengzhen He, Yele Sun, Viral Shah, Randall V. Martin, Sajeev Philip, Shaojie Song, Yue Zhao, Zhouqing Xie, Lin Zhang, and Becky Alexander
Atmos. Chem. Phys., 19, 6107–6123, https://doi.org/10.5194/acp-19-6107-2019, https://doi.org/10.5194/acp-19-6107-2019, 2019
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Sulfate is a key species contributing to particle formation and growth during wintertime Chinese haze events. This study combines observations and modeling of oxygen isotope signatures in sulfate aerosol to investigate its formation mechanisms, with a focus on heterogeneous production on aerosol surface via H2O2, O3, and NO2 and trace metal catalyzed oxidation. Contributions from different formation pathways are presented.
Zhenying Xu, Mingxu Liu, Minsi Zhang, Yu Song, Shuxiao Wang, Lin Zhang, Tingting Xu, Tiantian Wang, Caiqing Yan, Tian Zhou, Yele Sun, Yuepeng Pan, Min Hu, Mei Zheng, and Tong Zhu
Atmos. Chem. Phys., 19, 5605–5613, https://doi.org/10.5194/acp-19-5605-2019, https://doi.org/10.5194/acp-19-5605-2019, 2019
Ru-Jin Huang, Yichen Wang, Junji Cao, Chunshui Lin, Jing Duan, Qi Chen, Yongjie Li, Yifang Gu, Jin Yan, Wei Xu, Roman Fröhlich, Francesco Canonaco, Carlo Bozzetti, Jurgita Ovadnevaite, Darius Ceburnis, Manjula R. Canagaratna, John Jayne, Douglas R. Worsnop, Imad El-Haddad, André S. H. Prévôt, and Colin D. O'Dowd
Atmos. Chem. Phys., 19, 2283–2298, https://doi.org/10.5194/acp-19-2283-2019, https://doi.org/10.5194/acp-19-2283-2019, 2019
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We found that in wintertime Shijiazhuang fine PM was mostly from primary emissions without sufficient atmospheric aging. In addition, secondary inorganic and organic aerosol dominated in pollution events under high-RH conditions, likely due to enhanced aqueous-phase chemistry, whereas primary organic aerosol dominated in pollution events under low-RH and stagnant conditions. Our results also highlighted the importance of meteorological conditions for PM pollution in this highly polluted city.
Junfeng Wang, Dantong Liu, Xinlei Ge, Yangzhou Wu, Fuzhen Shen, Mindong Chen, Jian Zhao, Conghui Xie, Qingqing Wang, Weiqi Xu, Jie Zhang, Jianlin Hu, James Allan, Rutambhara Joshi, Pingqing Fu, Hugh Coe, and Yele Sun
Atmos. Chem. Phys., 19, 447–458, https://doi.org/10.5194/acp-19-447-2019, https://doi.org/10.5194/acp-19-447-2019, 2019
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This work is part of the UK-China APHH campaign. We used a laser-only Aerodyne soot particle aerosol mass spectrometer, for the first time, to investigate the concentrations, size distributions and chemical compositions for those ambient submicron aerosol particles only with black carbon as cores. Our findings are valuable to understand the BC properties and processes in the densely populated megacities.
Mingxu Liu, Xin Huang, Yu Song, Tingting Xu, Shuxiao Wang, Zhijun Wu, Min Hu, Lin Zhang, Qiang Zhang, Yuepeng Pan, Xuejun Liu, and Tong Zhu
Atmos. Chem. Phys., 18, 17933–17943, https://doi.org/10.5194/acp-18-17933-2018, https://doi.org/10.5194/acp-18-17933-2018, 2018
Yangyang Zhang, Aohan Tang, Dandan Wang, Qingqing Wang, Katie Benedict, Lin Zhang, Duanyang Liu, Yi Li, Jeffrey L. Collett Jr., Yele Sun, and Xuejun Liu
Atmos. Chem. Phys., 18, 16385–16398, https://doi.org/10.5194/acp-18-16385-2018, https://doi.org/10.5194/acp-18-16385-2018, 2018
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Our study is the first to continually monitor the vertical concentration profile of NH3 in urban Beijing. Weekly concentrations averaged 13.3 ± 4.8 μg m−3. The highest NH3 concentrations were always observed between 32 and 63 m, decreasing toward the surface and toward higher altitudes. Our results demonstrate a NH3 rich atmosphere in urban Beijing, from the ground to at least 320 m. Regional transport from the south (intensive agricultural regions) contributed high NH3 concentrations in Beijing.
Hansen Cao, Tzung-May Fu, Lin Zhang, Daven K. Henze, Christopher Chan Miller, Christophe Lerot, Gonzalo González Abad, Isabelle De Smedt, Qiang Zhang, Michel van Roozendael, François Hendrick, Kelly Chance, Jie Li, Junyu Zheng, and Yuanhong Zhao
Atmos. Chem. Phys., 18, 15017–15046, https://doi.org/10.5194/acp-18-15017-2018, https://doi.org/10.5194/acp-18-15017-2018, 2018
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Our top-down estimates for annual total Chinese NMVOC emissions was 30.7 to 49.5 Tg y−1, including 16.4 to 23.6 Tg y−1 from anthropogenic sources, 12.2 to 22.8 Tg y−1 from biogenic sources, and 2.08 to 3.13 Tg y−1 from biomass burning. Our four inversions consistently showed that the emissions of Chinese anthropogenic NMVOC precursors of glyoxal were larger than the a priori estimates. The glyoxal and formaldehyde constraints helped distinguish the NMVOC species from different sources.
Wei Zhou, Jian Zhao, Bin Ouyang, Archit Mehra, Weiqi Xu, Yuying Wang, Thomas J. Bannan, Stephen D. Worrall, Michael Priestley, Asan Bacak, Qi Chen, Conghui Xie, Qingqing Wang, Junfeng Wang, Wei Du, Yingjie Zhang, Xinlei Ge, Penglin Ye, James D. Lee, Pingqing Fu, Zifa Wang, Douglas Worsnop, Roderic Jones, Carl J. Percival, Hugh Coe, and Yele Sun
Atmos. Chem. Phys., 18, 11581–11597, https://doi.org/10.5194/acp-18-11581-2018, https://doi.org/10.5194/acp-18-11581-2018, 2018
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We present measurements of gas-phase N2O5 and ClNO2 by ToF-CIMS during summer in urban Beijing as part of the APHH campaign. High reactivity of N2O5 indicative of active nocturnal chemistry was observed. The lifetime of N2O5 as a function of aerosol surface area and relative humidity was characterized, and N2O5 uptake coefficients were estimated. We also found that the N2O5 loss in this study is mainly attributed to its indirect loss via reactions of NO3 with VOCs and NO.
Wen Xu, Lei Liu, Miaomiao Cheng, Yuanhong Zhao, Lin Zhang, Yuepeng Pan, Xiuming Zhang, Baojing Gu, Yi Li, Xiuying Zhang, Jianlin Shen, Li Lu, Xiaosheng Luo, Yu Zhao, Zhaozhong Feng, Jeffrey L. Collett Jr., Fusuo Zhang, and Xuejun Liu
Atmos. Chem. Phys., 18, 10931–10954, https://doi.org/10.5194/acp-18-10931-2018, https://doi.org/10.5194/acp-18-10931-2018, 2018
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Our main results demonstrate that atmospheric Nr pollution in eastern China is more serious in the northern region than in the southern region. Any effects of current emission controls are not yet apparent in Nr pollution. NH3 emissions from fertilizer use were the largest contributor (36 %) to total inorganic Nr deposition. Our results provide useful information for policy-makers that mitigation of NH3 emissions should be a priority to tackle serious N deposition.
Ru-Jin Huang, Junji Cao, Yang Chen, Lu Yang, Jincan Shen, Qihua You, Kai Wang, Chunshui Lin, Wei Xu, Bo Gao, Yongjie Li, Qi Chen, Thorsten Hoffmann, Colin D. O'Dowd, Merete Bilde, and Marianne Glasius
Atmos. Meas. Tech., 11, 3447–3456, https://doi.org/10.5194/amt-11-3447-2018, https://doi.org/10.5194/amt-11-3447-2018, 2018
Jennifer Kaiser, Daniel J. Jacob, Lei Zhu, Katherine R. Travis, Jenny A. Fisher, Gonzalo González Abad, Lin Zhang, Xuesong Zhang, Alan Fried, John D. Crounse, Jason M. St. Clair, and Armin Wisthaler
Atmos. Chem. Phys., 18, 5483–5497, https://doi.org/10.5194/acp-18-5483-2018, https://doi.org/10.5194/acp-18-5483-2018, 2018
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Isoprene emissions from vegetation have a large effect on atmospheric chemistry and air quality. Here we use the adjoint of GEOS-Chem in an inversion of OMI formaldehyde observations to produce top-down estimates of isoprene emissions in the southeast US during the summer of 2013. We find that MEGAN v2.1 is biased high on average by 40 %. Our downward correction of isoprene emissions leads to a small reduction in modeled surface O3 and decreases the contribution of isoprene to organic aerosol.
Xiao Lu, Lin Zhang, Xiong Liu, Meng Gao, Yuanhong Zhao, and Jingyuan Shao
Atmos. Chem. Phys., 18, 3101–3118, https://doi.org/10.5194/acp-18-3101-2018, https://doi.org/10.5194/acp-18-3101-2018, 2018
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Deteriorating tropospheric ozone pollution over India may not only affect local human health and vegetation but also perturb global ozone distribution. This study analyzes the processes controlling lower tropospheric ozone over India using OMI satellite observations (2006–2014) and model simulations (1990–2010). We show that the South Asian monsoon largely controls the seasonal cycle and interannual variability of Indian lower tropospheric ozone via changes in ozone production and transport.
Lin Zhang, Youfan Chen, Yuanhong Zhao, Daven K. Henze, Liye Zhu, Yu Song, Fabien Paulot, Xuejun Liu, Yuepeng Pan, Yi Lin, and Binxiang Huang
Atmos. Chem. Phys., 18, 339–355, https://doi.org/10.5194/acp-18-339-2018, https://doi.org/10.5194/acp-18-339-2018, 2018
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Substantial differences exist in current estimates of agricultural ammonia emissions in China, hindering understanding of their environmental consequences. This study applies both bottom-up and top-down methods to better quantify agricultural ammonia sources in China using observations from satellite and surface networks interpreted by a chemical transport model. Our estimate of annual Chinese anthropogenic ammonia emission is 11.7 tg (teragram) for 2008 with a strong seasonality peak in summer.
Louis Marelle, Jean-Christophe Raut, Kathy S. Law, Larry K. Berg, Jerome D. Fast, Richard C. Easter, Manish Shrivastava, and Jennie L. Thomas
Geosci. Model Dev., 10, 3661–3677, https://doi.org/10.5194/gmd-10-3661-2017, https://doi.org/10.5194/gmd-10-3661-2017, 2017
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We develop the WRF-Chem 3.5.1 model to improve simulations of aerosols and ozone in the Arctic. Both species are important air pollutants and climate forcers, but models often struggle to reproduce observations in the Arctic. Our developments concern pollutant emissions, mixing, chemistry, and removal, including processes related to snow and sea ice. The effect of these changes are quantitatively validated against observations, showing significant improvements compared to the original model.
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.
Yuanhong Zhao, Lin Zhang, Amos P. K. Tai, Youfan Chen, and Yuepeng Pan
Atmos. Chem. Phys., 17, 9781–9796, https://doi.org/10.5194/acp-17-9781-2017, https://doi.org/10.5194/acp-17-9781-2017, 2017
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Human activities have substantially enhanced atmospheric deposition of reactive nitrogen, inducing complex environmental consequences. This study presents a first quantitative investigation of how anthropogenic nitrogen deposition could impact surface ozone air quality through surface–atmosphere exchange processes. We find important surface ozone changes driven by nitrogen deposition, which can be comparable with those due to historical climate and land use changes.
Wen Xu, Wei Song, Yangyang Zhang, Xuejun Liu, Lin Zhang, Yuanhong Zhao, Duanyang Liu, Aohan Tang, Daowei Yang, Dandan Wang, Zhang Wen, Yuepeng Pan, David Fowler, Jeffrey L. Collett Jr., Jan Willem Erisman, Keith Goulding, Yi Li, and Fusuo Zhang
Atmos. Chem. Phys., 17, 31–46, https://doi.org/10.5194/acp-17-31-2017, https://doi.org/10.5194/acp-17-31-2017, 2017
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This paper evaluates the effectiveness of emission control measures implemented in Beijing during the Parade Blue period by integrating our own results, official-released data and modeling data. We demonstrate that emission control measures make a major contribution to air quality improvement in Beijing and surrounding regions. We conclude a joint local and regional control of secondary aerosol precursors to be key to curbing air pollution in Beijing.
Xiao Lu, Lin Zhang, Xu Yue, Jiachen Zhang, Daniel A. Jaffe, Andreas Stohl, Yuanhong Zhao, and Jingyuan Shao
Atmos. Chem. Phys., 16, 14687–14702, https://doi.org/10.5194/acp-16-14687-2016, https://doi.org/10.5194/acp-16-14687-2016, 2016
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Increasing wildfire activities in the mountainous western US may present a challenge for the region to attain a recently revised ozone air quality standard in summer. We quantify the wildfire influence on the ozone variability, trends, and number of high ozone days over this region in summers 1989–2010 using a Lagrangian dispersion model and statistical regression models.
Chun Zhao, Maoyi Huang, Jerome D. Fast, Larry K. Berg, Yun Qian, Alex Guenther, Dasa Gu, Manish Shrivastava, Ying Liu, Stacy Walters, Gabriele Pfister, Jiming Jin, John E. Shilling, and Carsten Warneke
Geosci. Model Dev., 9, 1959–1976, https://doi.org/10.5194/gmd-9-1959-2016, https://doi.org/10.5194/gmd-9-1959-2016, 2016
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In this study, the latest version of MEGAN is coupled within CLM4 in WRF-Chem. In this implementation, MEGAN shares a consistent vegetation map with CLM4. This improved modeling framework is used to investigate the impact of two land surface schemes on BVOCs and examine the sensitivity of BVOCs to vegetation distributions in California. This study indicates that more effort is needed to obtain the most appropriate and accurate land cover data sets for climate and air quality models.
W. Xu, X. S. Luo, Y. P. Pan, L. Zhang, A. H. Tang, J. L. Shen, Y. Zhang, K. H. Li, Q. H. Wu, D. W. Yang, Y. Y. Zhang, J. Xue, W. Q. Li, Q. Q. Li, L. Tang, S. H. Lu, T. Liang, Y. A. Tong, P. Liu, Q. Zhang, Z. Q. Xiong, X. J. Shi, L. H. Wu, W. Q. Shi, K. Tian, X. H. Zhong, K. Shi, Q. Y. Tang, L. J. Zhang, J. L. Huang, C. E. He, F. H. Kuang, B. Zhu, H. Liu, X. Jin, Y. J. Xin, X. K. Shi, E. Z. Du, A. J. Dore, S. Tang, J. L. Collett Jr., K. Goulding, Y. X. Sun, J. Ren, F. S. Zhang, and X. J. Liu
Atmos. Chem. Phys., 15, 12345–12360, https://doi.org/10.5194/acp-15-12345-2015, https://doi.org/10.5194/acp-15-12345-2015, 2015
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The annual average concentrations (1.3-47.0µg N m-3) and dry plus wet/bulk deposition fluxes (2.9-83.3kg N ha-1 yr-1) of inorganic Nr species ranked by land use as urban > rural > background sites and by regions as north China > southeast China > southwest China > northeast China > northwest China > Tibetan Plateau, reflecting the impact of anthropogenic Nr emission. Average dry and wet/bulk N deposition fluxes were 20.6 ± 11.2 and 19.3 ± 9.2kg kg N ha-1 yr-1 across China, respectively.
A. Lupascu, R. Easter, R. Zaveri, M. Shrivastava, M. Pekour, J. Tomlinson, Q. Yang, H. Matsui, A. Hodzic, Q. Zhang, and J. D. Fast
Atmos. Chem. Phys., 15, 12283–12313, https://doi.org/10.5194/acp-15-12283-2015, https://doi.org/10.5194/acp-15-12283-2015, 2015
W. W. Hu, P. Campuzano-Jost, B. B. Palm, D. A. Day, A. M. Ortega, P. L. Hayes, J. E. Krechmer, Q. Chen, M. Kuwata, Y. J. Liu, S. S. de Sá, K. McKinney, S. T. Martin, M. Hu, S. H. Budisulistiorini, M. Riva, J. D. Surratt, J. M. St. Clair, G. Isaacman-Van Wertz, L. D. Yee, A. H. Goldstein, S. Carbone, J. Brito, P. Artaxo, J. A. de Gouw, A. Koss, A. Wisthaler, T. Mikoviny, T. Karl, L. Kaser, W. Jud, A. Hansel, K. S. Docherty, M. L. Alexander, N. H. Robinson, H. Coe, J. D. Allan, M. R. Canagaratna, F. Paulot, and J. L. Jimenez
Atmos. Chem. Phys., 15, 11807–11833, https://doi.org/10.5194/acp-15-11807-2015, https://doi.org/10.5194/acp-15-11807-2015, 2015
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This work summarized all the studies reporting isoprene epoxydiols-derived secondary organic aerosol (IEPOX-SOA) measured globally by aerosol mass spectrometer and compare them with modeled gas-phase IEPOX, with results suggestive of the importance of IEPOX-SOA for regional and global OA budgets. A real-time tracer of IEPOX-SOA is thoroughly evaluated for the first time by combing multiple field and chamber studies. A quick and easy empirical method on IEPOX-SOA estimation is also presented.
Y. Zhao, L. Zhang, Y. Pan, Y. Wang, F. Paulot, and D. K. Henze
Atmos. Chem. Phys., 15, 10905–10924, https://doi.org/10.5194/acp-15-10905-2015, https://doi.org/10.5194/acp-15-10905-2015, 2015
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Rapid Asian industrialization has led to increased atmospheric nitrogen deposition downwind. This work analyzes the sources and processes controlling atmospheric nitrogen deposition to the northwestern Pacific. Both nitrogen emissions and meteorology, largely controlled by the East Asian Monsoon, determine the seasonality of nitrogen deposition. Ascribing deposition over the marginal seas to nitrogen sources from different regions and sectors shows important contribution from fertilizer use.
W. Tao, J. Liu, G. A. Ban-Weiss, D. A. Hauglustaine, L. Zhang, Q. Zhang, Y. Cheng, Y. Yu, and S. Tao
Atmos. Chem. Phys., 15, 8597–8614, https://doi.org/10.5194/acp-15-8597-2015, https://doi.org/10.5194/acp-15-8597-2015, 2015
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We examine the responses of a range of meteorological and air quality indicators to the expansion of urban land using WRF/Chem. Sensitivity studies indicate that the responses of pollutant concentrations to the spatial extent of urbanization are linear near the surface but nonlinear at higher altitudes. The results of process analysis demonstrate that urban heat island circulation and a deeper boundary layer with stronger turbulent intensities play a significant role in relocating pollutants.
Q. Chen, D. K. Farmer, L. V. Rizzo, T. Pauliquevis, M. Kuwata, T. G. Karl, A. Guenther, J. D. Allan, H. Coe, M. O. Andreae, U. Pöschl, J. L. Jimenez, P. Artaxo, and S. T. Martin
Atmos. Chem. Phys., 15, 3687–3701, https://doi.org/10.5194/acp-15-3687-2015, https://doi.org/10.5194/acp-15-3687-2015, 2015
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Submicron particle mass concentration in the Amazon during the wet season of 2008 was dominated by organic material. The PMF analysis finds a comparable importance of gas-phase (gas-to-particle condensation) and particle-phase (reactive uptake of isoprene oxidation products, especially of epoxydiols to acidic haze, fog, or cloud droplets) production of secondary organic material during the study period, together accounting for >70% of the organic-particle mass concentration.
L. K. Berg, M. Shrivastava, R. C. Easter, J. D. Fast, E. G. Chapman, Y. Liu, and R. A. Ferrare
Geosci. Model Dev., 8, 409–429, https://doi.org/10.5194/gmd-8-409-2015, https://doi.org/10.5194/gmd-8-409-2015, 2015
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This work presents a new methodology for representing regional-scale impacts of cloud processing on both aerosol and trace gases in sub-grid-scale convective clouds. Using the new methodology, we can better simulate the aerosol lifecycle over large areas. The results presented in this work highlight the potential change in column-integrated amounts of black carbon, organic aerosol, and sulfate aerosol, which were found to range from -50% for black carbon to +40% for sulfate.
M. R. Canagaratna, J. L. Jimenez, J. H. Kroll, Q. Chen, S. H. Kessler, P. Massoli, L. Hildebrandt Ruiz, E. Fortner, L. R. Williams, K. R. Wilson, J. D. Surratt, N. M. Donahue, J. T. Jayne, and D. R. Worsnop
Atmos. Chem. Phys., 15, 253–272, https://doi.org/10.5194/acp-15-253-2015, https://doi.org/10.5194/acp-15-253-2015, 2015
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Atomic oxygen-to-carbon (O:C), hydrogen-to-carbon (H:C), and organic mass-to-organic carbon (OM:OC) ratios of ambient organic aerosol (OA) species provide key constraints for understanding their sources and impacts. Here an improved method for obtaining accurate O:C, H:C, and OM:OC with a widely used aerosol mass spectrometer is developed. These results imply that OA is more oxidized than previously estimated and indicate the need for new chemical mechanisms that simulate ambient oxidation.
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.
J. D. Fast, J. Allan, R. Bahreini, J. Craven, L. Emmons, R. Ferrare, P. L. Hayes, A. Hodzic, J. Holloway, C. Hostetler, J. L. Jimenez, H. Jonsson, S. Liu, Y. Liu, A. Metcalf, A. Middlebrook, J. Nowak, M. Pekour, A. Perring, L. Russell, A. Sedlacek, J. Seinfeld, A. Setyan, J. Shilling, M. Shrivastava, S. Springston, C. Song, R. Subramanian, J. W. Taylor, V. Vinoj, Q. Yang, R. A. Zaveri, and Q. Zhang
Atmos. Chem. Phys., 14, 10013–10060, https://doi.org/10.5194/acp-14-10013-2014, https://doi.org/10.5194/acp-14-10013-2014, 2014
L. Zhang, D. J. Jacob, X. Yue, N. V. Downey, D. A. Wood, and D. Blewitt
Atmos. Chem. Phys., 14, 5295–5309, https://doi.org/10.5194/acp-14-5295-2014, https://doi.org/10.5194/acp-14-5295-2014, 2014
G. C. M. Vinken, K. F. Boersma, A. van Donkelaar, and L. Zhang
Atmos. Chem. Phys., 14, 1353–1369, https://doi.org/10.5194/acp-14-1353-2014, https://doi.org/10.5194/acp-14-1353-2014, 2014
R. A. Ellis, D. J. Jacob, M. P. Sulprizio, L. Zhang, C. D. Holmes, B. A. Schichtel, T. Blett, E. Porter, L. H. Pardo, and J. A. Lynch
Atmos. Chem. Phys., 13, 9083–9095, https://doi.org/10.5194/acp-13-9083-2013, https://doi.org/10.5194/acp-13-9083-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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
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
Effect of dust on rainfall over the Red Sea coast based on WRF-Chem model simulations
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
A new assessment of global and regional budgets, fluxes and lifetimes of atmospheric reactive N and S gases and aerosols
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
Modelling changes in secondary inorganic aerosol formation and nitrogen deposition in Europe from 2005 to 2030
Extension of the AIOMFAC model by iodine and carbonate species: applications for aerosol acidity and cloud droplet activation
A numerical framework for simulating the atmospheric variability of supermicron marine biogenic ice nucleating particles
Prediction of secondary organic aerosol from the multiphase reaction of gasoline vapor by using volatility–reactivity base lumping
Secondary Organic Aerosol Formation via Multiphase Reaction of Hydrocarbons in Urban Atmospheres Using the CAMx Model Integrated with the UNIPAR model
Modelling the gas–particle partitioning and water uptake of isoprene-derived secondary organic aerosol at high and low relative humidity
Contrasting source contributions of Arctic black carbon to atmospheric concentrations, deposition flux, and atmospheric and snow radiative effects
Modeling secondary organic aerosol formation from volatile chemical products
Why is the city's responsibility for its air pollution often underestimated? A focus on PM2.5
Quantifying the structural uncertainty of the aerosol mixing state representation in a modal model
Changes in PM2.5 concentrations and their sources in the US from 1990 to 2010
A predictive thermodynamic framework of cloud droplet activation for chemically unresolved aerosol mixtures, including surface tension, non-ideality, and bulk–surface partitioning
Impacts of emission changes in China from 2010 to 2017 on domestic and intercontinental air quality and health effect
Exploring the sensitivity of atmospheric nitrate concentrations to nitric acid uptake rate using the Met Office's Unified Model
Improving the representation of HONO chemistry in CMAQ and examining its impact on haze over China
How alkaline compounds control atmospheric aerosol particle acidity
Aerosol transport pathways and source attribution in China during the COVID-19 outbreak
Nonlinear responses of particulate nitrate to NOx emission controls in the megalopolises of China
Insight into PM2.5 sources by applying positive matrix factorization (PMF) at urban and rural sites of Beijing
Evaluation and intercomparison of wildfire smoke forecasts from multiple modeling systems for the 2019 Williams Flats fire
A comprehensive observation-based multiphase chemical model analysis of sulfur dioxide oxidations in both summer and winter
Predicting gas–particle partitioning coefficients of atmospheric molecules with machine learning
Development of a new emission reallocation method for industrial sources in China
Projections of shipping emissions and the related impact on air pollution and human health in the Nordic region
A predictive model for salt nanoparticle formation using heterodimer stability calculations
Using GECKO-A to derive mechanistic understanding of secondary organic aerosol formation from the ubiquitous but understudied camphene
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.
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.
Sagar Prasad Parajuli, Georgiy L. Stenchikov, Alexander Ukhov, Suleiman Mostamandi, Paul A. Kucera, Duncan Axisa, William I. Gustafson Jr., and Yannian Zhu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-164, https://doi.org/10.5194/acp-2022-164, 2022
Revised manuscript accepted for ACP
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Rainfall affects the distribution of surface and ground water resources, which are constantly declining over the Middle East and North Africa (MENA) region 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 more positive fundamental role of dust particles in modulating rainfall formation and distribution.
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.
Yao Ge, Massimo Vieno, David Stevenson, Peter Wind, and Mathew Heal
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-82, https://doi.org/10.5194/acp-2022-82, 2022
Revised manuscript accepted for ACP
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Reactive N and S gases and particle are critical determinants of air quality. We reports a comprehensive analysis of the concentrations, wet and dry deposition, fluxes and lifetimes of these species globally, and 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.
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.
Jan Eiof Jonson, Hilde Fagerli, Thomas Scheuschner, and Svetlana Tsyro
Atmos. Chem. Phys., 22, 1311–1331, https://doi.org/10.5194/acp-22-1311-2022, https://doi.org/10.5194/acp-22-1311-2022, 2022
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Ammonia emissions are expected to decrease less than SOx and NOx emissions between 2005 and 2030. As the formation of PM2.5 particles from ammonia depends on the ratio between ammonia on one hand and sulfate (from SOx) and HNO3 (from NOx) on the other hand, the efficiency of particle formation from ammonia is decreasing. Depositions of reduced nitrogen are decreasing much less than oxidized nitrogen. The critical loads for nitrogen deposition will also be exceeded in much of Europe in 2030.
Hang Yin, Jing Dou, Liviana Klein, Ulrich K. Krieger, Alison Bain, Brandon J. Wallace, Thomas C. Preston, and Andreas Zuend
Atmos. Chem. Phys., 22, 973–1013, https://doi.org/10.5194/acp-22-973-2022, https://doi.org/10.5194/acp-22-973-2022, 2022
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Iodine and carbonate species are important components in marine and dust aerosols, respectively. We introduce an extended version of the AIOMFAC thermodynamic mixing model, which includes the ions I−, IO3−, HCO3−, CO32−, OH−, and CO2(aq) as new species, and we discuss two methods for solving the carbonate dissociation equilibria numerically. We also present new experimental water activity data for aqueous iodide and iodate systems.
Isabelle Steinke, Paul J. DeMott, Grant B. Deane, Thomas C. J. Hill, Mathew Maltrud, Aishwarya Raman, and Susannah M. Burrows
Atmos. Chem. Phys., 22, 847–859, https://doi.org/10.5194/acp-22-847-2022, https://doi.org/10.5194/acp-22-847-2022, 2022
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Over the oceans, sea spray aerosol is an important source of particles that may initiate the formation of cloud ice, which then has implications for the radiative properties of marine clouds. In our study, we focus on marine biogenic particles that are emitted episodically and develop a numerical framework to describe these emissions. We find that further cloud-resolving model studies and targeted observations are needed to fully understand the climate impacts from marine biogenic particles.
Sanghee Han and Myoseon Jang
Atmos. Chem. Phys., 22, 625–639, https://doi.org/10.5194/acp-22-625-2022, https://doi.org/10.5194/acp-22-625-2022, 2022
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The gasoline SOA formation potential was simulated by using the UNIPAR model coupled with CB6r3 mechanism under varying NOx levels, aerosol acidity, humidity, temperature, and concentrations of aqueous salts and gasoline vapor. The model predicts SOA formation via multiphase reactions in the absence of wall bias. The simulation shows that both heterogeneous reactions in the aqueous phase and the implementation of model parameters corrected for GWP are critical to accurately predict SOA mass.
Zechen Yu, Myoseon Jang, Soontae Kim, Kyuwon Son, Sanghee Han, Azad Madhu, and Jinsoo Park
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-1002, https://doi.org/10.5194/acp-2021-1002, 2022
Revised manuscript accepted for ACP
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The UNIPAR model was incorporated with the CAMx model to predict the ambient concentration of organic matter in urban atmospheres during the KORUS-AQ campaign. The CAMx-UNIPAR model 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.
Dalrin Ampritta Amaladhasan, Claudia Heyn, Christopher R. Hoyle, Imad El Haddad, Miriam Elser, Simone M. Pieber, Jay G. Slowik, Antonio Amorim, Jonathan Duplissy, Sebastian Ehrhart, Vladimir Makhmutov, Ugo Molteni, Matti Rissanen, Yuri Stozhkov, Robert Wagner, Armin Hansel, Jasper Kirkby, Neil M. Donahue, Rainer Volkamer, Urs Baltensperger, Martin Gysel-Beer, and Andreas Zuend
Atmos. Chem. Phys., 22, 215–244, https://doi.org/10.5194/acp-22-215-2022, https://doi.org/10.5194/acp-22-215-2022, 2022
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We use a combination of models for gas-phase chemical reactions and equilibrium gas–particle partitioning of isoprene-derived secondary organic aerosols (SOAs) informed by dark ozonolysis experiments conducted in the CLOUD chamber. Our predictions cover high to low relative humidities (RHs) and quantify how SOA mass yields are enhanced at high RH as well as the impact of inorganic seeds of distinct hygroscopicities and acidities on the coupled partitioning of water and semi-volatile organics.
Hitoshi Matsui, Tatsuhiro Mori, Sho Ohata, Nobuhiro Moteki, Naga Oshima, Kumiko Goto-Azuma, Makoto Koike, and Yutaka Kondo
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-1091, https://doi.org/10.5194/acp-2021-1091, 2022
Revised manuscript accepted for ACP
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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.
Elyse A. Pennington, Karl M. Seltzer, Benjamin N. Murphy, Momei Qin, John H. Seinfeld, and Havala O. T. Pye
Atmos. Chem. Phys., 21, 18247–18261, https://doi.org/10.5194/acp-21-18247-2021, https://doi.org/10.5194/acp-21-18247-2021, 2021
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Volatile chemical products (VCPs) are commonly used consumer and industrial items that contribute to the formation of atmospheric aerosol. We implemented the emissions and chemistry of VCPs in a regional-scale model and compared predictions with measurements made in Los Angeles. Our results reduced model bias and suggest that VCPs may contribute up to half of anthropogenic secondary organic aerosol in Los Angeles and are an important source of human-influenced particular matter in urban areas.
Philippe Thunis, Alain Clappier, Alexander de Meij, Enrico Pisoni, Bertrand Bessagnet, and Leonor Tarrason
Atmos. Chem. Phys., 21, 18195–18212, https://doi.org/10.5194/acp-21-18195-2021, https://doi.org/10.5194/acp-21-18195-2021, 2021
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Air pollution's origin in cities is still a point of discussion, and approaches to assess the city's responsibility for its pollution are not harmonized and thus not comparable, resulting in sometimes contradicting interpretations. We show that methodological choices can easily lead to differences of a factor of 2 in terms of responsibility outcome and stress that methodological choices and assumptions most often lead to a systematic and important underestimation of the city's responsibility.
Zhonghua Zheng, Matthew West, Lei Zhao, Po-Lun Ma, Xiaohong Liu, and Nicole Riemer
Atmos. Chem. Phys., 21, 17727–17741, https://doi.org/10.5194/acp-21-17727-2021, https://doi.org/10.5194/acp-21-17727-2021, 2021
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Aerosol mixing state is an important emergent property that affects aerosol radiative forcing and aerosol–cloud interactions, but it has not been easy to constrain this property globally. We present a framework for evaluating the error in aerosol mixing state induced by aerosol representation assumptions, which is one of the important contributors to structural uncertainty in aerosol models. Our study provides insights into potential improvements to model process representation for aerosols.
Ksakousti Skyllakou, Pablo Garcia Rivera, Brian Dinkelacker, Eleni Karnezi, Ioannis Kioutsioukis, Carlos Hernandez, Peter J. Adams, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 17115–17132, https://doi.org/10.5194/acp-21-17115-2021, https://doi.org/10.5194/acp-21-17115-2021, 2021
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Significant reductions in pollutant emissions took place in the US from 1990 to 2010. The reductions in sulfur dioxide emissions from electric-generating units have dominated the reductions in fine particle mass. The reductions in transportation emissions have led to a 30 % reduction of elemental concentrations and of organic particulate matter by a factor of 3. On the other hand, changes in biomass burning and biogenic secondary organic aerosol have been modest.
Nønne L. Prisle
Atmos. Chem. Phys., 21, 16387–16411, https://doi.org/10.5194/acp-21-16387-2021, https://doi.org/10.5194/acp-21-16387-2021, 2021
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A mass-based Gibbs adsorption model is presented to enable predictive Köhler calculations of droplet growth and activation with considerations of surface partitioning, surface tension, and non-ideal water activity for chemically complex and unresolved surface active aerosol mixtures, including actual atmospheric samples. The model is used to calculate cloud condensation nuclei (CCN) activity of aerosol particles comprising strongly surface-active model atmospheric humic-like substances (HULIS).
Yuqiang Zhang, Drew Shindell, Karl Seltzer, Lu Shen, Jean-Francois Lamarque, Qiang Zhang, Bo Zheng, Jia Xing, Zhe Jiang, and Lei Zhang
Atmos. Chem. Phys., 21, 16051–16065, https://doi.org/10.5194/acp-21-16051-2021, https://doi.org/10.5194/acp-21-16051-2021, 2021
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In this study, we use a global chemical transport model to simulate the effects on global air quality and human health due to emission changes in China from 2010 to 2017. By performing sensitivity analysis, we found that the air pollution control policies not only decrease the air pollutant concentration but also bring significant co-benefits in air quality to downwind regions. The benefits for the improved air pollution are dominated by PM2.5.
Anthony C. Jones, Adrian Hill, Samuel Remy, N. Luke Abraham, Mohit Dalvi, Catherine Hardacre, Alan J. Hewitt, Ben Johnson, Jane P. Mulcahy, and Steven T. Turnock
Atmos. Chem. Phys., 21, 15901–15927, https://doi.org/10.5194/acp-21-15901-2021, https://doi.org/10.5194/acp-21-15901-2021, 2021
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Ammonium nitrate is hard to model because it forms and evaporates rapidly. One approach is to relate its equilibrium concentration to temperature, humidity, and the amount of nitric acid and ammonia gases. Using this approach, we limit the rate at which equilibrium is reached using various condensation rates in a climate model. We show that ammonium nitrate concentrations are highly sensitive to the condensation rate. Our results will help improve the representation of nitrate in climate models.
Shuping Zhang, Golam Sarwar, Jia Xing, Biwu Chu, Chaoyang Xue, Arunachalam Sarav, Dian Ding, Haotian Zheng, Yujing Mu, Fengkui Duan, Tao Ma, and Hong He
Atmos. Chem. Phys., 21, 15809–15826, https://doi.org/10.5194/acp-21-15809-2021, https://doi.org/10.5194/acp-21-15809-2021, 2021
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Six heterogeneous HONO chemistry updates in CMAQ significantly improve HONO concentration. HONO production is primarily controlled by the heterogeneous reactions on ground and aerosol surfaces during haze. Additional HONO chemistry updates increase OH and production of secondary aerosols: sulfate, nitrate, and SOA.
Vlassis A. Karydis, Alexandra P. Tsimpidi, Andrea Pozzer, and Jos Lelieveld
Atmos. Chem. Phys., 21, 14983–15001, https://doi.org/10.5194/acp-21-14983-2021, https://doi.org/10.5194/acp-21-14983-2021, 2021
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Aerosol particle pH is well-buffered by alkaline compounds, notably NH3 and crustal elements. NH3 is found to supply remarkable buffering capacity on a global scale, from the polluted continents to the remote oceans. Potential future changes in agricultural NH3 must be accompanied by strong reductions of SO2 and NOx to avoid particles becoming highly acidic, with implications for human health (aerosol toxicity), ecosystems (acid deposition), clouds, and climate (aerosol hygroscopicity).
Lili Ren, Yang Yang, Hailong Wang, Pinya Wang, Lei Chen, Jia Zhu, and Hong Liao
Atmos. Chem. Phys., 21, 15431–15445, https://doi.org/10.5194/acp-21-15431-2021, https://doi.org/10.5194/acp-21-15431-2021, 2021
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Due to the COVID-19 pandemic, human activities were strictly restricted in China. Even though anthropogenic aerosol emissions largely decreased, haze events still occurred. Our results shows that PM2.5 over the North China Plain is largely contributed by local sources. For other regions in China, PM2.5 is largely contributed from nonlocal sources. As emission reduction is a future goal, aerosol long-range transport and unfavorable meteorology are increasingly important to air quality.
Mengmeng Li, Zihan Zhang, Quan Yao, Tijian Wang, Min Xie, Shu Li, Bingliang Zhuang, and Yong Han
Atmos. Chem. Phys., 21, 15135–15152, https://doi.org/10.5194/acp-21-15135-2021, https://doi.org/10.5194/acp-21-15135-2021, 2021
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We establish the nonlinear responses between nitrate and NOx in China. Reduction of NOx results in linearly lower nitrate in summer–autumn whereas an increase of winter nitrate until an inflexion point at 40–50 % reduction due to the excess oxidants. NH3 and VOCs are effective in controlling nitrate pollution, whereas decreasing the SO2 and NOx emissions may have counterintuitive effects on nitrate aerosols. This paper helps understand the nonlinear aerosol and photochemistry feedback.
Deepchandra Srivastava, Jingsha Xu, Tuan V. Vu, Di Liu, Linjie Li, Pingqing Fu, Siqi Hou, Natalia Moreno Palmerola, Zongbo Shi, and Roy M. Harrison
Atmos. Chem. Phys., 21, 14703–14724, https://doi.org/10.5194/acp-21-14703-2021, https://doi.org/10.5194/acp-21-14703-2021, 2021
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This study presents the source apportionment of PM2.5 performed by positive matrix factorization (PMF) at urban and rural sites in Beijing. These factors are interpreted as traffic emissions, biomass burning, road and soil dust, coal and oil combustion, and secondary inorganics. PMF failed to resolve some sources identified by CMB and AMS and appears to overestimate the dust sources. Comparison with earlier PMF studies from the Beijing area highlights inconsistent findings using this method.
Xinxin Ye, Pargoal Arab, Ravan Ahmadov, Eric James, Georg A. Grell, Bradley Pierce, Aditya Kumar, Paul Makar, Jack Chen, Didier Davignon, Greg R. Carmichael, Gonzalo Ferrada, Jeff McQueen, Jianping Huang, Rajesh Kumar, Louisa Emmons, Farren L. Herron-Thorpe, Mark Parrington, Richard Engelen, Vincent-Henri Peuch, Arlindo da Silva, Amber Soja, Emily Gargulinski, Elizabeth Wiggins, Johnathan W. Hair, Marta Fenn, Taylor Shingler, Shobha Kondragunta, Alexei Lyapustin, Yujie Wang, Brent Holben, David M. Giles, and Pablo E. Saide
Atmos. Chem. Phys., 21, 14427–14469, https://doi.org/10.5194/acp-21-14427-2021, https://doi.org/10.5194/acp-21-14427-2021, 2021
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Wildfire smoke has crucial impacts on air quality, while uncertainties in the numerical forecasts remain significant. We present an evaluation of 12 real-time forecasting systems. Comparison of predicted smoke emissions suggests a large spread in magnitudes, with temporal patterns deviating from satellite detections. The performance for AOD and surface PM2.5 and their discrepancies highlighted the role of accurately represented spatiotemporal emission profiles in improving smoke forecasts.
Huan Song, Keding Lu, Can Ye, Huabin Dong, Shule Li, Shiyi Chen, Zhijun Wu, Mei Zheng, Limin Zeng, Min Hu, and Yuanhang Zhang
Atmos. Chem. Phys., 21, 13713–13727, https://doi.org/10.5194/acp-21-13713-2021, https://doi.org/10.5194/acp-21-13713-2021, 2021
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Secondary sulfate aerosols are an important component of fine particles in severe air pollution events. We calculated the sulfate formation rates via a state-of-the-art multiphase model constrained to the observed values. We showed that transition metals in urban aerosols contribute significantly to sulfate formation during haze periods and thus play an important role in mitigation strategies and public health measures in megacities worldwide.
Emma Lumiaro, Milica Todorović, Theo Kurten, Hanna Vehkamäki, and Patrick Rinke
Atmos. Chem. Phys., 21, 13227–13246, https://doi.org/10.5194/acp-21-13227-2021, https://doi.org/10.5194/acp-21-13227-2021, 2021
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The study of climate change relies on climate models, which require an understanding of aerosol formation. We train a machine-learning model to predict the partitioning coefficients of atmospheric molecules, which govern condensation into aerosols. The model can make instant predictions based on molecular structures with accuracy surpassing that of standard computational methods. This will allow the screening of low-volatility molecules that contribute most to aerosol formation.
Yun Fat Lam, Chi Chiu Cheung, Xuguo Zhang, Joshua S. Fu, and Jimmy Chi Hung Fung
Atmos. Chem. Phys., 21, 12895–12908, https://doi.org/10.5194/acp-21-12895-2021, https://doi.org/10.5194/acp-21-12895-2021, 2021
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In recent years, air pollution forecasting has become an important municipal service of the government. In this study, a new spatial allocation method based on satellite remote sensing and GIS techniques was developed to address the spatial deficiency of industrial source emissions in China, providing a substantial improvement on NO2 and PM2.5 forecast for the Pearl River Delta/Greater Bay Area.
Camilla Geels, Morten Winther, Camilla Andersson, Jukka-Pekka Jalkanen, Jørgen Brandt, Lise M. Frohn, Ulas Im, Wing Leung, and Jesper H. Christensen
Atmos. Chem. Phys., 21, 12495–12519, https://doi.org/10.5194/acp-21-12495-2021, https://doi.org/10.5194/acp-21-12495-2021, 2021
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In this study, we set up new shipping emissions scenarios and use two chemistry transport models and a health assessment model to assess the development of air quality and related health impacts in the Nordic region. Shipping alone is associated with about 850 premature deaths during present-day conditions, decreasing to approximately 550–600 cases in the 2050 scenarios.
Sabrina Chee, Kelley Barsanti, James N. Smith, and Nanna Myllys
Atmos. Chem. Phys., 21, 11637–11654, https://doi.org/10.5194/acp-21-11637-2021, https://doi.org/10.5194/acp-21-11637-2021, 2021
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We explored molecular properties affecting atmospheric particle formation efficiency and derived a parameterization between particle formation rate and heterodimer concentration, which showed good agreement to previously reported experimental data. Considering the simplicity of calculating heterodimer concentration, this approach has potential to improve estimates of global cloud condensation nuclei in models that are limited by the computational expense of calculating particle formation rate.
Isaac Kwadjo Afreh, Bernard Aumont, Marie Camredon, and Kelley Claire Barsanti
Atmos. Chem. Phys., 21, 11467–11487, https://doi.org/10.5194/acp-21-11467-2021, https://doi.org/10.5194/acp-21-11467-2021, 2021
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This is the first mechanistic modeling study of secondary organic aerosol (SOA) from the understudied monoterpene, camphene. The semi-explicit chemical model GECKO-A predicted camphene SOA yields that were ~2 times α-pinene. Using 50/50 α-pinene + limonene as a surrogate for camphene increased predicted SOA mass from biomass burning fuels by up to ~100 %. The accurate representation of camphene in air quality models can improve predictions of SOA when camphene is a dominant monoterpene.
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Gaubert, B., Emmons, L. K., Raeder, K., Tilmes, S., Miyazaki, K., Arellano Jr., A. F., Elguindi, N., Granier, C., Tang, W., Barré, J., Worden, H. M., Buchholz, R. R., Edwards, D. P., Franke, P., Anderson, J. L., Saunois, M., Schroeder, J., Woo, J.-H., Simpson, I. J., Blake, D. R., Meinardi, S., Wennberg, P. O., Crounse, J., Teng, A., Kim, M., Dickerson, R. R., He, H., Ren, X., Pusede, S. E., and Diskin, G. S.: Correcting model biases of CO in East Asia: impact on oxidant distributions during KORUS-AQ, Atmos. Chem. Phys., 20, 14617–14647, https://doi.org/10.5194/acp-20-14617-2020, 2020.
Geng, G., Zheng, Y., Zhang, Q., Xue, T., Zhao, H., Tong, D., Zheng, B., Li, M., Liu, F., Hong, C., He, K., and Davis, S.:
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Kasibhatla, P., Sherwen, T., Evans, M. J., Carpenter, L. J., Reed, C., Alexander, B., Chen, Q., Sulprizio, M. P., Lee, J. D., Read, K. A., Bloss, W., Crilley, L. R., Keene, W. C., Pszenny, A. A. P., and Hodzic, A.: Global impact of nitrate photolysis in sea-salt aerosol on NOx, OH, and O3 in the marine boundary layer, Atmos. Chem. Phys., 18, 11185–11203, https://doi.org/10.5194/acp-18-11185-2018, 2018.
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1.5-Dimensional volatility basis set approach for modeling organic aerosol in CAMx and CMAQ,
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Short summary
We apply process-based and observation-constrained schemes to simulate organic aerosol in China and conduct comprehensive model–observation comparisons. The results show that anthropogenic semivolatile and intermediate-volatility organic compounds (SVOCs and IVOCs) are the main sources of secondary organic aerosol (SOA) in polluted regions, for which the residential sector is perhaps the predominant contributor. The hydroxyl radical level is also important for SOA modeling in polluted regions.
We apply process-based and observation-constrained schemes to simulate organic aerosol in China...
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