Articles | Volume 21, issue 21
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.
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.
Process-based and observation-constrained SOA simulations in China: the role of semivolatile and intermediate-volatility organic compounds and OH levels
Ruqian Miao
State Key Joint Laboratory of Environmental Simulation and Pollution Control, BIC-ESAT and IJRC, College of Environmental Sciences and Engineering, Peking University, Beijing, 100871, China
State Key Joint Laboratory of Environmental Simulation and Pollution Control, BIC-ESAT and IJRC, College of Environmental Sciences and Engineering, Peking University, Beijing, 100871, China
Manish Shrivastava
Pacific Northwest National Laboratory, Richland, Washington 99352, USA
Youfan Chen
Sichuan Academy of Environmental Policy and Planning, Chengdu, Sichuan, 610041, China
Lin Zhang
Laboratory for Climate and Ocean–Atmosphere Studies, Department of Atmospheric and Oceanic Sciences, School of Physics, Peking University, Beijing, 100871, China
Jianlin Hu
Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control, Jiangsu Engineering Technology Research Center of Environmental Cleaning Materials, Collaborative Innovation Center of Atmospheric Environment and Equipment Technology, School of Environmental Science and Engineering, Nanjing University of Information Science and Technology, Nanjing, Jiangsu, 210044, China
Yan Zheng
State Key Joint Laboratory of Environmental Simulation and Pollution Control, BIC-ESAT and IJRC, College of Environmental Sciences and Engineering, Peking University, Beijing, 100871, China
Keren Liao
State Key Joint Laboratory of Environmental Simulation and Pollution Control, BIC-ESAT and IJRC, College of Environmental Sciences and Engineering, Peking University, Beijing, 100871, China
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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.
Xu Feng, Haipeng Lin, Tzung-May Fu, Melissa P. Sulprizio, Jiawei Zhuang, Daniel J. Jacob, Heng Tian, Yaping Ma, Lijuan Zhang, Xiaolin Wang, Qi Chen, and Zhiwei Han
Geosci. Model Dev., 14, 3741–3768, https://doi.org/10.5194/gmd-14-3741-2021, https://doi.org/10.5194/gmd-14-3741-2021, 2021
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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.
Yaman Liu, Xinyi Dong, Minghuai Wang, Louisa K. Emmons, Yawen Liu, Yuan Liang, Xiao Li, and Manish Shrivastava
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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Secondary organic aerosol (SOA) is considered one of the most important uncertainties in climate modeling. We evaluate SOA performance in the Community Earth System Model version 2.1 (CESM2.1) configured with the Community Atmosphere Model version 6 with chemistry (CAM6-Chem) through a long-term simulation (1988–2019) with observations in the United States, which indicates monoterpene-formed SOA contributes most to the overestimation of SOA at the surface and underestimation in the upper air.
Youwen Sun, Hao Yin, Cheng Liu, Lin Zhang, Yuan Cheng, Mathias Palm, Justus Notholt, Xiao Lu, Corinne Vigouroux, Bo Zheng, Wei Wang, Nicholas Jones, Changong Shan, Min Qin, Yuan Tian, Qihou Hu, Fanhao Meng, and Jianguo Liu
Atmos. Chem. Phys., 21, 6365–6387, https://doi.org/10.5194/acp-21-6365-2021, https://doi.org/10.5194/acp-21-6365-2021, 2021
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This study mapped the drivers of HCHO variability from 2015 to 2019 over eastern China. Hydroxyl (OH) radical production rates from HCHO photolysis were evaluated. The relative contributions of emitted and photochemical sources to the observed HCHO abundance were analyzed. Contributions of various emission sources and geographical regions to the observed HCHO summertime enhancements were determined.
Mengdi Song, Xin Li, Suding Yang, Xuena Yu, Songxiu Zhou, Yiming Yang, Shiyi Chen, Huabin Dong, Keren Liao, Qi Chen, Keding Lu, Ningning Zhang, Junji Cao, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 21, 4939–4958, https://doi.org/10.5194/acp-21-4939-2021, https://doi.org/10.5194/acp-21-4939-2021, 2021
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Due to their lower diffusion capacities and higher conversion capacities, urban areas in Xi’an experienced severe ozone pollution in the summer. In this study, a campaign of comprehensive field observations and VOC grid sampling was conducted in Xi’an from 20 June to 20 July 2019. We found that Xi'an has a strong local emission source of VOCs, and vehicle exhaust was the primary VOC source. In addition, alkenes, aromatics, and oxygenated VOCs played a dominant role in secondary transformations.
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
Zhongjing Jiang, Jing Li, Xiao Lu, Cheng Gong, Lin Zhang, and Hong Liao
Atmos. Chem. Phys., 21, 2601–2613, https://doi.org/10.5194/acp-21-2601-2021, https://doi.org/10.5194/acp-21-2601-2021, 2021
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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 %.
Zhihao Shi, Lin Huang, Jingyi Li, Qi Ying, Hongliang Zhang, and Jianlin Hu
Atmos. Chem. Phys., 20, 13455–13466, https://doi.org/10.5194/acp-20-13455-2020, https://doi.org/10.5194/acp-20-13455-2020, 2020
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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.
Cited articles
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A technology-based global inventory of black and organic carbon emissions from combustion,
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CO Emissions Inferred From Surface CO Observations Over China in December 2013 and 2017,
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125, e2019JD031808, https://doi.org/10.1029/2019JD031808, 2020.
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Fisher, J. A., Jacob, D. J., Travis, K. R., Kim, P. S., Marais, E. A., Chan Miller, C., Yu, K., Zhu, L., Yantosca, R. M., Sulprizio, M. P., Mao, J., Wennberg, P. O., Crounse, J. D., Teng, A. P., Nguyen, T. B., St. Clair, J. M., Cohen, R. C., Romer, P., Nault, B. A., Wooldridge, P. J., Jimenez, J. L., Campuzano-Jost, P., Day, D. A., Hu, W., Shepson, P. B., Xiong, F., Blake, D. R., Goldstein, A. H., Misztal, P. K., Hanisco, T. F., Wolfe, G. M., Ryerson, T. B., Wisthaler, A., and Mikoviny, T.: Organic nitrate chemistry and its implications for nitrogen budgets in an isoprene- and monoterpene-rich atmosphere: constraints from aircraft (SEAC4RS) and ground-based (SOAS) observations in the Southeast US, Atmos. Chem. Phys., 16, 5969–5991, https://doi.org/10.5194/acp-16-5969-2016, 2016.
Fountoukis, C. and Nenes, A.: ISORROPIA II: a computationally efficient thermodynamic equilibrium model for K+–Ca2+–Mg2+– –Na+– – –Cl−–H2O aerosols, Atmos. Chem. Phys., 7, 4639–4659, https://doi.org/10.5194/acp-7-4639-2007, 2007.
Gani, S., Bhandari, S., Seraj, S., Wang, D. S., Patel, K., Soni, P., Arub, Z., Habib, G., Hildebrandt Ruiz, L., and Apte, J. S.: Submicron aerosol composition in the world's most polluted megacity: the Delhi Aerosol Supersite study, Atmos. Chem. Phys., 19, 6843–6859, https://doi.org/10.5194/acp-19-6843-2019, 2019.
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.:
Drivers of PM2.5 air pollution deaths in China 2002-2017,
Nat. Geosci.,
14, 645–650, https://doi.org/10.1038/s41561-021-00792-3, 2021.
Giglio, L., Randerson, J. T., and van der Werf, G. R.:
Analysis of daily, monthly, and annual burned area using the fourth-generation global fire emissions database (GFED4),
J. Geophys. Res.-Biogeo.,
118, 317–328, https://doi.org/10.1002/jgrg.20042, 2013.
Gkatzelis, G. I., Papanastasiou, D. K., Karydis, V. A., Hohaus, T., Liu, Y., Schmitt, S. H., Schlag, P., Fuchs, H., Novelli, A., Chen, Q., Cheng, X., Broch, S., Dong, H., Holland, F., Li, X., Liu, Y., Ma, X., Reimer, D., Rohrer, F., Shao, M., Tan, Z., Taraborrelli, D., Tillmann, R., Wang, H., Wang, Y., Wu, Y., Wu, Z., Zeng, L., Zheng, J., Hu, M., Lu, K., Hofzumahaus, A., Zhang, Y., Wahner, A., and Kiendler-Scharr, A.:
Uptake of Water-soluble Gas-phase Oxidation Products Drives Organic Particulate Pollution in Beijing,
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48, e2020GL091351, https://doi.org/10.1029/2020GL091351, 2021.
Grieshop, A. P., Logue, J. M., Donahue, N. M., and Robinson, A. L.: Laboratory investigation of photochemical oxidation of organic aerosol from wood fires 1: measurement and simulation of organic aerosol evolution, Atmos. Chem. Phys., 9, 1263–1277, https://doi.org/10.5194/acp-9-1263-2009, 2009.
Guenther, A. B., Jiang, X., Heald, C. L., Sakulyanontvittaya, T., Duhl, T., Emmons, L. K., and Wang, X.: The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1): an extended and updated framework for modeling biogenic emissions, Geosci. Model Dev., 5, 1471–1492, https://doi.org/10.5194/gmd-5-1471-2012, 2012.
Han, C., Yang, W., Wu, Q., Yang, H., and Xue, X.:
Heterogeneous Photochemical Conversion of NO2 to HONO on the Humic Acid Surface under Simulated Sunlight,
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Modeling organic aerosols over east China using a volatility basis-set approach with aging mechanism in a regional air quality model,
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Hayes, P. L., Ortega, A. M., Cubison, M. J., Froyd, K. D., Zhao, Y., Cliff, S. S., Hu, W. W., Toohey, D. W., Flynn, J. H., Lefer, B. L., Grossberg, N., Alvarez, S., Rappenglück, B., Taylor, J. W., Allan, J. D., Holloway, J. S., Gilman, J. B., Kuster, W. C., de Gouw, J. A., Massoli, P., Zhang, X., Liu, J., Weber, R. J., Corrigan, A. L., Russell, L. M., Isaacman, G., Worton, D. R., Kreisberg, N. M., Goldstein, A. H., Thalman, R., Waxman, E. M., Volkamer, R., Lin, Y. H., Surratt, J. D., Kleindienst, T. E., Offenberg, J. H., Dusanter, S., Griffith, S., Stevens, P. S., Brioude, J., Angevine, W. M., and Jimenez, J. L.:
Organic aerosol composition and sources in Pasadena, California, during the 2010 CalNex campaign,
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Hodzic, A. and Jimenez, J. L.: Modeling anthropogenically controlled secondary organic aerosols in a megacity: a simplified framework for global and climate models, Geosci. Model Dev., 4, 901–917, https://doi.org/10.5194/gmd-4-901-2011, 2011.
Hodzic, A., Kasibhatla, P. S., Jo, D. S., Cappa, C. D., Jimenez, J. L., Madronich, S., and Park, R. J.: Rethinking the global secondary organic aerosol (SOA) budget: stronger production, faster removal, shorter lifetime, Atmos. Chem. Phys., 16, 7917–7941, https://doi.org/10.5194/acp-16-7917-2016, 2016.
Hoesly, R. M., Smith, S. J., Feng, L., Klimont, Z., Janssens-Maenhout, G., Pitkanen, T., Seibert, J. J., Vu, L., Andres, R. J., Bolt, R. M., Bond, T. C., Dawidowski, L., Kholod, N., Kurokawa, J.-I., Li, M., Liu, L., Lu, Z., Moura, M. C. P., O'Rourke, P. R., and Zhang, Q.: Historical (1750–2014) anthropogenic emissions of reactive gases and aerosols from the Community Emissions Data System (CEDS), Geosci. Model Dev., 11, 369–408, https://doi.org/10.5194/gmd-11-369-2018, 2018.
Hu, J., Wang, P., Ying, Q., Zhang, H., Chen, J., Ge, X., Li, X., Jiang, J., Wang, S., Zhang, J., Zhao, Y., and Zhang, Y.: Modeling biogenic and anthropogenic secondary organic aerosol in China, Atmos. Chem. Phys., 17, 77–92, https://doi.org/10.5194/acp-17-77-2017, 2017.
Huang, L., Wang, Q., Wang, Y., Emery, C., Zhu, A., Zhu, Y., Yin, S., Yarwood, G., Zhang, K., and Li, L.: Simulation of secondary organic aerosol over the Yangtze River Delta region: The impacts from the emissions of intermediate volatility organic compounds and the SOA modeling framework, Atmos. Environ., 246, 118079, https://doi.org/10.1016/j.atmosenv.2020.118079, 2021.
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Concentration and sources of atmospheric nitrous acid (HONO) at an urban site in Western China,
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Jathar, S. H., Farina, S. C., Robinson, A. L., and Adams, P. J.: The influence of semi-volatile and reactive primary emissions on the abundance and properties of global organic aerosol, Atmos. Chem. Phys., 11, 7727–7746, https://doi.org/10.5194/acp-11-7727-2011, 2011.
Jathar, S. H., Gordon, T. D., Hennigan, C. J., Pye, H. O., Pouliot, G., Adams, P. J., Donahue, N. M., and Robinson, A. L.:
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Jiang, J., Aksoyoglu, S., El-Haddad, I., Ciarelli, G., Denier van der Gon, H. A. C., Canonaco, F., Gilardoni, S., Paglione, M., Minguillón, M. C., Favez, O., Zhang, Y., Marchand, N., Hao, L., Virtanen, A., Florou, K., O'Dowd, C., Ovadnevaite, J., Baltensperger, U., and Prévôt, A. S. H.: Sources of organic aerosols in Europe: a modeling study using CAMx with modified volatility basis set scheme, Atmos. Chem. Phys., 19, 15247–15270, https://doi.org/10.5194/acp-19-15247-2019, 2019.
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.
Khare, P. and Gentner, D. R.: Considering the future of anthropogenic gas-phase organic compound emissions and the increasing influence of non-combustion sources on urban air quality, Atmos. Chem. Phys., 18, 5391–5413, https://doi.org/10.5194/acp-18-5391-2018, 2018.
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Kong, L., Tang, X., Zhu, J., Wang, Z., Fu, J. S., Wang, X., Itahashi, S., Yamaji, K., Nagashima, T., Lee, H.-J., Kim, C.-H., Lin, C.-Y., Chen, L., Zhang, M., Tao, Z., Li, J., Kajino, M., Liao, H., Wang, Z., Sudo, K., Wang, Y., Pan, Y., Tang, G., Li, M., Wu, Q., Ge, B., and Carmichael, G. R.: Evaluation and uncertainty investigation of the NO2, CO and NH3 modeling over China under the framework of MICS-Asia III, Atmos. Chem. Phys., 20, 181–202, https://doi.org/10.5194/acp-20-181-2020, 2020.
Koo, B., Knipping, E., and Yarwood, G.:
1.5-Dimensional volatility basis set approach for modeling organic aerosol in CAMx and CMAQ,
Atmos. Environ.,
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Photochemical Aqueous-Phase Reactions Induce Rapid Daytime Formation of Oxygenated Organic Aerosol on the North China Plain,
Environ. Sci. Technol.,
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Long-term characterization of aerosol chemistry in cold season from 2013 to 2020 in Beijing, China,
Environ. Pollut.,
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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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