Articles | Volume 24, issue 8
https://doi.org/10.5194/acp-24-4809-2024
© Author(s) 2024. 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-24-4809-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
23 Apr 2024
Research article |
| 23 Apr 2024
| 23 Apr 2024
Simulated phase state and viscosity of secondary organic aerosols over China
Zhiqiang Zhang
State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China
College of Earth and Planetary Sciences, University of Chinese Academy of Sciences, Beijing 100049, China
State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China
College of Earth and Planetary Sciences, University of Chinese Academy of Sciences, Beijing 100049, China
Haiyan Ran
State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China
College of Earth and Planetary Sciences, University of Chinese Academy of Sciences, Beijing 100049, China
Junling An
State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China
College of Earth and Planetary Sciences, University of Chinese Academy of Sciences, Beijing 100049, China
Yu Qu
State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China
College of Earth and Planetary Sciences, University of Chinese Academy of Sciences, Beijing 100049, China
State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China
Weiqi Xu
State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China
College of Earth and Planetary Sciences, University of Chinese Academy of Sciences, Beijing 100049, China
Weiwei Hu
State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China
Hongbin Xie
Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education), School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China
Zifa Wang
State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China
College of Earth and Planetary Sciences, University of Chinese Academy of Sciences, Beijing 100049, China
State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China
College of Earth and Planetary Sciences, University of Chinese Academy of Sciences, Beijing 100049, China
Manabu Shiraiwa
Department of Chemistry, University of California, Irvine, Irvine, CA 92697-2025, USA
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This study investigated the role of the secondary organic aerosol (SOA) loading on the molecular composition of wintertime urban aerosols by ultrahigh-resolution mass spectrometry. Results demonstrate that the SOA loading is an important factor associated with the oxidation degree, nitrate group content, and chemodiversity of nitrooxy–organosulfates. Our study also found that the hydrolysis of nitrooxy–organosulfates is a possible pathway for the formation of organosulfates.
Tingting Feng, Yingkun Wang, Weiwei Hu, Ming Zhu, Wei Song, Wei Chen, Yanyan Sang, Zheng Fang, Wei Deng, Hua Fang, Xu Yu, Cheng Wu, Bin Yuan, Shan Huang, Min Shao, Xiaofeng Huang, Lingyan He, Young Ro Lee, Lewis Gregory Huey, Francesco Canonaco, Andre S. H. Prevot, and Xinming Wang
Atmos. Chem. Phys., 23, 611–636, https://doi.org/10.5194/acp-23-611-2023, https://doi.org/10.5194/acp-23-611-2023, 2023
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To investigate the impact of aging processes on organic aerosols (OA), we conducted a comprehensive field study at a continental remote site using an on-line mass spectrometer. The results show that OA in the Chinese outflows were strongly influenced by upwind anthropogenic emissions. The aging processes can significantly decrease the OA volatility and result in a varied viscosity of OA under different circumstances, signifying the complex physiochemical properties of OA in aged plumes.
Meredith Schervish and Manabu Shiraiwa
Atmos. Chem. Phys., 23, 221–233, https://doi.org/10.5194/acp-23-221-2023, https://doi.org/10.5194/acp-23-221-2023, 2023
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Secondary organic aerosols (SOAs) can exhibit complex non-ideal behavior and adopt an amorphous semisolid state. We simulate condensation of semi-volatile compounds into a phase-separated particle to investigate the effect of non-ideality and particle phase state on the equilibration timescale of SOA partitioning. Our results provide useful insights into the interpretation of experimental observations and the description and treatment of SOA in aerosol models.
Haichao Wang, Bin Yuan, E Zheng, Xiaoxiao Zhang, Jie Wang, Keding Lu, Chenshuo Ye, Lei Yang, Shan Huang, Weiwei Hu, Suxia Yang, Yuwen Peng, Jipeng Qi, Sihang Wang, Xianjun He, Yubin Chen, Tiange Li, Wenjie Wang, Yibo Huangfu, Xiaobing Li, Mingfu Cai, Xuemei Wang, and Min Shao
Atmos. Chem. Phys., 22, 14837–14858, https://doi.org/10.5194/acp-22-14837-2022, https://doi.org/10.5194/acp-22-14837-2022, 2022
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We present intensive field measurement of ClNO2 in the Pearl River Delta in 2019. Large variation in the level, formation, and atmospheric impacts of ClNO2 was found in different air masses. ClNO2 formation was limited by the particulate chloride (Cl−) and aerosol surface area. Our results reveal that Cl− originated from various anthropogenic emissions rather than sea sources and show minor contribution to the O3 pollution and photochemistry.
Yuying Wang, Rong Hu, Qiuyan Wang, Zhanqing Li, Maureen Cribb, Yele Sun, Xiaorui Song, Yi Shang, Yixuan Wu, Xin Huang, and Yuxiang Wang
Atmos. Chem. Phys., 22, 14133–14146, https://doi.org/10.5194/acp-22-14133-2022, https://doi.org/10.5194/acp-22-14133-2022, 2022
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The mixing state of size-resolved soot particles and their influencing factors were investigated. The results suggest anthropogenic emissions and aging processes have diverse impacts on the mixing state of soot particles in different modes. Considering that the mixing state of soot particles is crucial to model aerosol absorption, this finding is important to study particle growth and the warming effect of black carbon aerosols.
Futing Wang, Ting Yang, Zifa Wang, Haibo Wang, Xi Chen, Yele Sun, Jianjun Li, Guigang Tang, and Wenxuan Chai
Atmos. Meas. Tech., 15, 6127–6144, https://doi.org/10.5194/amt-15-6127-2022, https://doi.org/10.5194/amt-15-6127-2022, 2022
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We develop a new algorithm to get the vertical mass concentration profiles of fine aerosol components based on the synergy of ground-based remote sensing for the first time. The comparisons with in situ observations and chemistry transport models validate the performance of the algorithm. Uncertainties caused by input parameters are also assessed in this paper. We expected that the algorithm can provide a new idea for lidar inversion and promote the development of aerosol component profiles.
Biao Luo, Ye Kuang, Shan Huang, Qicong Song, Weiwei Hu, Wei Li, Yuwen Peng, Duohong Chen, Dingli Yue, Bin Yuan, and Min Shao
Atmos. Chem. Phys., 22, 12401–12415, https://doi.org/10.5194/acp-22-12401-2022, https://doi.org/10.5194/acp-22-12401-2022, 2022
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We performed comprehensive analysis on biomass burning organic aerosol (BBOA) size distributions, as well as mass scattering and absorption efficiencies, with an improved method of on-line quantification of brown carbon absorptions. Both BBOA volume size distribution and retrieved refractive index depend highly on combustion conditions represented by the black carbon content, which has significant implications for BBOA climate effect simulations.
Chao Yan, Yicheng Shen, Dominik Stolzenburg, Lubna Dada, Ximeng Qi, Simo Hakala, Anu-Maija Sundström, Yishuo Guo, Antti Lipponen, Tom V. Kokkonen, Jenni Kontkanen, Runlong Cai, Jing Cai, Tommy Chan, Liangduo Chen, Biwu Chu, Chenjuan Deng, Wei Du, Xiaolong Fan, Xu-Cheng He, Juha Kangasluoma, Joni Kujansuu, Mona Kurppa, Chang Li, Yiran Li, Zhuohui Lin, Yiliang Liu, Yuliang Liu, Yiqun Lu, Wei Nie, Jouni Pulliainen, Xiaohui Qiao, Yonghong Wang, Yifan Wen, Ye Wu, Gan Yang, Lei Yao, Rujing Yin, Gen Zhang, Shaojun Zhang, Feixue Zheng, Ying Zhou, Antti Arola, Johanna Tamminen, Pauli Paasonen, Yele Sun, Lin Wang, Neil M. Donahue, Yongchun Liu, Federico Bianchi, Kaspar R. Daellenbach, Douglas R. Worsnop, Veli-Matti Kerminen, Tuukka Petäjä, Aijun Ding, Jingkun Jiang, and Markku Kulmala
Atmos. Chem. Phys., 22, 12207–12220, https://doi.org/10.5194/acp-22-12207-2022, https://doi.org/10.5194/acp-22-12207-2022, 2022
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Atmospheric new particle formation (NPF) is a dominant source of atmospheric ultrafine particles. In urban environments, traffic emissions are a major source of primary pollutants, but their contribution to NPF remains under debate. During the COVID-19 lockdown, traffic emissions were significantly reduced, providing a unique chance to examine their relevance to NPF. Based on our comprehensive measurements, we demonstrate that traffic emissions alone are not able to explain the NPF in Beijing.
Mengying Li, Shaocai Yu, Xue Chen, Zhen Li, Yibo Zhang, Zhe Song, Weiping Liu, Pengfei Li, Xiaoye Zhang, Meigen Zhang, Yele Sun, Zirui Liu, Caiping Sun, Jingkun Jiang, Shuxiao Wang, Benjamin N. Murphy, Kiran Alapaty, Rohit Mathur, Daniel Rosenfeld, and John H. Seinfeld
Atmos. Chem. Phys., 22, 11845–11866, https://doi.org/10.5194/acp-22-11845-2022, https://doi.org/10.5194/acp-22-11845-2022, 2022
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This study constructed an emission inventory of condensable particulate matter (CPM) in China with a focus on organic aerosols (OAs), based on collected CPM emission information. The results show that OA emissions are enhanced twofold for the years 2014 and 2017 after the inclusion of CPM in the new inventory. Sensitivity cases demonstrated the significant contributions of CPM emissions from stationary combustion and mobile sources to primary, secondary, and total OA concentrations.
Jingwen Xue, Fangfang Ma, Jonas Elm, Jingwen Chen, and Hong-Bin Xie
Atmos. Chem. Phys., 22, 11543–11555, https://doi.org/10.5194/acp-22-11543-2022, https://doi.org/10.5194/acp-22-11543-2022, 2022
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·OH/·Cl initiated indole reactions mainly form organonitrates, alkoxy radicals and hydroperoxide products, showing a varying mechanism from previously reported amines reactions. This study reveals carcinogenic nitrosamines cannot be formed in indole oxidation reactions despite radicals formed from -NH- H abstraction. The results are important to understand the atmospheric impact of indole oxidation and extend current understanding on the atmospheric chemistry of organic nitrogen compounds.
Lichao Yang, Wansuo Duan, Zifa Wang, and Wenyi Yang
Atmos. Chem. Phys., 22, 11429–11453, https://doi.org/10.5194/acp-22-11429-2022, https://doi.org/10.5194/acp-22-11429-2022, 2022
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The initial meteorological state has a great impact on PM2.5 forecasts. Assimilating additional observations is an effective way to improve the accuracy of the initial meteorological state. Here we used an advanced optimization approach to identify where we should preferentially place the meteorological observations associated with PM2.5 forecasts in the Beijing–Tianjin–Hebei region of China. We provide evidence that the target observation strategy is effective for improving PM2.5 forecasts.
Zhiqiang Zhang, Yele Sun, Chun Chen, Bo You, Aodong Du, Weiqi Xu, Yan Li, Zhijie Li, Lu Lei, Wei Zhou, Jiaxing Sun, Yanmei Qiu, Lianfang Wei, Pingqing Fu, and Zifa Wang
Atmos. Chem. Phys., 22, 10409–10423, https://doi.org/10.5194/acp-22-10409-2022, https://doi.org/10.5194/acp-22-10409-2022, 2022
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We present a comprehensive characterization of water-soluble organic aerosol and the first mass spectral characterization of water-insoluble organic aerosol in the cold season in Beijing by integrating online and offline aerosol mass spectrometer measurements. WSOA comprised dominantly secondary OA and showed large changes during the transition season from autumn to winter. WIOA was characterized by prominent hydrocarbon ions series, low oxidation states, and significant day–night differences.
Yihang Yu, Peng Cheng, Huirong Li, Wenda Yang, Baobin Han, Wei Song, Weiwei Hu, Xinming Wang, Bin Yuan, Min Shao, Zhijiong Huang, Zhen Li, Junyu Zheng, Haichao Wang, and Xiaofang Yu
Atmos. Chem. Phys., 22, 8951–8971, https://doi.org/10.5194/acp-22-8951-2022, https://doi.org/10.5194/acp-22-8951-2022, 2022
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We have investigated the budget of HONO at an urban site in Guangzhou. Budget and comprehensive uncertainty analysis suggest that at such locations as ours, HONO direct emissions and NO + OH can become comparable or even surpass other HONO sources that typically receive greater attention and interest, such as the NO2 heterogeneous source and the unknown daytime photolytic source. Our findings emphasize the need to reduce the uncertainties of both conventional and novel HONO sources and sinks.
Mingfu Cai, Shan Huang, Baoling Liang, Qibin Sun, Li Liu, Bin Yuan, Min Shao, Weiwei Hu, Wei Chen, Qicong Song, Wei Li, Yuwen Peng, Zelong Wang, Duohong Chen, Haobo Tan, Hanbin Xu, Fei Li, Xuejiao Deng, Tao Deng, Jiaren Sun, and Jun Zhao
Atmos. Chem. Phys., 22, 8117–8136, https://doi.org/10.5194/acp-22-8117-2022, https://doi.org/10.5194/acp-22-8117-2022, 2022
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This study investigated the size dependence and diurnal variation in organic aerosol hygroscopicity, volatility, and cloud condensation nuclei (CCN) activity. We found that the physical properties of OA could vary in a large range at different particle sizes and affected the number concentration of CCN (NCCN) at all supersaturations. Our results highlight the importance of evaluating the atmospheric evolution processes of OA at different size ranges and their impact on climate effects.
Jiaxing Sun, Yele Sun, Conghui Xie, Weiqi Xu, Chun Chen, Zhe Wang, Lei Li, Xubing Du, Fugui Huang, Yan Li, Zhijie Li, Xiaole Pan, Nan Ma, Wanyun Xu, Pingqing Fu, and Zifa Wang
Atmos. Chem. Phys., 22, 7619–7630, https://doi.org/10.5194/acp-22-7619-2022, https://doi.org/10.5194/acp-22-7619-2022, 2022
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We analyzed the chemical composition and mixing state of BC-containing particles at urban and rural sites in winter in the North China Plain and evaluated their impact on light absorption enhancement. BC was dominantly mixed with organic carbon, nitrate, and sulfate, and the mixing state evolved significantly as a function of relative humidity (RH) at both sites. The absorption enhancement depended strongly on coated secondary inorganic aerosol and was up to ~1.3–1.4 during aging processes.
Junjun Deng, Hao Ma, Xinfeng Wang, Shujun Zhong, Zhimin Zhang, Jialei Zhu, Yanbing Fan, Wei Hu, Libin Wu, Xiaodong Li, Lujie Ren, Chandra Mouli Pavuluri, Xiaole Pan, Yele Sun, Zifa Wang, Kimitaka Kawamura, and Pingqing Fu
Atmos. Chem. Phys., 22, 6449–6470, https://doi.org/10.5194/acp-22-6449-2022, https://doi.org/10.5194/acp-22-6449-2022, 2022
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Light-absorbing brown carbon (BrC) plays an important role in climate change and atmospheric chemistry. Here we investigated the seasonal and diurnal variations in water-soluble BrC in PM2.5 in the megacity Tianjin in coastal China. Results of the source apportionments from the combination with organic molecular compositions and optical properties of water-soluble BrC reveal a large contribution from primary bioaerosol particles to BrC in the urban atmosphere.
Haibo Wang, Ting Yang, Zifa Wang, Jianjun Li, Wenxuan Chai, Guigang Tang, Lei Kong, and Xueshun Chen
Geosci. Model Dev., 15, 3555–3585, https://doi.org/10.5194/gmd-15-3555-2022, https://doi.org/10.5194/gmd-15-3555-2022, 2022
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In this paper, we develop an online data coupled assimilation system (NAQPMS-PDAF) with the Eulerian atmospheric chemistry-transport model. NAQPMS-PDAF allows efficient use of large computational resources. The application and performance of the system are investigated by assimilating 1 month of vertical aerosol observations. The results show that NAQPMS-PDAF can significantly improve the performance of aerosol vertical structure simulation and reduce the uncertainty to a large extent.
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.
Jingnan Shi, Juan Hong, Nan Ma, Qingwei Luo, Yao He, Hanbing Xu, Haobo Tan, Qiaoqiao Wang, Jiangchuan Tao, Yaqing Zhou, Shuang Han, Long Peng, Linhong Xie, Guangsheng Zhou, Wanyun Xu, Yele Sun, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 22, 4599–4613, https://doi.org/10.5194/acp-22-4599-2022, https://doi.org/10.5194/acp-22-4599-2022, 2022
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In this study, we investigated the hygroscopicity of submicron aerosols at a rural site in the North China Plain during the winter of 2018, using a HTDMA and a CV-ToF-ACSM. We observed differences in aerosol hygroscopicity during two distinct episodes with different primary emissions and secondary aerosol formation processes. These results provide an improved understanding of the complex influence of sources and aerosol evolution processes on their hygroscopicity.
Wenjie Wang, Bin Yuan, Yuwen Peng, Hang Su, Yafang Cheng, Suxia Yang, Caihong Wu, Jipeng Qi, Fengxia Bao, Yibo Huangfu, Chaomin Wang, Chenshuo Ye, Zelong Wang, Baolin Wang, Xinming Wang, Wei Song, Weiwei Hu, Peng Cheng, Manni Zhu, Junyu Zheng, and Min Shao
Atmos. Chem. Phys., 22, 4117–4128, https://doi.org/10.5194/acp-22-4117-2022, https://doi.org/10.5194/acp-22-4117-2022, 2022
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From thorough measurements of numerous oxygenated volatile organic compounds, we show that their photodissociation can be important for radical production and ozone formation in the atmosphere. This effect was underestimated in previous studies, as measurements of them were lacking.
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.
Jingwei Zhang, Chaofan Lian, Weigang Wang, Maofa Ge, Yitian Guo, Haiyan Ran, Yusheng Zhang, Feixue Zheng, Xiaolong Fan, Chao Yan, Kaspar R. Daellenbach, Yongchun Liu, Markku Kulmala, and Junling An
Atmos. Chem. Phys., 22, 3275–3302, https://doi.org/10.5194/acp-22-3275-2022, https://doi.org/10.5194/acp-22-3275-2022, 2022
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This study added six potential HONO sources to the WRF-Chem model, evaluated their impact on HONO and O3 concentrations, including surface and vertical concentrations. The simulations extend our knowledge on atmospheric HONO sources, especially for nitrate photolysis. The study also explains the HONO difference in O3 formation on clean and hazy days, and reveals key potential HONO sources to O3 enhancements in haze-aggravating processes with a co-occurrence of high PM2.5 and O3 concentrations.
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.
Douglas A. Day, Pedro Campuzano-Jost, Benjamin A. Nault, Brett B. Palm, Weiwei Hu, Hongyu Guo, Paul J. Wooldridge, Ronald C. Cohen, Kenneth S. Docherty, J. Alex Huffman, Suzane S. de Sá, Scot T. Martin, and Jose L. Jimenez
Atmos. Meas. Tech., 15, 459–483, https://doi.org/10.5194/amt-15-459-2022, https://doi.org/10.5194/amt-15-459-2022, 2022
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Particle-phase nitrates are an important component of atmospheric aerosols and chemistry. In this paper, we systematically explore the application of aerosol mass spectrometry (AMS) to quantify the organic and inorganic nitrate fractions of aerosols in the atmosphere. While AMS has been used for a decade to quantify nitrates, methods are not standardized. We make recommendations for a more universal approach based on this analysis of a large range of field and laboratory observations.
Jing Cai, Cheng Wu, Jiandong Wang, Wei Du, Feixue Zheng, Simo Hakala, Xiaolong Fan, Biwu Chu, Lei Yao, Zemin Feng, Yongchun Liu, Yele Sun, Jun Zheng, Chao Yan, Federico Bianchi, Markku Kulmala, Claudia Mohr, and Kaspar R. Daellenbach
Atmos. Chem. Phys., 22, 1251–1269, https://doi.org/10.5194/acp-22-1251-2022, https://doi.org/10.5194/acp-22-1251-2022, 2022
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This study investigates the connection between organic aerosol (OA) molecular composition and particle absorptive properties in autumn in Beijing. We find that the molecular properties of OA compounds in different episodes influence particle light absorption properties differently: the light absorption enhancement of black carbon and light absorption coefficient of brown carbon were mostly related to more oxygenated OA (low C number and four O atoms) and aromatics/nitro-aromatics, respectively.
Jiaxing Sun, Zhe Wang, Wei Zhou, Conghui Xie, Cheng Wu, Chun Chen, Tingting Han, Qingqing Wang, Zhijie Li, Jie Li, Pingqing Fu, Zifa Wang, and Yele Sun
Atmos. Chem. Phys., 22, 561–575, https://doi.org/10.5194/acp-22-561-2022, https://doi.org/10.5194/acp-22-561-2022, 2022
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We analyzed 9-year measurements of BC and aerosol optical properties from 2012 to 2020 in Beijing, China. Our results showed large reductions in BC and light extinction coefficient due to the Clean Air Action Plan. As a response, both SSA and mass extinction efficiency (MEE) showed considerable increases, demonstrating a future challenge in visibility improvement. The primary and secondary BrC was also separated and quantified, and the changes in radiative forcing of BC and BrC were estimated.
Qian Ye, Jie Li, Xueshun Chen, Huansheng Chen, Wenyi Yang, Huiyun Du, Xiaole Pan, Xiao Tang, Wei Wang, Lili Zhu, Jianjun Li, Zhe Wang, and Zifa Wang
Geosci. Model Dev., 14, 7573–7604, https://doi.org/10.5194/gmd-14-7573-2021, https://doi.org/10.5194/gmd-14-7573-2021, 2021
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We developed a global tropospheric atmospheric chemistry source–receptor model. This model can quantify the contributions of multiple air pollutants from various source regions in one simulation without introducing the nonlinear error of atmospheric chemistry. The S-R relationships of PM2.5 and O3 from a global high-resolution (0.5° × 0.5°) simulation were given and compared with previous studies. This model will be useful for creating a link between the scientific community and policymakers.
Yuting Zhang, Hang Liu, Shandong Lei, Wanyun Xu, Yu Tian, Weijie Yao, Xiaoyong Liu, Qi Liao, Jie Li, Chun Chen, Yele Sun, Pingqing Fu, Jinyuan Xin, Junji Cao, Xiaole Pan, and Zifa Wang
Atmos. Chem. Phys., 21, 17631–17648, https://doi.org/10.5194/acp-21-17631-2021, https://doi.org/10.5194/acp-21-17631-2021, 2021
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In this study, the authors used a single-particle soot photometer (SP2) to characterize the particle size, mixing state, and optical properties of black carbon aerosols in rural areas of the North China Plain in winter. Relatively warm and high-RH environments (RH > 50 %, −4° < T < 4 °) were more favorable to rBC aging than dry and cold environments (RH < 60 %, T < −8°). The paper emphasizes the importance of meteorological parameters in the mixing state of black carbon.
Hongyi Ding, Le Cao, Haimei Jiang, Wenxing Jia, Yong Chen, and Junling An
Geosci. Model Dev., 14, 6135–6153, https://doi.org/10.5194/gmd-14-6135-2021, https://doi.org/10.5194/gmd-14-6135-2021, 2021
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We performed a WRF model study to figure out the mechanism of how the change in minimum eddy diffusivity (Kzmin) in the planetary boundary layer (PBL) closure scheme (ACM2) affects the simulated near-surface temperature in Beijing, China. Moreover, the influence of changing Kzmin on the temperature prediction in areas with different land-use categories was studied. The model performance using a functional-type Kzmin for capturing the temperature change in this area was also clarified.
Sihui Jiang, Fang Zhang, Jingye Ren, Lu Chen, Xing Yan, Jieyao Liu, Yele Sun, and Zhanqing Li
Atmos. Chem. Phys., 21, 14293–14308, https://doi.org/10.5194/acp-21-14293-2021, https://doi.org/10.5194/acp-21-14293-2021, 2021
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New particle formation (NPF) can be a large source of CCN and affect weather and climate. Here we show that the NPF contributes largely to cloud droplet number concentration (Nd) but is suppressed at high particle number concentrations in Beijing due to water vapor competition. We also reveal a considerable impact of primary sources on the evaluation in the urban atmosphere. Our study has great significance for assessing NPF-associated effects on climate in polluted regions.
Hong Ren, Wei Hu, Lianfang Wei, Siyao Yue, Jian Zhao, Linjie Li, Libin Wu, Wanyu Zhao, Lujie Ren, Mingjie Kang, Qiaorong Xie, Sihui Su, Xiaole Pan, Zifa Wang, Yele Sun, Kimitaka Kawamura, and Pingqing Fu
Atmos. Chem. Phys., 21, 12949–12963, https://doi.org/10.5194/acp-21-12949-2021, https://doi.org/10.5194/acp-21-12949-2021, 2021
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This study presents vertical profiles of biogenic and anthropogenic secondary organic aerosols (SOAs) in the urban boundary layer based on a 325 m tower in Beijing in late summer. The increases in the isoprene and toluene SOAs with height were found to be more related to regional transport, whereas the decrease in those from monoterpenes and sesquiterpene were more subject to local emissions. Such complicated vertical distributions of SOA should be considered in future modeling work.
Junhua Wang, Baozhu Ge, Xueshun Chen, Jie Li, Keding Lu, Yayuan Dong, Lei Kong, Zifa Wang, and Yuanhang Zhang
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2021-259, https://doi.org/10.5194/gmd-2021-259, 2021
Revised manuscript not accepted
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This paper developed a novel quantitative decoupling analysis (QDA) method to quantify the contributions of emission, meteorology, chemical reaction, and their nonlinear interactions on PM2.5 and applied it to a pollution episode in Beijing. This method can provides the researchers and policy makers with valuable information for understanding of key factors to heavy pollution, but also help the modelers to find out the sources of uncertainties among numerical models.
Yang Yang, Minqiang Zhou, Ting Wang, Bo Yao, Pengfei Han, Denghui Ji, Wei Zhou, Yele Sun, Gengchen Wang, and Pucai Wang
Atmos. Chem. Phys., 21, 11741–11757, https://doi.org/10.5194/acp-21-11741-2021, https://doi.org/10.5194/acp-21-11741-2021, 2021
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This study introduces the in situ CO2 measurement system installed in Beijing (urban), Xianghe (suburban), and Xinglong (rural) in North China for the first time. The spatial and temporal variations in CO2 mole fractions at the three sites between June 2018 and April 2020 are discussed on both seasonal and diurnal scales.
Qiaorong Xie, Sihui Su, Jing Chen, Yuqing Dai, Siyao Yue, Hang Su, Haijie Tong, Wanyu Zhao, Lujie Ren, Yisheng Xu, Dong Cao, Ying Li, Yele Sun, Zifa Wang, Cong-Qiang Liu, Kimitaka Kawamura, Guibin Jiang, Yafang Cheng, and Pingqing Fu
Atmos. Chem. Phys., 21, 11453–11465, https://doi.org/10.5194/acp-21-11453-2021, https://doi.org/10.5194/acp-21-11453-2021, 2021
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This study investigated the role of nighttime chemistry during Chinese New Year's Eve that enhances the formation of nitrooxy organosulfates in the aerosol phase. Results show that anthropogenic precursors, together with biogenic ones, considerably contribute to the formation of low-volatility nitrooxy OSs. Our study provides detailed molecular composition of firework-related aerosols, which gives new insights into the physicochemical properties and potential health effects of urban aerosols.
Benjamin A. Nault, Duseong S. Jo, Brian C. McDonald, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Jason C. Schroder, James Allan, Donald R. Blake, Manjula R. Canagaratna, Hugh Coe, Matthew M. Coggon, Peter F. DeCarlo, Glenn S. Diskin, Rachel Dunmore, Frank Flocke, Alan Fried, Jessica B. Gilman, Georgios Gkatzelis, Jacqui F. Hamilton, Thomas F. Hanisco, Patrick L. Hayes, Daven K. Henze, Alma Hodzic, James Hopkins, Min Hu, L. Greggory Huey, B. Thomas Jobson, William C. Kuster, Alastair Lewis, Meng Li, Jin Liao, M. Omar Nawaz, Ilana B. Pollack, Jeffrey Peischl, Bernhard Rappenglück, Claire E. Reeves, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Min Shao, Jacob M. Sommers, James Walega, Carsten Warneke, Petter Weibring, Glenn M. Wolfe, Dominique E. Young, Bin Yuan, Qiang Zhang, Joost A. de Gouw, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 11201–11224, https://doi.org/10.5194/acp-21-11201-2021, https://doi.org/10.5194/acp-21-11201-2021, 2021
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Secondary organic aerosol (SOA) is an important aspect of poor air quality for urban regions around the world, where a large fraction of the population lives. However, there is still large uncertainty in predicting SOA in urban regions. Here, we used data from 11 urban campaigns and show that the variability in SOA production in these regions is predictable and is explained by key emissions. These results are used to estimate the premature mortality associated with SOA in urban regions.
Ying Wei, Xueshun Chen, Huansheng Chen, Yele Sun, Wenyi Yang, Huiyun Du, Qizhong Wu, Dan Chen, Xiujuan Zhao, Jie Li, and Zifa Wang
Geosci. Model Dev., 14, 4411–4428, https://doi.org/10.5194/gmd-14-4411-2021, https://doi.org/10.5194/gmd-14-4411-2021, 2021
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The sub-grid particle formation (SGPF) in plumes plays an important role in air pollution and climate. We coupled an SGPF scheme to a chemical transport model with an aerosol microphysics module and applied it to investigate the SGPF impact over China. The scheme clearly improved the model performance in simulating aerosol components and particle number at typical sites influenced by point sources. The results indicate the significant effects of SGPF on aerosol particles in industrial areas.
Haijie Tong, Fobang Liu, Alexander Filippi, Jake Wilson, Andrea M. Arangio, Yun Zhang, Siyao Yue, Steven Lelieveld, Fangxia Shen, Helmi-Marja K. Keskinen, Jing Li, Haoxuan Chen, Ting Zhang, Thorsten Hoffmann, Pingqing Fu, William H. Brune, Tuukka Petäjä, Markku Kulmala, Maosheng Yao, Thomas Berkemeier, Manabu Shiraiwa, and Ulrich Pöschl
Atmos. Chem. Phys., 21, 10439–10455, https://doi.org/10.5194/acp-21-10439-2021, https://doi.org/10.5194/acp-21-10439-2021, 2021
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We measured radical yields of aqueous PM2.5 extracts and found lower yields at higher concentrations of PM2.5. Abundances of water-soluble transition metals and aromatics in PM2.5 were positively correlated with the relative fraction of •OH but negatively correlated with the relative fraction of C-centered radicals among detected radicals. Composition-dependent reactive species yields may explain differences in the reactivity and health effects of PM2.5 in clean versus polluted air.
Ye Kuang, Shan Huang, Biao Xue, Biao Luo, Qicong Song, Wei Chen, Weiwei Hu, Wei Li, Pusheng Zhao, Mingfu Cai, Yuwen Peng, Jipeng Qi, Tiange Li, Sihang Wang, Duohong Chen, Dingli Yue, Bin Yuan, and Min Shao
Atmos. Chem. Phys., 21, 10375–10391, https://doi.org/10.5194/acp-21-10375-2021, https://doi.org/10.5194/acp-21-10375-2021, 2021
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We found that organic aerosol factors with identified sources perform much better than oxidation level parameters in characterizing variations in organic aerosol hygroscopicity, and secondary aerosol formations associated with different sources have distinct effects on organic aerosol hygroscopicity. It reveals that source-oriented organic aerosol hygroscopicity investigations might result in more appropriate parameterization approaches in chemical and climate models.
Tommaso Galeazzo, Richard Valorso, Ying Li, Marie Camredon, Bernard Aumont, and Manabu Shiraiwa
Atmos. Chem. Phys., 21, 10199–10213, https://doi.org/10.5194/acp-21-10199-2021, https://doi.org/10.5194/acp-21-10199-2021, 2021
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We simulate SOA viscosity with explicit modeling of gas-phase oxidation of isoprene and α-pinene. While the viscosity dependence on relative humidity and mass loadings is captured well by simulations, the model underestimates measured viscosity, indicating missing processes. Kinetic limitations and reduction in mass accommodation may cause an increase in viscosity. The developed model is powerful for investigation of the interplay among gas reactions, chemical composition and phase state.
Hua Fang, Xiaoqing Huang, Yanli Zhang, Chenglei Pei, Zuzhao Huang, Yujun Wang, Yanning Chen, Jianhong Yan, Jianqiang Zeng, Shaoxuan Xiao, Shilu Luo, Sheng Li, Jun Wang, Ming Zhu, Xuewei Fu, Zhenfeng Wu, Runqi Zhang, Wei Song, Guohua Zhang, Weiwei Hu, Mingjin Tang, Xiang Ding, Xinhui Bi, and Xinming Wang
Atmos. Chem. Phys., 21, 10005–10013, https://doi.org/10.5194/acp-21-10005-2021, https://doi.org/10.5194/acp-21-10005-2021, 2021
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A tunnel test was initiated to measure the vehicular IVOC emissions under real-world driving conditions. Higher SOA formation estimated from vehicular IVOCs compared to those from traditional VOCs emphasized the greater importance of IVOCs in modulating urban SOA. The results also revealed that non-road diesel-fueled engines greatly contributed to IVOCs in China.
Baozhu Ge, Danhui Xu, Oliver Wild, Xuefeng Yao, Junhua Wang, Xueshun Chen, Qixin Tan, Xiaole Pan, and Zifa Wang
Atmos. Chem. Phys., 21, 9441–9454, https://doi.org/10.5194/acp-21-9441-2021, https://doi.org/10.5194/acp-21-9441-2021, 2021
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In this study, an improved sequential sampling method is developed and implemented to estimate the contribution of below-cloud and in-cloud wet deposition over four years of measurements in Beijing. We find that the contribution of below-cloud scavenging for Ca2+, SO4 2–, and NH4+ decreases from above 50 % in 2014 to below 40 % in 2017. This suggests that the Action Plan has mitigated particulate matter pollution in the surface layer and hence decreased scavenging due to the washout process.
Xueshun Chen, Fangqun Yu, Wenyi Yang, Yele Sun, Huansheng Chen, Wei Du, Jian Zhao, Ying Wei, Lianfang Wei, Huiyun Du, Zhe Wang, Qizhong Wu, Jie Li, Junling An, and Zifa Wang
Atmos. Chem. Phys., 21, 9343–9366, https://doi.org/10.5194/acp-21-9343-2021, https://doi.org/10.5194/acp-21-9343-2021, 2021
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Atmospheric aerosol particles have significant climate and health effects that depend on aerosol size, composition, and mixing state. A new global-regional nested aerosol model with an advanced particle microphysics module and a volatility basis set organic aerosol module was developed to simulate aerosol microphysical processes. Simulations strongly suggest the important role of anthropogenic organic species in particle formation over the areas influenced by anthropogenic sources.
Syuichi Itahashi, Baozhu Ge, Keiichi Sato, Zhe Wang, Junichi Kurokawa, Jiani Tan, Kan Huang, Joshua S. Fu, Xuemei Wang, Kazuyo Yamaji, Tatsuya Nagashima, Jie Li, Mizuo Kajino, Gregory R. Carmichael, and Zifa Wang
Atmos. Chem. Phys., 21, 8709–8734, https://doi.org/10.5194/acp-21-8709-2021, https://doi.org/10.5194/acp-21-8709-2021, 2021
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This study presents the detailed analysis of acid deposition over southeast Asia based on the Model Inter-Comparison Study for Asia (MICS-Asia) phase III. Simulated wet deposition is evaluated with observation data from the Acid Deposition Monitoring Network in East Asia (EANET). The difficulties of models to capture observations are related to the model performance on precipitation. The precipitation-adjusted approach was applied, and the distribution of wet deposition was successfully revised.
Chenshuo Ye, Bin Yuan, Yi Lin, Zelong Wang, Weiwei Hu, Tiange Li, Wei Chen, Caihong Wu, Chaomin Wang, Shan Huang, Jipeng Qi, Baolin Wang, Chen Wang, Wei Song, Xinming Wang, E Zheng, Jordan E. Krechmer, Penglin Ye, Zhanyi Zhang, Xuemei Wang, Douglas R. Worsnop, and Min Shao
Atmos. Chem. Phys., 21, 8455–8478, https://doi.org/10.5194/acp-21-8455-2021, https://doi.org/10.5194/acp-21-8455-2021, 2021
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We performed measurements of gaseous and particulate organic compounds using a state-of-the-art online mass spectrometer in urban air. Using the dataset, we provide a holistic chemical characterization of oxygenated organic compounds in the polluted urban atmosphere, which can serve as a reference for the future field measurements of organic compounds in cities.
Siqi Hou, Di Liu, Jingsha Xu, Tuan V. Vu, Xuefang Wu, Deepchandra Srivastava, Pingqing Fu, Linjie Li, Yele Sun, Athanasia Vlachou, Vaios Moschos, Gary Salazar, Sönke Szidat, André S. H. Prévôt, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 21, 8273–8292, https://doi.org/10.5194/acp-21-8273-2021, https://doi.org/10.5194/acp-21-8273-2021, 2021
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This study provides a newly developed method which combines radiocarbon (14C) with organic tracers to enable source apportionment of primary and secondary fossil vs. non-fossil sources of carbonaceous aerosols at an urban and a rural site of Beijing. The source apportionment results were compared with those by chemical mass balance and AMS/ACSM-PMF methods. Correlations of WINSOC and WSOC with different sources of OC were also performed to elucidate the formation mechanisms of SOC.
Weiqi Xu, Masayuki Takeuchi, Chun Chen, Yanmei Qiu, Conghui Xie, Wanyun Xu, Nan Ma, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Meas. Tech., 14, 3693–3705, https://doi.org/10.5194/amt-14-3693-2021, https://doi.org/10.5194/amt-14-3693-2021, 2021
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Here we developed a method for estimation of particulate organic nitrates (pON) from the measurements of a high-resolution aerosol mass spectrometer coupled with a thermodenuder based on the volatility differences between inorganic nitrate and pON. The results generally had improvements in reducing negative values due to the influences of a high concentration of inorganic nitrate and a constant ratio of NO+ to NO2+ of organic nitrates (RON).
Jiangchuan Tao, Ye Kuang, Nan Ma, Juan Hong, Yele Sun, Wanyun Xu, Yanyan Zhang, Yao He, Qingwei Luo, Linhong Xie, Hang Su, and Yafang Cheng
Atmos. Chem. Phys., 21, 7409–7427, https://doi.org/10.5194/acp-21-7409-2021, https://doi.org/10.5194/acp-21-7409-2021, 2021
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The mechanism of secondary aerosol (SA) formation can be affected by relative humidity (RH) and has different influences on the particle CCN activity under different RH conditions. In the North China Plain, we find different responses of CCN activity and enhancements of CCN number concentration to SA formation under different RH conditions. In addition, variations of aerosol mixing state due to SA formation contribute some of the largest uncertainties in predicting CCN number concentration.
Jingsha Xu, Di Liu, Xuefang Wu, Tuan V. Vu, Yanli Zhang, Pingqing Fu, Yele Sun, Weiqi Xu, Bo Zheng, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 21, 7321–7341, https://doi.org/10.5194/acp-21-7321-2021, https://doi.org/10.5194/acp-21-7321-2021, 2021
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Source apportionment of fine aerosols in an urban site of Beijing used a chemical mass balance (CMB) model. Seven primary sources (industrial/residential coal burning, biomass burning, gasoline/diesel vehicles, cooking and vegetative detritus) explained an average of 75.7 % and 56.1 % of fine OC in winter and summer, respectively. CMB was found to resolve more primary OA sources than AMS-PMF, but the latter apportioned more secondary OA sources.
Jake Wilson, Ulrich Pöschl, Manabu Shiraiwa, and Thomas Berkemeier
Atmos. Chem. Phys., 21, 6175–6198, https://doi.org/10.5194/acp-21-6175-2021, https://doi.org/10.5194/acp-21-6175-2021, 2021
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This work explores the gas–particle partitioning of PAHs on soot with a kinetic model. We show that the equilibration timescale depends on PAH molecular structure, temperature, and particle number concentration. We explore scenarios in which the particulate fraction is perturbed from equilibrium by chemical loss and discuss implications for chemical transport models that assume instantaneous equilibration at each model time step.
Steven J. Campbell, Kate Wolfer, Battist Utinger, Joe Westwood, Zhi-Hui Zhang, Nicolas Bukowiecki, Sarah S. Steimer, Tuan V. Vu, Jingsha Xu, Nicholas Straw, Steven Thomson, Atallah Elzein, Yele Sun, Di Liu, Linjie Li, Pingqing Fu, Alastair C. Lewis, Roy M. Harrison, William J. Bloss, Miranda Loh, Mark R. Miller, Zongbo Shi, and Markus Kalberer
Atmos. Chem. Phys., 21, 5549–5573, https://doi.org/10.5194/acp-21-5549-2021, https://doi.org/10.5194/acp-21-5549-2021, 2021
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In this study, we quantify PM2.5 oxidative potential (OP), a metric widely suggested as a potential measure of particle toxicity, in Beijing in summer and winter using four acellular assays. We correlate PM2.5 OP with a comprehensive range of atmospheric and particle composition measurements, demonstrating inter-assay differences and seasonal variation of PM2.5 OP. Using multivariate statistical analysis, we highlight specific particle chemical components and sources that influence OP.
Weiqi Xu, Chun Chen, Yanmei Qiu, Ying Li, Zhiqiang Zhang, Eleni Karnezi, Spyros N. Pandis, Conghui Xie, Zhijie Li, Jiaxing Sun, Nan Ma, Wanyun Xu, Pingqing Fu, Zifa Wang, Jiang Zhu, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Chem. Phys., 21, 5463–5476, https://doi.org/10.5194/acp-21-5463-2021, https://doi.org/10.5194/acp-21-5463-2021, 2021
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Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in the North China Plain (NCP) were investigated in summer and winter. Our results showed that organic aerosol (OA) in winter in the NCP is more volatile than that in summer due to enhanced primary emissions from coal combustion and biomass burning. We also found that OA existed mainly as a solid in winter in Beijing but as semisolids in Beijing in summer and Gucheng in winter.
Santosh Kumar Verma, Kimitaka Kawamura, Fei Yang, Pingqing Fu, Yugo Kanaya, and Zifa Wang
Atmos. Chem. Phys., 21, 4959–4978, https://doi.org/10.5194/acp-21-4959-2021, https://doi.org/10.5194/acp-21-4959-2021, 2021
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We studied aerosol samples collected in autumn 2007 with day and night intervals in a rural site of Mangshan, north of Beijing, for sugar compounds (SCs) that are abundant organic aerosol components and can influence the air quality and climate. We found higher concentrations of biomass burning (BB) products at nighttime than daytime, whereas pollen tracers and other SCs showed an opposite diurnal trend, because this site is meteorologically characterized by a mountain/valley breeze.
Tabish Umar Ansari, Oliver Wild, Edmund Ryan, Ying Chen, Jie Li, and Zifa Wang
Atmos. Chem. Phys., 21, 4471–4485, https://doi.org/10.5194/acp-21-4471-2021, https://doi.org/10.5194/acp-21-4471-2021, 2021
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We use novel modelling approaches to quantify the lingering effects of 1 d local and regional emission controls on subsequent days, the effects of longer continuous emission controls of individual sectors over different regions, and the effects of combined emission controls of multiple sectors and regions on air quality in Beijing under varying weather conditions to inform precise short-term emission control policies for avoiding heavy haze pollution in Beijing.
Duseong S. Jo, Alma Hodzic, Louisa K. Emmons, Simone Tilmes, Rebecca H. Schwantes, Michael J. Mills, Pedro Campuzano-Jost, Weiwei Hu, Rahul A. Zaveri, Richard C. Easter, Balwinder Singh, Zheng Lu, Christiane Schulz, Johannes Schneider, John E. Shilling, Armin Wisthaler, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 3395–3425, https://doi.org/10.5194/acp-21-3395-2021, https://doi.org/10.5194/acp-21-3395-2021, 2021
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Secondary organic aerosol (SOA) is a major component of submicron particulate matter, but there are a lot of uncertainties in the future prediction of SOA. We used CESM 2.1 to investigate future IEPOX SOA concentration changes. The explicit chemistry predicted substantial changes in IEPOX SOA depending on the future scenario, but the parameterization predicted weak changes due to simplified chemistry, which shows the importance of correct physicochemical dependencies in future SOA prediction.
Lei Kong, Xiao Tang, Jiang Zhu, Zifa Wang, Jianjun Li, Huangjian Wu, Qizhong Wu, Huansheng Chen, Lili Zhu, Wei Wang, Bing Liu, Qian Wang, Duohong Chen, Yuepeng Pan, Tao Song, Fei Li, Haitao Zheng, Guanglin Jia, Miaomiao Lu, Lin Wu, and Gregory R. Carmichael
Earth Syst. Sci. Data, 13, 529–570, https://doi.org/10.5194/essd-13-529-2021, https://doi.org/10.5194/essd-13-529-2021, 2021
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China's air pollution has changed substantially since 2013. Here we have developed a 6-year-long high-resolution air quality reanalysis dataset over China from 2013 to 2018 to illustrate such changes and to provide a basic dataset for relevant studies. Surface fields of PM2.5, PM10, SO2, NO2, CO, and O3 concentrations are provided, and the evaluation results indicate that the reanalysis dataset has excellent performance in reproducing the magnitude and variation of air pollution in China.
Lei Liu, Jian Zhang, Yinxiao Zhang, Yuanyuan Wang, Liang Xu, Qi Yuan, Dantong Liu, Yele Sun, Pingqing Fu, Zongbo Shi, and Weijun Li
Atmos. Chem. Phys., 21, 2251–2265, https://doi.org/10.5194/acp-21-2251-2021, https://doi.org/10.5194/acp-21-2251-2021, 2021
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We found that large numbers of light-absorbing primary organic particles with high viscosity, especially tarballs, from domestic coal and biomass burning occurred in rural and even urban hazes in the winter of North China. For the first time, we characterized the atmospheric aging process of these burning-related primary organic particles by microscopic analysis and further evaluated their light absorption enhancement resulting from the “lensing effect” of secondary inorganic coatings.
Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Archit Mehra, Stephen D. Worrall, Asan Bacak, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, William J. Bloss, Tuan Vu, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lujie Ren, W. Joe F. Acton, C. Nicholas Hewitt, Xinming Wang, Pingqing Fu, and Dwayne E. Heard
Atmos. Chem. Phys., 21, 2125–2147, https://doi.org/10.5194/acp-21-2125-2021, https://doi.org/10.5194/acp-21-2125-2021, 2021
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To understand how emission controls will impact ozone, an understanding of the sources and sinks of OH and the chemical cycling between peroxy radicals is needed. This paper presents measurements of OH, HO2 and total RO2 taken in central Beijing. The radical observations are compared to a detailed chemistry model, which shows that under low NO conditions, there is a missing OH source. Under high NOx conditions, the model under-predicts RO2 and impacts our ability to model ozone.
Manabu Shiraiwa and Ulrich Pöschl
Atmos. Chem. Phys., 21, 1565–1580, https://doi.org/10.5194/acp-21-1565-2021, https://doi.org/10.5194/acp-21-1565-2021, 2021
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Mass accommodation is a crucial process in secondary organic aerosol partitioning that depends on volatility, diffusivity, reactivity, and particle penetration depth of the chemical species involved. For efficient kinetic modeling, we introduce an effective mass accommodation coefficient that accounts for the above influencing factors, can be applied in the common Fuchs–Sutugin approximation, and helps to resolve inconsistencies and shortcomings of earlier experimental and model investigations.
Sabin Kasparoglu, Ying Li, Manabu Shiraiwa, and Markus D. Petters
Atmos. Chem. Phys., 21, 1127–1141, https://doi.org/10.5194/acp-21-1127-2021, https://doi.org/10.5194/acp-21-1127-2021, 2021
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Viscosity is important because it determines the lifetime, impact, and fate of particulate matter. We collected new data to rigorously test a framework that is used to constrain the phase state in global simulations. We find that the framework is accurate as long as appropriate compound specific inputs are available.
Liya Ma, Yujiao Zhu, Mei Zheng, Yele Sun, Lei Huang, Xiaohuan Liu, Yang Gao, Yanjie Shen, Huiwang Gao, and Xiaohong Yao
Atmos. Chem. Phys., 21, 183–200, https://doi.org/10.5194/acp-21-183-2021, https://doi.org/10.5194/acp-21-183-2021, 2021
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In this study, we investigate three patterns of new particles growing to CCN (cloud condensation nuclei) size, i.e., one-stage growth and two-stage growth-A and growth-B patterns. Combining the observations of gaseous pollutants and measured or modeled particulate chemical species, the three growth patterns were discussed regarding the spatial heterogeneity, formation of secondary aerosols, and evaporation of semivolatile particulates as was the survival probability of new particles to CCN size.
Hajime Akimoto, Tatsuya Nagashima, Natsumi Kawano, Li Jie, Joshua S. Fu, and Zifa Wang
Atmos. Chem. Phys., 20, 15003–15014, https://doi.org/10.5194/acp-20-15003-2020, https://doi.org/10.5194/acp-20-15003-2020, 2020
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In order to perform proper model simulation of ozone near the ground in the coastal area of northeastern Asia, it has been found that it is very important to select appropriate dry deposition velocities of ozone on the oceanic water of specific area of the northwestern Pacific. Empirical measurement of the mixing ratios and dry deposition flux of ozone over the ocean in this area is highly recommended.
Caihong Wu, Chaomin Wang, Sihang Wang, Wenjie Wang, Bin Yuan, Jipeng Qi, Baolin Wang, Hongli Wang, Chen Wang, Wei Song, Xinming Wang, Weiwei Hu, Shengrong Lou, Chenshuo Ye, Yuwen Peng, Zelong Wang, Yibo Huangfu, Yan Xie, Manni Zhu, Junyu Zheng, Xuemei Wang, Bin Jiang, Zhanyi Zhang, and Min Shao
Atmos. Chem. Phys., 20, 14769–14785, https://doi.org/10.5194/acp-20-14769-2020, https://doi.org/10.5194/acp-20-14769-2020, 2020
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Based on measurements from an online mass spectrometer, we quantify volatile organic compound (VOC) concentrations from numerous ions of the mass spectrometer, using information from laboratory-obtained calibration results. We find that most VOC concentrations are from oxygenated VOCs (OVOCs). We further show that these OVOCs also contribute significantly to OH reactivity. Our results suggest the important role of OVOCs in VOC emissions and chemistry in urban air.
Eloise J. Slater, Lisa K. Whalley, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Leigh R. Crilley, Louisa Kramer, William Bloss, Tuan Vu, Yele Sun, Weiqi Xu, Siyao Yue, Lujie Ren, W. Joe F. Acton, C. Nicholas Hewitt, Xinming Wang, Pingqing Fu, and Dwayne E. Heard
Atmos. Chem. Phys., 20, 14847–14871, https://doi.org/10.5194/acp-20-14847-2020, https://doi.org/10.5194/acp-20-14847-2020, 2020
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The paper details atmospheric chemistry in a megacity (Beijing), focussing on radicals which mediate the formation of secondary pollutants such as ozone and particles. Highly polluted conditions were experienced, including the highest ever levels of nitric oxide (NO), with simultaneous radical measurements. Radical concentrations were large during "haze" events, demonstrating active photochemistry. Modelling showed that our understanding of the chemistry at high NOx levels is incomplete.
Jingsha Xu, Shaojie Song, Roy M. Harrison, Congbo Song, Lianfang Wei, Qiang Zhang, Yele Sun, Lu Lei, Chao Zhang, Xiaohong Yao, Dihui Chen, Weijun Li, Miaomiao Wu, Hezhong Tian, Lining Luo, Shengrui Tong, Weiran Li, Junling Wang, Guoliang Shi, Yanqi Huangfu, Yingze Tian, Baozhu Ge, Shaoli Su, Chao Peng, Yang Chen, Fumo Yang, Aleksandra Mihajlidi-Zelić, Dragana Đorđević, Stefan J. Swift, Imogen Andrews, Jacqueline F. Hamilton, Ye Sun, Agung Kramawijaya, Jinxiu Han, Supattarachai Saksakulkrai, Clarissa Baldo, Siqi Hou, Feixue Zheng, Kaspar R. Daellenbach, Chao Yan, Yongchun Liu, Markku Kulmala, Pingqing Fu, and Zongbo Shi
Atmos. Meas. Tech., 13, 6325–6341, https://doi.org/10.5194/amt-13-6325-2020, https://doi.org/10.5194/amt-13-6325-2020, 2020
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An interlaboratory comparison was conducted for the first time to examine differences in water-soluble inorganic ions (WSIIs) measured by 10 labs using ion chromatography (IC) and by two online aerosol chemical speciation monitor (ACSM) methods. Major ions including SO42−, NO3− and NH4+ agreed well in 10 IC labs and correlated well with ACSM data. WSII interlab variability strongly affected aerosol acidity results based on ion balance, but aerosol pH computed by ISORROPIA II was very similar.
Chaomin Wang, Bin Yuan, Caihong Wu, Sihang Wang, Jipeng Qi, Baolin Wang, Zelong Wang, Weiwei Hu, Wei Chen, Chenshuo Ye, Wenjie Wang, Yele Sun, Chen Wang, Shan Huang, Wei Song, Xinming Wang, Suxia Yang, Shenyang Zhang, Wanyun Xu, Nan Ma, Zhanyi Zhang, Bin Jiang, Hang Su, Yafang Cheng, Xuemei Wang, and Min Shao
Atmos. Chem. Phys., 20, 14123–14138, https://doi.org/10.5194/acp-20-14123-2020, https://doi.org/10.5194/acp-20-14123-2020, 2020
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We utilized a novel online mass spectrometry method to measure the total concentration of higher alkanes at each carbon number at two different sites in China, allowing us to take into account SOA contributions from all isomers for higher alkanes. We found that higher alkanes account for significant fractions of SOA formation at the two sites. The contributions are comparable to or even higher than single-ring aromatics, the most-recognized SOA precursors in urban air.
Junfeng Wang, Jianhuai Ye, Dantong Liu, Yangzhou Wu, Jian Zhao, Weiqi Xu, Conghui Xie, Fuzhen Shen, Jie Zhang, Paul E. Ohno, Yiming Qin, Xiuyong Zhao, Scot T. Martin, Alex K. Y. Lee, Pingqing Fu, Daniel J. Jacob, Qi Zhang, Yele Sun, Mindong Chen, and Xinlei Ge
Atmos. Chem. Phys., 20, 14091–14102, https://doi.org/10.5194/acp-20-14091-2020, https://doi.org/10.5194/acp-20-14091-2020, 2020
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We compared the organics in total submicron matter and those coated on BC cores during summertime in Beijing and found large differences between them. Traffic-related OA was associated significantly with BC, while cooking-related OA did not coat BC. In addition, a factor likely originated from primary biomass burning OA was only identified in BC-containing particles. Such a unique BBOA requires further field and laboratory studies to verify its presence and elucidate its properties and impacts.
Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Hongyu Guo, Duseong S. Jo, Anne V. Handschy, Demetrios Pagonis, Jason C. Schroder, Melinda K. Schueneman, Michael J. Cubison, Jack E. Dibb, Alma Hodzic, Weiwei Hu, Brett B. Palm, and Jose L. Jimenez
Atmos. Meas. Tech., 13, 6193–6213, https://doi.org/10.5194/amt-13-6193-2020, https://doi.org/10.5194/amt-13-6193-2020, 2020
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Collecting particulate matter, or aerosols, onto filters to be analyzed offline is a widely used method to investigate the mass concentration and chemical composition of the aerosol, especially the inorganic portion. Here, we show that acidic aerosol (sulfuric acid) collected onto filters and then exposed to high ammonia mixing ratios (from human emissions) will lead to biases in the ammonium collected onto filters, and the uptake of ammonia is rapid (< 10 s), which impacts the filter data.
Chao Peng, Yu Wang, Zhijun Wu, Lanxiadi Chen, Ru-Jin Huang, Weigang Wang, Zhe Wang, Weiwei Hu, Guohua Zhang, Maofa Ge, Min Hu, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 20, 13877–13903, https://doi.org/10.5194/acp-20-13877-2020, https://doi.org/10.5194/acp-20-13877-2020, 2020
Yiqi Zheng, Joel A. Thornton, Nga Lee Ng, Hansen Cao, Daven K. Henze, Erin E. McDuffie, Weiwei Hu, Jose L. Jimenez, Eloise A. Marais, Eric Edgerton, and Jingqiu Mao
Atmos. Chem. Phys., 20, 13091–13107, https://doi.org/10.5194/acp-20-13091-2020, https://doi.org/10.5194/acp-20-13091-2020, 2020
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This study aims to address a challenge in biosphere–atmosphere interactions: to what extent can biogenic organic aerosol (OA) be modified through human activities? From three surface network observations, we show OA is weakly dependent on sulfate and aerosol acidity in the summer southeast US, on both long-term trends and monthly variability. The results are in strong contrast to a global model, GEOS-Chem, suggesting the need to revisit the representation of aqueous-phase secondary OA formation.
Jing Cai, Biwu Chu, Lei Yao, Chao Yan, Liine M. Heikkinen, Feixue Zheng, Chang Li, Xiaolong Fan, Shaojun Zhang, Daoyuan Yang, Yonghong Wang, Tom V. Kokkonen, Tommy Chan, Ying Zhou, Lubna Dada, Yongchun Liu, Hong He, Pauli Paasonen, Joni T. Kujansuu, Tuukka Petäjä, Claudia Mohr, Juha Kangasluoma, Federico Bianchi, Yele Sun, Philip L. Croteau, Douglas R. Worsnop, Veli-Matti Kerminen, Wei Du, Markku Kulmala, and Kaspar R. Daellenbach
Atmos. Chem. Phys., 20, 12721–12740, https://doi.org/10.5194/acp-20-12721-2020, https://doi.org/10.5194/acp-20-12721-2020, 2020
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By applying both OA PMF and size PMF at the same urban measurement site in Beijing, similar particle source types, including vehicular emissions, cooking emissions and secondary formation-related sources, were resolved by both frameworks and agreed well. It is also found that in the absence of new particle formation, vehicular and cooking emissions dominate the particle number concentration, while secondary particulate matter governed PM2.5 mass during spring and summer in Beijing.
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.
Hwajin Kim, Qi Zhang, and Yele Sun
Atmos. Chem. Phys., 20, 11527–11550, https://doi.org/10.5194/acp-20-11527-2020, https://doi.org/10.5194/acp-20-11527-2020, 2020
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Severe spring haze and influences of long-range transport in the Seoul metropolitan area (SMA) in March 2019 were investigated. Simultaneous downwind (SMA) and upwind (Beijing) measurements using AMS and ACSM over the same period showed that PM species can be transported in approximately 2 d. Nitrate was the most responsible, and sulfate and two regional-transport-influenced SOAs also contributed. Enhancement of Pb also showed that the haze in the SMA was influenced by the regional transport.
Liuwei Kong, Miao Feng, Yafei Liu, Yingying Zhang, Chen Zhang, Chenlu Li, Yu Qu, Junling An, Xingang Liu, Qinwen Tan, Nianliang Cheng, Yijun Deng, Ruixiao Zhai, and Zheng Wang
Atmos. Chem. Phys., 20, 11181–11199, https://doi.org/10.5194/acp-20-11181-2020, https://doi.org/10.5194/acp-20-11181-2020, 2020
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Secondary inorganic aerosols have an important contribution to PM2.5. Based on 3 years of atmospheric observation data, this study systematically analyzed the pollution levels and chemical conversion characteristics of nitrate, sulfate and ammonium in PM2.5 in Chengdu, southwest China, and analyzed the emission and regional transport characteristics of their gaseous precursors. This conclusion can provide an important reference for the current air pollution control.
Baozhu Ge, Syuichi Itahashi, Keiichi Sato, Danhui Xu, Junhua Wang, Fan Fan, Qixin Tan, Joshua S. Fu, Xuemei Wang, Kazuyo Yamaji, Tatsuya Nagashima, Jie Li, Mizuo Kajino, Hong Liao, Meigen Zhang, Zhe Wang, Meng Li, Jung-Hun Woo, Junichi Kurokawa, Yuepeng Pan, Qizhong Wu, Xuejun Liu, and Zifa Wang
Atmos. Chem. Phys., 20, 10587–10610, https://doi.org/10.5194/acp-20-10587-2020, https://doi.org/10.5194/acp-20-10587-2020, 2020
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Performances of the simulated deposition for different reduced N (Nr) species in China were conducted with the Model Inter-Comparison Study for Asia. Results showed that simulated wet deposition of oxidized N was overestimated in northeastern China and underestimated in south China, but Nr was underpredicted in all regions by all models. Oxidized N has larger uncertainties than Nr, indicating that the chemical reaction process is one of the most importance factors affecting model performance.
Wanyu Zhao, Hong Ren, Kimitaka Kawamura, Huiyun Du, Xueshun Chen, Siyao Yue, Qiaorong Xie, Lianfang Wei, Ping Li, Xin Zeng, Shaofei Kong, Yele Sun, Zifa Wang, and Pingqing Fu
Atmos. Chem. Phys., 20, 10331–10350, https://doi.org/10.5194/acp-20-10331-2020, https://doi.org/10.5194/acp-20-10331-2020, 2020
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Our observations provide detailed information on the abundance and vertical distribution of dicarboxylic acids, oxoacids and α-dicarbonyls in PM2.5 collected at three heights based on a 325 m meteorological tower in Beijing in summer. Our results demonstrate that organic acids at the ground surface are largely associated with local traffic emissions, while long-range atmospheric transport followed by photochemical ageing contributes more in the urban boundary layer than the ground surface.
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.
Ying Li, Douglas A. Day, Harald Stark, Jose L. Jimenez, and Manabu Shiraiwa
Atmos. Chem. Phys., 20, 8103–8122, https://doi.org/10.5194/acp-20-8103-2020, https://doi.org/10.5194/acp-20-8103-2020, 2020
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Viscosity is an important property of organic aerosols, but viscosity measurements of ambient organic aerosols are scarce. We developed a method to predict glass transition temperatures using volatility and the atomic oxygen-to-carbon ratio. The method was applied to field observations of volatility distributions to predict viscosity of ambient organic aerosols, yielding consistent results with ambient particle phase-state measurements and global simulations.
Junchen Guo, Shengzhen Zhou, Mingfu Cai, Jun Zhao, Wei Song, Weixiong Zhao, Weiwei Hu, Yele Sun, Yao He, Chengqiang Yang, Xuezhe Xu, Zhisheng Zhang, Peng Cheng, Qi Fan, Jian Hang, Shaojia Fan, Xinming Wang, and Xuemei Wang
Atmos. Chem. Phys., 20, 7595–7615, https://doi.org/10.5194/acp-20-7595-2020, https://doi.org/10.5194/acp-20-7595-2020, 2020
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We characterized non-refractory submicron particulate matter (PM1.0) during winter in Guangzhou, south China. Chemical composition and key sources of ambient PM1.0 are revealed, highlighting the significant role of SOA. The relationship with SOA and peroxy radicals indicated gas-phase oxidation contributed predominantly to SOA formation during non-pollution periods, while heterogeneous/multiphase reactions played more important roles in SOA formation during pollution periods.
Daniel J. Bryant, William J. Dixon, James R. Hopkins, Rachel E. Dunmore, Kelly L. Pereira, Marvin Shaw, Freya A. Squires, Thomas J. Bannan, Archit Mehra, Stephen D. Worrall, Asan Bacak, Hugh Coe, Carl J. Percival, Lisa K. Whalley, Dwayne E. Heard, Eloise J. Slater, Bin Ouyang, Tianqu Cui, Jason D. Surratt, Di Liu, Zongbo Shi, Roy Harrison, Yele Sun, Weiqi Xu, Alastair C. Lewis, James D. Lee, Andrew R. Rickard, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 20, 7531–7552, https://doi.org/10.5194/acp-20-7531-2020, https://doi.org/10.5194/acp-20-7531-2020, 2020
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Using the chemical composition of offline filter samples, we report that a large share of oxidized organic aerosol in Beijing during summer is due to isoprene secondary organic aerosol (iSOA). iSOA organosulfates showed a strong correlation with the product of ozone and particulate sulfate. This highlights the role of both photochemistry and the availability of particulate sulfate in heterogeneous reactions and further demonstrates that iSOA formation is controlled by anthropogenic emissions.
Jiani Tan, Joshua S. Fu, Gregory R. Carmichael, Syuichi Itahashi, Zhining Tao, Kan Huang, Xinyi Dong, Kazuyo Yamaji, Tatsuya Nagashima, Xuemei Wang, Yiming Liu, Hyo-Jung Lee, Chuan-Yao Lin, Baozhu Ge, Mizuo Kajino, Jia Zhu, Meigen Zhang, Hong Liao, and Zifa Wang
Atmos. Chem. Phys., 20, 7393–7410, https://doi.org/10.5194/acp-20-7393-2020, https://doi.org/10.5194/acp-20-7393-2020, 2020
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This study evaluated the performance of 12 chemical transport models from MICS-Asia III for predicting the particulate matter (PM) over East Asia. Four model processes were investigated as the possible reasons for model bias with measurements and the factors causing inconsistent predictions of PM from different models: (1) model inputs, (2) gas–particle conversion, (3) dust emission modules and (4) removal mechanisms (wet and dry depositions). The influence of each process was discussed.
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.
Weiqi Xu, Yao He, Yanmei Qiu, Chun Chen, Conghui Xie, Lu Lei, Zhijie Li, Jiaxing Sun, Junyao Li, Pingqing Fu, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Meas. Tech., 13, 3205–3219, https://doi.org/10.5194/amt-13-3205-2020, https://doi.org/10.5194/amt-13-3205-2020, 2020
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We characterized mass spectral features of organic aerosol (OA) and water-soluble OA (WSOA) from 21 cooking, crop straw, wood, and coal burning experiments using aerosol mass spectrometers with standard and capture vaporizers, and we demonstrated the applications of source spectral profiles in improving source apportionment of ambient OA at a highly polluted rural site in the North China Plain in winter.
Jing Yang, Wanyu Zhao, Lianfang Wei, Qiang Zhang, Yue Zhao, Wei Hu, Libin Wu, Xiaodong Li, Chandra Mouli Pavuluri, Xiaole Pan, Yele Sun, Zifa Wang, Cong-Qiang Liu, Kimitaka Kawamura, and Pingqing Fu
Atmos. Chem. Phys., 20, 6841–6860, https://doi.org/10.5194/acp-20-6841-2020, https://doi.org/10.5194/acp-20-6841-2020, 2020
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Our observations provide novel detailed information on the atmospheric abundances and spatial distributions of dicarboxylic acids, oxoacids, and α-dicarbonyls in marine aerosols collected from the South China Sea to the East Indian Ocean. Our results demonstrate that the continental outflow of both biogenic and anthropogenic precursors followed by photochemical aging is one of the main sources and formation processes of marine organic aerosols over the tropical oceanic regions.
Qiaorong Xie, Sihui Su, Shuang Chen, Yisheng Xu, Dong Cao, Jing Chen, Lujie Ren, Siyao Yue, Wanyu Zhao, Yele Sun, Zifa Wang, Haijie Tong, Hang Su, Yafang Cheng, Kimitaka Kawamura, Guibin Jiang, Cong-Qiang Liu, and Pingqing Fu
Atmos. Chem. Phys., 20, 6803–6820, https://doi.org/10.5194/acp-20-6803-2020, https://doi.org/10.5194/acp-20-6803-2020, 2020
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Current knowledge on firework-related organic aerosols is very limited. Here the detailed molecular composition of organics in urban aerosols was characterized using ultrahigh-resolution FT-ICR mass spectrometry. Our findings highlight that firework emission leads to a sharp increase in CHO, CHNO, and CHOS containing high-molecular-weight species, particularly aromatic-like substances, which affect the physicochemical properties such as the light absorption and health effects of urban aerosols.
Shengzhen Zhou, Luolin Wu, Junchen Guo, Weihua Chen, Xuemei Wang, Jun Zhao, Yafang Cheng, Zuzhao Huang, Jinpu Zhang, Yele Sun, Pingqing Fu, Shiguo Jia, Jun Tao, Yanning Chen, and Junxia Kuang
Atmos. Chem. Phys., 20, 6435–6453, https://doi.org/10.5194/acp-20-6435-2020, https://doi.org/10.5194/acp-20-6435-2020, 2020
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In this work, measurements of size-segregated aerosols were conducted at three altitudes (ground level, 118 m, and 488 m) on the 610 m high Canton Tower in southern China. Vertical variations of PM and size-segregated chemical compositions were investigated. The results indicated that meteorological parameters and atmospheric aqueous and heterogeneous reactions together led to aerosol formation and haze episodes in the Pearl River Delta region during the measurement periods.
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.
Hang Liu, Xiaole Pan, Dantong Liu, Xiaoyong Liu, Xueshun Chen, Yu Tian, Yele Sun, Pingqing Fu, and Zifa Wang
Atmos. Chem. Phys., 20, 5771–5785, https://doi.org/10.5194/acp-20-5771-2020, https://doi.org/10.5194/acp-20-5771-2020, 2020
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The bare black carbon (BC) was in a fractal structure. With coating thickness increasing, BC changed from a fractal structure to a core–shell structure. In the ambient atmosphere, plenty of BC particles were not in a perfect core–shell structure. This study brought attention to the combined effects of morphology and coating thickness on the absorption enhancement of BC-containing particles, which is helpful for determining the climatic effects of BC.
Yonghong Wang, Matthieu Riva, Hongbin Xie, Liine Heikkinen, Simon Schallhart, Qiaozhi Zha, Chao Yan, Xu-Cheng He, Otso Peräkylä, and Mikael Ehn
Atmos. Chem. Phys., 20, 5145–5155, https://doi.org/10.5194/acp-20-5145-2020, https://doi.org/10.5194/acp-20-5145-2020, 2020
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Chamber experiments were conducted with alpha-pinene and chlorine under low- and high-nitrogen-oxide (NOX) conditions. We estimated the HOM yields from chlorine-initiated oxidation of alpha-pinene under low-NOX conditions to be around 1.8 %, though with a uncertainty range (0.8 %–4 %) due to lack of suitable calibration methods. Our study clearly demonstrates that the chlorine-atom-initiated oxidation of alpha-pinene can produce low-volatility organic compounds.
Fanhao Meng, Min Qin, Ke Tang, Jun Duan, Wu Fang, Shuaixi Liang, Kaidi Ye, Pinhua Xie, Yele Sun, Conghui Xie, Chunxiang Ye, Pingqing Fu, Jianguo Liu, and Wenqing Liu
Atmos. Chem. Phys., 20, 5071–5092, https://doi.org/10.5194/acp-20-5071-2020, https://doi.org/10.5194/acp-20-5071-2020, 2020
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Nitrous acid (HONO), a major precursor of the OH radical, plays a key role in atmospheric chemistry, but its sources are still debated. The first high-resolution vertical measurements of HONO and NO2 were conducted in Beijing to investigate the nocturnal sources of HONO at different stages of pollution. The ground surface dominated HONO production by heterogeneous conversion of NO2 during clean episodes, but the aerosol production was an important nighttime HONO source during haze episodes.
Chenjie Yu, Dantong Liu, Kurtis Broda, Rutambhara Joshi, Jason Olfert, Yele Sun, Pingqing Fu, Hugh Coe, and James D. Allan
Atmos. Chem. Phys., 20, 3645–3661, https://doi.org/10.5194/acp-20-3645-2020, https://doi.org/10.5194/acp-20-3645-2020, 2020
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This study presents the first atmospheric application of a new morphology-independent measurement for the quantification of the mixing state of rBC-containing particles in urban Beijing as part of the UK–China APHH campaign. An inversion method has been applied for better quantification of rBC mixing state. The mass-resolved rBC mixing state information presented here has implications for detailed models of BC, its optical properties and its atmospheric life cycle.
Shaofeng Xu, Lujie Ren, Yunchao Lang, Shengjie Hou, Hong Ren, Lianfang Wei, Libin Wu, Junjun Deng, Wei Hu, Xiaole Pan, Yele Sun, Zifa Wang, Hang Su, Yafang Cheng, and Pingqing Fu
Atmos. Chem. Phys., 20, 3623–3644, https://doi.org/10.5194/acp-20-3623-2020, https://doi.org/10.5194/acp-20-3623-2020, 2020
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Current knowledge on the size distribution of biogenic primary organic aerosols in urban regions with heavy haze pollution is very limited. Here we performed a year-round study focusing on the organic molecular composition of size-segregated aerosol samples collected in urban Beijing during haze and non-haze days to elucidate the seasonal contributions of biomass burning, fungal spores, and plant debris to organic carbon as well as the influences from local emissions and long-range transport.
Leigh R. Crilley, Ajit Singh, Louisa J. Kramer, Marvin D. Shaw, Mohammed S. Alam, Joshua S. Apte, William J. Bloss, Lea Hildebrandt Ruiz, Pingqing Fu, Weiqi Fu, Shahzad Gani, Michael Gatari, Evgenia Ilyinskaya, Alastair C. Lewis, David Ng'ang'a, Yele Sun, Rachel C. W. Whitty, Siyao Yue, Stuart Young, and Francis D. Pope
Atmos. Meas. Tech., 13, 1181–1193, https://doi.org/10.5194/amt-13-1181-2020, https://doi.org/10.5194/amt-13-1181-2020, 2020
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There is considerable interest in using low-cost optical particle counters (OPCs) for particle mass measurements; however, there is no agreed upon method with respect to calibration. Here we exploit a number of datasets globally to demonstrate that particle composition and relative humidity are the key factors affecting measured concentrations from a low-cost OPC, and we present a simple correction methodology that corrects for this influence.
Lu Lei, Conghui Xie, Dawei Wang, Yao He, Qingqing Wang, Wei Zhou, Wei Hu, Pingqing Fu, Yong Chen, Xiaole Pan, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Chem. Phys., 20, 2877–2890, https://doi.org/10.5194/acp-20-2877-2020, https://doi.org/10.5194/acp-20-2877-2020, 2020
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We characterized aerosol composition and sources near two steel plants in a coastal region in fall and spring seasons. Our results showed substantially different aerosol composition and sources between the two seasons. We observed significant impacts of steel plant emissions on aerosol chemistry nearby, and we found that aerosol particles emitted from the steel plants were dominated by ammonium sulfate/bisulfate; NOx/CO and NOx/SO2 were distinct from those in the absence of industrial plumes.
Syuichi Itahashi, Baozhu Ge, Keiichi Sato, Joshua S. Fu, Xuemei Wang, Kazuyo Yamaji, Tatsuya Nagashima, Jie Li, Mizuo Kajino, Hong Liao, Meigen Zhang, Zhe Wang, Meng Li, Junichi Kurokawa, Gregory R. Carmichael, and Zifa Wang
Atmos. Chem. Phys., 20, 2667–2693, https://doi.org/10.5194/acp-20-2667-2020, https://doi.org/10.5194/acp-20-2667-2020, 2020
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This study gives an overview of acid deposition from the Model Inter-Comparison Study for Asia (MICS-Asia) phase III. Wet deposition simulated by a total of nine models is evaluated with observation data from the Acid Deposition Monitoring Network in East Asia (EANET). The total deposition maps comparing to emissions over Asia are presented. To seek a way to improve the model performance, ensemble approaches and the precipitation-adjusted method are discussed.
Zhining Tao, Mian Chin, Meng Gao, Tom Kucsera, Dongchul Kim, Huisheng Bian, Jun-ichi Kurokawa, Yuesi Wang, Zirui Liu, Gregory R. Carmichael, Zifa Wang, and Hajime Akimoto
Atmos. Chem. Phys., 20, 2319–2339, https://doi.org/10.5194/acp-20-2319-2020, https://doi.org/10.5194/acp-20-2319-2020, 2020
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One goal of the Model Inter-Comparison Study for Asia (MICS-Asia) Phase III is to identify strengths and weaknesses of current air quality models to provide insights into reducing uncertainties. This study identified that a 15 km grid would be the optimal horizontal resolution in terms of performance and resource usage to capture average and extreme air quality over East Asia and is thus suggested for use in future MICS-Asia modeling activities if the investigation domain remains the same.
Meng Gao, Zirui Liu, Bo Zheng, Dongsheng Ji, Peter Sherman, Shaojie Song, Jinyuan Xin, Cheng Liu, Yuesi Wang, Qiang Zhang, Jia Xing, Jingkun Jiang, Zifa Wang, Gregory R. Carmichael, and Michael B. McElroy
Atmos. Chem. Phys., 20, 1497–1505, https://doi.org/10.5194/acp-20-1497-2020, https://doi.org/10.5194/acp-20-1497-2020, 2020
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We quantified the relative influences of anthropogenic emissions and meteorological conditions on PM2.5 concentrations in Beijing over the winters of 2002–2016. Meteorological conditions over the study period would have led to an increase of haze in Beijing, but the strict emission control measures have suppressed the unfavorable influences of the recent climate.
Meng Gao, Zhiwei Han, Zhining Tao, Jiawei Li, Jeong-Eon Kang, Kan Huang, Xinyi Dong, Bingliang Zhuang, Shu Li, Baozhu Ge, Qizhong Wu, Hyo-Jung Lee, Cheol-Hee Kim, Joshua S. Fu, Tijian Wang, Mian Chin, Meng Li, Jung-Hun Woo, Qiang Zhang, Yafang Cheng, Zifa Wang, and Gregory R. Carmichael
Atmos. Chem. Phys., 20, 1147–1161, https://doi.org/10.5194/acp-20-1147-2020, https://doi.org/10.5194/acp-20-1147-2020, 2020
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Topic 3 of the Model Inter-Comparison Study for Asia (MICS-Asia) Phase III examines how online coupled air quality models perform in simulating high aerosol pollution in the North China Plain region during wintertime haze events and evaluates the importance of aerosol radiative feedbacks. This paper discusses the estimates of aerosol radiative forcing, aerosol feedbacks, and possible causes for the differences among the models.
Xinxin Fan, Jieyao Liu, Fang Zhang, Lu Chen, Don Collins, Weiqi Xu, Xiaoai Jin, Jingye Ren, Yuying Wang, Hao Wu, Shangze Li, Yele Sun, and Zhanqing Li
Atmos. Chem. Phys., 20, 915–929, https://doi.org/10.5194/acp-20-915-2020, https://doi.org/10.5194/acp-20-915-2020, 2020
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Aerosol effects on visibility and climate are influenced by their hygroscopicity. By contrasting data from two techniques between summer and winter in Beijing, we investigate the effect of aerosol aging, mixing state, and local sources on its hygroscopicity. We revealed that inappropriate use of the density of BC and organics results in large uncertainty in calculating aerosols hygroscopicity. Our results are helpful for parameterization in models.
Xiaoai Jin, Yuying Wang, Zhanqing Li, Fang Zhang, Weiqi Xu, Yele Sun, Xinxin Fan, Guangyu Chen, Hao Wu, Jingye Ren, Qiuyan Wang, and Maureen Cribb
Atmos. Chem. Phys., 20, 901–914, https://doi.org/10.5194/acp-20-901-2020, https://doi.org/10.5194/acp-20-901-2020, 2020
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In this study the aerosol liquid water content (ALWC) is determined from aerosol hygroscopic growth factor (GF) measurement (ALWCHTDMA) and also simulated by the ISORROPIA II thermodynamic model (ALWCISO). We found that ALWC contributed by organics (ALWCOrg) accounts for 30 % ± 22 % of the total ALWC in winter in Beijing. A case study reveals that ALWCOrg plays an important role in the formation of secondary aerosols through multiphase reactions at the initial stage of a heavy-haze episode.
Ye Kuang, Yao He, Wanyun Xu, Pusheng Zhao, Yafang Cheng, Gang Zhao, Jiangchuan Tao, Nan Ma, Hang Su, Yanyan Zhang, Jiayin Sun, Peng Cheng, Wenda Yang, Shaobin Zhang, Cheng Wu, Yele Sun, and Chunsheng Zhao
Atmos. Chem. Phys., 20, 865–880, https://doi.org/10.5194/acp-20-865-2020, https://doi.org/10.5194/acp-20-865-2020, 2020
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A new method was developed to calculate hygroscopicity parameter κ of organic aerosols (κOA) based on aerosol light-scattering measurements and bulk aerosol chemical-composition measurements. Derived high-time-resolution κOA varied in a wide range (near 0 to 0.25), and the organic aerosol oxidation degree significantly impacts variations in κOA. Distinct diurnal variation in κOA is found, and its relationship with oxygenated organic aerosol is discussed.
Lei Kong, Xiao Tang, Jiang Zhu, Zifa Wang, Joshua S. Fu, Xuemei Wang, Syuichi Itahashi, Kazuyo Yamaji, Tatsuya Nagashima, Hyo-Jung Lee, Cheol-Hee Kim, Chuan-Yao Lin, Lei Chen, Meigen Zhang, Zhining Tao, Jie Li, Mizuo Kajino, Hong Liao, Zhe Wang, Kengo Sudo, Yuesi Wang, Yuepeng Pan, Guiqian Tang, Meng Li, Qizhong Wu, Baozhu Ge, and Gregory R. Carmichael
Atmos. Chem. Phys., 20, 181–202, https://doi.org/10.5194/acp-20-181-2020, https://doi.org/10.5194/acp-20-181-2020, 2020
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Evaluation and uncertainty investigation of NO2, CO and NH3 modeling over China were conducted in this study using 14 chemical transport model results from MICS-Asia III. All models largely underestimated CO concentrations and showed very poor performance in reproducing the observed monthly variations of NH3 concentrations. Potential factors related to such deficiencies are investigated and discussed in this paper.
Yanbing Fan, Cong-Qiang Liu, Linjie Li, Lujie Ren, Hong Ren, Zhimin Zhang, Qinkai Li, Shuang Wang, Wei Hu, Junjun Deng, Libin Wu, Shujun Zhong, Yue Zhao, Chandra Mouli Pavuluri, Xiaodong Li, Xiaole Pan, Yele Sun, Zifa Wang, Kimitaka Kawamura, Zongbo Shi, and Pingqing Fu
Atmos. Chem. Phys., 20, 117–137, https://doi.org/10.5194/acp-20-117-2020, https://doi.org/10.5194/acp-20-117-2020, 2020
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This study provides useful knowledge on the abundance, sources, and formation processes of organic aerosols in the coastal megacity of Tianjin, North China, based on the investigation of the molecular composition, diurnal variation, and winter/summer differences under the influence of land/sea breezes and the Asian summer monsoon.
Danhui Xu, Baozhu Ge, Xueshun Chen, Yele Sun, Nianliang Cheng, Mei Li, Xiaole Pan, Zhiqiang Ma, Yuepeng Pan, and Zifa Wang
Atmos. Chem. Phys., 19, 15569–15581, https://doi.org/10.5194/acp-19-15569-2019, https://doi.org/10.5194/acp-19-15569-2019, 2019
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Wet deposition is one of the most important and efficient removal mechanisms in the evolution of the air pollution. Due to the lack of a localized parameterization scheme and some mechanisms being neglected in theoretical estimations and modeling calculations, below-cloud wet scavenging coefficients (BWSC) have large uncertainties. We compare the BWSCs under the same conditions to perform a multi-method evaluation in order to describe their characteristics.
Hang Liu, Xiaole Pan, Yu Wu, Dawei Wang, Yu Tian, Xiaoyong Liu, Lu Lei, Yele Sun, Pingqing Fu, and Zifa Wang
Atmos. Chem. Phys., 19, 14791–14804, https://doi.org/10.5194/acp-19-14791-2019, https://doi.org/10.5194/acp-19-14791-2019, 2019
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The relationship among the effective density, rBC's coating thickness, and rBC's morphology was investigated. rBC with larger effective density adopted a more regular shape due to more coating thickness. The effective density distribution of ambient rBC was also measured. From the information of effective density, the ambient rBC mainly adopts an irregular shape, which can cause large uncertainties in the rBC's optical properties.
Jie Li, Tatsuya Nagashima, Lei Kong, Baozhu Ge, Kazuyo Yamaji, Joshua S. Fu, Xuemei Wang, Qi Fan, Syuichi Itahashi, Hyo-Jung Lee, Cheol-Hee Kim, Chuan-Yao Lin, Meigen Zhang, Zhining Tao, Mizuo Kajino, Hong Liao, Meng Li, Jung-Hun Woo, Jun-ichi Kurokawa, Zhe Wang, Qizhong Wu, Hajime Akimoto, Gregory R. Carmichael, and Zifa Wang
Atmos. Chem. Phys., 19, 12993–13015, https://doi.org/10.5194/acp-19-12993-2019, https://doi.org/10.5194/acp-19-12993-2019, 2019
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This study evaluated and intercompared 14 CTMs with ozone observations in East Asia, within the framework of the Model Inter-Comparison Study for ASIA Phase III (MICS-Asia III). Potential causes of the discrepancies between model results and observation were investigated by assessing the planetary boundary layer heights, emission fluxes, dry deposition, chemistry and vertical transport among models. Finally, a multi-model estimate of pollution distributions was provided.
Mijung Song, Adrian M. Maclean, Yuanzhou Huang, Natalie R. Smith, Sandra L. Blair, Julia Laskin, Alexander Laskin, Wing-Sy Wong DeRieux, Ying Li, Manabu Shiraiwa, Sergey A. Nizkorodov, and Allan K. Bertram
Atmos. Chem. Phys., 19, 12515–12529, https://doi.org/10.5194/acp-19-12515-2019, https://doi.org/10.5194/acp-19-12515-2019, 2019
Lei Chen, Yi Gao, Meigen Zhang, Joshua S. Fu, Jia Zhu, Hong Liao, Jialin Li, Kan Huang, Baozhu Ge, Xuemei Wang, Yun Fat Lam, Chuan-Yao Lin, Syuichi Itahashi, Tatsuya Nagashima, Mizuo Kajino, Kazuyo Yamaji, Zifa Wang, and Jun-ichi Kurokawa
Atmos. Chem. Phys., 19, 11911–11937, https://doi.org/10.5194/acp-19-11911-2019, https://doi.org/10.5194/acp-19-11911-2019, 2019
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Simulated aerosol concentrations from 14 CTMs within the framework of MICS-Asia III are detailedly evaluated with an extensive set of measurements in East Asia. Similarities and differences among model performances are also analyzed. Although more considerable capacities for reproducing the aerosol concentrations and their variations are shown in current CTMs than those in MICS-Asia II, more efforts are needed to reduce diversities of simulated aerosol concentrations among air quality models.
Weiqi Xu, Conghui Xie, Eleni Karnezi, Qi Zhang, Junfeng Wang, Spyros N. Pandis, Xinlei Ge, Jingwei Zhang, Junling An, Qingqing Wang, Jian Zhao, Wei Du, Yanmei Qiu, Wei Zhou, Yao He, Ying Li, Jie Li, Pingqing Fu, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Chem. Phys., 19, 10205–10216, https://doi.org/10.5194/acp-19-10205-2019, https://doi.org/10.5194/acp-19-10205-2019, 2019
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We present the first aerosol volatility measurements in Beijing in summer using a thermodenuder coupled with aerosol mass spectrometers. Our results showed that organic aerosol (OA) comprised mainly semi-volatile organic compounds in summer, and the freshly oxidized secondary OA was the most volatile component. We also found quite different volatility distributions in black-carbon-containing primary and secondary OA, ambient OA, ambient secondary OA and the WRF-Chem model.
Erin Evoy, Adrian M. Maclean, Grazia Rovelli, Ying Li, Alexandra P. Tsimpidi, Vlassis A. Karydis, Saeid Kamal, Jos Lelieveld, Manabu Shiraiwa, Jonathan P. Reid, and Allan K. Bertram
Atmos. Chem. Phys., 19, 10073–10085, https://doi.org/10.5194/acp-19-10073-2019, https://doi.org/10.5194/acp-19-10073-2019, 2019
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We measured the diffusion rates of organic molecules in a number of proxies for secondary organic aerosol (SOA) and compared measured diffusion with predictions from two relations: the Stokes–Einstein relation and a fractional Stokes–Einstein relation. The fractional relation does a better job of predicting diffusion rates in this case. Output from an atmospheric model shows that mixing times predicted using the two relations differ by up to 1 order of magnitude at an altitude of ~ 3 km.
Michael Hollaway, Oliver Wild, Ting Yang, Yele Sun, Weiqi Xu, Conghui Xie, Lisa Whalley, Eloise Slater, Dwayne Heard, and Dantong Liu
Atmos. Chem. Phys., 19, 9699–9714, https://doi.org/10.5194/acp-19-9699-2019, https://doi.org/10.5194/acp-19-9699-2019, 2019
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This study, for the first time, uses combinations of aerosol and lidar data to drive an offline photolysis scheme. Absorbing species are shown to have the greatest impact on photolysis rate constants in the winter and scattering aerosol are shown to dominate responses in the summer. During haze episodes, aerosols are shown to produce a greater impact than cloud cover. The findings demonstrate the potential photochemical impacts of haze pollution in a highly polluted urban environment.
Huiyun Du, Jie Li, Xueshun Chen, Zifa Wang, Yele Sun, Pingqing Fu, Jianjun Li, Jian Gao, and Ying Wei
Atmos. Chem. Phys., 19, 9351–9370, https://doi.org/10.5194/acp-19-9351-2019, https://doi.org/10.5194/acp-19-9351-2019, 2019
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Regional transport and heterogeneous reactions play crucial roles in haze formation. Using a chemical transport model, we found that chemical transformation of SO2 along the transport pathway from source regions to Beijing was the major source of sulfate. Heterogeneous chemistry had a stronger effect under high humidity and high pollution levels. Aerosols underwent aging during transport which altered the aerosol size and the degree of aging.
Olli-Pekka Tikkanen, Väinö Hämäläinen, Grazia Rovelli, Antti Lipponen, Manabu Shiraiwa, Jonathan P. Reid, Kari E. J. Lehtinen, and Taina Yli-Juuti
Atmos. Chem. Phys., 19, 9333–9350, https://doi.org/10.5194/acp-19-9333-2019, https://doi.org/10.5194/acp-19-9333-2019, 2019
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We assessed how well the organic aerosol particle composition and viscosity can be captured by optimizing process models to match particle evaporation data. We performed the analysis for both artificial and real evaporation data and tested two optimization algorithms. Our findings show that the optimization method yields a good estimate for the studied properties. The timescale of the evaporation data and particle size was found to be important in identifying the volatility of organic compounds.
Duseong S. Jo, Alma Hodzic, Louisa K. Emmons, Eloise A. Marais, Zhe Peng, Benjamin A. Nault, Weiwei Hu, Pedro Campuzano-Jost, and Jose L. Jimenez
Geosci. Model Dev., 12, 2983–3000, https://doi.org/10.5194/gmd-12-2983-2019, https://doi.org/10.5194/gmd-12-2983-2019, 2019
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We developed a parameterization method for IEPOX-SOA based on the detailed chemical mechanism. Our parameterizations were tested using a box model and 3-D chemical transport model, which accurately captured the spatiotemporal distribution and response to changes in emissions compared to the explicit full chemistry, while being more computationally efficient. The method developed in this study can be applied to global climate models for long-term studies with a lower computational cost.
Tabish Umar Ansari, Oliver Wild, Jie Li, Ting Yang, Weiqi Xu, Yele Sun, and Zifa Wang
Atmos. Chem. Phys., 19, 8651–8668, https://doi.org/10.5194/acp-19-8651-2019, https://doi.org/10.5194/acp-19-8651-2019, 2019
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We explore the effectiveness of short-term emission controls on haze events in Beijing in October–November 2014 with high-resolution model studies. The model captures observed hourly variation in key pollutants well, but representation of boundary layer processes remains a key constraint. The controls contributed to improved air quality in early November but would not have been sufficient had the meteorology been less favourable. We quantify the much more stringent controls needed in that case.
Xiaole Pan, Hang Liu, Yu Wu, Yu Tian, Yele Sun, Conghui Xie, Xiaoyong Liu, Tianhai Cheng, and Zifa Wang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-433, https://doi.org/10.5194/acp-2019-433, 2019
Revised manuscript not accepted
Ying Wei, Xueshun Chen, Huansheng Chen, Jie Li, Zifa Wang, Wenyi Yang, Baozhu Ge, Huiyun Du, Jianqi Hao, Wei Wang, Jianjun Li, Yele Sun, and Huili Huang
Atmos. Chem. Phys., 19, 8269–8296, https://doi.org/10.5194/acp-19-8269-2019, https://doi.org/10.5194/acp-19-8269-2019, 2019
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This study presents a full description and evaluation of a global–regional nested aerosol and atmospheric chemistry model (IAP-AACM). The simulation for 2014 is evaluated against model datasets and a range of observational datasets. The results show that IAP-AACM is within the range of other models, and reproduces both spatial and seasonal variation of trace gases and aerosols over most areas well. In future, we recommend improving the model's ability to capture high spatial variation of PM2.5.
Zongbo Shi, Tuan Vu, Simone Kotthaus, Roy M. Harrison, Sue Grimmond, Siyao Yue, Tong Zhu, James Lee, Yiqun Han, Matthias Demuzere, Rachel E. Dunmore, Lujie Ren, Di Liu, Yuanlin Wang, Oliver Wild, James Allan, W. Joe Acton, Janet Barlow, Benjamin Barratt, David Beddows, William J. Bloss, Giulia Calzolai, David Carruthers, David C. Carslaw, Queenie Chan, Lia Chatzidiakou, Yang Chen, Leigh Crilley, Hugh Coe, Tie Dai, Ruth Doherty, Fengkui Duan, Pingqing Fu, Baozhu Ge, Maofa Ge, Daobo Guan, Jacqueline F. Hamilton, Kebin He, Mathew Heal, Dwayne Heard, C. Nicholas Hewitt, Michael Hollaway, Min Hu, Dongsheng Ji, Xujiang Jiang, Rod Jones, Markus Kalberer, Frank J. Kelly, Louisa Kramer, Ben Langford, Chun Lin, Alastair C. Lewis, Jie Li, Weijun Li, Huan Liu, Junfeng Liu, Miranda Loh, Keding Lu, Franco Lucarelli, Graham Mann, Gordon McFiggans, Mark R. Miller, Graham Mills, Paul Monk, Eiko Nemitz, Fionna O'Connor, Bin Ouyang, Paul I. Palmer, Carl Percival, Olalekan Popoola, Claire Reeves, Andrew R. Rickard, Longyi Shao, Guangyu Shi, Dominick Spracklen, David Stevenson, Yele Sun, Zhiwei Sun, Shu Tao, Shengrui Tong, Qingqing Wang, Wenhua Wang, Xinming Wang, Xuejun Wang, Zifang Wang, Lianfang Wei, Lisa Whalley, Xuefang Wu, Zhijun Wu, Pinhua Xie, Fumo Yang, Qiang Zhang, Yanli Zhang, Yuanhang Zhang, and Mei Zheng
Atmos. Chem. Phys., 19, 7519–7546, https://doi.org/10.5194/acp-19-7519-2019, https://doi.org/10.5194/acp-19-7519-2019, 2019
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APHH-Beijing is a collaborative international research programme to study the sources, processes and health effects of air pollution in Beijing. This introduction to the special issue provides an overview of (i) the APHH-Beijing programme, (ii) the measurement and modelling activities performed as part of it and (iii) the air quality and meteorological conditions during joint intensive field campaigns as a core activity within APHH-Beijing.
Linlin Wang, Junkai Liu, Zhiqiu Gao, Yubin Li, Meng Huang, Sihui Fan, Xiaoye Zhang, Yuanjian Yang, Shiguang Miao, Han Zou, Yele Sun, Yong Chen, and Ting Yang
Atmos. Chem. Phys., 19, 6949–6967, https://doi.org/10.5194/acp-19-6949-2019, https://doi.org/10.5194/acp-19-6949-2019, 2019
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Urban boundary layer (UBL) affects the physical and chemical processes of the pollutants, and UBL structure can also be altered by pollutants. This paper presents the interactions between air pollution and the UBL structure by using the field data mainly collected from a 325 m meteorology tower, as well as from a Doppler wind lidar, during a severe heavy pollution event that occurred during 1–4 December 2016 in Beijing.
Dantong Liu, Rutambhara Joshi, Junfeng Wang, Chenjie Yu, James D. Allan, Hugh Coe, Michael J. Flynn, Conghui Xie, James Lee, Freya Squires, Simone Kotthaus, Sue Grimmond, Xinlei Ge, Yele Sun, and Pingqing Fu
Atmos. Chem. Phys., 19, 6749–6769, https://doi.org/10.5194/acp-19-6749-2019, https://doi.org/10.5194/acp-19-6749-2019, 2019
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This study provides source attribution and characterization of BC in the Beijing urban environment in both winter and summer. For the first time, the physically and chemically based source apportionments are compared to evaluate the primary source contribution and secondary processing of BC-containing particles. A method is proposed to isolate the BC from the transportation sector and coal combustion sources.
Xionghui Qiu, Qi Ying, Shuxiao Wang, Lei Duan, Jian Zhao, Jia Xing, Dian Ding, Yele Sun, Baoxian Liu, Aijun Shi, Xiao Yan, Qingcheng Xu, and Jiming Hao
Atmos. Chem. Phys., 19, 6737–6747, https://doi.org/10.5194/acp-19-6737-2019, https://doi.org/10.5194/acp-19-6737-2019, 2019
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Current chemical transport models cannot capture the diurnal and nocturnal variation in atmospheric nitrate, which may be relative to the missing atmospheric chlorine chemistry. In this work, the Community Multiscale Air Quality (CMAQ) model with improved chlorine heterogeneous chemistry is applied to simulate the impact of chlorine chemistry on summer nitrate concentrations in Beijing. The results of this work can improve our understanding of nitrate formation.
Jialin Li, Meigen Zhang, Guiqian Tang, Yele Sun, Fangkun Wu, and Yongfu Xu
Atmos. Chem. Phys., 19, 6481–6495, https://doi.org/10.5194/acp-19-6481-2019, https://doi.org/10.5194/acp-19-6481-2019, 2019
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There are large uncertainties in the sources of secondary organic aerosol (SOA). Simulations of SOA concentrations in China with aqueous SOA formation pathway updated and glyoxal simulation improved reveal that dicarbonyl-derived SOA (AAQ) can explain a significant fraction of the unaccounted SOA sources. The mean AAQ can contribute 60.6 % and 64.5 % to the total concentration of SOA in summer and fall, respectively.
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.
Ying Li and Manabu Shiraiwa
Atmos. Chem. Phys., 19, 5959–5971, https://doi.org/10.5194/acp-19-5959-2019, https://doi.org/10.5194/acp-19-5959-2019, 2019
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Timescales for secondary organic aerosols (SOA) to reach equilibrium were estimated under various temperatures and relative humidities. Equilibration timescales in free troposphere can be longer than hours or days, even at moderate or relatively high relative humidities. These results provide critical insights into thermodynamic or kinetic treatments of SOA partitioning for accurate predictions of gas- and particle-phase concentrations of semi-volatile compounds in chemical transport models.
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
Kate R. Smith, Peter M. Edwards, Peter D. Ivatt, James D. Lee, Freya Squires, Chengliang Dai, Richard E. Peltier, Mat J. Evans, Yele Sun, and Alastair C. Lewis
Atmos. Meas. Tech., 12, 1325–1336, https://doi.org/10.5194/amt-12-1325-2019, https://doi.org/10.5194/amt-12-1325-2019, 2019
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Clusters of low-cost, low-power atmospheric gas sensors were built into a sensor instrument to monitor NO2 and O3 in Beijing, alongside reference instruments, aiming to improve the reliability of sensor measurements. Clustering identical sensors and using the median sensor signal was used to minimize drift over short and medium timescales. Three different machine learning techniques were used for all the sensor data in an attempt to correct for cross-interferences, which worked to some degree.
Hui Wang, Junmin Lin, Qizhong Wu, Huansheng Chen, Xiao Tang, Zifa Wang, Xueshun Chen, Huaqiong Cheng, and Lanning Wang
Geosci. Model Dev., 12, 749–764, https://doi.org/10.5194/gmd-12-749-2019, https://doi.org/10.5194/gmd-12-749-2019, 2019
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A new framework was designed for the widely used Carbon Bond Mechanism Z (CBM-Z) gas-phase chemical kinetics kernel to adapt the single-instruction, multiple-data (SIMD) technology in next-generation processors like Knights Landing (KNL) to improve their calculation performance. The optimization is aimed at implementing the fine-grain level parallelization of CBM-Z. The test results showed significant acceleration with our optimization on both CPU and KNL platforms.
Shino Toma, Steve Bertman, Christopher Groff, Fulizi Xiong, Paul B. Shepson, Paul Romer, Kaitlin Duffey, Paul Wooldridge, Ronald Cohen, Karsten Baumann, Eric Edgerton, Abigail R. Koss, Joost de Gouw, Allen Goldstein, Weiwei Hu, and Jose L. Jimenez
Atmos. Chem. Phys., 19, 1867–1880, https://doi.org/10.5194/acp-19-1867-2019, https://doi.org/10.5194/acp-19-1867-2019, 2019
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Acyl peroxy nitrates (APN) were measured near the ground in Alabama using GC in summer 2013 to study biosphere–atmosphere interactions. APN were lower than measured in the SE USA over the past 2 decades. Historical data showed APN in 2013 was limited by NOx and production was dominated by biogenic precursors more than in the past. Isoprene-derived MPAN correlated with isoprene hydroxynitrates as NOx-dependent products. MPAN varied with aerosol growth, but not with N-containing particles.
Shaojie Song, Meng Gao, Weiqi Xu, Yele Sun, Douglas R. Worsnop, John T. Jayne, Yuzhong Zhang, Lei Zhu, Mei Li, Zhen Zhou, Chunlei Cheng, Yibing Lv, Ying Wang, Wei Peng, Xiaobin Xu, Nan Lin, Yuxuan Wang, Shuxiao Wang, J. William Munger, Daniel J. Jacob, and Michael B. McElroy
Atmos. Chem. Phys., 19, 1357–1371, https://doi.org/10.5194/acp-19-1357-2019, https://doi.org/10.5194/acp-19-1357-2019, 2019
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Chemistry responsible for sulfate production in northern China winter haze remains mysterious. We propose a potentially key pathway through the reaction of formaldehyde and sulfur dioxide that has not been accounted for in previous studies. The special atmospheric conditions favor the formation and existence of their complex, hydroxymethanesulfonate (HMS).
Jun Chen, Zhanqing Li, Min Lv, Yuying Wang, Wei Wang, Yingjie Zhang, Haofei Wang, Xing Yan, Yele Sun, and Maureen Cribb
Atmos. Chem. Phys., 19, 1327–1342, https://doi.org/10.5194/acp-19-1327-2019, https://doi.org/10.5194/acp-19-1327-2019, 2019
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The hygroscopic growth function of aerosol particles is derived from Raman lidar, whose dependence on aerosol chemical composition is investigated using data from an aerosol chemical speciation monitor (ACSM) and a hygroscopic tandem differential mobility analyzer (H-TDMA) deployed in China. Two distinct cases were chosen with marked differences in their hygroscopic growth, which was fitted by the Kasten model. The differences were attributed to different amounts of chemical species.
Juhi Nagori, Ruud H. H. Janssen, Juliane L. Fry, Maarten Krol, Jose L. Jimenez, Weiwei Hu, and Jordi Vilà-Guerau de Arellano
Atmos. Chem. Phys., 19, 701–729, https://doi.org/10.5194/acp-19-701-2019, https://doi.org/10.5194/acp-19-701-2019, 2019
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Secondary organic aerosol (SOA) is produced through a complex interaction of sunlight, volatile organic compounds emitted from trees, anthropogenic emissions, and atmospheric chemistry. We are able to successfully model the formation and diurnal evolution of SOA using a model that takes into consideration the surface and boundary layer dynamics (1–2 km from the surface) and photochemistry above the southeastern US with data collected during the SOAS campaign to constrain the model.
Hajime Akimoto, Tatsuya Nagashima, Jie Li, Joshua S. Fu, Dongsheng Ji, Jiani Tan, and Zifa Wang
Atmos. Chem. Phys., 19, 603–615, https://doi.org/10.5194/acp-19-603-2019, https://doi.org/10.5194/acp-19-603-2019, 2019
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The regional model intercomparison study called MICS-Asia III revealed that substantial discrepancy still exists for surface ozone simulation in East Asia, even though common emissions, meteorological field, and boundary conditions have been used among the models. Three factors have been identified as possible causes of such discrepancy, (1) chemistry sub-models, (2) heterogeneous reactions, and (3) vertical transport parameters, and each component has been discussed.
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.
Qiang Huang, Jiubin Chen, Weilin Huang, John R. Reinfelder, Pingqing Fu, Shengliu Yuan, Zhongwei Wang, Wei Yuan, Hongming Cai, Hong Ren, Yele Sun, and Li He
Atmos. Chem. Phys., 19, 315–325, https://doi.org/10.5194/acp-19-315-2019, https://doi.org/10.5194/acp-19-315-2019, 2019
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Although the specific reactions and mechanisms in fine aerosols could not be explicitly determined from this field study, our results provide isotopic evidence that local daily photochemical reduction of divalent Hg is of critical importance to the fate of PM2.5-Hg in urban atmospheres and that, in addition to variation in sources, photochemical reduction appears to be an important process that affects both the particle mass-specific abundance and isotopic composition of PM2.5-Hg.
Xiaole Pan, Baozhu Ge, Zhe Wang, Yu Tian, Hang Liu, Lianfang Wei, Siyao Yue, Itsushi Uno, Hiroshi Kobayashi, Tomoaki Nishizawa, Atsushi Shimizu, Pingqing Fu, and Zifa Wang
Atmos. Chem. Phys., 19, 219–232, https://doi.org/10.5194/acp-19-219-2019, https://doi.org/10.5194/acp-19-219-2019, 2019
Conghui Xie, Weiqi Xu, Junfeng Wang, Qingqing Wang, Dantong Liu, Guiqian Tang, Ping Chen, Wei Du, Jian Zhao, Yingjie Zhang, Wei Zhou, Tingting Han, Qingyun Bian, Jie Li, Pingqing Fu, Zifa Wang, Xinlei Ge, James Allan, Hugh Coe, and Yele Sun
Atmos. Chem. Phys., 19, 165–179, https://doi.org/10.5194/acp-19-165-2019, https://doi.org/10.5194/acp-19-165-2019, 2019
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We present the first simultaneous real-time online measurements of aerosol optical properties at ground level and at 260 m on a meteorological tower in urban Beijing in winter. The vertical similarities and differences in scattering and absorption coefficients were characterized. The increases in MAC of BC were mainly associated with the coating materials on rBC. Coal combustion was the dominant source contribution of brown carbon followed by biomass burning and SOA in winter in Beijing.
Yu Tian, Xiaole Pan, Tomoaki Nishizawa, Hiroshi Kobayashi, Itsushi Uno, Xiquan Wang, Atsushi Shimizu, and Zifa Wang
Atmos. Chem. Phys., 18, 18203–18217, https://doi.org/10.5194/acp-18-18203-2018, https://doi.org/10.5194/acp-18-18203-2018, 2018
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East Asia is characterized by severe anthropogenic pollution and dust storms due to fuel consumption and the downwind location of dust sources. We studied the mixing states of dust and pollutants using an optical particle counter equipped with a polarization detection module, providing a deeper understanding of possible mechanisms of aerosols’ morphological change. In Beijing, the heterogeneous processes in the mixture of dust and emitted pollutants have a great influence on smog formation.
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.
Yingjie Zhang, Wei Du, Yuying Wang, Qingqing Wang, Haofei Wang, Haitao Zheng, Fang Zhang, Hongrong Shi, Yuxuan Bian, Yongxiang Han, Pingqing Fu, Francesco Canonaco, André S. H. Prévôt, Tong Zhu, Pucai Wang, Zhanqing Li, and Yele Sun
Atmos. Chem. Phys., 18, 14637–14651, https://doi.org/10.5194/acp-18-14637-2018, https://doi.org/10.5194/acp-18-14637-2018, 2018
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We have a comprehensive characterization of aerosol chemistry and particle growth events at a downwind site of a highly polluted city in the North China Plain. Aerosol particles at the urban downwind site were highly aged and mainly from secondary formation. New particle growth events were also frequently observed on both clean and polluted days. While both sulfate and SOA played important roles in particle growth during clean periods, SOA was more important than sulfate during polluted events.
Lei Liu, Jian Zhang, Liang Xu, Qi Yuan, Dao Huang, Jianmin Chen, Zongbo Shi, Yele Sun, Pingqing Fu, Zifa Wang, Daizhou Zhang, and Weijun Li
Atmos. Chem. Phys., 18, 14681–14693, https://doi.org/10.5194/acp-18-14681-2018, https://doi.org/10.5194/acp-18-14681-2018, 2018
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Using transmission electron microscopy, we studied individual cloud droplet residual and interstitial particles collected in cloud events at Mt. Tai in the polluted North China region. We found that individual cloud droplets were an extremely complicated mixture containing abundant refractory soot (i.e., black carbon), fly ash, and metals. The complicated cloud droplets have not been reported in clean continental or marine air before.
Mingjie Kang, Pingqing Fu, Kimitaka Kawamura, Fan Yang, Hongliang Zhang, Zhengchen Zang, Hong Ren, Lujie Ren, Ye Zhao, Yele Sun, and Zifa Wang
Atmos. Chem. Phys., 18, 13947–13967, https://doi.org/10.5194/acp-18-13947-2018, https://doi.org/10.5194/acp-18-13947-2018, 2018
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Molecular characterization and spatial distribution of biogenic primary organic aerosol (POA) and secondary organic aerosol (SOA) in the marine atmosphere are not well known. Here, we analysed the organic molecular composition of marine aerosols collected during a marine cruise in the East China Sea during May–June 2014. Our results suggest that the Asian continent can be a natural emitter of biogenic POA and SOA, which can be transported to the downwind marine atmosphere.
Suzane S. de Sá, Brett B. Palm, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Gabriel Isaacman-VanWertz, Lindsay D. Yee, Joel Brito, Samara Carbone, Igor O. Ribeiro, Glauber G. Cirino, Yingjun Liu, Ryan Thalman, Arthur Sedlacek, Aaron Funk, Courtney Schumacher, John E. Shilling, Johannes Schneider, Paulo Artaxo, Allen H. Goldstein, Rodrigo A. F. Souza, Jian Wang, Karena A. McKinney, Henrique Barbosa, M. Lizabeth Alexander, Jose L. Jimenez, and Scot T. Martin
Atmos. Chem. Phys., 18, 12185–12206, https://doi.org/10.5194/acp-18-12185-2018, https://doi.org/10.5194/acp-18-12185-2018, 2018
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This study aimed at understanding and quantifying the changes in mass concentration and composition of submicron airborne particulate matter (PM) in Amazonia due to urban pollution. Downwind of Manaus, PM concentrations increased by up to 200 % under polluted compared with background conditions. The observed changes included contributions from both primary and secondary processes. The differences in organic PM composition suggested a shift in the pathways of secondary production with pollution.
Yuying Wang, Zhanqing Li, Yingjie Zhang, Wei Du, Fang Zhang, Haobo Tan, Hanbing Xu, Tianyi Fan, Xiaoai Jin, Xinxin Fan, Zipeng Dong, Qiuyan Wang, and Yele Sun
Atmos. Chem. Phys., 18, 11739–11752, https://doi.org/10.5194/acp-18-11739-2018, https://doi.org/10.5194/acp-18-11739-2018, 2018
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Very different aerosol hygroscopicities and mixing states were found at these sites in the North China Plain. The PDF for 40–200 nm particles showed the particles were highly aged and internally mixed at Xingtai because of high pollution and strong photochemical reactions. A good proxy for the chemical comical composition (kappa = 0.31) in calculating CCN concentration was found. Importantly, our study investigated the influence of industrial emissions on the aerosol properties.
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.
Lindsay D. Yee, Gabriel Isaacman-VanWertz, Rebecca A. Wernis, Meng Meng, Ventura Rivera, Nathan M. Kreisberg, Susanne V. Hering, Mads S. Bering, Marianne Glasius, Mary Alice Upshur, Ariana Gray Bé, Regan J. Thomson, Franz M. Geiger, John H. Offenberg, Michael Lewandowski, Ivan Kourtchev, Markus Kalberer, Suzane de Sá, Scot T. Martin, M. Lizabeth Alexander, Brett B. Palm, Weiwei Hu, Pedro Campuzano-Jost, Douglas A. Day, Jose L. Jimenez, Yingjun Liu, Karena A. McKinney, Paulo Artaxo, Juarez Viegas, Antonio Manzi, Maria B. Oliveira, Rodrigo de Souza, Luiz A. T. Machado, Karla Longo, and Allen H. Goldstein
Atmos. Chem. Phys., 18, 10433–10457, https://doi.org/10.5194/acp-18-10433-2018, https://doi.org/10.5194/acp-18-10433-2018, 2018
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Biogenic volatile organic compounds react in the atmosphere to form secondary organic aerosol, yet the chemical pathways remain unclear. We collected filter samples and deployed a semi-volatile thermal desorption aerosol gas chromatograph in the central Amazon. We measured 30 sesquiterpenes and 4 diterpenes and find them to be important for reactive ozone loss. We estimate that sesquiterpene oxidation contributes at least 0.4–5 % (median 1 %) of observed submicron organic aerosol mass.
Yele Sun, Weiqi Xu, Qi Zhang, Qi Jiang, Francesco Canonaco, André S. H. Prévôt, Pingqing Fu, Jie Li, John Jayne, Douglas R. Worsnop, and Zifa Wang
Atmos. Chem. Phys., 18, 8469–8489, https://doi.org/10.5194/acp-18-8469-2018, https://doi.org/10.5194/acp-18-8469-2018, 2018
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We present a 2–year analysis of organic aerosol (OA) from highly time–resolved measurements by an aerosol chemical speciation monitor in the megacity of Beijing. The sources of OA were analyzed with the advanced factor analysis of a multilinear engine (ME-2). Our results showed very different seasonal patterns, relative humidity and temperature dependence, and sources regions among different OA factors. The sources and processes of OA factors, and their roles in haze pollution are elucidated.
Xiao-Xiao Zhang, Brenton Sharratt, Lian-You Liu, Zi-Fa Wang, Xiao-Le Pan, Jia-Qiang Lei, Shi-Xin Wu, Shuang-Yan Huang, Yu-Hong Guo, Jie Li, Xiao Tang, Ting Yang, Yu Tian, Xue-Shun Chen, Jian-Qi Hao, Hai-Tao Zheng, Yan-Yan Yang, and Yan-Li Lyu
Atmos. Chem. Phys., 18, 8353–8371, https://doi.org/10.5194/acp-18-8353-2018, https://doi.org/10.5194/acp-18-8353-2018, 2018
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The impact of a strong East Asian dust event during 2–7 May 2017 was quantified and assessed based upon environmental observations, lidar measurements, and satellite products along with simulation techniques. This dust storm impacted a wide area of China and other Asian nations and reached North America within 1 week. Dust storms are a significant contributor to the global dust budget. Asian dust storms such as that observed in early May 2017 may lead to wider climate forcing on a global scale.
Jie Zhang, Sara Lance, Jeffrey M. Freedman, Yele Sun, Brian A. Crandall, Xiuli Wei, and James J. Schwab
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-529, https://doi.org/10.5194/acp-2018-529, 2018
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The impact of fireworks (FW) events on air quality was studied using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and collocated instruments during the Independence Day (July 4) holiday. The Independence Day FW events resulted in significant increases in both organic and inorganic (potassium, sulfate, chloride) chemical components, and the contribution from different aerosol sources was discussed.
Shaojie Song, Meng Gao, Weiqi Xu, Jingyuan Shao, Guoliang Shi, Shuxiao Wang, Yuxuan Wang, Yele Sun, and Michael B. McElroy
Atmos. Chem. Phys., 18, 7423–7438, https://doi.org/10.5194/acp-18-7423-2018, https://doi.org/10.5194/acp-18-7423-2018, 2018
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Severe haze events occur frequently over northern China, especially in winter. Acidity plays a critical role in the formation of secondary PM2.5 and its toxicity. Using field measurements of gases and particles to critically evaluate two thermodynamic models routinely employed to determine particle acidity, we found that China's winter haze particles are generally within a moderately acidic range (pH 4–5) and not highly acidic (0) or neutral (7) as has been previously reported in the literature.
Jingye Ren, Fang Zhang, Yuying Wang, Don Collins, Xinxin Fan, Xiaoai Jin, Weiqi Xu, Yele Sun, Maureen Cribb, and Zhanqing Li
Atmos. Chem. Phys., 18, 6907–6921, https://doi.org/10.5194/acp-18-6907-2018, https://doi.org/10.5194/acp-18-6907-2018, 2018
Wing-Sy Wong DeRieux, Ying Li, Peng Lin, Julia Laskin, Alexander Laskin, Allan K. Bertram, Sergey A. Nizkorodov, and Manabu Shiraiwa
Atmos. Chem. Phys., 18, 6331–6351, https://doi.org/10.5194/acp-18-6331-2018, https://doi.org/10.5194/acp-18-6331-2018, 2018
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The phase transition of organic particles between glassy and semi-solid states occurs at the glass transition temperature. We developed a method to predict glass transition temperatures and the viscosity of secondary organic aerosols using molecular composition, with consistent results with viscosity measurements. The viscosity of biomass burning particles was also estimated using the chemical composition measured by high-resolution mass spectrometry with two different ionization techniques.
Meng Gao, Zhiwei Han, Zirui Liu, Meng Li, Jinyuan Xin, Zhining Tao, Jiawei Li, Jeong-Eon Kang, Kan Huang, Xinyi Dong, Bingliang Zhuang, Shu Li, Baozhu Ge, Qizhong Wu, Yafang Cheng, Yuesi Wang, Hyo-Jung Lee, Cheol-Hee Kim, Joshua S. Fu, Tijian Wang, Mian Chin, Jung-Hun Woo, Qiang Zhang, Zifa Wang, and Gregory R. Carmichael
Atmos. Chem. Phys., 18, 4859–4884, https://doi.org/10.5194/acp-18-4859-2018, https://doi.org/10.5194/acp-18-4859-2018, 2018
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Topic 3 of the Model Inter-Comparison Study for Asia (MICS-Asia) Phase III examines how online coupled air quality models perform in simulating high aerosol pollution in the North China Plain region during wintertime haze events and evaluates the importance of aerosol radiative and microphysical feedbacks. A comprehensive overview of the MICS-ASIA III Topic 3 study design is presented.
Wei Zhou, Qingqing Wang, Xiujuan Zhao, Weiqi Xu, Chen Chen, Wei Du, Jian Zhao, Francesco Canonaco, André S. H. Prévôt, Pingqing Fu, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Chem. Phys., 18, 3951–3968, https://doi.org/10.5194/acp-18-3951-2018, https://doi.org/10.5194/acp-18-3951-2018, 2018
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We present a 3-month analysis of submicron aerosols that were measured at 260 m on a meteorological tower in Beijing, China. The sources of organic aerosol (OA) were analyzed by using a multi-linear engine (ME-2). Our results showed significant changes in both primary and secondary OA composition from the non-heating season to the heating season. We also observed a considerable contribution (10–13%) of cooking OA at 260 m and very different OA composition between ground level and 260 m.
Wanyu Zhao, Kimitaka Kawamura, Siyao Yue, Lianfang Wei, Hong Ren, Yu Yan, Mingjie Kang, Linjie Li, Lujie Ren, Senchao Lai, Jie Li, Yele Sun, Zifa Wang, and Pingqing Fu
Atmos. Chem. Phys., 18, 2749–2767, https://doi.org/10.5194/acp-18-2749-2018, https://doi.org/10.5194/acp-18-2749-2018, 2018
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In this paper, we investigate the seasonal trends in concentrations and compound-specific stable carbon isotope ratios of low molecular weight dicarboxylic acids (C2–C12) and related compounds in fine aerosols (PM2.5) in Beijing. Our study demonstrates that, in addition to the production via photo-oxidation, high abundances of diacids and related compounds in Beijing are largely associated with anthropogenic primary emissions such as biomass burning, fossil fuel combustion and plastic burning.
Qingqing Wang, Yele Sun, Weiqi Xu, Wei Du, Libo Zhou, Guiqian Tang, Chen Chen, Xueling Cheng, Xiujuan Zhao, Dongsheng Ji, Tingting Han, Zhe Wang, Jie Li, and Zifa Wang
Atmos. Chem. Phys., 18, 2495–2509, https://doi.org/10.5194/acp-18-2495-2018, https://doi.org/10.5194/acp-18-2495-2018, 2018
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We conducted the first real-time continuous vertical measurements of particle extinction, NO2, and BC from ground level to 260 m during two severe winter haze episodes in urban Beijing, China. Our results show very complex and dynamic vertical profiles that interact closely with boundary layer and meteorological conditions. Further analysis demonstrate that vertical convection, temperature inversion, and local emissions are three major factors affecting the changes in vertical profiles.
Mallory L. Hinks, Julia Montoya-Aguilera, Lucas Ellison, Peng Lin, Alexander Laskin, Julia Laskin, Manabu Shiraiwa, Donald Dabdub, and Sergey A. Nizkorodov
Atmos. Chem. Phys., 18, 1643–1652, https://doi.org/10.5194/acp-18-1643-2018, https://doi.org/10.5194/acp-18-1643-2018, 2018
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We have observed a strong effect of relative humidity on the composition of particulate matter produced from the oxidation of toluene in clean air. At higher relative humidity, there was a significant reduction in the fraction of high-molecular-weight compounds present in the particles. The amount of particulate matter also decreased at higher relative humidity. The main implication of this study is that water vapor participates in the photooxidation of toluene in a complicated way.
Zheng Fang, Wei Deng, Yanli Zhang, Xiang Ding, Mingjin Tang, Tengyu Liu, Qihou Hu, Ming Zhu, Zhaoyi Wang, Weiqiang Yang, Zhonghui Huang, Wei Song, Xinhui Bi, Jianmin Chen, Yele Sun, Christian George, and Xinming Wang
Atmos. Chem. Phys., 17, 14821–14839, https://doi.org/10.5194/acp-17-14821-2017, https://doi.org/10.5194/acp-17-14821-2017, 2017
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Primary emissions and aging of open straw burning plumes were characterized in ambient dilution conditions in a chamber. Rich in alkenes, the plumes have high O3 formation potential. The emissions of specific particulate and gaseous compounds were less when the straws were fully burned. Organic aerosol (OA) mass increased by a factor of 2–8 with 3–9 h photo-oxidation, yet > 70 % of the mass cannot be explained by the known precursors. OA gained more O- and N-containing compounds during aging.
Yunjiang Zhang, Lili Tang, Philip L. Croteau, Olivier Favez, Yele Sun, Manjula R. Canagaratna, Zhuang Wang, Florian Couvidat, Alexandre Albinet, Hongliang Zhang, Jean Sciare, André S. H. Prévôt, John T. Jayne, and Douglas R. Worsnop
Atmos. Chem. Phys., 17, 14501–14517, https://doi.org/10.5194/acp-17-14501-2017, https://doi.org/10.5194/acp-17-14501-2017, 2017
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We conducted the first field measurements of non-refractory fine aerosols (NR-PM2.5) in a megacity of eastern China using a PM2.5-ACSM along with a PM1-ACSM measurement. Inter-comparisons demonstrated that the NR-PM2.5 components can be characterized. Substantial mass fractions of aerosol species were observed in the size range of 1–2.5 μm, with sulfate and SOA being the two largest contributors. The impacts of aerosol water driven by secondary inorganic aerosols on SOA formation were explored.
Man Mei Chim, Chiu Tung Cheng, James F. Davies, Thomas Berkemeier, Manabu Shiraiwa, Andreas Zuend, and Man Nin Chan
Atmos. Chem. Phys., 17, 14415–14431, https://doi.org/10.5194/acp-17-14415-2017, https://doi.org/10.5194/acp-17-14415-2017, 2017
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In this work, we report that methyl-substituted succinic acid present at or near the surface of aqueous organic droplets can be efficiently oxidized by gas-phase OH radicals. The alkoxy radical chemistry appears to be an important reaction pathway. In addition, our model simulations reveal the relative importance of functionalization and fragmentation processes, alongside volatilization, in the evolution of the particle-phase reaction, which is largely dependent on the extent of oxidation.
Xiaole Pan, Yugo Kanaya, Fumikazu Taketani, Takuma Miyakawa, Satoshi Inomata, Yuichi Komazaki, Hiroshi Tanimoto, Zhe Wang, Itsushi Uno, and Zifa Wang
Atmos. Chem. Phys., 17, 13001–13016, https://doi.org/10.5194/acp-17-13001-2017, https://doi.org/10.5194/acp-17-13001-2017, 2017
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Characteristics of refractory black carbon (rBC) from open biomass burning (OBB) have a great impact on regional pollution and climate, in particular in East Asia. However, experimental study on characteristics of rBC from agricultural residue burning in East China was limited. This study performed laboratory experiments: we found that emission of rBC is highly related to flaming burning, and non-rBC to smoldering burning. Rapid condensation of semi-volatile organics resulted in coated rBC.
Qing Mu, Gerhard Lammel, Christian N. Gencarelli, Ian M. Hedgecock, Ying Chen, Petra Přibylová, Monique Teich, Yuxuan Zhang, Guangjie Zheng, Dominik van Pinxteren, Qiang Zhang, Hartmut Herrmann, Manabu Shiraiwa, Peter Spichtinger, Hang Su, Ulrich Pöschl, and Yafang Cheng
Atmos. Chem. Phys., 17, 12253–12267, https://doi.org/10.5194/acp-17-12253-2017, https://doi.org/10.5194/acp-17-12253-2017, 2017
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Polycyclic aromatic hydrocarbons (PAHs) are hazardous pollutants with the largest emissions in East Asia. The regional WRF-Chem-PAH model has been developed to reflect the state-of-the-art understanding of current PAHs studies with several new or updated features. It is able to reasonably well simulate the concentration levels and particulate mass fractions of PAHs near the sources and at a remote outflow region of East Asia, in high spatial and temporal resolutions.
Wei Hu, Min Hu, Wei-Wei Hu, Jing Zheng, Chen Chen, Yusheng Wu, and Song Guo
Atmos. Chem. Phys., 17, 9979–10000, https://doi.org/10.5194/acp-17-9979-2017, https://doi.org/10.5194/acp-17-9979-2017, 2017
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Seasonal changes in chemical compositions, sources, and evolution for submicron aerosols in the megacity Beijing were investigated based on high-resolution AMS measurements. Carbonaceous fraction (OA+BC) constituted over 50 % of PM1 in autumn due to primary emissions, while SNA contributed 60 % to PM1 in other seasons. Secondary components (OOA+SNA) contributed ~ 60–80 % to PM1, suggesting that secondary formation played an important role in PM pollution. OA was in a relatively high oxidation state.
Weiwei Hu, Pedro Campuzano-Jost, Douglas A. Day, Philip Croteau, Manjula R. Canagaratna, John T. Jayne, Douglas R. Worsnop, and Jose L. Jimenez
Atmos. Meas. Tech., 10, 2897–2921, https://doi.org/10.5194/amt-10-2897-2017, https://doi.org/10.5194/amt-10-2897-2017, 2017
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Aerosol mass spectrometers (AMS) from ARI are used widely to measure the non-refractory species in PM1. Recently, a new capture vapourizer (CV) has been designed to reduce the need for a bounce-related CE correction in the commonly used standard vapourizer (SV) installed in AMS. To test the CV, the fragments, CE and size distributions of four pure inorganic species in the CV-AMS are investigated in various laboratory experiments. Results from the co-located SV-AMS are also shown as a comparison.
Yujiao Zhu, Caiqing Yan, Renyi Zhang, Zifa Wang, Mei Zheng, Huiwang Gao, Yang Gao, and Xiaohong Yao
Atmos. Chem. Phys., 17, 9469–9484, https://doi.org/10.5194/acp-17-9469-2017, https://doi.org/10.5194/acp-17-9469-2017, 2017
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This study reports the distinct effects of street canyons on new particle formation (NPF) under warm or cold ambient temperature conditions because of on-road vehicle emissions; i.e., stronger condensation sinks are responsible for the reduced NPF in the springtime, but efficient nucleation and partitioning of gaseous species contribute to the enhanced NPF in the wintertime. The oxidization of biogenic organics is suggested to play an important role in growing new particles.
Hui Wang, Huansheng Chen, Qizhong Wu, Junmin Lin, Xueshun Chen, Xinwei Xie, Rongrong Wang, Xiao Tang, and Zifa Wang
Geosci. Model Dev., 10, 2891–2904, https://doi.org/10.5194/gmd-10-2891-2017, https://doi.org/10.5194/gmd-10-2891-2017, 2017
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We introduced some methods to port our Global Nested Air Quality Prediction Modeling System (GNAQPMS) model on Intel Knight Landing (KNL). In this paper, we introduced both common and specific methods to accelerate out model better. With the guidance of the resources material on Intel Websites (http://www.intel.com/content/www/us/en/products/processors/xeon-phi.html) and relative books, this paper could be an example for the model developers to take advantage of KNL for their model.
Thomas Berkemeier, Markus Ammann, Ulrich K. Krieger, Thomas Peter, Peter Spichtinger, Ulrich Pöschl, Manabu Shiraiwa, and Andrew J. Huisman
Atmos. Chem. Phys., 17, 8021–8029, https://doi.org/10.5194/acp-17-8021-2017, https://doi.org/10.5194/acp-17-8021-2017, 2017
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Kinetic process models are efficient tools used to unravel the mechanisms governing chemical and physical transformation in multiphase atmospheric chemistry. However, determination of kinetic parameters such as reaction rate or diffusion coefficients from multiple data sets is often difficult or ambiguous. This study presents a novel optimization algorithm and framework to determine these parameters in an automated fashion and to gain information about parameter uncertainty and uniqueness.
Wei Du, Jian Zhao, Yuying Wang, Yingjie Zhang, Qingqing Wang, Weiqi Xu, Chen Chen, Tingting Han, Fang Zhang, Zhanqing Li, Pingqing Fu, Jie Li, Zifa Wang, and Yele Sun
Atmos. Chem. Phys., 17, 6797–6811, https://doi.org/10.5194/acp-17-6797-2017, https://doi.org/10.5194/acp-17-6797-2017, 2017
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We conducted the first simultaneous measurements of size-resolved particle number concentrations at ground level and 260 m in urban Beijing. The vertical differences strongly depend on particle sizes, with accumulation-mode particles being highly correlated at the two heights. We further demonstrated that regional emission controls have a dominant impact on accumulation-mode particles, while the influences on Aitken particles were much smaller due to the enhanced NPF events.
Suzane S. de Sá, Brett B. Palm, Pedro Campuzano-Jost, Douglas A. Day, Matthew K. Newburn, Weiwei Hu, Gabriel Isaacman-VanWertz, Lindsay D. Yee, Ryan Thalman, Joel Brito, Samara Carbone, Paulo Artaxo, Allen H. Goldstein, Antonio O. Manzi, Rodrigo A. F. Souza, Fan Mei, John E. Shilling, Stephen R. Springston, Jian Wang, Jason D. Surratt, M. Lizabeth Alexander, Jose L. Jimenez, and Scot T. Martin
Atmos. Chem. Phys., 17, 6611–6629, https://doi.org/10.5194/acp-17-6611-2017, https://doi.org/10.5194/acp-17-6611-2017, 2017
Ting Yang, Zifa Wang, Wei Zhang, Alex Gbaguidi, Nobuo Sugimoto, Xiquan Wang, Ichiro Matsui, and Yele Sun
Atmos. Chem. Phys., 17, 6215–6225, https://doi.org/10.5194/acp-17-6215-2017, https://doi.org/10.5194/acp-17-6215-2017, 2017
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Predicting air pollution events over megacities requires, notably, continuous and accurate determination of the boundary layer height (BLH). Based on gravity wave theory, a new approach (CRGM) is developed to overcome existing algorithms' weakness in order to accurately reproduce the fluctuations of the BLH under various atmospheric pollution conditions from lidar observation. Comprehensive evaluation highlights strong effectiveness of this new method.
Yuying Wang, Fang Zhang, Zhanqing Li, Haobo Tan, Hanbing Xu, Jingye Ren, Jian Zhao, Wei Du, and Yele Sun
Atmos. Chem. Phys., 17, 5239–5251, https://doi.org/10.5194/acp-17-5239-2017, https://doi.org/10.5194/acp-17-5239-2017, 2017
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A series of strict emission control measures were implemented in Beijing and the surrounding seven provinces to ensure good air quality during the 2015 China Victory Day parade, rendering a unique opportunity to investigate anthropogenic impact of aerosol properties. Submicron aerosol hygroscopicity and volatility were measured during and after the control period. By comparison we found aerosol particles became more hydrophobic and volatile due to the emission control measures.
Jian Zhao, Wei Du, Yingjie Zhang, Qingqing Wang, Chen Chen, Weiqi Xu, Tingting Han, Yuying Wang, Pingqing Fu, Zifa Wang, Zhanqing Li, and Yele Sun
Atmos. Chem. Phys., 17, 3215–3232, https://doi.org/10.5194/acp-17-3215-2017, https://doi.org/10.5194/acp-17-3215-2017, 2017
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We conducted aerosol particle composition measurements at ground level and 260 m with two aerosol mass spectrometers in Beijing during the 2015 China Victory Day parade. Our results showed a stronger impact of emission controls on inorganic aerosol than OA. A larger decrease in more oxidized SOA than the less oxidized one during the control period was also observed. Our results indicate that emission controls and the changes in meteorological conditions have affected SOA formation mechanisms.
Xiao-Xiao Zhang, Brenton Sharratt, Xi Chen, Zi-Fa Wang, Lian-You Liu, Yu-Hong Guo, Jie Li, Huan-Sheng Chen, and Wen-Yi Yang
Atmos. Chem. Phys., 17, 1699–1711, https://doi.org/10.5194/acp-17-1699-2017, https://doi.org/10.5194/acp-17-1699-2017, 2017
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To improve our understanding of the fate and transport of airborne dust, there is a need for long-term records of dust deposition and concentration. This study characterized the spatial and temporal distribution in dust deposition and concentration in central Asia. The occurrence of high dust deposition and concentration suggests this region is a potential contributor to the global dust budget. This work will strengthen our comprehension of aerosol transport in global desertification regions.
Shurui Chen, Liang Xu, Yinxiao Zhang, Bing Chen, Xinfeng Wang, Xiaoye Zhang, Mei Zheng, Jianmin Chen, Wenxing Wang, Yele Sun, Pingqing Fu, Zifa Wang, and Weijun Li
Atmos. Chem. Phys., 17, 1259–1270, https://doi.org/10.5194/acp-17-1259-2017, https://doi.org/10.5194/acp-17-1259-2017, 2017
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Many studies have focused on the unusually severe hazes instead of the more frequent light and moderate hazes (22–63 %) in winter in the North China Plain (NCP). The morphology, mixing state, and size of organic aerosols in the L & M hazes were characterized. We conclude that the direct emissions from residential coal stoves without any pollution controls in rural and urban outskirts contribute large amounts of primary OM particles to the regional L & M hazes in winter in the NCP.
Havala O. T. Pye, Benjamin N. Murphy, Lu Xu, Nga L. Ng, Annmarie G. Carlton, Hongyu Guo, Rodney Weber, Petros Vasilakos, K. Wyat Appel, Sri Hapsari Budisulistiorini, Jason D. Surratt, Athanasios Nenes, Weiwei Hu, Jose L. Jimenez, Gabriel Isaacman-VanWertz, Pawel K. Misztal, and Allen H. Goldstein
Atmos. Chem. Phys., 17, 343–369, https://doi.org/10.5194/acp-17-343-2017, https://doi.org/10.5194/acp-17-343-2017, 2017
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We use a chemical transport model to examine how organic compounds in the atmosphere interact with water present in particles. Organic compounds themselves lead to water uptake, and organic compounds interact with water associated with inorganic compounds in the rural southeast atmosphere. Including interactions of organic compounds with water requires a treatment of nonideality to more accurately represent aerosol observations during the Southern Oxidant and Aerosol Study (SOAS) 2013.
Biwu Chu, Xiao Zhang, Yongchun Liu, Hong He, Yele Sun, Jingkun Jiang, Junhua Li, and Jiming Hao
Atmos. Chem. Phys., 16, 14219–14230, https://doi.org/10.5194/acp-16-14219-2016, https://doi.org/10.5194/acp-16-14219-2016, 2016
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The interactive effects between inorganic and organic species under highly complex pollution conditions remain uncertain and were studied in a smog chamber. This study indicated that the synergistic formation of secondary inorganic and organic aerosol might increase the secondary aerosol load in the atmosphere and contribute haze pollution in eastern China. These synergistic effects were related to the heterogeneous process on aerosol surface and need to be considered in air quality models.
Wei Hu, Min Hu, Wei-Wei Hu, Hongya Niu, Jing Zheng, Yusheng Wu, Wentai Chen, Chen Chen, Lingyu Li, Min Shao, Shaodong Xie, and Yuanhang Zhang
Atmos. Chem. Phys., 16, 13213–13230, https://doi.org/10.5194/acp-16-13213-2016, https://doi.org/10.5194/acp-16-13213-2016, 2016
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An Aerodyne high-resolution time-of-flight AMS was deployed at a suburban site in the Sichuan Basin, southwestern China, under high emission intensity, and unique geographical and adverse meteorological conditions. OA was the most abundant component (36 %) in PM1, characterized by a relatively high oxidation state. The contributions of BBOA and BC to PM1 were high in primary emission episodes, highlighting the critical influence of biomass burning.
Andrea M. Arangio, Haijie Tong, Joanna Socorro, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 16, 13105–13119, https://doi.org/10.5194/acp-16-13105-2016, https://doi.org/10.5194/acp-16-13105-2016, 2016
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We have quantified environmentally persistent free radicals and reactive oxygen species (ROS) in size-segregated atmospheric aerosol particles. We suggest that ROS were formed by decomposition of secondary organic aerosols interacting with transition metal ions and quinones contained in humic-like substances. The results have significant implications for aqueous-phase and cloud processing of organic aerosols as well as adverse health effects upon respiratory deposition of aerosol particles.
Pascale S. J. Lakey, Thomas Berkemeier, Manuel Krapf, Josef Dommen, Sarah S. Steimer, Lisa K. Whalley, Trevor Ingham, Maria T. Baeza-Romero, Ulrich Pöschl, Manabu Shiraiwa, Markus Ammann, and Dwayne E. Heard
Atmos. Chem. Phys., 16, 13035–13047, https://doi.org/10.5194/acp-16-13035-2016, https://doi.org/10.5194/acp-16-13035-2016, 2016
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Chemical oxidation in the atmosphere removes pollutants and greenhouse gases but generates undesirable products such as secondary organic aerosol. Radicals are key intermediates in oxidation, but how they interact with aerosols is still not well understood. Here we use a laser to measure the loss of radicals onto oxidised aerosols generated in a smog chamber. The loss of radicals was controlled by the thickness or viscosity of the aerosols, confirmed by using sugar aerosols of known thickness.
Natasha Hodas, Andreas Zuend, Katherine Schilling, Thomas Berkemeier, Manabu Shiraiwa, Richard C. Flagan, and John H. Seinfeld
Atmos. Chem. Phys., 16, 12767–12792, https://doi.org/10.5194/acp-16-12767-2016, https://doi.org/10.5194/acp-16-12767-2016, 2016
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Discontinuities in apparent hygroscopicity below and above water saturation have been observed for organic and mixed organic-inorganic aerosol particles in both laboratory studies and in the ambient atmosphere. This work explores the extent to which such discontinuities are influenced by organic component molecular mass and viscosity, non-ideal thermodynamic interactions between aerosol components, and the combination of these factors.
Meng Gao, Gregory R. Carmichael, Pablo E. Saide, Zifeng Lu, Man Yu, David G. Streets, and Zifa Wang
Atmos. Chem. Phys., 16, 11837–11851, https://doi.org/10.5194/acp-16-11837-2016, https://doi.org/10.5194/acp-16-11837-2016, 2016
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The WRF-Chem model was used to examine how the winter PM2.5 concentrations change in response to changes in emissions and meteorology in North China from 1960 to 2010. The discussions in this study indicate that dramatic changes in emissions are the main cause of increasing haze events in North China, and long-term trends in atmospheric circulations maybe another important cause. We also found aerosol feedbacks have been significantly enhanced from 1960 to 2010, due to higher aerosol loadings.
Weiwei Hu, Brett B. Palm, Douglas A. Day, Pedro Campuzano-Jost, Jordan E. Krechmer, Zhe Peng, Suzane S. de Sá, Scot T. Martin, M. Lizabeth Alexander, Karsten Baumann, Lina Hacker, Astrid Kiendler-Scharr, Abigail R. Koss, Joost A. de Gouw, Allen H. Goldstein, Roger Seco, Steven J. Sjostedt, Jeong-Hoo Park, Alex B. Guenther, Saewung Kim, Francesco Canonaco, André S. H. Prévôt, William H. Brune, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 11563–11580, https://doi.org/10.5194/acp-16-11563-2016, https://doi.org/10.5194/acp-16-11563-2016, 2016
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IEPOX-SOA is biogenically derived secondary organic aerosol under anthropogenic influence, which has been shown to comprise a substantial fraction of OA globally. We investigated the lifetime of ambient IEPOX-SOA in the SE US and Amazonia, with an oxidation flow reactor and thermodenuder coupled with MS-based instrumentation. The low volatility and long lifetime of IEPOX-SOA against OH radicals' oxidation (> 2 weeks) was observed, which can help to constrain OA impact on air quality and climate.
Aki Pajunoja, Weiwei Hu, Yu J. Leong, Nathan F. Taylor, Pasi Miettinen, Brett B. Palm, Santtu Mikkonen, Don R. Collins, Jose L. Jimenez, and Annele Virtanen
Atmos. Chem. Phys., 16, 11163–11176, https://doi.org/10.5194/acp-16-11163-2016, https://doi.org/10.5194/acp-16-11163-2016, 2016
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The phase state of ambient particles was inferred from bounce measurements conducted at a rural site in central Alabama during the SOAS campaign. The organic-dominated ambient particles are mostly in the liquid phase at summertime conditions but they turn semisolid when dried in the measurement setup. Bounce humidograms reveal that the hygroscopicity and oxidation of the particles decreases the liquefying RH. The effect of oxidation is emphasized by oxidation flow reactor measurements.
Xiaole Pan, Itsushi Uno, Yukari Hara, Kazuo Osada, Shigekazu Yamamoto, Zhe Wang, Nobuo Sugimoto, Hiroshi Kobayashi, and Zifa Wang
Atmos. Chem. Phys., 16, 9863–9873, https://doi.org/10.5194/acp-16-9863-2016, https://doi.org/10.5194/acp-16-9863-2016, 2016
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Polarization properties of aerosol particles at a suburban site in the western Japan was studied on the basis of long-term observation and trajectory analysis. This study provides the detailed information on the polarization characteristics of particles from different origins, and proposed a reliable criterion to classify spherical and non-spherical particles. This study introduced a new method to investigate the mixed state of dust particle with anthropogenic pollutant.
Junfeng Wang, Xinlei Ge, Yanfang Chen, Yafei Shen, Qi Zhang, Yele Sun, Jianzhong Xu, Shun Ge, Huan Yu, and Mindong Chen
Atmos. Chem. Phys., 16, 9109–9127, https://doi.org/10.5194/acp-16-9109-2016, https://doi.org/10.5194/acp-16-9109-2016, 2016
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Highly time- and chemically resolved submicron aerosol properties were characterized online for the first time during springtime in Nanjing by using the Aerodyne SP-AMS. Both chemical and size information of black carbon together with other aerosol species were simultaneously determined. An in-depth analysis of the data elucidates the sources and evolution processes of the fine aerosols in the YRD region. Our findings are valuable for air quality remediation in the densely populated regions.
Yele Sun, Wei Du, Pingqing Fu, Qingqing Wang, Jie Li, Xinlei Ge, Qi Zhang, Chunmao Zhu, Lujie Ren, Weiqi Xu, Jian Zhao, Tingting Han, Douglas R. Worsnop, and Zifa Wang
Atmos. Chem. Phys., 16, 8309–8329, https://doi.org/10.5194/acp-16-8309-2016, https://doi.org/10.5194/acp-16-8309-2016, 2016
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We have a comprehensive characterization of the sources, variations and processes of submicron aerosols in Beijing in winter using HR-AMS and GC/MS measurements. The primary sources including traffic, cooking, biomass burning and coal combustion emissions, and secondary components were separated and quantified with PMF. Our results elucidated the important roles of primary emissions, particularly coal combustion, and aqueous-phase processing in the formation of severe air pollution in winter.
Amber M. Ortega, Patrick L. Hayes, Zhe Peng, Brett B. Palm, Weiwei Hu, Douglas A. Day, Rui Li, Michael J. Cubison, William H. Brune, Martin Graus, Carsten Warneke, Jessica B. Gilman, William C. Kuster, Joost de Gouw, Cándido Gutiérrez-Montes, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 7411–7433, https://doi.org/10.5194/acp-16-7411-2016, https://doi.org/10.5194/acp-16-7411-2016, 2016
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An oxidation flow reactor (OFR) was deployed to study secondary organic aerosol (SOA) formation and aging of urban emissions at a wide range of OH exposures during the CalNex campaign in Pasadena, CA, in 2010. Results include linking SOA formation to short-lived reactive compounds, similar elemental composition of reactor-aged emissions to atmospheric aging, changes in OA mass due to condensation of oxidized gas-phase species and heterogeneous oxidation of particle-phase species.
Xiao Tang, Jiang Zhu, ZiFa Wang, Alex Gbaguidi, CaiYan Lin, JinYuan Xin, Tao Song, and Bo Hu
Atmos. Chem. Phys., 16, 6395–6405, https://doi.org/10.5194/acp-16-6395-2016, https://doi.org/10.5194/acp-16-6395-2016, 2016
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Chemical data assimilation through adjusting precursor emissions has brought out notable impacts on improving ozone forecasts in previous studies. This paper, from another point of view, investigated in detail the impacts of adjusting nitrogen oxide emissions on the forecasts of nitrogen dioxide through assimilating ozone observations. Limitations of the existing chemical data assimilation methods in a highly nonlinear system were identified and highlighted.
Fang Zhang, Zhanqing Li, Yanan Li, Yele Sun, Zhenzhu Wang, Ping Li, Li Sun, Pucai Wang, Maureen Cribb, Chuanfeng Zhao, Tianyi Fan, Xin Yang, and Qingqing Wang
Atmos. Chem. Phys., 16, 5413–5425, https://doi.org/10.5194/acp-16-5413-2016, https://doi.org/10.5194/acp-16-5413-2016, 2016
Zhe Peng, Douglas A. Day, Amber M. Ortega, Brett B. Palm, Weiwei Hu, Harald Stark, Rui Li, Kostas Tsigaridis, William H. Brune, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 4283–4305, https://doi.org/10.5194/acp-16-4283-2016, https://doi.org/10.5194/acp-16-4283-2016, 2016
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Oxidation flow reactors (OFRs) are promising tools of studying atmospheric oxidation processes. Elevated concentrations of both OH and non-OH oxidants in OFRs leave room for speculation that non-OH chemistry can play a major role. Through systematic modeling, we find conditions where non-OH VOC fate is significant and show that, in most field studies of SOA using OFRs, non-OH VOC fate in OFRs was insignificant. We also provide guidelines helping OFR users avoid significant non-OH VOC oxidation.
Ying Li, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 16, 3327–3344, https://doi.org/10.5194/acp-16-3327-2016, https://doi.org/10.5194/acp-16-3327-2016, 2016
Wei Deng, Qihou Hu, Tengyu Liu, Xinming Wang, Yanli Zhang, Xiang Ding, Yele Sun, Xinhui Bi, Jianzhen Yu, Weiqiang Yang, Xinyu Huang, Zhou Zhang, Zhonghui Huang, Quanfu He, A. Mellouki, and Christian George
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2016-50, https://doi.org/10.5194/acp-2016-50, 2016
Revised manuscript not accepted
Haijie Tong, Andrea M. Arangio, Pascale S. J. Lakey, Thomas Berkemeier, Fobang Liu, Christopher J. Kampf, William H. Brune, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 16, 1761–1771, https://doi.org/10.5194/acp-16-1761-2016, https://doi.org/10.5194/acp-16-1761-2016, 2016
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We provide experimental evidence that terpene and isoprene SOA form substantial amounts of OH radicals upon interaction with liquid water and iron. Our measurements and model results imply that the chemical reactivity of SOA in the atmosphere, particularly in clouds, can be faster than previously thought. Inhalation and deposition of SOA particles in the human respiratory tract may lead to a substantial release of OH radicals in vivo, causing oxidative stress and adverse aerosol health effects.
M. Gao, G. R. Carmichael, Y. Wang, P. E. Saide, M. Yu, J. Xin, Z. Liu, and Z. Wang
Atmos. Chem. Phys., 16, 1673–1691, https://doi.org/10.5194/acp-16-1673-2016, https://doi.org/10.5194/acp-16-1673-2016, 2016
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The WRF-Chem model was applied to study the 2010 winter haze in North China. Air pollutants outside Beijing contributed about 64.5 % to the PM2.5 levels in Beijing during this haze event, and most of them are from south Hebei, Tianjin city, Shandong and Henan provinces. In addition, aerosol feedback has important impacts on surface temperature, Relative Humidity (RH) and wind speeds, and these meteorological variables affect aerosol distribution and formation in turn.
E. A. Marais, D. J. Jacob, J. L. Jimenez, P. Campuzano-Jost, D. A. Day, W. Hu, J. Krechmer, L. Zhu, P. S. Kim, C. C. Miller, J. A. Fisher, K. Travis, K. Yu, T. F. Hanisco, G. M. Wolfe, H. L. Arkinson, H. O. T. Pye, K. D. Froyd, J. Liao, and V. F. McNeill
Atmos. Chem. Phys., 16, 1603–1618, https://doi.org/10.5194/acp-16-1603-2016, https://doi.org/10.5194/acp-16-1603-2016, 2016
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Isoprene secondary organic aerosol (SOA) is a dominant aerosol component in the southeast US, but models routinely underestimate isoprene SOA with traditional schemes based on chamber studies operated under conditions not representative of isoprene-emitting forests. We develop a new irreversible uptake mechanism to reproduce isoprene SOA yields (3.3 %) and composition, and find a factor of 2 co-benefit of SO2 emission controls on reducing sulfate and organic aerosol in the southeast US.
T. Liu, X. Wang, Q. Hu, W. Deng, Y. Zhang, X. Ding, X. Fu, F. Bernard, Z. Zhang, S. Lü, Q. He, X. Bi, J. Chen, Y. Sun, J. Yu, P. Peng, G. Sheng, and J. Fu
Atmos. Chem. Phys., 16, 675–689, https://doi.org/10.5194/acp-16-675-2016, https://doi.org/10.5194/acp-16-675-2016, 2016
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The formation of SOA and sulfate aerosols from the photooxidation of gasoline vehicle exhaust (GVE) when mixing with SO2 was investigated in a smog chamber. We found that the presence of GVE enhanced the conversion of SO2 to sulfate predominantly through reactions with stabilized Criegee intermediates. On the other hand, the elevated particle acidity enhanced the SOA production from GVE. This study indicated that SO2 and GVE could enhance each other in forming secondary aerosols.
W. Q. Xu, Y. L. Sun, C. Chen, W. Du, T. T. Han, Q. Q. Wang, P. Q. Fu, Z. F. Wang, X. J. Zhao, L. B. Zhou, D. S. Ji, P. C. Wang, and D. R. Worsnop
Atmos. Chem. Phys., 15, 13681–13698, https://doi.org/10.5194/acp-15-13681-2015, https://doi.org/10.5194/acp-15-13681-2015, 2015
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We have investigated the response of aerosol composition, size distributions, and oxidation properties to emission controls during the 2014 Asia- Pacific Economic Cooperation (APEC) summit in Beijing. Our results showed substantial changes of aerosol bulk composition during APEC with the most reductions in secondary aerosols in large accumulation modes, demonstrating that that emission controls over regional scales can substantially reduce secondary particulates.
W. J. Li, S. R. Chen, Y. S. Xu, X. C. Guo, Y. L. Sun, X. Y. Yang, Z. F. Wang, X. D. Zhao, J. M. Chen, and W. X. Wang
Atmos. Chem. Phys., 15, 13365–13376, https://doi.org/10.5194/acp-15-13365-2015, https://doi.org/10.5194/acp-15-13365-2015, 2015
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We found that anthropogenic soot, fly ash, and visible organic particles likely adhere to the surface of secondary inorganic particles larger than 200nm due to coagulation. Biomass burning and coal combustion both constantly contribute to anthropogenic particles in the Qinghai-Tibet Plateau (QTP) background atmosphere. Organic coating and soot on the surface of the aged particles could have different impacts on their hygroscopic and optical properties in the QTP compared to the urban aerosols.
C. Chen, Y. L. Sun, W. Q. Xu, W. Du, L. B. Zhou, T. T. Han, Q. Q. Wang, P. Q. Fu, Z. F. Wang, Z. Q. Gao, Q. Zhang, and D. R. Worsnop
Atmos. Chem. Phys., 15, 12879–12895, https://doi.org/10.5194/acp-15-12879-2015, https://doi.org/10.5194/acp-15-12879-2015, 2015
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A comprehensive characterization of submicron aerosol composition and sources at 260m in urban Beijing during APEC 2014 is presented. Aerosol species were shown to decrease substantially by 40–80% during APEC, whereas the bulk composition was relatively similar to the result of synergetic controls of secondary precursors. Our results elucidated that the good air quality during APEC was the combined result of emission controls and meteorological effects, with the former playing the dominant role.
J. Zheng, J. Zhu, Z. Wang, F. Fang, C. C. Pain, and J. Xiang
Geosci. Model Dev., 8, 3421–3440, https://doi.org/10.5194/gmd-8-3421-2015, https://doi.org/10.5194/gmd-8-3421-2015, 2015
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A new anisotropic hr-adaptive mesh technique has been applied to modelling of multiscale transport phenomena. Over existing air quality models typically based on static-structured grids using a locally nesting technique, the advantage of the anisotropic hr-adaptive model has the ability to adapt the mesh according to the evolving pollutant distribution and flow features. To illustrate its capability, comparisons have been made between the results obtained using adaptive and uniform meshes.
W. Du, Y. L. Sun, Y. S. Xu, Q. Jiang, Q. Q. Wang, W. Yang, F. Wang, Z. P. Bai, X. D. Zhao, and Y. C. Yang
Atmos. Chem. Phys., 15, 10811–10824, https://doi.org/10.5194/acp-15-10811-2015, https://doi.org/10.5194/acp-15-10811-2015, 2015
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A fall field campaign was conducted at a national background site (3295m a.s.l.) over the Tibetan Plateau. The submicron aerosol was dominated by organics (43%) and sulfate (28%). Secondary organic aerosol (SOA) dominated OA (85%), 17% of which being aged biomass burning OA. New particle formation and growth events were frequently observed, with an average particle growth rate of 2.0nm per hour. The important role of organics in particle growth in the Tibetan Plateau was also demonstrated.
H. S. Chen, Z. F. Wang, J. Li, X. Tang, B. Z. Ge, X. L. Wu, O. Wild, and G. R. Carmichael
Geosci. Model Dev., 8, 2857–2876, https://doi.org/10.5194/gmd-8-2857-2015, https://doi.org/10.5194/gmd-8-2857-2015, 2015
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A new global nested atmospheric mercury transport model was developed and introduced. Model performance was found significantly better in North America and Europe than in East Asia. Nested simulation has been conducted in East Asia and shows improved skill at capturing the high spatial variability of Hg concentrations and deposition. The trans-boundary transport of Chinese primary anthropogenic mercury emissions was quantified for the first time.
Y. L. Sun, Z. F. Wang, W. Du, Q. Zhang, Q. Q. Wang, P. Q. Fu, X. L. Pan, J. Li, J. Jayne, and D. R. Worsnop
Atmos. Chem. Phys., 15, 10149–10165, https://doi.org/10.5194/acp-15-10149-2015, https://doi.org/10.5194/acp-15-10149-2015, 2015
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We conducted the first long-term real-time measurement of submicron aerosol composition in Beijing using an ACSM for 1 year. The seasonal variations of mass concentrations and chemical composition of submicron aerosol were investigated in detail, and the meteorological effects on aerosol chemistry, particularly temperature and relative humidity, were elucidated. Finally, the potential source areas of aerosol species during four seasons were identified.
Y. Tang, J. An, F. Wang, Y. Li, Y. Qu, Y. Chen, and J. Lin
Atmos. Chem. Phys., 15, 9381–9398, https://doi.org/10.5194/acp-15-9381-2015, https://doi.org/10.5194/acp-15-9381-2015, 2015
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High daytime HONO mixing ratios in experiments suggest that an unknown daytime HONO source (P unknown) could exist. P unknown≈19.60×NO2×J(NO2) was obtained using observed data from 13 field experiments across the globe, then coupled into the WRF-Chem model. Simulations indicated that elevated P unknown was found in the coastal regions of China; the additional HONO sources, especially the P unknown produced significant increases of radicals in the major cities, and accelerated the radical cycles.
E. F. Mikhailov, G. N. Mironov, C. Pöhlker, X. Chi, M. L. Krüger, M. Shiraiwa, J.-D. Förster, U. Pöschl, S. S. Vlasenko, T. I. Ryshkevich, M. Weigand, A. L. D. Kilcoyne, and M. O. Andreae
Atmos. Chem. Phys., 15, 8847–8869, https://doi.org/10.5194/acp-15-8847-2015, https://doi.org/10.5194/acp-15-8847-2015, 2015
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Our manuscript describes the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the ZOTTO in central Siberia (61º N, 89º E). The hygroscopic growth measurements were supplemented with chemical analyses of the samples. In addition, the microstructure and chemical composition of aerosol particles were analyzed by x-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM).
Y. R. Yang, X. G. Liu, Y. Qu, J. L. An, R. Jiang, Y. H. Zhang, Y. L. Sun, Z. J. Wu, F. Zhang, W. Q. Xu, and Q. X. Ma
Atmos. Chem. Phys., 15, 8165–8178, https://doi.org/10.5194/acp-15-8165-2015, https://doi.org/10.5194/acp-15-8165-2015, 2015
X. Pan, Y. Kanaya, H. Tanimoto, S. Inomata, Z. Wang, S. Kudo, and I. Uno
Atmos. Chem. Phys., 15, 6101–6111, https://doi.org/10.5194/acp-15-6101-2015, https://doi.org/10.5194/acp-15-6101-2015, 2015
Q. Jiang, Y. L. Sun, Z. Wang, and Y. Yin
Atmos. Chem. Phys., 15, 6023–6034, https://doi.org/10.5194/acp-15-6023-2015, https://doi.org/10.5194/acp-15-6023-2015, 2015
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Aerosol composition and sources during the Chinese spring festival are characterized in detail. The roles of fireworks and secondary aerosol in fine particle pollution were elucidated. We observed large reductions of primary species, whereas changes of secondary aerosol during the holiday period were minor. This has significant implications; reducing primary emissions on a local scale during severe haze episodes might have a limited effect on improving air quality in megacities.
M. J. Tang, M. Shiraiwa, U. Pöschl, R. A. Cox, and M. Kalberer
Atmos. Chem. Phys., 15, 5585–5598, https://doi.org/10.5194/acp-15-5585-2015, https://doi.org/10.5194/acp-15-5585-2015, 2015
Y. J. Zhang, L. L. Tang, Z. Wang, H. X. Yu, Y. L. Sun, D. Liu, W. Qin, F. Canonaco, A. S. H. Prévôt, H. L. Zhang, and H. C. Zhou
Atmos. Chem. Phys., 15, 1331–1349, https://doi.org/10.5194/acp-15-1331-2015, https://doi.org/10.5194/acp-15-1331-2015, 2015
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The chemical composition, sources, and evolution processes of PM1 were investigated with an Aerodyne ACSM during harvest seasons in the Yangtze River delta, China. Two biomass burning organic aerosol (BBOA) factors derived from PMF model were assessed. The oxidized BBOA contributes ~80% of the total BBOA loadings in the BB plumes. Evidence that BBOA may be oxidized to more aged and less volatile organics during the aging process was suggested.
T. Berkemeier, M. Shiraiwa, U. Pöschl, and T. Koop
Atmos. Chem. Phys., 14, 12513–12531, https://doi.org/10.5194/acp-14-12513-2014, https://doi.org/10.5194/acp-14-12513-2014, 2014
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Glassy organic particles can serve as ice nuclei at low temperatures. We provide a rationale for these findings using a numerical aerosol diffusion model that describes particle phase state and its kinetics during simulated atmospheric updrafts dependent upon composition, size, updraft velocity, temperature and humidity. Our simulations suggest that aerosols from anthropogenic aromatic organics can be particularly relevant for ice cloud formation.
Q. Z. Wu, W. S. Xu, A. J. Shi, Y. T. Li, X. J. Zhao, Z. F. Wang, J. X. Li, and L. N. Wang
Geosci. Model Dev., 7, 2243–2259, https://doi.org/10.5194/gmd-7-2243-2014, https://doi.org/10.5194/gmd-7-2243-2014, 2014
M. Shiraiwa, T. Berkemeier, K. A. Schilling-Fahnestock, J. H. Seinfeld, and U. Pöschl
Atmos. Chem. Phys., 14, 8323–8341, https://doi.org/10.5194/acp-14-8323-2014, https://doi.org/10.5194/acp-14-8323-2014, 2014
C. L. Loza, J. S. Craven, L. D. Yee, M. M. Coggon, R. H. Schwantes, M. Shiraiwa, X. Zhang, K. A. Schilling, N. L. Ng, M. R. Canagaratna, P. J. Ziemann, R. C. Flagan, and J. H. Seinfeld
Atmos. Chem. Phys., 14, 1423–1439, https://doi.org/10.5194/acp-14-1423-2014, https://doi.org/10.5194/acp-14-1423-2014, 2014
Y. Kanaya, H. Akimoto, Z.-F. Wang, P. Pochanart, K. Kawamura, Y. Liu, J. Li, Y. Komazaki, H. Irie, X.-L. Pan, F. Taketani, K. Yamaji, H. Tanimoto, S. Inomata, S. Kato, J. Suthawaree, K. Okuzawa, G. Wang, S. G. Aggarwal, P. Q. Fu, T. Wang, J. Gao, Y. Wang, and G. Zhuang
Atmos. Chem. Phys., 13, 8265–8283, https://doi.org/10.5194/acp-13-8265-2013, https://doi.org/10.5194/acp-13-8265-2013, 2013
K. Kawamura, E. Tachibana, K. Okuzawa, S. G. Aggarwal, Y. Kanaya, and Z. F. Wang
Atmos. Chem. Phys., 13, 8285–8302, https://doi.org/10.5194/acp-13-8285-2013, https://doi.org/10.5194/acp-13-8285-2013, 2013
Y. Zhang, K. Sartelet, S. Zhu, W. Wang, S.-Y. Wu, X. Zhang, K. Wang, P. Tran, C. Seigneur, and Z.-F. Wang
Atmos. Chem. Phys., 13, 6845–6875, https://doi.org/10.5194/acp-13-6845-2013, https://doi.org/10.5194/acp-13-6845-2013, 2013
N. He, K. Kawamura, K. Okuzawa, Y. Kanaya, and Z. F. Wang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-13-16699-2013, https://doi.org/10.5194/acpd-13-16699-2013, 2013
Revised manuscript not accepted
K. Kawamura, K. Okuzawa, S. G. Aggarwal, H. Irie, Y. Kanaya, and Z. Wang
Atmos. Chem. Phys., 13, 5369–5380, https://doi.org/10.5194/acp-13-5369-2013, https://doi.org/10.5194/acp-13-5369-2013, 2013
Y. L. Sun, Z. F. Wang, P. Q. Fu, T. Yang, Q. Jiang, H. B. Dong, J. Li, and J. J. Jia
Atmos. Chem. Phys., 13, 4577–4592, https://doi.org/10.5194/acp-13-4577-2013, https://doi.org/10.5194/acp-13-4577-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
Retrieval of refractive index and water content for the coating materials of aged black carbon aerosol based on optical properties: a theoretical analysis
Predicting hygroscopic growth of organosulfur aerosol particles using COSMOtherm
Dust aerosol from the Aralkum Desert influences the radiation budget and atmospheric dynamics of Central Asia
Global modeling of aerosol nucleation with a semi-explicit chemical mechanism for highly oxygenated organic molecules (HOMs)
Synergistic effects of the winter North Atlantic Oscillation (NAO) and El Niño–Southern Oscillation (ENSO) on dust activities in North China during the following spring
Aerosol composition, air quality, and boundary layer dynamics in the urban background of Stuttgart in winter
Measurement report: Source attribution and estimation of black carbon levels in an urban hotspot of the central Po Valley – an integrated approach combining high-resolution dispersion modelling and micro-aethalometers
Microphysical modelling of aerosol scavenging by different types of clouds: description and validation of the approach
Insights into the sources of ultrafine particle numbers at six European urban sites obtained by investigating COVID-19 lockdowns
In-plume and out-of-plume analysis of aerosol–cloud interactions derived from the 2014–2015 Holuhraun volcanic eruption
Impacts of atmospheric circulation patterns and cloud inhibition on aerosol radiative effect and boundary layer structure during winter air pollution in Sichuan Basin, China
Investigating the sign of stratocumulus adjustments to aerosols in the ICON global storm-resolving model
A model study investigating the sensitivity of aerosol forcing to the volatilities of semi-volatile organic compounds
Decomposing the effective radiative forcing of anthropogenic aerosols based on CMIP6 Earth system models
The role of interfacial tension in the size-dependent phase separation of atmospheric aerosol particles
Modeling impacts of dust mineralogy on fast climate response
Representation of iron aerosol size distributions is critical in evaluating atmospheric soluble iron input to the ocean
Uncertainties in laboratory-measured shortwave refractive indices of mineral dust aerosols and derived optical properties: a theoretical assessment
Diagnosing uncertainties in global biomass burning emission inventories and their impact on modeled air pollutants
Role of atmospheric aerosols in severe winter fog over the Indo-Gangetic Plain of India: a case study
Long-term variability in black carbon emissions constrained by gap-filled absorption aerosol optical depth and associated premature mortality in China
Intercomparison of aerosol optical depths from four reanalyses and their multi-reanalysis consensus
Global aviation contrail climate effects from 2019 to 2021
Multi-model effective radiative forcing of the 2020 sulphur cap for shipping
Rapid iodine oxoacid nucleation enhanced by dimethylamine in broad marine regions
Simulations of the impact of cloud condensation nuclei and ice-nucleating particles perturbations on the microphysics and radar reflectivity factor of stratiform mixed-phase clouds
Warming effects of reduced sulfur emissions from shipping
Aerosols in the central Arctic cryosphere: satellite and model integrated insights during Arctic spring and summer
Observationally constrained regional variations of shortwave absorption by iron oxides emphasize the cooling effect of dust
Droplet collection efficiencies inferred from satellite retrievals constrain effective radiative forcing of aerosol–cloud interactions
Global aerosol-type classification using a new hybrid algorithm and Aerosol Robotic Network data
Comparing the simulated influence of biomass burning plumes on low-level clouds over the southeastern Atlantic under varying smoke conditions
A global dust emission dataset for estimating dust radiative forcings in climate models
Improved simulations of biomass burning aerosol optical properties and lifetimes in the NASA GEOS Model during the ORACLES-I campaign
Revealing dominant patterns of aerosols regimes in the lower troposphere and their evolution from preindustrial times to the future in global climate model simulations
Sharp increase in Saharan dust intrusions over the western Euro-Mediterranean in February–March 2020–2022 and associated atmospheric circulation
Temporal and spatial variations in dust activity in Australia based on remote sensing and reanalysis datasets
Sensitivity of global direct aerosol shortwave radiative forcing to uncertainties in aerosol optical properties
Molecular-level study on the role of methanesulfonic acid in iodine oxoacid nucleation
Improving estimation of a record breaking East Asian dust storm emission with lagged aerosol Ångström Exponent observations
Regional to global distributions, trends, and drivers of biogenic volatile organic compound emission from 2001 to 2020
Impacts of ice-nucleating particles on cirrus clouds and radiation derived from global model simulations with MADE3 in EMAC
Seasonal characteristics of emission, distribution, and radiative effect of marine organic aerosols over the western Pacific Ocean: an investigation with a coupled regional climate aerosol model
Fire–precipitation interactions amplify the quasi-biennial variability in fires over southern Mexico and Central America
Improved estimates of smoke exposure during Australia fire seasons: importance of quantifying plume injection heights
New particle formation induced by anthropogenic–biogenic interactions on the southeastern Tibetan Plateau
Investigation of observed dust trends over the Middle East region in NASA Goddard Earth Observing System (GEOS) model simulations
Impact of Biomass Burning Aerosols (BBA) on the tropical African climate in an ocean-atmosphere-aerosols coupled climate model
A new process-based and scale-aware desert dust emission scheme for global climate models – Part II: Evaluation in the Community Earth System Model version 2 (CESM2)
The key role of atmospheric absorption in the Asian Summer Monsoon response to dust emissions in CMIP6 models
Jia Liu, Cancan Zhu, Donghui Zhou, and Jinbao Han
Atmos. Chem. Phys., 24, 12341–12354, https://doi.org/10.5194/acp-24-12341-2024, https://doi.org/10.5194/acp-24-12341-2024, 2024
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The hydrophilic coatings of aged black carbon (BC) particles absorb moisture during the hygroscopic growth process, but it is difficult to characterize how much water is absorbed under different relative humidities (RHs). In this study, we propose a method to obtain the water content in the coatings based on the equivalent complex refractive index retrieved from optical properties. This method is verified from a theoretical perspective, and it performs well for thickly coated BC at high RHs.
Zijun Li, Angela Buchholz, and Noora Hyttinen
Atmos. Chem. Phys., 24, 11717–11725, https://doi.org/10.5194/acp-24-11717-2024, https://doi.org/10.5194/acp-24-11717-2024, 2024
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Evaluating organosulfur (OS) hygroscopicity is important for assessing aerosol–cloud climate interactions in the post-fossil-fuel future, when SO2 emissions decrease and OS compounds become increasingly important. Here a state-of-the-art quantum-chemistry-based method was used to predict the hygroscopic growth factors (HGFs) of a group of atmospherically relevant OS compounds and their mixtures with (NH4)2SO4. A good agreement was observed between their model-estimated and experimental HGFs.
Jamie R. Banks, Bernd Heinold, and Kerstin Schepanski
Atmos. Chem. Phys., 24, 11451–11475, https://doi.org/10.5194/acp-24-11451-2024, https://doi.org/10.5194/acp-24-11451-2024, 2024
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The Aralkum is a new desert in Central Asia formed by the desiccation of the Aral Sea. This has created a source of atmospheric dust, with implications for the balance of solar and thermal radiation. Simulating these effects using a dust transport model, we find that Aralkum dust adds radiative cooling effects to the surface and atmosphere on average but also adds heating events. Increases in surface pressure due to Aralkum dust strengthen the Siberian High and weaken the summer Asian heat low.
Xinyue Shao, Minghuai Wang, Xinyi Dong, Yaman Liu, Wenxiang Shen, Stephen R. Arnold, Leighton A. Regayre, Meinrat O. Andreae, Mira L. Pöhlker, Duseong S. Jo, Man Yue, and Ken S. Carslaw
Atmos. Chem. Phys., 24, 11365–11389, https://doi.org/10.5194/acp-24-11365-2024, https://doi.org/10.5194/acp-24-11365-2024, 2024
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Highly oxygenated organic molecules (HOMs) play an important role in atmospheric new particle formation (NPF). By semi-explicitly coupling the chemical mechanism of HOMs and a comprehensive nucleation scheme in a global climate model, the updated model shows better agreement with measurements of nucleation rate, growth rate, and NPF event frequency. Our results reveal that HOM-driven NPF leads to a considerable increase in particle and cloud condensation nuclei burden globally.
Falei Xu, Shuang Wang, Yan Li, and Juan Feng
Atmos. Chem. Phys., 24, 10689–10705, https://doi.org/10.5194/acp-24-10689-2024, https://doi.org/10.5194/acp-24-10689-2024, 2024
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This study examines how the winter North Atlantic Oscillation (NAO) and El Niño–Southern Oscillation (ENSO) affect dust activities in North China during the following spring. The results show that the NAO and ENSO, particularly in their negative phases, greatly influence dust activities. When both are negative, their combined effect on dust activities is even greater. This research highlights the importance of these climate patterns in predicting spring dust activities in North China.
Hengheng Zhang, Wei Huang, Xiaoli Shen, Ramakrishna Ramisetty, Junwei Song, Olga Kiseleva, Christopher Claus Holst, Basit Khan, Thomas Leisner, and Harald Saathoff
Atmos. Chem. Phys., 24, 10617–10637, https://doi.org/10.5194/acp-24-10617-2024, https://doi.org/10.5194/acp-24-10617-2024, 2024
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Our study unravels how stagnant winter conditions elevate aerosol levels in Stuttgart. Cloud cover at night plays a pivotal role, impacting morning air quality. Validating a key model, our findings aid accurate air quality predictions, crucial for effective pollution mitigation in urban areas.
Giorgio Veratti, Alessandro Bigi, Michele Stortini, Sergio Teggi, and Grazia Ghermandi
Atmos. Chem. Phys., 24, 10475–10512, https://doi.org/10.5194/acp-24-10475-2024, https://doi.org/10.5194/acp-24-10475-2024, 2024
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In a study of two consecutive winter seasons, we used measurements and modelling tools to identify the levels and sources of black carbon pollution in a medium-sized urban area of the Po Valley, Italy. Our findings show that biomass burning and traffic-related emissions (especially from Euro 4 diesel cars) significantly contribute to BC concentrations. This research offers crucial insights for policymakers and urban planners aiming to improve air quality in cities.
Pascal Lemaitre, Arnaud Quérel, Alexis Dépée, Alice Guerra Devigne, Marie Monier, Thibault Hiron, Chloé Soto Minguez, Daniel Hardy, and Andrea Flossmann
Atmos. Chem. Phys., 24, 9713–9732, https://doi.org/10.5194/acp-24-9713-2024, https://doi.org/10.5194/acp-24-9713-2024, 2024
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A new in-cloud scavenging scheme is proposed. It is based on a microphysical model of cloud formation and may be applied to long-distance atmospheric transport models (> 100 km) and climatic models. This model is applied to the two most extreme precipitating cloud types in terms of both relative humidity and vertical extension: cumulonimbus and stratus.
Alex Rowell, James Brean, David C. S. Beddows, Tuukka Petäjä, Máté Vörösmarty, Imre Salma, Jarkko V. Niemi, Hanna E. Manninen, Dominik van Pinxteren, Thomas Tuch, Kay Weinhold, Zongbo Shi, and Roy M. Harrison
Atmos. Chem. Phys., 24, 9515–9531, https://doi.org/10.5194/acp-24-9515-2024, https://doi.org/10.5194/acp-24-9515-2024, 2024
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Different sources of airborne particles in the atmospheres of four European cities were distinguished by recognising their particle size distributions using a statistical procedure, positive matrix factorisation. The various sources responded differently to the changes in emissions associated with COVID-19 lockdowns, and the reasons are investigated. While traffic emissions generally decreased, particles formed from reactions of atmospheric gases decreased in some cities but increased in others.
Amy H. Peace, Ying Chen, George Jordan, Daniel G. Partridge, Florent Malavelle, Eliza Duncan, and Jim M. Haywood
Atmos. Chem. Phys., 24, 9533–9553, https://doi.org/10.5194/acp-24-9533-2024, https://doi.org/10.5194/acp-24-9533-2024, 2024
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Natural aerosols from volcanic eruptions can help us understand how anthropogenic aerosols modify climate. We use observations and model simulations of the 2014–2015 Holuhraun eruption plume to examine aerosol–cloud interactions in September 2014. We find a shift to clouds with smaller, more numerous cloud droplets in the first 2 weeks of the eruption. In the third week, the background meteorology and previous conditions experienced by air masses modulate the aerosol perturbation to clouds.
Hua Lu, Min Xie, Bingliang Zhuang, Danyang Ma, Bojun Liu, Yangzhihao Zhan, Tijian Wang, Shu Li, Mengmeng Li, and Kuanguang Zhu
Atmos. Chem. Phys., 24, 8963–8982, https://doi.org/10.5194/acp-24-8963-2024, https://doi.org/10.5194/acp-24-8963-2024, 2024
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To identify cloud, aerosol, and planetary boundary layer (PBL) interactions from an air quality perspective, we summarized two pollution patterns characterized by denser liquid cloud and by obvious cloud radiation interaction (CRI). Numerical simulation experiments showed CRI could cause a 50 % reduction in aerosol radiation interaction (ARI) under a low-trough system. The results emphasized the nonnegligible role of CRI and its inhibition of ARI under wet and cloudy pollution synoptic patterns.
Emilie Fons, Ann Kristin Naumann, David Neubauer, Theresa Lang, and Ulrike Lohmann
Atmos. Chem. Phys., 24, 8653–8675, https://doi.org/10.5194/acp-24-8653-2024, https://doi.org/10.5194/acp-24-8653-2024, 2024
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Aerosols can modify the liquid water path (LWP) of stratocumulus and, thus, their radiative effect. We compare storm-resolving model and satellite data that disagree on the sign of LWP adjustments and diagnose this discrepancy with causal inference. We find that strong precipitation, the absence of wet scavenging, and cloud deepening under a weak inversion contribute to positive LWP adjustments to aerosols in the model, despite weak negative effects from cloud-top entrainment enhancement.
Muhammed Irfan, Thomas Kühn, Taina Yli-Juuti, Anton Laakso, Eemeli Holopainen, Douglas R. Worsnop, Annele Virtanen, and Harri Kokkola
Atmos. Chem. Phys., 24, 8489–8506, https://doi.org/10.5194/acp-24-8489-2024, https://doi.org/10.5194/acp-24-8489-2024, 2024
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The study examines how the volatility of semi-volatile organic compounds affects secondary organic aerosol (SOA) formation and climate. Our simulations show that uncertainties in these volatilities influence aerosol mass and climate impacts. Accurate representation of these compounds in climate models is crucial for predicting global climate patterns.
Alkiviadis Kalisoras, Aristeidis K. Georgoulias, Dimitris Akritidis, Robert J. Allen, Vaishali Naik, Chaincy Kuo, Sophie Szopa, Pierre Nabat, Dirk Olivié, Twan van Noije, Philippe Le Sager, David Neubauer, Naga Oshima, Jane Mulcahy, Larry W. Horowitz, and Prodromos Zanis
Atmos. Chem. Phys., 24, 7837–7872, https://doi.org/10.5194/acp-24-7837-2024, https://doi.org/10.5194/acp-24-7837-2024, 2024
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Effective radiative forcing (ERF) is a metric for estimating how human activities and natural agents change the energy flow into and out of the Earth’s climate system. We investigate the anthropogenic aerosol ERF, and we estimate the contribution of individual processes to the total ERF using simulations from Earth system models within the Coupled Model Intercomparison Project Phase 6 (CMIP6). Our findings highlight that aerosol–cloud interactions drive ERF variability during the last 150 years.
Ryan Schmedding and Andreas Zuend
EGUsphere, https://doi.org/10.5194/egusphere-2024-1690, https://doi.org/10.5194/egusphere-2024-1690, 2024
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Four different approaches for computing the interfacial tension between liquid phases in aerosol particles were tested for particles with diameters from 10 nm to more than 5 μm. Antonov's rule led to the strongest reductions in the onset relative humidity of liquid–liquid phase separation and reproduced measured interfacial tensions for highly immiscible systems. A modified form of the Butler equation was able to best reproduce measured interfacial tensions in more miscible systems.
Qianqian Song, Paul Ginoux, María Gonçalves Ageitos, Ron L. Miller, Vincenzo Obiso, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 7421–7446, https://doi.org/10.5194/acp-24-7421-2024, https://doi.org/10.5194/acp-24-7421-2024, 2024
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We implement and simulate the distribution of eight dust minerals in the GFDL AM4.0 model. We found that resolving the eight minerals reduces dust absorption compared to the homogeneous dust used in the standard GFDL AM4.0 model that assumes a globally uniform hematite content of 2.7 % by volume. Resolving dust mineralogy results in significant impacts on radiation, land surface temperature, surface winds, and precipitation over North Africa in summer.
Mingxu Liu, Hitoshi Matsui, Douglas Hamilton, Sagar Rathod, Kara Lamb, and Natalie Mahowald
EGUsphere, https://doi.org/10.5194/egusphere-2024-1454, https://doi.org/10.5194/egusphere-2024-1454, 2024
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Atmospheric aerosol deposition provides iron to promote marine primary production, yet its amount remains highly uncertain. This study demonstrates that iron-containing particle size at emission is a critical factor in regulating their input to open oceans by performing global aerosol simulations. Further observational constraints on this are needed to reduce modelling uncertainties.
Senyi Kong, Zheng Wang, and Lei Bi
Atmos. Chem. Phys., 24, 6911–6935, https://doi.org/10.5194/acp-24-6911-2024, https://doi.org/10.5194/acp-24-6911-2024, 2024
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The retrieval of refractive indices of dust aerosols from laboratory optical measurements is commonly done assuming spherical particles. This paper aims to investigate the uncertainties in the shortwave refractive indices and corresponding optical properties by considering non-spherical and inhomogeneous models for dust samples. The study emphasizes the significance of using non-spherical models for simulating dust aerosols.
Wenxuan Hua, Sijia Lou, Xin Huang, Lian Xue, Ke Ding, Zilin Wang, and Aijun Ding
Atmos. Chem. Phys., 24, 6787–6807, https://doi.org/10.5194/acp-24-6787-2024, https://doi.org/10.5194/acp-24-6787-2024, 2024
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In this study, we diagnose uncertainties in carbon monoxide and organic carbon emissions from four inventories for seven major wildfire-prone regions. Uncertainties in vegetation classification methods, fire detection products, and cloud obscuration effects lead to bias in these biomass burning (BB) emission inventories. By comparing simulations with measurements, we provide certain inventory recommendations. Our study has implications for reducing uncertainties in emissions in further studies.
Chandrakala Bharali, Mary Barth, Rajesh Kumar, Sachin D. Ghude, Vinayak Sinha, and Baerbel Sinha
Atmos. Chem. Phys., 24, 6635–6662, https://doi.org/10.5194/acp-24-6635-2024, https://doi.org/10.5194/acp-24-6635-2024, 2024
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This study examines the role of atmospheric aerosols in winter fog over the Indo-Gangetic Plains of India using WRF-Chem. The increase in RH with aerosol–radiation feedback (ARF) is found to be important for fog formation as it promotes the growth of aerosols in the polluted environment. Aqueous-phase chemistry in the fog increases PM2.5 concentration, further affecting ARF. ARF and aqueous-phase chemistry affect the fog intensity and the timing of fog formation by ~1–2 h.
Wenxin Zhao, Yu Zhao, Yu Zheng, Dong Chen, Jinyuan Xin, Kaitao Li, Huizheng Che, Zhengqiang Li, Mingrui Ma, and Yun Hang
Atmos. Chem. Phys., 24, 6593–6612, https://doi.org/10.5194/acp-24-6593-2024, https://doi.org/10.5194/acp-24-6593-2024, 2024
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We evaluate the long-term (2000–2020) variabilities of aerosol absorption optical depth, black carbon emissions, and associated health risks in China with an integrated framework that combines multiple observations and modeling techniques. We demonstrate the remarkable emission abatement resulting from the implementation of national pollution controls and show how human activities affected the emissions with a spatiotemporal heterogeneity, thus supporting differentiated policy-making by region.
Peng Xian, Jeffrey S. Reid, Melanie Ades, Angela Benedetti, Peter R. Colarco, Arlindo da Silva, Tom F. Eck, Johannes Flemming, Edward J. Hyer, Zak Kipling, Samuel Rémy, Tsuyoshi Thomas Sekiyama, Taichu Tanaka, Keiya Yumimoto, and Jianglong Zhang
Atmos. Chem. Phys., 24, 6385–6411, https://doi.org/10.5194/acp-24-6385-2024, https://doi.org/10.5194/acp-24-6385-2024, 2024
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The study compares and evaluates monthly AOD of four reanalyses (RA) and their consensus (i.e., ensemble mean). The basic verification characteristics of these RA versus both AERONET and MODIS retrievals are presented. The study discusses the strength of each RA and identifies regions where divergence and challenges are prominent. The RA consensus usually performs very well on a global scale in terms of how well it matches the observational data, making it a good choice for various applications.
Roger Teoh, Zebediah Engberg, Ulrich Schumann, Christiane Voigt, Marc Shapiro, Susanne Rohs, and Marc E. J. Stettler
Atmos. Chem. Phys., 24, 6071–6093, https://doi.org/10.5194/acp-24-6071-2024, https://doi.org/10.5194/acp-24-6071-2024, 2024
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The radiative forcing (RF) due to aviation contrails is comparable to that caused by CO2. We estimate that global contrail net RF in 2019 was 62.1 mW m−2. This is ~1/2 the previous best estimate for 2018. Contrail RF varies regionally due to differences in conditions required for persistent contrails. COVID-19 reduced contrail RF by 54% in 2020 relative to 2019. Globally, 2 % of all flights account for 80 % of the annual contrail energy forcing, suggesting a opportunity to mitigate contrail RF.
Ragnhild Bieltvedt Skeie, Rachael Byrom, Øivind Hodnebrog, Caroline Jouan, and Gunnar Myhre
EGUsphere, https://doi.org/10.5194/egusphere-2024-1394, https://doi.org/10.5194/egusphere-2024-1394, 2024
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In 2020 new regulations by the International Maritime Organization of sulphur emissions came into force that reduced emissions of SO2 from the shipping sector by approximately 80 %. In this study, we use multiple models to calculate by how much the Earth energy balance changed due to the emission reduction, the so called effective radiative forcing. The calculated effective radiative forcing is weak, comparable to the effect of the increase in CO2 over the last two to three years.
Haotian Zu, Biwu Chu, Yiqun Lu, Ling Liu, and Xiuhui Zhang
Atmos. Chem. Phys., 24, 5823–5835, https://doi.org/10.5194/acp-24-5823-2024, https://doi.org/10.5194/acp-24-5823-2024, 2024
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The nucleation of iodic acid (HIO3) and iodous acid (HIO2) was proven to be critical in marine areas. However, HIO3–HIO2 nucleation cannot effectively derive the rapid nucleation in some polluted coasts. We find a significant enhancement of dimethylamine (DMA) on the HIO3–HIO2 nucleation in marine and polar regions with abundant DMA sources, which may establish reasonable connections between the HIO3–HIO2 nucleation and the rapid formation of new particles in polluted marine and polar regions.
Junghwa Lee, Patric Seifert, Tempei Hashino, Maximilian Maahn, Fabian Senf, and Oswald Knoth
Atmos. Chem. Phys., 24, 5737–5756, https://doi.org/10.5194/acp-24-5737-2024, https://doi.org/10.5194/acp-24-5737-2024, 2024
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Spectral bin model simulations of an idealized supercooled stratiform cloud were performed with the AMPS model for variable CCN and INP concentrations. We performed radar forward simulations with PAMTRA to transfer the simulations into radar observational space. The derived radar reflectivity factors were compared to observational studies of stratiform mixed-phase clouds. These studies report a similar response of the radar reflectivity factor to aerosol perturbations as we found in our study.
Masaru Yoshioka, Daniel P. Grosvenor, Ben B. B. Booth, Colin P. Morice, and Kenneth S. Carslaw
EGUsphere, https://doi.org/10.5194/egusphere-2024-1428, https://doi.org/10.5194/egusphere-2024-1428, 2024
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Sulfur emissions from shipping has been reduced by about 80 % as a result of the new regulation introduced in 2020. This has reduced aerosol in the atmosphere and its cooling effect through interactions with clouds. As a result, our coupled climate model simulations predict a global warming of 0.04 K averaged over three decades, potentially surpassing the Paris target of 1.5 K or contributing to recent temperature spikes, particularly notable in the Arctic with a mean warming of 0.15 K.
Basudev Swain, Marco Vountas, Aishwarya Singh, Nidhi L. Anchan, Adrien Deroubaix, Luca Lelli, Yanick Ziegler, Sachin S. Gunthe, Hartmut Bösch, and John P. Burrows
Atmos. Chem. Phys., 24, 5671–5693, https://doi.org/10.5194/acp-24-5671-2024, https://doi.org/10.5194/acp-24-5671-2024, 2024
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Arctic amplification (AA) accelerates the warming of the central Arctic cryosphere and affects aerosol dynamics. Limited observations hinder a comprehensive analysis. This study uses AEROSNOW aerosol optical density (AOD) data and GEOS-Chem simulations to assess AOD variability. Discrepancies highlight the need for improved observational integration into models to refine our understanding of aerosol effects on cloud microphysics, ice nucleation, and radiative forcing under evolving AA.
Vincenzo Obiso, María Gonçalves Ageitos, Carlos Pérez García-Pando, Jan P. Perlwitz, Gregory L. Schuster, Susanne E. Bauer, Claudia Di Biagio, Paola Formenti, Kostas Tsigaridis, and Ron L. Miller
Atmos. Chem. Phys., 24, 5337–5367, https://doi.org/10.5194/acp-24-5337-2024, https://doi.org/10.5194/acp-24-5337-2024, 2024
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We calculate the dust direct radiative effect (DRE) in an Earth system model accounting for regionally varying soil mineralogy through a new observationally constrained method. Linking dust absorption at solar wavelengths to the varying amount of specific minerals (i.e., iron oxides) improves the modeled range of dust single scattering albedo compared to observations and increases the global cooling by dust. Our results may contribute to improved estimates of the dust DRE and its climate impact.
Charlotte M. Beall, Po-Lun Ma, Matthew W. Christensen, Johannes Mülmenstädt, Adam Varble, Kentaroh Suzuki, and Takuro Michibata
Atmos. Chem. Phys., 24, 5287–5302, https://doi.org/10.5194/acp-24-5287-2024, https://doi.org/10.5194/acp-24-5287-2024, 2024
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Single-layer warm liquid clouds cover nearly one-third of the Earth's surface, and uncertainties regarding the impact of aerosols on their radiative properties pose a significant challenge to climate prediction. Here, we demonstrate how satellite observations can be used to constrain Earth system model estimates of the radiative forcing from the interactions of aerosols with clouds due to warm rain processes.
Xiaoli Wei, Qian Cui, Leiming Ma, Feng Zhang, Wenwen Li, and Peng Liu
Atmos. Chem. Phys., 24, 5025–5045, https://doi.org/10.5194/acp-24-5025-2024, https://doi.org/10.5194/acp-24-5025-2024, 2024
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A new aerosol-type classification algorithm has been proposed. It includes an optical database built by Mie scattering and a complex refractive index working as a baseline to identify different aerosol types. The new algorithm shows high accuracy and efficiency. Hence, a global map of aerosol types was generated to characterize aerosol types across the five continents. It will help improve the accuracy of aerosol inversion and determine the sources of aerosol pollution.
Alejandro Baró Pérez, Michael S. Diamond, Frida A.-M. Bender, Abhay Devasthale, Matthias Schwarz, Julien Savre, Juha Tonttila, Harri Kokkola, Hyunho Lee, David Painemal, and Annica M. L. Ekman
Atmos. Chem. Phys., 24, 4591–4610, https://doi.org/10.5194/acp-24-4591-2024, https://doi.org/10.5194/acp-24-4591-2024, 2024
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We use a numerical model to study interactions between humid light-absorbing aerosol plumes, clouds, and radiation over the southeast Atlantic. We find that the warming produced by the aerosols reduces cloud cover, especially in highly polluted situations. Aerosol impacts on drizzle play a minor role. However, aerosol effects on cloud reflectivity and moisture-induced changes in cloud cover dominate the climatic response and lead to an overall cooling by the biomass burning plumes.
Danny M. Leung, Jasper F. Kok, Longlei Li, David M. Lawrence, Natalie M. Mahowald, Simone Tilmes, and Erik Kluzek
EGUsphere, https://doi.org/10.5194/egusphere-2024-1124, https://doi.org/10.5194/egusphere-2024-1124, 2024
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This study derives a desert dust emission dataset for 1841–2000, by employing a combination of observed dust records from sedimentary cores as well as reanalyzed global dust cycle constraints. We evaluate the ability of global models to replicate the observed historical dust variability by using the emission dataset to force a historical simulation in an Earth system model. We show that prescribing our emissions forces the model to match better against observations than other mechanistic models.
Sampa Das, Peter R. Colarco, Huisheng Bian, and Santiago Gassó
Atmos. Chem. Phys., 24, 4421–4449, https://doi.org/10.5194/acp-24-4421-2024, https://doi.org/10.5194/acp-24-4421-2024, 2024
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The smoke aerosols emitted from vegetation burning can alter the regional energy budget via multiple pathways. We utilized detailed observations from the NASA ORACLES airborne campaign based in Namibia during September 2016 to improve the representation of smoke aerosol properties and lifetimes in our GEOS Earth system model. The improved model simulations are for the first time able to capture the observed changes in the smoke absorption during long-range plume transport.
Jingmin Li, Mattia Righi, Johannes Hendricks, Christof G. Beer, Ulrike Burkhardt, and Anja Schmidt
EGUsphere, https://doi.org/10.5194/egusphere-2024-1024, https://doi.org/10.5194/egusphere-2024-1024, 2024
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Aiming to understand underlying patterns and trends in aerosols, we characterize the spatial patterns and long-term evolution of lower tropospheric aerosols by clustering multiple aerosol properties from preindustrial times to the year 2050 under three SSP scenarios. The results provide a clear and condensed picture of the spatial extent and distribution of aerosols for different time periods and emission scenarios.
Emilio Cuevas-Agulló, David Barriopedro, Rosa Delia García, Silvia Alonso-Pérez, Juan Jesús González-Alemán, Ernest Werner, David Suárez, Juan José Bustos, Gerardo García-Castrillo, Omaira García, África Barreto, and Sara Basart
Atmos. Chem. Phys., 24, 4083–4104, https://doi.org/10.5194/acp-24-4083-2024, https://doi.org/10.5194/acp-24-4083-2024, 2024
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During February–March (FM) 2020–2022, unusually intense dust storms from northern Africa hit the western Euro-Mediterranean (WEM). Using dust products from satellites and atmospheric reanalysis for 2003–2022, results show that cut-off lows and European blocking are key drivers of FM dust intrusions over the WEM. A higher frequency of cut-off lows associated with subtropical ridges is observed in the late 2020–2022 period.
Yahui Che, Bofu Yu, and Katherine Bracco
Atmos. Chem. Phys., 24, 4105–4128, https://doi.org/10.5194/acp-24-4105-2024, https://doi.org/10.5194/acp-24-4105-2024, 2024
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Dust events occur more frequently during the Austral spring and summer in dust regions, including central Australia, the southwest of Western Australia, and the northern and southern regions of eastern Australia using remote sensing and reanalysis datasets. High-concentration dust is distributed around central Australia and in the downwind northern and southern Australia. Typically, around 50 % of the dust lifted settles on Australian land, with the remaining half being deposited in the ocean.
Jonathan Elsey, Nicolas Bellouin, and Claire Ryder
Atmos. Chem. Phys., 24, 4065–4081, https://doi.org/10.5194/acp-24-4065-2024, https://doi.org/10.5194/acp-24-4065-2024, 2024
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Aerosols influence the Earth's energy balance. The uncertainty in this radiative forcing is large depending partly on uncertainty in measurements of aerosol optical properties. We have developed a freely available new framework of millions of radiative transfer simulations spanning aerosol uncertainty and assess the impact on radiative forcing uncertainty. We find that reducing these uncertainties would reduce radiative forcing uncertainty, but non-aerosol uncertainties must also be considered.
Jing Li, Nan Wu, Biwu Chu, An Ning, and Xiuhui Zhang
Atmos. Chem. Phys., 24, 3989–4000, https://doi.org/10.5194/acp-24-3989-2024, https://doi.org/10.5194/acp-24-3989-2024, 2024
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Iodic acid (HIO3) nucleates with iodous acid (HIO2) efficiently in marine areas; however, whether methanesulfonic acid (MSA) can synergistically participate in the HIO3–HIO2-based nucleation is unclear. We provide molecular-level evidence that MSA can efficiently promote the formation of HIO3–HIO2-based clusters using a theoretical approach. The proposed MSA-enhanced iodine nucleation mechanism may help us to deeply understand marine new particle formation events with bursts of iodine particles.
Yueming Cheng, Tie Dai, Junji Cao, Daisuke Goto, Jianbing Jin, Teruyuki Nakajima, and Guangyu Shi
EGUsphere, https://doi.org/10.5194/egusphere-2024-840, https://doi.org/10.5194/egusphere-2024-840, 2024
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In March 2021, East Asia experienced an outbreak of severe dust storms after an absence of one and a half decades. Here, we innovative used the time-lagged ground-based aerosol size information with the fixed-lag ensemble Kalman smoother to optimize the dust emission and reproduce the dust storm. This work is valuable for the quantification of health damage, aviation risks, and profound impacts on the Earth system, but also to reveal the climatic driving force and the process of desertification.
Hao Wang, Xiaohong Liu, Chenglai Wu, and Guangxing Lin
Atmos. Chem. Phys., 24, 3309–3328, https://doi.org/10.5194/acp-24-3309-2024, https://doi.org/10.5194/acp-24-3309-2024, 2024
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We quantified different global- and regional-scale drivers of biogenic volatile organic compound (BVOC) emission trends over the past 20 years. The results show that global greening trends significantly boost BVOC emissions and deforestation reduces BVOC emissions in South America and Southeast Asia. Elevated temperature in Europe and increased soil moisture in East and South Asia enhance BVOC emissions. The results deepen our understanding of long-term BVOC emission trends in hotspots.
Christof G. Beer, Johannes Hendricks, and Mattia Righi
Atmos. Chem. Phys., 24, 3217–3240, https://doi.org/10.5194/acp-24-3217-2024, https://doi.org/10.5194/acp-24-3217-2024, 2024
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Ice-nucleating particles (INPs) have important influences on cirrus clouds and the climate system; however, the understanding of their global impacts is still uncertain. We perform numerical simulations with a global aerosol–climate model to analyse INP-induced cirrus changes and the resulting climate impacts. We evaluate various sources of uncertainties, e.g. the ice-nucleating ability of INPs and the role of model dynamics, and provide a new estimate for the global INP–cirrus effect.
Jiawei Li, Zhiwei Han, Pingqing Fu, Xiaohong Yao, and Mingjie Liang
Atmos. Chem. Phys., 24, 3129–3161, https://doi.org/10.5194/acp-24-3129-2024, https://doi.org/10.5194/acp-24-3129-2024, 2024
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Organic aerosols of marine origin are important for aerosol climatic effects but are poorly understood. For the first time, an online coupled regional chemistry–climate model is applied to explore the characteristics of emission, distribution, and direct and indirect radiative effects of marine organic aerosols over the western Pacific, which reveals an important role of marine organic aerosols in perturbing cloud and radiation and promotes understanding of global aerosol climatic impact.
Yawen Liu, Yun Qian, Philip J. Rasch, Kai Zhang, Lai-yung Ruby Leung, Yuhang Wang, Minghuai Wang, Hailong Wang, Xin Huang, and Xiu-Qun Yang
Atmos. Chem. Phys., 24, 3115–3128, https://doi.org/10.5194/acp-24-3115-2024, https://doi.org/10.5194/acp-24-3115-2024, 2024
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Fire management has long been a challenge. Here we report that spring-peak fire activity over southern Mexico and Central America (SMCA) has a distinct quasi-biennial signal by measuring multiple fire metrics. This signal is initially driven by quasi-biennial variability in precipitation and is further amplified by positive feedback of fire–precipitation interaction at short timescales. This work highlights the importance of fire–climate interactions in shaping fires on an interannual scale.
Xu Feng, Loretta J. Mickley, Michelle L. Bell, Tianjia Liu, Jenny A. Fisher, and Maria Val Martin
Atmos. Chem. Phys., 24, 2985–3007, https://doi.org/10.5194/acp-24-2985-2024, https://doi.org/10.5194/acp-24-2985-2024, 2024
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During severe wildfire seasons, smoke can have a significant impact on air quality in Australia. Our study demonstrates that characterization of the smoke plume injection fractions greatly affects estimates of surface smoke PM2.5. Using the plume behavior predicted by the machine learning method leads to the best model agreement with observed surface PM2.5 in key cities across Australia, with smoke PM2.5 accounting for 5 %–52 % of total PM2.5 on average during fire seasons from 2009 to 2020.
Shiyi Lai, Ximeng Qi, Xin Huang, Sijia Lou, Xuguang Chi, Liangduo Chen, Chong Liu, Yuliang Liu, Chao Yan, Mengmeng Li, Tengyu Liu, Wei Nie, Veli-Matti Kerminen, Tuukka Petäjä, Markku Kulmala, and Aijun Ding
Atmos. Chem. Phys., 24, 2535–2553, https://doi.org/10.5194/acp-24-2535-2024, https://doi.org/10.5194/acp-24-2535-2024, 2024
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By combining in situ measurements and chemical transport modeling, this study investigates new particle formation (NPF) on the southeastern Tibetan Plateau. We found that the NPF was driven by the presence of biogenic gases and the transport of anthropogenic precursors. The NPF was vertically heterogeneous and shaped by the vertical mixing. This study highlights the importance of anthropogenic–biogenic interactions and meteorological dynamics in NPF in this climate-sensitive region.
Adriana Rocha-Lima, Peter R. Colarco, Anton S. Darmenov, Edward P. Nowottnick, Arlindo M. da Silva, and Luke D. Oman
Atmos. Chem. Phys., 24, 2443–2464, https://doi.org/10.5194/acp-24-2443-2024, https://doi.org/10.5194/acp-24-2443-2024, 2024
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Observations show an increasing aerosol optical depth trend in the Middle East between 2003–2012. We evaluate the NASA Goddard Earth Observing System (GEOS) model's ability to capture these trends and examine the meteorological and surface parameters driving dust emissions. Our results highlight the importance of data assimilation for long-term trends of atmospheric aerosols and support the hypothesis that vegetation cover loss may have contributed to increasing dust emissions in the period.
Marc Mallet, Aurore Voldoire, Fabien Solmon, Pierre Nabat, Thomas Drugé, and Romain Roehrig
EGUsphere, https://doi.org/10.5194/egusphere-2024-496, https://doi.org/10.5194/egusphere-2024-496, 2024
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This study investigates the interactions between smoke aerosols and climate in tropical Africa using a coupled ocean-atmosphere-aerosol climate model. The work shows that smoke plumes have a significant impact by increasing the low cloud fraction, decreasing the ocean and continental surface temperature and by reducing the precipitation of the coastal Western Africa. It also highlights the key role of the ocean temperature response and its feedbacks for the September to November season.
Danny M. Leung, Jasper F. Kok, Longlei Li, Natalie M. Mahowald, David M. Lawrence, Simone Tilmes, Erik Kluzek, Martina Klose, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 2287–2318, https://doi.org/10.5194/acp-24-2287-2024, https://doi.org/10.5194/acp-24-2287-2024, 2024
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This study uses a premier Earth system model to evaluate a new desert dust emission scheme proposed in our companion paper. We show that our scheme accounts for more dust emission physics, hence matching better against observations than other existing dust emission schemes do. Our scheme's dust emissions also couple tightly with meteorology, hence likely improving the modeled dust sensitivity to climate change. We believe this work is vital for improving dust representation in climate models.
Alcide Zhao, Laura Wilcox, and Claire Ryder
EGUsphere, https://doi.org/10.5194/egusphere-2023-3075, https://doi.org/10.5194/egusphere-2023-3075, 2024
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Climate models include desert dust aerosols, which interact with radiation and can change circulation patterns. We assess the effect of dust on the Indian and East Asian summer monsoons through multi-model experiments where dust emissions are doubled, isolating the effect of dust for the first time. We find that dust results in an enhanced Indian summer monsoon and a southward shift of equatorial rainfall. Our results show the importance of accurate dust representation in climate model.
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Short summary
Secondary organic aerosols (SOAs) can exist in liquid, semi-solid, or amorphous solid states, which are rarely accounted for in current chemical transport models. We predict the phase state of SOA particles over China and find that in northwestern China SOA particles are mostly highly viscous or glassy solid. Our results indicate that the particle phase state should be considered in SOA formation in chemical transport models for more accurate prediction of SOA mass concentrations.
Secondary organic aerosols (SOAs) can exist in liquid, semi-solid, or amorphous solid states,...
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