Articles | Volume 24, issue 14
https://doi.org/10.5194/acp-24-8473-2024
© 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-24-8473-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Measurement report: Impact of cloud processes on secondary organic aerosols at a forested mountain site in southeastern China
Zijun 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
Weiqi Xu
CORRESPONDING AUTHOR
State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China
Yi 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
Xiangyu 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
Aodong Du
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
Yinzhou Zhang
State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China
Hongqin Qiao
Institute for Environmental and Climate Research, Jinan University, Guangzhou 511143, China
Institute for Environmental and Climate Research, Jinan University, Guangzhou 511143, China
Xiaole Pan
State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, 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
Xueling Cheng
State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China
Lanzhong Liu
Shanghuang Eco-Environmental Observatory of Chinese Academy of Sciences, Jinhua 321203, China
Qingyan Fu
Shanghai Environmental Monitoring Center, Shanghai 200235, China
Douglas R. Worsnop
Aerodyne Research Inc., Billerica, Massachusetts 01821, USA
Jie Li
State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, 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
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Yuhang Hao, Peizhao Li, Yafeng Gou, Zhenshuai Wang, Mi Tian, Yang Chen, Ye Kuang, Hanbing Xu, Fenglian Wan, Yuqian Luo, Wei Huang, and Jing Chen
EGUsphere, https://doi.org/10.5194/egusphere-2024-3242, https://doi.org/10.5194/egusphere-2024-3242, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Intensified heatwaves with the global warming have influenced new particle formation (NPF) and related aerosol physicochemical properties. We show that aerosol optical hygroscopicity (f(RH)) was generally higher on NPF event days than non-event cases, likely due to enhanced secondary formation and subsequent growth of both pre-existing and newly formed particles with stronger photooxidation specifically under persistent heatwaves. This would further impact the aerosol direct radiative forcing.
Valter Mickwitz, Otso Peräkylä, Frans Graeffe, Douglas Worsnop, and Mikael Ehn
EGUsphere, https://doi.org/10.5194/egusphere-2024-3047, https://doi.org/10.5194/egusphere-2024-3047, 2024
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
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This work presents and evaluates an algorithm that automatically conducts the steps of fitting peaks and identifying formulas, necessary but time consuming steps for most applications of mass spectrometry within atmospheric science. The aim of the algorithm is to save researchers working on these tasks significant amounts of time, and allow them to proceed with their analysis. The work demonstrates that this algorithm can achieve the goal of speeding up analysis, and provide accurate formulas.
Lei Kong, Xiao Tang, Zifa Wang, Jiang Zhu, Jianjun Li, Huangjian Wu, Qizhong Wu, Huansheng Chen, Lili Zhu, Wei Wang, Bing Liu, Qian Wang, Duohong Chen, Yuepeng Pan, Jie Li, Lin Wu, and Gregory R. Carmichael
Earth Syst. Sci. Data, 16, 4351–4387, https://doi.org/10.5194/essd-16-4351-2024, https://doi.org/10.5194/essd-16-4351-2024, 2024
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A new long-term inversed emission inventory for Chinese air quality (CAQIEI) is developed in this study, which contains constrained monthly emissions of NOx, SO2, CO, PM2.5, PM10, and NMVOCs in China from 2013 to 2020 with a horizontal resolution of 15 km. Emissions of different air pollutants and their changes during 2013–2020 were investigated and compared with previous emission inventories, which sheds new light on the complex variations of air pollutant emissions in China.
Ye Kuang, Biao Luo, Shan Huang, Junwen Liu, Weiwei Hu, Yuweng Peng, Duohong Chen, Dingli Yue, Wanyun Xu, Bin Yuan, and Min Shao
EGUsphere, https://doi.org/10.5194/egusphere-2024-2654, https://doi.org/10.5194/egusphere-2024-2654, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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This research reveals the potential importance of nighttime NO3 radical chemistry and aerosol water in the rapid formation of secondary brown carbon from biomass burning emissions. The findings enhance our understanding of nighttime biomass burning evolution and its implications for climate and regional air quality, especially regarding interactions with aerosol water and water-rich fogs and clouds.
Ye Kuang, Jiangchuan Tao, Hanbin Xu, Li Liu, Pengfei Liu, Wanyun Xu, Weiqi Xu, Yele Sun, and Chunsheng Zhao
EGUsphere, https://doi.org/10.5194/egusphere-2024-2698, https://doi.org/10.5194/egusphere-2024-2698, 2024
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This study presents a novel optical framework to measure supersaturation, a fundamental parameter in cloud physics, by observing the scattering properties of particles that have or have not grown into cloud droplets. The technique offers high-resolution measurements, capturing essential fluctuations in supersaturation necessary for understanding cloud physics.
Weiqi Xu, Ye Kuang, Wanyun Xu, Zhiqiang Zhang, Biao Luo, Xiaoyi Zhang, Jiangchuang Tao, Hongqin Qiao, Li Liu, and Yele Sun
Atmos. Chem. Phys., 24, 9387–9399, https://doi.org/10.5194/acp-24-9387-2024, https://doi.org/10.5194/acp-24-9387-2024, 2024
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We deployed an advanced aerosol–fog sampling system at a rural site in the North China Plain to investigate impacts of aerosol hygroscopic growth and activation on the physicochemical properties of submicron aerosols. Observed results highlighted remarkably different aqueous processing of primary and secondary submicron aerosol components under distinct ambient relative humidity (RH) conditions and that RH levels significantly impact aerosol sampling through the aerosol swelling effect.
Tianle Pan, Andrew T. Lambe, Weiwei Hu, Yicong He, Minghao Hu, Huaishan Zhou, Xinming Wang, Qingqing Hu, Hui Chen, Yue Zhao, Yuanlong Huang, Doug R. Worsnop, Zhe Peng, Melissa A. Morris, Douglas A. Day, Pedro Campuzano-Jost, Jose-Luis Jimenez, and Shantanu H. Jathar
Atmos. Meas. Tech., 17, 4915–4939, https://doi.org/10.5194/amt-17-4915-2024, https://doi.org/10.5194/amt-17-4915-2024, 2024
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This study systematically characterizes the temperature enhancement in the lamp-enclosed oxidation flow reactor (OFR). The enhancement varied multiple dimensional factors, emphasizing the complexity of temperature inside of OFR. The effects of temperature on the flow field and gas- or particle-phase reaction inside OFR were also evaluated with experiments and model simulations. Finally, multiple mitigation strategies were demonstrated to minimize this temperature increase.
Jiangchuan Tao, Biao Luo, Weiqi Xu, Gang Zhao, Hanbin Xu, Biao Xue, Miaomiao Zhai, Wanyun Xu, Huarong Zhao, Sanxue Ren, Guangsheng Zhou, Li Liu, Ye Kuang, and Yele Sun
Atmos. Chem. Phys., 24, 9131–9154, https://doi.org/10.5194/acp-24-9131-2024, https://doi.org/10.5194/acp-24-9131-2024, 2024
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Using simultaneous measurements of DMA–CCNC, H(/V)TDMA, and DMA–SP2, impacts of primary emissions and secondary aerosol formations on changes in aerosol physicochemical properties were comprehensively investigated. It was found that intercomparisons among aerosol mixing-state parameters derived from different techniques can help us gain more insight into aerosol physical properties which, in turn, will aid the investigation of emission characteristics and secondary aerosol formation pathways.
Huiyun Du, Jie Li, Xueshun Chen, Gabriele Curci, Fangqun Yu, Yele Sun, Xu Dao, Song Guo, Zhe Wang, Wenyi Yang, Lianfang Wei, and Zifa Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-1432, https://doi.org/10.5194/egusphere-2024-1432, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Inadequate consideration of mixing state and coatings on BC hinders aerosol radiation forcing quantification. While core-shell mixing results match observations closely, partial internal mixing and coating are more realistic. The fraction of embedded BC and coating aerosols resolved by a microphysics module were used to constrain the mixing state. This led to a 30~43 % absorption enhancement decrease over Northern China, offering valuable insights for the assessment of BC's radiative effects.
Shuai Wang, Mengyuan Zhang, Hui Zhao, Peng Wang, Sri Harsha Kota, Qingyan Fu, Cong Liu, and Hongliang Zhang
Earth Syst. Sci. Data, 16, 3565–3577, https://doi.org/10.5194/essd-16-3565-2024, https://doi.org/10.5194/essd-16-3565-2024, 2024
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Long-term, open-source, gap-free daily ground-level PM2.5 and PM10 datasets for India (LongPMInd) were reconstructed using a robust machine learning model to support health assessment and air quality management.
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.
Zichen Wu, Xueshun Chen, Zifa Wang, Huansheng Chen, Zhe Wang, Qing Mu, Lin Wu, Wending Wang, Xiao Tang, Jie Li, Ying Li, Qizhong Wu, Yang Wang, Zhiyin Zou, and Zijian Jiang
EGUsphere, https://doi.org/10.5194/egusphere-2024-1437, https://doi.org/10.5194/egusphere-2024-1437, 2024
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We developed a model to simulate polycyclic aromatic hydrocarbons (PAHs) from global to regional scales. The model can well reproduce the distribution of PAHs. The concentration of BaP (indicator species for PAHs) could exceed the target values of 1 ng m-3 over some areas (e.g., in central Europe, India, and eastern China). The change of BaP is less than PM2.5 from 2013 to 2018. China still faces significant potential health risks posed by BaP although "the Action Plan" has been implemented.
Ming Chu, Xing Wei, Shangfei Hai, Yang Gao, Huiwang Gao, Yujiao Zhu, Biwu Chu, Nan Ma, Juan Hong, Yele Sun, and Xiaohong Yao
Atmos. Chem. Phys., 24, 6769–6786, https://doi.org/10.5194/acp-24-6769-2024, https://doi.org/10.5194/acp-24-6769-2024, 2024
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We used a 20-bin WRF-Chem model to simulate NPF events in the NCP during a three-week observational period in the summer of 2019. The model was able to reproduce the observations during June 29–July 6, which was characterized by a high frequency of NPF occurrence.
Diego Aliaga, Victoria A. Sinclair, Radovan Krejci, Marcos Andrade, Paulo Artaxo, Luis Blacutt, Runlong Cai, Samara Carbone, Yvette Gramlich, Liine Heikkinen, Dominic Heslin-Rees, Wei Huang, Veli-Matti Kerminen, Alkuin Maximilian Koenig, Markku Kulmala, Paolo Laj, Valeria Mardoñez-Balderrama, Claudia Mohr, Isabel Moreno, Pauli Paasonen, Wiebke Scholz, Karine Sellegri, Laura Ticona, Gaëlle Uzu, Fernando Velarde, Alfred Wiedensohler, Doug Worsnop, Cheng Wu, Chen Xuemeng, Qiaozhi Zha, and Federico Bianchi
Aerosol Research Discuss., https://doi.org/10.5194/ar-2024-15, https://doi.org/10.5194/ar-2024-15, 2024
Revised manuscript accepted for AR
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This study examines new particle formation (NPF) in the Bolivian Andes at Chacaltaya mountain (CHC) and the urban El Alto-La Paz area (EAC). Days are clustered into four categories based on NPF intensity. Differences in particle size, precursor gases, and pollution levels are found. High NPF intensities increased Aitken mode particle concentrations at both sites, while volcanic influence selectively diminished NPF intensity at CHC but not EAC. This study highlights NPF dynamics in the Andes.
Zhaojin An, Rujing Yin, Xinyan Zhao, Xiaoxiao Li, Yi Yuan, Junchen Guo, Yuyang Li, Xue Li, Dandan Li, Yaowei Li, Dongbin Wang, Chao Yan, Kebin He, Douglas R. Worsnop, Frank N. Keutsch, and Jingkun Jiang
EGUsphere, https://doi.org/10.5194/egusphere-2024-1325, https://doi.org/10.5194/egusphere-2024-1325, 2024
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Online Vocus-PTR measurements show the compositions and seasonal variations of organic vapors in urban Beijing. With enhanced sensitivity and mass resolution, various sub-ppt level species and organics with multiple oxygens (≥3) were discovered. The fast photooxidation process in summer leads to an increase in both concentration and proportion of organics with multiple oxygens. While in other seasons, the variations of them could be influenced by primary emissions.
Hongyi Li, Ting Yang, Lars Nerger, Dawei Zhang, Di Zhang, Guigang Tang, Haibo Wang, Yele Sun, Pingqing Fu, Hang Su, and Zifa Wang
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2024-78, https://doi.org/10.5194/gmd-2024-78, 2024
Revised manuscript accepted for GMD
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To accurately characterize the spatiotemporal distribution of PM2.5 chemical components, we developed a hybrid nonlinear data assimilation system (NAQPMS-PDAF v2.0), which is optimal for chemical components with non-Gaussian and nonlinear properties. NAQPMS-PDAF v2.0 has superior computing efficiency and excels when used a small ensemble size. The one-month assimilation experiments show that NAQPMS-PDAF v2.0 can significantly improve the simulation performance of chemical components.
Shuai Wang, Mengyuan Zhang, Yueqi Gao, Peng Wang, Qingyan Fu, and Hongliang Zhang
Geosci. Model Dev., 17, 3617–3629, https://doi.org/10.5194/gmd-17-3617-2024, https://doi.org/10.5194/gmd-17-3617-2024, 2024
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Numerical models are widely used in air pollution modeling but suffer from significant biases. The machine learning model designed in this study shows high efficiency in identifying such biases. Meteorology (relative humidity and cloud cover), chemical composition (secondary organic components and dust aerosols), and emission sources (residential activities) are diagnosed as the main drivers of bias in modeling PM2.5, a typical air pollutant. The results will help to improve numerical models.
Zhiqiang Zhang, Ying Li, Haiyan Ran, Junling An, Yu Qu, Wei Zhou, Weiqi Xu, Weiwei Hu, Hongbin Xie, Zifa Wang, Yele Sun, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 4809–4826, https://doi.org/10.5194/acp-24-4809-2024, https://doi.org/10.5194/acp-24-4809-2024, 2024
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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.
Fangbing Li, Dan Dan Huang, Linhui Tian, Bin Yuan, Wen Tan, Liang Zhu, Penglin Ye, Douglas Worsnop, Ka In Hoi, Kai Meng Mok, and Yong Jie Li
Atmos. Meas. Tech., 17, 2415–2427, https://doi.org/10.5194/amt-17-2415-2024, https://doi.org/10.5194/amt-17-2415-2024, 2024
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The responses of protonated, adduct, and fragmented ions of 21 volatile organic compounds (VOCs) were investigated with varying instrument settings and relative humidity (RH) in a Vocus proton-transfer-reaction mass spectrometer (PTR-MS). The protonated ions of most VOCs studied show < 15 % variation in sensitivity, except for some long-chain aldehydes. The relationship between sensitivity and PTR rate constant is complicated by the influences from ion transmission and protonated ion fraction.
Mahen Konwar, Benjamin Werden, Edward C. Fortner, Sudarsan Bera, Mercy Varghese, Subharthi Chowdhuri, Kurt Hibert, Philip Croteau, John Jayne, Manjula Canagaratna, Neelam Malap, Sandeep Jayakumar, Shivsai A. Dixit, Palani Murugavel, Duncan Axisa, Darrel Baumgardner, Peter F. DeCarlo, Doug R. Worsnop, and Thara Prabhakaran
Atmos. Meas. Tech., 17, 2387–2400, https://doi.org/10.5194/amt-17-2387-2024, https://doi.org/10.5194/amt-17-2387-2024, 2024
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In a warm cloud seeding experiment hygroscopic particles are released to alter cloud processes to induce early raindrops. During the Cloud–Aerosol Interaction and Precipitation Enhancement Experiment, airborne mini aerosol mass spectrometers analyse the particles on which clouds form. The seeded clouds showed higher concentrations of chlorine and potassium, the oxidizing agents of flares. Small cloud droplet concentrations increased, and seeding particles were detected in deep cloud depths.
Markku Kulmala, Diego Aliaga, Santeri Tuovinen, Runlong Cai, Heikki Junninen, Chao Yan, Federico Bianchi, Yafang Cheng, Aijun Ding, Douglas R. Worsnop, Tuukka Petäjä, Katrianne Lehtipalo, Pauli Paasonen, and Veli-Matti Kerminen
Aerosol Research, 2, 49–58, https://doi.org/10.5194/ar-2-49-2024, https://doi.org/10.5194/ar-2-49-2024, 2024
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Atmospheric new particle formation (NPF), together with secondary production of particulate matter in the atmosphere, dominates aerosol particle number concentrations and submicron particle mass loads in many environments globally. In this opinion paper, we describe the paradigm shift to understand NPF in a continuous way instead of using traditional binary event–non-event analysis.
Jian Zhao, Valter Mickwitz, Yuanyuan Luo, Ella Häkkinen, Frans Graeffe, Jiangyi Zhang, Hilkka Timonen, Manjula Canagaratna, Jordan E. Krechmer, Qi Zhang, Markku Kulmala, Juha Kangasluoma, Douglas Worsnop, and Mikael Ehn
Atmos. Meas. Tech., 17, 1527–1543, https://doi.org/10.5194/amt-17-1527-2024, https://doi.org/10.5194/amt-17-1527-2024, 2024
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Organic aerosol constitutes a significant portion of atmospheric fine particles but is less characterized due to its vast number of constituents. Recently, we developed a system for online measurements of particle-phase highly oxygenated organic molecules (HOMs). In this work, we systematically characterized the system, developed a new unit to enhance its performance, and demonstrated the essential role of thermograms in inferring volatility and quantifying HOMs in organic aerosols.
Jiangyi Zhang, Jian Zhao, Yuanyuan Luo, Valter Mickwitz, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 24, 2885–2911, https://doi.org/10.5194/acp-24-2885-2024, https://doi.org/10.5194/acp-24-2885-2024, 2024
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Due to the intrinsic connection between the formation pathways of O3 and HOMs, the ratio of HOM dimers or non-nitrate monomers to HOM organic nitrates could be used to determine O3 formation regimes. Owing to the fast formation and short lifetimes of HOMs, HOM-based indicating ratios can describe O3 formation in real time. Despite the success of our approach in this simple laboratory system, applicability to the much more complex atmosphere remains to be determined.
Xinlei Ge, Yele Sun, Justin Trousdell, Mindong Chen, and Qi Zhang
Atmos. Meas. Tech., 17, 423–439, https://doi.org/10.5194/amt-17-423-2024, https://doi.org/10.5194/amt-17-423-2024, 2024
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This study aims to enhance the application of the Aerodyne high-resolution aerosol mass spectrometer (HR-AMS) in characterizing organic nitrogen (ON) species within aerosol particles and droplets. A thorough analysis was conducted on 75 ON standards that represent a diverse spectrum of ambient ON types. The results underscore the capacity of the HR-AMS in examining the concentration and chemistry of atmospheric ON compounds, thereby offering insights into their sources and environmental impacts.
Diego Aliaga, Santeri Tuovinen, Tinghan Zhang, Janne Lampilahti, Xinyang Li, Lauri Ahonen, Tom Kokkonen, Tuomo Nieminen, Simo Hakala, Pauli Paasonen, Federico Bianchi, Doug Worsnop, Veli-Matti Kerminen, and Markku Kulmala
Aerosol Research, 1, 81–92, https://doi.org/10.5194/ar-1-81-2023, https://doi.org/10.5194/ar-1-81-2023, 2023
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We introduce a novel method for evaluating days when small particles are formed in the atmosphere. Instead of the traditional binary division between event and non-event days, our method, known as "nano ranking analysis", provides a continuous, non-categorical metric for each day. By utilizing data from Hyytiälä, Finland, we show that our approach effectively quantifies these events. This innovative method paves the way for a deeper understanding of the factors influencing particle formation.
Song Gao, Yong Yang, Xiao Tong, Linyuan Zhang, Yusen Duan, Guigang Tang, Qiang Wang, Changqing Lin, Qingyan Fu, Lipeng Liu, and Lingning Meng
Atmos. Meas. Tech., 16, 5709–5723, https://doi.org/10.5194/amt-16-5709-2023, https://doi.org/10.5194/amt-16-5709-2023, 2023
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We optimized and conducted an experimental program for the real-time monitoring of non-methane hydrocarbon instruments using the direct method. Changing the enrichment and specially designed columns further improved the test effect. The results correct the measurement errors that have prevailed for many years and can lay a foundation for the evaluation of volatile organic compounds in the regional ambient air and provide direction for the measurement of low-concentration ambient air pollutants.
Lu Zhang, Michal Segal-Rozenhaimer, Haochi Che, Caroline Dang, Junying Sun, Ye Kuang, and Paola Formenti
EGUsphere, https://doi.org/10.5194/egusphere-2023-2319, https://doi.org/10.5194/egusphere-2023-2319, 2023
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Our study examined the interaction between atmospheric particles and moisture over the south-eastern Atlantic Ocean during the biomass burning seasons in Africa. We found that organic components of these particles play a more important role in aerosol-moisture interactions than previously expected. This discovery is important as such interactions impact radiation and climate. Current climate models might need better representations of the moisture-absorbing properties of organic aerosols.
Da Lu, Hao Li, Mengke Tian, Guochen Wang, Xiaofei Qin, Na Zhao, Juntao Huo, Fan Yang, Yanfen Lin, Jia Chen, Qingyan Fu, Yusen Duan, Xinyi Dong, Congrui Deng, Sabur F. Abdullaev, and Kan Huang
Atmos. Chem. Phys., 23, 13853–13868, https://doi.org/10.5194/acp-23-13853-2023, https://doi.org/10.5194/acp-23-13853-2023, 2023
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Environmental conditions during dust are usually not favorable for secondary aerosol formation. However in this study, an unusual dust event was captured in a Chinese mega-city and showed “anomalous” meteorology and a special dust backflow transport pathway. The underlying formation mechanisms of secondary aerosols are probed in the context of this special dust event. This study shows significant implications for the varying dust aerosol chemistry in the future changing climate.
Andrew T. Lambe, Bin Bai, Masayuki Takeuchi, Nicole Orwat, Paul M. Zimmerman, Mitchell W. Alton, Nga L. Ng, Andrew Freedman, Megan S. Claflin, Drew R. Gentner, Douglas R. Worsnop, and Pengfei Liu
Atmos. Chem. Phys., 23, 13869–13882, https://doi.org/10.5194/acp-23-13869-2023, https://doi.org/10.5194/acp-23-13869-2023, 2023
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We developed a new method to generate nitrate radicals (NO3) for atmospheric chemistry applications that works by irradiating mixtures containing ceric ammonium nitrate with a UV light at room temperature. It has several advantages over traditional NO3 sources. We characterized its performance over a range of mixture and reactor conditions as well as other irradiation products. Proof of concept was demonstrated by generating and characterizing oxidation products of the β-pinene + NO3 reaction.
Aodong Du, Jiaxing Sun, Hang Liu, Weiqi Xu, Wei Zhou, Yuting Zhang, Lei Li, Xubing Du, Yan Li, Xiaole Pan, Zifa Wang, and Yele Sun
Atmos. Chem. Phys., 23, 13597–13611, https://doi.org/10.5194/acp-23-13597-2023, https://doi.org/10.5194/acp-23-13597-2023, 2023
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We characterized the impacts of emission controls on particle mixing state and density during the Beijing Olympic Winter Games using a SPAMS in tandem with a DMA and an AAC. OC and sulfate-containing particles increased, while those from primary emissions decreased. The effective particle densities increased and varied largely for different particles, highlighting the impacts of aging and formation processes on the changes of particle density and mixing state.
Lu Zhang, Michal Segal-Rozenhaimer, Haochi Che, Caroline Dang, Junying Sun, Ye Kuang, Paola Formenti, and Steven Howell
EGUsphere, https://doi.org/10.5194/egusphere-2023-2199, https://doi.org/10.5194/egusphere-2023-2199, 2023
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Using airborne measurements over the South-East Atlantic, our study explored how aerosols—tiny atmospheric particles—interact with moisture over the ocean, especially during the biomass burning season. We noticed unique patterns in their behavior at different altitudes and introduced a predictive model for this moisture interaction. Our results aid our understanding of aerosol-moisture interactions and benefit the research of aerosol radiative effect in this climatically significant region.
Tao Wang, Hang Liu, Jie Li, Shuai Wang, Youngseob Kim, Yele Sun, Wenyi Yang, Huiyun Du, Zhe Wang, and Zifa Wang
Geosci. Model Dev., 16, 5585–5599, https://doi.org/10.5194/gmd-16-5585-2023, https://doi.org/10.5194/gmd-16-5585-2023, 2023
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This paper developed a two-way coupled module in a new version of a regional urban–street network model, IAQMS-street v2.0, in which the mass flux from streets to background is considered. Test cases are defined to evaluate the performance of IAQMS-street v2.0 in Beijing by comparing it with that simulated by IAQMS-street v1.0 and a regional model. The contribution of local emissions and the influence of on-road vehicle control measures on air quality are evaluated by using IAQMS-street v2.0.
Xu-Cheng He, Jiali Shen, Siddharth Iyer, Paxton Juuti, Jiangyi Zhang, Mrisha Koirala, Mikko M. Kytökari, Douglas R. Worsnop, Matti Rissanen, Markku Kulmala, Norbert M. Maier, Jyri Mikkilä, Mikko Sipilä, and Juha Kangasluoma
Atmos. Meas. Tech., 16, 4461–4487, https://doi.org/10.5194/amt-16-4461-2023, https://doi.org/10.5194/amt-16-4461-2023, 2023
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In this study, the upgraded multi-scheme chemical ionisation inlet 2 is presented. Sulfuric acid, hypoiodous acid, iodine, sulfur dioxide, and hydroperoxyl radicals are calibrated, and the improved ion optics allow us to detect sulfuric acid and iodine-containing molecules at as low as a few parts per quadrillion by volume. Additionally, we confirm the reliable detection of iodic acid using both the nitrate and bromide chemical ionisation methods under atmospherically relevant conditions.
Xi Chen, Ting Yang, Zifa Wang, Futing Wang, and Haibo Wang
Atmos. Meas. Tech., 16, 4289–4302, https://doi.org/10.5194/amt-16-4289-2023, https://doi.org/10.5194/amt-16-4289-2023, 2023
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Uncertainties remain great in the planetary boundary layer height (PBLH) determination from radiosonde, especially during the transition period of different PBL regimes. We combine seven existing methods along with statistical modification on gradient-based methods. We find that the ensemble method can eliminate the overestimation of PBLH and reduce the inconsistency between individual methods. The ensemble method improves the effectiveness of PBLH determination to 62.6 %.
Meng Wang, Yusen Duan, Zhuozhi Zhang, Qi Yuan, Xinwei Li, Shuwen Han, Juntao Huo, Jia Chen, Yanfen Lin, Qingyan Fu, Tao Wang, Junji Cao, and Shun-cheng Lee
Atmos. Chem. Phys., 23, 10313–10324, https://doi.org/10.5194/acp-23-10313-2023, https://doi.org/10.5194/acp-23-10313-2023, 2023
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Hourly elemental carbon (EC) and NOx were continuously measured for 5 years (2016–2020) at a sampling site near a highway in western Shanghai. We use a machine learning model to rebuild the measured EC and NOx, and a business-as-usual (BAU) scenario was assumed in 2020 and compared with the measured EC and NOx.
Yong Zhang, Jie Tian, Qiyuan Wang, Lu Qi, Manousos Ioannis Manousakas, Yuemei Han, Weikang Ran, Yele Sun, Huikun Liu, Renjian Zhang, Yunfei Wu, Tianqu Cui, Kaspar Rudolf Daellenbach, Jay Gates Slowik, André S. H. Prévôt, and Junji Cao
Atmos. Chem. Phys., 23, 9455–9471, https://doi.org/10.5194/acp-23-9455-2023, https://doi.org/10.5194/acp-23-9455-2023, 2023
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PM2.5 pollution still frequently occurs in northern China during winter, and it is necessary to figure out the causes of air pollution based on intensive real-time measurement. The findings elaborate the chemical characteristics and source contributions of PM2.5 in three pilot cities, reveal potential formation mechanisms of secondary aerosols, and highlight the importance of controlling biomass burning and inhibiting generation of secondary aerosol for air quality improvement.
Yingqi Zheng, Minttu Havu, Huizhi Liu, Xueling Cheng, Yifan Wen, Hei Shing Lee, Joyson Ahongshangbam, and Leena Järvi
Geosci. Model Dev., 16, 4551–4579, https://doi.org/10.5194/gmd-16-4551-2023, https://doi.org/10.5194/gmd-16-4551-2023, 2023
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The performance of the Surface Urban Energy and Water Balance Scheme (SUEWS) is evaluated against the observed surface exchanges (fluxes) of heat and carbon dioxide in a densely built neighborhood in Beijing. The heat flux modeling is noticeably improved by using the observed maximum conductance and by optimizing the vegetation phenology modeling. SUEWS also performs well in simulating carbon dioxide flux.
Lichao Yang, Wansuo Duan, and Zifa Wang
Geosci. Model Dev., 16, 3827–3848, https://doi.org/10.5194/gmd-16-3827-2023, https://doi.org/10.5194/gmd-16-3827-2023, 2023
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An approach is proposed to refine a ground meteorological observation network to improve the PM2.5 forecasts in the Beijing–Tianjin–Hebei region. A cost-effective observation network is obtained and makes the relevant PM2.5 forecasts assimilate fewer observations but achieve the forecasting skill comparable to or higher than that obtained by assimilating all ground station observations, suggesting that many of the current ground stations can be greatly scattered to avoid much unnecessary work.
Hang Liu, Xiaole Pan, Shandong Lei, Yuting Zhang, Aodong Du, Weijie Yao, Guiqian Tang, Tao Wang, Jinyuan Xin, Jie Li, Yele Sun, Junji Cao, and Zifa Wang
Atmos. Chem. Phys., 23, 7225–7239, https://doi.org/10.5194/acp-23-7225-2023, https://doi.org/10.5194/acp-23-7225-2023, 2023
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We provide the average vertical profiles of black carbon (BC) concentration, size distribution and coating thickness at different times of the day in an urban area based on 112 vertical profiles. In addition, it is found that BC in the residual layer generally has a thicker coating, higher absorption enhancement and hygroscopicity than on the surface. Such aged BC could enter into the boundary layer and influence the BC properties in the early morning.
Lucía Caudillo, Mihnea Surdu, Brandon Lopez, Mingyi Wang, Markus Thoma, Steffen Bräkling, Angela Buchholz, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Martin Heinritzi, Antonio Amorim, David M. Bell, Zoé Brasseur, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Xu-Cheng He, Houssni Lamkaddam, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Roy L. Mauldin, Bernhard Mentler, Antti Onnela, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Birte Rörup, Wiebke Scholz, Jiali Shen, Dominik Stolzenburg, Christian Tauber, Ping Tian, António Tomé, Nsikanabasi Silas Umo, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, André Welti, Marcel Zauner-Wieczorek, Urs Baltensperger, Richard C. Flagan, Armin Hansel, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Douglas R. Worsnop, Imad El Haddad, Neil M. Donahue, Alexander L. Vogel, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 23, 6613–6631, https://doi.org/10.5194/acp-23-6613-2023, https://doi.org/10.5194/acp-23-6613-2023, 2023
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In this study, we present an intercomparison of four different techniques for measuring the chemical composition of nanoparticles. The intercomparison was performed based on the observed chemical composition, calculated volatility, and analysis of the thermograms. We found that the methods generally agree on the most important compounds that are found in the nanoparticles. However, they do see different parts of the organic spectrum. We suggest potential explanations for these differences.
Fei Li, Biao Luo, Miaomiao Zhai, Li Liu, Gang Zhao, Hanbing Xu, Tao Deng, Xuejiao Deng, Haobo Tan, Ye Kuang, and Jun Zhao
Atmos. Chem. Phys., 23, 6545–6558, https://doi.org/10.5194/acp-23-6545-2023, https://doi.org/10.5194/acp-23-6545-2023, 2023
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A field campaign was conducted to study black carbon (BC) mass size distributions and mixing states connected to traffic emissions using a system that combines a differential mobility analyzer and single-particle soot photometer. Results showed that the black carbon content of traffic emissions has a considerable influence on both BC mass size distributions and mixing states, which has crucial implications for accurately representing BC from various sources in regional and climate models.
Wen Lu, Bin Zhu, Shuqi Yan, Jie Li, and Zifa Wang
EGUsphere, https://doi.org/10.5194/egusphere-2023-1089, https://doi.org/10.5194/egusphere-2023-1089, 2023
Preprint archived
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Parameterized the minimum turbulent diffusivity (Kzmin) by sensible heat flux and latent heat flux and embedded it into the WRF-Chem model. New scheme improved the underestimation of turbulence diffusion underestimation and overestimation of surface PM2.5 under stable boundary layer simulation over eastern China. The physical relationship between Kzmin and two factors was discussed. Process analysis showed that vertical mixing is the key process to improve surface PM2.5 simulations.
Lei Kong, Xiao Tang, Jiang Zhu, Zifa Wang, Yele Sun, Pingqing Fu, Meng Gao, Huangjian Wu, Miaomiao Lu, Qian Wu, Shuyuan Huang, Wenxuan Sui, Jie Li, Xiaole Pan, Lin Wu, Hajime Akimoto, and Gregory R. Carmichael
Atmos. Chem. Phys., 23, 6217–6240, https://doi.org/10.5194/acp-23-6217-2023, https://doi.org/10.5194/acp-23-6217-2023, 2023
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A multi-air-pollutant inversion system has been developed in this study to estimate emission changes in China during COVID-19 lockdown. The results demonstrate that the lockdown is largely a nationwide road traffic control measure with NOx emissions decreasing by ~40 %. Emissions of other species only decreased by ~10 % due to smaller effects of lockdown on other sectors. Assessment results further indicate that the lockdown only had limited effects on the control of PM2.5 and O3 in China.
Juan Hong, Min Tang, Qiaoqiao Wang, Nan Ma, Shaowen Zhu, Shaobin Zhang, Xihao Pan, Linhong Xie, Guo Li, Uwe Kuhn, Chao Yan, Jiangchuan Tao, Ye Kuang, Yao He, Wanyun Xu, Runlong Cai, Yaqing Zhou, Zhibin Wang, Guangsheng Zhou, Bin Yuan, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 23, 5699–5713, https://doi.org/10.5194/acp-23-5699-2023, https://doi.org/10.5194/acp-23-5699-2023, 2023
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A comprehensive investigation of the characteristics of new particle formation (NPF) events was conducted at a rural site on the North China Plain (NCP), China, during the wintertime of 2018 by covering the particle number size distribution down to sub–3 nm. Potential mechanisms for NPF under the current environment were explored, followed by a further discussion on the factors governing the occurrence of NPF at this rural site compared with other regions (e.g., urban areas) in the NCP region.
Joanna E. Dyson, 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, Stephen D. Worrall, Asan Bacak, Archit Mehra, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, C. Nicholas Hewitt, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, W. Joe F. Acton, William J. Bloss, Supattarachai Saksakulkrai, Jingsha Xu, Zongbo Shi, Roy M. Harrison, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lianfang Wei, Pingqing Fu, Xinming Wang, Stephen R. Arnold, and Dwayne E. Heard
Atmos. Chem. Phys., 23, 5679–5697, https://doi.org/10.5194/acp-23-5679-2023, https://doi.org/10.5194/acp-23-5679-2023, 2023
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The hydroxyl (OH) and closely coupled hydroperoxyl (HO2) radicals are vital for their role in the removal of atmospheric pollutants. In less polluted regions, atmospheric models over-predict HO2 concentrations. In this modelling study, the impact of heterogeneous uptake of HO2 onto aerosol surfaces on radical concentrations and the ozone production regime in Beijing in the summertime is investigated, and the implications for emissions policies across China are considered.
Daniel John Katz, Aroob Abdelhamid, Harald Stark, Manjula R. Canagaratna, Douglas R. Worsnop, and Eleanor C. Browne
Atmos. Chem. Phys., 23, 5567–5585, https://doi.org/10.5194/acp-23-5567-2023, https://doi.org/10.5194/acp-23-5567-2023, 2023
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Ambient ion chemical composition measurements provide insight into trace gases that are precursors for the formation and growth of new aerosol particles. We use a new data analysis approach to increase the chemical information from these measurements. We analyze results from an agricultural region, a little studied land use type that is ~41 % of global land use, and find that the composition of gases important for aerosol formation and growth differs significantly from that in other ecosystems.
Miaomiao Zhai, Ye Kuang, Li Liu, Yao He, Biao Luo, Wanyun Xu, Jiangchuan Tao, Yu Zou, Fei Li, Changqin Yin, Chunhui Li, Hanbing Xu, and Xuejiao Deng
Atmos. Chem. Phys., 23, 5119–5133, https://doi.org/10.5194/acp-23-5119-2023, https://doi.org/10.5194/acp-23-5119-2023, 2023
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Using year-long aerosol mass spectrometer measurements, roles of secondary organic aerosols (SOA) during haze formations in an urban area of southern China were systematically analyzed. Almost all severe haze events were accompanied by continuous daytime and nighttime SOA formations, whereas coordinated gas-phase photochemistry and aqueous-phase reactions likely played significant roles in quick daytime SOA formations, and nitrate radicals played significant roles in nighttime SOA formations.
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-2023-22, https://doi.org/10.5194/gmd-2023-22, 2023
Revised manuscript not accepted
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We developed a quantitative decoupling analysis (QDA) method to quantify the contributions of emissions, meteorology, chemical reactions, and their nonlinear interactions on PM2.5. We found the effects of adverse meteorological conditions and the importance of nonlinear interactions. This method can provide valuable information for understanding of key factors to heavy pollution, but also help the modelers to find out the sources of uncertainties in numerical models.
Qiaozhi Zha, Wei Huang, Diego Aliaga, Otso Peräkylä, Liine Heikkinen, Alkuin Maximilian Koenig, Cheng Wu, Joonas Enroth, Yvette Gramlich, Jing Cai, Samara Carbone, Armin Hansel, Tuukka Petäjä, Markku Kulmala, Douglas Worsnop, Victoria Sinclair, Radovan Krejci, Marcos Andrade, Claudia Mohr, and Federico Bianchi
Atmos. Chem. Phys., 23, 4559–4576, https://doi.org/10.5194/acp-23-4559-2023, https://doi.org/10.5194/acp-23-4559-2023, 2023
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We investigate the chemical composition of atmospheric cluster ions from January to May 2018 at the high-altitude research station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes. With state-of-the-art mass spectrometers and air mass history analysis, the measured cluster ions exhibited distinct diurnal and seasonal patterns, some of which contributed to new particle formation. Our study will improve the understanding of atmospheric ions and their role in high-altitude new particle formation.
Shixian Zhai, Daniel J. Jacob, Drew C. Pendergrass, Nadia K. Colombi, Viral Shah, Laura Hyesung Yang, Qiang Zhang, Shuxiao Wang, Hwajin Kim, Yele Sun, Jin-Soo Choi, Jin-Soo Park, Gan Luo, Fangqun Yu, Jung-Hun Woo, Younha Kim, Jack E. Dibb, Taehyoung Lee, Jin-Seok Han, Bruce E. Anderson, Ke Li, and Hong Liao
Atmos. Chem. Phys., 23, 4271–4281, https://doi.org/10.5194/acp-23-4271-2023, https://doi.org/10.5194/acp-23-4271-2023, 2023
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Anthropogenic fugitive dust in East Asia not only causes severe coarse particulate matter air pollution problems, but also affects fine particulate nitrate. Due to emission control efforts, coarse PM decreased steadily. We find that the decrease of coarse PM is a major driver for a lack of decrease of fine particulate nitrate, as it allows more nitric acid to form fine particulate nitrate. The continuing decrease of coarse PM requires more stringent ammonia and nitrogen oxides emission controls.
Ella Häkkinen, Jian Zhao, Frans Graeffe, Nicolas Fauré, Jordan E. Krechmer, Douglas Worsnop, Hilkka Timonen, Mikael Ehn, and Juha Kangasluoma
Atmos. Meas. Tech., 16, 1705–1721, https://doi.org/10.5194/amt-16-1705-2023, https://doi.org/10.5194/amt-16-1705-2023, 2023
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Highly oxygenated compounds contribute to the formation and growth of atmospheric organic aerosol and thus impact the global climate. Knowledge of their transformations and fate after condensing into the particle phase has been limited by the lack of suitable detection techniques. Here, we present an online method for measuring highly oxygenated compounds from organic aerosol. We evaluate the performance of the method and demonstrate that the method is applicable to different organic species.
Jian Zhao, Ella Häkkinen, Frans Graeffe, Jordan E. Krechmer, Manjula R. Canagaratna, Douglas R. Worsnop, Juha Kangasluoma, and Mikael Ehn
Atmos. Chem. Phys., 23, 3707–3730, https://doi.org/10.5194/acp-23-3707-2023, https://doi.org/10.5194/acp-23-3707-2023, 2023
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Based on the combined measurements of gas- and particle-phase highly oxygenated organic molecules (HOMs) from α-pinene ozonolysis, enhancement of dimers in particles was observed. We conducted experiments wherein the dimer to monomer (D / M) ratios of HOMs in the gas phase were modified (adding CO / NO) to investigate the effects of the corresponding D / M ratios in the particles. These results are important for a better understanding of secondary organic aerosol formation in the atmosphere.
Yizhen Wu, Juntao Huo, Gan Yang, Yuwei Wang, Lihong Wang, Shijian Wu, Lei Yao, Qingyan Fu, and Lin Wang
Atmos. Chem. Phys., 23, 2997–3014, https://doi.org/10.5194/acp-23-2997-2023, https://doi.org/10.5194/acp-23-2997-2023, 2023
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Based on a field campaign in a suburban area of Shanghai during summer 2021, we calculated formaldehyde (HCHO) production rates from 24 volatile organic compounds (VOCs). In addition, HCHO photolysis, reactions with OH radicals, and dry deposition were considered for the estimation of HCHO loss rates. Our results reveal the key precursors of HCHO and suggest that HCHO wet deposition may be an important loss term on cloudy and rainy days, which needs to be further investigated.
Shujun Zhong, Shuang Chen, Junjun Deng, Yanbing Fan, Qiang Zhang, Qiaorong Xie, Yulin Qi, Wei Hu, Libin Wu, Xiaodong Li, Chandra Mouli Pavuluri, Jialei Zhu, Xin Wang, Di Liu, Xiaole Pan, Yele Sun, Zifa Wang, Yisheng Xu, Haijie Tong, Hang Su, Yafang Cheng, Kimitaka Kawamura, and Pingqing Fu
Atmos. Chem. Phys., 23, 2061–2077, https://doi.org/10.5194/acp-23-2061-2023, https://doi.org/10.5194/acp-23-2061-2023, 2023
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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.
Changqin Yin, Jianming Xu, Wei Gao, Liang Pan, Yixuan Gu, Qingyan Fu, and Fan Yang
Atmos. Chem. Phys., 23, 1329–1343, https://doi.org/10.5194/acp-23-1329-2023, https://doi.org/10.5194/acp-23-1329-2023, 2023
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The particle matter (PM2.5) at the top of the 632 m high Shanghai Tower was found to be higher than the surface from June to October due to unexpected larger PM2.5 levels during early to middle afternoon at Shanghai Tower. We suppose the significant chemical production of secondary species existed in the mid-upper planetary boundary layer. We found a high nitrate concentration at the tower site for both daytime and nighttime in winter, implying efficient gas-phase and heterogeneous formation.
Xiaofei Qin, Shengqian Zhou, Hao Li, Guochen Wang, Cheng Chen, Chengfeng Liu, Xiaohao Wang, Juntao Huo, Yanfen Lin, Jia Chen, Qingyan Fu, Yusen Duan, Kan Huang, and Congrui Deng
Atmos. Chem. Phys., 22, 15851–15865, https://doi.org/10.5194/acp-22-15851-2022, https://doi.org/10.5194/acp-22-15851-2022, 2022
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Using artificial neural network modeling and an explainable analysis approach, natural surface emissions (NSEs) were identified as a main driver of gaseous elemental mercury (GEM) variations during the COVID-19 lockdown. A sharp drop in GEM concentrations due to a significant reduction in anthropogenic emissions may disrupt the surface–air exchange balance of Hg, leading to increases in NSEs. This implies that NSEs may pose challenges to the future control of Hg pollution.
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.
Meng Wang, Yusen Duan, Wei Xu, Qiyuan Wang, Zhuozhi Zhang, Qi Yuan, Xinwei Li, Shuwen Han, Haijie Tong, Juntao Huo, Jia Chen, Shan Gao, Zhongbiao Wu, Long Cui, Yu Huang, Guangli Xiu, Junji Cao, Qingyan Fu, and Shun-cheng Lee
Atmos. Chem. Phys., 22, 12789–12802, https://doi.org/10.5194/acp-22-12789-2022, https://doi.org/10.5194/acp-22-12789-2022, 2022
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In this study, we report the long-term measurement of organic carbon (OC) and elementary carbon (EC) in PM2.5 with hourly time resolution conducted at a regional site in Shanghai from 2016 to 2020. The results from this study provide critical information about the long-term trend of carbonaceous aerosol, in particular secondary OC, in one of the largest megacities in the world and are helpful for developing pollution control measures from a long-term planning perspective.
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.
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.
Lisa J. Beck, Siegfried Schobesberger, Heikki Junninen, Janne Lampilahti, Antti Manninen, Lubna Dada, Katri Leino, Xu-Cheng He, Iida Pullinen, Lauriane L. J. Quéléver, Anna Franck, Pyry Poutanen, Daniela Wimmer, Frans Korhonen, Mikko Sipilä, Mikael Ehn, Douglas R. Worsnop, Veli-Matti Kerminen, Tuukka Petäjä, Markku Kulmala, and Jonathan Duplissy
Atmos. Chem. Phys., 22, 8547–8577, https://doi.org/10.5194/acp-22-8547-2022, https://doi.org/10.5194/acp-22-8547-2022, 2022
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The presented article introduces an overview of atmospheric ions and their composition above the boreal forest. We provide the results of an extensive airborne measurement campaign with an air ion mass spectrometer and particle measurements, showing their diurnal evolution within the boundary layer and free troposphere. In addition, we compare the airborne dataset with the co-located data from the ground at SMEAR II station, Finland.
Lauriane L. J. Quéléver, Lubna Dada, Eija Asmi, Janne Lampilahti, Tommy Chan, Jonathan E. Ferrara, Gustavo E. Copes, German Pérez-Fogwill, Luis Barreira, Minna Aurela, Douglas R. Worsnop, Tuija Jokinen, and Mikko Sipilä
Atmos. Chem. Phys., 22, 8417–8437, https://doi.org/10.5194/acp-22-8417-2022, https://doi.org/10.5194/acp-22-8417-2022, 2022
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Understanding how aerosols form is crucial for correctly modeling the climate and improving future predictions. This work provides extensive analysis of aerosol particles and their precursors at Marambio Station, Antarctic Peninsula. We show that sulfuric acid, ammonia, and dimethylamine are key contributors to the frequent new particle formation events observed at the site. We discuss nucleation mechanisms and highlight the need for targeted measurement to fully understand these processes.
Li Liu, Ye Kuang, Miaomiao Zhai, Biao Xue, Yao He, Jun Tao, Biao Luo, Wanyun Xu, Jiangchuan Tao, Changqin Yin, Fei Li, Hanbing Xu, Tao Deng, Xuejiao Deng, Haobo Tan, and Min Shao
Atmos. Chem. Phys., 22, 7713–7726, https://doi.org/10.5194/acp-22-7713-2022, https://doi.org/10.5194/acp-22-7713-2022, 2022
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Using simultaneous measurements of a humidified nephelometer system and an aerosol chemical speciation monitor in winter in Guangzhou, the strongest scattering ability of more oxidized oxygenated organic aerosol (MOOA) among aerosol components considering their dry-state scattering ability and water uptake ability was revealed, leading to large impacts of MOOA on visibility degradation. This has important implications for visibility improvement in China and aerosol radiative effect simulation.
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.
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.
Han Zang, Yue Zhao, Juntao Huo, Qianbiao Zhao, Qingyan Fu, Yusen Duan, Jingyuan Shao, Cheng Huang, Jingyu An, Likun Xue, Ziyue Li, Chenxi Li, and Huayun Xiao
Atmos. Chem. Phys., 22, 4355–4374, https://doi.org/10.5194/acp-22-4355-2022, https://doi.org/10.5194/acp-22-4355-2022, 2022
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Particulate nitrate plays an important role in wintertime haze pollution in eastern China, yet quantitative constraints on detailed nitrate formation mechanisms remain limited. Here we quantified the contributions of the heterogeneous N2O5 hydrolysis (66 %) and gas-phase OH + NO2 reaction (32 %) to nitrate formation in this region and identified the atmospheric oxidation capacity (i.e., availability of O3 and OH radicals) as the driving factor of nitrate formation from both processes.
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.
Mikko Sipilä, Nina Sarnela, Kimmo Neitola, Totti Laitinen, Deniz Kemppainen, Lisa Beck, Ella-Maria Duplissy, Salla Kuittinen, Tuuli Lehmusjärvi, Janne Lampilahti, Veli-Matti Kerminen, Katrianne Lehtipalo, Pasi P. Aalto, Petri Keronen, Erkki Siivola, Pekka A. Rantala, Douglas R. Worsnop, Markku Kulmala, Tuija Jokinen, and Tuukka Petäjä
Atmos. Chem. Phys., 21, 17559–17576, https://doi.org/10.5194/acp-21-17559-2021, https://doi.org/10.5194/acp-21-17559-2021, 2021
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Metallurgical industry in Kola peninsula is a large source of air pollution in the (sub-)Arctic domain. Sulfur dioxide emissions from the ore smelters are transported across large areas. We investigated sulfur dioxide and its transformation to sulfuric acid aerosol particles during winter months in Finnish Lapland, close to Kola industrial areas. We observed intense formation of new aerosol particles despite the low solar radiation intensity, often required for new particle formation elsewhere.
Chenyang Bi, Jordan E. Krechmer, Graham O. Frazier, Wen Xu, Andrew T. Lambe, Megan S. Claflin, Brian M. Lerner, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 6835–6850, https://doi.org/10.5194/amt-14-6835-2021, https://doi.org/10.5194/amt-14-6835-2021, 2021
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Iodide-adduct chemical ionization mass spectrometry (I-CIMS) has been widely used to analyze airborne organics. In this study, I-CIMS sensitivities of isomers within a formula are found to generally vary by 1 and up to 2 orders of magnitude. Comparisons between measured and predicted moles, obtained using a voltage-scanning calibration approach, show that predictions for individual compounds or formulas might carry high uncertainty, yet the summed moles of analytes agree reasonably well.
Yuliang Liu, Wei Nie, Yuanyuan Li, Dafeng Ge, Chong Liu, Zhengning Xu, Liangduo Chen, Tianyi Wang, Lei Wang, Peng Sun, Ximeng Qi, Jiaping Wang, Zheng Xu, Jian Yuan, Chao Yan, Yanjun Zhang, Dandan Huang, Zhe Wang, Neil M. Donahue, Douglas Worsnop, Xuguang Chi, Mikael Ehn, and Aijun Ding
Atmos. Chem. Phys., 21, 14789–14814, https://doi.org/10.5194/acp-21-14789-2021, https://doi.org/10.5194/acp-21-14789-2021, 2021
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Oxygenated organic molecules (OOMs) are crucial intermediates linking volatile organic compounds to secondary organic aerosols. Using nitrate time-of-flight chemical ionization mass spectrometry in eastern China, we performed positive matrix factorization (PMF) on binned OOM mass spectra. We reconstructed over 1000 molecules from 14 derived PMF factors and identified about 72 % of the observed OOMs as organic nitrates, highlighting the decisive role of NOx in OOM formation in populated areas.
Mao Xiao, Christopher R. Hoyle, Lubna Dada, Dominik Stolzenburg, Andreas Kürten, Mingyi Wang, Houssni Lamkaddam, Olga Garmash, Bernhard Mentler, Ugo Molteni, Andrea Baccarini, Mario Simon, Xu-Cheng He, Katrianne Lehtipalo, Lauri R. Ahonen, Rima Baalbaki, Paulus S. Bauer, Lisa Beck, David Bell, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, António Dias, Jonathan Duplissy, Henning Finkenzeller, Hamish Gordon, Victoria Hofbauer, Changhyuk Kim, Theodore K. Koenig, Janne Lampilahti, Chuan Ping Lee, Zijun Li, Huajun Mai, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Serge Mathot, Roy L. Mauldin, Wei Nie, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti Rissanen, Siegfried Schobesberger, Simone Schuchmann, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Robert Wagner, Yonghong Wang, Lena Weitz, Daniela Wimmer, Yusheng Wu, Chao Yan, Penglin Ye, Qing Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Ken Carslaw, Joachim Curtius, Armin Hansel, Rainer Volkamer, Paul M. Winkler, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Jasper Kirkby, Neil M. Donahue, Urs Baltensperger, Imad El Haddad, and Josef Dommen
Atmos. Chem. Phys., 21, 14275–14291, https://doi.org/10.5194/acp-21-14275-2021, https://doi.org/10.5194/acp-21-14275-2021, 2021
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Experiments at CLOUD show that in polluted environments new particle formation (NPF) is largely driven by the formation of sulfuric acid–base clusters, stabilized by amines, high ammonia concentrations or lower temperatures. While oxidation products of aromatics can nucleate, they play a minor role in urban NPF. Our experiments span 4 orders of magnitude variation of observed NPF rates in ambient conditions. We provide a framework based on NPF and growth rates to interpret ambient observations.
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.
Xiaolong Fan, Jing Cai, Chao Yan, Jian Zhao, Yishuo Guo, Chang Li, Kaspar R. Dällenbach, Feixue Zheng, Zhuohui Lin, Biwu Chu, Yonghong Wang, Lubna Dada, Qiaozhi Zha, Wei Du, Jenni Kontkanen, Theo Kurtén, Siddhart Iyer, Joni T. Kujansuu, Tuukka Petäjä, Douglas R. Worsnop, Veli-Matti Kerminen, Yongchun Liu, Federico Bianchi, Yee Jun Tham, Lei Yao, and Markku Kulmala
Atmos. Chem. Phys., 21, 11437–11452, https://doi.org/10.5194/acp-21-11437-2021, https://doi.org/10.5194/acp-21-11437-2021, 2021
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We observed significant concentrations of gaseous HBr and HCl throughout the winter and springtime in urban Beijing, China. Our results indicate that gaseous HCl and HBr are most likely originated from anthropogenic emissions such as burning activities, and the gas–aerosol partitioning may play a crucial role in contributing to the gaseous HCl and HBr. These observations suggest that there is an important recycling pathway of halogen species in inland megacities.
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.
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.
Liine Heikkinen, Mikko Äijälä, Kaspar R. Daellenbach, Gang Chen, Olga Garmash, Diego Aliaga, Frans Graeffe, Meri Räty, Krista Luoma, Pasi Aalto, Markku Kulmala, Tuukka Petäjä, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 21, 10081–10109, https://doi.org/10.5194/acp-21-10081-2021, https://doi.org/10.5194/acp-21-10081-2021, 2021
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In many locations worldwide aerosol particles have been shown to be made up of organic aerosol (OA). The boreal forest is a region where aerosol particles possess a high OA mass fraction. Here, we studied OA composition using the longest time series of OA composition ever obtained from a boreal environment. For this purpose, we tested a new analysis framework and discovered that most of the OA was highly oxidized, with strong seasonal behaviour reflecting different sources in summer and winter.
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.
Mingyi Wang, Xu-Cheng He, Henning Finkenzeller, Siddharth Iyer, Dexian Chen, Jiali Shen, Mario Simon, Victoria Hofbauer, Jasper Kirkby, Joachim Curtius, Norbert Maier, Theo Kurtén, Douglas R. Worsnop, Markku Kulmala, Matti Rissanen, Rainer Volkamer, Yee Jun Tham, Neil M. Donahue, and Mikko Sipilä
Atmos. Meas. Tech., 14, 4187–4202, https://doi.org/10.5194/amt-14-4187-2021, https://doi.org/10.5194/amt-14-4187-2021, 2021
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Atmospheric iodine species are often short-lived with low abundance and have thus been challenging to measure. We show that the bromide chemical ionization mass spectrometry, compatible with both the atmospheric pressure and reduced pressure interfaces, can simultaneously detect various gas-phase iodine species. Combining calibration experiments and quantum chemical calculations, we quantify detection sensitivities to HOI, HIO3, I2, and H2SO4, giving detection limits down to < 106 molec. cm-3.
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.
Chenyang Bi, Jordan E. Krechmer, Graham O. Frazier, Wen Xu, Andrew T. Lambe, Megan S. Claflin, Brian M. Lerner, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 3895–3907, https://doi.org/10.5194/amt-14-3895-2021, https://doi.org/10.5194/amt-14-3895-2021, 2021
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Measurement techniques that can achieve molecular characterizations are necessary to understand the differences of fate and transport within isomers produced in the atmospheric oxidation process. In this work, we develop an instrument to conduct isomer-resolved measurements of particle-phase organics. We assess the number of isomers per chemical formula in atmospherically relevant samples and examine the feasibility of extending the use of an existing instrument to a broader range of analytes.
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.
Kun Zhang, Ling Huang, Qing Li, Juntao Huo, Yusen Duan, Yuhang Wang, Elly Yaluk, Yangjun Wang, Qingyan Fu, and Li Li
Atmos. Chem. Phys., 21, 5905–5917, https://doi.org/10.5194/acp-21-5905-2021, https://doi.org/10.5194/acp-21-5905-2021, 2021
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Recently, high O3 concentrations were frequently observed in rural areas of the Yangtze River Delta (YRD) region under stagnant conditions. Using an online measurement and observation-based model, we investigated the budget of ROx radicals and the influence of isoprene chemistry on O3 formation. Our results underline that isoprene chemistry in the rural atmosphere becomes important with the participation of anthropogenic NOx.
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.
Hui Wang, Qizhong Wu, Alex B. Guenther, Xiaochun Yang, Lanning Wang, Tang Xiao, Jie Li, Jinming Feng, Qi Xu, and Huaqiong Cheng
Atmos. Chem. Phys., 21, 4825–4848, https://doi.org/10.5194/acp-21-4825-2021, https://doi.org/10.5194/acp-21-4825-2021, 2021
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We assessed the influence of the greening trend on BVOC emission in China. The comparison among different scenarios showed that vegetation changes resulting from land cover management are the main driver of BVOC emission change in China. Climate variability contributed significantly to interannual variations but not much to the long-term trend during the study period.
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.
Haiyan Li, Manjula R. Canagaratna, Matthieu Riva, Pekka Rantala, Yanjun Zhang, Steven Thomas, Liine Heikkinen, Pierre-Marie Flaud, Eric Villenave, Emilie Perraudin, Douglas Worsnop, Markku Kulmala, Mikael Ehn, and Federico Bianchi
Atmos. Chem. Phys., 21, 4123–4147, https://doi.org/10.5194/acp-21-4123-2021, https://doi.org/10.5194/acp-21-4123-2021, 2021
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For the first time, we performed binPMF analysis on the complex mass spectra acquired with the Vocus PTR-TOF in two European pine forests and identified various primary emission sources and secondary oxidation processes of atmospheric organic vapors, i.e., terpenes and their oxidation products, with varying oxidation degrees. Further insights were gained regarding monoterpene and sesquiterpene reactions based on the interpretation results.
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.
Runlong Cai, Chao Yan, Dongsen Yang, Rujing Yin, Yiqun Lu, Chenjuan Deng, Yueyun Fu, Jiaxin Ruan, Xiaoxiao Li, Jenni Kontkanen, Qiang Zhang, Juha Kangasluoma, Yan Ma, Jiming Hao, Douglas R. Worsnop, Federico Bianchi, Pauli Paasonen, Veli-Matti Kerminen, Yongchun Liu, Lin Wang, Jun Zheng, Markku Kulmala, and Jingkun Jiang
Atmos. Chem. Phys., 21, 2457–2468, https://doi.org/10.5194/acp-21-2457-2021, https://doi.org/10.5194/acp-21-2457-2021, 2021
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Based on long-term measurements, we discovered that the collision of H2SO4–amine clusters is the governing mechanism that initializes fast new particle formation in the polluted atmospheric environment of urban Beijing. The mechanism and the governing factors for H2SO4–amine nucleation in the polluted atmosphere are quantitatively investigated in this study.
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.
Arttu Ylisirniö, Luis M. F. Barreira, Iida Pullinen, Angela Buchholz, John Jayne, Jordan E. Krechmer, Douglas R. Worsnop, Annele Virtanen, and Siegfried Schobesberger
Atmos. Meas. Tech., 14, 355–367, https://doi.org/10.5194/amt-14-355-2021, https://doi.org/10.5194/amt-14-355-2021, 2021
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FIGAERO-ToF-CIMS enables online volatility measurements of chemical compounds in ambient aerosols. Previously published volatility calibration results however differ from each other significantly. In this study we investigate the reason for this discrepancy. We found a major source of error in the widely used syringe deposition method and propose a new method for volatility calibration by using atomized calibration compounds.
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.
Rutambhara Joshi, Dantong Liu, Eiko Nemitz, Ben Langford, Neil Mullinger, Freya Squires, James Lee, Yunfei Wu, Xiaole Pan, Pingqing Fu, Simone Kotthaus, Sue Grimmond, Qiang Zhang, Ruili Wu, Oliver Wild, Michael Flynn, Hugh Coe, and James Allan
Atmos. Chem. Phys., 21, 147–162, https://doi.org/10.5194/acp-21-147-2021, https://doi.org/10.5194/acp-21-147-2021, 2021
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Black carbon (BC) is a component of particulate matter which has significant effects on climate and human health. Sources of BC include biomass burning, transport, industry and domestic cooking and heating. In this study, we measured BC emissions in Beijing, finding a dominance of traffic emissions over all other sources. The quantitative method presented here has benefits for revising widely used emissions inventories and for understanding BC sources with impacts on air quality and climate.
Megan S. Claflin, Demetrios Pagonis, Zachary Finewax, Anne V. Handschy, Douglas A. Day, Wyatt L. Brown, John T. Jayne, Douglas R. Worsnop, Jose L. Jimenez, Paul J. Ziemann, Joost de Gouw, and Brian M. Lerner
Atmos. Meas. Tech., 14, 133–152, https://doi.org/10.5194/amt-14-133-2021, https://doi.org/10.5194/amt-14-133-2021, 2021
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We have developed a field-deployable gas chromatograph with thermal desorption preconcentration and detector switching between two high-resolution mass spectrometers for in situ measurements of volatile organic compounds (VOCs). This system combines chromatography with both proton transfer and electron ionization to offer fast time response and continuous molecular speciation. This technique was applied during the 2018 ATHLETIC campaign to characterize VOC emissions in an indoor environment.
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.
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.
Liqing Hao, Eetu Kari, Ari Leskinen, Douglas R. Worsnop, and Annele Virtanen
Atmos. Chem. Phys., 20, 14393–14405, https://doi.org/10.5194/acp-20-14393-2020, https://doi.org/10.5194/acp-20-14393-2020, 2020
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Our work presents the observational results of secondary organic aerosol (SOA) formation in the presence of ammonia. The particle-phase ammonium was continuously produced even after SOA formation had ceased. The gas-phase organic acids were observed to contribute to the formed particle-phase ammonium salts. This study suggests that the presence of ammonia may change the mass and chemical composition of large-size SOA particles and can potentially alter the aerosol impact on climate change.
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.
Yongjoo Choi, Yugo Kanaya, Masayuki Takigawa, Chunmao Zhu, Seung-Myung Park, Atsushi Matsuki, Yasuhiro Sadanaga, Sang-Woo Kim, Xiaole Pan, and Ignacio Pisso
Atmos. Chem. Phys., 20, 13655–13670, https://doi.org/10.5194/acp-20-13655-2020, https://doi.org/10.5194/acp-20-13655-2020, 2020
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.
Rui Li, Qiongqiong Wang, Xiao He, Shuhui Zhu, Kun Zhang, Yusen Duan, Qingyan Fu, Liping Qiao, Yangjun Wang, Ling Huang, Li Li, and Jian Zhen Yu
Atmos. Chem. Phys., 20, 12047–12061, https://doi.org/10.5194/acp-20-12047-2020, https://doi.org/10.5194/acp-20-12047-2020, 2020
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821, https://doi.org/10.5194/acp-20-11809-2020, https://doi.org/10.5194/acp-20-11809-2020, 2020
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With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
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.
Archit Mehra, Jordan E. Krechmer, Andrew Lambe, Chinmoy Sarkar, Leah Williams, Farzaneh Khalaj, Alex Guenther, John Jayne, Hugh Coe, Douglas Worsnop, Celia Faiola, and Manjula Canagaratna
Atmos. Chem. Phys., 20, 10953–10965, https://doi.org/10.5194/acp-20-10953-2020, https://doi.org/10.5194/acp-20-10953-2020, 2020
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Emissions of volatile organic compounds (VOCs) from plants are important for tropospheric ozone and secondary organic aerosol (SOA) formation. Real plant emissions are much more diverse than the few proxies widely used for studies of plant SOA. Here we present the first study of SOA from Californian sage plants and the oxygenated monoterpenes representing their major emissions. We identify SOA products and show the importance of the formation of highly oxygenated organic molecules and oligomers.
Xiaofei Qin, Leiming Zhang, Guochen Wang, Xiaohao Wang, Qingyan Fu, Jian Xu, Hao Li, Jia Chen, Qianbiao Zhao, Yanfen Lin, Juntao Huo, Fengwen Wang, Kan Huang, and Congrui Deng
Atmos. Chem. Phys., 20, 10985–10996, https://doi.org/10.5194/acp-20-10985-2020, https://doi.org/10.5194/acp-20-10985-2020, 2020
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The uncertainties in mercury emissions are much larger from natural sources than anthropogenic sources. A method was developed to quantify the contributions of natural surface emissions to ambient GEM based on PMF modeling. The annual GEM concentration in eastern China showed a decreasing trend from 2015 to 2018, while the relative contribution of natural surface emissions increased significantly from 41 % in 2015 to 57 % in 2018, gradually surpassing those from anthropogenic sources.
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.
Archit Mehra, Yuwei Wang, Jordan E. Krechmer, Andrew Lambe, Francesca Majluf, Melissa A. Morris, Michael Priestley, Thomas J. Bannan, Daniel J. Bryant, Kelly L. Pereira, Jacqueline F. Hamilton, Andrew R. Rickard, Mike J. Newland, Harald Stark, Philip Croteau, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, Lin Wang, and Hugh Coe
Atmos. Chem. Phys., 20, 9783–9803, https://doi.org/10.5194/acp-20-9783-2020, https://doi.org/10.5194/acp-20-9783-2020, 2020
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Aromatic volatile organic compounds (VOCs) emitted from anthropogenic activity are important for tropospheric ozone and secondary organic aerosol (SOA) formation. Here we present a detailed chemical characterisation of SOA from four C9-aromatic isomers and a polycyclic aromatic hydrocarbon (PAH). We identify and compare their oxidation products in the gas and particle phases, showing the different relative importance of oxidation pathways and proportions of highly oxygenated organic molecules.
Yuwei Wang, Archit Mehra, Jordan E. Krechmer, Gan Yang, Xiaoyu Hu, Yiqun Lu, Andrew Lambe, Manjula Canagaratna, Jianmin Chen, Douglas Worsnop, Hugh Coe, and Lin Wang
Atmos. Chem. Phys., 20, 9563–9579, https://doi.org/10.5194/acp-20-9563-2020, https://doi.org/10.5194/acp-20-9563-2020, 2020
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A series of OH-initiated oxidation experiments of trimethylbenzene were investigated in the absence and presence of NOx. Many C9 products with 1–11 oxygen atoms and C18 products presumably formed from dimerization of C9 peroxy radicals were observed, hinting at the extensive existence of autoxidation and accretion reaction pathways. The presence of NOx would suppress the formation of highly oxygenated C18 molecules and enhance the formation of organonitrates and even dinitrate compounds.
Mario Simon, Lubna Dada, Martin Heinritzi, Wiebke Scholz, Dominik Stolzenburg, Lukas Fischer, Andrea C. Wagner, Andreas Kürten, Birte Rörup, Xu-Cheng He, João Almeida, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Lisa Beck, Anton Bergen, Federico Bianchi, Steffen Bräkling, Sophia Brilke, Lucia Caudillo, Dexian Chen, Biwu Chu, António Dias, Danielle C. Draper, Jonathan Duplissy, Imad El-Haddad, Henning Finkenzeller, Carla Frege, Loic Gonzalez-Carracedo, Hamish Gordon, Manuel Granzin, Jani Hakala, Victoria Hofbauer, Christopher R. Hoyle, Changhyuk Kim, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Bernhard Mentler, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Lauriane L. J. Quéléver, Ananth Ranjithkumar, Matti P. Rissanen, Simon Schallhart, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee J. Tham, António R. Tomé, Miguel Vazquez-Pufleau, Alexander L. Vogel, Robert Wagner, Mingyi Wang, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, Yusheng Wu, Mao Xiao, Chao Yan, Penglin Ye, Qing Ye, Marcel Zauner-Wieczorek, Xueqin Zhou, Urs Baltensperger, Josef Dommen, Richard C. Flagan, Armin Hansel, Markku Kulmala, Rainer Volkamer, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 9183–9207, https://doi.org/10.5194/acp-20-9183-2020, https://doi.org/10.5194/acp-20-9183-2020, 2020
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Highly oxygenated organic compounds (HOMs) have been identified as key vapors involved in atmospheric new-particle formation (NPF). The molecular distribution, HOM yield, and NPF from α-pinene oxidation experiments were measured at the CLOUD chamber over a wide tropospheric-temperature range. This study shows on a molecular scale that despite the sharp reduction in HOM yield at lower temperatures, the reduced volatility counteracts this effect and leads to an overall increase in the NPF rate.
Angela Buchholz, Arttu Ylisirniö, Wei Huang, Claudia Mohr, Manjula Canagaratna, Douglas R. Worsnop, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 20, 7693–7716, https://doi.org/10.5194/acp-20-7693-2020, https://doi.org/10.5194/acp-20-7693-2020, 2020
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To understand the role of aerosol particles in the atmosphere, it is necessary to know their detailed chemical composition and physical properties, especially volatility. The thermal desorption data from FIGAERO–CIMS provides both but are difficult to analyse. With positive matrix factorisation, we can separate instrument background from the real signal. Compounds can be classified by their apparent volatility, and the contribution of thermal decomposition in the instrument can be identified.
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.
Jian Xu, Jia Chen, Na Zhao, Guochen Wang, Guangyuan Yu, Hao Li, Juntao Huo, Yanfen Lin, Qingyan Fu, Hongyu Guo, Congrui Deng, Shan-Hu Lee, Jianmin Chen, and Kan Huang
Atmos. Chem. Phys., 20, 7259–7269, https://doi.org/10.5194/acp-20-7259-2020, https://doi.org/10.5194/acp-20-7259-2020, 2020
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This study provided evidence that gas-particle partitioning of ammonia, as opposed to ammonia concentration, plays a critical role in the haze formation. A reduction in ammonia emissions alone may not reduce air pollution effectively, at least at rural agricultural sites in China.
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.
Yanjun Zhang, Otso Peräkylä, Chao Yan, Liine Heikkinen, Mikko Äijälä, Kaspar R. Daellenbach, Qiaozhi Zha, Matthieu Riva, Olga Garmash, Heikki Junninen, Pentti Paatero, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 20, 5945–5961, https://doi.org/10.5194/acp-20-5945-2020, https://doi.org/10.5194/acp-20-5945-2020, 2020
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By utilizing a new analysis approach, we investigated atmospheric oxidation of biogenic volatile emissions in a Finnish forest, measured by chemical ionization mass spectrometry. We identified several new compound groups, including low-volatility accretion products and their formation pathways. Results from this study are important for understanding atmospheric aerosol formation, as well as providing new perspectives on future lab studies and data analysis of short-lived species.
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.
Arttu Ylisirniö, Angela Buchholz, Claudia Mohr, Zijun Li, Luis Barreira, Andrew Lambe, Celia Faiola, Eetu Kari, Taina Yli-Juuti, Sergey A. Nizkorodov, Douglas R. Worsnop, Annele Virtanen, and Siegfried Schobesberger
Atmos. Chem. Phys., 20, 5629–5644, https://doi.org/10.5194/acp-20-5629-2020, https://doi.org/10.5194/acp-20-5629-2020, 2020
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We studied the chemical composition and volatility of secondary organic aerosol (SOA) particles formed from emissions of Scots pines and compared those results to SOA formed from α-pinene and from a sesquiterpene mixture. We found that SOA formed from single precursors cannot capture the properties of SOA formed from real plant emissions.
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.
Jing Duan, Ru-Jin Huang, Yongjie Li, Qi Chen, Yan Zheng, Yang Chen, Chunshui Lin, Haiyan Ni, Meng Wang, Jurgita Ovadnevaite, Darius Ceburnis, Chunying Chen, Douglas R. Worsnop, Thorsten Hoffmann, Colin O'Dowd, and Junji Cao
Atmos. Chem. Phys., 20, 3793–3807, https://doi.org/10.5194/acp-20-3793-2020, https://doi.org/10.5194/acp-20-3793-2020, 2020
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We characterized secondary aerosol formation in Beijing. Our results showed that relative humidity (RH) and Ox have opposite effects on sulfate and nitrate formation in summer and winter. The wintertime more-oxidized OOA (MO-OOA) showed a good correlation with aerosol liquid water content (ALWC). Meanwhile, the dependence of less-oxidized OOA (LO-OOA) and the mass ratio of LO-OOA to MO-OOA in Ox both degraded when RH > 60 %, suggesting that RH or ALWC may also affect LO-OOA formation.
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.
Liine Heikkinen, Mikko Äijälä, Matthieu Riva, Krista Luoma, Kaspar Dällenbach, Juho Aalto, Pasi Aalto, Diego Aliaga, Minna Aurela, Helmi Keskinen, Ulla Makkonen, Pekka Rantala, Markku Kulmala, Tuukka Petäjä, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 20, 3151–3180, https://doi.org/10.5194/acp-20-3151-2020, https://doi.org/10.5194/acp-20-3151-2020, 2020
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Atmospheric aerosols are solid or liquid particles suspended in the air. They are known as a health risk, but they also influence the Earth's climate. The composition of aerosols becomes important when predicting their effect on climate. We show both seasonal and year-to-year variability of aerosol chemical composition in the boreal forest of Finland. We observed a consistent bimodal seasonal trend: a biogenic summertime maximum and an anthropogenic wintertime maximum in the mass concentration.
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.
Michael Biggart, Jenny Stocker, Ruth M. Doherty, Oliver Wild, Michael Hollaway, David Carruthers, Jie Li, Qiang Zhang, Ruili Wu, Simone Kotthaus, Sue Grimmond, Freya A. Squires, James Lee, and Zongbo Shi
Atmos. Chem. Phys., 20, 2755–2780, https://doi.org/10.5194/acp-20-2755-2020, https://doi.org/10.5194/acp-20-2755-2020, 2020
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Ambient air pollution is a major cause of premature death in China. We examine the street-scale variation of pollutant levels in Beijing using air pollution dispersion and chemistry model ADMS-Urban. Campaign measurements are compared with simulated pollutant levels, providing a valuable means of evaluating the impact of key processes on urban air quality. Air quality modelling at such fine scales is essential for human exposure studies and for informing choices on future emission controls.
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.
Haiyan Li, Matthieu Riva, Pekka Rantala, Liine Heikkinen, Kaspar Daellenbach, Jordan E. Krechmer, Pierre-Marie Flaud, Douglas Worsnop, Markku Kulmala, Eric Villenave, Emilie Perraudin, Mikael Ehn, and Federico Bianchi
Atmos. Chem. Phys., 20, 1941–1959, https://doi.org/10.5194/acp-20-1941-2020, https://doi.org/10.5194/acp-20-1941-2020, 2020
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We deployed the recently developed Vocus PTR-TOF in the French Landes forest during summertime to gain insights into terpene chemistry. In addition to isoprene, monoterpenes, sesquiterpenes, and the low-volatility diterpenes, various terpene reaction products are characterized. Through the analysis of terpene chemistry, we demonstrate the capability of the Vocus PTR-TOF for the detection of oxidized reaction products, highlighting its importance in investigating atmospheric oxidation processes.
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.
Yongjoo Choi, Yugo Kanaya, Seung-Myung Park, Atsushi Matsuki, Yasuhiro Sadanaga, Sang-Woo Kim, Itsushi Uno, Xiaole Pan, Meehye Lee, Hyunjae Kim, and Dong Hee Jung
Atmos. Chem. Phys., 20, 83–98, https://doi.org/10.5194/acp-20-83-2020, https://doi.org/10.5194/acp-20-83-2020, 2020
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The relationship between black carbon (BC) and carbon monoxide (CO) can differ by the different structure of fuel consumption. By investigating the representativeness of the BC and CO emission inventory for real-world comparison with reliable observations, this study suggested that accurate CO emissions should be preferentially investigated to enhance the accuracy of the BC emission rate over East Asia.
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.
Alexander Zaytsev, Abigail R. Koss, Martin Breitenlechner, Jordan E. Krechmer, Kevin J. Nihill, Christopher Y. Lim, James C. Rowe, Joshua L. Cox, Joshua Moss, Joseph R. Roscioli, Manjula R. Canagaratna, Douglas R. Worsnop, Jesse H. Kroll, and Frank N. Keutsch
Atmos. Chem. Phys., 19, 15117–15129, https://doi.org/10.5194/acp-19-15117-2019, https://doi.org/10.5194/acp-19-15117-2019, 2019
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Aromatic hydrocarbons contribute significantly to the production of tropospheric ozone and secondary organic aerosol (SOA). Here later-generation low-volatility oxygenated products from toluene and 1,2,4-TMB oxidation by OH are detected in the gas and particle phases. We show that these products, previously identified as highly oxygenated molecules (HOMs), are formed in more than one pathway with differing numbers of reaction steps with OH. They also make up a significant fraction of SOA.
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.
Gang Zhao, Jiangchuan Tao, Ye Kuang, Chuanyang Shen, Yingli Yu, and Chunsheng Zhao
Atmos. Chem. Phys., 19, 13175–13188, https://doi.org/10.5194/acp-19-13175-2019, https://doi.org/10.5194/acp-19-13175-2019, 2019
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Characteristics of the black carbon size distribution (BCMSD) are studied by using our developed measurement system. Results show that the BCMSDs have two modes and the mean peak diameters are 150 nm and 503 nm, respectively. The coarser mode varies significantly under different pollution conditions, which gives rise to significant variation in aerosol bulk optical properties. Our study reveals that the BCMSD as well as the mixing state in estimating aerosol radiative forcing matters.
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.
Xuan Zhang, Haofei Zhang, Wen Xu, Xiaokang Wu, Geoffrey S. Tyndall, John J. Orlando, John T. Jayne, Douglas R. Worsnop, and Manjula R. Canagaratna
Atmos. Meas. Tech., 12, 5535–5545, https://doi.org/10.5194/amt-12-5535-2019, https://doi.org/10.5194/amt-12-5535-2019, 2019
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We develop a new technique to characterize organic nitrates as intact molecules in atmospheric aerosols, and we apply this technique to identify hydroxy nitrates in secondary organic aerosols produced from the photochemical oxidation of isoprene.
Eleni Dovrou, Christopher Y. Lim, Manjula R. Canagaratna, Jesse H. Kroll, Douglas R. Worsnop, and Frank N. Keutsch
Atmos. Meas. Tech., 12, 5303–5315, https://doi.org/10.5194/amt-12-5303-2019, https://doi.org/10.5194/amt-12-5303-2019, 2019
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Measurement techniques commonly used to analyze particulate matter composition can result in the possible misidentification of sulfur-containing species, especially for the case of sulfate and hydroxymethanesulfonate (HMS). The efficiency and limitations of these techniques, along with a method that enables further studies of the contribution of sulfur-containing species, S(IV) versus S(VI), to particulate matter under low-light atmospheric conditions, are described in this work.
Leonid Nichman, Martin Wolf, Paul Davidovits, Timothy B. Onasch, Yue Zhang, Doug R. Worsnop, Janarjan Bhandari, Claudio Mazzoleni, and Daniel J. Cziczo
Atmos. Chem. Phys., 19, 12175–12194, https://doi.org/10.5194/acp-19-12175-2019, https://doi.org/10.5194/acp-19-12175-2019, 2019
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Previous studies showed widespread ice nucleation activity of soot. In this systematic study we investigated the factors that affect the heterogeneous ice nucleation activity of soot surrogates in the cirrus cloud regime. Our observations are consistent with an ice nucleation mechanism of pore condensation followed by freezing. The results show significant variations in ice nucleation activity as a function of size, morphology, and surface chemistry of the black-carbon-containing particles.
Xiaoxiao Li, Shaojie Song, Wei Zhou, Jiming Hao, Douglas R. Worsnop, and Jingkun Jiang
Atmos. Chem. Phys., 19, 12163–12174, https://doi.org/10.5194/acp-19-12163-2019, https://doi.org/10.5194/acp-19-12163-2019, 2019
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Aerosol liquid water is ubiquitous in ambient aerosol. Using long-term aerosol chemical composition to model the aerosol water in Beijing, we found that water absorbed by organics contributes a significant fraction to the total aerosol water. We emphasize the hygroscopicity of organics is highly variable and should be taken into consideration in modelling. A positive feedback loop between organic hygroscopicity and aerosol water was found as one of the driving factors of severe haze in Beijing.
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.
Wanyun Xu, Ye Kuang, Chunsheng Zhao, Jiangchuan Tao, Gang Zhao, Yuxuan Bian, Wen Yang, Yingli Yu, Chuanyang Shen, Linlin Liang, Gen Zhang, Weili Lin, and Xiaobin Xu
Atmos. Chem. Phys., 19, 10557–10570, https://doi.org/10.5194/acp-19-10557-2019, https://doi.org/10.5194/acp-19-10557-2019, 2019
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The study of HONO, the primary source of OH radicals, is crucial for atmospheric photochemistry and heterogeneous chemistry. Heterogeneous NO2 conversion was shown to be one of the missing sources of HONO on the North China Plain, but the reaction path is still under debate. In this work, evidence was found that NH3 was the key factor that promoted the hydrolysis of NO2, leading to the explosive growth of HONO and nitrate, suggesting that NH3 emission control measures are urgently needed.
Jing Duan, Ru-Jin Huang, Chunshui Lin, Wenting Dai, Meng Wang, Yifang Gu, Ying Wang, Haobin Zhong, Yan Zheng, Haiyan Ni, Uli Dusek, Yang Chen, Yongjie Li, Qi Chen, Douglas R. Worsnop, Colin D. O'Dowd, and Junji Cao
Atmos. Chem. Phys., 19, 10319–10334, https://doi.org/10.5194/acp-19-10319-2019, https://doi.org/10.5194/acp-19-10319-2019, 2019
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We present the seasonal distinction of secondary aerosol formation in urban Beijing. Both photochemical oxidation and aqueous-phase processing played important roles in SOA (secondary organic aerosol) formation during all three seasons; while for sulfate formation, gas-phase photochemical oxidation was the major pathway in late summer, aqueous-phase reactions were more responsible during early winter, and both processes had contributions during autumn.
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.
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.
Jianming Xu, Xuexi Tie, Wei Gao, Yanfen Lin, and Qingyan Fu
Atmos. Chem. Phys., 19, 9017–9035, https://doi.org/10.5194/acp-19-9017-2019, https://doi.org/10.5194/acp-19-9017-2019, 2019
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The PM2.5 in China has decreased significantly in recent years as a result of the implementation of the Chinese Clean Air Action Plan in 2013, while the O3 pollution is getting worse, especially in megacities. The work aims to better understand the elevated O3 pollution in the megacity of Shanghai, China, and its response to emission changes, which is important for developing an effective emission control strategy in the future.
Sanna Saarikoski, Leah R. Williams, Steven R. Spielman, Gregory S. Lewis, Arantzazu Eiguren-Fernandez, Minna Aurela, Susanne V. Hering, Kimmo Teinilä, Philip Croteau, John T. Jayne, Thorsten Hohaus, Douglas R. Worsnop, and Hilkka Timonen
Atmos. Meas. Tech., 12, 3907–3920, https://doi.org/10.5194/amt-12-3907-2019, https://doi.org/10.5194/amt-12-3907-2019, 2019
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An air-to-air ultrafine particle concentrator (Aerosol Dynamics Inc. concentrator; ADIc) has been tailored for the low (~ 0.08 L min−1) inlet flow of aerosol mass spectrometers, and it provides a factor of 8–21 enrichment in the concentration of particles. The ADIc was evaluated in laboratory and field measurements. The results showed that the concentration factor depends primarily on the ratio between the sample flow and the output flow and is independent of particle size above about 10 nm.
Yanjun Zhang, Otso Peräkylä, Chao Yan, Liine Heikkinen, Mikko Äijälä, Kaspar R. Daellenbach, Qiaozhi Zha, Matthieu Riva, Olga Garmash, Heikki Junninen, Pentti Paatero, Douglas Worsnop, and Mikael Ehn
Atmos. Meas. Tech., 12, 3761–3776, https://doi.org/10.5194/amt-12-3761-2019, https://doi.org/10.5194/amt-12-3761-2019, 2019
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Recent advancements in atmospheric mass spectrometry provide large amounts of new information but at the same time present considerable challenges for the data analysis, for example, in high-resolution peak identification and separation. To address these problems, this study presents a simple and novel method, which succeeds in analyzing both synthetic and ambient datasets. We believe it will become a powerful approach in the data analysis of mass spectra.
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.
Yugo Kanaya, Kazuyuki Miyazaki, Fumikazu Taketani, Takuma Miyakawa, Hisahiro Takashima, Yuichi Komazaki, Xiaole Pan, Saki Kato, Kengo Sudo, Takashi Sekiya, Jun Inoue, Kazutoshi Sato, and Kazuhiro Oshima
Atmos. Chem. Phys., 19, 7233–7254, https://doi.org/10.5194/acp-19-7233-2019, https://doi.org/10.5194/acp-19-7233-2019, 2019
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Ozone and carbon monoxide levels were uniquely observed (for > 10 000 h) over oceans from 67° S to 75° N. Tropospheric chemistry reanalysis v2 reproduced the observed evolution of pollution plumes from continents but underpredicted and overpredicted ozone levels in the Arctic and in the western Pacific equatorial region, respectively. Processes to explain the gaps are proposed, including halogen-mediated destruction in the low latitudes. Our open data set will complement the TOAR data collection.
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.
Yue Liu, Mei Zheng, Mingyuan Yu, Xuhui Cai, Huiyun Du, Jie Li, Tian Zhou, Caiqing Yan, Xuesong Wang, Zongbo Shi, Roy M. Harrison, Qiang Zhang, and Kebin He
Atmos. Chem. Phys., 19, 6595–6609, https://doi.org/10.5194/acp-19-6595-2019, https://doi.org/10.5194/acp-19-6595-2019, 2019
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This study is part of the UK–China APHH campaign. To identify both source types and source regions at the same time, this study developed a combined method including receptor model, footprint model, and air quality model for the first time to investigate sources of PM2.5 during haze episodes in Beijing. It is an expansion of the application of the receptor model and is helpful for formulating effective control strategies to improve air quality in this region.
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.
Xinning Wang, Yin Shen, Yanfen Lin, Jun Pan, Yan Zhang, Peter K. K. Louie, Mei Li, and Qingyan Fu
Atmos. Chem. Phys., 19, 6315–6330, https://doi.org/10.5194/acp-19-6315-2019, https://doi.org/10.5194/acp-19-6315-2019, 2019
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Shipping emissions were measured online at Shanghai Port, and their impacts on local air quality at the port and in the surrounding area were quantitatively assessed. Ship emission plumes were readily detectable before they dissipated. We captured ship emission plumes using synchronized peaks of SO2 and vanadium particles. By measuring the pollutant concentrations during plumes and their occurrence frequency, we made quantitative estimations of ship emission impacts on port air quality.
Junlan Feng, Yan Zhang, Shanshan Li, Jingbo Mao, Allison P. Patton, Yuyan Zhou, Weichun Ma, Cong Liu, Haidong Kan, Cheng Huang, Jingyu An, Li Li, Yin Shen, Qingyan Fu, Xinning Wang, Juan Liu, Shuxiao Wang, Dian Ding, Jie Cheng, Wangqi Ge, Hong Zhu, and Katherine Walker
Atmos. Chem. Phys., 19, 6167–6183, https://doi.org/10.5194/acp-19-6167-2019, https://doi.org/10.5194/acp-19-6167-2019, 2019
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This study aims to estimate the emissions, air quality and population exposure impacts of shipping in 2015, prior to the implementation of the DECAs. It shows that ship emissions within 12 NM of the shore could account for over 55 % of the shipping impact on air pollution in the YRD in summer. Ships entering the Yangtze River and other inland waterways of Shanghai contribute 40–80 % of the ship-related air pollution and population exposure,which both have important implications regarding policy.
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.
Xiaofei Qin, Xiaohao Wang, Yijie Shi, Guangyuan Yu, Na Zhao, Yanfen Lin, Qingyan Fu, Dongfang Wang, Zhouqing Xie, Congrui Deng, and Kan Huang
Atmos. Chem. Phys., 19, 5923–5940, https://doi.org/10.5194/acp-19-5923-2019, https://doi.org/10.5194/acp-19-5923-2019, 2019
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The seasonal pattern of atmospheric mercury species over a regional transport intersection zone in east China indicated impacts from both natural re-emissions and anthropogenic emissions. Quasi-local sources were more important than long-range transport for mercury, opposite from particles. Shipping activities were especially outstanding emissions. Abnormally high GOM was ascribed to the high oxidant levels. The gas–particle partition inhibited the formation of GOM under high particle levels.
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
Matthieu Riva, Pekka Rantala, Jordan E. Krechmer, Otso Peräkylä, Yanjun Zhang, Liine Heikkinen, Olga Garmash, Chao Yan, Markku Kulmala, Douglas Worsnop, and Mikael Ehn
Atmos. Meas. Tech., 12, 2403–2421, https://doi.org/10.5194/amt-12-2403-2019, https://doi.org/10.5194/amt-12-2403-2019, 2019
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The impact of aerosol particles on climate and air quality remains poorly understood due to multiple factors. One of the current limitations is the incomplete understanding of the contribution of oxygenated species, formed from the oxidation of volatile organic compounds (VOCs) to aerosol formation. Taking advantage of recent mass spectrometric developments, we have evaluated and compared the capability of multiple state-of-the-art mass spectrometers to detect a wide variety of oxygenated VOCs.
Angela Buchholz, Andrew T. Lambe, Arttu Ylisirniö, Zijun Li, Olli-Pekka Tikkanen, Celia Faiola, Eetu Kari, Liqing Hao, Olli Luoma, Wei Huang, Claudia Mohr, Douglas R. Worsnop, Sergey A. Nizkorodov, Taina Yli-Juuti, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 19, 4061–4073, https://doi.org/10.5194/acp-19-4061-2019, https://doi.org/10.5194/acp-19-4061-2019, 2019
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We studied the evaporation of α-pinene secondary organic aerosol particles in clean air to derive their volatility from the observed size changes. We found that the particles became more resilient to evaporation with increased oxidative age, possibly increasing their lifetime in the atmosphere. Also, increased relative humidity increased the particle evaporation. Mass spectrometry measurements of the particles at different stages of evaporation revealed some water-induced composition changes.
Zhaofeng Tan, Keding Lu, Meiqing Jiang, Rong Su, Hongli Wang, Shengrong Lou, Qingyan Fu, Chongzhi Zhai, Qinwen Tan, Dingli Yue, Duohong Chen, Zhanshan Wang, Shaodong Xie, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 19, 3493–3513, https://doi.org/10.5194/acp-19-3493-2019, https://doi.org/10.5194/acp-19-3493-2019, 2019
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We evaluated the atmospheric oxidation capacity (AOC) in four Chinese megacities during photochemically polluted seasons. The chemical production of ozone and particle nitrate was diagnosed through a box model, which can be attributed to daytime radical chemistry. Our work highlights that the formation of both ozone and fine particles is largely driven by the atmospheric radical chemistry in China. Consequently, we suggest future pollution mitigation strategies should consider the role of AOC.
Rachel E. O'Brien, Kelsey J. Ridley, Manjula R. Canagaratna, John T. Jayne, Philip L. Croteau, Douglas R. Worsnop, Sri Hapsari Budisulistiorini, Jason D. Surratt, Christopher L. Follett, Daniel J. Repeta, and Jesse H. Kroll
Atmos. Meas. Tech., 12, 1659–1671, https://doi.org/10.5194/amt-12-1659-2019, https://doi.org/10.5194/amt-12-1659-2019, 2019
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Analysis of the elemental composition of organic mixtures can provide insights into the sources and aging of environmental samples. Here we describe a method that allows characterization of this type of material using micrograms of material by a combination of a small-volume ultrasonic nebulizer and an aerosol mass spectrometer. This technique enables rapid analysis of complex organic mixtures using approximately an order of magnitude less sample than standard analyses.
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.
Ru-Jin Huang, Yichen Wang, Junji Cao, Chunshui Lin, Jing Duan, Qi Chen, Yongjie Li, Yifang Gu, Jin Yan, Wei Xu, Roman Fröhlich, Francesco Canonaco, Carlo Bozzetti, Jurgita Ovadnevaite, Darius Ceburnis, Manjula R. Canagaratna, John Jayne, Douglas R. Worsnop, Imad El-Haddad, André S. H. Prévôt, and Colin D. O'Dowd
Atmos. Chem. Phys., 19, 2283–2298, https://doi.org/10.5194/acp-19-2283-2019, https://doi.org/10.5194/acp-19-2283-2019, 2019
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We found that in wintertime Shijiazhuang fine PM was mostly from primary emissions without sufficient atmospheric aging. In addition, secondary inorganic and organic aerosol dominated in pollution events under high-RH conditions, likely due to enhanced aqueous-phase chemistry, whereas primary organic aerosol dominated in pollution events under low-RH and stagnant conditions. Our results also highlighted the importance of meteorological conditions for PM pollution in this highly polluted city.
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.
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.
Andrew T. Lambe, Jordan E. Krechmer, Zhe Peng, Jason R. Casar, Anthony J. Carrasquillo, Jonathan D. Raff, Jose L. Jimenez, and Douglas R. Worsnop
Atmos. Meas. Tech., 12, 299–311, https://doi.org/10.5194/amt-12-299-2019, https://doi.org/10.5194/amt-12-299-2019, 2019
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This paper is an evaluation of methods used to generate OH radicals under conditions with high concentrations of NO and NO2 to simulate oxidation chemistry in polluted urban atmospheres over equivalent atmospheric timescales of ~ 1 day.
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.
Liqing Hao, Olga Garmash, Mikael Ehn, Pasi Miettinen, Paola Massoli, Santtu Mikkonen, Tuija Jokinen, Pontus Roldin, Pasi Aalto, Taina Yli-Juuti, Jorma Joutsensaari, Tuukka Petäjä, Markku Kulmala, Kari E. J. Lehtinen, Douglas R. Worsnop, and Annele Virtanen
Atmos. Chem. Phys., 18, 17705–17716, https://doi.org/10.5194/acp-18-17705-2018, https://doi.org/10.5194/acp-18-17705-2018, 2018
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An aerosol mass spectrometer was used to characterize aerosol chemical composition during new particle formation periods. The time profiles of mass concentrations and chemical composition of observed aerosol particles are subjected to joint effects of boundary layer dilution, atmospheric chemistry and aerosol mixing in different boundary layers. During the nighttime, the increase in organic aerosol mass correlated well with the increase in condensed highly oxygenated organic molecules' mass.
Qiaozhi Zha, Chao Yan, Heikki Junninen, Matthieu Riva, Nina Sarnela, Juho Aalto, Lauriane Quéléver, Simon Schallhart, Lubna Dada, Liine Heikkinen, Otso Peräkylä, Jun Zou, Clémence Rose, Yonghong Wang, Ivan Mammarella, Gabriel Katul, Timo Vesala, Douglas R. Worsnop, Markku Kulmala, Tuukka Petäjä, Federico Bianchi, and Mikael Ehn
Atmos. Chem. Phys., 18, 17437–17450, https://doi.org/10.5194/acp-18-17437-2018, https://doi.org/10.5194/acp-18-17437-2018, 2018
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Vertical measurements of highly oxygenated molecules (HOMs) below and above the forest canopy were performed for the first time in a boreal forest during September 2016. Our results highlight that near-ground HOM measurements may only be representative of a small fraction of the entire nocturnal boundary layer, which may sequentially influence the growth of newly formed particles and SOA formation close to ground surface, where the majority of measurements are conducted.
Yangyang Zhang, Aohan Tang, Dandan Wang, Qingqing Wang, Katie Benedict, Lin Zhang, Duanyang Liu, Yi Li, Jeffrey L. Collett Jr., Yele Sun, and Xuejun Liu
Atmos. Chem. Phys., 18, 16385–16398, https://doi.org/10.5194/acp-18-16385-2018, https://doi.org/10.5194/acp-18-16385-2018, 2018
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Our study is the first to continually monitor the vertical concentration profile of NH3 in urban Beijing. Weekly concentrations averaged 13.3 ± 4.8 μg m−3. The highest NH3 concentrations were always observed between 32 and 63 m, decreasing toward the surface and toward higher altitudes. Our results demonstrate a NH3 rich atmosphere in urban Beijing, from the ground to at least 320 m. Regional transport from the south (intensive agricultural regions) contributed high NH3 concentrations in Beijing.
Hansen Cao, Tzung-May Fu, Lin Zhang, Daven K. Henze, Christopher Chan Miller, Christophe Lerot, Gonzalo González Abad, Isabelle De Smedt, Qiang Zhang, Michel van Roozendael, François Hendrick, Kelly Chance, Jie Li, Junyu Zheng, and Yuanhong Zhao
Atmos. Chem. Phys., 18, 15017–15046, https://doi.org/10.5194/acp-18-15017-2018, https://doi.org/10.5194/acp-18-15017-2018, 2018
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Our top-down estimates for annual total Chinese NMVOC emissions was 30.7 to 49.5 Tg y−1, including 16.4 to 23.6 Tg y−1 from anthropogenic sources, 12.2 to 22.8 Tg y−1 from biogenic sources, and 2.08 to 3.13 Tg y−1 from biomass burning. Our four inversions consistently showed that the emissions of Chinese anthropogenic NMVOC precursors of glyoxal were larger than the a priori estimates. The glyoxal and formaldehyde constraints helped distinguish the NMVOC species from different sources.
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.
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.
Gang Zhao, Chunsheng Zhao, Ye Kuang, Yuxuan Bian, Jiangchuan Tao, Chuanyang Shen, and Yingli Yu
Atmos. Chem. Phys., 18, 9049–9060, https://doi.org/10.5194/acp-18-9049-2018, https://doi.org/10.5194/acp-18-9049-2018, 2018
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The aerosol asymmetry factor (g) is one of the most important factors for assessing direct aerosol radiative forcing (DARF) and remote sensing. So far, few studies have focused on the measurements and parameterization of g. Our study shows that relative humidity has significant impacts on g and DARF due to aerosol hygroscopic growth. For the first time, a novel method based on measurements from the humidified nephelometer system is proposed to calculate g accurately with high time resolution.
Yue Zhang, Shachi Katira, Andrew Lee, Andrew T. Lambe, Timothy B. Onasch, Wen Xu, William A. Brooks, Manjula R. Canagaratna, Andrew Freedman, John T. Jayne, Doug R. Worsnop, Paul Davidovits, David Chandler, and Charles E. Kolb
Atmos. Meas. Tech., 11, 3479–3490, https://doi.org/10.5194/amt-11-3479-2018, https://doi.org/10.5194/amt-11-3479-2018, 2018
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We have adopted a new technique for measuring glass-forming properties of atmospherically relevant organic aerosols at submicron sizes and relatively low mass concentrations. Aerosol particles are deposited in the form of a thin film with interdigitated electrodes using electrostatic precipitation. Broadband dielectric spectroscopy is used to measure the kinetically controlled glass transition temperatures of glycerol and citric acid aerosols with three atmospheric relevant cooling rates.
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.
Ye Kuang, Chun Sheng Zhao, Gang Zhao, Jiang Chuan Tao, Wanyun Xu, Nan Ma, and Yu Xuan Bian
Atmos. Meas. Tech., 11, 2967–2982, https://doi.org/10.5194/amt-11-2967-2018, https://doi.org/10.5194/amt-11-2967-2018, 2018
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Aerosol water has become an important topic recently because of its implications for multiphase secondary aerosol formation during severe haze events in Asia. This is a timely paper on this topic; a novel method is proposed to calculate ambient aerosol liquid water contents based only on measurements of a three-wavelength humidified nephelometer system. The advantage of this method is that this technique can provide continuous measurements of the changing ambient conditions.
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
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.
Qiongzhen Wang, Xinyi Dong, Joshua S. Fu, Jian Xu, Congrui Deng, Yilun Jiang, Qingyan Fu, Yanfen Lin, Kan Huang, and Guoshun Zhuang
Atmos. Chem. Phys., 18, 3505–3521, https://doi.org/10.5194/acp-18-3505-2018, https://doi.org/10.5194/acp-18-3505-2018, 2018
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A synergy of ground-based atmospheric chemistry observation, lidar, and numerical modeling was used to investigate a super dust event passing over Shanghai. The degree of dust that was modified by anthropogenic sources highly depended on the transport pathways. A community regional air quality model with improved dust scheme reproduced reasonable dust chemistry results. The chemical and optical properties of evolving dust are crucial for evaluating the climatic effects of dust.
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.
Nina Sarnela, Tuija Jokinen, Jonathan Duplissy, Chao Yan, Tuomo Nieminen, Mikael Ehn, Siegfried Schobesberger, Martin Heinritzi, Sebastian Ehrhart, Katrianne Lehtipalo, Jasmin Tröstl, Mario Simon, Andreas Kürten, Markus Leiminger, Michael J. Lawler, Matti P. Rissanen, Federico Bianchi, Arnaud P. Praplan, Jani Hakala, Antonio Amorim, Marc Gonin, Armin Hansel, Jasper Kirkby, Josef Dommen, Joachim Curtius, James N. Smith, Tuukka Petäjä, Douglas R. Worsnop, Markku Kulmala, Neil M. Donahue, and Mikko Sipilä
Atmos. Chem. Phys., 18, 2363–2380, https://doi.org/10.5194/acp-18-2363-2018, https://doi.org/10.5194/acp-18-2363-2018, 2018
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Atmospheric trace gases can form small molecular clusters, which can grow to larger sizes through the condensation of vapours. This process is called new particle formation. In this paper we studied the formation of sulfuric acid and highly oxygenated molecules, the key compounds in atmospheric new particle formation, in chamber experiments and introduced a way to simulate these ozonolysis products of α-pinene in a simple manner.
Jiangchuan Tao, Chunsheng Zhao, Ye Kuang, Gang Zhao, Chuanyang Shen, Yingli Yu, Yuxuan Bian, and Wanyun Xu
Atmos. Meas. Tech., 11, 895–906, https://doi.org/10.5194/amt-11-895-2018, https://doi.org/10.5194/amt-11-895-2018, 2018
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Existing chamber technologies for direct measurements of number concentration of cloud condensation nuclei (NCCN) are sophisticated and expensive. In this paper, a new method is proposed to calculate NCCN based only on measurements of a humidified nephelometer system which have accounted for influences of both aerosol size and aerosol hygroscopicity on NCCN calculation. This new method makes NCCN measurements more convenient and is capable of obtaining NCCN at lower supersaturations.
Carla Frege, Ismael K. Ortega, Matti P. Rissanen, Arnaud P. Praplan, Gerhard Steiner, Martin Heinritzi, Lauri Ahonen, António Amorim, Anne-Kathrin Bernhammer, Federico Bianchi, Sophia Brilke, Martin Breitenlechner, Lubna Dada, António Dias, Jonathan Duplissy, Sebastian Ehrhart, Imad El-Haddad, Lukas Fischer, Claudia Fuchs, Olga Garmash, Marc Gonin, Armin Hansel, Christopher R. Hoyle, Tuija Jokinen, Heikki Junninen, Jasper Kirkby, Andreas Kürten, Katrianne Lehtipalo, Markus Leiminger, Roy Lee Mauldin, Ugo Molteni, Leonid Nichman, Tuukka Petäjä, Nina Sarnela, Siegfried Schobesberger, Mario Simon, Mikko Sipilä, Dominik Stolzenburg, António Tomé, Alexander L. Vogel, Andrea C. Wagner, Robert Wagner, Mao Xiao, Chao Yan, Penglin Ye, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Paul M. Winkler, Josef Dommen, and Urs Baltensperger
Atmos. Chem. Phys., 18, 65–79, https://doi.org/10.5194/acp-18-65-2018, https://doi.org/10.5194/acp-18-65-2018, 2018
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It was recently shown that biogenic highly oxygenated molecules (HOMs) form particles in the absence of sulfuric acid and ions enhance the nucleation rate. Here we compare the molecular composition of positive and negative HOM clusters at 25, 5 and −25 °C. At lower temperatures the HOM average oxygen-to-carbon ratio decreases indicating a reduction in the rate of autoxidation due to rather high activation energy. The experimental findings are supported by quantum chemical calculations.
Robert Wagner, Chao Yan, Katrianne Lehtipalo, Jonathan Duplissy, Tuomo Nieminen, Juha Kangasluoma, Lauri R. Ahonen, Lubna Dada, Jenni Kontkanen, Hanna E. Manninen, Antonio Dias, Antonio Amorim, Paulus S. Bauer, Anton Bergen, Anne-Kathrin Bernhammer, Federico Bianchi, Sophia Brilke, Stephany Buenrostro Mazon, Xuemeng Chen, Danielle C. Draper, Lukas Fischer, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Jani Hakala, Liine Heikkinen, Martin Heinritzi, Victoria Hofbauer, Christopher R. Hoyle, Jasper Kirkby, Andreas Kürten, Alexander N. Kvashnin, Tiia Laurila, Michael J. Lawler, Huajun Mai, Vladimir Makhmutov, Roy L. Mauldin III, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Felix Piel, Lauriane L. J. Quéléver, Matti P. Rissanen, Nina Sarnela, Simon Schallhart, Kamalika Sengupta, Mario Simon, Dominik Stolzenburg, Yuri Stozhkov, Jasmin Tröstl, Yrjö Viisanen, Alexander L. Vogel, Andrea C. Wagner, Mao Xiao, Penglin Ye, Urs Baltensperger, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Martin Gallagher, Armin Hansel, James N. Smith, António Tomé, Paul M. Winkler, Douglas Worsnop, Mikael Ehn, Mikko Sipilä, Veli-Matti Kerminen, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys., 17, 15181–15197, https://doi.org/10.5194/acp-17-15181-2017, https://doi.org/10.5194/acp-17-15181-2017, 2017
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.
Itsushi Uno, Kazuo Osada, Keiya Yumimoto, Zhe Wang, Syuichi Itahashi, Xiaole Pan, Yukari Hara, Yugo Kanaya, Shigekazu Yamamoto, and Thomas Duncan Fairlie
Atmos. Chem. Phys., 17, 14181–14197, https://doi.org/10.5194/acp-17-14181-2017, https://doi.org/10.5194/acp-17-14181-2017, 2017
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We analyzed long-term fine- and coarse-mode nitrate and related aerosols synergetic observations at Fukuoka, Japan. GEOS Chem model including dust and sea-salt acid uptake processes was used to assess the observed seasonal variation, and the impact of long-range transport from the Asian continent. A numerical model reproduced the seasonal variations of fine aerosols. For coarse nitrate, large-scale dust-nitrate outflow from China was confirmed during all dust events between January and June.
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.
Gang Zhao, Chunsheng Zhao, Ye Kuang, Jiangchuan Tao, Wangshu Tan, Yuxuan Bian, Jing Li, and Chengcai Li
Atmos. Chem. Phys., 17, 12133–12143, https://doi.org/10.5194/acp-17-12133-2017, https://doi.org/10.5194/acp-17-12133-2017, 2017
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In this paper, influences of aerosol hygroscopic growth on the lidar ratio are studied. Results indicate that both the magnitude and vertical structures of the retrieved aerosol extinction coefficient (σext) profile from lidar signals are significantly biased. This study proposes a feasible method for reducing the bias of retrieving the σext profile and this method can be implemented in operational retrieval of the aerosol σext profile and for pollution monitoring.
Eben S. Cross, Leah R. Williams, David K. Lewis, Gregory R. Magoon, Timothy B. Onasch, Michael L. Kaminsky, Douglas R. Worsnop, and John T. Jayne
Atmos. Meas. Tech., 10, 3575–3588, https://doi.org/10.5194/amt-10-3575-2017, https://doi.org/10.5194/amt-10-3575-2017, 2017
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Low-cost air quality sensor technologies offer new opportunities for fast and distributed measurements of air pollution, but a persistent characterization gap remains when it comes to evaluating sensor performance under realistic environmental sampling conditions. We present results from a newly developed integrated AQ-sensor system (ARISense) and demonstrate the utility of using high-dimensional model representation to improve the conversion of raw sensor signal to ambient concentration.
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.
Yuxuan Bian, Chunsheng Zhao, Wanyun Xu, Gang Zhao, Jiangchuan Tao, and Ye Kuang
Atmos. Meas. Tech., 10, 2313–2322, https://doi.org/10.5194/amt-10-2313-2017, https://doi.org/10.5194/amt-10-2313-2017, 2017
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Aerosol phase function is crucial for understanding the climate effects of aerosols. So far, there is a lack of instruments for measuring the aerosol phase function directly and accurately in laboratory studies and in situ measurements. A novel portable instrument with high angular range and resolution named
charge-coupled device-laser aerosol detective system(CCD-LADS) has been developed and validated for the measurement of the phase function of ambient aerosols in this study.
Andrew Lambe, Paola Massoli, Xuan Zhang, Manjula Canagaratna, John Nowak, Conner Daube, Chao Yan, Wei Nie, Timothy Onasch, John Jayne, Charles Kolb, Paul Davidovits, Douglas Worsnop, and William Brune
Atmos. Meas. Tech., 10, 2283–2298, https://doi.org/10.5194/amt-10-2283-2017, https://doi.org/10.5194/amt-10-2283-2017, 2017
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This work enables the study of NOx-influenced secondary organic aerosol formation chemistry in oxidation flow reactors to an extent that was not previously possible. The method uses reactions of exited oxygen O(1D) radicals (formed from ozone photolysis at 254 nm or nitrous oxide photolysis at 185 nm) with nitrous oxide (N2O) to produce NO. We demonstrate proof of concept using chemical ionization mass spectrometer measurements to detect gas-phase oxidation products of isoprene and α -pinene.
Jing Zheng, Min Hu, Zhuofei Du, Dongjie Shang, Zhaoheng Gong, Yanhong Qin, Jingyao Fang, Fangting Gu, Mengren Li, Jianfei Peng, Jie Li, Yuqia Zhang, Xiaofeng Huang, Lingyan He, Yusheng Wu, and Song Guo
Atmos. Chem. Phys., 17, 6853–6864, https://doi.org/10.5194/acp-17-6853-2017, https://doi.org/10.5194/acp-17-6853-2017, 2017
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By monitoring aerosol properties as a function of high-resolution chemical composition, this study sheds light on the evolution processes of particles in the Tibetan Plateau background environment during the pre-monsoon season. A positive matrix factorization analysis integrated with a mesoscale meteorological model clearly shows that the southeastern edge of the Tibetan Plateau was affected by air pollutants transported from active biomass burning areas in South Asia.
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.
Ye Kuang, Chunsheng Zhao, Jiangchuan Tao, Yuxuan Bian, Nan Ma, and Gang Zhao
Atmos. Chem. Phys., 17, 6651–6662, https://doi.org/10.5194/acp-17-6651-2017, https://doi.org/10.5194/acp-17-6651-2017, 2017
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A novel approach is proposed in this research to derive the aerosol hygroscopicity parameter based only on measurements from a humidified nephelometer system without any additional information about particle number size distribution and black carbon. New findings in this research can bridge the gap between κ-Köhler theory and the aerosol light-scattering enhancement factor and will make the humidified nephelometer system more convenient when it comes to aerosol hygroscopicity research.
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.
Hilkka Timonen, Panu Karjalainen, Erkka Saukko, Sanna Saarikoski, Päivi Aakko-Saksa, Pauli Simonen, Timo Murtonen, Miikka Dal Maso, Heino Kuuluvainen, Matthew Bloss, Erik Ahlberg, Birgitta Svenningsson, Joakim Pagels, William H. Brune, Jorma Keskinen, Douglas R. Worsnop, Risto Hillamo, and Topi Rönkkö
Atmos. Chem. Phys., 17, 5311–5329, https://doi.org/10.5194/acp-17-5311-2017, https://doi.org/10.5194/acp-17-5311-2017, 2017
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The effect of fuel ethanol content (10–100 %) on primary emissions and the subsequent secondary aerosol formation was investigated for a Euro 5 flex-fuel gasoline vehicle. The emissions were characterized during the New European Driving Cycle (NEDC) using high time-resolution instruments. The chemical composition of the exhaust particulate matter was studied using a soot particle aerosol mass spectrometer (SP-AMS), and the secondary aerosol formation was studied with an oxidation chamber.
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.
Juan Hong, Mikko Äijälä, Silja A. K. Häme, Liqing Hao, Jonathan Duplissy, Liine M. Heikkinen, Wei Nie, Jyri Mikkilä, Markku Kulmala, Nønne L. Prisle, Annele Virtanen, Mikael Ehn, Pauli Paasonen, Douglas R. Worsnop, Ilona Riipinen, Tuukka Petäjä, and Veli-Matti Kerminen
Atmos. Chem. Phys., 17, 4387–4399, https://doi.org/10.5194/acp-17-4387-2017, https://doi.org/10.5194/acp-17-4387-2017, 2017
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Estimates of volatility of secondary organic aerosols was characterized in a boreal forest environment of Hyytiälä, southern Finland. This was done by interpreting field measurements using a volatility tandem differential mobility analyzer (VTDMA) with a kinetic evaporation model and by applying positive matrix factorization (PMF) to high-resolution aerosol mass spectrometer data. About 16 % of the variation can be explained by the linear regression between the results from these two methods.
Ellis Shipley Robinson, Timothy B. Onasch, Douglas Worsnop, and Neil M. Donahue
Atmos. Meas. Tech., 10, 1139–1154, https://doi.org/10.5194/amt-10-1139-2017, https://doi.org/10.5194/amt-10-1139-2017, 2017
Wei Nie, Juan Hong, Silja A. K. Häme, Aijun Ding, Yugen Li, Chao Yan, Liqing Hao, Jyri Mikkilä, Longfei Zheng, Yuning Xie, Caijun Zhu, Zheng Xu, Xuguang Chi, Xin Huang, Yang Zhou, Peng Lin, Annele Virtanen, Douglas R. Worsnop, Markku Kulmala, Mikael Ehn, Jianzhen Yu, Veli-Matti Kerminen, and Tuukka Petäjä
Atmos. Chem. Phys., 17, 3659–3672, https://doi.org/10.5194/acp-17-3659-2017, https://doi.org/10.5194/acp-17-3659-2017, 2017
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HULIS are demonstrated to be important low-volatility, or even extremely low volatility, compounds in the organic aerosol phase. This sheds new light on the connection between atmospheric HULIS and ELVOCs. The interaction between HULIS and ammonium sulfate was found to decrease the volatility of the HULIS part in HULIS-AS mixed samples, indicating multiphase processes have the potential to lower the volatility of organic compounds in the aerosol phase.
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.
Mikko Äijälä, Liine Heikkinen, Roman Fröhlich, Francesco Canonaco, André S. H. Prévôt, Heikki Junninen, Tuukka Petäjä, Markku Kulmala, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 17, 3165–3197, https://doi.org/10.5194/acp-17-3165-2017, https://doi.org/10.5194/acp-17-3165-2017, 2017
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Mass spectrometric measurements commonly yield data on hundreds of variables over thousands of points in time. Refining and synthesising this “raw” data into chemical information necessitates the use of advanced, statistics-based data analysis techniques. Here we present an example of combining data dimensionality reduction (factorisation) with exploratory classification (clustering) and show that the results complement and broaden our current perspectives on aerosol chemical classification.
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.
Lei Yao, Ming-Yi Wang, Xin-Ke Wang, Yi-Jun Liu, Hang-Fei Chen, Jun Zheng, Wei Nie, Ai-Jun Ding, Fu-Hai Geng, Dong-Fang Wang, Jian-Min Chen, Douglas R. Worsnop, and Lin Wang
Atmos. Chem. Phys., 16, 14527–14543, https://doi.org/10.5194/acp-16-14527-2016, https://doi.org/10.5194/acp-16-14527-2016, 2016
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We present the development of a high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) method, utilizing protonated ethanol as reagent ions to simultaneously detect atmospheric gaseous amines (C1 to C6) and amides (C1 to C6). Deployment of this ethanol HR-ToF-CIMS has been demonstrated in a field campaign in urban Shanghai, China, detecting amines (from a few pptv to hundreds of pptv) and amides (from tens of pptv to a few ppbv).
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.
Petri Tiitta, Ari Leskinen, Liqing Hao, Pasi Yli-Pirilä, Miika Kortelainen, Julija Grigonyte, Jarkko Tissari, Heikki Lamberg, Anni Hartikainen, Kari Kuuspalo, Aki-Matti Kortelainen, Annele Virtanen, Kari E. J. Lehtinen, Mika Komppula, Simone Pieber, André S. H. Prévôt, Timothy B. Onasch, Douglas R. Worsnop, Hendryk Czech, Ralf Zimmermann, Jorma Jokiniemi, and Olli Sippula
Atmos. Chem. Phys., 16, 13251–13269, https://doi.org/10.5194/acp-16-13251-2016, https://doi.org/10.5194/acp-16-13251-2016, 2016
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Real-time measurements of OA aging and SOA formation from logwood combustion were conducted under dark and UV oxidation. Substantial SOA formation was observed in all experiments, leading to twice the initial OA mass emphasizing the importance of the burning conditions for the aging processes. The results prove that emissions are subject to intensive chemical processing in the atmosphere; e.g. the most of the POA was found to become oxidized after the ozone addition, forming aged POA.
Xuan Zhang, Jordan E. Krechmer, Michael Groessl, Wen Xu, Stephan Graf, Michael Cubison, John T. Jayne, Jose L. Jimenez, Douglas R. Worsnop, and Manjula R. Canagaratna
Atmos. Chem. Phys., 16, 12945–12959, https://doi.org/10.5194/acp-16-12945-2016, https://doi.org/10.5194/acp-16-12945-2016, 2016
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We develop a novel two-dimensional space to probe the molecular composition of atmospheric organic aerosols.
Chao Yan, Wei Nie, Mikko Äijälä, Matti P. Rissanen, Manjula R. Canagaratna, Paola Massoli, Heikki Junninen, Tuija Jokinen, Nina Sarnela, Silja A. K. Häme, Siegfried Schobesberger, Francesco Canonaco, Lei Yao, André S. H. Prévôt, Tuukka Petäjä, Markku Kulmala, Mikko Sipilä, Douglas R. Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 16, 12715–12731, https://doi.org/10.5194/acp-16-12715-2016, https://doi.org/10.5194/acp-16-12715-2016, 2016
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Highly oxidized multifunctional compounds (HOMs) are known to have a significant contribution to secondary aerosol formation, yet their dominating formation pathways remain unclear in the atmosphere. We apply positive matrix factorization (PMF) on HOM data, and successfully retrieve factors representing different formation pathways. The results improve our understanding of HOM formation, and provide new perspectives on using PMF to study the variation of short-lived specie.
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.
Yugo Kanaya, Xiaole Pan, Takuma Miyakawa, Yuichi Komazaki, Fumikazu Taketani, Itsushi Uno, and Yutaka Kondo
Atmos. Chem. Phys., 16, 10689–10705, https://doi.org/10.5194/acp-16-10689-2016, https://doi.org/10.5194/acp-16-10689-2016, 2016
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Wet removal of atmospheric black carbon particles was quantitatively characterized in terms of accumulated precipitation along a backward trajectory (APT) using long-term observations at Fukue Island, western Japan, receiving Asian continental outflow with variable degrees of influence from precipitation. The emission inventory of BC over East Asia was assessed in terms of the observed BC/CO ratios. Model simulations should be diagnosed with these improved knowledge on the emission and removal.
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.
Hilkka Timonen, Mike Cubison, Minna Aurela, David Brus, Heikki Lihavainen, Risto Hillamo, Manjula Canagaratna, Bettina Nekat, Rolf Weller, Douglas Worsnop, and Sanna Saarikoski
Atmos. Meas. Tech., 9, 3263–3281, https://doi.org/10.5194/amt-9-3263-2016, https://doi.org/10.5194/amt-9-3263-2016, 2016
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The applicability, methods and limitations of constrained peak fitting on mass spectra of low mass resolving power (m∕Δm50 ∼ 500) recorded with a time-of-flight aerosol chemical speciation monitor (ToF-ACSM) are explored. Calibration measurements and ambient data are used to exemplify the methods that should be applied to maximise data quality and assess confidence in peak-fitting results.
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.
Jordan E. Krechmer, Michael Groessl, Xuan Zhang, Heikki Junninen, Paola Massoli, Andrew T. Lambe, Joel R. Kimmel, Michael J. Cubison, Stephan Graf, Ying-Hsuan Lin, Sri H. Budisulistiorini, Haofei Zhang, Jason D. Surratt, Richard Knochenmuss, John T. Jayne, Douglas R. Worsnop, Jose-Luis Jimenez, and Manjula R. Canagaratna
Atmos. Meas. Tech., 9, 3245–3262, https://doi.org/10.5194/amt-9-3245-2016, https://doi.org/10.5194/amt-9-3245-2016, 2016
Nan Ma, Chunsheng Zhao, Jiangchuan Tao, Zhijun Wu, Simonas Kecorius, Zhibin Wang, Johannes Größ, Hongjian Liu, Yuxuan Bian, Ye Kuang, Monique Teich, Gerald Spindler, Konrad Müller, Dominik van Pinxteren, Hartmut Herrmann, Min Hu, and Alfred Wiedensohler
Atmos. Chem. Phys., 16, 8593–8607, https://doi.org/10.5194/acp-16-8593-2016, https://doi.org/10.5194/acp-16-8593-2016, 2016
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New particle formation (NPF) is one of main sources of cloud condensation nuclei (CCN) in the atmosphere. Based on in situ measurements, we found that CCN activity of newly formed particles largely differs in different NPF events. It is therefore difficult to find a simple parameterization of CCN activity for NPF events. Using a fixed size-resolved activation ratio curve or critical diameter is very likely to result in large biases up to 50 % in the calculated NCCN during NPF events.
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.
Karoliina Ignatius, Thomas B. Kristensen, Emma Järvinen, Leonid Nichman, Claudia Fuchs, Hamish Gordon, Paul Herenz, Christopher R. Hoyle, Jonathan Duplissy, Sarvesh Garimella, Antonio Dias, Carla Frege, Niko Höppel, Jasmin Tröstl, Robert Wagner, Chao Yan, Antonio Amorim, Urs Baltensperger, Joachim Curtius, Neil M. Donahue, Martin W. Gallagher, Jasper Kirkby, Markku Kulmala, Ottmar Möhler, Harald Saathoff, Martin Schnaiter, Antonio Tomé, Annele Virtanen, Douglas Worsnop, and Frank Stratmann
Atmos. Chem. Phys., 16, 6495–6509, https://doi.org/10.5194/acp-16-6495-2016, https://doi.org/10.5194/acp-16-6495-2016, 2016
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Viscous solid or semi-solid secondary organic aerosol (SOA) may influence cloud properties through ice nucleation in the atmosphere. Here, we observed heterogeneous ice nucleation of viscous α-pinene SOA at temperatures between −39 °C and −37.2 °C with ice saturation ratios significantly below the homogeneous freezing limit. Global modelling suggests that viscous biogenic SOA are present in regions where cirrus formation takes place and could contribute to the global ice nuclei budget.
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
Emma Järvinen, Karoliina Ignatius, Leonid Nichman, Thomas B. Kristensen, Claudia Fuchs, Christopher R. Hoyle, Niko Höppel, Joel C. Corbin, Jill Craven, Jonathan Duplissy, Sebastian Ehrhart, Imad El Haddad, Carla Frege, Hamish Gordon, Tuija Jokinen, Peter Kallinger, Jasper Kirkby, Alexei Kiselev, Karl-Heinz Naumann, Tuukka Petäjä, Tamara Pinterich, Andre S. H. Prevot, Harald Saathoff, Thea Schiebel, Kamalika Sengupta, Mario Simon, Jay G. Slowik, Jasmin Tröstl, Annele Virtanen, Paul Vochezer, Steffen Vogt, Andrea C. Wagner, Robert Wagner, Christina Williamson, Paul M. Winkler, Chao Yan, Urs Baltensperger, Neil M. Donahue, Rick C. Flagan, Martin Gallagher, Armin Hansel, Markku Kulmala, Frank Stratmann, Douglas R. Worsnop, Ottmar Möhler, Thomas Leisner, and Martin Schnaiter
Atmos. Chem. Phys., 16, 4423–4438, https://doi.org/10.5194/acp-16-4423-2016, https://doi.org/10.5194/acp-16-4423-2016, 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
M. Dal Maso, L. Liao, J. Wildt, A. Kiendler-Scharr, E. Kleist, R. Tillmann, M. Sipilä, J. Hakala, K. Lehtipalo, M. Ehn, V.-M. Kerminen, M. Kulmala, D. Worsnop, and T. Mentel
Atmos. Chem. Phys., 16, 1955–1970, https://doi.org/10.5194/acp-16-1955-2016, https://doi.org/10.5194/acp-16-1955-2016, 2016
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In this paper, we present the first direct laboratory observations of nanoparticle formation from sulfuric acid and realistic BVOC precursor vapour mixtures performed at atmospherically relevant concentration levels. We found that the formation rate was proportional to the product of sulphuric acid and biogenic VOC emission strength, and that the formation rates were consistent with a mechanism in which nucleating BVOC oxidation products are rapidly formed and activate with sulfuric acid.
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.
C. R. Hoyle, C. Fuchs, E. Järvinen, H. Saathoff, A. Dias, I. El Haddad, M. Gysel, S. C. Coburn, J. Tröstl, A.-K. Bernhammer, F. Bianchi, M. Breitenlechner, J. C. Corbin, J. Craven, N. M. Donahue, J. Duplissy, S. Ehrhart, C. Frege, H. Gordon, N. Höppel, M. Heinritzi, T. B. Kristensen, U. Molteni, L. Nichman, T. Pinterich, A. S. H. Prévôt, M. Simon, J. G. Slowik, G. Steiner, A. Tomé, A. L. Vogel, R. Volkamer, A. C. Wagner, R. Wagner, A. S. Wexler, C. Williamson, P. M. Winkler, C. Yan, A. Amorim, J. Dommen, J. Curtius, M. W. Gallagher, R. C. Flagan, A. Hansel, J. Kirkby, M. Kulmala, O. Möhler, F. Stratmann, D. R. Worsnop, and U. Baltensperger
Atmos. Chem. Phys., 16, 1693–1712, https://doi.org/10.5194/acp-16-1693-2016, https://doi.org/10.5194/acp-16-1693-2016, 2016
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A significant portion of sulphate, an important constituent of atmospheric aerosols, is formed via the aqueous phase oxidation of sulphur dioxide by ozone. The rate of this reaction has previously only been measured over a relatively small temperature range. Here, we use the state of the art CLOUD chamber at CERN to perform the first measurements of this reaction rate in super-cooled droplets, confirming that the existing extrapolation of the reaction rate to sub-zero temperatures is accurate.
L. Xu, L. R. Williams, D. E. Young, J. D. Allan, H. Coe, P. Massoli, E. Fortner, P. Chhabra, S. Herndon, W. A. Brooks, J. T. Jayne, D. R. Worsnop, A. C. Aiken, S. Liu, K. Gorkowski, M. K. Dubey, Z. L. Fleming, S. Visser, A. S. H. Prévôt, and N. L. Ng
Atmos. Chem. Phys., 16, 1139–1160, https://doi.org/10.5194/acp-16-1139-2016, https://doi.org/10.5194/acp-16-1139-2016, 2016
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We investigate the spatial distribution of submicron aerosol in the greater London area as part of the Clean Air for London (ClearfLo) project in winter 2012. Although the concentrations of organic aerosol (OA) are similar between a rural and an urban site, the OA sources are different. We also examine the volatility of submicron aerosol at the rural site and find that the non-volatile organics have similar sources or have undergone similar chemical processing as refractory black carbon.
A. W. H. Chan, N. M. Kreisberg, T. Hohaus, P. Campuzano-Jost, Y. Zhao, D. A. Day, L. Kaser, T. Karl, A. Hansel, A. P. Teng, C. R. Ruehl, D. T. Sueper, J. T. Jayne, D. R. Worsnop, J. L. Jimenez, S. V. Hering, and A. H. Goldstein
Atmos. Chem. Phys., 16, 1187–1205, https://doi.org/10.5194/acp-16-1187-2016, https://doi.org/10.5194/acp-16-1187-2016, 2016
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Using a novel instrument, we have made measurements of organic compounds that can exist as a gas or particle in the rural atmosphere. Through hourly measurements, we have identified the sources and atmospheric processes of these compounds, which are important for modeling the climate and health impact of these emissions.
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.
D. M. Lienhard, A. J. Huisman, U. K. Krieger, Y. Rudich, C. Marcolli, B. P. Luo, D. L. Bones, J. P. Reid, A. T. Lambe, M. R. Canagaratna, P. Davidovits, T. B. Onasch, D. R. Worsnop, S. S. Steimer, T. Koop, and T. Peter
Atmos. Chem. Phys., 15, 13599–13613, https://doi.org/10.5194/acp-15-13599-2015, https://doi.org/10.5194/acp-15-13599-2015, 2015
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New data of water diffusivity in secondary organic aerosol (SOA) material and organic/inorganic model mixtures is presented over an extensive temperature range. Our data suggest that water diffusion in SOA is sufficiently fast so that it is unlikely to have significant consequences on the direct climatic effect under tropospheric conditions. Glass formation in SOA is unlikely to restrict homogeneous ice nucleation.
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.
S. Carbone, T. Onasch, S. Saarikoski, H. Timonen, K. Saarnio, D. Sueper, T. Rönkkö, L. Pirjola, A. Häyrinen, D. Worsnop, and R. Hillamo
Atmos. Meas. Tech., 8, 4803–4815, https://doi.org/10.5194/amt-8-4803-2015, https://doi.org/10.5194/amt-8-4803-2015, 2015
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The purpose of this study was to develop a method for the quantification of trace metal content in black carbon aerosol in real time, such as combustion-related emissions, by using the SP-AMS. The properties of 13 different trace metals (Na, Al, Ca, V, Cr, Fe, Mn, Ni, Cu, Zn, Rb, Sr and Ba) were investigated in a controlled laboratory experiment. The results from the laboratory tests were applied to study fine particles in emissions of a heavy-fuel-oil-fired heating station.
J. C. Corbin, A. Othman, J. D. Allan, D. R. Worsnop, J. D. Haskins, B. Sierau, U. Lohmann, and A. A. Mensah
Atmos. Meas. Tech., 8, 4615–4636, https://doi.org/10.5194/amt-8-4615-2015, https://doi.org/10.5194/amt-8-4615-2015, 2015
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Peak-integration uncertainties in the Aerodyne high-resolution aerosol mass spectrometer (AMS) are analyzed in detail using a combination of empirical data analysis and Monte Carlo approaches. The most general conclusion, applicable to any mass spectrometer, is that non-zero mass accuracy leads to a percentage error in constrained peak fits, even for well-resolved peaks. For overlapping peaks, this mass-accuracy effect may be viewed as a reduction in the effective m/z-calibration precision.
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.
R. Fröhlich, M. J. Cubison, J. G. Slowik, N. Bukowiecki, F. Canonaco, P. L. Croteau, M. Gysel, S. Henne, E. Herrmann, J. T. Jayne, M. Steinbacher, D. R. Worsnop, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 15, 11373–11398, https://doi.org/10.5194/acp-15-11373-2015, https://doi.org/10.5194/acp-15-11373-2015, 2015
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This manuscript presents the first long-term (14-month) and highly time-resolved (10 min) measurements of NR-PM1 aerosol chemical composition at a high-altitude site (JFJ, Switzerland, 3580m a.s.l.). The elevated location allowed the investigation of free tropospheric aerosol year round. Total and relative mass loadings, diurnal variations as well as seasonal variations are discussed together with geographical origin, organic aerosol sources and the influence of the planetary boundary layer.
M. Sipilä, N. Sarnela, T. Jokinen, H. Junninen, J. Hakala, M. P. Rissanen, A. Praplan, M. Simon, A. Kürten, F. Bianchi, J. Dommen, J. Curtius, T. Petäjä, and D. R. Worsnop
Atmos. Meas. Tech., 8, 4001–4011, https://doi.org/10.5194/amt-8-4001-2015, https://doi.org/10.5194/amt-8-4001-2015, 2015
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Atmospheric concentrations of amines are poorly known mainly due to challenges related to their reliable high-sensitivity detection. We have created a method and instrument that is capable for detecting amines with lowest limit of detection of around 0.01 parts per trillion. Application of the instrument in the field study indicates that concentrations of dimethyl amine in a boreal forest site are below 0.03ppt, not enough to account for the observed new particle formation rates.
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.
A. Kürten, S. Münch, L. Rondo, F. Bianchi, J. Duplissy, T. Jokinen, H. Junninen, N. Sarnela, S. Schobesberger, M. Simon, M. Sipilä, J. Almeida, A. Amorim, J. Dommen, N. M. Donahue, E. M. Dunne, R. C. Flagan, A. Franchin, J. Kirkby, A. Kupc, V. Makhmutov, T. Petäjä, A. P. Praplan, F. Riccobono, G. Steiner, A. Tomé, G. Tsagkogeorgas, P. E. Wagner, D. Wimmer, U. Baltensperger, M. Kulmala, D. R. Worsnop, and J. Curtius
Atmos. Chem. Phys., 15, 10701–10721, https://doi.org/10.5194/acp-15-10701-2015, https://doi.org/10.5194/acp-15-10701-2015, 2015
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New particle formation (NPF) is an important atmospheric process. At cold temperatures in the upper troposphere the binary (H2SO4-H2O) and ternary (H2SO4-H2O-NH3) system are thought to be important for NPF. Sulfuric acid monomer (H2SO4) and sulfuric acid dimer ((H2SO4)2) concentrations were measured between 208 and 248K for these systems and dimer evaporation rates were derived. These data will help to better understand and predict binary and ternary nucleation at low temperatures.
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. 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
F. D. Lopez-Hilfiker, C. Mohr, M. Ehn, F. Rubach, E. Kleist, J. Wildt, Th. F. Mentel, A. J. Carrasquillo, K. E. Daumit, J. F. Hunter, J. H. Kroll, D. R. Worsnop, and J. A. Thornton
Atmos. Chem. Phys., 15, 7765–7776, https://doi.org/10.5194/acp-15-7765-2015, https://doi.org/10.5194/acp-15-7765-2015, 2015
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We measured a large suite organic compounds using a recently developed Filter Inlet for Gases and AEROsols (FIGAERO) coupled to a (HR-ToF-CIMS). The instrument was deployed on environmental simulation chambers to study monoterpene oxidation as a secondary organic aerosol (SOA) source. We find that approximately 50% of the detected particle phase mass is associated with compounds having effective vapor pressures 4, or more, orders of magnitude lower than commonly measured products.
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.
Y. Kuang, C. S. Zhao, J. C. Tao, and N. Ma
Atmos. Chem. Phys., 15, 5761–5772, https://doi.org/10.5194/acp-15-5761-2015, https://doi.org/10.5194/acp-15-5761-2015, 2015
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In this paper, it is found that the diurnal variations of single scattering albedo (SSA) and asymmetry factor (g) for ambient aerosol are both evident and far different from those of dry state aerosol in the North China Plain (NCP. The diurnal changes of SSA and g have significant impacts on the estimation of daily average direct aerosol radiative effect (DARE) at the top of the atmosphere. In addition, several suggestions are proposed to improve the accurate prediction of DARE in the NCP.
A. P. Praplan, S. Schobesberger, F. Bianchi, M. P. Rissanen, M. Ehn, T. Jokinen, H. Junninen, A. Adamov, A. Amorim, J. Dommen, J. Duplissy, J. Hakala, A. Hansel, M. Heinritzi, J. Kangasluoma, J. Kirkby, M. Krapf, A. Kürten, K. Lehtipalo, F. Riccobono, L. Rondo, N. Sarnela, M. Simon, A. Tomé, J. Tröstl, P. M. Winkler, C. Williamson, P. Ye, J. Curtius, U. Baltensperger, N. M. Donahue, M. Kulmala, and D. R. Worsnop
Atmos. Chem. Phys., 15, 4145–4159, https://doi.org/10.5194/acp-15-4145-2015, https://doi.org/10.5194/acp-15-4145-2015, 2015
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Our study shows, based on data from three atmospheric pressure interface time-of-flight mass spectrometers measuring in parallel charged and neutral molecules and molecular clusters, how oxidised organic compounds bind to inorganic ions (e.g. bisulfate, nitrate, ammonium). This ionisation is selective for compounds with lower molar mass due to their limited amount and variety of functional groups. We also found that extremely low volatile organic compounds (ELVOCs) can be formed immediately.
A. T. Lambe, P. S. Chhabra, T. B. Onasch, W. H. Brune, J. F. Hunter, J. H. Kroll, M. J. Cummings, J. F. Brogan, Y. Parmar, D. R. Worsnop, C. E. Kolb, and P. Davidovits
Atmos. Chem. Phys., 15, 3063–3075, https://doi.org/10.5194/acp-15-3063-2015, https://doi.org/10.5194/acp-15-3063-2015, 2015
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We compared the chemistry and yields of SOA generated from OH oxidation of gas-phase precursors in a flow reactor (high OH, short residence time) and environmental chambers (low OH, long residence time). We find that chemical composition of SOA produced in the flow reactor and in chambers is similar. SOA yields measured in the flow reactor are lower than in chambers. Seed particles increase the yield of SOA produced in the flow reactor and may account in part for higher SOA yields in chambers.
S. Xiao, M. Y. Wang, L. Yao, M. Kulmala, B. Zhou, X. Yang, J. M. Chen, D. F. Wang, Q. Y. Fu, D. R. Worsnop, and L. Wang
Atmos. Chem. Phys., 15, 1769–1781, https://doi.org/10.5194/acp-15-1769-2015, https://doi.org/10.5194/acp-15-1769-2015, 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.
I. Nuaaman, S.-M. Li, K. L. Hayden, T. B. Onasch, P. Massoli, D. Sueper, D. R. Worsnop, T. S. Bates, P. K. Quinn, and R. McLaren
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-2085-2015, https://doi.org/10.5194/acpd-15-2085-2015, 2015
Revised manuscript has not been submitted
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In this paper, we focus on the measurement and reporting of mass concentrations of particulate chloride and sea salt in a marine area off the coast of California using a High Resolution Aerosol Mass Spectrometer. We outline a method of deconvolving the total aerosol chloride mass into refractory and non-refractory components, previously not reported in the literature. This can be important in regions where refractory sea salt aerosols can contribute to the aerosol chloride signal measured with t
M. R. Canagaratna, J. L. Jimenez, J. H. Kroll, Q. Chen, S. H. Kessler, P. Massoli, L. Hildebrandt Ruiz, E. Fortner, L. R. Williams, K. R. Wilson, J. D. Surratt, N. M. Donahue, J. T. Jayne, and D. R. Worsnop
Atmos. Chem. Phys., 15, 253–272, https://doi.org/10.5194/acp-15-253-2015, https://doi.org/10.5194/acp-15-253-2015, 2015
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Atomic oxygen-to-carbon (O:C), hydrogen-to-carbon (H:C), and organic mass-to-organic carbon (OM:OC) ratios of ambient organic aerosol (OA) species provide key constraints for understanding their sources and impacts. Here an improved method for obtaining accurate O:C, H:C, and OM:OC with a widely used aerosol mass spectrometer is developed. These results imply that OA is more oxidized than previously estimated and indicate the need for new chemical mechanisms that simulate ambient oxidation.
S. Schobesberger, A. Franchin, F. Bianchi, L. Rondo, J. Duplissy, A. Kürten, I. K. Ortega, A. Metzger, R. Schnitzhofer, J. Almeida, A. Amorim, J. Dommen, E. M. Dunne, M. Ehn, S. Gagné, L. Ickes, H. Junninen, A. Hansel, V.-M. Kerminen, J. Kirkby, A. Kupc, A. Laaksonen, K. Lehtipalo, S. Mathot, A. Onnela, T. Petäjä, F. Riccobono, F. D. Santos, M. Sipilä, A. Tomé, G. Tsagkogeorgas, Y. Viisanen, P. E. Wagner, D. Wimmer, J. Curtius, N. M. Donahue, U. Baltensperger, M. Kulmala, and D. R. Worsnop
Atmos. Chem. Phys., 15, 55–78, https://doi.org/10.5194/acp-15-55-2015, https://doi.org/10.5194/acp-15-55-2015, 2015
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We used an ion mass spectrometer at CERN's CLOUD chamber to investigate the detailed composition of ammonia--sulfuric acid ion clusters (of both polarities) as they initially form and then grow into aerosol particles, at atmospherically relevant conditions. We found that these clusters’ composition is mainly determined by the ratio of the precursor vapors and ranges from ammonia-free clusters to clusters containing > 1 ammonia per sulfuric acid. Acid--base bindings are a key formation mechanism.
P. S. Chhabra, A. T. Lambe, M. R. Canagaratna, H. Stark, J. T. Jayne, T. B. Onasch, P. Davidovits, J. R. Kimmel, and D. R. Worsnop
Atmos. Meas. Tech., 8, 1–18, https://doi.org/10.5194/amt-8-1-2015, https://doi.org/10.5194/amt-8-1-2015, 2015
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Authors of this publication used acetate chemical ionization mass spectrometry (acetate-CIMS) to measure experimental products of alpha-pinene and naphthalene oxidation formed in a flow reactor. Acetate-CIMS instrumentation is selective toward carboxylic acid compounds which are readily formed in atmospheric photooxidation processes. Spectral information was used to identify previously measured products of both systems and to estimate their volatilities.
J.-E. Petit, O. Favez, J. Sciare, F. Canonaco, P. Croteau, G. Močnik, J. Jayne, D. Worsnop, and E. Leoz-Garziandia
Atmos. Chem. Phys., 14, 13773–13787, https://doi.org/10.5194/acp-14-13773-2014, https://doi.org/10.5194/acp-14-13773-2014, 2014
L. Q. Hao, A. Kortelainen, S. Romakkaniemi, H. Portin, A. Jaatinen, A. Leskinen, M. Komppula, P. Miettinen, D. Sueper, A. Pajunoja, J. N. Smith, K. E. J. Lehtinen, D. R. Worsnop, A. Laaksonen, and A. Virtanen
Atmos. Chem. Phys., 14, 13483–13495, https://doi.org/10.5194/acp-14-13483-2014, https://doi.org/10.5194/acp-14-13483-2014, 2014
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Positive matrix factorization (PMF) was applied to the unified high-resolution mass spectra organic species with NO+ and NO2+ ions from the measurement in a mixed region between the boreal forestland and the urban area. The PMF analysis succeeded in separating the mixed spectra into three distinct organic factors and one inorganic factor. The particulate organic nitrate was distinguished by PMF for the first time, with a contribution of one-third of the total nitrate mass.
M. D. Willis, A. K. Y. Lee, T. B. Onasch, E. C. Fortner, L. R. Williams, A. T. Lambe, D. R. Worsnop, and J. P. D. Abbatt
Atmos. Meas. Tech., 7, 4507–4516, https://doi.org/10.5194/amt-7-4507-2014, https://doi.org/10.5194/amt-7-4507-2014, 2014
M. Sipilä, T. Jokinen, T. Berndt, S. Richters, R. Makkonen, N. M. Donahue, R. L. Mauldin III, T. Kurtén, P. Paasonen, N. Sarnela, M. Ehn, H. Junninen, M. P. Rissanen, J. Thornton, F. Stratmann, H. Herrmann, D. R. Worsnop, M. Kulmala, V.-M. Kerminen, and T. Petäjä
Atmos. Chem. Phys., 14, 12143–12153, https://doi.org/10.5194/acp-14-12143-2014, https://doi.org/10.5194/acp-14-12143-2014, 2014
L. Rondo, A. Kürten, S. Ehrhart, S. Schobesberger, A. Franchin, H. Junninen, T. Petäjä, M. Sipilä, D. R. Worsnop, and J. Curtius
Atmos. Meas. Tech., 7, 3849–3859, https://doi.org/10.5194/amt-7-3849-2014, https://doi.org/10.5194/amt-7-3849-2014, 2014
S. Decesari, J. Allan, C. Plass-Duelmer, B. J. Williams, M. Paglione, M. C. Facchini, C. O'Dowd, R. M. Harrison, J. K. Gietl, H. Coe, L. Giulianelli, G. P. Gobbi, C. Lanconelli, C. Carbone, D. Worsnop, A. T. Lambe, A. T. Ahern, F. Moretti, E. Tagliavini, T. Elste, S. Gilge, Y. Zhang, and M. Dall'Osto
Atmos. Chem. Phys., 14, 12109–12132, https://doi.org/10.5194/acp-14-12109-2014, https://doi.org/10.5194/acp-14-12109-2014, 2014
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We made use of multiple spectrometric techniques for characterizing the aerosol chemical composition and mixing in the Po Valley in the summer.
The oxygenated organic aerosol (OOA) concentrations were correlated with simple tracers for recirculated planetary boundary layer air.
A full internal mixing between black carbon (BC) and the non-refractory aerosol components was never observed. Local sources in the Po Valley were responsible for the production of organic particles unmixed with BC.
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
T. R. Dallmann, T. B. Onasch, T. W. Kirchstetter, D. R. Worton, E. C. Fortner, S. C. Herndon, E. C. Wood, J. P. Franklin, D. R. Worsnop, A. H. Goldstein, and R. A. Harley
Atmos. Chem. Phys., 14, 7585–7599, https://doi.org/10.5194/acp-14-7585-2014, https://doi.org/10.5194/acp-14-7585-2014, 2014
S. Saarikoski, S. Carbone, M. J. Cubison, R. Hillamo, P. Keronen, C. Sioutas, D. R. Worsnop, and J. L. Jimenez
Atmos. Meas. Tech., 7, 2121–2135, https://doi.org/10.5194/amt-7-2121-2014, https://doi.org/10.5194/amt-7-2121-2014, 2014
S. H. Budisulistiorini, M. R. Canagaratna, P. L. Croteau, K. Baumann, E. S. Edgerton, M. S. Kollman, N. L. Ng, V. Verma, S. L. Shaw, E. M. Knipping, D. R. Worsnop, J. T. Jayne, R.J. Weber, and J. D. Surratt
Atmos. Meas. Tech., 7, 1929–1941, https://doi.org/10.5194/amt-7-1929-2014, https://doi.org/10.5194/amt-7-1929-2014, 2014
A. Setyan, C. Song, M. Merkel, W. B. Knighton, T. B. Onasch, M. R. Canagaratna, D. R. Worsnop, A. Wiedensohler, J. E. Shilling, and Q. Zhang
Atmos. Chem. Phys., 14, 6477–6494, https://doi.org/10.5194/acp-14-6477-2014, https://doi.org/10.5194/acp-14-6477-2014, 2014
M. Crippa, F. Canonaco, V. A. Lanz, M. Äijälä, J. D. Allan, S. Carbone, G. Capes, D. Ceburnis, M. Dall'Osto, D. A. Day, P. F. DeCarlo, M. Ehn, A. Eriksson, E. Freney, L. Hildebrandt Ruiz, R. Hillamo, J. L. Jimenez, H. Junninen, A. Kiendler-Scharr, A.-M. Kortelainen, M. Kulmala, A. Laaksonen, A. A. Mensah, C. Mohr, E. Nemitz, C. O'Dowd, J. Ovadnevaite, S. N. Pandis, T. Petäjä, L. Poulain, S. Saarikoski, K. Sellegri, E. Swietlicki, P. Tiitta, D. R. Worsnop, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 14, 6159–6176, https://doi.org/10.5194/acp-14-6159-2014, https://doi.org/10.5194/acp-14-6159-2014, 2014
M. Paglione, S. Saarikoski, S. Carbone, R. Hillamo, M. C. Facchini, E. Finessi, L. Giulianelli, C. Carbone, S. Fuzzi, F. Moretti, E. Tagliavini, E. Swietlicki, K. Eriksson Stenström, A. S. H. Prévôt, P. Massoli, M. Canaragatna, D. Worsnop, and S. Decesari
Atmos. Chem. Phys., 14, 5089–5110, https://doi.org/10.5194/acp-14-5089-2014, https://doi.org/10.5194/acp-14-5089-2014, 2014
F. D. Lopez-Hilfiker, C. Mohr, M. Ehn, F. Rubach, E. Kleist, J. Wildt, Th. F. Mentel, A. Lutz, M. Hallquist, D. Worsnop, and J. A. Thornton
Atmos. Meas. Tech., 7, 983–1001, https://doi.org/10.5194/amt-7-983-2014, https://doi.org/10.5194/amt-7-983-2014, 2014
L. Liu, F. Hu, and X.-L. Cheng
Nonlin. Processes Geophys., 21, 463–475, https://doi.org/10.5194/npg-21-463-2014, https://doi.org/10.5194/npg-21-463-2014, 2014
J. Kangasluoma, C. Kuang, D. Wimmer, M. P. Rissanen, K. Lehtipalo, M. Ehn, D. R. Worsnop, J. Wang, M. Kulmala, and T. Petäjä
Atmos. Meas. Tech., 7, 689–700, https://doi.org/10.5194/amt-7-689-2014, https://doi.org/10.5194/amt-7-689-2014, 2014
P. Tiitta, V. Vakkari, P. Croteau, J. P. Beukes, P. G. van Zyl, M. Josipovic, A. D. Venter, K. Jaars, J. J. Pienaar, N. L. Ng, M. R. Canagaratna, J. T. Jayne, V.-M. Kerminen, H. Kokkola, M. Kulmala, A. Laaksonen, D. R. Worsnop, and L. Laakso
Atmos. Chem. Phys., 14, 1909–1927, https://doi.org/10.5194/acp-14-1909-2014, https://doi.org/10.5194/acp-14-1909-2014, 2014
H. Kokkola, P. Yli-Pirilä, M. Vesterinen, H. Korhonen, H. Keskinen, S. Romakkaniemi, L. Hao, A. Kortelainen, J. Joutsensaari, D. R. Worsnop, A. Virtanen, and K. E. J. Lehtinen
Atmos. Chem. Phys., 14, 1689–1700, https://doi.org/10.5194/acp-14-1689-2014, https://doi.org/10.5194/acp-14-1689-2014, 2014
R. L. N. Yatavelli, H. Stark, S. L. Thompson, J. R. Kimmel, M. J. Cubison, D. A. Day, P. Campuzano-Jost, B. B. Palm, A. Hodzic, J. A. Thornton, J. T. Jayne, D. R. Worsnop, and J. L. Jimenez
Atmos. Chem. Phys., 14, 1527–1546, https://doi.org/10.5194/acp-14-1527-2014, https://doi.org/10.5194/acp-14-1527-2014, 2014
A. L. Corrigan, L. M. Russell, S. Takahama, M. Äijälä, M. Ehn, H. Junninen, J. Rinne, T. Petäjä, M. Kulmala, A. L. Vogel, T. Hoffmann, C. J. Ebben, F. M. Geiger, P. Chhabra, J. H. Seinfeld, D. R. Worsnop, W. Song, J. Auld, and J. Williams
Atmos. Chem. Phys., 13, 12233–12256, https://doi.org/10.5194/acp-13-12233-2013, https://doi.org/10.5194/acp-13-12233-2013, 2013
L. R. Williams, L. A. Gonzalez, J. Peck, D. Trimborn, J. McInnis, M. R. Farrar, K. D. Moore, J. T. Jayne, W. A. Robinson, D. K. Lewis, T. B. Onasch, M. R. Canagaratna, A. Trimborn, M. T. Timko, G. Magoon, R. Deng, D. Tang, E. de la Rosa Blanco, A. S. H. Prévôt, K. A. Smith, and D. R. Worsnop
Atmos. Meas. Tech., 6, 3271–3280, https://doi.org/10.5194/amt-6-3271-2013, https://doi.org/10.5194/amt-6-3271-2013, 2013
R. Fröhlich, M. J. Cubison, J. G. Slowik, N. Bukowiecki, A. S. H. Prévôt, U. Baltensperger, J. Schneider, J. R. Kimmel, M. Gonin, U. Rohner, D. R. Worsnop, and J. T. Jayne
Atmos. Meas. Tech., 6, 3225–3241, https://doi.org/10.5194/amt-6-3225-2013, https://doi.org/10.5194/amt-6-3225-2013, 2013
M. R. Pennington, B. R. Bzdek, J. W. DePalma, J. N. Smith, A.-M. Kortelainen, L. Hildebrandt Ruiz, T. Petäjä, M. Kulmala, D. R. Worsnop, and M. V. Johnston
Atmos. Chem. Phys., 13, 10215–10225, https://doi.org/10.5194/acp-13-10215-2013, https://doi.org/10.5194/acp-13-10215-2013, 2013
M. Dall'Osto, X. Querol, A. Alastuey, M. C. Minguillon, M. Alier, F. Amato, M. Brines, M. Cusack, J. O. Grimalt, A. Karanasiou, T. Moreno, M. Pandolfi, J. Pey, C. Reche, A. Ripoll, R. Tauler, B. L. Van Drooge, M. Viana, R. M. Harrison, J. Gietl, D. Beddows, W. Bloss, C. O'Dowd, D. Ceburnis, G. Martucci, N. L. Ng, D. Worsnop, J. Wenger, E. Mc Gillicuddy, J. Sodeau, R. Healy, F. Lucarelli, S. Nava, J. L. Jimenez, F. Gomez Moreno, B. Artinano, A. S. H. Prévôt, L. Pfaffenberger, S. Frey, F. Wilsenack, D. Casabona, P. Jiménez-Guerrero, D. Gross, and N. Cots
Atmos. Chem. Phys., 13, 8991–9019, https://doi.org/10.5194/acp-13-8991-2013, https://doi.org/10.5194/acp-13-8991-2013, 2013
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
H. Keskinen, A. Virtanen, J. Joutsensaari, G. Tsagkogeorgas, J. Duplissy, S. Schobesberger, M. Gysel, F. Riccobono, J. G. Slowik, F. Bianchi, T. Yli-Juuti, K. Lehtipalo, L. Rondo, M. Breitenlechner, A. Kupc, J. Almeida, A. Amorim, E. M. Dunne, A. J. Downard, S. Ehrhart, A. Franchin, M.K. Kajos, J. Kirkby, A. Kürten, T. Nieminen, V. Makhmutov, S. Mathot, P. Miettinen, A. Onnela, T. Petäjä, A. Praplan, F. D. Santos, S. Schallhart, M. Sipilä, Y. Stozhkov, A. Tomé, P. Vaattovaara, D. Wimmer, A. Prevot, J. Dommen, N. M. Donahue, R.C. Flagan, E. Weingartner, Y. Viisanen, I. Riipinen, A. Hansel, J. Curtius, M. Kulmala, D. R. Worsnop, U. Baltensperger, H. Wex, F. Stratmann, and A. Laaksonen
Atmos. Chem. Phys., 13, 5587–5600, https://doi.org/10.5194/acp-13-5587-2013, https://doi.org/10.5194/acp-13-5587-2013, 2013
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
S. Lance, T. Raatikainen, T. B. Onasch, D. R. Worsnop, X.-Y. Yu, M. L. Alexander, M. R. Stolzenburg, P. H. McMurry, J. N. Smith, and A. Nenes
Atmos. Chem. Phys., 13, 5049–5062, https://doi.org/10.5194/acp-13-5049-2013, https://doi.org/10.5194/acp-13-5049-2013, 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
J. E. Shilling, R. A. Zaveri, J. D. Fast, L. Kleinman, M. L. Alexander, M. R. Canagaratna, E. Fortner, J. M. Hubbe, J. T. Jayne, A. Sedlacek, A. Setyan, S. Springston, D. R. Worsnop, and Q. Zhang
Atmos. Chem. Phys., 13, 2091–2113, https://doi.org/10.5194/acp-13-2091-2013, https://doi.org/10.5194/acp-13-2091-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
The annual cycle and sources of relevant aerosol precursor vapors in the central Arctic during the MOSAiC expedition
Opinion: How will advances in aerosol science inform our understanding of the health impacts of outdoor particulate pollution?
Measurement report: Intra-annual variability of black carbon and brown carbon and their interrelation with meteorological conditions over Gangtok, Sikkim
Long-range transport of air pollutants increases the concentration of hazardous components of PM2.5 in northern South America
Dominant influence of biomass combustion and cross-border transport on nitrogen-containing organic compound levels in the southeastern Tibetan Plateau
Impacts of elevated anthropogenic emissions on physicochemical characteristics of black-carbon-containing particles over the Tibetan Plateau
Online characterization of primary and secondary emissions of particulate matter and acidic molecules from a modern fleet of city buses
Atmospheric evolution of environmentally persistent free radicals in the rural North China Plain: effects on water solubility and PM2.5 oxidative potential
Two distinct ship emission profiles for organic-sulfate source apportionment of PM in sulfur emission control areas
Automated compound speciation, cluster analysis, and quantification of organic vapors and aerosols using comprehensive two-dimensional gas chromatography and mass spectrometry
Measurement report: Occurrence of aminiums in PM2.5 during winter in China – aminium outbreak during polluted episodes and potential constraints
Bridging gas and aerosol properties between the northeastern US and Bermuda: analysis of eight transit flights
The behaviour of charged particles (ions) during new particle formation events in urban Leipzig, Germany
Exploring the sources of light-absorbing carbonaceous aerosols by integrating observational and modeling results: insights from Northeast China
Measurement report: Characteristics of airborne black-carbon-containing particles during the 2021 summer COVID-19 lockdown in a typical Yangtze River Delta city, China
Aerosol optical properties within the atmospheric boundary layer predicted from ground-based observations compared to Raman lidar retrievals during RITA-2021
Hygroscopic growth and activation changed submicron aerosol composition and properties in the North China Plain
Measurement report: Formation of tropospheric brown carbon in a lifting air mass
Vertical variability of aerosol properties and trace gases over a remote marine region: a case study over Bermuda
Differences in aerosol and cloud properties along the central California coast when winds change from northerly to southerly
International airport emissions and their impact on local air quality: chemical speciation of ambient aerosols at Madrid–Barajas Airport during the AVIATOR campaign
Significant role of biomass burning in heavy haze formation in a megacity: Molecular-level insights from intensive PM2.5 sampling on winter hazy days
The local ship speed reduction effect on black carbon emissions measured at a remote marine station
High-altitude aerosol chemical characterization and source identification: insights from the CALISHTO campaign
Measurement report: Impact of emission control measures on environmental persistent free radicals and reactive oxygen species – a short-term case study in Beijing
Characterizing water solubility of fresh and aged secondary organic aerosol in PM2.5 with the stable carbon isotope technique
Critical contribution of chemically diverse carbonyl molecules to the oxidative potential of atmospheric aerosols
Seasonal Investigation of Ultrafine Particle Composition in an Eastern Amazonian Rainforest
Measurement report: Vanadium-containing ship exhaust particles detected in and above the marine boundary layer in the remote atmosphere
Diverging trends in aerosol sulfate and nitrate measured in the remote North Atlantic in Barbados are attributed to clean air policies, African smoke, and anthropogenic emissions
Technical note: Quantified organic aerosol subsaturated hygroscopicity by a simple optical scatter monitor system through field measurements
Diverse sources and aging change the mixing state and ice nucleation properties of aerosol particles over the western Pacific and Southern Ocean
The water-insoluble organic carbon in PM2.5 of typical Chinese urban areas: light-absorbing properties, potential sources, radiative forcing effects, and a possible light-absorbing continuum
Measurement report: Size-resolved secondary organic aerosol formation modulated by aerosol water uptake in wintertime haze
In situ measurement of organic aerosol molecular markers in urban Hong Kong during a summer period: temporal variations and source apportionment
Technical note: Determining chemical composition of atmospheric single particles by a standard-free mass calibration algorithm
Different formation pathways of nitrogen-containing organic compounds in aerosols and fog water in northern China
Impact of weather patterns and meteorological factors on PM2.5 and O3 responses to the COVID-19 lockdown in China
Daytime and nighttime aerosol soluble iron formation in clean and slightly polluted moist air in a coastal city in eastern China
Non-negligible secondary contribution to brown carbon in autumn and winter: inspiration from particulate nitrated and oxygenated aromatic compounds in urban Beijing
A Multi-site Passive Approach for Studying the Emissions and Evolution of Smoke from Prescribed Fires
Non-sea-salt aerosols that contain trace bromine and iodine are widespread in the remote troposphere
Simultaneous organic aerosol source apportionment at two Antarctic sites reveals large-scale and ecoregion-specific components
Measurement report: Optical characterization, seasonality, and sources of brown carbon in fine aerosols from Tianjin, North China: year-round observations
High-resolution analyses of concentrations and sizes of black carbon particles deposited on northwest Greenland over the past 350 years – Part 2: Seasonal and temporal trends in black carbon originated from fossil fuel combustion and biomass burning
Bayesian inference-based estimation of hourly primary and secondary organic carbon in suburban Hong Kong: multi-temporal-scale variations and evolution characteristics during PM2.5 episodes
Formation and chemical evolution of SOA in two different environments: A dual chamber study
Enhanced daytime secondary aerosol formation driven by gas-particle partitioning in downwind urban plumes
Multiple eco-regions contribute to the seasonal cycle of Antarctic aerosol size distributions
Impact assessment of terrestrial and marine air-mass on the constituents and intermixing of bioaerosols over coastal atmosphere
Matthew Boyer, Diego Aliaga, Lauriane L. J. Quéléver, Silvia Bucci, Hélène Angot, Lubna Dada, Benjamin Heutte, Lisa Beck, Marina Duetsch, Andreas Stohl, Ivo Beck, Tiia Laurila, Nina Sarnela, Roseline C. Thakur, Branka Miljevic, Markku Kulmala, Tuukka Petäjä, Mikko Sipilä, Julia Schmale, and Tuija Jokinen
Atmos. Chem. Phys., 24, 12595–12621, https://doi.org/10.5194/acp-24-12595-2024, https://doi.org/10.5194/acp-24-12595-2024, 2024
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We analyze the seasonal cycle and sources of gases that are relevant for the formation of aerosol particles in the central Arctic. Since theses gases can form new particles, they can influence Arctic climate. We show that the sources of these gases are associated with changes in the Arctic environment during the year, especially with respect to sea ice. Therefore, the concentration of these gases will likely change in the future as the Arctic continues to warm.
Imad El Haddad, Danielle Vienneau, Kaspar R. Daellenbach, Robin Modini, Jay G. Slowik, Abhishek Upadhyay, Petros N. Vasilakos, David Bell, Kees de Hoogh, and Andre S. H. Prevot
Atmos. Chem. Phys., 24, 11981–12011, https://doi.org/10.5194/acp-24-11981-2024, https://doi.org/10.5194/acp-24-11981-2024, 2024
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This opinion paper explores how advances in aerosol science inform our understanding of the health impacts of outdoor particulate pollution. We advocate for a shift in the way we target PM pollution, focusing on the most harmful anthropogenic emissions. We highlight key observations, modelling developments, and emission measurements needed to achieve this shift.
Pramod Kumar, Khushboo Sharma, Ankita Malu, Rajeev Rajak, Aparna Gupta, Bidyutjyoti Baruah, Shailesh Yadav, Thupstan Angchuk, Jayant Sharma, Rakesh Kumar Ranjan, Anil Kumar Misra, and Nishchal Wanjari
Atmos. Chem. Phys., 24, 11585–11601, https://doi.org/10.5194/acp-24-11585-2024, https://doi.org/10.5194/acp-24-11585-2024, 2024
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This work monitors and assesses air pollution, especially black and brown carbon, its controlling factor, and its effect on the environment of Sikkim Himalayan region. The huge urban sprawl in recent decades has led to regional human-induced air pollution in the region. Black carbon was highest in April 2021 and March 2022, exceeding the WHO limit. The monsoon season causes huge rainfall over the region, which reduces the pollutants by scavenging (rainout and washout).
Maria P. Velásquez-García, K. Santiago Hernández, James A. Vergara-Correa, Richard J. Pope, Miriam Gómez-Marín, and Angela M. Rendón
Atmos. Chem. Phys., 24, 11497–11520, https://doi.org/10.5194/acp-24-11497-2024, https://doi.org/10.5194/acp-24-11497-2024, 2024
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In the Aburrá Valley, northern South America, local emissions determine air quality conditions. However, we found that external sources, such as regional fires, Saharan dust, and volcanic emissions, increase particulate concentrations and worsen chemical composition by introducing elements like heavy metals. Dry winds and source variability contribute to seasonal influences on these events. This study assesses the air quality risks posed by such events, which can affect broad regions worldwide.
Meng Wang, Qiyuan Wang, Steven Sai Hang Ho, Jie Tian, Yong Zhang, Shun-cheng Lee, and Junji Cao
Atmos. Chem. Phys., 24, 11175–11189, https://doi.org/10.5194/acp-24-11175-2024, https://doi.org/10.5194/acp-24-11175-2024, 2024
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We studied nitrogen-containing organic compounds (NOCs) in particulate matter <2.5 µm particles on the southeastern Tibetan Plateau. We found that biomass burning and transboundary transport are the main sources of NOCs in the high-altitude area. Understanding these aerosol sources informs how they add to regional and potentially global climate changes. Our findings could help shape effective environmental policies to enhance air quality and address climate impacts in this sensitive region.
Jinbo Wang, Jiaping Wang, Yuxuan Zhang, Tengyu Liu, Xuguang Chi, Xin Huang, Dafeng Ge, Shiyi Lai, Caijun Zhu, Lei Wang, Qiaozhi Zha, Ximeng Qi, Wei Nie, Congbin Fu, and Aijun Ding
Atmos. Chem. Phys., 24, 11063–11080, https://doi.org/10.5194/acp-24-11063-2024, https://doi.org/10.5194/acp-24-11063-2024, 2024
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In this study, we found large spatial discrepancies in the physical and chemical properties of black carbon over the Tibetan Plateau (TP). Elevated anthropogenic emissions from low-altitude regions can significantly change the mass concentration, mixing state and chemical composition of black-carbon-containing aerosol in the TP region, further altering its light absorption ability. Our study emphasizes the vulnerability of remote plateau regions to intense anthropogenic influences.
Liyuan Zhou, Qianyun Liu, Christian M. Salvador, Michael Le Breton, Mattias Hallquist, Jian Zhen Yu, Chak K. Chan, and Åsa M. Hallquist
Atmos. Chem. Phys., 24, 11045–11061, https://doi.org/10.5194/acp-24-11045-2024, https://doi.org/10.5194/acp-24-11045-2024, 2024
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Our research on city bus emissions reveals that alternative fuels (compressed natural gas and biofuels) reduce fresh particle emissions compared to diesel. However, all fuels lead to secondary air pollution. Aiming at guiding better environmental policies, we studied 76 buses using advanced emission measurement techniques. This work sheds light on the complex effects of bus fuels on urban air quality, emphasizing the need for comprehensive evaluations of future transportation technologies.
Xu Yang, Fobang Liu, Shuqi Yang, Yuling Yang, Yanan Wang, Jingjing Li, Mingyu Zhao, Zhao Wang, Kai Wang, Chi He, and Haijie Tong
Atmos. Chem. Phys., 24, 11029–11043, https://doi.org/10.5194/acp-24-11029-2024, https://doi.org/10.5194/acp-24-11029-2024, 2024
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A study in the rural North China Plain showed environmentally persistent free radicals (EPFRs) in atmospheric particulate matter (PM), with a notable water-soluble fraction likely from atmospheric oxidation during transport. Significant positive correlations between EPFRs and the water-soluble oxidative potential of PM2.5 were found, primarily attributable to the water-soluble fractions of EPFRs. These findings emphasize understanding EPFRs' atmospheric evolution for climate and health impacts.
Kirsten N. Fossum, Chunshui Lin, Niall O'Sullivan, Lu Lei, Stig Hellebust, Darius Ceburnis, Aqeel Afzal, Anja Tremper, David Green, Srishti Jain, Steigvilė Byčenkienė, Colin O'Dowd, John Wenger, and Jurgita Ovadnevaite
Atmos. Chem. Phys., 24, 10815–10831, https://doi.org/10.5194/acp-24-10815-2024, https://doi.org/10.5194/acp-24-10815-2024, 2024
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The chemical composition and sources of submicron aerosol in the Dublin Port area were investigated over a month-long campaign. Two distinct types of ship emissions were identified and characterised: sulfate-rich plumes from the use of heavy fuel oil with scrubbers and organic-rich plumes from the use of low-sulfur fuels. The latter were more frequent, emitting double the particle number and having a typical V / Ni ratio for ship emission.
Xiao He, Xuan Zheng, Shuwen Guo, Lewei Zeng, Ting Chen, Bohan Yang, Shupei Xiao, Qiongqiong Wang, Zhiyuan Li, Yan You, Shaojun Zhang, and Ye Wu
Atmos. Chem. Phys., 24, 10655–10666, https://doi.org/10.5194/acp-24-10655-2024, https://doi.org/10.5194/acp-24-10655-2024, 2024
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This study introduces an innovative method for identifying and quantifying complex organic vapors and aerosols. By combining advanced analytical techniques and new algorithms, we categorized thousands of compounds from heavy-duty diesel vehicles and ambient air and highlighted specific tracers for emission sources. The innovative approach enhances peak identification, reduces quantification uncertainties, and offers new insights for air quality management and atmospheric chemistry.
Yu Xu, Tang Liu, Yi-Jia Ma, Qi-Bin Sun, Hong-Wei Xiao, Hao Xiao, Hua-Yun Xiao, and Cong-Qiang Liu
Atmos. Chem. Phys., 24, 10531–10542, https://doi.org/10.5194/acp-24-10531-2024, https://doi.org/10.5194/acp-24-10531-2024, 2024
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This study investigates the characteristics of aminiums and ammonium in PM2.5 on clean and polluted winter days in 11 Chinese cities, highlighting the possibility of the competitive uptake of ammonia versus amines on acidic aerosols or the displacement of aminiums by ammonia under high-ammonia conditions. The overall results deepen the understanding of the spatiotemporal differences in aminium characteristics and formation in China.
Cassidy Soloff, Taiwo Ajayi, Yonghoon Choi, Ewan C. Crosbie, Joshua P. DiGangi, Glenn S. Diskin, Marta A. Fenn, Richard A. Ferrare, Francesca Gallo, Johnathan W. Hair, Miguel Ricardo A. Hilario, Simon Kirschler, Richard H. Moore, Taylor J. Shingler, Michael A. Shook, Kenneth L. Thornhill, Christiane Voigt, Edward L. Winstead, Luke D. Ziemba, and Armin Sorooshian
Atmos. Chem. Phys., 24, 10385–10408, https://doi.org/10.5194/acp-24-10385-2024, https://doi.org/10.5194/acp-24-10385-2024, 2024
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Using aircraft measurements over the northwestern Atlantic between the US East Coast and Bermuda and trajectory modeling of continental outflow, we identify trace gas and particle properties that exhibit gradients with offshore distance and quantify these changes with high-resolution measurements of concentrations and particle chemistry, size, and scattering properties. This work furthers our understanding of the complex interactions between continental and marine environments.
Alex Rowell, James Brean, David C. S. Beddows, Zongbo Shi, Avinash Kumar, Matti Rissanen, Miikka Dal Maso, Peter Mettke, Kay Weinhold, Maik Merkel, and Roy M. Harrison
Atmos. Chem. Phys., 24, 10349–10361, https://doi.org/10.5194/acp-24-10349-2024, https://doi.org/10.5194/acp-24-10349-2024, 2024
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Ions enhance the formation and growth rates of new particles, affecting the Earth's radiation budget. Despite these effects, there is little published data exploring the sources of ions in the urban environment and their role in new particle formation (NPF). Here we show that natural ion sources dominate in urban environments, while traffic is a secondary source. Ions contribute up to 12.7 % of the formation rate of particles, indicating that they are important for forming urban PM.
Yuan Cheng, Xu-bing Cao, Sheng-qiang Zhu, Zhi-qing Zhang, Jiu-meng Liu, Hong-liang Zhang, Qiang Zhang, and Ke-bin He
Atmos. Chem. Phys., 24, 9869–9883, https://doi.org/10.5194/acp-24-9869-2024, https://doi.org/10.5194/acp-24-9869-2024, 2024
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The agreement between observational and modeling results is essential for the development of efficient air pollution control strategies. Here we constrained the modeling results of carbonaceous aerosols by field observation in Northeast China, a historically overlooked but recently targeted region of national clean-air actions. Our study suggested that the simulation of agricultural fire emissions and secondary organic aerosols remains challenging.
Yuan Dai, Junfeng Wang, Houjun Wang, Shijie Cui, Yunjiang Zhang, Haiwei Li, Yun Wu, Ming Wang, Eleonora Aruffo, and Xinlei Ge
Atmos. Chem. Phys., 24, 9733–9748, https://doi.org/10.5194/acp-24-9733-2024, https://doi.org/10.5194/acp-24-9733-2024, 2024
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Short-term strict emission control can improve air quality, but its effectiveness needs assessment. During the 2021 summer COVID-19 lockdown in Yangzhou, we found that PM2.5 levels did not decrease despite reduced primary emissions. Aged black-carbon particles increased substantially due to higher O3 levels and transported pollutants. High humidity and low wind also played key roles. The results highlight the importance of a regionally balanced control strategy for future air quality management.
Xinya Liu, Diego Alves Gouveia, Bas Henzing, Arnoud Apituley, Arjan Hensen, Danielle van Dinther, Rujin Huang, and Ulrike Dusek
Atmos. Chem. Phys., 24, 9597–9614, https://doi.org/10.5194/acp-24-9597-2024, https://doi.org/10.5194/acp-24-9597-2024, 2024
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The vertical distribution of aerosol optical properties is important for their effect on climate. This is usually measured by lidar, which has limitations, most notably the assumption of a lidar ratio. Our study shows that routine surface-level aerosol measurements are able to predict this lidar ratio reasonably well within the lower layers of the atmosphere and thus provide a relatively simple and cost-effective method to improve lidar measurements.
Weiqi Xu, Ye Kuang, Wanyun Xu, Zhiqiang Zhang, Biao Luo, Xiaoyi Zhang, Jiangchuang Tao, Hongqin Qiao, Li Liu, and Yele Sun
Atmos. Chem. Phys., 24, 9387–9399, https://doi.org/10.5194/acp-24-9387-2024, https://doi.org/10.5194/acp-24-9387-2024, 2024
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We deployed an advanced aerosol–fog sampling system at a rural site in the North China Plain to investigate impacts of aerosol hygroscopic growth and activation on the physicochemical properties of submicron aerosols. Observed results highlighted remarkably different aqueous processing of primary and secondary submicron aerosol components under distinct ambient relative humidity (RH) conditions and that RH levels significantly impact aerosol sampling through the aerosol swelling effect.
Can Wu, Xiaodi Liu, Ke Zhang, Si Zhang, Cong Cao, Jianjun Li, Rui Li, Fan Zhang, and Gehui Wang
Atmos. Chem. Phys., 24, 9263–9275, https://doi.org/10.5194/acp-24-9263-2024, https://doi.org/10.5194/acp-24-9263-2024, 2024
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Brown carbon (BrC) is prevalent in the troposphere and can efficiently absorb solar and terrestrial radiation. Our observations show that the enhanced light absorption of BrC relative to black carbon at the tropopause can be attributed to the formation of nitrogen-containing organic compounds through the aqueous-phase reactions of carbonyls with ammonium.
Taiwo Ajayi, Yonghoon Choi, Ewan C. Crosbie, Joshua P. DiGangi, Glenn S. Diskin, Marta A. Fenn, Richard A. Ferrare, Johnathan W. Hair, Miguel Ricardo A. Hilario, Chris A. Hostetler, Simon Kirschler, Richard H. Moore, Taylor J. Shingler, Michael A. Shook, Cassidy Soloff, Kenneth L. Thornhill, Christiane Voigt, Edward L. Winstead, Luke D. Ziemba, and Armin Sorooshian
Atmos. Chem. Phys., 24, 9197–9218, https://doi.org/10.5194/acp-24-9197-2024, https://doi.org/10.5194/acp-24-9197-2024, 2024
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This study uses airborne data to examine vertical profiles of trace gases, aerosol particles, and meteorological variables over a remote marine area (Bermuda). Results show distinct differences based on both air mass source region (North America, Ocean, Caribbean/North Africa) and altitude for a given air mass type. This work highlights the sensitivity of remote marine areas to long-range transport and the importance of considering the vertical dependence of trace gas and aerosol properties.
Kira Zeider, Grace Betito, Anthony Bucholtz, Peng Xian, Annette Walker, and Armin Sorooshian
Atmos. Chem. Phys., 24, 9059–9083, https://doi.org/10.5194/acp-24-9059-2024, https://doi.org/10.5194/acp-24-9059-2024, 2024
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The predominant wind direction along the California coast (northerly) reverses several times during the summer (to southerly). The effects of these wind reversals on aerosol and cloud characteristics are not well understood. Using data from multiple datasets we found that southerly flow periods had enhanced signatures of anthropogenic emissions due to shipping and continental sources, and clouds had more but smaller droplets.
Saleh Alzahrani, Doğuşhan Kılıç, Michael Flynn, Paul I. Williams, and James Allan
Atmos. Chem. Phys., 24, 9045–9058, https://doi.org/10.5194/acp-24-9045-2024, https://doi.org/10.5194/acp-24-9045-2024, 2024
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This paper investigates emissions from aviation activities at an international airport to evaluate their impact on local air quality. The study provides detailed insights into the chemical composition of aerosols and key pollutants in the airport environment. Source apportionment analysis using positive matrix factorisation (PMF) identified three significant sources: less oxidised oxygenated organic aerosol, alkane organic aerosol, and more oxidised oxygenated organic aerosol.
Mingjie Kang, Mengying Bao, Wenhuai Song, Aduburexiati Abulimiti, Fang Cao, Sönke Szidat, and Yanlin Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2024-2098, https://doi.org/10.5194/egusphere-2024-2098, 2024
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Reports on the molecular level knowledge of high temporal resolution PM2.5 components on hazy days are still limited. This study investigated many individual PM2.5 species and sources. The results show biomass burning (BB) was the main source of organic carbon. Moreover, BB enhanced fungal spore emissions and secondary aerosol formation. The contribution of non-fossils increased with increasing haze pollution. These findings suggest BB may be an important driver of haze events in winter.
Mikko Heikkilä, Krista Luoma, Timo Mäkelä, and Tiia Grönholm
Atmos. Chem. Phys., 24, 8927–8941, https://doi.org/10.5194/acp-24-8927-2024, https://doi.org/10.5194/acp-24-8927-2024, 2024
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Black carbon (BC) concentration was measured from 211 ship exhaust gas plumes at a remote marine station. Emission factors of BC were calculated in grams per kilogram of fuel. Ships with an exhaust gas cleaning system (EGCS) were found to have median BC emissions per fuel consumed 5 times lower than ships without an EGCS. However, this might be because of non-EGCS ships running at low engine loads rather than the EGCS itself. A local speed restriction would increase BC emissions of ships.
Olga Zografou, Maria Gini, Prodromos Fetfatzis, Konstantinos Granakis, Romanos Foskinis, Manousos Ioannis Manousakas, Fotios Tsopelas, Evangelia Diapouli, Eleni Dovrou, Christina N. Vasilakopoulou, Alexandros Papayannis, Spyros N. Pandis, Athanasios Nenes, and Konstantinos Eleftheriadis
Atmos. Chem. Phys., 24, 8911–8926, https://doi.org/10.5194/acp-24-8911-2024, https://doi.org/10.5194/acp-24-8911-2024, 2024
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Characterization of PM1 and positive matrix factorization (PMF) source apportionment of organic and inorganic fractions were conducted at the high-altitude station (HAC)2. Cloud presence reduced PM1, affecting sulfate more than organics. Free-troposphere (FT) conditions showed more black carbon (eBC) than planetary boundary layer (PBL) conditions.
Yuanyuan Qin, Xinghua Zhang, Wei Huang, Juanjuan Qin, Xiaoyu Hu, Yuxuan Cao, Tianyi Zhao, Yang Zhang, Jihua Tan, Ziyin Zhang, Xinming Wang, and Zhenzhen Wang
Atmos. Chem. Phys., 24, 8737–8750, https://doi.org/10.5194/acp-24-8737-2024, https://doi.org/10.5194/acp-24-8737-2024, 2024
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Environmental persistent free radicals (EPFRs) and reactive oxygen species (ROSs) play an active role in the atmosphere. Despite control measures having effectively reduced their emissions, reductions were less than in PM2.5. Emission control measures performed well in achieving Parade Blue, but reducing the impact of the atmosphere on human health remains challenging. Thus, there is a need to reassess emission control measures to better address the challenges posed by EPFRs and ROSs.
Fenghua Wei, Xing Peng, Liming Cao, Mengxue Tang, Ning Feng, Xiaofeng Huang, and Lingyan He
Atmos. Chem. Phys., 24, 8507–8518, https://doi.org/10.5194/acp-24-8507-2024, https://doi.org/10.5194/acp-24-8507-2024, 2024
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The water solubility of secondary organic aerosols (SOAs) is a crucial factor in determining their hygroscopicity and climatic impact. Stable carbon isotope and mass spectrometry techniques were combined to assess the water solubility of SOAs with different aging degrees in a coastal megacity in China. This work revealed a much higher water-soluble fraction of aged SOA compared to fresh SOA, indicating that the aging degree of SOA has considerable impacts on its water solubility.
Feifei Li, Shanshan Tang, Jitao Lv, Shiyang Yu, Xu Sun, Dong Cao, Yawei Wang, and Guibin Jiang
Atmos. Chem. Phys., 24, 8397–8411, https://doi.org/10.5194/acp-24-8397-2024, https://doi.org/10.5194/acp-24-8397-2024, 2024
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Targeted derivatization and non-targeted analysis with Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) were used to reveal the molecular composition of carbonyl molecules in PM2.5, and the important role of carbonyls in increasing the oxidative potential of organic aerosol was found in real samples.
Adam E. Thomas, Hayley S. Glicker, Alex B. Guenther, Roger Seco, Oscar Vega Bustillos, Julio Tota, Rodrigo A. F. Souza, and James N. Smith
EGUsphere, https://doi.org/10.5194/egusphere-2024-2230, https://doi.org/10.5194/egusphere-2024-2230, 2024
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We present measurements of the composition of ultrafine particles collected from the eastern Amazon, a relatively understudied region that is subjected to increasing human influence. We find that while isoprene chemistry is likely significant to ultrafine particle growth throughout the year, compounds related to other sources such as biological spore emissions and biomass burning exhibit striking seasonal differences, implying an extensive variation in regional ultrafine particle sources.
Maya Abou-Ghanem, Daniel M. Murphy, Gregory P. Schill, Michael J. Lawler, and Karl D. Froyd
Atmos. Chem. Phys., 24, 8263–8275, https://doi.org/10.5194/acp-24-8263-2024, https://doi.org/10.5194/acp-24-8263-2024, 2024
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Using particle analysis by laser mass spectrometry, we examine vanadium-containing ship exhaust particles measured on NASA's DC-8 during the Atmospheric Tomography Mission (ATom). Our results reveal ship exhaust particles are sufficiently widespread in the marine atmosphere and experience atmospheric aging. Finally, we use laboratory calibrations to determine the vanadium, sulfate, and organic single-particle mass fractions of vanadium-containing ship exhaust particles.
Cassandra J. Gaston, Joseph M. Prospero, Kristen Foley, Havala O. T. Pye, Lillian Custals, Edmund Blades, Peter Sealy, and James A. Christie
Atmos. Chem. Phys., 24, 8049–8066, https://doi.org/10.5194/acp-24-8049-2024, https://doi.org/10.5194/acp-24-8049-2024, 2024
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To understand how changing emissions have impacted aerosols in remote regions, we measured nitrate and sulfate in Barbados and compared them to model predictions from EPA’s Air QUAlity TimE Series (EQUATES). Nitrate was stable, except for spikes in 2008 and 2010 due to transported smoke. Sulfate decreased in the 1990s due to reductions in sulfur dioxide (SO2) in the US and Europe; then it increased in the 2000s, likely due to anthropogenic emissions from Africa.
Jie Zhang, Tianyu Zhu, Alexandra Catena, Yaowei Li, Margaret Schwab, Pengfei Liu, Akua Asa-Awuku, and James Schwab
EGUsphere, https://doi.org/10.5194/egusphere-2024-1390, https://doi.org/10.5194/egusphere-2024-1390, 2024
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This study shows the derived organic aerosol hygroscopicity under high humidity conditions based on a simple optical scatter monitor system, including two nephelometric monitors (pDR-1500), after knowing the aerosol chemical composition.
Jiao Xue, Tian Zhang, Keyhong Park, Jinpei Yan, Young Jun Yoon, Jiyeon Park, and Bingbing Wang
Atmos. Chem. Phys., 24, 7731–7754, https://doi.org/10.5194/acp-24-7731-2024, https://doi.org/10.5194/acp-24-7731-2024, 2024
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Ice formation by particles is an important way of making mixed-phase and ice clouds. We found that particles collected in the marine atmosphere exhibit diverse ice nucleation abilities and mixing states. Sea salt mixed-sulfate particles were enriched in ice-nucleating particles. Selective aging on sea salt particles made particle populations more externally mixed. Characterizations of particles and their mixing state are needed for a better understanding of aerosol–cloud interactions.
Yangzhi Mo, Jun Li, Guangcai Zhong, Sanyuan Zhu, Shizhen Zhao, Jiao Tang, Hongxing Jiang, Zhineng Cheng, Chongguo Tian, Yingjun Chen, and Gan Zhang
Atmos. Chem. Phys., 24, 7755–7772, https://doi.org/10.5194/acp-24-7755-2024, https://doi.org/10.5194/acp-24-7755-2024, 2024
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In this study, we found that biomass burning (31.0 %) and coal combustion (31.1 %) were the dominant sources of water-insoluble organic carbon in China, with coal combustion sources exhibiting the strongest light-absorbing capacity. Additionally, we propose a light-absorbing carbonaceous continuum, revealing that components enriched with fossil sources tend to have stronger light-absorbing capacity, higher aromaticity, higher molecular weights, and greater recalcitrance in the atmosphere.
Jing Duan, Ru-Jin Huang, Ying Wang, Wei Xu, Haobin Zhong, Chunshui Lin, Wei Huang, Yifang Gu, Jurgita Ovadnevaite, Darius Ceburnis, and Colin O'Dowd
Atmos. Chem. Phys., 24, 7687–7698, https://doi.org/10.5194/acp-24-7687-2024, https://doi.org/10.5194/acp-24-7687-2024, 2024
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The chemical composition of atmospheric particles has shown significant changes in recent years. We investigated the potential effects of changes in inorganics on aerosol water uptake and, thus, secondary organic aerosol formation in wintertime haze based on the size-resolved measurements of non-refractory fine particulate matter (NR-PM2.5) in Xi’an, northwestern China. We highlight the key role of aerosol water as a medium to link inorganics and organics in their multiphase processes.
Hongyong Li, Xiaopu Lyu, Likun Xue, Yunxi Huo, Dawen Yao, Haoxian Lu, and Hai Guo
Atmos. Chem. Phys., 24, 7085–7100, https://doi.org/10.5194/acp-24-7085-2024, https://doi.org/10.5194/acp-24-7085-2024, 2024
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Organic aerosol is ubiquitous in the atmosphere and largely explains the gap between current levels of fine particulate matter in many cities and the World Health Organization guideline values. This study highlights the dominant contributions of cooking emissions to organic aerosol when marine air prevailed in Hong Kong, which were occasionally overwhelmed by aromatics-derived secondary organic aerosol in continental ouflows.
Shao Shi, Jinghao Zhai, Xin Yang, Yechun Ruan, Yuanlong Huang, Xujian Chen, Antai Zhang, Jianhuai Ye, Guomao Zheng, Baohua Cai, Yaling Zeng, Yixiang Wang, Chunbo Xing, Yujie Zhang, Tzung-May Fu, Lei Zhu, Huizhong Shen, and Chen Wang
Atmos. Chem. Phys., 24, 7001–7012, https://doi.org/10.5194/acp-24-7001-2024, https://doi.org/10.5194/acp-24-7001-2024, 2024
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The determination of ions in the mass spectra of individual particles remains uncertain. We have developed a standard-free mass calibration algorithm applicable to more than 98 % of ambient particles. With our algorithm, ions with ~ 0.05 Th mass difference could be determined. Therefore, many more atmospheric species could be determined and involved in the source apportionment of aerosols, the study of chemical reaction mechanisms, and the analysis of single-particle mixing states.
Wei Sun, Xiaodong Hu, Yuzhen Fu, Guohua Zhang, Yujiao Zhu, Xinfeng Wang, Caiqing Yan, Likun Xue, He Meng, Bin Jiang, Yuhong Liao, Xinming Wang, Ping'an Peng, and Xinhui Bi
Atmos. Chem. Phys., 24, 6987–6999, https://doi.org/10.5194/acp-24-6987-2024, https://doi.org/10.5194/acp-24-6987-2024, 2024
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The formation pathways of nitrogen-containing compounds (NOCs) in the atmosphere remain unclear. We investigated the composition of aerosols and fog water by state-of-the-art mass spectrometry and compared the formation pathways of NOCs. We found that NOCs in aerosols were mainly formed through nitration reaction, while ammonia addition played a more important role in fog water. The results deepen our understanding of the processes of organic particulate pollution.
Fuzhen Shen, Michaela I. Hegglin, and Yue Yuan
Atmos. Chem. Phys., 24, 6539–6553, https://doi.org/10.5194/acp-24-6539-2024, https://doi.org/10.5194/acp-24-6539-2024, 2024
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We attempt to use a novel structural self-organising map and machine learning models to identify a weather system and quantify the importance of each meteorological factor in driving the unexpected PM2.5 and O3 changes under the specific weather system during the COVID-19 lockdown in China. The result highlights that temperature under the double-centre high-pressure system plays the most crucial role in abnormal events.
Wenshuai Li, Yuxuan Qi, Yingchen Liu, Guanru Wu, Yanjing Zhang, Jinhui Shi, Wenjun Qu, Lifang Sheng, Wencai Wang, Daizhou Zhang, and Yang Zhou
Atmos. Chem. Phys., 24, 6495–6508, https://doi.org/10.5194/acp-24-6495-2024, https://doi.org/10.5194/acp-24-6495-2024, 2024
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Aerosol particles from mainland can transport to oceans and deposit, providing soluble Fe and affecting phytoplankton growth. Thus, we studied the dissolution process of aerosol Fe and found that photochemistry played a key role in promoting Fe dissolution in clean conditions. RH-dependent reactions were more influential in slightly polluted conditions. These results highlight the distinct roles of two weather-related parameters (radiation and RH) in influencing geochemical cycles related to Fe.
Yanqin Ren, Zhenhai Wu, Yuanyuan Ji, Fang Bi, Junling Li, Haijie Zhang, Hao Zhang, Hong Li, and Gehui Wang
Atmos. Chem. Phys., 24, 6525–6538, https://doi.org/10.5194/acp-24-6525-2024, https://doi.org/10.5194/acp-24-6525-2024, 2024
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Nitrated aromatic compounds (NACs) and oxygenated derivatives of polycyclic aromatic hydrocarbons (OPAHs) in PM2.5 were examined from an urban area in Beijing during the autumn and winter. The OPAH and NAC concentrations were much higher during heating than before heating. They majorly originated from the combustion of biomass and automobile emissions, and the secondary generation was the major contributor throughout the whole sampling period.
Rime El Asmar, Zongrun Li, David J. Tanner, Yongtao Hu, Susan O’Neill, L. Gregory Huey, M. Talat Odman, and Rodney J. Weber
EGUsphere, https://doi.org/10.5194/egusphere-2024-1485, https://doi.org/10.5194/egusphere-2024-1485, 2024
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Prescribed burning is an important method for managing ecosystems and preventing wildfires, however, smoke from prescribed fires can have a significant impact on air quality. Here, using a network of fixed sites and sampling throughout an extended prescribed burning period in two different years, we characterize the emissions and evolution up to 8 hours of PM2.5 mass, BC, and BrC in smoke from burning of forested lands in the southeastern US.
Gregory P. Schill, Karl D. Froyd, Daniel M. Murphy, Christina J. Williamson, Charles Brock, Tomás Sherwen, Mat J. Evans, Eric A. Ray, Eric C. Apel, Rebecca S. Hornbrook, Alan J. Hills, Jeff Peischl, Tomas B. Ryerson, Chelsea R. Thompson, Ilann Bourgeois, Donald R. Blake, Joshua P. DiGangi, and Glenn S. Diskin
EGUsphere, https://doi.org/10.5194/egusphere-2024-1399, https://doi.org/10.5194/egusphere-2024-1399, 2024
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Using single-particle mass spectrometry, we show that trace concentrations of bromine and iodine are ubiquitous in remote tropospheric aerosol, and suggest that aerosols are an important part of the global reactive iodine budget. Comparisons to a global climate model with detailed iodine chemistry are favorable in the background atmosphere; however, the model cannot replicate our measurements near the ocean surface, in biomass burning plumes, and in the stratosphere.
Marco Paglione, David C. S. Beddows, Anna Jones, Thomas Lachlan-Cope, Matteo Rinaldi, Stefano Decesari, Francesco Manarini, Mara Russo, Karam Mansour, Roy M. Harrison, Andrea Mazzanti, Emilio Tagliavini, and Manuel Dall'Osto
Atmos. Chem. Phys., 24, 6305–6322, https://doi.org/10.5194/acp-24-6305-2024, https://doi.org/10.5194/acp-24-6305-2024, 2024
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Applying factor analysis techniques to H-NMR spectra, we present the organic aerosol (OA) source apportionment of PM1 samples collected in parallel at two Antarctic stations, namely Signy and Halley, allowing investigation of aerosol–climate interactions in an unperturbed atmosphere. Our results show remarkable differences between pelagic (open-ocean) and sympagic (sea-ice-influenced) air masses and indicate that various sources and processes are controlling Antarctic aerosols.
Zhichao Dong, Chandra Mouli Pavuluri, Peisen Li, Zhanjie Xu, Junjun Deng, Xueyan Zhao, Xiaomai Zhao, Pingqing Fu, and Cong-Qiang Liu
Atmos. Chem. Phys., 24, 5887–5905, https://doi.org/10.5194/acp-24-5887-2024, https://doi.org/10.5194/acp-24-5887-2024, 2024
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Comprehensive study of optical properties of brown carbon (BrC) in fine aerosols from Tianjin, China, implied that biological emissions are major sources of BrC in summer, whereas fossil fuel combustion and biomass burning emissions are in cold periods. The direct radiation absorption caused by BrC in short wavelengths contributed about 40 % to that caused by BrC in 300–700 nm. Water-insoluble but methanol-soluble BrC contains more protein-like chromophores (PLOM) than that of water-soluble BrC.
Kumiko Goto-Azuma, Yoshimi Ogawa-Tsukagawa, Kaori Fukuda, Koji Fujita, Motohiro Hirabayashi, Remi Dallmayr, Jun Ogata, Nobuhiro Moteki, Tatsuhiro Mori, Sho Ohata, Yutaka Kondo, Makoto Koike, Sumito Matoba, and Teruo Aoki
EGUsphere, https://doi.org/10.5194/egusphere-2024-1498, https://doi.org/10.5194/egusphere-2024-1498, 2024
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Monthly records spanning 350 years from a Greenland ice core reveal trends in black carbon (BC) concentrations and sizes. BC concentrations have risen since the late 19th century due to the inflow of anthropogenic BC, with these particles being larger than those from biomass burning (BB). High BB BC concentration peaks in summer originating from BB could reduce albedo. However, BB BC showed no upward trend until the early 2000s. Our findings are crucial for validating aerosol and climate models.
Shan Wang, Kezheng Liao, Zijing Zhang, Yuk Ying Cheng, Qiongqiong Wang, Hanzhe Chen, and Jian Zhen Yu
Atmos. Chem. Phys., 24, 5803–5821, https://doi.org/10.5194/acp-24-5803-2024, https://doi.org/10.5194/acp-24-5803-2024, 2024
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In this work, hourly primary and secondary organic carbon were estimated by a novel Bayesian inference approach in suburban Hong Kong. Their multi-temporal-scale variations and evolution characteristics during PM2.5 episodes were examined. The methodology could serve as a guide for other locations with similar monitoring capabilities. The observation-based results are helpful for understanding the evolving nature of secondary organic aerosols and refining the accuracy of model simulations.
Andreas Aktypis, Dontavious Sippial, Christina Vasilakopoulou, Angeliki Matrali, Christos Kaltsonoudis, Andrea Simonati, Marco Paglione, Matteo Rinaldi, Stefano Decesari, and Spyros Pandis
EGUsphere, https://doi.org/10.5194/egusphere-2024-1317, https://doi.org/10.5194/egusphere-2024-1317, 2024
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A dual chamber system was deployed in two different environments (Po Valley, Italy and Pertouli forest, Greece) to study the potential of ambient air directly injected into the chambers, to form secondary aerosol. In the Po Valley, the system reacts rapidly forming large amounts of SOA, while in Pertouli the corresponding SOA formation chemistry appears to have been practically terminated before the beginning of most experiments, so there is little additional SOA formation potential left.
Mingfu Cai, Chenshuo Ye, Bin Yuan, Shan Huang, E Zheng, Suxia Yang, Zelong Wang, Yi Lin, Tiange Li, Weiwei Hu, Wei Chen, Qicong Song, Wei Li, Yuwen Peng, Baolin Liang, Qibin Sun, Jun Zhao, Duohong Chen, Jiaren Sun, Zhiyong Yang, and Min Shao
EGUsphere, https://doi.org/10.5194/egusphere-2024-887, https://doi.org/10.5194/egusphere-2024-887, 2024
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This study investigated the daytime secondary organic aerosol (SOA) formation in urban plumes. We observed a significant daytime SOA formation through gas-particle partitioning when the site was affected by urban plumes. Box model simulation indicated that urban pollutants (nitrogen oxide and volatile organic compounds) could enhance the oxidizing capacity, while the elevated volatile organic compounds were mainly responsible for promoting daytime SOA formation.
James Brean, David C. S. Beddows, Eija Asmi, Ari Virkkula, Lauriane L. J. Quéléver, Mikko Sipilä, Floortje Van Den Heuvel, Thomas Lachlan-Cope, Anna Jones, Markus Frey, Angelo Lupi, Jiyeon Park, Young Jun Yoon, Ralf Weller, Giselle L. Marincovich, Gabriela C. Mulena, Roy M. Harrison, and Manuel Dall´Osto
EGUsphere, https://doi.org/10.5194/egusphere-2024-987, https://doi.org/10.5194/egusphere-2024-987, 2024
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Our results emphasize how understanding the geographical variation in surface types across the Antarctic is key to understanding secondary aerosol sources.
Qun He, Zhaowen Wang, Houfeng Liu, Pengju Xu, Rongbao Duan, Caihong Xu, Jianmin Chen, and Min Wei
EGUsphere, https://doi.org/10.5194/egusphere-2024-841, https://doi.org/10.5194/egusphere-2024-841, 2024
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Coastal environments provide an ideal setting for investigating the intermixing processes of terrestrial and marine aerosols. Terrestrial air mass constituted a larger proportion during severe air pollution, harboring more animal and human pathogens. A relative shift towards marine air-mass with respect to pollution elimination, where saprophytic bacteria and fungi were predominant. Mixed air-mass reveals the intermixing processes of terrestrial and marine sources.
Cited articles
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Chen, Q., Heald, C. L., Jimenez, J. L., Canagaratna, M. R., Zhang, Q., He, L.-Y., Huang, X.-F., Campuzano-Jost, P., Palm, B. B., Poulain, L., Kuwara, M., Martin, S. T., Abbatt, J. P. D., Lee, A. K. Y., and Liggio, J.: Elemental composition of organic aerosol: The gap between ambient and laboratory measurements, Geophys. Res. Lett., 42, 4182–4189, https://doi.org/10.1002/2015GL063693, 2015.
Chen, Y., Xu, L., Humphry, T., Hettiyadura, A. P. S., Ovadnevaite, J., Huang, S., Poulain, L., Schroder, J. C., Campuzano-Jost, P., Jimenez, J. L., Herrmann, H., O'Dowd, C., Stone, E. A., and Ng, N. L.: Response of the Aerodyne Aerosol Mass Spectrometer to Inorganic Sulfates and Organosulfur Compounds: Applications in Field and Laboratory Measurements, Environ. Sci. Technol., 53, 5176–5186, https://doi.org/10.1021/acs.est.9b00884, 2019.
Chen, C.-L., Chen, T.-Y., Hung, H.-M., Tsai, P.-W., Chou, C. C.-K., and Chen, W.-N.: The influence of upslope fog on hygroscopicity and chemical composition of aerosols at a forest site in Taiwan, Atmos. Environ., 246, 118150, https://doi.org/10.1016/j.atmosenv.2020.118150, 2021.
DeCarlo, P. F., Ulbrich, I. M., Crounse, J., de Foy, B., Dunlea, E. J., Aiken, A. C., Knapp, D., Weinheimer, A. J., Campos, T., Wennberg, P. O., and Jimenez, J. L.: Investigation of the sources and processing of organic aerosol over the Central Mexican Plateau from aircraft measurements during MILAGRO, Atmos. Chem. Phys., 10, 5257–5280, https://doi.org/10.5194/acp-10-5257-2010, 2010.
De Gouw, J. and Jimenez, J. L.: Organic Aerosols in the Earth's Atmosphere, Environ. Sci. Technol., 43, 7614–7618, https://doi.org/10.1021/es9006004, 2009.
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Du, W., Sun, Y. L., Xu, Y. S., Jiang, Q., Wang, Q. Q., Yang, W., Wang, F., Bai, Z. P., Zhao, X. D., and Yang, Y. C.: Chemical characterization of submicron aerosol and particle growth events at a national background site (3295 m a.s.l.) on the Tibetan Plateau, Atmos. Chem. Phys., 15, 10811–10824, https://doi.org/10.5194/acp-15-10811-2015, 2015.
Fang, W. Z., Evangeliou, N., Eckhardt, S., Xing, J., Zhang, H. L., Xiao, H., Zhao, M. X., and Kim, S-W.: Increased contribution of biomass burning to haze events in Shanghai since China's clean air actions, Commun. Earth Environ., 4, 310, https://doi.org/10.1038/s43247-023-00979-z, 2023.
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Fry, J. L., Kiendler-Scharr, A., Rollins, A. W., Wooldridge, P. J., Brown, S. S., Fuchs, H., Dubé, W., Mensah, A., dal Maso, M., Tillmann, R., Dorn, H.-P., Brauers, T., and Cohen, R. C.: Organic nitrate and secondary organic aerosol yield from NO3 oxidation of β-pinene evaluated using a gas-phase kinetics/aerosol partitioning model, Atmos. Chem. Phys., 9, 1431–1449, https://doi.org/10.5194/acp-9-1431-2009, 2009.
Fry, J. L., Draper, D. C., Zarzana, K. J., Campuzano-Jost, P., Day, D. A., Jimenez, J. L., Brown, S. S., Cohen, R. C., Kaser, L., Hansel, A., Cappellin, L., Karl, T., Hodzic Roux, A., Turnipseed, A., Cantrell, C., Lefer, B. L., and Grossberg, N.: Observations of gas- and aerosol-phase organic nitrates at BEACHON-RoMBAS 2011, Atmos. Chem. Phys., 13, 8585–8605, https://doi.org/10.5194/acp-13-8585-2013, 2013.
Gao, M., Zhou, S. Z., He, Y., Zhang, G. H., Ma, N., Li, Y., Li, F. H., Yang, Y. X., Peng, L., Zhao, J., Bi, X. H., Hu, W. W., Sun, Y. L., Wang, B. G., and Wang, X. M.: In Situ Observation of Multiphase Oxidation-Driven Secondary Organic Aerosol Formation during Cloud Processing at a Mountain Site in Southern China, Environ. Sci. Technol. Lett., 10, 573–581, https://doi.org/10.1021/acs.estlett.3c00331, 2023.
Ge, X. L., Zhang, Q., Sun, Y. L., Ruehl, C. R., and Setyan, A.: Effect of aqueous-phase. processing on aerosol chemistry and size distributions in Fresno, California, during wintertime, Environ. Chem., 9, 221–235, 2012.
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Short summary
We investigated aerosol composition and sources and the interaction between secondary organic aerosol (SOA) and clouds at a regional mountain site in southeastern China. Clouds efficiently scavenge more oxidized SOA; however, cloud evaporation leads to the production of less oxidized SOA. The unexpectedly high presence of nitrate in aerosol particles indicates that nitrate formed in polluted areas has undergone interactions with clouds, significantly influencing the regional background site.
We investigated aerosol composition and sources and the interaction between secondary organic...
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