Articles | Volume 24, issue 4
https://doi.org/10.5194/acp-24-2399-2024
© 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-24-2399-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
26 Feb 2024
Research article |
| 26 Feb 2024
| 26 Feb 2024
Particle phase state and aerosol liquid water greatly impact secondary aerosol formation: insights into phase transition and its role in haze events
Xiangxinyue Meng
State Key Joint Laboratory of Environmental Simulation and Pollution Control, International Joint Laboratory for Regional Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China
Zhijun Wu
CORRESPONDING AUTHOR
State Key Joint Laboratory of Environmental Simulation and Pollution Control, International Joint Laboratory for Regional Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China
Collaborative Innovation Center of Atmospheric Environment and Equipment Technology, Nanjing University of Information Science and Technology, Nanjing 210044, China
Jingchuan Chen
State Key Joint Laboratory of Environmental Simulation and Pollution Control, International Joint Laboratory for Regional Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China
Yanting Qiu
State Key Joint Laboratory of Environmental Simulation and Pollution Control, International Joint Laboratory for Regional Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China
Taomou Zong
State Key Joint Laboratory of Environmental Simulation and Pollution Control, International Joint Laboratory for Regional Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China
Mijung Song
Department of Earth and Environmental Sciences, Jeonbuk National University, Jeonju, 54896, Republic of Korea
Jiyi Lee
Department of Environmental Science and Engineering, Ewha Womans University, Seoul, 03760, Republic of Korea
State Key Joint Laboratory of Environmental Simulation and Pollution Control, International Joint Laboratory for Regional Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China
Collaborative Innovation Center of Atmospheric Environment and Equipment Technology, Nanjing University of Information Science and Technology, Nanjing 210044, China
Related authors
Tao Qiu, Yanting Qiu, Yongyi Yuan, Rui Su, Xiangxinyue Meng, Jialiang Ma, Xiaofan Wang, Yu Gu, Zhijun Wu, Yang Ning, Xiuyi Hua, Dapeng Liang, and Deming Dong
EGUsphere, https://doi.org/10.5194/egusphere-2025-1808, https://doi.org/10.5194/egusphere-2025-1808, 2025
Short summary
Short summary
Our research reveals that some species from biomass burning and coal combustion dominate the light absorption of organic aerosols during winter. Cold weather helps these species accumulate in aerosols by slowing their degradation and altering atmospheric chemical processes. This means colder regions might experience stronger and more persistent climate impacts. Our findings highlight the importance of local temperatures and pollution sources when tackling climate challenges.
Yu Wang, Aristeidis Voliotis, Yunqi Shao, Taomou Zong, Xiangxinyue Meng, Mao Du, Dawei Hu, Ying Chen, Zhijun Wu, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 21, 11303–11316, https://doi.org/10.5194/acp-21-11303-2021, https://doi.org/10.5194/acp-21-11303-2021, 2021
Short summary
Short summary
Aerosol phase behaviour plays a profound role in atmospheric physicochemical processes. We designed dedicated chamber experiments to study the phase state of secondary organic aerosol from biogenic and anthropogenic mixed precursors. Our results highlight the key role of the organic–inorganic ratio and relative humidity in phase state, but the sources and organic composition are less important. The result provides solid laboratory evidence for understanding aerosol phase in a complex atmosphere.
Yu Li, Momei Qin, Weiwei Hu, Bin Zhao, Ying Li, Havala O. T. Pye, Jingyi Li, Linghan Zeng, Song Guo, Min Hu, and Jianlin Hu
EGUsphere, https://doi.org/10.5194/egusphere-2025-2879, https://doi.org/10.5194/egusphere-2025-2879, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
We evaluated how well a widely used air quality model simulates key properties of organic particles in the atmosphere, such as volatility and oxygen content, which influence how particles age, spread, and affect both air quality and climate. Using observations from eastern China, we found the model underestimated particle mass and misrepresented their chemical makeup. Our results highlight the need for improved emissions and chemical treatments to better predict air quality and climate impacts.
Jianjiong Mao, Lei Jiang, Zhicheng Feng, Jingyi Li, Yanhong Zhu, Momei Qin, Song Guo, Min Hu, and Jianlin Hu
EGUsphere, https://doi.org/10.5194/egusphere-2025-2992, https://doi.org/10.5194/egusphere-2025-2992, 2025
This preprint is open for discussion and under review for Geoscientific Model Development (GMD).
Short summary
Short summary
Tiny air particles impact air quality and climate change. Our study improved their prediction in China by modeling two key formation processes: ions + sulfuric acid (daytime) and sulfuric acid + dimethylamine (morning/evening). This improved model increases predictions by 36–84 % in Beijing and Nanjing. These advancements enable better demonstrate how these chemical processes significantly influence China's particulate pollution.
Ruiqi Man, Yishu Zhu, Zhijun Wu, Peter Aaron Alpert, Bingbing Wang, Jing Dou, Jie Chen, Yan Zheng, Yanli Ge, Qi Chen, Shiyi Chen, Xiangrui Kong, Markus Ammann, and Min Hu
EGUsphere, https://doi.org/10.5194/egusphere-2025-2301, https://doi.org/10.5194/egusphere-2025-2301, 2025
Short summary
Short summary
The particle chemical morphology is important to atmospheric multiphase and heterogeneous chemistry. This work directly observed the core-shell structure and water uptake behavior of individual submicron aerosol particles at an urban site and elucidated the potential impact on particle reactive uptake and heterogeneous reactions.
Jingye Ren, Songjian Zou, Honghao Xu, Guiquan Liu, Zhe Wang, Anran Zhang, Chuanfeng Zhao, Min Hu, Dongjie Shang, Lizi Tang, Ru-Jin Huang, Yele Sun, and Fang Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2025-1483, https://doi.org/10.5194/egusphere-2025-1483, 2025
Short summary
Short summary
In this study, a new framework of cloud condensation nuclei (CCN) prediction in polluted region has been developed and it achieves well prediction of hourly-to-yearly scale across North China Plain. The study reveals a significant long-term decreasing trend of CCN concentration at typical supersaturations due to a rapid reduction in aerosol concentrations from 2014 to 2018. This improvement of our new model would be helpful to aerosols climate effect assessment in models.
Shubin Li, Yujue Wang, Yiwen Zhang, Yizhe Yi, Yuchen Wang, Yuqi Guo, Chao Yu, Yue Jiang, Jinhui Shi, Chao Zhang, Jialei Zhu, Wei Hu, Jianzhen Yu, Xiaohong Yao, Huiwang Gao, and Min Hu
EGUsphere, https://doi.org/10.5194/egusphere-2025-2154, https://doi.org/10.5194/egusphere-2025-2154, 2025
Short summary
Short summary
Organosulfates (OSs) are an unrecognized and potentially important component in marine organic aerosols. In this study, we quantified and characterized the OSs over East Asian marginal seas. The chemical nature and spatiotemporal distribution of OSs were modified by the joint influence of marine emissions and transported terrestrial pollutants. The results highlight the vital roles of OSs in shaping organic aerosol formation and sulfur cycle during summer in marine boundary layer.
Kaiqi Wang, Kai Bi, Shuling Chen, Markus Hartmann, Zhijun Wu, Jiyu Gao, Xiaoyu Xu, Yuhan Cheng, Mengyu Huang, Yunbo Chen, Huiwen Xue, Bingbing Wang, Yaqiong Hu, Xiongying Zhang, Xincheng Ma, Ruijie Li, Ping Tian, Ottmar Möhler, Heike Wex, Frank Startmann, Jie Chen, and Xianda Gong
EGUsphere, https://doi.org/10.5194/egusphere-2025-1873, https://doi.org/10.5194/egusphere-2025-1873, 2025
Short summary
Short summary
Understanding how ice forms in clouds is crucial for predicting weather and climate; however, accurately measuring the ice-nucleating particles that trigger ice formation remains challenging. We developed an advanced instrument called the Freezing Ice Nucleation Detection Analyzer. By refining temperature control, automating freezing detection, and rigorously testing, we demonstrated that this instrument can reliably measure ice-nucleating particles across diverse conditions.
Tao Qiu, Yanting Qiu, Yongyi Yuan, Rui Su, Xiangxinyue Meng, Jialiang Ma, Xiaofan Wang, Yu Gu, Zhijun Wu, Yang Ning, Xiuyi Hua, Dapeng Liang, and Deming Dong
EGUsphere, https://doi.org/10.5194/egusphere-2025-1808, https://doi.org/10.5194/egusphere-2025-1808, 2025
Short summary
Short summary
Our research reveals that some species from biomass burning and coal combustion dominate the light absorption of organic aerosols during winter. Cold weather helps these species accumulate in aerosols by slowing their degradation and altering atmospheric chemical processes. This means colder regions might experience stronger and more persistent climate impacts. Our findings highlight the importance of local temperatures and pollution sources when tackling climate challenges.
Yu-Kai Tong, Zhijun Wu, Min Hu, and Anpei Ye
Atmos. Chem. Phys., 24, 2937–2950, https://doi.org/10.5194/acp-24-2937-2024, https://doi.org/10.5194/acp-24-2937-2024, 2024
Short summary
Short summary
The interplay between aerosols and moisture is one of the most crucial atmospheric processes. However, to date, literature results on the influence of phase separation on water diffusion in aerosols are divergent. This work directly unveiled the water diffusion process in single suspended phase-separated microdroplets and quantitatively analyzed the diffusion rate and extent. The results show that diffusion limitations and certain molecule clusters existed in the phase-separated aerosols.
Can Ye, Keding Lu, Xuefei Ma, Wanyi Qiu, Shule Li, Xinping Yang, Chaoyang Xue, Tianyu Zhai, Yuhan Liu, Xuan Li, Yang Li, Haichao Wang, Zhaofeng Tan, Xiaorui Chen, Huabin Dong, Limin Zeng, Min Hu, and Yuanhang Zhang
Atmos. Chem. Phys., 23, 15455–15472, https://doi.org/10.5194/acp-23-15455-2023, https://doi.org/10.5194/acp-23-15455-2023, 2023
Short summary
Short summary
In this study, combining comprehensive field measurements and a box model, we found NO2 conversion on the ground surface was the most important source for HONO production among the proposed heterogeneous and gas-phase HONO sources. In addition, HONO was found to evidently enhance O3 production and aggravate O3 pollution in summer in China. Our study improved our understanding of the relative importance of different HONO sources and the crucial role of HONO in O3 formation in polluted areas.
Xiaodong Xie, Jianlin Hu, Momei Qin, Song Guo, Min Hu, Dongsheng Ji, Hongli Wang, Shengrong Lou, Cheng Huang, Chong Liu, Hongliang Zhang, Qi Ying, Hong Liao, and Yuanhang Zhang
Atmos. Chem. Phys., 23, 10563–10578, https://doi.org/10.5194/acp-23-10563-2023, https://doi.org/10.5194/acp-23-10563-2023, 2023
Short summary
Short summary
The atmospheric age of particles reflects how long particles have been formed and suspended in the atmosphere, which is closely associated with the evolution processes of particles. An analysis of the atmospheric age of PM2.5 provides a unique perspective on the evolution processes of different PM2.5 components. The results also shed lights on how to design effective emission control actions under unfavorable meteorological conditions.
Taomou Zong, Zhijun Wu, Junrui Wang, Kai Bi, Wenxu Fang, Yanrong Yang, Xuena Yu, Zhier Bao, Xiangxinyue Meng, Yuheng Zhang, Song Guo, Yang Chen, Chunshan Liu, Yue Zhang, Shao-Meng Li, and Min Hu
Atmos. Meas. Tech., 16, 3679–3692, https://doi.org/10.5194/amt-16-3679-2023, https://doi.org/10.5194/amt-16-3679-2023, 2023
Short summary
Short summary
This study developed and characterized an indoor chamber system (AIR) to simulate atmospheric multiphase chemistry processes. The AIR chamber can accurately control temperature and relative humidity (RH) over a broad range and simulate diurnal variation of ambient atmospheric RH. The aerosol generation unit can generate organic-coating seed particles with different phase states. The AIR chamber demonstrates high-quality performance in simulating secondary aerosol formation.
Hejun Hu, Haichao Wang, Keding Lu, Jie Wang, Zelong Zheng, Xuezhen Xu, Tianyu Zhai, Xiaorui Chen, Xiao Lu, Wenxing Fu, Xin Li, Limin Zeng, Min Hu, Yuanhang Zhang, and Shaojia Fan
Atmos. Chem. Phys., 23, 8211–8223, https://doi.org/10.5194/acp-23-8211-2023, https://doi.org/10.5194/acp-23-8211-2023, 2023
Short summary
Short summary
Nitrate radical chemistry is critical to the degradation of volatile organic compounds (VOCs) and secondary organic aerosol formation. This work investigated the level, seasonal variation, and trend of nitrate radical reactivity towards volatile organic compounds (kNO3) in Beijing. We show the key role of isoprene and styrene in regulating seasonal variation in kNO3 and rebuild a long-term record of kNO3 based on the reported VOC measurements.
Lizi Tang, Min Hu, Dongjie Shang, Xin Fang, Jianjiong Mao, Wanyun Xu, Jiacheng Zhou, Weixiong Zhao, Yaru Wang, Chong Zhang, Yingjie Zhang, Jianlin Hu, Limin Zeng, Chunxiang Ye, Song Guo, and Zhijun Wu
Atmos. Chem. Phys., 23, 4343–4359, https://doi.org/10.5194/acp-23-4343-2023, https://doi.org/10.5194/acp-23-4343-2023, 2023
Short summary
Short summary
There was an evident distinction in the frequency of new particle formation (NPF) events at Nam Co station on the Tibetan Plateau: 15 % in pre-monsoon season and 80 % in monsoon season. The frequent NPF events in monsoon season resulted from the higher frequency of southerly air masses, which brought the organic precursors to participate in the NPF process. It increased the amount of aerosol and CCN compared with those in pre-monsoon season, which may markedly affect earth's radiation balance.
Ruiqi Man, Zhijun Wu, Taomou Zong, Aristeidis Voliotis, Yanting Qiu, Johannes Größ, Dominik van Pinxteren, Limin Zeng, Hartmut Herrmann, Alfred Wiedensohler, and Min Hu
Atmos. Chem. Phys., 22, 12387–12399, https://doi.org/10.5194/acp-22-12387-2022, https://doi.org/10.5194/acp-22-12387-2022, 2022
Short summary
Short summary
Regional and total deposition doses for different age groups were quantified based on explicit hygroscopicity measurements. We found that particle hygroscopic growth led to a reduction (~24 %) in the total dose. The deposition rate of hygroscopic particles was higher in the daytime, while hydrophobic particles exhibited a higher rate at night and during rush hours. The results will deepen the understanding of the impact of hygroscopicity and the mixing state on deposition patterns in the lungs.
Gang Zhao, Tianyi Tan, Shuya Hu, Zhuofei Du, Dongjie Shang, Zhijun Wu, Song Guo, Jing Zheng, Wenfei Zhu, Mengren Li, Limin Zeng, and Min Hu
Atmos. Chem. Phys., 22, 10861–10873, https://doi.org/10.5194/acp-22-10861-2022, https://doi.org/10.5194/acp-22-10861-2022, 2022
Short summary
Short summary
Black carbon is the second strongest absorbing component in the atmosphere that exerts warming effects on climate. One critical challenge in quantifying the ambient black carbon's radiative effects is addressing the BC microphysical properties. In this study, the microphysical properties of the aged and fresh BC particles are synthetically analyzed under different atmospheres. The measurement results can be further used in models to help constrain the uncertainties of the BC radiative effects.
Kai Song, Song Guo, Yuanzheng Gong, Daqi Lv, Yuan Zhang, Zichao Wan, Tianyu Li, Wenfei Zhu, Hui Wang, Ying Yu, Rui Tan, Ruizhe Shen, Sihua Lu, Shuangde Li, Yunfa Chen, and Min Hu
Atmos. Chem. Phys., 22, 9827–9841, https://doi.org/10.5194/acp-22-9827-2022, https://doi.org/10.5194/acp-22-9827-2022, 2022
Short summary
Short summary
Emissions from four typical Chinese domestic cooking and fried chicken using four kinds of oils were investigated to illustrate the impact of cooking style and oil. Of the estimated SOA, 10.2 %–32.0 % could be explained by S/IVOC oxidation. Multiway principal component analysis (MPCA) emphasizes the importance of the unsaturated fatty acid-alkadienal volatile product mechanism (oil autoxidation) accelerated by the cooking and heating procedure.
Rani Jeong, Joseph Lilek, Andreas Zuend, Rongshuang Xu, Man Nin Chan, Dohyun Kim, Hi Gyu Moon, and Mijung Song
Atmos. Chem. Phys., 22, 8805–8817, https://doi.org/10.5194/acp-22-8805-2022, https://doi.org/10.5194/acp-22-8805-2022, 2022
Short summary
Short summary
In this study, the viscosities of particles of sucrose–H2O, AS–H2O, and sucrose–AS–H2O for OIRs of 4:1, 1:1, and 1:4 for decreasing RH, were quantified by poke-and-flow and bead-mobility techniques at 293 ± 1 K. Based on the viscosity results, the particles of binary and ternary systems ranged from liquid to semisolid, and even the solid state depending on the RH. Moreover, we compared the measured viscosities of ternary systems to the predicted viscosities with excellent agreement.
Cuiqi Zhang, Zhijun Wu, Jingchuan Chen, Jie Chen, Lizi Tang, Wenfei Zhu, Xiangyu Pei, Shiyi Chen, Ping Tian, Song Guo, Limin Zeng, Min Hu, and Zamin A. Kanji
Atmos. Chem. Phys., 22, 7539–7556, https://doi.org/10.5194/acp-22-7539-2022, https://doi.org/10.5194/acp-22-7539-2022, 2022
Short summary
Short summary
The immersion ice nucleation effectiveness of aerosols from multiple sources in the urban environment remains elusive. In this study, we demonstrate that the immersion ice-nucleating particle (INP) concentration increased dramatically during a dust event in an urban atmosphere. Pollutant aerosols, including inorganic salts formed through secondary transformation (SIA) and black carbon (BC), might not act as effective INPs under mixed-phase cloud conditions.
Haoran Zhang, Nan Li, Keqin Tang, Hong Liao, Chong Shi, Cheng Huang, Hongli Wang, Song Guo, Min Hu, Xinlei Ge, Mindong Chen, Zhenxin Liu, Huan Yu, and Jianlin Hu
Atmos. Chem. Phys., 22, 5495–5514, https://doi.org/10.5194/acp-22-5495-2022, https://doi.org/10.5194/acp-22-5495-2022, 2022
Short summary
Short summary
We developed a new algorithm with low economic/technique costs to identify primary and secondary components of PM2.5. Our model was shown to be reliable by comparison with different observation datasets. We systematically explored the patterns and changes in the secondary PM2.5 pollution in China at large spatial and time scales. We believe that this method is a promising tool for efficiently estimating primary and secondary PM2.5, and has huge potential for future PM mitigation.
Yun Lin, Yuan Wang, Bowen Pan, Jiaxi Hu, Song Guo, Misti Levy Zamora, Pengfei Tian, Qiong Su, Yuemeng Ji, Jiayun Zhao, Mario Gomez-Hernandez, Min Hu, and Renyi Zhang
Atmos. Chem. Phys., 22, 4951–4967, https://doi.org/10.5194/acp-22-4951-2022, https://doi.org/10.5194/acp-22-4951-2022, 2022
Short summary
Short summary
Severe regional haze events, which are characterized by exceedingly high levels of fine particulate matter (PM), occur frequently in many developing countries (such as China and India), with profound implications for human health, weather, and climate. Our work establishes a synthetic view for the dominant regional features during severe haze events, unraveling rapid in situ PM production and inefficient transport, both of which are amplified by atmospheric stagnation.
Gang Zhao, Tianyi Tan, Yishu Zhu, Min Hu, and Chunsheng Zhao
Atmos. Chem. Phys., 21, 18055–18063, https://doi.org/10.5194/acp-21-18055-2021, https://doi.org/10.5194/acp-21-18055-2021, 2021
Short summary
Short summary
In this study, the black carbon (BC) mixing state index (χ) is developed to quantify the dispersion of ambient black carbon aerosol mixing states based on binary systems of BC and other non-black carbon components. We demonstrate that the BC light absorption enhancement increases with χ for the same MR, which indicates that χ can be employed as a factor to constrain the light absorption enhancement of ambient BC.
Zirui Zhang, Wenfei Zhu, Min Hu, Kefan Liu, Hui Wang, Rongzhi Tang, Ruizhe Shen, Ying Yu, Rui Tan, Kai Song, Yuanju Li, Wenbin Zhang, Zhou Zhang, Hongming Xu, Shijin Shuai, Shuangde Li, Yunfa Chen, Jiayun Li, Yuesi Wang, and Song Guo
Atmos. Chem. Phys., 21, 15221–15237, https://doi.org/10.5194/acp-21-15221-2021, https://doi.org/10.5194/acp-21-15221-2021, 2021
Short summary
Short summary
We comprehensively investigated the mass growth potential, oxidation degree, formation pathway, and mass spectra features of typical urban-lifestyle secondary organic aerosols (SOAs) including vehicle SOAs and cooking SOAs. The mass spectra we acquired could provide necessary references to estimate the mass fractions of vehicle and cooking SOAs in the atmosphere, which would greatly decrease the uncertainty in air quality evaluation and health risk assessment in urban areas.
Wenfei Zhu, Song Guo, Zirui Zhang, Hui Wang, Ying Yu, Zheng Chen, Ruizhe Shen, Rui Tan, Kai Song, Kefan Liu, Rongzhi Tang, Yi Liu, Shengrong Lou, Yuanju Li, Wenbin Zhang, Zhou Zhang, Shijin Shuai, Hongming Xu, Shuangde Li, Yunfa Chen, Min Hu, Francesco Canonaco, and Andre S. H. Prévôt
Atmos. Chem. Phys., 21, 15065–15079, https://doi.org/10.5194/acp-21-15065-2021, https://doi.org/10.5194/acp-21-15065-2021, 2021
Short summary
Short summary
The experiments of primary emissions and secondary organic aerosol (SOA) formation from urban lifestyle sources (cooking and vehicles) were conducted. The mass spectral features of primary organic aerosol (POA) and SOA were characterized by using a high-resolution time-of-flight aerosol mass spectrometer. This work, for the first time, establishes the vehicle and cooking SOA source profiles and can be further used as source constraints in the OA source apportionment in the ambient atmosphere.
Huan Song, Keding Lu, Can Ye, Huabin Dong, Shule Li, Shiyi Chen, Zhijun Wu, Mei Zheng, Limin Zeng, Min Hu, and Yuanhang Zhang
Atmos. Chem. Phys., 21, 13713–13727, https://doi.org/10.5194/acp-21-13713-2021, https://doi.org/10.5194/acp-21-13713-2021, 2021
Short summary
Short summary
Secondary sulfate aerosols are an important component of fine particles in severe air pollution events. We calculated the sulfate formation rates via a state-of-the-art multiphase model constrained to the observed values. We showed that transition metals in urban aerosols contribute significantly to sulfate formation during haze periods and thus play an important role in mitigation strategies and public health measures in megacities worldwide.
Yu Wang, Aristeidis Voliotis, Yunqi Shao, Taomou Zong, Xiangxinyue Meng, Mao Du, Dawei Hu, Ying Chen, Zhijun Wu, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 21, 11303–11316, https://doi.org/10.5194/acp-21-11303-2021, https://doi.org/10.5194/acp-21-11303-2021, 2021
Short summary
Short summary
Aerosol phase behaviour plays a profound role in atmospheric physicochemical processes. We designed dedicated chamber experiments to study the phase state of secondary organic aerosol from biogenic and anthropogenic mixed precursors. Our results highlight the key role of the organic–inorganic ratio and relative humidity in phase state, but the sources and organic composition are less important. The result provides solid laboratory evidence for understanding aerosol phase in a complex atmosphere.
Benjamin A. Nault, Duseong S. Jo, Brian C. McDonald, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Jason C. Schroder, James Allan, Donald R. Blake, Manjula R. Canagaratna, Hugh Coe, Matthew M. Coggon, Peter F. DeCarlo, Glenn S. Diskin, Rachel Dunmore, Frank Flocke, Alan Fried, Jessica B. Gilman, Georgios Gkatzelis, Jacqui F. Hamilton, Thomas F. Hanisco, Patrick L. Hayes, Daven K. Henze, Alma Hodzic, James Hopkins, Min Hu, L. Greggory Huey, B. Thomas Jobson, William C. Kuster, Alastair Lewis, Meng Li, Jin Liao, M. Omar Nawaz, Ilana B. Pollack, Jeffrey Peischl, Bernhard Rappenglück, Claire E. Reeves, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Min Shao, Jacob M. Sommers, James Walega, Carsten Warneke, Petter Weibring, Glenn M. Wolfe, Dominique E. Young, Bin Yuan, Qiang Zhang, Joost A. de Gouw, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 11201–11224, https://doi.org/10.5194/acp-21-11201-2021, https://doi.org/10.5194/acp-21-11201-2021, 2021
Short summary
Short summary
Secondary organic aerosol (SOA) is an important aspect of poor air quality for urban regions around the world, where a large fraction of the population lives. However, there is still large uncertainty in predicting SOA in urban regions. Here, we used data from 11 urban campaigns and show that the variability in SOA production in these regions is predictable and is explained by key emissions. These results are used to estimate the premature mortality associated with SOA in urban regions.
Young-Chul Song, Joseph Lilek, Jae Bong Lee, Man Nin Chan, Zhijun Wu, Andreas Zuend, and Mijung Song
Atmos. Chem. Phys., 21, 10215–10228, https://doi.org/10.5194/acp-21-10215-2021, https://doi.org/10.5194/acp-21-10215-2021, 2021
Short summary
Short summary
We report viscosity of binary mixtures of organic material / H2O and inorganic salts / H2O, as well as ternary mixtures of organic material / inorganic salts/ H2O, over the atmospheric relative humidity (RH) range. The viscosity measurements indicate that the studied mixed organic–inorganic particles range in phase state from liquid to semi-solid or even solid across the atmospheric RH range at a temperature of 293 K.
Gang Zhao, Yishu Zhu, Zhijun Wu, Taomou Zong, Jingchuan Chen, Tianyi Tan, Haichao Wang, Xin Fang, Keding Lu, Chunsheng Zhao, and Min Hu
Atmos. Chem. Phys., 21, 9995–10004, https://doi.org/10.5194/acp-21-9995-2021, https://doi.org/10.5194/acp-21-9995-2021, 2021
Short summary
Short summary
New particle formation is thought to contribute half of the global cloud condensation nuclei. We find that the new particle formation is more likely to happen in the upper boundary layer than that at the ground, which can be partially explained by the aerosol–radiation interaction. Our study emphasizes the influence of aerosol–radiation interaction on the NPF.
Tianyi Tan, Min Hu, Zhuofei Du, Gang Zhao, Dongjie Shang, Jing Zheng, Yanhong Qin, Mengren Li, Yusheng Wu, Limin Zeng, Song Guo, and Zhijun Wu
Atmos. Chem. Phys., 21, 8499–8510, https://doi.org/10.5194/acp-21-8499-2021, https://doi.org/10.5194/acp-21-8499-2021, 2021
Short summary
Short summary
Every year in the pre-monsoon season, the black carbon (BC) aerosols originated from biomass burning in southern Asia are easily transported to the Tibetan Plateau (TP) by the convenience of westerly wind. This study reveals that the BC aerosols in the aged biomass burning plumes strongly enhance the total light absorption over the TP, and the aging process during the long-range transport will further strengthen the radiative heating of those BC aerosols.
Laurent Poulain, Benjamin Fahlbusch, Gerald Spindler, Konrad Müller, Dominik van Pinxteren, Zhijun Wu, Yoshiteru Iinuma, Wolfram Birmili, Alfred Wiedensohler, and Hartmut Herrmann
Atmos. Chem. Phys., 21, 3667–3684, https://doi.org/10.5194/acp-21-3667-2021, https://doi.org/10.5194/acp-21-3667-2021, 2021
Short summary
Short summary
We present results from source apportionment analysis on the carbonaceous aerosol particles, including organic aerosol (OA) and equivalent black carbon (eBC), allowing us to distinguish local emissions from long-range transport for OA and eBC sources. By merging online chemical measurements and considering particle number size distribution, the different air masses reaching the sampling place were described and discussed, based on their respective chemical composition and size distribution.
Jingchuan Chen, Zhijun Wu, Jie Chen, Naama Reicher, Xin Fang, Yinon Rudich, and Min Hu
Atmos. Chem. Phys., 21, 3491–3506, https://doi.org/10.5194/acp-21-3491-2021, https://doi.org/10.5194/acp-21-3491-2021, 2021
Short summary
Short summary
Asian mineral dust is a crucial contributor to global ice-nucleating particles (INPs), while its size-resolved information on freezing activity is extremely rare. Here we conducted the first known INP measurements of size-resolved airborne East Asian dust particles. An explicit size dependence of both INP concentration and surface
ice-active-site density was observed. The new parameterizations can be widely applied in models to better characterize and predict ice nucleation activities of dust.
Hoi Ki Lam, Rongshuang Xu, Jack Choczynski, James F. Davies, Dongwan Ham, Mijung Song, Andreas Zuend, Wentao Li, Ying-Lung Steve Tse, and Man Nin Chan
Atmos. Chem. Phys., 21, 2053–2066, https://doi.org/10.5194/acp-21-2053-2021, https://doi.org/10.5194/acp-21-2053-2021, 2021
Short summary
Short summary
This work demonstrates that organic compounds present at or near the surface of aerosols can be subjected to oxidation initiated by gas-phase oxidants, such as hydroxyl radicals (OH). The heterogeneous reactivity is sensitive to their surface concentrations, which are determined by the phase separation behavior. This results of this work emphasize the effects of phase separation and potentially distinct aerosol morphologies on the chemical transformation of atmospheric aerosols.
Christian Mark Garcia Salvador, Rongzhi Tang, Michael Priestley, Linjie Li, Epameinondas Tsiligiannis, Michael Le Breton, Wenfei Zhu, Limin Zeng, Hui Wang, Ying Yu, Min Hu, Song Guo, and Mattias Hallquist
Atmos. Chem. Phys., 21, 1389–1406, https://doi.org/10.5194/acp-21-1389-2021, https://doi.org/10.5194/acp-21-1389-2021, 2021
Short summary
Short summary
High-frequency online measurement of gas- and particle-phase nitro-aromatic compounds (NACs) at a rural site in China, heavily influenced by biomass burning events, enabled the analysis of the production pathway of NACs, including an explanation of strong persistence in the daytime. The contribution of secondary processes was significant, even during the dominant wintertime influence of primary emissions, suggesting the important role of regional secondary chemistry, i.e. photochemical smog.
Chao Peng, Yu Wang, Zhijun Wu, Lanxiadi Chen, Ru-Jin Huang, Weigang Wang, Zhe Wang, Weiwei Hu, Guohua Zhang, Maofa Ge, Min Hu, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 20, 13877–13903, https://doi.org/10.5194/acp-20-13877-2020, https://doi.org/10.5194/acp-20-13877-2020, 2020
Yujue Wang, Min Hu, Nan Xu, Yanhong Qin, Zhijun Wu, Liwu Zeng, Xiaofeng Huang, and Lingyan He
Atmos. Chem. Phys., 20, 13721–13734, https://doi.org/10.5194/acp-20-13721-2020, https://doi.org/10.5194/acp-20-13721-2020, 2020
Short summary
Short summary
Field straw residue burning is a widespread type of biomass burning in Asia, while its emissions are poorly understood. In this study, we designed lab-controlled experiments to comprehensively investigate the emission factors, chemical compositions and light absorption properties of both water-soluble and water-insoluble carbonaceous aerosols emitted from straw burning. The results clearly highlight the significant influences of burning conditions and combustion efficiency on the emissions.
Young-Chul Song, Ariana G. Bé, Scot T. Martin, Franz M. Geiger, Allan K. Bertram, Regan J. Thomson, and Mijung Song
Atmos. Chem. Phys., 20, 11263–11273, https://doi.org/10.5194/acp-20-11263-2020, https://doi.org/10.5194/acp-20-11263-2020, 2020
Short summary
Short summary
We report the liquid–liquid phase separation (LLPS) of organic aerosol consisting of α-pinene- and β-caryophyllene-derived ozonolysis products and commercial organic compounds. As compositional complexity increased from one to two organic species, LLPS occurred over a wider range of average O : C values (increasing from 0.44 to 0.67). These results provide further evidence that LLPS is likely frequent in organic aerosol particles in the troposphere, even in the absence of inorganic salt.
Cited articles
Abbatt, J. P. D., Lee, A. K. Y., and Thornton, J. A.: Quantifying trace gas uptake to tropospheric aerosol: recent advances and remaining challenges, Chem. Soc. Rev, 41, 6555–6581, 2012.
Angell, C. A.: Relaxation in Liquids, Polymers and Plastic Crystals – Strong Fragile Patterns and Problems, J. Non-Cryst. Solids, 131, 13–31, 1991.
Bateman, A. P., Belassein, H., and Martin, S. T.: Impactor Apparatus for the Study of Particle Rebound: Relative Humidity and Capillary Forces, Aerosol Sci. Technol., 48, 42–52, https://doi.org/10.1080/02786826.2013.853866, 2014.
Bateman, A. P., Gong, Z. H., Liu, P. F., Sato, B., Cirino, G., Zhang, Y., Artaxo, P., Bertram, A. K., Manzi, A. O., Rizzo, L. V., Souza, R. A. F., Zaveri, R. A., and Martin, S. T.: Sub-micrometre particulate matter is primarily in liquid form over Amazon rainforest, Nat. Geosci., 9, 34–37, https://doi.org/10.1038/Ngeo2599, 2016.
Bateman, A. P., Gong, Z., Harder, T. H., de Sá, S. S., Wang, B., Castillo, P., China, S., Liu, Y., O'Brien, R. E., Palm, B. B., Shiu, H.-W., Cirino, G. G., Thalman, R., Adachi, K., Alexander, M. L., Artaxo, P., Bertram, A. K., Buseck, P. R., Gilles, M. K., Jimenez, J. L., Laskin, A., Manzi, A. O., Sedlacek, A., Souza, R. A. F., Wang, J., Zaveri, R., and Martin, S. T.: Anthropogenic influences on the physical state of submicron particulate matter over a tropical forest, Atmos. Chem. Phys., 17, 1759–1773, https://doi.org/10.5194/acp-17-1759-2017, 2017.
Berkemeier, T., Steimer, S. S., Krieger, U. K., Peter, T., Pöschl, U., Ammann, M., and Shiraiwa, M.: Ozone uptake on glassy, semi-solid and liquid organic matter and the role of reactive oxygen intermediates in atmospheric aerosol chemistry, Phys. Chem. Chem. Phys., 18, 12662–12674, https://doi.org/10.1039/C6CP00634E, 2016.
Canagaratna, M. R., Jimenez, J. L., Kroll, J. H., Chen, Q., Kessler, S. H., Massoli, P., Hildebrandt Ruiz, L., Fortner, E., Williams, L. R., Wilson, K. R., Surratt, J. D., Donahue, N. M., Jayne, J. T., and Worsnop, D. R.: Elemental ratio measurements of organic compounds using aerosol mass spectrometry: characterization, improved calibration, and implications, Atmos. Chem. Phys., 15, 253–272, https://doi.org/10.5194/acp-15-253-2015, 2015.
Carlton, A. G. and Turpin, B. J.: Particle partitioning potential of organic compounds is highest in the Eastern US and driven by anthropogenic water, Atmos. Chem. Phys., 13, 10203–10214, https://doi.org/10.5194/acp-13-10203-2013, 2013.
Cerully, K. M., Bougiatioti, A., Hite Jr., J. R., Guo, H., Xu, L., Ng, N. L., Weber, R., and Nenes, A.: On the link between hygroscopicity, volatility, and oxidation state of ambient and water-soluble aerosols in the southeastern United States, Atmos. Chem. Phys., 15, 8679–8694, https://doi.org/10.5194/acp-15-8679-2015, 2015.
Chang, R. Y.-W., Slowik, J. G., Shantz, N. C., Vlasenko, A., Liggio, J., Sjostedt, S. J., Leaitch, W. R., and Abbatt, J. P. D.: The hygroscopicity parameter (κ) of ambient organic aerosol at a field site subject to biogenic and anthropogenic influences: relationship to degree of aerosol oxidation, Atmos. Chem. Phys., 10, 5047–5064, https://doi.org/10.5194/acp-10-5047-2010, 2010.
Chen, Y., Wang, Y., Nenes, A., Wild, O., Song, S. J., Hu, D. W., Liu, D. T., He, J. J., Ruiz, L. H., Apte, J. S., Gunthe, S. S., and Liu, P. F.: Ammonium Chloride Associated Aerosol Liquid Water Enhances Haze in Delhi, India br, Environ. Sci. Technol., 56, 7163–7173, https://doi.org/10.1021/acs.est.2c00650, 2022.
Cheng, Y., Zheng, G., Wei, C., Mu, Q., Zheng, B., Wang, Z., Gao, M., Zhang, Q., He, K., Carmichael, G., Pöschl, U., and Su, H.: Reactive nitrogen chemistry in aerosol water as a source of sulfate during haze events in China, Sci. Adv., 2, e1601530, https://doi.org/10.1126/sciadv.1601530, 2016.
Ciobanu, V. G., Marcolli, C., Krieger, U. K., Weers, U., and Peter, T.: Liquid-Liquid Phase Separation in Mixed Organic/Inorganic Aerosol Particles, J. Phys. Chem. A, 113, 10966–10978, 2009.
DeRieux, W.-S. W., Li, Y., Lin, P., Laskin, J., Laskin, A., Bertram, A. K., Nizkorodov, S. A., and Shiraiwa, M.: Predicting the glass transition temperature and viscosity of secondary organic material using molecular composition, Atmos. Chem. Phys., 18, 6331–6351, https://doi.org/10.5194/acp-18-6331-2018, 2018.
Dette, H. P., Qi, M., Schröder, D. C., Godt, A., and Koop, T.: Glass-Forming Properties of 3-Methylbutane-1,2,3-tricarboxylic Acid and Its Mixtures with Water and Pinonic Acid, J. Phys. Chem. A, 118, 7024–7033, https://doi.org/10.1021/jp505910w, 2014.
Duplissy, J., DeCarlo, P. F., Dommen, J., Alfarra, M. R., Metzger, A., Barmpadimos, I., Prevot, A. S. H., Weingartner, E., Tritscher, T., Gysel, M., Aiken, A. C., Jimenez, J. L., Canagaratna, M. R., Worsnop, D. R., Collins, D. R., Tomlinson, J., and Baltensperger, U.: Relating hygroscopicity and composition of organic aerosol particulate matter, Atmos. Chem. Phys., 11, 1155–1165, https://doi.org/10.5194/acp-11-1155-2011, 2011.
El-Sayed, M. M. H., Wang, Y. Q., and Hennigan, C. J.: Direct atmospheric evidence for the irreversible formation of aqueous secondary organic aerosol, Geophys. Res. Lett., 42, 5577–5586, https://doi.org/10.1002/2015gl064556, 2015.
Ervens, B., Turpin, B. J., and Weber, R. J.: Secondary organic aerosol formation in cloud droplets and aqueous particles (aqSOA): a review of laboratory, field and model studies, Atmos. Chem. Phys., 11, 11069–11102, https://doi.org/10.5194/acp-11-11069-2011, 2011.
Fountoukis, C. and Nenes, A.: ISORROPIA II: a computationally efficient thermodynamic equilibrium model for K+–Ca2+–Mg2+–
Galloway, M. M., Chhabra, P. S., Chan, A. W. H., Surratt, J. D., Flagan, R. C., Seinfeld, J. H., and Keutsch, F. N.: Glyoxal uptake on ammonium sulphate seed aerosol: reaction products and reversibility of uptake under dark and irradiated conditions, Atmos. Chem. Phys., 9, 3331–3345, https://doi.org/10.5194/acp-9-3331-2009, 2009.
Gkatzelis, G. I., Papanastasiou, D. K., Karydis, V. A., Hohaus, T., Liu, Y., Schmitt, S. H., Schlag, P., Fuchs, H., Novelli, A., Chen, Q., Cheng, X., Broch, S., Dong, H., Holland, F., Li, X., Liu, Y. H., Ma, X. F., Reimer, D., Rohrer, F., Shao, M., Tan, Z., Taraborrelli, D., Tillmann, R., Wang, H. C., Wang, Y., Wu, Y. S., Wu, Z. J., Zeng, L. M., Zheng, J., Hu, M., Lu, K. D., Hofzumahaus, A., Zhang, Y. H., Wahner, A., and Kiendler-Scharr, A.: Uptake of Water-soluble Gas-phase Oxidation Products Drives Organic Particulate Pollution in Beijing, Geophys. Res. Lett., 48, e2020GL091351, https://doi.org/10.1029/2020GL091351, 2021.
Gunthe, S. S., Rose, D., Su, H., Garland, R. M., Achtert, P., Nowak, A., Wiedensohler, A., Kuwata, M., Takegawa, N., Kondo, Y., Hu, M., Shao, M., Zhu, T., Andreae, M. O., and Pöschl, U.: Cloud condensation nuclei (CCN) from fresh and aged air pollution in the megacity region of Beijing, Atmos. Chem. Phys., 11, 11023–11039, https://doi.org/10.5194/acp-11-11023-2011, 2011.
Guo, H., Xu, L., Bougiatioti, A., Cerully, K. M., Capps, S. L., Hite Jr., J. R., Carlton, A. G., Lee, S.-H., Bergin, M. H., Ng, N. L., Nenes, A., and Weber, R. J.: Fine-particle water and pH in the southeastern United States, Atmos. Chem. Phys., 15, 5211–5228, https://doi.org/10.5194/acp-15-5211-2015, 2015.
Gysel, M., Crosier, J., Topping, D. O., Whitehead, J. D., Bower, K. N., Cubison, M. J., Williams, P. I., Flynn, M. J., McFiggans, G. B., and Coe, H.: Closure study between chemical composition and hygroscopic growth of aerosol particles during TORCH2, Atmos. Chem. Phys., 7, 6131–6144, https://doi.org/10.5194/acp-7-6131-2007, 2007.
Herrmann, H., Schaefer, T., Tilgner, A., Styler, S. A., Weller, C., Teich, M., and Otto, T.: Tropospheric Aqueous-Phase Chemistry: Kinetics, Mechanisms, and Its Coupling to a Changing Gas Phase, Chem. Rev., 115, 4259–4334, https://doi.org/10.1021/cr500447k, 2015.
Hodas, N., Sullivan, A. P., Skog, K., Keutsch, F. N., Collett, J. L., Decesari, S., Facchini, M. C., Carlton, A. G., Laaksonen, A., and Turpin, B. J.: Aerosol Liquid Water Driven by Anthropogenic Nitrate: Implications for Lifetimes of Water-Soluble Organic Gases and Potential for Secondary Organic Aerosol Formation, Environ. Sci. Technol., 48, 11127–11136, 2014.
Hodas, N., Zuend, A., Mui, W., Flagan, R. C., and Seinfeld, J. H.: Influence of particle-phase state on the hygroscopic behavior of mixed organic–inorganic aerosols, Atmos. Chem. Phys., 15, 5027–5045, https://doi.org/10.5194/acp-15-5027-2015, 2015.
Hu, S. Y., Zhao, G., Tan, T. Y., Li, C. C., Zong, T. M., Xu, N., Zhu, W. F., and Hu, M.: Current challenges of improving visibility due to increasing nitrate fraction in PM2.5 during the haze days in Beijing, China, Environ. Pollut., 290, 118032, https://doi.org/10.1016/j.envpol.2021.118032, 2021.
Iinuma, Y., Muller, C., Berndt, T., Boge, O., Claeys, M., and Herrmann, H.: Evidence for the existence of organosulfates from beta-pinene ozonolysis in ambient secondary organic aerosol, Environ. Sci. Technol., 41, 6678–6683, https://doi.org/10.1021/es070938t, 2007.
Jia, L., Xu, Y., and Duan, M.: Explosive formation of secondary organic aerosol due to aerosol-fog interactions, Sci. Total Environ., 866, 161338, https://doi.org/10.1016/j.scitotenv.2022.161338, 2023.
Jin, X., Wang, Y., Li, Z., Zhang, F., Xu, W., Sun, Y., Fan, X., Chen, G., Wu, H., Ren, J., Wang, Q., and Cribb, M.: Significant contribution of organics to aerosol liquid water content in winter in Beijing, China, Atmos. Chem. Phys., 20, 901–914, https://doi.org/10.5194/acp-20-901-2020, 2020.
Knopf, D. A. and Alpert, P. A.: Atmospheric ice nucleation, Nat. Rev. Phys., 5, 203–217, https://doi.org/10.1038/s42254-023-00570-7, 2023.
Koop, T., Bookhold, J., Shiraiwa, M., and Pöschl, U.: Glass transition and phase state of organic compounds: dependency on molecular properties and implications for secondary organic aerosols in the atmosphere, Phys. Chem. Chem. Phys., 13, 19238–19255, https://doi.org/10.1039/c1cp22617g, 2011.
Kuang, Y., He, Y., Xu, W., Zhao, P., Cheng, Y., Zhao, G., Tao, J., Ma, N., Su, H., Zhang, Y., Sun, J., Cheng, P., Yang, W., Zhang, S., Wu, C., Sun, Y., and Zhao, C.: Distinct diurnal variation in organic aerosol hygroscopicity and its relationship with oxygenated organic aerosol, Atmos. Chem. Phys., 20, 865–880, https://doi.org/10.5194/acp-20-865-2020, 2020.
Lei, L., Zhou, W., Chen, C., He, Y., Li, Z. J., Sun, J. X., Tang, X., Fu, P. Q., Wang, Z. F., and Sun, Y. L.: Long-term characterization of aerosol chemistry in cold season from 2013 to 2020 in Beijing, China, Environ. Pollut., 268, 115952, https://doi.org/10.1016/j.envpol.2020.115952, 2021.
Lelieveld, J., Evans, J. S., Fnais, M., Giannadaki, D., and Pozzer, A.: The contribution of outdoor air pollution sources to premature mortality on a global scale, Nature, 525, 367–371, https://doi.org/10.1038/nature15371, 2015.
Li, X., Song, S., Zhou, W., Hao, J., Worsnop, D. R., and Jiang, J.: Interactions between aerosol organic components and liquid water content during haze episodes in Beijing, Atmos. Chem. Phys., 19, 12163–12174, https://doi.org/10.5194/acp-19-12163-2019, 2019.
Li, Y. and Shiraiwa, M.: Timescales of secondary organic aerosols to reach equilibrium at various temperatures and relative humidities, Atmos. Chem. Phys., 19, 5959–5971, https://doi.org/10.5194/acp-19-5959-2019, 2019.
Li, Y. J., Sun, Y., Zhang, Q., Li, X., Li, M., Zhou, Z., and Chan, C. K.: Real-time chemical characterization of atmospheric particulate matter in China: A review, Atmos. Environ., 158, 270–304, https://doi.org/10.1016/j.atmosenv.2017.02.027, 2017.
Li, Z., Smith, K. A., and Cappa, C. D.: Influence of relative humidity on the heterogeneous oxidation of secondary organic aerosol, Atmos. Chem. Phys., 18, 14585–14608, https://doi.org/10.5194/acp-18-14585-2018, 2018.
Lim, Y. B., Tan, Y., Perri, M. J., Seitzinger, S. P., and Turpin, B. J.: Aqueous chemistry and its role in secondary organic aerosol (SOA) formation, Atmos. Chem. Phys., 10, 10521–10539, https://doi.org/10.5194/acp-10-10521-2010, 2010.
Lim, Y. B., Tan, Y., and Turpin, B. J.: Chemical insights, explicit chemistry, and yields of secondary organic aerosol from OH radical oxidation of methylglyoxal and glyoxal in the aqueous phase, Atmos. Chem. Phys., 13, 8651–8667, https://doi.org/10.5194/acp-13-8651-2013, 2013.
Liu, P., Song, M., Zhao, T., Gunthe, S. S., Ham, S., He, Y., Qin, Y. M., Gong, Z., Amorim, J. C., Bertram, A. K., and Martin, S. T.: Resolving the mechanisms of hygroscopic growth and cloud condensation nuclei activity for organic particulate matter, Nat. Commun., 9, 4076, https://doi.org/10.1038/s41467-018-06622-2, 2018.
Liu, T., Clegg, S. L., and Abbatt, J. P. D.: Fast oxidation of sulfur dioxide by hydrogen peroxide in deliquesced aerosol particles, P. Natl. Acad. Sci. USA, 117, 1354–1359, https://doi.org/10.1073/pnas.1916401117, 2020.
Liu, Y., Wu, Z., Wang, Y., Xiao, Y., Gu, F., Zheng, J., Tan, T., Shang, D., Wu, Y., Zeng, L., Hu, M., Bateman, A. P., and Martin, S. T.: Submicrometer Particles Are in the Liquid State during Heavy Haze Episodes in the Urban Atmosphere of Beijing, China, Environ. Sci. Technol. Lett., 4, 427–432, https://doi.org/10.1021/acs.estlett.7b00352, 2017.
Liu, Y., Wu, Z., Huang, X., Shen, H., Bai, Y., Qiao, K., Meng, X., Hu, W., Tang, M., and He, L.: Aerosol Phase State and Its Link to Chemical Composition and Liquid Water Content in a Subtropical Coastal Megacity, Environ. Sci. Technol., 53, 5027–5033, https://doi.org/10.1021/acs.est.9b01196, 2019.
Liu, Y. C., Meng, X. X., Wu, Z. J., Huang, D. D., Wang, H. L., Chen, J., Chen, J. C., Zong, T. M., Fang, X., Tan, T. Y., Zhao, G., Chen, S. Y., Zeng, L. W., Guo, S., Huang, X. F., He, L. Y., Zeng, L. M., and Hu, M.: The particle phase state during the biomass burning events, Sci. Total Environ., 792, 148035, https://doi.org/10.1016/j.scitotenv.2021.148035, 2021.
Ma, W., Zheng, F. X., Zhang, Y. S., Chen, X., Zhan, J. L., Hua, C. J., Song, B. Y., Wang, Z. C., Xie, J. L., Yan, C., Kulmala, M., and Liu, Y. C.: Weakened Gas-to-Particle Partitioning of Oxygenated Organic Molecules in Liquified Aerosol Particles, Environ. Sci. Technol. Lett., 9, 837–843, https://doi.org/10.1021/acs.estlett.2c00556, 2022.
Marshall, F. H., Berkemeier, T., Shiraiwa, M., Nandy, L., Ohm, P. B., Dutcher, C. S., and Reid, J. P.: Influence of particle viscosity on mass transfer and heterogeneous ozonolysis kinetics in aqueous-sucrose-maleic acid aerosol, Phys. Chem. Chem. Phys., 20, 15560–15573, 2018.
Matthew, B. M., Middlebrook, A. M., and Onasch, T. B.: Collection efficiencies in an Aerodyne Aerosol Mass Spectrometer as a function of particle phase for laboratory generated aerosols, Aerosol Sci. Technol., 42, 884–898, https://doi.org/10.1080/02786820802356797, 2008.
Meng, X. X. Y., Wu, Z. J., Guo, S., Wang, H., Liu, K. F., Zong, T. M., Liu, Y. C., Zhang, W. B., Zhang, Z., Chen, S. Y., Zeng, L. M., Hallquist, M., Shuai, S. J., and Hu, M.: Humidity-Dependent Phase State of Gasoline Vehicle Emission-Related Aerosols, Environ. Sci. Technol., 55, 832–841, 2021.
Mikhailov, E., Vlasenko, S., Martin, S. T., Koop, T., and Pöschl, U.: Amorphous and crystalline aerosol particles interacting with water vapor: conceptual framework and experimental evidence for restructuring, phase transitions and kinetic limitations, Atmos. Chem. Phys., 9, 9491–9522, https://doi.org/10.5194/acp-9-9491-2009, 2009.
Mu, Q., Shiraiwa, M., Octaviani, M., Ma, N., Ding, A. J., Su, H., Lammel, G., Poschl, U., and Cheng, Y. F.: Temperature effect on phase state and reactivity controls atmospheric multiphase chemistry and transport of PAHs, Sci. Adv., 4, eaap7314, https://doi.org/10.1126/sciadv.aap7314, 2018.
Murray, B. J., Wilson, T. W., Dobbie, S., Cui, Z. Q., Al-Jumur, S. M. R. K., Mohler, O., Schnaiter, M., Wagner, R., Benz, S., Niemand, M., Saathoff, H., Ebert, V., Wagner, S., and Karcher, B.: Heterogeneous nucleation of ice particles on glassy aerosols under cirrus conditions, Nat. Geosci., 3, 233–237, 2010.
Ng, N. L., Canagaratna, M. R., Zhang, Q., Jimenez, J. L., Tian, J., Ulbrich, I. M., Kroll, J. H., Docherty, K. S., Chhabra, P. S., Bahreini, R., Murphy, S. M., Seinfeld, J. H., Hildebrandt, L., Donahue, N. M., DeCarlo, P. F., Lanz, V. A., Prévôt, A. S. H., Dinar, E., Rudich, Y., and Worsnop, D. R.: Organic aerosol components observed in Northern Hemispheric datasets from Aerosol Mass Spectrometry, Atmos. Chem. Phys., 10, 4625–4641, https://doi.org/10.5194/acp-10-4625-2010, 2010.
Ng, N. L., Herndon, S. C., Trimborn, A., Canagaratna, M. R., Croteau, P. L., Onasch, T. B., Sueper, D., Worsnop, D. R., Zhang, Q., Sun, Y. L., and Jayne, J. T.: An Aerosol Chemical Speciation Monitor (ACSM) for Routine Monitoring of the Composition and Mass Concentrations of Ambient Aerosol, Aerosol Sci. Technol., 45, 780–794, https://doi.org/10.1080/02786826.2011.560211, 2011.
Nguyen, T. K. V., Zhang, Q., Jimenez, J. L., Pike, M., and Carlton, A. G.: Liquid Water: Ubiquitous Contributor to Aerosol Mass, Environ. Sci. Technol. Lett., 3, 257–263, 2016.
Pajunoja, A., Hu, W., Leong, Y. J., Taylor, N. F., Miettinen, P., Palm, B. B., Mikkonen, S., Collins, D. R., Jimenez, J. L., and Virtanen, A.: Phase state of ambient aerosol linked with water uptake and chemical aging in the southeastern US, Atmos. Chem. Phys., 16, 11163–11176, https://doi.org/10.5194/acp-16-11163-2016, 2016.
Peckhaus, A., Grass, S., Treuel, L., and Zellner, R.: Deliquescence and Efflorescence Behavior of Ternary Inorganic/Organic/Water Aerosol Particles, J. Phys. Chem. A, 116, 6199–6210, https://doi.org/10.1021/jp211522t, 2012.
Peng, C., Chen, L. X. D., and Tang, M. J.: A database for deliquescence and efflorescence relative humidities of compounds with atmospheric relevance, Fund. Res.-China, 2, 578–587, https://doi.org/10.1016/j.fmre.2021.11.021, 2022.
Petters, M. D. and Kreidenweis, S. M.: A single parameter representation of hygroscopic growth and cloud condensation nucleus activity, Atmos. Chem. Phys., 7, 1961–1971, https://doi.org/10.5194/acp-7-1961-2007, 2007.
Petters, S. S., Kreidenweis, S. M., Grieshop, A. P., Ziemann, P. J., and Petters, M. D.: Temperature- and Humidity-Dependent Phase States of Secondary Organic Aerosols, Geophys. Res. Lett., 46, 1005–1013, https://doi.org/10.1029/2018GL080563, 2019.
Pöschl, U.: Atmospheric Aerosols: Composition, Transformation, Climate and Health Effects, Angew. Chem. Int. Edit., 44, 7520–7540, https://doi.org/10.1002/anie.200501122, 2005.
Ravishankara, A. R.: Heterogeneous and multiphase chemistry in the troposphere, Science, 276, 1058–1065, 1997.
Rothfuss, N. E. and Petters, M. D.: Influence of Functional Groups on the Viscosity of Organic Aerosol, Environ. Sci. Technol., 51, 271–279, https://doi.org/10.1021/acs.est.6b04478, 2017.
Saukko, E., Lambe, A. T., Massoli, P., Koop, T., Wright, J. P., Croasdale, D. R., Pedernera, D. A., Onasch, T. B., Laaksonen, A., Davidovits, P., Worsnop, D. R., and Virtanen, A.: Humidity-dependent phase state of SOA particles from biogenic and anthropogenic precursors, Atmos. Chem. Phys., 12, 7517–7529, https://doi.org/10.5194/acp-12-7517-2012, 2012.
Seinfeld, J. H. and Pandis, S. N.: Atmospheric Chemistry and Physics: From Air Pollution to Climate Change, Wiley, ISBN 978-0471720188, 2006.
Seinfeld, J. H., Bretherton, C., Carslaw, K. S., Coe, H., DeMott, P. J., Dunlea, E. J., Feingold, G., Ghan, S., Guenther, A. B., Kahn, R., Kraucunas, I., Kreidenweis, S. M., Molina, M. J., Nenes, A., Penner, J. E., Prather, K. A., Ramanathan, V., Ramaswamy, V., Rasch, P. J., Ravishankara, A. R., Rosenfeld, D., Stephens, G., and Wood, R.: Improving our fundamental understanding of the role of aerosol-cloud interactions in the climate system, P. Natl. Acad. Sci. USA, 113, 5781–5790, https://doi.org/10.1073/pnas.1514043113, 2016.
Shen, H., Chen, Z., Li, H., Qian, X., Qin, X., and Shi, W.: Gas-Particle Partitioning of Carbonyl Compounds in the Ambient Atmosphere, Environ. Sci. Technol., 52, 10997–11006, https://doi.org/10.1021/acs.est.8b01882, 2018.
Shiraiwa, M., Ammann, M., Koop, T., and Pöschl, U.: Gas uptake and chemical aging of semisolid organic aerosol particles, P. Natl. Acad. Sci. USA, 108, 11003–11008, https://doi.org/10.1073/pnas.1103045108, 2011.
Shiraiwa, M., Zuend, A., Bertram, A. K., and Seinfeld, J. H.: Gas-particle partitioning of atmospheric aerosols: interplay of physical state, non-ideal mixing and morphology, Phys. Chem. Chem. Phys., 15, 11441–11453, 2013.
Shiraiwa, M., Li, Y., Tsimpidi, A. P., Karydis, V. A., Berkemeier, T., Pandis, S. N., Lelieveld, J., Koop, T., and Pöschl, U.: Global distribution of particle phase state in atmospheric secondary organic aerosols, Nat. Commun., 8, 15002, https://doi.org/10.1038/ncomms15002, 2017.
Song, M., Jeong, R., Kim, D., Qiu, Y., Meng, X., Wu, Z., Zuend, A., Ha, Y., Kim, C., Kim, H., Gaikwad, S., Jang, K.-S., Lee, J. Y., and Ahn, J.: Comparison of Phase States of PM2.5 over Megacities, Seoul and Beijing, and Their Implications on Particle Size Distribution, Environ. Sci. Technol., 56, 17581–17590, https://doi.org/10.1021/acs.est.2c06377, 2022.
Song, M. J., Marcolli, C., Krieger, U. K., Lienhard, D. M., and Peter, T.: Morphologies of mixed organic/inorganic/aqueous aerosol droplets, Faraday Discuss., 165, 289–316, 2013.
Sun, Y. L., Wang, Z. F., Fu, P. Q., Yang, T., Jiang, Q., Dong, H. B., Li, J., and Jia, J. J.: Aerosol composition, sources and processes during wintertime in Beijing, China, Atmos. Chem. Phys., 13, 4577–4592, https://doi.org/10.5194/acp-13-4577-2013, 2013.
Sun, Y., Du, W., Wang, Q., Zhang, Q., Chen, C., Chen, Y., Chen, Z., Fu, P., Wang, Z., Gao, Z., and Worsnop, D. R.: Real-Time Characterization of Aerosol Particle Composition above the Urban Canopy in Beijing: Insights into the Interactions between the Atmospheric Boundary Layer and Aerosol Chemistry, Environ. Sci. Technol., 49, 11340–11347, https://doi.org/10.1021/acs.est.5b02373, 2015.
Surratt, J. D., Kroll, J. H., Kleindienst, T. E., Edney, E. O., Claeys, M., Sorooshian, A., Ng, N. L., Offenberg, J. H., Lewandowski, M., Jaoui, M., Flagan, R. C., and Seinfeld, J. H.: Evidence for organosulfates in secondary organic aerosol, Environ. Sci. Technol., 41, 517–527, https://doi.org/10.1021/es062081q, 2007.
Tang, M. J., Cox, R. A., and Kalberer, M.: Compilation and evaluation of gas phase diffusion coefficients of reactive trace gases in the atmosphere: volume 1. Inorganic compounds, Atmos. Chem. Phys., 14, 9233–9247, https://doi.org/10.5194/acp-14-9233-2014, 2014.
Tillmann, R., Hallquist, M., Jonsson, Å. M., Kiendler-Scharr, A., Saathoff, H., Iinuma, Y., and Mentel, Th. F.: Influence of relative humidity and temperature on the production of pinonaldehyde and OH radicals from the ozonolysis of α-pinene, Atmos. Chem. Phys., 10, 7057–7072, https://doi.org/10.5194/acp-10-7057-2010, 2010.
Ushijima, S. B., Huynh, E., Davis, R. D., and Tolbert, M. A.: Seeded Crystal Growth of Internally Mixed Organic-Inorganic Aerosols: Impact of Organic Phase State, J. Phys. Chem. A, 125, 8668–8679, https://doi.org/10.1021/acs.jpca.1c04471, 2021.
Wang, H., Chen, X., Lu, K., Tan, Z., Ma, X., Wu, Z., Li, X., Liu, Y., Shang, D., Wu, Y., Zeng, L., Hu, M., Schmitt, S., Kiendler-Scharr, A., Wahner, A., and Zhang, Y.: Wintertime N2O5 uptake coefficients over the North China Plain, Sci. Bull., 65, 765–774, https://doi.org/10.1016/j.scib.2020.02.006, 2020.
Wang, J. F., Ye, J. H., Zhang, Q., Zhao, J., Wu, Y. Z., Li, J. Y., Liu, D. T., Li, W. J., Zhang, Y. G., Wu, C., Xie, C. H., Qin, Y. M., Lei, Y. L., Huang, X. P., Guo, J. P., Liu, P. F., Fu, P. Q., Li, Y. J., Lee, H. C., Choi, H., Zhang, J., Liao, H., Chen, M. D., Sun, Y. L., Ge, X. L., Martin, S. T., and Jacob, D. J.: Aqueous production of secondary organic aerosol from fossil-fuel emissions in winter Beijing haze, P. Natl. Acad. Sci. USA, 118, e2022179118, https://doi.org/10.1073/pnas.2022179118, 2021.
Wang, Y., Chen, Y., Wu, Z., Shang, D., Bian, Y., Du, Z., Schmitt, S. H., Su, R., Gkatzelis, G. I., Schlag, P., Hohaus, T., Voliotis, A., Lu, K., Zeng, L., Zhao, C., Alfarra, M. R., McFiggans, G., Wiedensohler, A., Kiendler-Scharr, A., Zhang, Y., and Hu, M.: Mutual promotion between aerosol particle liquid water and particulate nitrate enhancement leads to severe nitrate-dominated particulate matter pollution and low visibility, Atmos. Chem. Phys., 20, 2161–2175, https://doi.org/10.5194/acp-20-2161-2020, 2020a.
Wang, Y., Hu, M., Wang, Y.-C., Li, X., Fang, X., Tang, R., Lu, S., Wu, Y., Guo, S., Wu, Z., Hallquist, M., and Yu, J. Z.: Comparative Study of Particulate Organosulfates in Contrasting Atmospheric Environments: Field Evidence for the Significant Influence of Anthropogenic Sulfate and NOx, Environ. Sci. Technol. Lett., 7, 787–794, https://doi.org/10.1021/acs.estlett.0c00550, 2020b.
Wang, Y., Li, Z., Wang, Q., Jin, X., Yan, P., Cribb, M., Li, Y., Yuan, C., Wu, H., Wu, T., Ren, R., and Cai, Z.: Enhancement of secondary aerosol formation by reduced anthropogenic emissions during Spring Festival 2019 and enlightenment for regional PM2.5 control in Beijing, Atmos. Chem. Phys., 21, 915–926, https://doi.org/10.5194/acp-21-915-2021, 2021.
Williams, B. J., Goldstein, A. H., Kreisberg, N. M., and Hering, S. V.: In situ measurements of gas/particle-phase transitions for atmospheric semivolatile organic compounds, P. Natl. Acad. Sci. USA, 107, 6676–6681, https://doi.org/10.1073/pnas.0911858107, 2010.
Wu, Z. J., Zheng, J., Shang, D. J., Du, Z. F., Wu, Y. S., Zeng, L. M., Wiedensohler, A., and Hu, M.: Particle hygroscopicity and its link to chemical composition in the urban atmosphere of Beijing, China, during summertime, Atmos. Chem. Phys., 16, 1123–1138, https://doi.org/10.5194/acp-16-1123-2016, 2016.
Wu, Z. J., Wang, Y., Tan, T. Y., Zhu, Y. S., Li, M. R., Shang, D. J., Wang, H. C., Lu, K. D., Guo, S., Zeng, L. M., and Zhang, Y. H.: Aerosol Liquid Water Driven by Anthropogenic Inorganic Salts: Implying Its Key Role in Haze Formation over the North China Plain, Environ. Sci. Technol. Lett., 5, 160–166, 2018.
Xu, W. Q., Han, T. T., Du, W., Wang, Q. Q., Chen, C., Zhao, J., Zhang, Y. J., Li, J., Fu, P. Q., Wang, Z. F., Worsnop, D. R., and Sun, Y. L.: Effects of Aqueous-Phase and Photochemical Processing on Secondary Organic Aerosol Formation and Evolution in Beijing, China, Environ. Sci. Technol., 51, 762–770, https://doi.org/10.1021/acs.est.6b04498, 2017.
Zhang, Q., Jimenez, J. L., Canagaratna, M. R., Ulbrich, I. M., Ng, N. L., Worsnop, D. R., and Sun, Y.: Understanding atmospheric organic aerosols via factor analysis of aerosol mass spectrometry: a review, Anal. Bioanal. Chem., 401, 3045–3067, https://doi.org/10.1007/s00216-011-5355-y, 2011.
Zhang, Y., Tang, L., Croteau, P. L., Favez, O., Sun, Y., Canagaratna, M. R., Wang, Z., Couvidat, F., Albinet, A., Zhang, H., Sciare, J., Prévôt, A. S. H., Jayne, J. T., and Worsnop, D. R.: Field characterization of the PM2.5 Aerosol Chemical Speciation Monitor: insights into the composition, sources, and processes of fine particles in eastern China, Atmos. Chem. Phys., 17, 14501–14517, https://doi.org/10.5194/acp-17-14501-2017, 2017.
Zhang, Y., Chen, Y. Z., Lambe, A. T., Olson, N. E., Lei, Z. Y., Craig, R. L., Zhang, Z. F., Gold, A., Onasch, T. B., Jayne, J. T., Worsnop, D. R., Gaston, C. J., Thornton, J. A., Vizuete, W., Ault, A. P., and Surratt, J. D.: Effect of the Aerosol-Phase State on Secondary Organic Aerosol Formation from the Reactive Uptake of Isoprene-Derived Epoxydiols (IEPDX), Environ. Sci. Technol. Lett., 5, 167–174, 2018.
Zhao, Z., Xu, Q., Yang, X., and Zhang, H.: Heterogeneous Ozonolysis of Endocyclic Unsaturated Organic Aerosol Proxies: Implications for Criegee Intermediate Dynamics and Later-Generation Reactions, ACS Earth Space Chem., 3, 344–356, https://doi.org/10.1021/acsearthspacechem.8b00177, 2019.
Zheng, B., Zhang, Q., Zhang, Y., He, K. B., Wang, K., Zheng, G. J., Duan, F. K., Ma, Y. L., and Kimoto, T.: Heterogeneous chemistry: a mechanism missing in current models to explain secondary inorganic aerosol formation during the January 2013 haze episode in North China, Atmos. Chem. Phys., 15, 2031–2049, https://doi.org/10.5194/acp-15-2031-2015, 2015.
Zheng, Y., Chen, Q., Cheng, X., Mohr, C., Cai, J., Huang, W., Shrivastava, M., Ye, P., Fu, P., Shi, X., Ge, Y., Liao, K., Miao, R., Qiu, X., Koenig, T. K., and Chen, S.: Precursors and Pathways Leading to Enhanced Secondary Organic Aerosol Formation during Severe Haze Episodes, Environ. Sci. Technol., 55, 15680–15693, https://doi.org/10.1021/acs.est.1c04255, 2021.
Zheng, Y., Miao, R. Q., Zhang, Q., Li, Y. W., Cheng, X., Liao, K. R., Koenig, T. K., Ge, Y. L., Tang, L. Z., Shang, D. J., Hu, M., Chen, S. Y., and Chen, Q.: Secondary Formation of Submicron and Supermicron Organic and Inorganic Aerosols in a Highly Polluted Urban Area, J. Geophys. Res.-Atmos., 128, e2022JD037865, https://doi.org/10.1029/2022jd037865, 2023.
Short summary
Our study revealed that particles predominantly exist in a semi-solid or solid state during clean winter days with RH below 30 %. However, a non-liquid to a liquid phase transition occurred when the aerosol liquid water (ALW) mass fraction surpassed 15 % (dry mass) at transition RH thresholds ranging from 40 % to 60 %. We also provide insights into the increasingly important roles of particle phase state variation and ALW in secondary particulate growth during haze formation in Beijing, China.
Our study revealed that particles predominantly exist in a semi-solid or solid state during...
Altmetrics
Final-revised paper
Preprint