Articles | Volume 21, issue 14
https://doi.org/10.5194/acp-21-11303-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-21-11303-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Phase state of secondary organic aerosol in chamber photo-oxidation of mixed precursors
Centre for Atmospheric Science, Department of Earth and Environmental Sciences, The University of Manchester, Manchester M13 9PL, UK
Aristeidis Voliotis
Centre for Atmospheric Science, Department of Earth and Environmental Sciences, The University of Manchester, Manchester M13 9PL, UK
Yunqi Shao
Centre for Atmospheric Science, Department of Earth and Environmental Sciences, The University of Manchester, Manchester M13 9PL, UK
Taomou Zong
State Key Joint Laboratory of Environmental Simulation and Pollution Control, International Joint Laboratory for Regional Pollution Control, Ministry of Education (IJRC), College of Environmental Sciences and
Engineering, Peking University, Beijing 100871, China
Xiangxinyue Meng
State Key Joint Laboratory of Environmental Simulation and Pollution Control, International Joint Laboratory for Regional Pollution Control, Ministry of Education (IJRC), College of Environmental Sciences and
Engineering, Peking University, Beijing 100871, China
Centre for Atmospheric Science, Department of Earth and Environmental Sciences, The University of Manchester, Manchester M13 9PL, UK
Dawei Hu
Centre for Atmospheric Science, Department of Earth and Environmental Sciences, The University of Manchester, Manchester M13 9PL, UK
Ying Chen
Lancaster Environment Centre, Lancaster University, Lancaster LA1 4YQ, UK
currently at: Exeter Climate Systems, University of Exeter, Exeter
EX4 4QE, UK
Zhijun Wu
State Key Joint Laboratory of Environmental Simulation and Pollution Control, International Joint Laboratory for Regional Pollution Control, Ministry of Education (IJRC), College of Environmental Sciences and
Engineering, Peking University, Beijing 100871, China
International Joint Laboratory for Regional Pollution Control, 52425 Jülich, Germany, and Beijing 100871, China
Collaborative Innovation Center of Atmospheric Environment and
Equipment Technology, Nanjing University of Information Science and Technology, Nanjing 210044, China
M. Rami Alfarra
Centre for Atmospheric Science, Department of Earth and Environmental Sciences, The University of Manchester, Manchester M13 9PL, UK
National Centre for Atmospheric Science, School of Earth and
Environmental Sciences, The University of Manchester, Manchester M13 9PL, UK
Qatar Environment and Energy Research Institute, Hamad Bin Khalifa University, Doha, Qatar
Gordon McFiggans
CORRESPONDING AUTHOR
Centre for Atmospheric Science, Department of Earth and Environmental Sciences, The University of Manchester, Manchester M13 9PL, UK
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This study analysed the average carbon oxidation state (OSc) during secondary organic aerosol formation from mixed volatile organic compounds (VOCs) using three mass spectrometry techniques. Notable discrepancies in OSc were observed across the techniques, with FIGAERO-CIMS keep reporting higher values. The results also shown that OSc in mixed VOC systems is influenced not only by products from individual precursors but also by unique compounds formed through interactions between VOC products.
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Atmos. Meas. Tech., 15, 539–559, https://doi.org/10.5194/amt-15-539-2022, https://doi.org/10.5194/amt-15-539-2022, 2022
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Atmos. Chem. Phys., 21, 14251–14273, https://doi.org/10.5194/acp-21-14251-2021, https://doi.org/10.5194/acp-21-14251-2021, 2021
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Secondary organic aerosol (SOA) formation from mixtures of volatile precursors can be affected by the molecular interactions of the products. Composition and volatility measurements of SOA formed from mixtures of anthropogenic and biogenic precursors reveal processes that can increase or decrease the SOA volatility. The unique products of the mixture were more oxygenated and less volatile than those from either precursor. Analytical context is provided to explore the SOA volatility in mixtures.
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Xiangxinyue Meng, Zhijun Wu, Jingchuan Chen, Yanting Qiu, Taomou Zong, Mijung Song, Jiyi Lee, and Min Hu
Atmos. Chem. Phys., 24, 2399–2414, https://doi.org/10.5194/acp-24-2399-2024, https://doi.org/10.5194/acp-24-2399-2024, 2024
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George Jordan, Florent Malavelle, Ying Chen, Amy Peace, Eliza Duncan, Daniel G. Partridge, Paul Kim, Duncan Watson-Parris, Toshihiko Takemura, David Neubauer, Gunnar Myhre, Ragnhild Skeie, Anton Laakso, and James Haywood
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Ailish M. Graham, Richard J. Pope, Martyn P. Chipperfield, Sandip S. Dhomse, Matilda Pimlott, Wuhu Feng, Vikas Singh, Ying Chen, Oliver Wild, Ranjeet Sokhi, and Gufran Beig
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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
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Chenwei Fang, Jim M. Haywood, Ju Liang, Ben T. Johnson, Ying Chen, and Bin Zhu
Atmos. Chem. Phys., 23, 8341–8368, https://doi.org/10.5194/acp-23-8341-2023, https://doi.org/10.5194/acp-23-8341-2023, 2023
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The responses of Asian summer monsoon duration and intensity to air pollution mitigation are identified given the net-zero future. We show that reducing scattering aerosols makes the rainy season longer and stronger across South Asia and East Asia but that absorbing aerosol reduction has the opposite effect. Our results hint at distinct monsoon responses to emission controls that target different aerosols.
Ernesto Reyes-Villegas, Douglas Lowe, Jill S. Johnson, Kenneth S. Carslaw, Eoghan Darbyshire, Michael Flynn, James D. Allan, Hugh Coe, Ying Chen, Oliver Wild, Scott Archer-Nicholls, Alex Archibald, Siddhartha Singh, Manish Shrivastava, Rahul A. Zaveri, Vikas Singh, Gufran Beig, Ranjeet Sokhi, and Gordon McFiggans
Atmos. Chem. Phys., 23, 5763–5782, https://doi.org/10.5194/acp-23-5763-2023, https://doi.org/10.5194/acp-23-5763-2023, 2023
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Organic aerosols (OAs), their sources and their processes remain poorly understood. The volatility basis set (VBS) approach, implemented in air quality models such as WRF-Chem, can be a useful tool to describe primary OA (POA) production and aging. However, the main disadvantage is its complexity. We used a Gaussian process simulator to reproduce model results and to estimate the sources of model uncertainty. We do this by comparing the outputs with OA observations made at Delhi, India, in 2018.
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
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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.
Aristeidis Voliotis, Mao Du, Yu Wang, Yunqi Shao, M. Rami Alfarra, Thomas J. Bannan, Dawei Hu, Kelly L. Pereira, Jaqueline F. Hamilton, Mattias Hallquist, Thomas F. Mentel, and Gordon McFiggans
Atmos. Chem. Phys., 22, 14147–14175, https://doi.org/10.5194/acp-22-14147-2022, https://doi.org/10.5194/acp-22-14147-2022, 2022
Short summary
Short summary
Mixing experiments are crucial and highly beneficial for our understanding of atmospheric chemical interactions. However, interpretation quickly becomes complex, and both the experimental design and evaluation need to be scrutinised carefully. Advanced online and offline compositional measurements can reveal substantial additional information to aid in the interpretation of yield data, including components uniquely found in mixtures and property changes in SOA formed from mixtures of VOCs.
Aristeidis Voliotis, Mao Du, Yu Wang, Yunqi Shao, Thomas J. Bannan, Michael Flynn, Spyros N. Pandis, Carl J. Percival, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 22, 13677–13693, https://doi.org/10.5194/acp-22-13677-2022, https://doi.org/10.5194/acp-22-13677-2022, 2022
Short summary
Short summary
The addition of a low-yield precursor to the reactive mixture of aVOC and bVOC can increase or decrease the SOA volatility that is system-dependent. Therefore, the SOA volatility of the mixtures cannot always be predicted based on the additivity. In complex mixtures the formation of lower-volatility products likely outweighs the formation of products with higher volatility. The unique products of each mixture contribute significantly to the signal, suggesting interactions can be important.
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
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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
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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.
Yunqi Shao, Aristeidis Voliotis, Mao Du, Yu Wang, Kelly Pereira, Jacqueline Hamilton, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 22, 9799–9826, https://doi.org/10.5194/acp-22-9799-2022, https://doi.org/10.5194/acp-22-9799-2022, 2022
Short summary
Short summary
This study explored the chemical properties of secondary organic aerosol (SOA) that formed from photo-oxidation of single and mixed biogenic and anthropogenic precursors. We showed that SOA chemical properties in a mixed vapour system are mainly affected by the
higher-yield precursor's oxidation products and products from
cross-product formation. This study also identifies potential tracer compounds in a mixed vapour system that might be used in SOA source attribution in future ambient studies.
Mao Du, Aristeidis Voliotis, Yunqi Shao, Yu Wang, Thomas J. Bannan, Kelly L. Pereira, Jacqueline F. Hamilton, Carl J. Percival, M. Rami Alfarra, and Gordon McFiggans
Atmos. Meas. Tech., 15, 4385–4406, https://doi.org/10.5194/amt-15-4385-2022, https://doi.org/10.5194/amt-15-4385-2022, 2022
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Atmospheric chemistry plays a key role in the understanding of aerosol formation and air pollution. We designed chamber experiments for the characterization of secondary organic aerosol (SOA) from a biogenic precursor with inorganic seed. Our results highlight the advantages of a combination of online FIGAERO-CIMS and offline LC-Orbitrap MS analytical techniques to characterize the chemical composition of SOA in chamber studies.
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
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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.
Siyuan Li, Dantong Liu, Shaofei Kong, Yangzhou Wu, Kang Hu, Huang Zheng, Yi Cheng, Shurui Zheng, Xiaotong Jiang, Shuo Ding, Dawei Hu, Quan Liu, Ping Tian, Delong Zhao, and Jiujiang Sheng
Atmos. Chem. Phys., 22, 6937–6951, https://doi.org/10.5194/acp-22-6937-2022, https://doi.org/10.5194/acp-22-6937-2022, 2022
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The understanding of secondary organic aerosols is hindered by the aerosol–gas evolution by different oxidation mechanisms. By concurrently measuring detailed mass spectra of aerosol and gas phases in a megacity online, we identified the primary and secondary source sectors and investigated the transformation between gas and aerosol phases influenced by photooxidation and moisture. The results will help us to understand the respective evolution of major sources in a typical urban environment.
Chenjie Yu, Dantong Liu, Kang Hu, Ping Tian, Yangzhou Wu, Delong Zhao, Huihui Wu, Dawei Hu, Wenbo Guo, Qiang Li, Mengyu Huang, Deping Ding, and James D. Allan
Atmos. Chem. Phys., 22, 4375–4391, https://doi.org/10.5194/acp-22-4375-2022, https://doi.org/10.5194/acp-22-4375-2022, 2022
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In this study, we applied a new technique to investigate the aerosol properties on both a mass and number basis and CCN abilities in Beijing suburban regions. The size-resolved aerosol chemical compositions and CCN activation measurement enable a detailed analysis of BC-containing particle hygroscopicity and its size-dependent contribution to the CCN activation. The results presented in this study will affect future models and human health studies.
Yu Wang, Aristeidis Voliotis, Dawei Hu, Yunqi Shao, Mao Du, Ying Chen, Judith Kleinheins, Claudia Marcolli, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 22, 4149–4166, https://doi.org/10.5194/acp-22-4149-2022, https://doi.org/10.5194/acp-22-4149-2022, 2022
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Aerosol water uptake plays a key role in atmospheric physicochemical processes. We designed chamber experiments on aerosol water uptake of secondary organic aerosol (SOA) from mixed biogenic and anthropogenic precursors with inorganic seed. Our results highlight this chemical composition influences the reconciliation of the sub- and super-saturated water uptake, providing laboratory evidence for understanding the chemical controls of water uptake of the multi-component aerosol.
Jessica Slater, Hugh Coe, Gordon McFiggans, Juha Tonttila, and Sami Romakkaniemi
Atmos. Chem. Phys., 22, 2937–2953, https://doi.org/10.5194/acp-22-2937-2022, https://doi.org/10.5194/acp-22-2937-2022, 2022
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This paper shows the specific impact of black carbon (BC) on the aerosol–planetary boundary layer (PBL) feedback and its influence on a Beijing haze episode. Overall, this paper shows that strong temperature inversions prevent BC heating within the PBL from significantly increasing PBL height, while BC above the PBL suppresses PBL development significantly through the day. From this we suggest a method by which both locally and regionally emitted BC may impact urban pollution episodes.
Yunqi Shao, Yu Wang, Mao Du, Aristeidis Voliotis, M. Rami Alfarra, Simon P. O'Meara, S. Fiona Turner, and Gordon McFiggans
Atmos. Meas. Tech., 15, 539–559, https://doi.org/10.5194/amt-15-539-2022, https://doi.org/10.5194/amt-15-539-2022, 2022
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A comprehensive description and characterisation of the Manchester Aerosol Chamber (MAC) was conducted. The MAC has good temperature and relative humidity homogeneity, fast mixing times, and comparable losses of gases and particles with other chambers. The MAC's bespoke control system allows improved duty cycles and repeatable experiments. Moreover, the effect of contamination on performance was also investigated. It is highly recommended to regularly track the chamber's performance.
Dawei Hu, M. Rami Alfarra, Kate Szpek, Justin M. Langridge, Michael I. Cotterell, Claire Belcher, Ian Rule, Zixia Liu, Chenjie Yu, Yunqi Shao, Aristeidis Voliotis, Mao Du, Brett Smith, Greg Smallwood, Prem Lobo, Dantong Liu, Jim M. Haywood, Hugh Coe, and James D. Allan
Atmos. Chem. Phys., 21, 16161–16182, https://doi.org/10.5194/acp-21-16161-2021, https://doi.org/10.5194/acp-21-16161-2021, 2021
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Here, we developed new techniques for investigating these properties in the laboratory and applied these to BC and BrC from different sources, including diesel exhaust, inverted propane flame and wood combustion. These have allowed us to quantify the changes in shape and chemical composition of different soots according to source and variables such as the moisture content of wood.
Aristeidis Voliotis, Yu Wang, Yunqi Shao, Mao Du, Thomas J. Bannan, Carl J. Percival, Spyros N. Pandis, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 21, 14251–14273, https://doi.org/10.5194/acp-21-14251-2021, https://doi.org/10.5194/acp-21-14251-2021, 2021
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Secondary organic aerosol (SOA) formation from mixtures of volatile precursors can be affected by the molecular interactions of the products. Composition and volatility measurements of SOA formed from mixtures of anthropogenic and biogenic precursors reveal processes that can increase or decrease the SOA volatility. The unique products of the mixture were more oxygenated and less volatile than those from either precursor. Analytical context is provided to explore the SOA volatility in mixtures.
Huan Song, Keding Lu, Can Ye, Huabin Dong, Shule Li, Shiyi Chen, Zhijun Wu, Mei Zheng, Limin Zeng, Min Hu, and Yuanhang Zhang
Atmos. Chem. Phys., 21, 13713–13727, https://doi.org/10.5194/acp-21-13713-2021, https://doi.org/10.5194/acp-21-13713-2021, 2021
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Secondary sulfate aerosols are an important component of fine particles in severe air pollution events. We calculated the sulfate formation rates via a state-of-the-art multiphase model constrained to the observed values. We showed that transition metals in urban aerosols contribute significantly to sulfate formation during haze periods and thus play an important role in mitigation strategies and public health measures in megacities worldwide.
Ernesto Reyes-Villegas, Upasana Panda, Eoghan Darbyshire, James M. Cash, Rutambhara Joshi, Ben Langford, Chiara F. Di Marco, Neil J. Mullinger, Mohammed S. Alam, Leigh R. Crilley, Daniel J. Rooney, W. Joe F. Acton, Will Drysdale, Eiko Nemitz, Michael Flynn, Aristeidis Voliotis, Gordon McFiggans, Hugh Coe, James Lee, C. Nicholas Hewitt, Mathew R. Heal, Sachin S. Gunthe, Tuhin K. Mandal, Bhola R. Gurjar, Shivani, Ranu Gadi, Siddhartha Singh, Vijay Soni, and James D. Allan
Atmos. Chem. Phys., 21, 11655–11667, https://doi.org/10.5194/acp-21-11655-2021, https://doi.org/10.5194/acp-21-11655-2021, 2021
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This paper shows the first multisite online measurements of PM1 in Delhi, India, with measurements over different seasons in Old Delhi and New Delhi in 2018. Organic aerosol (OA) source apportionment was performed using positive matrix factorisation (PMF). Traffic was the main primary aerosol source for both OAs and black carbon, seen with PMF and Aethalometer model analysis, indicating that control of primary traffic exhaust emissions would make a significant reduction to Delhi air pollution.
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
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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
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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
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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.
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.
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
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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
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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.
Michael Priestley, Thomas J. Bannan, Michael Le Breton, Stephen D. Worrall, Sungah Kang, Iida Pullinen, Sebastian Schmitt, Ralf Tillmann, Einhard Kleist, Defeng Zhao, Jürgen Wildt, Olga Garmash, Archit Mehra, Asan Bacak, Dudley E. Shallcross, Astrid Kiendler-Scharr, Åsa M. Hallquist, Mikael Ehn, Hugh Coe, Carl J. Percival, Mattias Hallquist, Thomas F. Mentel, and Gordon McFiggans
Atmos. Chem. Phys., 21, 3473–3490, https://doi.org/10.5194/acp-21-3473-2021, https://doi.org/10.5194/acp-21-3473-2021, 2021
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A significant fraction of emissions from human activity consists of aromatic hydrocarbons, e.g. benzene, which oxidise to form new compounds important for particle growth. Characterisation of benzene oxidation products highlights the range of species produced as well as their chemical properties and contextualises them within relevant frameworks, e.g. MCM. Cluster analysis of the oxidation product time series distinguishes behaviours of CHON compounds that could aid in identifying functionality.
Simon Patrick O'Meara, Shuxuan Xu, David Topping, M. Rami Alfarra, Gerard Capes, Douglas Lowe, Yunqi Shao, and Gordon McFiggans
Geosci. Model Dev., 14, 675–702, https://doi.org/10.5194/gmd-14-675-2021, https://doi.org/10.5194/gmd-14-675-2021, 2021
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User-friendly and open-source software for simulating aerosol chambers is a valuable tool for research scientists in designing and analysing their experiments. This paper describes a new version of such software and will therefore provide a useful reference for those applying it. Central to the paper is an assessment of the software's accuracy through comparison against previously published simulations.
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
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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.
Jessica Slater, Juha Tonttila, Gordon McFiggans, Paul Connolly, Sami Romakkaniemi, Thomas Kühn, and Hugh Coe
Atmos. Chem. Phys., 20, 11893–11906, https://doi.org/10.5194/acp-20-11893-2020, https://doi.org/10.5194/acp-20-11893-2020, 2020
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The feedback effect between aerosol particles, radiation and meteorology reduces turbulent motion and results in increased surface aerosol concentrations during Beijing haze. Observational analysis and regional modelling studies have examined the feedback effect but these studies are limited. In this work, we set up a high-resolution model for the Beijing environment to examine the sensitivity of the aerosol feedback effect to initial meteorological conditions and aerosol loading.
Cited articles
Alfarra, M. R., Coe, H., Allan, J. D., Bower, K. N., Boudries, H., Canagaratna, M. R., Jimenez, J. L., Jayne, J. T., Garforth, A. A., Li, S.-M., and Worsnop, D. R.: Characterization of urban and rural organic particulate in the Lower Fraser Valley using two Aerodyne Aerosol Mass Spectrometers, Atmos. Environ., 38, 5745–5758, https://doi.org/10.1016/j.atmosenv.2004.01.054, 2004.
Alfarra, M. R., Hamilton, J. F., Wyche, K. P., Good, N., Ward, M. W., Carr, T., Barley, M. H., Monks, P. S., Jenkin, M. E., Lewis, A. C., and McFiggans, G. B.: The effect of photochemical ageing and initial precursor concentration on the composition and hygroscopic properties of β-caryophyllene secondary organic aerosol, Atmos. Chem. Phys., 12, 6417–6436, https://doi.org/10.5194/acp-12-6417-2012, 2012.
Allan, J. D., Jimenez, J. L., Williams, P. I., Alfarra, M. R., Bower, K. N.,
Jayne, J. T., Coe, H., and Worsnop, D. R.: Quantitative sampling using an
Aerodyne aerosol mass spectrometer 1. Techniques of data interpretation and
error analysis, J. Geophys. Res.-Atmos., 108, 4090, https://doi.org/10.1029/2002jd002358, 2003.
Allan, J. D., Delia, A. E., Coe, H., Bower, K. N., Alfarra, M. R., Jimenez, J. L., Middlebrook, A. M., Drewnick, F., Onasch, T. B., Canagaratna, M. R., Jayne, J. T., and Worsnop, D. R.: A generalised method for the extraction of chemically resolved mass spectra from Aerodyne aerosol mass spectrometer data, J. Aerosol Sci., 35, 909–922, https://doi.org/10.1016/j.jaerosci.2004.02.007, 2004.
Bateman, A. P., Belassein, H., and Martin, S. T.: Impactor Apparatus for the Study of Particle Rebound: Relative Humidity and Capillary Forces, Aerosol Sci. Tech., 48, 42–52, https://doi.org/10.1080/02786826.2013.853866, 2014.
Bateman, A. P., Bertram, A. K., and Martin, S. T.: Hygroscopic Influence on the Semisolid-to-Liquid Transition of Secondary Organic Materials, J. Phys. Chem. A, 119, 4386–4395, https://doi.org/10.1021/jp508521c, 2015a.
Bateman, A. P., Gong, Z., Liu, P., 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, https://doi.org/10.1038/ngeo2599, 2015b.
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.
Bertram, A. K., Martin, S. T., Hanna, S. J., Smith, M. L., Bodsworth, A., Chen, Q., Kuwata, M., Liu, A., You, Y., and Zorn, S. R.: Predicting the relative humidities of liquid-liquid phase separation, efflorescence, and deliquescence of mixed particles of ammonium sulfate, organic material, and water using the organic-to-sulfate mass ratio of the particle and the oxygen-to-carbon elemental ratio of the organic component, Atmos. Chem. Phys., 11, 10995–11006, https://doi.org/10.5194/acp-11-10995-2011, 2011.
Bruns, E. A., Perraud, V., Zelenyuk, A., Ezell, M. J., Johnson, S. N., Yu, Y., Imre, D., Finlayson-Pitts, B. J., and Alexander, M. L.: Comparison of FTIR and Particle Mass Spectrometry for the Measurement of Particulate Organic Nitrates, Environ. Sci. Technol., 44, 1056–1061, https://doi.org/10.1021/es9029864, 2010.
Coeur-Tourneur, C., Henry, F., Janquin, M.-A., and Brutier, L.: Gas-phase reaction of hydroxyl radicals with m-, o- and p-cresol, Int. J. Chem. Kinet., 38, 553–562, https://doi.org/10.1002/kin.20186, 2006.
Coggon, M. M., Lim, C. Y., Koss, A. R., Sekimoto, K., Yuan, B., Gilman, J. B., Hagan, D. H., Selimovic, V., Zarzana, K. J., Brown, S. S., Roberts, J. M., Müller, M., Yokelson, R., Wisthaler, A., Krechmer, J. E., Jimenez, J. L., Cappa, C., Kroll, J. H., de Gouw, J., and Warneke, C.: OH chemistry of non-methane organic gases (NMOGs) emitted from laboratory and ambient biomass burning smoke: evaluating the influence of furans and oxygenated aromatics on ozone and secondary NMOG formation, Atmos. Chem. Phys., 19, 14875–14899, https://doi.org/10.5194/acp-19-14875-2019, 2019.
Dahneke, B.: The capture of aerosol particles by surfaces, J. Colloid Interf. Sci., 37, 342–353, https://doi.org/10.1016/0021-9797(71)90302-X, 1971.
DeCarlo, P. F., Kimmel, J. R., Trimborn, A., Northway, M. J., Jayne, J. T., Aiken, A. C., Gonin, M., Fuhrer, K., Horvath, T., Docherty, K. S., Worsnop, D. R., and Jimenez, J. L.: Field-Deployable, High-Resolution, Time-of-Flight Aerosol Mass Spectrometer, Anal. Chem., 78, 8281–8289, https://doi.org/10.1021/ac061249n, 2006.
Farmer, D. K., Matsunaga, A., Docherty, K. S., Surratt, J. D.,
Seinfeld, J. H., Ziemann, P. J., and Jimenez, J. L.: Response of an aerosol
mass spectrometer to organonitrates and organosulfates and implications for
atmospheric chemistry, P. Natl. Acad. Sci. USA, 107, 6670–6675, https://doi.org/10.1073/pnas.0912340107, 2010.
Fishbein, L.: An overview of environmental and toxicological aspects of aromatic hydrocarbons II. Toluene, Sci. Total Environ., 42, 267–288, https://doi.org/10.1016/0048-9697(85)90062-2, 1985.
Freedman, M. A.: Phase separation in organic aerosol, Chem. Soc. Rev., 46, 7694–7705, https://doi.org/10.1039/C6CS00783J, 2017.
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.
Good, N., Coe, H., and McFiggans, G.: Instrumentational operation and analytical methodology for the reconciliation of aerosol water uptake under sub- and supersaturated conditions, Atmos. Meas. Tech., 3, 1241–1254, https://doi.org/10.5194/amt-3-1241-2010, 2010.
Henry, F., Coeur-Tourneur, C., Ledoux, F., Tomas, A., and Menu, D.: Secondary organic aerosol formation from the gas phase reaction of hydroxyl radicals with m-, o- and p-cresol, Atmos. Environ., 42, 3035–3045, https://doi.org/10.1016/j.atmosenv.2007.12.043, 2008.
Ignatius, K., Kristensen, T. B., Järvinen, E., Nichman, L., Fuchs, C., Gordon, H., Herenz, P., Hoyle, C. R., Duplissy, J., Garimella, S., Dias, A., Frege, C., Höppel, N., Tröstl, J., Wagner, R., Yan, C., Amorim, A., Baltensperger, U., Curtius, J., Donahue, N. M., Gallagher, M. W., Kirkby, J., Kulmala, M., Möhler, O., Saathoff, H., Schnaiter, M., Tomé, A., Virtanen, A., Worsnop, D., and Stratmann, F.: Heterogeneous ice nucleation of viscous secondary organic aerosol produced from ozonolysis of α-pinene, Atmos. Chem. Phys., 16, 6495–6509, https://doi.org/10.5194/acp-16-6495-2016, 2016.
Jayne, J. T., Leard, D. C., Zhang, X., Davidovits, P., Smith, K. A., Kolb, C. E., and Worsnop, D. R.: Development of an Aerosol Mass Spectrometer for Size and Composition Analysis of Submicron Particles, Aerosol Sci. Tech., 33, 49–70, https://doi.org/10.1080/027868200410840, 2000.
Jimenez, J. L., Jayne, J. T., Shi, Q., Kolb, C. E., Worsnop, D. R., Yourshaw, I., Seinfeld, J. H., Flagan, R. C., Zhang, X., Smith, K. A., Morris, J. W., and Davidovits, P.: Ambient aerosol sampling using the Aerodyne Aerosol Mass Spectrometer, J. Geophys. Res.-Atmos., 108, https://doi.org/10.1029/2001JD001213, 2003.
Jimenez, J. L., Canagaratna, M. R., Donahue, N. M., Prevot, A. S. H., Zhang, Q., Kroll, J. H., DeCarlo, P. F., Allan, J. D., Coe, H., Ng, N. L., Aiken, A. C., Docherty, K. S., Ulbrich, I. M., Grieshop, A. P., Robinson, A. L., Duplissy, J., Smith, J. D., Wilson, K. R., Lanz, V. A., Hueglin, C., Sun, Y. L., Tian, J., Laaksonen, A., Raatikainen, T., Rautiainen, J., Vaattovaara, P., Ehn, M., Kulmala, M., Tomlinson, J. M., Collins, D. R., Cubison, M. J., Dunlea, J., Huffman, J. A., Onasch, T. B., Alfarra, M. R., Williams, P. I., Bower, K., Kondo, Y., Schneider, J., Drewnick, F., Borrmann, S., Weimer, S., Demerjian, K., Salcedo, D., Cottrell, L., Griffin, R., Takami, A., Miyoshi, T., Hatakeyama, S., Shimono, A., Sun, J. Y., Zhang, Y. M., Dzepina, K., Kimmel, J. R., Sueper, D., Jayne, J. T., Herndon, S. C., Trimborn, A. M., Williams, L. R., Wood, E. C., Middlebrook, A. M., Kolb, C. E., Baltensperger, U., and Worsnop, D. R.: Evolution of Organic Aerosols in the Atmosphere, Science, 326, 1525–1529, https://doi.org/10.1126/science.1180353, 2009.
Kiendler-Scharr, A., Mensah, A. A., Friese, E., Topping, D., Nemitz, E., Prevot, A. S. H., Äijälä, M., Allan, J., Canonaco, F., Canagaratna, M., Carbone, S., Crippa, M., Dall Osto, M., Day, D. A., De Carlo, P., Di Marco, C. F., Elbern, H., Eriksson, A., Freney, E., Hao, L., Herrmann, H., Hildebrandt, L., Hillamo, R., Jimenez, J. L., Laaksonen, A., McFiggans, G., Mohr, C., O'Dowd, C., Otjes, R., Ovadnevaite, J., Pandis, S. N., Poulain, L., Schlag, P., Sellegri, K., Swietlicki, E., Tiitta, P., Vermeulen, A., Wahner, A., Worsnop, D., and Wu, H.-C.: Ubiquity of organic nitrates from nighttime chemistry in the European submicron aerosol, Geophys. Res. Lett., 43, 7735–7744, https://doi.org/10.1002/2016gl069239, 2016.
Koop, T., Bookhold, J., Shiraiwa, M., and Poschl, 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.
Koss, A. R., Sekimoto, K., Gilman, J. B., Selimovic, V., Coggon, M. M., Zarzana, K. J., Yuan, B., Lerner, B. M., Brown, S. S., Jimenez, J. L., Krechmer, J., Roberts, J. M., Warneke, C., Yokelson, R. J., and de Gouw, J.: Non-methane organic gas emissions from biomass burning: identification, quantification, and emission factors from PTR-ToF during the FIREX 2016 laboratory experiment, Atmos. Chem. Phys., 18, 3299–3319, https://doi.org/10.5194/acp-18-3299-2018, 2018.
Kreidenweis, S. and Asa-Awuku, A.: Aerosol Hygroscopicity: Particle Water
Content and Its Role in Atmospheric Processes, Elsevier Science, Sciencedirect, 331–361, 2014.
Krieger, U. K., Marcolli, C., and Reid, J. P.: Exploring the complexity of aerosol particle properties and processes using single particle techniques, Chem. Soc. Rev., 41, 6631–6662, https://doi.org/10.1039/C2CS35082C, 2012.
Kuwata, M. and Martin, S. T.: Phase of atmospheric secondary
organic material affects its reactivity, P. Natl. Acad. Sci. USA, 109, 17354–17359, https://doi.org/10.1073/pnas.1209071109, 2012.
Li, Y. J., Liu, P. F., Bergoend, C., Bateman, A. P., and Martin, S. T.: Rebounding hygroscopic inorganic aerosol particles: Liquids, gels, and hydrates, Aerosol Sci. Tech., 51, 388–396, https://doi.org/10.1080/02786826.2016.1263384, 2017.
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. Tech. 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.
MAC/NCAS-MAN – Manchester chamber group: SOA from mixed precursors, available at: https://data.eurochamp.org/data-access/chamber-experiments/, last access date: 24 July 2021.
Martin, S. T.: Phase Transitions of Aqueous Atmospheric Particles, Chem. Rev., 100, 3403–3454, https://doi.org/10.1021/cr990034t, 2000.
McFiggans, G., Mentel, T. F., Wildt, J., Pullinen, I., Kang, S., Kleist, E., Schmitt, S., Springer, M., Tillmann, R., Wu, C., Zhao, D., Hallquist, M., Faxon, C., Le Breton, M., Hallquist, Å. M., Simpson, D., Bergström, R., Jenkin, M. E., Ehn, M., Thornton, J. A., Alfarra, M. R., Bannan, T. J., Percival, C. J., Priestley, M., Topping, D., and Kiendler-Scharr, A.: Secondary organic aerosol reduced by mixture of atmospheric vapours, Nature, 565, 587–593, https://doi.org/10.1038/s41586-018-0871-y, 2019.
Murray, B. J.: Inhibition of ice crystallisation in highly viscous aqueous organic acid droplets, Atmos. Chem. Phys., 8, 5423–5433, https://doi.org/10.5194/acp-8-5423-2008, 2008.
Murray, B. J., Wilson, T. W., Dobbie, S., Cui, Z., Al-Jumur, S. M. R. K., Möhler, O., Schnaiter, M., Wagner, R., Benz, S., Niemand, M., Saathoff, H., Ebert, V., Wagner, S., and Kärcher, B.: Heterogeneous nucleation of ice particles on glassy aerosols under cirrus conditions, Nat. Geosci., 3, 233, https://doi.org/10.1038/ngeo817, 2010.
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.
Pedernera, D. A.: Glass formation in upper tropospheric aerosol particles, PhD thesis, Bielefeld University, available at:
http://pub.uni-bielefeld.de/publication/2303351 (last access: 24 July 2021), 2008.
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.
Pöschl, U.: Gas–particle interactions of tropospheric aerosols: Kinetic and thermodynamic perspectives of multiphase chemical reactions, amorphous organic substances, and the activation of cloud condensation nuclei, Atmospheric Research, 101, 562–573, https://doi.org/10.1016/j.atmosres.2010.12.018, 2011.
Reid, J. P., Bertram, A. K., Topping, D. O., Laskin, A., Martin, S. T., Petters, M. D., Pope, F. D., and Rovelli, G.: The viscosity of atmospherically relevant organic particles, Nat. Commun., 9, 956, https://doi.org/10.1038/s41467-018-03027-z, 2018.
Renbaum-Wolff, L., Grayson, J. W., Bateman, A. P., Kuwata, M.,
Sellier, M., Murray, B. J., Shilling, J. E., Martin, S. T., and
Bertram, A. K.: Viscosity of α-pinene secondary organic material and
implications for particle growth and reactivity, P. Natl. Acad. Sci. USA, 110, 8014–8019, https://doi.org/10.1073/pnas.1219548110, 2013.
Reyes-Villegas, E., Priestley, M., Ting, Y.-C., Haslett, S., Bannan, T., Le Breton, M., Williams, P. I., Bacak, A., Flynn, M. J., Coe, H., Percival, C., and Allan, J. D.: Simultaneous aerosol mass spectrometry and chemical ionisation mass spectrometry measurements during a biomass burning event in the UK: insights into nitrate chemistry, Atmos. Chem. Phys., 18, 4093–4111, https://doi.org/10.5194/acp-18-4093-2018, 2018.
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.
Saukko, E., Zorn, S., Kuwata, M., Keskinen, J., and Virtanen, A.: Phase State and Deliquescence Hysteresis of Ammonium-Sulfate-Seeded Secondary Organic Aerosol, Aerosol Sci. Tech., 49, 531–537, https://doi.org/10.1080/02786826.2015.1050085, 2015.
Shao, Y., Wang, Y., Du, M., Voliotis, A., Alfarra, M. R., Turner, S. F., and
McFiggans, G.: Characterisation of the Manchester Aerosol Chamber facility,
Atmos. Meas. Tech. Discuss. [preprint], https://doi.org/10.5194/amt-2021-147, in
review, 2021.
Shilling, J. E., Zawadowicz, M. A., Liu, J., Zaveri, R. A., and Zelenyuk, A.: Photochemical Aging Alters Secondary Organic Aerosol Partitioning Behavior, ACS Earth and Space Chemistry, 3, 2704–2716, https://doi.org/10.1021/acsearthspacechem.9b00248, 2019.
Shiraiwa, M. and Seinfeld, J. H.: Equilibration timescale of atmospheric secondary organic aerosol partitioning, Geophys. Res. Lett., 39, L24801, https://doi.org/10.1029/2012gl054008, 2012.
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., 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.
Slade, J. H., Shiraiwa, M., Arangio, A., Su, H., Pöschl, U., Wang, J., and Knopf, D. A.: Cloud droplet activation through oxidation of organic aerosol influenced by temperature and particle phase state, Geophys. Res. Lett., 44, 1583–1591, https://doi.org/10.1002/2016gl072424, 2017.
Slade, J. H., Ault, A. P., Bui, A. T., Ditto, J. C., Lei, Z., Bondy, A. L., Olson, N. E., Cook, R. D., Desrochers, S. J., Harvey, R. M., Erickson, M. H., Wallace, H. W., Alvarez, S. L., Flynn, J. H., Boor, B. E., Petrucci, G. A., Gentner, D. R., Griffin, R. J., and Shepson, P. B.: Bouncier Particles at Night: Biogenic Secondary Organic Aerosol Chemistry and Sulfate Drive Diel Variations in the Aerosol Phase in a Mixed Forest, Environ. Sci. Technol., 53, 4977–4987, https://doi.org/10.1021/acs.est.8b07319, 2019.
Smith, M. L., Kuwata, M., and Martin, S. T.: Secondary Organic Material Produced by the Dark Ozonolysis of α-Pinene Minimally Affects the Deliquescence and Efflorescence of Ammonium Sulfate, Aerosol Sci. Tech., 45, 244–261, https://doi.org/10.1080/02786826.2010.532178, 2011.
Smith, M. L., Bertram, A. K., and Martin, S. T.: Deliquescence, efflorescence, and phase miscibility of mixed particles of ammonium sulfate and isoprene-derived secondary organic material, Atmos. Chem. Phys., 12, 9613–9628, https://doi.org/10.5194/acp-12-9613-2012, 2012.
Smith, M. L., You, Y., Kuwata, M., Bertram, A. K., and Martin, S. T.: Phase Transitions and Phase Miscibility of Mixed Particles of Ammonium Sulfate, Toluene-Derived Secondary Organic Material, and Water, J. Phys. Chem. A, 117, 8895–8906, https://doi.org/10.1021/jp405095e, 2013.
Song, M., Marcolli, C., Krieger, U. K., Zuend, A., and Peter, T.:
Liquid-liquid phase separation in aerosol particles: Dependence on O:C, organic functionalities, and compositional complexity, Geophys. Res. Lett., 39, L19801, https://doi.org/10.1029/2012GL052807, 2012.
Stein, S. W., Turpin, B. J., Cai, X., Huang, P.-F., and McMurry, P. H.: Measurements of relative humidity-dependent bounce and density for atmospheric particles using the DMA-impactor technique, Atmos. Environ., 28, 1739–1746, https://doi.org/10.1016/1352-2310(94)90136-8, 1994.
Tang, I. N. and Munkelwitz, H. R.: Composition and temperature dependence of the deliquescence properties of hygroscopic aerosols, Atmos. Environ. A-Gen., 27, 467–473, https://doi.org/10.1016/0960-1686(93)90204-C, 1993.
Vaden, T. D., Imre, D., Beránek, J., Shrivastava, M., and
Zelenyuk, A.: Evaporation kinetics and phase of laboratory and ambient
secondary organic aerosol, P. Natl. Acad. Sci. USA, 108, 2190–2195, https://doi.org/10.1073/pnas.1013391108, 2011.
Virtanen, A., Joutsensaari, J., Koop, T., Kannosto, J., Yli-Pirilä, P., Leskinen, J., Mäkelä, J. M., Holopainen, J. K., Pöschl, U., Kulmala, M., Worsnop, D. R., and Laaksonen, A.: An amorphous solid state of biogenic secondary organic aerosol particles, Nature, 467, 824, https://doi.org/10.1038/nature09455, 2010.
You, Y., Smith, M. L., Song, M., Martin, S. T., and Bertram, A. K.:
Liquid–liquid phase separation in atmospherically relevant particles
consisting of organic species and inorganic salts, Int. Rev. Phys. Chem., 33, 43–77, https://doi.org/10.1080/0144235X.2014.890786, 2014.
Zaveri, R. A., Easter, R. C., Shilling, J. E., and Seinfeld, J. H.: Modeling kinetic partitioning of secondary organic aerosol and size distribution dynamics: representing effects of volatility, phase state, and particle-phase reaction, Atmos. Chem. Phys., 14, 5153–5181, https://doi.org/10.5194/acp-14-5153-2014, 2014.
Zhang, Y., Chen, Y., Lambe, A. T., Olson, N. E., Lei, Z., Craig, R. L., Zhang, Z., 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 (IEPOX), Environ. Sci. Tech. Lett., 5, 167–174, https://doi.org/10.1021/acs.estlett.8b00044, 2018.
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.
Aerosol phase behaviour plays a profound role in atmospheric physicochemical processes. We...
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