Articles | Volume 21, issue 13
https://doi.org/10.5194/acp-21-10215-2021
© 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-21-10215-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
07 Jul 2021
Research article |
| 07 Jul 2021
| 07 Jul 2021
Viscosity and phase state of aerosol particles consisting of sucrose mixed with inorganic salts
Young-Chul Song
Department of Earth and Environmental Sciences, Jeonbuk National University, Jeonju, Republic of Korea
The Earth and Environmental Science System Research Center, Jeonbuk National University, Jeonju, Republic of Korea
Joseph Lilek
Department of Atmospheric and Oceanic Sciences, McGill University, Montréal, Quebec, Canada
Jae Bong Lee
Innovative System Safety Research Division, Korea Atomic Energy Research Institute, Daejeon, Republic of Korea
Man Nin Chan
Earth System Science Programme, Faculty of Science, The Chinese University of Hong Kong, Hong Kong, China
The Institute of Environment, Energy, and Sustainability, The Chinese University of Hong Kong, Hong Kong, China
Zhijun Wu
Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing, China
Andreas Zuend
Department of Atmospheric and Oceanic Sciences, McGill University, Montréal, Quebec, Canada
Mijung Song
CORRESPONDING AUTHOR
Department of Earth and Environmental Sciences, Jeonbuk National University, Jeonju, Republic of Korea
The Earth and Environmental Science System Research Center, Jeonbuk National University, Jeonju, Republic of Korea
Department of Environment and Energy, Jeonbuk National University, Jeonju, Republic of Korea
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This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
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Dalrin Ampritta Amaladhasan, Dan Hassan-Barthaux, and Andreas Zuend
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Brown Carbon (BrC) is considered as one of the least understood atmospheric warming agents. BrC’s photobleaching has been determined as a key reason to the uncertainty in its global radiative effect, which has been poorly constrained. This study revelas the source-dependent BrC photobleaching rates, and explained this difference from molecular perspective. Consequently, the OH oxidation reactivity of molecular composition of different types of BrC determines their distinct photobleaching rates.
Yanting Qiu, Junrui Wang, Tao Qiu, Jiajie Li, Yanxin Bai, Teng Liu, Ruiqi Man, Taomou Zong, Wenxu Fang, Jiawei Yang, Yu Xie, Zeyu Feng, Chenhui Li, Ying Wei, Kai Bi, Dapeng Liang, Ziqi Gao, Zhijun Wu, Yuchen Wang, and Min Hu
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Atmos. Chem. Phys., 26, 2319–2329, https://doi.org/10.5194/acp-26-2319-2026, https://doi.org/10.5194/acp-26-2319-2026, 2026
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We investigated the temperature- and relative-humidity-dependent viscosity of organic aerosols using sucrose-water droplets as a model. The results show that particles remain liquid near the Earth’s surface but become semi-solid or glassy at higher altitudes. These viscosity changes influence chemical reactions such as nitrogen oxide uptake, improving understanding of air quality and climate processes.
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Atmos. Chem. Phys., 26, 349–363, https://doi.org/10.5194/acp-26-349-2026, https://doi.org/10.5194/acp-26-349-2026, 2026
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Gaseous and particulate organic compounds emitted from cooking are significant contributors to urban air pollution. A key scientific challenge lies in understanding the changes in their gas-particle partitioning during atmospheric oxidation. This complexity hinders the formulation of effective control policies.
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Mineral dust can initiate ice formation in clouds, affecting cloud properties and regional climate. Using an improved model, we examined their contrasting impacts in mixed-phase and ice clouds over East Asia. In mixed-phase clouds, dust promotes liquid-to-ice conversion and reduces cloud reflectivity, causing moderate warming, whereas in ice clouds, it greatly enhances ice formation and leads to stronger warming. This study advances understanding of aerosol–cloud–climate interactions.
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Ryan Schmedding and Andreas Zuend
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Xiangxinyue Meng, Zhijun Wu, Jingchuan Chen, Yanting Qiu, Taomou Zong, Mijung Song, Jiyi Lee, and Min Hu
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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.
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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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.
Ryan Schmedding and Andreas Zuend
Atmos. Chem. Phys., 23, 7741–7765, https://doi.org/10.5194/acp-23-7741-2023, https://doi.org/10.5194/acp-23-7741-2023, 2023
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Aerosol particles below 100 nm in diameter have high surface-area-to-volume ratios. The enrichment of compounds in the surface of an aerosol particle may lead to depletion of that species in the interior bulk of the particle. We present a framework for modeling the equilibrium bulk–surface partitioning of mixed organic–inorganic particles, including cases of co-condensation of semivolatile organic compounds and species with extremely limited solubility in the bulk or surface of a particle.
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.
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.
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
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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
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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.
Rongshuang Xu, Sze In Madeleine Ng, Wing Sze Chow, Yee Ka Wong, Yuchen Wang, Donger Lai, Zhongping Yao, Pui-Kin So, Jian Zhen Yu, and Man Nin Chan
Atmos. Chem. Phys., 22, 5685–5700, https://doi.org/10.5194/acp-22-5685-2022, https://doi.org/10.5194/acp-22-5685-2022, 2022
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To date, while over a hundred organosulfates (OSs) have been detected in atmospheric aerosols, many of them are still unidentified, with unknown precursors and formation processes. We found the heterogeneous OH oxidation of an α-pinene-derived organosulfate (C10H17O5SNa, αpOS-249, αpOS-249) can proceed at an efficient rate and transform into more oxygenated OSs, which have been commonly detected in atmospheric aerosols and α-pinene-derived SOA in chamber studies.
Joseph Lilek and Andreas Zuend
Atmos. Chem. Phys., 22, 3203–3233, https://doi.org/10.5194/acp-22-3203-2022, https://doi.org/10.5194/acp-22-3203-2022, 2022
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Depending on temperature and chemical makeup, certain aerosols can be highly viscous or glassy, with atmospheric implications. We have therefore implemented two major upgrades to the predictive viscosity model AIOMFAC-VISC. First, we created a new viscosity model for aqueous electrolyte solutions containing an arbitrary number of ion species. Second, we integrated the electrolyte model within the existing AIOMFAC-VISC framework to enable viscosity predictions for organic–inorganic mixtures.
Hang Yin, Jing Dou, Liviana Klein, Ulrich K. Krieger, Alison Bain, Brandon J. Wallace, Thomas C. Preston, and Andreas Zuend
Atmos. Chem. Phys., 22, 973–1013, https://doi.org/10.5194/acp-22-973-2022, https://doi.org/10.5194/acp-22-973-2022, 2022
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Iodine and carbonate species are important components in marine and dust aerosols, respectively. We introduce an extended version of the AIOMFAC thermodynamic mixing model, which includes the ions I−, IO3−, HCO3−, CO32−, OH−, and CO2(aq) as new species, and we discuss two methods for solving the carbonate dissociation equilibria numerically. We also present new experimental water activity data for aqueous iodide and iodate systems.
Dalrin Ampritta Amaladhasan, Claudia Heyn, Christopher R. Hoyle, Imad El Haddad, Miriam Elser, Simone M. Pieber, Jay G. Slowik, Antonio Amorim, Jonathan Duplissy, Sebastian Ehrhart, Vladimir Makhmutov, Ugo Molteni, Matti Rissanen, Yuri Stozhkov, Robert Wagner, Armin Hansel, Jasper Kirkby, Neil M. Donahue, Rainer Volkamer, Urs Baltensperger, Martin Gysel-Beer, and Andreas Zuend
Atmos. Chem. Phys., 22, 215–244, https://doi.org/10.5194/acp-22-215-2022, https://doi.org/10.5194/acp-22-215-2022, 2022
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We use a combination of models for gas-phase chemical reactions and equilibrium gas–particle partitioning of isoprene-derived secondary organic aerosols (SOAs) informed by dark ozonolysis experiments conducted in the CLOUD chamber. Our predictions cover high to low relative humidities (RHs) and quantify how SOA mass yields are enhanced at high RH as well as the impact of inorganic seeds of distinct hygroscopicities and acidities on the coupled partitioning of water and semi-volatile organics.
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.
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
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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.
Cited articles
Abdulagatov, I. M., Zeinalova, A. A., and Azizov, N. D.:
Viscosity of the aqueous Ca(NO3)2 solutions at temperatures from 298 to 573 K and at pressures up to 40 MPa,
J. Chem. Eng. Data,
49, 1444–1450, https://doi.org/10.1021/je049853n, 2004.
Athanasiadis, A., Fitzgerald, C., Davidson, N. M., Giorio, C., Botchway, S. W., Ward, A. D., Kalberer, M., Pope, F. D., and Kuimova, M. K.:
Dynamic viscosity mapping of the oxidation of squalene aerosol particles,
Phys. Chem. Chem. Phys.,
18, 30385–30393, https://doi.org/10.1039/C6CP05674A, 2016.
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, 2015.
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, 2016.
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.
Bhattarai, G., Lee, J. B., Kim, M. H., Ham, S., So, H. S., Oh, S.,
Sim, H. J., Lee, J. C., Song, M., and Kook, S. H.: Maternal exposure
to fine particulate matter during pregnancy induces progressive
senescence of hematopoietic stem cells under preferential
30 impairment of the bone marrow microenvironment and aids development
of myeloproliferative disease, Leukemia 34, 1481–1484, https://doi.org/10.1038/s41375-019-0665-8, 2020
Cheng, Z., Luo, L., Wang, S., Wang, Y., Sharma, S., Shimadera, H., Wang, X., Bressi, M., de Miranda, R. M., Jiang, J., Zhou, W., Fajardo, O., Yan, N., and Hao, J.:
Status and characteristics of ambient PM2.5 pollution in global megacities,
Environ. Int.,
89–90, 212–221, https://doi.org/10.1016/j.envint.2016.02.003, 2016.
Davies, J. F. and Wilson, K. R.:
Nanoscale interfacial gradients formed by the reactive uptake of OH radicals onto viscous aerosol surfaces,
Chem. Sci.,
6, 7020–7027, https://doi.org/10.1039/C5SC02326B, 2015.
George, I. J. and Abbatt, J. P. D.: Heterogeneous oxidation of atmospheric aerosol particles by gas-phase radicals, Nat. Chem., 2, 713–722, 2010.
Gervasi, N. R., Topping, D. O., and Zuend, A.: A predictive group-contribution model for the viscosity of aqueous organic aerosol, Atmos. Chem. Phys., 20, 2987–3008, https://doi.org/10.5194/acp-20-2987-2020, 2020.
Grayson, J. W., Song, M., Sellier, M., and Bertram, A. K.: Validation of the poke-flow technique combined with simulations of fluid flow for determining viscosities in samples with small volumes and high viscosities, Atmos. Meas. Tech., 8, 2463–2472, https://doi.org/10.5194/amt-8-2463-2015, 2015.
Grayson, J. W., Zhang, Y., Mutzel, A., Renbaum-Wolff, L., Böge, O., Kamal, S., Herrmann, H., Martin, S. T., and Bertram, A. K.: Effect of varying experimental conditions on the viscosity of α-pinene derived secondary organic material, Atmos. Chem. Phys., 16, 6027–6040, https://doi.org/10.5194/acp-16-6027-2016, 2016.
Grayson, J. W., Evoy, E., Song, M., Chu, Y., Maclean, A., Nguyen, A., Upshur, M. A., Ebrahimi, M., Chan, C. K., Geiger, F. M., Thomson, R. J., and Bertram, A. K.: The effect of hydroxyl functional groups and molar mass on the viscosity of non-crystalline organic and organic–water particles, Atmos. Chem. Phys., 17, 8509–8524, https://doi.org/10.5194/acp-17-8509-2017, 2017.
Guo, L., Gu, W., Peng, C., Wang, W., Li, Y. J., Zong, T., Tang, Y., Wu, Z., Lin, Q., Ge, M., Zhang, G., Hu, M., Bi, X., Wang, X., and Tang, M.: A comprehensive study of hygroscopic properties of calcium- and magnesium-containing salts: implication for hygroscopicity of mineral dust and sea salt aerosols, Atmos. Chem. Phys., 19, 2115–2133, https://doi.org/10.5194/acp-19-2115-2019, 2019.
Gupta, D., Eom, H.-J., Cho, H.-R., and Ro, C.-U.: Hygroscopic behavior of NaCl–MgCl2 mixture particles as nascent sea-spray aerosol surrogates and observation of efflorescence during humidification, Atmos. Chem. Phys., 15, 11273–11290, https://doi.org/10.5194/acp-15-11273-2015, 2015.
Ham, S., Babar, Z. B., Lee, J. B., Lim, H.-J., and Song, M.: Liquid–liquid phase separation in secondary organic aerosol particles produced from α-pinene ozonolysis and α-pinene photooxidation with/without ammonia, Atmos. Chem. Phys., 19, 9321–9331, https://doi.org/10.5194/acp-19-9321-2019, 2019.
Hao, L. Q., Kortelainen, A., Romakkaniemi, S., Portin, H., Jaatinen, A., Leskinen, A., Komppula, M., Miettinen, P., Sueper, D., Pajunoja, A., Smith, J. N., Lehtinen, K. E. J., Worsnop, D. R., Laaksonen, A., and Virtanen, A.: Atmospheric submicron aerosol composition and particulate organic nitrate formation in a boreal forestland–urban mixed region, Atmos. Chem. Phys., 14, 13483–13495, https://doi.org/10.5194/acp-14-13483-2014, 2014.
Haynes, W. M.:
CRC handbook of chemistry and physics, 97rd edn.,
CRC Press, New York, 2015.
Hinks, M. L., Brady, M. V, Lignell, H., Song, M., Grayson, J. W., Bertram, A. K., Lin, P., Laskin, A., Laskin, J., and Nizkorodov, S. A.:
Effect of viscosity on photodegradation rates in complex secondary organic aerosol materials,
Phys. Chem. Chem. Phys.,
18, 8785–8793, https://doi.org/10.1039/c5cp05226b, 2016.
Hosny, N. A., Fitzgerald, C., Tong, C., Kalberer, M., Kuimova, M. K., and Pope, F. D.: Fluorescent lifetime imaging of atmospheric aerosols: a direct probe of aerosol viscosity, Faraday Discuss., 165, 343–356, https://doi.org/10.1039/C3FD00041A, 2013.
Hosny, N. A., Fitzgerald, C., Vysniauskas, A., Athanasiadis, T., Berkemeier, T., Uygur, N., Pöschl, U., Shiraiwa, M., Kalberer, M., Pope, F. D., and Kuimova, M. K.:
Direct imaging of changes in aerosol particle viscosity upon hydration and chemical aging,
Chem. Sci.,
7, 1357–1367, https://doi.org/10.1039/C5SC02959G, 2016.
Huang, R. J., Zhang, Y., Bozzetti, C., Ho, K. F., Cao, J. J., Han, Y., Daellenbach, K. R., Slowik, J. G., Platt, S. M., Canonaco, F., Zotter, P., Wolf, R., Pieber, S. M., Bruns, E. A., Crippa, M., Ciarelli, G., Piazzalunga, A., Schwikowski, M., Abbaszade, G., Schnelle-Kreis, J., Zimmermann, R., An, Z., Szidat, S., Baltensperger, U., El Haddad, I., and Prévôt, A. S. H.:
High secondary aerosol contribution to particulate pollution during haze events in China,
Nature,
514, 218–222, https://doi.org/10.1038/nature13774, 2015.
Huang, Y., Mahrt, F., Xu, S., Shiraiwa, M., Zuend, A., and Bertram, A. K.:
Coexistence of three liquid phases in individual atmospheric aerosol particles,
P. Natl. Acad. Sci. USA,
118, e2102512118, https://doi.org/10.1073/pnas.2102512118, 2021.
Ji, Z. R., Zhang, Y., Pang, S. F., and Zhang, Y. H.: Crystal nucleation and crystal growth and mass transfer in internally mixed sucrose/NaNO3 particles, J. Phys. Chem. A, 121, 7968–7975, https://doi.org/10.1021/acs.jpca.7b08004, 2017.
Kanakidou, M., Seinfeld, J. H., Pandis, S. N., Barnes, I., Dentener, F. J., Facchini, M. C., Van Dingenen, R., Ervens, B., Nenes, A., Nielsen, C. J., Swietlicki, E., Putaud, J. P., Balkanski, Y., Fuzzi, S., Horth, J., Moortgat, G. K., Winterhalter, R., Myhre, C. E. L., Tsigaridis, K., Vignati, E., Stephanou, E. G., and Wilson, J.: Organic aerosol and global climate modelling: a review, Atmos. Chem. Phys., 5, 1053–1123, https://doi.org/10.5194/acp-5-1053-2005, 2005.
Kaufman, Y. J., Tanré, D., and Boucher, O.:
A satellite view of aerosols in the climate system,
Nature,
419, 215–223, 2002.
Kidd, C., Perraud, V., Wingen, L. M., and Finlayson-Pitts, B. J.:
Integrating phase and composition of secondary organic aerosol from the ozonolysis of α-pinene,
P. Natl. Acad. Sci. USA,
111, 7552–7, https://doi.org/10.1073/pnas.1322558111, 2014.
Kim, Y., Sartelet, K., and Couvidat, F.: Modeling the effect of non-ideality, dynamic mass transfer and viscosity on SOA formation in a 3-D air quality model, Atmos. Chem. Phys., 19, 1241–1261, https://doi.org/10.5194/acp-19-1241-2019, 2019.
Knopf, D. A., Alpert, P., and Wang, B.:
The role of organic aerosol in atmospheric ice nucleation – A Review,
ACS Earth Sp. Chem.,
2, 168–202, https://doi.org/10.1021/acsearthspacechem.7b00120, 2018.
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.
Kulmala, M., Asmi, A., Lappalainen, H. K., Baltensperger, U., Brenguier, J.-L., Facchini, M. C., Hansson, H.-C., Hov, Ø., O'Dowd, C. D., Pöschl, U., Wiedensohler, A., Boers, R., Boucher, O., de Leeuw, G., Denier van der Gon, H. A. C., Feichter, J., Krejci, R., Laj, P., Lihavainen, H., Lohmann, U., McFiggans, G., Mentel, T., Pilinis, C., Riipinen, I., Schulz, M., Stohl, A., Swietlicki, E., Vignati, E., Alves, C., Amann, M., Ammann, M., Arabas, S., Artaxo, P., Baars, H., Beddows, D. C. S., Bergström, R., Beukes, J. P., Bilde, M., Burkhart, J. F., Canonaco, F., Clegg, S. L., Coe, H., Crumeyrolle, S., D'Anna, B., Decesari, S., Gilardoni, S., Fischer, M., Fjaeraa, A. M., Fountoukis, C., George, C., Gomes, L., Halloran, P., Hamburger, T., Harrison, R. M., Herrmann, H., Hoffmann, T., Hoose, C., Hu, M., Hyvärinen, A., Hõrrak, U., Iinuma, Y., Iversen, T., Josipovic, M., Kanakidou, M., Kiendler-Scharr, A., Kirkevåg, A., Kiss, G., Klimont, Z., Kolmonen, P., Komppula, M., Kristjánsson, J.-E., Laakso, L., Laaksonen, A., Labonnote, L., Lanz, V. A., Lehtinen, K. E. J., Rizzo, L. V., Makkonen, R., Manninen, H. E., McMeeking, G., Merikanto, J., Minikin, A., Mirme, S., Morgan, W. T., Nemitz, E., O'Donnell, D., Panwar, T. S., Pawlowska, H., Petzold, A., Pienaar, J. J., Pio, C., Plass-Duelmer, C., Prévôt, A. S. H., Pryor, S., Reddington, C. L., Roberts, G., Rosenfeld, D., Schwarz, J., Seland, Ø., Sellegri, K., Shen, X. J., Shiraiwa, M., Siebert, H., Sierau, B., Simpson, D., Sun, J. Y., Topping, D., Tunved, P., Vaattovaara, P., Vakkari, V., Veefkind, J. P., Visschedijk, A., Vuollekoski, H., Vuolo, R., Wehner, B., Wildt, J., Woodward, S., Worsnop, D. R., van Zadelhoff, G.-J., Zardini, A. A., Zhang, K., van Zyl, P. G., Kerminen, V.-M., S Carslaw, K., and Pandis, S. N.: General overview: European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) – integrating aerosol research from nano to global scales, Atmos. Chem. Phys., 11, 13061–13143, https://doi.org/10.5194/acp-11-13061-2011, 2011.
Kuwata, M. and Martin, S. T.:
Phase of atmospheric secondary organic material affects its reactivity,
P. Natl. Acad. Sci. USA,
109, 17354-17359, 2012.
Ladino, L. A., Zhou, S., Yakobi-Hancock, J. D., Aljawhary, D., and Abbatt, J. P. D.:
Factors controlling the ice nucleating abilities of α-pinene SOA particles,
J. Geophys. Res.,
119, 9041–9051, https://doi.org/10.1002/2014JD021578, 2014.
Laliberté, M.:
Model for calculating the viscosity of aqueous aolutions,
J. Chem. Eng. Data,
52, 1507–1508, https://doi.org/10.1021/je700232s, 2007.
Laliberté, M.:
A model for calculating the heat capacity of aqueous solutions, with updated density and viscosity data,
J. Chem. Eng. Data,
54, 1725–1760, https://doi.org/10.1021/je8008123, 2009.
Laskin, A., Iedema, M. J., Ichkovich, A., Graber, E. R., Taraniuk, I., and Rudich, Y.:
Direct observation of completely processed calcium carbonate dust particles,
Faraday Discuss.,
130, 453–468, https://doi.org/10.1039/b417366j, 2005.
Li, J., Forrester, S. M., and Knopf, D. A.: Heterogeneous oxidation of amorphous organic aerosol surrogates by O3, NO3, and OH at typical tropospheric temperatures, Atmos. Chem. Phys., 20, 6055–6080, https://doi.org/10.5194/acp-20-6055-2020, 2020.
Li, X. H., Zhao, L. J., Dong, J. L., Xiao, H. S., and Zhang, Y. H.:
Confocal raman studies of Mg(NO3)2 aerosol particles deposited on a quartz substrate: supersaturated structures and complicated phase transitions,
J. Phys. Chem. B,
112, 5032–5038, https://doi.org/10.1021/jp709938x, 2008.
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.
Lilek, J. and Zuend, A.: A predictive viscosity model for aqueous electrolytes and mixed organic–inorganic aerosol phase,
in preparation, 2021.
Liu, Y. J., Zhu, T., Zhao, D. F., and Zhang, Z. F.: Investigation of the hygroscopic properties of Ca(NO3)2 and internally mixed Ca(NO3)2
Maclean, A. M., Smith, N. R., Li, Y., Huang, Y., Hettiyadura, A. P. S., Crescenzo, G. V., Shiraiwa, M., Laskin, A., Nizkorodov, S. A., and Bertram, A. K.:
Humidity-Dependent Viscosity of Secondary Organic Aerosol from Ozonolysis of β-Caryophyllene: Measurements, Predictions, and Implications,
ACS Earth Sp. Chem.,
5, 305–318, https://doi.org/10.1021/acsearthspacechem.0c00296, 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.
Murphy, D. M., Cziczo, D. J., Froyd, K. D., Hudson, P. K., Matthew, B. M., Middlebrook, A. M., Peltier, R. E., Sullivan, A., Thomson, D. S., and Weber, R. J.:
Single-peptide mass spectrometry of tropospheric aerosol particles,
J. Geophys. Res.-Atmos.,
111, 1–15, https://doi.org/10.1029/2006JD007340, 2006.
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, 233–237, https://doi.org/10.1038/ngeo817, 2010.
Murray, B. J., Haddrell, A. E., Peppe, S., Davies, J. F., Reid, J. P., O'Sullivan, D., Price, H. C., Kumar, R., Saunders, R. W., Plane, J. M. C., Umo, N. S., and Wilson, T. W.: Glass formation and unusual hygroscopic growth of iodic acid solution droplets with relevance for iodine mediated particle formation in the marine boundary layer, Atmos. Chem. Phys., 12, 8575–8587, https://doi.org/10.5194/acp-12-8575-2012, 2012.
Pan, X., Uno, I., Wang, Z., Nishizawa, T., Sugimoto, N., Yamamoto, S., Kobayashi, H., Sun, Y., Fu, P., Tang, X., and Wang, Z.:
Real-time observational evidence of changing Asian dust morphology with the mixing of heavy anthropogenic pollution,
Sci. Rep.-UK,
7, 1–8, https://doi.org/10.1038/s41598-017-00444-w, 2017.
Pant, A., Parsons, M. T., and Bertram, A. K.: Crystallization of aqueous ammonium sulfate particles internally mixed with soot and kaolinite: Crystallization relative humidities and nucleation rates, J. Phys. Chem. A, 110, 8701–8709, https://doi.org/10.1021/Jp060985s, 2006.
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.
Power, R. M., Simpson, S. H., Reid, J. P., and Hudson, A. J.:
The Transition from liquid to solid-like behaviour in ultrahigh viscosity aerosol particles,
Chem. Sci.,
4, 2597–2604, https://doi.org/10.1039/c3sc50682g, 2013.
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, 8014–9, https://doi.org/10.1073/pnas.1219548110, 2013.
Richards, D. S., Trobaugh, K. L., Hajek-Herrera, J., Price, C. L., Sheldon, C. S., Davies, J. F., and Davis, R. D.:
Ion-molecule interactions enable unexpected phase transitions in organic-inorganic aerosol,
Science Advances,
6, 1–12. https://doi.org/10.1126/sciadv.abb5643, 2020a.
Richards, D. S., Trobaugh, K. L., Hajek-Herrera, J., and Davis, R. D.:
Dual-Balance Electrodynamic Trap as a Microanalytical Tool for Identifying Gel Transitions and Viscous Properties of Levitated Aerosol Particles,
Anal. Chem.,
92, 3086–3094, https://doi.org/10.1021/acs.analchem.9b04487, 2020b.
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.
Rovelli, G., Song, Y. C., Maclean, A. M., Topping, D. O., Bertram, A. K., and Reid, J. P.:
Comparison of approaches for measuring and predicting the viscosity of ternary component aerosol particles,
Anal. Chem.,
91, 5074–5082, https://doi.org/10.1021/acs.analchem.8b05353, 2019.
Russell, P. B., Kinne, S. A., and Bergstrom, R. W.:
Aerosol climate effects: local radiative forcing and column closure experiments,
J. Geophys. Res.-Atmos.,
102, 9397–9407, https://doi.org/10.1029/97jd00112, 1997.
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.
Schmedding, R., Rasool, Q. Z., Zhang, Y., Pye, H. O. T., Zhang, H., Chen, Y., Surratt, J. D., Lopez-Hilfiker, F. D., Thornton, J. A., Goldstein, A. H., and Vizuete, W.: Predicting secondary organic aerosol phase state and viscosity and its effect on multiphase chemistry in a regional-scale air quality model, Atmos. Chem. Phys., 20, 8201–8225, https://doi.org/10.5194/acp-20-8201-2020, 2020.
Sellier, M., Grayson, J. W., Renbaum-Wolff, L., Song, M., and Bertram, A. K.: Estimating the viscosity of a highly viscous liquid droplet through the relaxation time of a dry spot, J. Rheol., 59, 733–750, https://doi.org/10.1122/1.4917240, 2015.
Shi, Z., Zhang, D., Hayashi, M., Ogata, H., Ji, H., and Fujiie, W.:
Influences of sulfate and nitrate on the hygroscopic behaviour of coarse dust particles,
Atmos. Environ.,
42, 822–827, https://doi.org/10.1016/j.atmosenv.2007.10.037, 2008.
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., Yee, L. D., Schilling, K. A., Loza, C. L., Craven, J. S., Zuend, A., Ziemann, P. J., and Seinfeld, J. H.: Size distribution dynamics reveal particle-phase chemistry in organic aerosol formation, P. Natl. Acad. Sci. USA, 110, 11746–11750, https://doi.org/10.1073/pnas.1307501110, 2013.
Slade, J. H. and Knopf, D. A.:
Multiphase OH oxidation kinetics of organic aerosol: The role of particle phase state and relative humidity,
Geophys. Res. Lett.,
41, 5297–5306. https://doi.org/10.1002/2014GL060582, 2014.
Song, M., Marcolli, C., Krieger, U. K., Zuend, A., and Peter, T.: Liquid-liquid phase separation and morphology of internally mixed dicarboxylic acids/ammonium sulfate/water particles, Atmos. Chem. Phys., 12, 2691–2712, https://doi.org/10.5194/acp-12-2691-2012, 2012.
Song, M., Liu, P. F., Hanna, S. J., Li, Y. J., Martin, S. T., and Bertram, A. K.: Relative humidity-dependent viscosities of isoprene-derived secondary organic material and atmospheric implications for isoprene-dominant forests, Atmos. Chem. Phys., 15, 5145–5159, https://doi.org/10.5194/acp-15-5145-2015, 2015.
Song, M., Liu, P. F., Hanna, S. J., Zaveri, R. A., Potter, K., You, Y., Martin, S. T., and Bertram, A. K.:
Relative humidity-dependent viscosity of secondary organic material from toluene photo-oxidation and possible implications for organic particulate matter over megacities, Atmos. Chem. Phys., 16, 8817–8830, https://doi.org/10.5194/acp-16-8817-2016, 2016.
Song, M., Maclean, A. M., Huang, Y., Smith, N. R., Blair, S. L., Laskin, J., Laskin, A., DeRieux, W.-S. W., Li, Y., Shiraiwa, M., Nizkorodov, S. A., and Bertram, A. K.:
Liquid–liquid phase separation and viscosity within secondary organic aerosol generated from diesel fuel vapors, Atmos. Chem. Phys., 19, 12515–12529, https://doi.org/10.5194/acp-19-12515-2019, 2019.
Song, Y. C., Ryu, J., Malek, M. A., Jung, H. J., and Ro, C. U.:
Chemical speciation of individual airborne particles by the combined use of quantitative energy-dispersive electron probe X-ray microanalysis and attenuated total reflection Fourier transform-infrared imaging techniques,
Anal. Chem.,
82, 7987–7998, https://doi.org/10.1021/ac1014113, 2010.
Song, Y.-C., Eom, H.-J., Jung, H.-J., Malek, M. A., Kim, H. K., Geng, H., and Ro, C.-U.: Investigation of aged Asian dust particles by the combined use of quantitative ED-EPMA and ATR-FTIR imaging, Atmos. Chem. Phys., 13, 3463–3480, https://doi.org/10.5194/acp-13-3463-2013, 2013.
Song, Y. C., Haddrell, A. E., Bzdek, B. R., Reid, J. P., Bannan, T., Topping, D. O., Percival, C., and Cai, C.:
Measurements and pedictions of binary component aerosol particle viscosity,
J. Phys. Chem. A,
120, 8123–8137, https://doi.org/10.1021/acs.jpca.6b07835, 2016.
Song, Y. C., Ingram, S., Arbon, R. E., Topping, D. O., Glowacki, D. R., and Reid, J. P.: Transient Cavity Dynamics and Divergence from the Stokes-Einstein Equation in Organic Aerosol, Chem. Sci., 11, 2999–3006, https://doi.org/10.1039/C9SC06228A, 2020.
Steimer, S. S., Berkemeier, T., Gilgen, A., Krieger, K. U., Peter, T., Shiraiwa, M., and Ammann, M.:
Shikimic acid ozonolysis kinetics in the transition from liquid aqueous solution to highly viscous glass,
Phys. Chem. Chem. Phys.,
17, 31101–31109, https://doi.org/10.1039/C5CP04544D, 2015.
Stokes, R. H. and Robinson, R. A.:
Interactions in aqueous nonelectrolyte solutions .i. solute-solvent equilibria,
J. Phys. Chem.,
70, 2126–2130, 1966.
Sullivan, R. C., Guazzotti, S. A., Sodeman, D. A., and Prather, K. A.: Direct observations of the atmospheric processing of Asian mineral dust, Atmos. Chem. Phys., 7, 1213–1236, https://doi.org/10.5194/acp-7-1213-2007, 2007.
Usher, C. R., Michel, A. E., and Grassian, V. H.:
Reactions on mineral dust,
Chem. Rev.,
103, 4883–4939, https://doi.org/10.1021/cr020657y, 2003.
Vaden, T. D., Imre, D., Beranek, 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, 824–827, https://doi.org/10.1038/nature09455, 2010.
Wahab, A., Mahiuddin, S., Hefter, G., and Kunz, W.:
Densities, ultrasonic velocities, viscosities, and electrical conductivities of aqueous solutions of Mg(OAc)2 and Mg(NO3)2,
J. Chem. Eng. Data,
51, 1609–1616, https://doi.org/10.1021/je060107n, 2006.
Wallace, B. J. and Preston, T. C.:
Water Uptake and Loss in Viscous Aerosol Particles with Concentration-Dependent Diffusivities,
J. Phys. Chem. A,
123, 3374–3382, https://doi.org/10.1021/acs.jpca.9b00907, 2019.
Wang, G., Zhang, R., Gomez, M. E., Yang, L., Levy Zamora, M., Hu, M., Lin, Y., Peng, J., Guo, S., Meng, J., Li, J., Cheng, C., Hu, T., Ren, Y., Wang, Y., Gao, J., Cao, J., An, Z., Zhou, W., Li, G., Wang, J., Tian, P., Marrero-Ortiz, W., Secrest, J., Du, Z., Zheng, J., Shang, D., Zeng, L., Shao, M., Wang, W., Huang, Y., Wang, Y., Zhu, Y., Li, Y., Hu, J., Pan, B., Cai, L., Cheng, Y., Ji, Y., Zhang, F., Rosenfeld, D., Liss, P. S., Duce, R. A., Kolb, C. E., and Molina, M. J.:
Persistent sulfate formation from London fog to Chinese haze,
P. Natl. Acad. Sci. USA,
113, 13630–13635, https://doi.org/10.1073/pnas.1616540113, 2016.
Wang, L. N., Cai, C., and Zhang, Y. H.: Kinetically determined hygroscopicity and efflorescence of sucrose-ammonium sulfate aerosol droplets under lower RH, J. Phys. Chem. B, 121, 8551–8557, https://doi.org/10.1021/acs.jpcb.7b05551, 2017.
Wang, S., Nan, J., Shi, C., Fu, Q., Gao, S., Wang, D., Cui, H., Saiz-Lopez, A., and Zhou, B.:
Atmospheric ammonia and its impacts on regional air quality over the megacity of Shanghai, China,
Sci. Rep.-UK,
5, 1–13, https://doi.org/10.1038/srep15842, 2015a.
Wang, Y., Ma, J. B., Zhou, Q., Pang, S. F., and Zhang, Y. H.:
Hygroscopicity of mixed glycerol
Winston, P. W. and Bates, D. H.:
Saturated solutions for the control of humidity in biological research,
Ecology,
41, 232–237, 1960.
Xiao, S. and Bertram, A. K.:
Reactive uptake kinetics of NO3 on multicomponent and multiphase organic mixtures containing unsaturated and saturated organics,
Phys. Chem. Chem. Phys,
13, 6628–6636, 2011.
Xu, R., Lam, H. K., Wilson, K. R., Davies, J. F., Song, M., Li, W., Tse, Y.-L. S., and Chan, M. N.: Effect of inorganic-to-organic mass ratio on the heterogeneous OH reaction rates of erythritol: implications for atmospheric chemical stability of 2-methyltetrols, Atmos. Chem. Phys., 20, 3879–3893, https://doi.org/10.5194/acp-20-3879-2020, 2020.
Yli-Juuti, T., Pajunoja, A., Tikkanen, O. P., Buchholz, A., Faiola, C., Väisänen, O., Hao, L., Kari, E., Peräkylä, O., Garmash, O., Shiraiwa, M., Ehn, M., Lehtinen, K., and Virtanen, A.:
Factors controlling the evaporation of secondary organic aerosol from α-pinene ozonolysis,
Geophys. Res. Lett.,
44, 2562–2570, https://doi.org/10.1002/2016GL072364, 2017.
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.
Zaveri, R. A., Shilling, J. E., Zelenyuk, A., Liu, J. M., Bell, D. M., D'Ambro, E. L., Gaston, C., Thornton, J. A., Laskin, A., Lin, P., Wilson, J., Easter, R. C., Wang, J., Bertram, A. K., Martin, S. T., Seinfeld, J. H., and Worsnop, D. R.: Growth kinetics and size distribution dynamics of viscous secondary organic aerosol, Environ. Sci. Technol., 52, 3, 1191–1199, https://doi.org/10.1021/acs.est.7b04623, 2018.
Zdanovskii, A. B.:
Trudy Solyanoi Laboratorii (Transactions of the Salt Laboratory),
Akad. Nauk SSSR,
6, 5–70, 1936.
Zdanovskii, A. B.:
New methods of calculating solubilities of electrolytes in multicomponent systems,
Zh. Fiz. Khim+.,
22, 1478–1485, 1948.
Zhang, Q., Jimenez, J. L., Canagaratna, M. R., Allan, J. D., Coe, H., Ulbrich, I., Alfarra, M. R., Takami, A., Middlebrook, A. M., Sun, Y. L., Dzepina, K., Dunlea, E., Docherty, K., DeCarlo, P. F., Salcedo, D., Onasch, T., Jayne, J. T., Miyoshi, T., Shimono, A., Hatakeyama, S., Takegawa, N., Kondo, Y., Schneider, J., Drewnick, F., Borrmann, S., Weimer, S., Demerjian, K., Williams, P., Bower, K., Bahreini, R., Cottrell, L., Griffin, R. J., Rautiainen, J., Sun, J. Y., Zhang, Y. M., and Worsnop, D. R.:
Ubiquity and dominance of oxygenated species in organic aerosols in anthropogenically-influenced Northern Hemisphere midlatitudes,
Geophys. Res. Lett.,
34, 1–6, https://doi.org/10.1029/2007GL029979, 2007.
Zhang, R., Wang, G., Guo, S., Zamora, M. L., Ying, Q., Lin, Y., Wang, W., Hu, M., and Wang, Y.:
Formation of urban fine particulate matter,
Chem. Rev.,
115, 3803–3855, https://doi.org/10.1021/acs.chemrev.5b00067, 2015.
Zhang, Y., Sanchez, M. S., Douet, C., Wang, Y., Bateman, A. P., Gong, Z., Kuwata, M., Renbaum-Wolff, L., Sato, B. B., Liu, P. F., Bertram, A. K., Geiger, F. M., and Martin, S. T.: Changing shapes and implied viscosities of suspended submicron particles, Atmos. Chem. Phys., 15, 7819–7829, https://doi.org/10.5194/acp-15-7819-2015, 2015.
Zieger, P., Vaisanen, O., Corbin, J. C., Partridge, D. G., Bastelberger, S., Mousavi-Fard, M., Rosati, B., Gysel, M., Krieger, U. K., Leck, C., Nenes, A., Riipinen, I., Virtanen, A., and Salter, M. E.:
Revising the hygroscopicity of inorganic sea salt particles,
Nat. Commun.,
8, 15883, https://doi.org/10.1038/ncomms15883, 2017.
Zobrist, B., Marcolli, C., Pedernera, D. A., and Koop, T.: Do atmospheric aerosols form glasses?, Atmos. Chem. Phys., 8, 5221–5244, https://doi.org/10.5194/acp-8-5221-2008, 2008.
Zobrist, B., Soonsin, V., Luo, B. P., Krieger, U. K., Marcolli, C., Peter, T., and Koop, T.:
Ultra-slow water diffusion in aqueous sucrose glasses,
Phys. Chem. Chem. Phys.,
13, 3514–26, https://doi.org/10.1039/c0cp01273d, 2011.
Zuend, A., Marcolli, C., Luo, B. P., and Peter, T.: A thermodynamic model of mixed organic-inorganic aerosols to predict activity coefficients, Atmos. Chem. Phys., 8, 4559–4593, https://doi.org/10.5194/acp-8-4559-2008, 2008.
Zuend, A., Marcolli, C., Booth, A. M., Lienhard, D. M., Soonsin, V., Krieger, U. K., Topping, D. O., McFiggans, G., Peter, T., and Seinfeld, J. H.: New and extended parameterization of the thermodynamic model AIOMFAC: calculation of activity coefficients for organic-inorganic mixtures containing carboxyl, hydroxyl, carbonyl, ether, ester, alkenyl, alkyl, and aromatic functional groups, Atmos. Chem. Phys., 11, 9155–9206, https://doi.org/10.5194/acp-11-9155-2011, 2011.
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.
We report viscosity of binary mixtures of organic material / H2O and inorganic salts / H2O, as...
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