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Preprints
https://doi.org/10.5194/acp-2020-768
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2020-768
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.

  18 Aug 2020

18 Aug 2020

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This preprint is currently under review for the journal ACP.

Toward closure between predicted and observed particle viscosity over a wide range temperature and relative humidity

Sabin Kasparoglu1, Ying Li2, Manabu Shiraiwa2, and Markus Petters1 Sabin Kasparoglu et al.
  • 1NC State University, Department of Marine, Earth, and Atmospheric Sciences, Raleigh, NC, 27695-8208
  • 2University of California, Irvine, Department of Chemistry, Irvine, CA, 92625, USA

Abstract. Atmospheric aerosols can exist in amorphous semi-solid or glassy phase states whose viscosity varies with atmospheric temperature and relative humidity. The temperature and humidity dependence of viscosity has been hypothesized to be predictable from the combination of a water-organic binary mixing rule of the glass transition temperature, a glass transition temperature scaled viscosity fragility parameterization, and a water uptake parameterization. This work presents a closure study between predicted and observed viscosity for sucrose and citric acid. Viscosity and glass transition temperature as a function of water content are compiled from literature data and used to constrain the fragility parameterization. New measurements characterizing viscosity of sub-100 nm particles using the dimer relaxation method are presented. These measurements extend the available data of temperature and humidity dependent viscosity to −28 ºC. Predicted relationships agree well with observations at room temperature and with measured isopleths of constant viscosity at ~107 Pa s and warmer than −28 ºC. Discrepancies at colder temperatures are observed for sucrose particle. Simulations with the kinetic multi-layer model of gas-particle interactions suggest that the observed deviations at colder temperature for sucrose can be attributed to kinetic limitations associated with water uptake at the timescales of the dimer relaxation experiments. Using the available information, updated equilibrium phase-state diagrams (−80 ºC < T < 40 ºC and 0 < RH < 100 %) for sucrose and citric acid are constructed and associated equilibration timescales are identified.

Sabin Kasparoglu et al.

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Sabin Kasparoglu et al.

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Latest update: 29 Sep 2020
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Short summary
Viscosity is important because it determines the lifetime, impact, and fate of particulate matter. We collected new data to rigorously test a framework that that is used to constrain the phase state in global simulations. We find that the framework is accurate as long as appropriate compound specific inputs are available.
Viscosity is important because it determines the lifetime, impact, and fate of particulate...
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