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Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
https://doi.org/10.5194/acp-2017-424
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
Research article
06 Jun 2017
Review status
This discussion paper is under review for the journal Atmospheric Chemistry and Physics (ACP).
Maxwell-Stefan diffusion: a framework for predicting condensed phase diffusion and phase separation in atmospheric aerosol
Kathryn Fowler, Paul J. Connolly, David O. Topping, and Simon O'Meara University of Manchester, School of Earth, Atmospheric and Environmental Science
Abstract. The composition of atmospheric aerosol particles has been found to influence their micro-physical properties and their interaction with water vapour in the atmosphere. Core-shell models have been used to investigate the relationship between composition, viscosity and equilibration time-scales. These models have traditionally relied on the Fickian laws of diffusion with no explicit account of non-ideal interactions. We introduce the Maxwell-Stefan diffusion framework as an alternative method, which explicitly accounts for non-ideal interactions through activity coefficients. E-folding time is the time it takes for the difference in surface and bulk concentration to change by an exponential factor and was used to investigate the interplay between viscosity and solubility and the effect this has on equilibration time-scales within individual aerosol particles. The e-folding time was estimated after instantaneous increases in relative humidity to binary systems of water and an organic component. At low water mole fractions, viscous effects were found to dominate mixing. However, at high water mole fractions, equilibration times were more sensitive to a range in solubility, shown through the greater variation in e-folding times. This is the first time the Maxwell-Stefan framework has been applied to an atmospheric aerosol core-shell model and shows that there is a complex interplay between the viscous and solubility effects on aerosol composition that requires further investigation.

Citation: Fowler, K., Connolly, P. J., Topping, D. O., and O'Meara, S.: Maxwell-Stefan diffusion: a framework for predicting condensed phase diffusion and phase separation in atmospheric aerosol, Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-424, in review, 2017.
Kathryn Fowler et al.
Kathryn Fowler et al.
Kathryn Fowler et al.

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This is the first time the Maxwell-Stefan framework has been applied to an atmospheric aerosol core-shell model and shows that there is a complex interplay between the viscous and solubility effects on aerosol composition. Understanding aerosol composition is essential to accurately model their interactions within atmospheric systems. We use simple binary systems to demonstrate how viscosity and solubility both play a role in affecting the rate of diffusion through aerosol particles.
This is the first time the Maxwell-Stefan framework has been applied to an atmospheric aerosol...
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