On the Statistical Mechanics of Mass Accommodation at Liquid-Vapor Interfaces

Kavli Affiliate: David T. Limmer

| First 5 Authors: Kritanjan Polley, Kevin R. Wilson, David T. Limmer, ,

| Summary:

We propose a framework for describing the dynamics associated with the
adsorption of small molecules to liquid-vapor interfaces, using an intermediate
resolution between traditional continuum theories that are bereft of molecular
detail and molecular dynamics simulations that are replete with them. In
particular, we develop an effective single particle equation of motion capable
of describing the physical processes that determine thermal and mass
accommodation probabilities. The effective equation is parameterized with
quantities that vary through space away from the liquid-vapor interface. Of
particular importance in describing the early time dynamics is the spatially
dependent friction, for which we propose a numerical scheme to evaluate from
molecular simulation. Taken together with potentials of mean force computable
with importance sampling methods, we illustrate how to compute the mass
accommodation coefficient and residence time distribution. Throughout, we
highlight the case of ozone adsorption in aqueous solutions and its dependence
on electrolyte composition.

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