On the Statistical Mechanics of Mass Accommodation at Liquid-Vapor Interfaces
Fuente:
arXiv
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| Autores principales: | , , |
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| Formato: | Preprint |
| Publicado: |
2024
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| _version_ | 1866916103873101824 |
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| author | Polley, Kritanjan Wilson, Kevin R. Limmer, David T. |
| author_facet | Polley, Kritanjan Wilson, Kevin R. Limmer, David T. |
| contents | 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. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2401_13234 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | On the Statistical Mechanics of Mass Accommodation at Liquid-Vapor Interfaces Polley, Kritanjan Wilson, Kevin R. Limmer, David T. Chemical Physics Statistical Mechanics 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. |
| title | On the Statistical Mechanics of Mass Accommodation at Liquid-Vapor Interfaces |
| topic | Chemical Physics Statistical Mechanics |
| url | https://arxiv.org/abs/2401.13234 |