On the microscopic origin of Soret coefficient minima in liquid mixtures

Temperature gradients induce mass separation in mixtures in a process called thermodiffusion and quantified by the Soret coefficient. The existence of minima in the Soret coefficient of aqueous solutions was controversial until fairly recently, where a combination of experiments and simulations prov...

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Bibliographic Details
Published in:arXiv.org 2022-07
Main Authors: Gittus, Oliver R, Bresme, Fernando
Format: Article
Language:English
Subjects:
Aqueous solutions
Atomic structure
Minima
Mixtures
Soret coefficient
Online Access:Get full text
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Summary:Temperature gradients induce mass separation in mixtures in a process called thermodiffusion and quantified by the Soret coefficient. The existence of minima in the Soret coefficient of aqueous solutions was controversial until fairly recently, where a combination of experiments and simulations provided evidence for the existence of this physical phenomenon. However, the physical origin of the minima and more importantly its generality, e.g. in non-aqueous liquid mixtures, is still an outstanding question. We report the existence of a minimum in liquid mixtures of non-polar liquids modelled as Lennard-Jones mixtures, demonstrating the generality of this phenomenon. The Soret coefficient minimum originates from a coincident minimum in the thermodynamic factor, and hence denotes a maximimzation of non-ideality mixing conditions. We explain the microscopic origin of this effect in terms of the atomic coordination structure of the mixtures.
ISSN:2331-8422
DOI:10.48550/arxiv.2207.12864