Explicit Solvents Reverse Temperature Dependence of Phase Behavior in Charged Fluids

Pierre J. Walker; Zhen-Gang Wang

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arXiv · 2610.14366

Explicit Solvents Reverse Temperature Dependence of Phase Behavior in Charged Fluids

Pierre J. Walker·Zhen-Gang Wang

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Abstract

In most theories of electrolyte and polyelectrolyte solutions, the solvent is treated implicitly as a dielectric continuum. While this approximation has enabled major advances, it neglects coupling between ionic and dipolar degrees of freedom. Using molecular dynamics simulations and the mean-spherical approximation, we show that this coupling qualitatively alters electrostatically driven phase behaviour. At finite ion concentrations, many-body ion-dipole correlations reverse the temperature dependence of effective electrostatic interactions, leading to upper-critical solution temperature (UCST) behaviour in direct contrast to the lower-critical solution temperature (LCST) behaviour predicted by implicit-solvent electrostatic theories. This phase reversal arises from ion-induced suppression of local dipolar screening, a collective effect inaccessible to pairwise implicit-solvent descriptions.

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Pierre J. Walker, Zhen-Gang Wang. 2026-10-09. Explicit Solvents Reverse Temperature Dependence of Phase Behavior in Charged Fluids. https://arxiv.org/abs/2610.14366

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