Cluster theory of Janus particles

TL;DR

This paper introduces a cluster approximation method for studying Janus particle fluids, effectively capturing the formation and distribution of clusters in the vapor-liquid coexistence region, aligning well with Monte Carlo simulation results.

Contribution

It develops a simplified statistical mechanics approach that separates intra- and inter-cluster effects, providing a new way to analyze clustering in Janus fluids with good agreement to simulations.

Findings

Qualitative agreement with Monte Carlo simulations using ideal-gas approximation.

Improved semi-quantitative results with hard-sphere cluster correlations.

Reveals dependence of cluster distribution on interaction range and thermodynamics.

Abstract

We apply a simple statistical mechanics cluster approximation for studying clustering in the Kern and Frenkel model of Janus fluids. The approach is motivated by recent Monte Carlo simulations work on the same model revealing that the vapor coexisting with the liquid phase contains clusters of different sizes and shapes whose equilibrium concentrations in general depend on the interaction range as well as on thermodynamic parameters. The approximation hinges on a separation between the intra- and inter-cluster contribution to thermodynamics, where only the former is explicitly computed by Monte Carlo simulations. Two levels of a simple liquid theory approximation are exploited for the description of the latter. In the first we use the ideal-gas expressions and obtain a qualitative agreement with extensive Monte Carlo bulk simulations. This can be improved to a semi-quantitative agreement, by using a hard-sphere description for the cluster-cluster correlations.