The entropy multiparticle-correlation expansion for a mixture of spherical and elongated particles

TL;DR

This paper derives a new multiparticle-correlation expansion for the excess entropy of classical particle mixtures, providing a theoretical basis for entropy-based ordering criteria applicable to colloidal systems with spherical and elongated particles.

Contribution

It introduces a novel approach to derive the multiparticle-correlation expansion of excess entropy, clarifying the significance of each term and applying it to mixtures of spherical and rod-like particles.

Findings

Provides a theoretical framework for entropy-based ordering in particle mixtures.

Details the case of spherical and rod-like particles in colloidal systems.

Discusses symmetries in pair-distribution functions under geometrical constraints.

Abstract

We derive the multiparticle-correlation expansion of the excess entropy of classical particles in the canonical ensemble using a new approach that elucidates the rationale behind each term in the expansion. This formula provides the theoretical framework for an entropy-based ordering criterion that has been already tested for a variety of model fluids and thermodynamic phenomena. In view of future investigations of the phase diagram of colloidal mixtures, we detail in this paper the case of a two-component system of spherical and rod-like particles and discuss the symmetries underlying both the self and distinct pair-distribution functions under various geometrical constraints.