A statistical theory of structure in many-particle systems with local interactions

TL;DR

This paper develops a statistical framework to understand the structure of many-particle systems with local interactions, linking local order measures to symmetry and entropy, with applications to gases, crystals, and liquids.

Contribution

It introduces a universal local order quantifier based on angular redundancy and establishes its relationship with symmetry and configurational entropy.

Findings

The local order quantifier satisfies a universal characterization.

A sharp lower bound relates order to local symmetry.

Closed-form distribution for highly coordinated particles.

Abstract

A theory of structure is formulated for systems of many structureless classical particles with stable local interactions in Euclidean space. Such systems are shown to have their structure in thermodynamic equilibrium determined exactly by a random field of fine local descriptions and approximately by coarsenings thereof. The degree of order in the local cluster consisting of a particle and its neighbors is identified as a universal source of coarse local descriptions and characterized by expressing the behavior of configurational entropy in local microscopic terms. A local measure of the angular redundancy in neighboring particle positions is found to satisfy this characterization and thereby established as a valid local order quantifier. A precise relationship between order and symmetry is obtained by bounding this quantifier sharply from below by a simple function of the local point group and the largest stabilizer under its action on the set of bond pairs. The marginal distribution of the quantifier is given in closed form for highly coordinated particles with broadly distributed bond angles. Applications are made to the ideal gas, perfect crystal, and simple liquid.