Thermodynamics of glasses: a first principle computation

TL;DR

This paper presents a first-principles computational approach to understanding the thermodynamics of fragile glasses, using a replica method and small cage expansion to derive key thermodynamic properties.

Contribution

It introduces a novel first-principles method for calculating glass thermodynamics from interatomic potentials using replica theory and small cage expansion.

Findings

Computed cage size and specific heat at low temperatures.

Confirmed the Dulong and Petit law for specific heat.

Derived the configurational entropy of glasses.

Abstract

We propose a first principle computation of the thermodynamics of simple fragile glasses starting from the two body interatomic potential. A replica formulation translates this problem into that of a gas of interacting molecules, each molecule being built of $m$ atoms, and having a gyration radius (related to the cage size) which vanishes at zero temperature. We use a small cage expansion, valid at low temperatures, which allows to compute the cage size, the specific heat (which follows the Dulong and Petit law), and the configurational entropy.