A theoretical examination of diffusive molecular dynamics

Abstract

Diffusive molecular dynamics is a novel model for materials incorporating atomistic resolution and reaching diffusive time scales. The main ideas of diffusive molecular dynamics are to first minimize an approximate variational Gaussian free energy of the system with respect to the mean atomic coordinates (averaging over many vibrational periods), and to then perform a diffusive step where atoms and vacancies (or two species in a binary alloy) flow on a diffusive time scale via a master equation. We present a mathematical framework for studying this algorithm based on relative entropy, also known as the Kullback-Leibler divergence. This adds flexibility in how the algorithm is implemented and interpreted. We then compare our formulation, relying on relative entropy and absolute continuity of measures, to existing formulations and find agreement.