Automated free energy calculation from atomistic simulations

TL;DR

This paper introduces automated workflows and computational tools for calculating Helmholtz and Gibbs free energies in atomistic simulations, enabling efficient and accurate thermodynamic property predictions across various conditions.

Contribution

The authors develop automated methods for free energy calculations that incorporate non-equilibrium thermodynamics and reversible scaling, enhancing accuracy and efficiency.

Findings

Validated accuracy of free energy calculations with examples.

Demonstrated efficiency in computing across temperature and pressure ranges.

Enabled alchemical and upscaling free energy evaluations.

Abstract

We devise automated workflows for the calculation of Helmholtz and Gibbs free energies and their temperature and pressure dependence and provide the corresponding computational tools. We employ non-equilibrium thermodynamics for evaluating the free energy of solid and liquid phases at a given temperature and reversible scaling for computing free energies over a wide range of temperatures, including the direct integration of $P$-$T$ coexistence lines. By changing the chemistry and the interatomic potential, alchemical and upscaling free energy calculations are possible. Several examples illustrate the accuracy and efficiency of our implementation.