Automated free energy calculation from atomistic simulations

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.