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.