A fast anharmonic free energy method with an application to vacancies in ZrC

Abstract

We propose an approach to calculate the anharmonic part of the volumetric-strain and temperature dependent free energy of a crystal. The method strikes an effective balance between accuracy and computational efficiency, showing a $\times 10$ speed-up on comparable free energy approaches at the level of density functional theory, with average errors less than 1 meV/atom. As a demonstration we make new predictions on the thermodynamics of substoichiometric ZrC${}_x$, including vacancy concentration and heat capacity.

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