Gamma-point lattice free energy estimates from O(1) force calculations

We present a new method for estimating the vibrational free energy of crystal (and molecular) structures employing only a single force calculation, for a particularly displaced configuration, in addition to the calculation of the ground state configuration. This displacement vector is the sum of the phonon eigenvectors obtained from a fast-relative to, e.g., density-functional theory (DFT)-Hessian calculation using interatomic potentials.

These potentials are based here on effective charges obtained from a DFT calculation of the ground state electronic charge density but could also be based on other, e.g., empiric approaches.