Exchange-correlation contributions to thermodynamic properties of the homogeneous electron gas from a cumulant Green's function approach

Abstract

Thermodynamic properties of the interacting homogeneous electron gas are calculated using a finite-temperature cumulant Green's function approach over a broad range of densities and temperatures up to the warm dense matter regime $T\ensuremath{\sim}{T}_{F}$, where ${T}_{F}$ is the Fermi degeneracy temperature. These properties can be separated into independent particle and exchange-correlation contributions, and our focus here is on the latter. Our approach is based on the Galitskii-Migdal-Koltun and electron number sum rules from the finite temperature many-body Green's function formalism, together with an extension of the cumulant Green's function to finite temperature. Previously this approach yielded exchange-correlation energies and potentials in good agreement with quantum Monte-Carlo calculations. Here the method is extended for various thermodynamic quantities including the chemical potential, total energy, Helmholtz free-energy, electronic equation of state, specific heat, and isothermal compressibility, which optionally include spin dependence. We find that the exchange-correlation contributions are weakly varying at low temperature but exhibit significant temperature dependence in the WDM regime, as well as a crossover from exchange- to correlation-dominated behavior. In contrast to the $T={0}^{+}$ limit, we also find that renormalization effects are largely but not completely suppressed at finite temperature. Comparisons with other approaches at various levels of approximation are also discussed.