Density functional theory of freezing with reference liquid

Abstract

The density functional theory of freezing is reformulated by introducing a reference liquid to describe the thermodynamic properties of the crystalline phase. The density of this liquid, which is a free parameter in the theory, is chosen so that the grand potential of the solid is stationary with respect to this parameter. The introduction of a reference liquid is shown to be equivalent to partial summation of higher-order terms of the perturbation series. The theory is applied to the hard sphere system. The calculated melting parameters as well as the properties of the high-density solid are in very good agreement with Monte Carlo results.