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Crystallization of fluids: Free-energy functional for symmetry breaking first-order freezing transition

A free-energy functional for a crystal that contains both the symmetry conserved and symmetry broken parts of the direct pair correlation function is developed. To test how accurately this free-energy functional describes the symmetry breaking first-order phase transition of freezing, we use it to investigate the crystallization of fluids interacting via the inverse power potential; u(r)=ϵ(σ/r)n. In agreement with simulation results we find that under the fluid-solid co-existence the f.c.c. structure is more stable for n=12, whereas for soft repulsions (n⩽6) the b.c.c. structure is more stable.