Crystal-liquid interfacial free energy of hard spheres via a novel thermodynamic integration scheme

Abstract

The hard sphere crystal-liquid interfacial free energy, (${\gamma }_{\mathrm{cl}}$), is determined from molecular dynamics simulations using a novel thermodynamic integration (TI) scheme. The advantage of this TI scheme compared to previous methods is to successfully circumvent hysteresis effects due to the movement of the crystal-liquid interface. This is accomplished by the use of extremely short-ranged and impenetrable Gaussian flat walls which prevent the drift of the interface while imposing a negligible free-energy penalty. We find that it is crucial to analyze finite-size effects in order to obtain reliable estimates of ${\gamma }_{\mathrm{cl}}$ in the thermodynamic limit.

arXiv comment10 pages, 6 figures

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Cited by in corpus (5)

• Colloidal Hard Spheres: Triumphs, Challenges and Mysteries
• Crystallization of hard spheres revisited. II. Thermodynamic modeling, nucleation work, and the surface of tension
• Direct calculation of the planar NaCl-aqueous solution interfacial free energy at the solubility limit
• Computation of the solid-liquid interfacial free energy in hard spheres by means of thermodynamic integration
• Free energy cost of forming an interface between a crystal and its frozen version