Communication: Computing the Tolman length for solid-liquid interfaces

BQ Cheng and M Ceriotti, JOURNAL OF CHEMICAL PHYSICS, 148, 231102 (2018).

DOI: 10.1063/1.5038396

The curvature dependence of interfacial free energy, which is crucial in quantitatively predicting nucleation kinetics and the stability of bubbles and droplets, is quantified by the Tolman length ffi. For solid- liquid interfaces, however, ffi has never been computed directly due to various theoretical and practical challenges. Here we perform a direct evaluation of the Tolman length from atomistic simulations of a solid- liquid planar interface in out-of-equilibrium conditions, by first computing the surface tension from the amplitude of thermal capillary fluctuations of a localized version of the Gibbs dividing surface and by then calculating howmuch the surface energy changes when it is defined relative to the equimolar dividing surface. We computed ffi for a model potential, and found a good agreement with the values indirectly inferred from nucleation simulations. The agreement not only validates our approach but also suggests that the nucleation free energy of the system can be perfectly described using classical nucleation theory if the Tolman length is taken into account. Published by AIP Publishing.

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