Method for computing short-range forces between solid-liquid interfaces driving grain boundary premelting

We present a molecular dynamics based method for accurately computing short-range structural forces resulting from the overlap of spatially diffuse solid-liquid interfaces at wetted grain boundaries close to the melting point. The method is based on monitoring the fluctuations of the liquid layer width at different temperatures to extract the excess interfacial free energy as a function of this width. The method is illustrated for a high-energy Σ9 twist boundary in pure Ni. The short-range repulsion driving premelting is found to be dominant in comparison to long-range dispersion and entropic forces and consistent with previous experimental findings that nanometer-scale layer widths may be observed only very close to the melting point.