Direct determination of Lennard-Jones crystal surface free energy by a computational cleavage method

AO Tipeev and JP Rino and ED Zanotto, JOURNAL OF CHEMICAL PHYSICS, 155, 094101 (2021).

DOI: 10.1063/5.0059882

The surface free energy of solids, gamma, plays a crucial role in all physical and chemical processes involving material surfaces. For the first time, we obtained gamma directly from molecular dynamics simulations using a crystal cleavage method. The approach was successfully realized in a Lennard-Jones system by inserting two movable external walls, each consisting of a single crystal layer, into a bulk crystal to create flat, defect-free surfaces. The cleavage technique designed allowed us to calculate the surface free energy according to its definition and avoid surface premelting. The temperature dependence of gamma was determined for the (100) and (110) crystal planes along the whole sublimation line and its metastable extension, up to T = 1.02 . T-m, where T-m is the melting point. Good agreement with indirect values of gamma(T) was found. The proposed computational cleavage method can be applied to other solids of interest, providing valuable insight into the understanding of chemical and physical surface processes, and demonstrates the successful import of the cleavage method, traditionally used in technical preparation and study of crystal surfaces, into a modern atomistic simulation.

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