Crystal-liquid interfacial free energy via thermodynamic integration
Ronald Benjamin, Jürgen Horbach
2014
Journal of Chemical Physics
A novel thermodynamic integration (TI) scheme is presented to compute the crystal-liquid interfacial free energy (γ_ cl) from molecular dynamics simulation. The scheme is applied to a Lennard-Jones system. By using extremely short-ranged and impenetrable Gaussian flat walls to confine the liquid and crystal phases, we overcome hysteresis problems of previous TI schemes that stem from the translational movement of the crystal-liquid interface. Our technique is applied to compute γ_ cl for the
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... 0), (110) and (111) orientation of the crystalline phase at three temperatures under coexistence conditions. For one case, namely the (100) interface at the temperature T=1.0 (in reduced units), we demonstrate that finite-size scaling in the framework of capillary wave theory can be used to estimate γ_ cl in the thermodynamic limit. Thereby, we show that our TI scheme is not associated with the suppression of capillary wave fluctuations.
doi:10.1063/1.4891220
pmid:25084945
fatcat:emkhnetb2vd63gelbryvomyzdi