Effective Surface Free Energy of Crystalline Phase Nuclei

Molecular-dynamics simulation by the mean lifetime, forward flux sampling, and seeding method has been employed to study the kinetics of the spontaneous crystallization of a supercooled Lennard-Jones liquid. The limiting values of supercooling (supercompression) of a liquid phase have been determined within wide ranges of temperature and pressure, with nucleation rate being varied by 195 orders of magnitude. The dependence of the effective surface free energy of crystalline phase nuclei on the dividing surface curvature has been calculated from the obtained data with the use of the classical nucleation theory. The calculations have been performed for three isotherms and four isobars. The first (Tolman length) and second corrections to the effective surface free energy for the interface curvature have been determined.