A quantitative theory and atomistic simulation study on the soft-sphere crystal–melt interfacial properties. I. Kinetic coefficients

Abstract

By employing non-equilibrium molecular dynamics (NEMD) simulations and time-dependent Ginzburg–Landau (TDGL) theory for solidification kinetics [Cryst. Growth Des. 20, 7862 (2020)], we predict the kinetic coefficients of FCC(100) crystal–melt interface (CMI) of soft-spheres modeled with an inverse-sixth-power repulsive potential. The collective dynamics of the local interfacial liquid phase at the equilibrium FCC(100) CMIs are calculated based on a recently proposed algorithm [J. Chem. Phys. 157, 084 709 (2022)] and are employed as the resulting parameter that eliminates the discrepancy between the predictions of the kinetic coefficient using the NEMD simulations and the TDGL solidification theory. A speedup of the two modes of the interfacial liquid collective dynamics (at wavenumbers equal to the principal and the secondary reciprocal lattice vector of the grown crystal) is observed. With the insights provided by the quantitative predictive theory, the variation of the solidification kinetic coefficient along the crystal–melt coexistence boundary is discussed. The combined methodology (simulation and theory) presented in this study could be further applied to investigate the role of the inter-atomic potential (e.g., softness parameter s = 1/n of the inverse-power repulsive potential) in the kinetic coefficient.