Numerical Scaling Studies of Kinetically-Limited Electrochemical Nucleation and Growth with Accelerated Stochastic Simulations

Abstract

A stochastic atomic-scale lattice-based numerical method based on the Exact Lattice First Passage Time method was developed for the simulation of the early stages of kinetically controlled electrochemical nucleation and growth. Electrochemical reaction and surface diffusion on a hexagonal lattice was accounted for in a pristine physical model system that included edge diffusion along steps, and movement over step edges with Ehrlich-Schwöbel barrier. Five cases were investigated: homoexpitaxy, heteroepitaxy, multi-layer growth, terraces, and confined regions. For each, the influence of the physical parameters, deposition conditions, and system geometry on growth morphology was investigated. Simulation based studies of multilayer surface morphology were able to distinguish between layer-by-layer and island growth modes. On stepped terraces, parameter regions associated with he surface diffusion to deposition flux ratio (D/F) and the Ehrlich-Schwöbel barrier were identified under which deposition occurred either at the step edge or by nucleation and growth of islands on the terraces. The probability of growing single crystals in a small confined region was found to scale with D/F and the radius squared.