Kinetic Monte Carlo study of the effect of hydrogen on the two-dimensional epitaxial growth of Ni(100)

The effects of hydrogen on Ni(100) submonolayer homoepitaxy have been investigated by kinetic Monto Carlo (KMC) simulations of the Ni growth process with and without the presence of a small hydrogen impurity. The two-dimensional KMC simulations are based upon rate constants for a set of uncorrelated Ni site-to-site hopping mobilities with and without the presence of hydrogen atoms which an found to act as a catalyst. The rate constant activation energies are determined by classical-potential total-energy calculations with semiclassical zero-point energy corrections for the hydrogen atom. This set of KMC simulations extends preliminary work on the activation energies which were reported along with their connection to available experiments in Ref. 1. We find that fast diffusion of H atoms occurs on the flat Ni(100) surface and the presence of these highly mobile H atoms is found to have significant effects on the mobility of lone Ni adatoms, and therefore also on the Ni islands which form during the epitaxial growth. The 11 atoms increase the mobility of lone Ni adatoms across the flat Ni(100) terrace by stabilizing the transition state for site-to-site hopping of the Ni adatom. While the effects of the H atom on the Ni mobility are primarily catalytic, the kinetically determined Ni island morphologies differ substantially as a function of 11 atom concentration over time periods which are long on the deposition time scale, and therefore the morphology differences can become frozen in place. Even quite low 11 atom coverage, by acting to increase lone Ni atom mobility, tends to decrease Ni island density which results in a corresponding increase in the average Ni island size. This suggests that the H atoms are acting as an antisurfactant in the Ni(100) homoepitaxy at low H coverage. [S0163-1829(99)06339-0].