Kinetic Monte-Carlo simulation of the homoepitaxial growth of MgO{001} thin films by molecular deposition

A lattice-based kinetic Monte-Carlo (KMC) code has been developed to investigate the MgO{001} crystal growth from deposition of MgO molecules, as a prototypical case of the growth of oxide thin films. The KMC approach has been designed on the basis of an extensive database including all possible diffusion mechanisms. The corresponding activation energies have been computed through first-principles calculations at zero temperature or from Arrhenius plots of the frequencies obtained by molecular dynamics simulations with empirical potentials. Crystal growth occurs layer by layer, as experimentally observed, and the diffusion of admolecules leads to a high capacity of nucleation, which is enhanced by vacancy diffusion. We have characterized the growth through surface roughness, size distribution and density of the islands, and filling ratios of the growing layers. Moreover, we have analysed the influence of each elementary mechanism on the growth. The best quality of the deposited layers is reached for temperatures larger than 700K and for pressures smaller than 0.1Torr. For these conditions, the simulated surface roughness is fully consistent with available experimental results. ► We develop a kinetic Monte-Carlo code to investigate the growth of oxide thin films. ► We model surface diffusion of molecules and vacancies. ► Inclusion of all diffusion mechanisms lead to layers of the highest quality. ► Simulated growth occurs layer by layer with surface roughness in agreement with experiments.