Kinetic Monte Carlo modeling of oxide thin film growth

In spite of the increasing interest in and application of ultrathin film oxides in commercial devices, the understanding of the mechanisms that control the growth of these films at the atomic scale remains limited and scarce. This limited understanding prevents the rational design of novel solutions based on precise control of the structure and properties of ultrathin films. Such a limited understanding stems in no minor part from the fact that most of the available modeling methods are unable to access and robustly sample the nanosecond to second timescales required to simulate both atomic deposition and surface reorganization at ultrathin films. To contribute to this knowledge gap, here we have combined molecular dynamics and adaptive kinetic Monte Carlo simulations to study the deposition and growth of oxide materials over an extended timescale of up to ∼0.5 ms. In our pilot studies, we have examined the growth of binary oxide thin films on oxide substrates. We have investigated three scenarios: (i) the lattice parameter of both the substrate and thin film are identical, (ii) the lattice parameter of the thin film is smaller than the substrate, and (iii) the lattice parameter is greater than the substrate. Our calculations allow for the diffusion of ions between deposition events and the identification of growth mechanisms in oxide thin films. We make a detailed comparison with previous calculations. Our results are in good agreement with the available experimental results and demonstrate important limitations in former calculations, which fail to sample phase space correctly at the temperatures of interest (typically 300-1000 K) with self-evident limitations for the representative modeling of thin films growth. We believe that the present pilot study and proposed combined methodology open up for extended computational support in the understanding and design of ultrathin film growth conditions tailored to specific applications.