Calculations of diffusion and diffusion-limited processes in Ni3Al using accelerated molecular dynamics

We present a systematic microscopic approach to diffusion and diffusion-limited processes in Ni3Al. These processes have been identified as controlling the deformation of the material under specific circumstances. The embedded atom method calculations are done using kinetic Monte Carlo combined with the Dimer method of finding saddlepoints. We compute the tracer diffusivities as functions of composition and temperature. The comparison with available experiments is good. We find that at temperatures below about 1000 K, the diffusivity is a sharp function of composition, showing a pronounced dip on the Ni-rich side at 76 at.% Ni. This agrees well with experiment, except that the experiments show this structure setting in a temperatures below about 1300 K. We show that the structure arises from the composition dependence of both the vacancy formation energy and pre-exponential of the diffusivity. We also compute the mobility of an anti-phase boundary perpendicular to its plane, and conclude that vacancy-assistance is very plausible. We conclude that the kMC + Dimer method works well for these problems above 700 K but less effectively below, owing to the presence of short-range, low-energy hops that tend to localize the vacancy and lower the efficiency of the calculation.