Bayesian inference of atomic diffusivity in a binary NI/AL system based on molecular dynamics

This work focuses on characterizing the integral features of atomic diffusion in Ni/Al nanolaminates based on molecular dynamics (MD) computations. Attention is focused on the simplified problem of extracting the diffusivity, D, in an isothermal system at high temperature. To this end, a mixing measure theory is developed that relies on analyzing the moments of the cumulative distribution functions (CDFs) of the constituents. The mixing measures obtained from replica simulations are exploited in a Bayesian inference framework, based on contrasting these measures with corresponding moments of a dimensionless concentration evolving according to a Fickian process. The noise inherent in the MD simulations is described as a Gaussian process, and this hypothesis is verified both a priori and using a posterior predictive check. Computed values of D for an initially unmixed system rapidly heated to 1500 K are found to be consistent with experimental correlation for diffusion of Ni into molten Al. On the contrary, large discrepancies with experimental predictions are observed when D is estimated based on large-time mean-square displacement (MSD) analysis, and when it is evaluated using the Arrhenius correlation calibrated against experimental measurements of self-propagating front velocities. Implications are finally drawn regarding extension of the present work and potential refinement of continuum modeling approaches.