Quantitative modeling of solute drag by vacancies in face-centered-cubic alloys

Transport coefficients, the elements of the so-called Onsager matrix, are essential quantities for modeling solid-state kinetics controlled by diffusion. In a face-centered-cubic structure, drag of solute atoms by vacancies can be caused by solute-vacancy binding at nearest neighbors. In order to investigate solute drag in alloys with interactions up to the third-nearest-neighbor sites, we extend an analytic method: the self-consistent mean field method. With this method, we calculate the Onsager matrix of model alloys to identify kinetic effects arising from individual and collective jump frequencies and assess the results on select cases using atomic kinetic Monte Carlo simulations. Using preexisting density functional theory data from various sources, we show that many impurities have low-temperature solute drag before changing to solute exchange at high temperatures. We evaluate the transition temperature for these alloys between these two regimes and compare the results with available experimental data. Some disagreement is found, which can be due both to experimental and numerical shortcomings. In order to guide diffusion calculations, the sensitivity of the Onsager matrix to the range of the kinetic correlation and to the input density functional theory data is studied.