Vacancy diffusion barrier spectrum and diffusion correlation in multicomponent alloys

Abstract

Vacancy diffusion serves a crucial role in many important kinetic behaviors and properties of multicomponent alloys. Essential questions, however, persist regarding how chemical complexity affects diffusion and what unique characteristics, if any, set these alloys apart from traditional metals. Using neural network kinetics model, we study vacancy diffusion in NbMoTa alloy across a broad temperature range (2600 to 800 K). Unlike pure metals, the two key diffusion parameters—diffusion correlation factor f and activation energy ΔG m —are not constant in alloys, but instead substantially decrease with decreasing temperature. This temperature dependence arises from a reduced number of active vacancy jump pathways at lower temperatures, leading to more correlated diffusion. Upon examining vacancy diffusion throughout the entire compositional space of the Nb-Mo-Ta system, we discover that the slowest vacancy diffusion surprisingly occurs in the non-equimolar region, rather than the equimolar concentration where the configurational entropy is highest. The diffusion barrier spectrum, characterizing the diffusion energy landscape, is an intrinsic material characteristic, which controls both f and ΔG m and, thereby, the diffusivity. Lastly, we find that the vacancy diffusion rate drops noticeably in the presence of local chemical order in the NbMoTa system, particularly for MoTa alloys with long-range B2 order.