Grain-Boundary Premelting in High-Entropy Transition Metal Carbides

Abstract

Grain-boundary segregation and thermally induced interfacial disordering were investigated in four high-entropy transition metal carbides using Monte Carlo (MC) sampling and molecular dynamics (MD) with the universal MACE-OMAT-0 machine-learning interatomic potential. MC sampling segregated the group-VI element (Cr, Mo, or W) and Zr to grain boundaries, where the group-VI content reached approximately 45 at.%, consistent with STEM-EDS observations. During MD heating, the grain-boundary Lindemann index, a normalized measure of interatomic distance fluctuations, reached the liquid-like threshold of $δ=0.15$ near $1390^{\circ}\mathrm{C}$ for the Cr-containing carbides, $1660^{\circ}\mathrm{C}$ for Mo, and $1890^{\circ}\mathrm{C}$ for W, while the grain interiors remained below the threshold. A chemically random (Cr,Hf,Ta,Ti,Zr)C reference crossed about $60^{\circ}\mathrm{C}$ later and showed less boundary-localized disorder, highlighting the role of interfacial chemistry in premelting. Species-resolved displacements showed enhanced grain-boundary mobility, particularly for carbon. Overall, Cr-rich interfaces showed the earliest and most extensive premelting-like response, followed by Mo- and W-containing boundaries.