Dynamic Heterogeneity, Cooperative Motion, and Johari-Goldstein $\beta$-Relaxation in a Metallic Glass-Forming Material Exhibiting a Fragile to Strong Transition

TL;DR

This study uses molecular dynamics simulations to explore the Johari-Goldstein β-relaxation in a metallic glass-forming alloy, revealing its connection to dynamic heterogeneity, diffusion, and a fragile-to-strong transition.

Contribution

It provides new insights into the microscopic nature of JG β-relaxation and its relation to dynamic heterogeneity and diffusion in a fragile-to-strong metallic glass.

Findings

JG β-relaxation time correlates with mobile particle cluster lifetime

Diffusion of smaller atoms dominates the relaxation process

Fragile-to-strong transition does not significantly alter dynamic heterogeneity

Abstract

We investigate the Johari-Goldstein (JG) $\beta$-relaxation process in a model metallic glass-forming (GF) material (Al90Sm10), previously studied extensively by both frequency-dependent mechanical measurements and simulation studies devoted to equilibrium properties, by molecular dynamics simulations based on validated and optimized interatomic potentials with the primary aim of better understanding the nature of this universal relaxation process from a dynamic heterogeneity (DH) perspective. The present relatively low temperature and long-time simulations reveal a direct correspondence between the JG $\beta$-relaxation time $\tau_{JG}$ and the lifetime of the mobile particle clusters $\tau_M$, defined as in previous DH studies, a relationship dual to the corresponding previously observed relationship between the $\alpha$-relaxation time $\tau_\alpha$ and the lifetime of immobile particle clusters $\tau_{IM}$. Moreover, we find that the average diffusion coefficient D nearly coincides with D$_{Al}$, of the smaller atomic species (Al), and that the hopping time associated with D coincides with $\tau_{JG}$ to within numerical uncertainty, both trends being in accord with experimental studies. This indicates that the JG $\alpha$-relaxation is dominated by the smaller atomic species and the observation of a direct relation between this relaxation process and rate of molecular diffusion in GF materials at low temperatures where the JG $\beta$-relaxation becomes the prevalent mode of structural relaxation. As an unanticipated aspect of our study, we find that Al90Sm10 exhibits fragile-to-strong (FS) glass-formation, as found in many other metallic GF liquids, but this fact does not greatly alter the geometrical nature of DH in this material and the relation of DH to dynamical properties.