Fast Dynamics in a Model Metallic Glass-forming Material

Abstract

We investigate the fast $\beta$- and Johari-Goldstein (JG) $\beta$-relaxation processes, along with the elastic scattering response of glass-forming (GF) liquids and the Boson peak, in a simulated Al-Sm GF material exhibiting a fragile-strong (FS) transition. These dynamical processes are universal in 'ordinary' GF fluids and collectively describe their 'fast dynamics', and we find these relaxation processes also arise in a GF liquid exhibiting a fragile-strong transition. String-like particle motion, having both an irreversible and reversible nature ('stringlets') component, occurs in the fast-dynamics regime, corresponding to a ps timescale. String-like collective motion associated with localized unstable modes facilitate irreversible and intermittent particle 'jumping' events at long times associated with the JG $\beta$-relaxation process, while stringlets associated with localized stable modes and corresponding perfectly reversible atomic motion give rise to the Boson peak. To further clarify the origin of the Boson peak, we calculate the density of states for both the stringlet particles and the 'normal' particles and find that the stringlet particles give rise to a Boson peak while the normal atoms do not. The growth of stringlets upon heating ultimately also leads to the 'softening' of these excitations, and the Boson peak frequency and shear modulus drop in concert with this softening. The growth of string-like collective motion upon heating in the fast-dynamics regime is further shown to be responsible for the growth in the intensity of the fast relaxation process. Relaxation in cooled liquids clearly involves a hierarchy of relaxation processes acting on rather different time and spatial scales.

arXiv commentAccepted for publication in the Journal of Chemical Physics

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