Beyond packing of hard spheres: The effects of core softness, non-additivity, intermediate-range repulsion, and many-body interactions on the glass-forming ability of bulk metallic glasses

TL;DR

This study uses molecular dynamics simulations to explore how features beyond hard-sphere interactions, like core softness and many-body effects, influence the glass-forming ability of bulk metallic glasses, revealing that hard-core interactions are most influential.

Contribution

It systematically investigates the impact of interatomic potential features beyond hard-sphere models on the glass-forming ability of BMGs using advanced simulations.

Findings

Hard-core interactions dominate GFA in alloys.

Other potential features modify GFA by 1-2 orders of magnitude.

Tuning many-body interactions affects pure metal GFA.

Abstract

When a liquid is cooled well below its melting temperature at a rate that exceeds the critical cooling rate $R_c$, the crystalline state is bypassed and an amorphous glassy state forms instead. $R_c$ (or the corresponding critical casting thickness $d_c$) characterizes the glass-forming ability (GFA) of each material. While silica is an excellent glass-former with small $R_c<10^{-2}$ K/s, pure metals and most alloys are poor glass-formers with large $R_c>10^{10}$ K/s. Only in the past thirty years have bulk metallic glasses (BMGs) been identified with $R_c$ approaching that for silica. Recent simulations have shown that hard-sphere models are able to identify the atomic size ratio and number fraction regime where BMGs exist with critical cooling rates more than 13 orders of magnitude smaller than those for pure metals. However, there are many other features of interatomic potentials beyond hard-core interactions. How do these other features affect the glass-forming ability of BMGs? We perform molecular dynamics simulations to determine how variations in the softness and non-additivity of the repulsive core and form of the interatomic pair potential at intermediate distances affect the GFA of binary alloys. These variations in the interatomic pair potential allow us to introduce geometric frustration and change the crystal phases that compete with glass formation. We also investigate the effect of tuning the strength of the many-body interactions from zero to the full embedded atom model on the GFA for pure metals. We then employ the full embedded atom model for binary BMGs and show that hard-core interactions play the dominant role in setting the GFA of alloys, while other features of the interatomic potential only change the GFA by one to two orders of magnitude.