Interatomic repulsion softness directly controls the fragility of supercooled metallic melts

TL;DR

This paper develops an analytical model linking atomic-scale interionic repulsion to the fragility and viscoelastic properties of supercooled metallic melts, enabling tailored alloy design based on electronic structure insights.

Contribution

It introduces a closed-form expression connecting interionic repulsion steepness to fragility, integrating electronic structure parameters with viscoelastic behavior in metallic glasses.

Findings

Fragility correlates linearly with Coulomb and electron-overlap repulsion energies.

The model accurately fits experimental data across various alloys.

Atomic-scale interactions determine macroscopic viscoelastic properties.

Abstract

We present an analytic scheme to connect the fragility and viscoelasticity of metallic glasses to the effective ion-ion interaction in the metal. This is achieved by an approximation of the short-range repulsive part of the interaction, combined with nonaffine lattice dynamics to obtain analytical expressions for the shear modulus, viscosity, and fragility in terms of the ion-ion interaction. By fitting the theoretical model to experimental data, we are able to link the steepness of the interionic repulsion to the Thomas-Fermi screened Coulomb repulsion and to the Born-Mayer valence-electron overlap repulsion for various alloys. The result is a simple closed-form expression for the fragility of the supercooled liquid metal in terms of few crucial atomic-scale interaction and anharmonicity parameters. In particular, a linear relationship is found between the fragility and the energy scales of both the screened Coulomb and the electron-overlap repulsions. This relationship opens up opportunities to fabricate alloys with tailored thermo-elasticity and fragility by rationally tuning the chemical composition of the alloy according to general principles. The analysis presented here brings a new way of looking at the link between the outer-shell electronic structure of metals and metalloids and the viscoelasticity and fragility thereof.