Does the repulsive interatomic potential determine fragility in metallic liquids?

TL;DR

This study links the fragility of metallic liquids to the steepness of their repulsive interatomic potentials, providing experimental evidence that stronger liquids exhibit steeper repulsive interactions.

Contribution

It demonstrates experimentally that the microscopic origin of fragility in metallic liquids is related to the steepness of the repulsive part of the interatomic potential.

Findings

Stronger metallic liquids have steeper repulsive potentials.

Fragility correlates with the steepness of the pair distribution function.

Experimental data from ten metallic alloys support this relationship.

Abstract

The dynamical behavior of liquids is frequently characterized by the fragility, which can be defined from the temperature dependence of the shear viscosity, {\eta}. For a strong liquid, the activation energy for {\eta} changes little with cooling towards the glass transition temperature, Tg. The change is much greater in fragile liquids, with the activation energy becoming very large near Tg. While fragility is widely recognized as an important concept, for example believed to play an important role in glass formation, the microscopic origin of fragility is poorly understood. Here, we present new experimental evidence showing that fragility reflects the strength of the repulsive part of the interatomic potential, which can be determined from the steepness of the pair distribution function near the hard-sphere cutoff. Based on an analysis of scattering data from ten different metallic alloy liquids, we show that stronger liquids have steeper repulsive potentials.