Relation of the fragility and heat capacity jump in the supercooled liquid region with the shear modulus relaxation in metallic glasses

Abstract

Fragility constitutes a major parameter of supercooled liquids. The phenomenological definition of this quantity is related to the rate of a change of the shear viscosity η at the glass transition temperature. Although a large number of correlations of the fragility with different properties of metallic glasses were reported, an adequate understanding of its physical nature is still lacking. Attempting to uncover this nature, we performed the calculation of the fragility within the framework of the interstitialcy theory (IT) combined with the elastic shoving model. We derived an analytical expression for the fragility, which shows its relation with the high-frequency shear modulus G in the supercooled liquid state. To verify this result, specially designed measurements of η and G were performed on seven Zr-, Cu- and Pd-based metallic glasses. It was found that the fragility calculated from shear modulus relaxation data is in excellent agreement with the fragility derived directly from shear viscosity measurements. We also calculated the heat capacity jump ΔC sql at the glass transition and showed that it is related to the fragility and, consequently, to shear modulus relaxation. The ΔC sql-value thus derived is in a good agreement with experimental data. It is concluded that the fragility and heat capacity jump in the supercooled liquid state can be determined by the evolution of the system of interstitial-type defects frozen-in from the melt upon glass production, as suggested by the IT. This connection is mediated by the high-frequency shear modulus.