The kinetic fragility of liquids as manifestation of the elastic softening

Abstract

We show that the fragility $m$, the steepness of the viscosity and relaxation time close to the vitrification, increases with the degree of elastic softening, i.e. the decrease of the elastic modulus with increasing temperature, in universal way. This provides a novel connection between the thermodynamics, via the modulus, and the kinetics. The finding is evidenced by numerical simulations and comparison with the experimental data of glassformers with widely different fragilities ($33\le m\le 115$), leading to a fragility-independent elastic master curve extending over eighteen decades in viscosity and relaxation time. The master curve is accounted for by a cavity model pointing out the roles of both the available free volume and the cage softness. A major implication of our findings is that ultraslow relaxations, hardly characterised experimentally, become predictable by linear elasticity. As an example, the viscosity of supercooled silica is derived over about fifteen decades with no adjustable parameters.

7 pages, 6 figures; Added new results, improved the theoretical section

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• Cage effect in supercooled molecular liquids: local anisotropies and collective solid-like response
• Non-Affine Displacements and the Non-Linear Response of a Strained Amorphous Solid
• The Initiation of Shear Band Formation in Deformed Metallic Glasses from Soft Localized Domains