Super-Arrhenius slowing down in the metastable liquid of hard spheres

Abstract

It is demonstrated that a straightforward extension of the Arrhenius law accurately describes diffusion in the thermodynamically stable liquid of hard spheres. A sharp negative deviation from this behaviour is observed as the liquid is compressed beyond its stability limit, which can be compared with super-Arrhenius slowing down in supercooled liquids. It is suggested that the observed dynamical transition is caused by extra entropy barriers arising in the free-energy landscape. This interpretation is corroborated by the observation of characteristic anomalies in the geometry of a particle trajectory.

Cited by in corpus (5)

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• Decoupling of diffusion from structural relaxation and spatial heterogeneity in a supercooled simple liquid
• Understanding Dynamics in Coarse-Grained Models: I. Universal Excess Entropy Scaling Relationship
• Cofinement, entropy, and single-particle dynamics of equilibrium hard-sphere mixtures
• The entropic origin of the enhancement of liquid diffusion at the confining wall