Why are glass-forming liquids non-Arrhenius?

Abstract

A major mystery of glass-forming liquids is the non-Arrhenius temperature-dependence of the average relaxation time. This paper briefly reviews the classical phenomenological models for this phenomenon - the free-volume model and the entropy model - and critiques against these models. We then discuss a recent model [Dyre, Olsen, and Christensen, Phys. Rev. B 53, 2171 (1996)] according to which the activation energy for the average relaxation time is determined by the work done in shoving aside the surrounding liquid to create space needed for a flow event. In this model the non-Arrhenius temperature-dependence is a consequence of the fact that the instantaneous (infinite-frequency) shear modulus increases upon cooling.