Why is the Dynamics of Glasses Super-Arrhenius?

Jean-Philippe Bouchaud
Condensed Matter, Disordered Systems and Neural Networks, Disordered Systems and Neural Networks (cond-mat.dis-nn)
2024-02-02 00:00:00
The steep increase of the relaxation time of glass forming liquids upon cooling is traditionally ascribed to an impending entropy crisis: since the system has "nowhere to go", dynamics must come to a halt. This classic argument, due to Adam \& Gibbs, has been bolstered and refined by the development of the Random First Order Transition (RFOT) theory, which fares remarkably well at reproducing most salient experimental facts of super-cooled liquids. All static predictions of RFOT, including the existence of a point-to-set length and the role of pinning sites, have been vindicated by detailed numerical simulations. Yet, there is no consensus that the basic mechanism explaining the glass transition is the one captured by RFOT. Strong doubts have emerged following the observation that adding or removing kinetic constraints can change the relaxation time by orders of magnitude, while leaving thermodynamics unchanged. This is at odds with the idea of a one-to-one mapping between excess entropy and relaxation time. In the following discussion paper presented at the Solvay conference in October 2023, we review areas of consensus and dissent of RFOT with other competing theoretical proposals, and propose possible paths for (partial) reconciliation. We further argue that extensive numerical simulations of the non-linear susceptibility of glasses, in particular in the aging regime, should shed important light on the mechanism at the origin of the super-Arrhenius behaviour of the relaxation time. In any case, more imagination is still needed to come up with experimental, theoretical or numerical ideas that would allow to finally settle the question of why glasses do not flow.
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