Competition between Barrier- and Entropy-Driven Activation in Glasses

TL;DR

This paper explores two types of activated dynamics in glasses—energy barrier hopping and entropic activation—showing how their dominance depends on system conditions and can lead to a phase transition at low temperatures.

Contribution

It introduces a framework distinguishing barrier-driven and entropy-driven activation mechanisms in glasses, clarifying their coexistence and dominance based on density of states and temperature.

Findings

Entropic activation can dominate over barrier hopping in glasses.

A phase transition between activation mechanisms can occur at low temperatures.

The framework reconciles facilitation and thermodynamic views of glass slowdown.

Abstract

In simplified models of glasses we clarify the existence of two different kinds of activated dynamics, which coexist, with one of the two dominating over the other. One is the energy barrier hopping that is typically used to picture activation, and the other one, which we call entropic activation, is driven by the scarcity of convenient directions. When entropic activation dominates, the height of the energy barriers is no longer the decisive to describe the system's slowdown. In our analysis, dominance of one mechanism over the other depends on the shape of the density of states and temperature. We also find that at low temperatures a phase transition between the two kinds of activation can occur. Our framework can be used to harmonize the facilitation and thermodynamic pictures of the slowdown of glasses.