Structural Origin of the Two-Step Glass Transition

TL;DR

This paper uncovers a structural origin of the two-step glass transition by analyzing local configurations and activation barriers in 2D colloidal rod systems, revealing how rotational freezing precedes translational arrest.

Contribution

It introduces a novel method to analyze structure-dynamics relations and identifies the activation barrier as the key to the two-step glass transition in glasses.

Findings

Identification of a two-step glass transition in 2D colloidal rods.

Discovery of local free energy minima separated by activation barriers.

Activation barrier for rotation causes the sequential freezing of motion.

Abstract

The glass transition is a long-standing problem in physics. Identifying the structural origin of the transition may lead to the ultimate solution to the problem. Here, for the first time, we discover such a structural origin by proposing a novel method to analyze structure-dynamics relation in glasses. An interesting two-step glass transition, with rotational glass transition preceding translational one, is identified experimentally in 2D colloidal rod systems. During the transition, parallel and perpendicularly packed rods are found to form local free energy minima in configurational space, separated by an activation barrier. This barrier increases significantly when rotational glass transition is approached; thereby the rotational motion is frozen while the translational one remains diffusive. We argue that the activation barrier for rotation is the origin of the two-step glass transition. Such an activation barrier between well-defined local configurations holds the key to understand the two-step glass transition in general.