Structures and dynamics of glass-forming colloidal liquids under spherical confinement

TL;DR

This study experimentally verifies the presence of amorphous-order particle clusters and static correlations in glass-forming colloidal liquids under spherical confinement, linking static structure to dynamic slowdown during the glass transition.

Contribution

The paper introduces a novel colloidal system with spherical confinement to experimentally observe amorphous order and static correlations, confirming theoretical predictions.

Findings

Development of static correlations in confined colloids.

Demonstration of the influence of static correlations on relaxation dynamics.

Quantitative relation between configurational entropy and static length scale.

Abstract

Recent theories predict that when a supercooled liquid approaches the glass transition, particle clusters with a special "amorphous order" nucleate within the liquid, which lead to static correlations dictating the dramatic slowdown of liquid relaxation. The prediction, however, has yet to be verified in 3D experiments. Here, we design a colloidal system, where particles are confined inside spherical cavities with an amorphous layer of particles pinned at the boundary. Using this novel system, we capture the amorphous-order particle clusters and demonstrate the development of a static correlation. Moreover, by investigating the dynamics of spherically confined samples, we reveal a profound influence of the static correlation on the relaxation of colloidal liquids. In analogy to glass-forming liquids with randomly pinned particles, we propose a simple relation for the change of the configurational entropy of confined colloidal liquids, which quantitatively explains our experimental findings and illustrates a divergent static length scale during the colloidal glass transition.