Local structure and dynamics in colloidal fluids and gels

TL;DR

This study investigates the transition from fluid to gel in colloid-polymer mixtures, revealing an intermediate cluster fluid state with finite bond lifetimes and heterogeneous dynamics, using 3D confocal microscopy.

Contribution

It provides detailed 3D structural and dynamical analysis of the fluid-gel transition, identifying a novel cluster fluid state with finite bond lifetimes and heterogeneity.

Findings

Identification of an intermediate 'cluster fluid' state.

Particles in clusters show correlated movement and heterogeneity.

Local structure remains similar between cluster fluid and gel states.

Abstract

Gels in soft-matter systems are an important nonergodic state of matter. We study a colloid-polymer mixture which is quenched by increasing the polymer concentration, from a fluid to a gel. Using confocal microscopy, we study both the static structure and dynamics in three dimensions (3D). Between the dynamically arrested gel and ergodic fluid comprised of isolated particles we find an intermediate 'cluster fluid' state, where the 'bonds' between the colloidal particles have a finite lifetime. The local dynamics are reminiscent of a fluid, while the local structure is almost identical to that of the gel. Simultaneous real-time local structural analysis and particle tracking in 3D at the single-particle level yields the following interesting information. Particles in the clusters move in a highly correlated manner, but, at the same time, exhibit significant dynamical heterogeneity, reflecting the enhanced mobility near the free surface. Deeper quenching eventually leads to a gel state where the 'bond' lifetime exceeds that of the experiment, although the local structure is almost identical to that of the 'cluster fluid'.