Local structure and dynamics in colloidal fluids and gels

¹  Institute of Industrial Science, University of Tokyo - Meguro-ku, Tokyo 153-8505, Japan
²  School of Chemistry, University of Bristol - Bristol BS8 1TS, UK, EU

Corresponding authors: paddy.royall@bristol.ac.uk tanaka@iis.u-tokyo.ac.jp

Received: 30 July 2008
Accepted: 7 October 2008

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”.