Spatial and temporal dynamical heterogeneities approaching the binary colloidal glass transition†

We study concentrated binary colloidal suspensions, a model system which has a glass transition as the volume fraction f of particles is increased. We use confocal microscopy to directly observe particle motion within dense samples with f ranging from 0.4 to 0.7. Our binary mixtures have a particle diameter ratio dS/dL 1⁄4 1/1.3 and particle number ratio NS/NL 1⁄4 1.56, which are chosen to inhibit crystallization and enable long-time observations. Near the glass transition we find that particle dynamics are heterogeneous in both space and time. The most mobile particles occur in spatially localized groups. The length scales characterizing these mobile regions grow slightly as the glass transition is approached, with the largest length scales seen being 4 small particle diameters. We also study temporal fluctuations using the dynamic susceptibility c4, and find that the fluctuations grow as the glass transition is approached. Analysis of both spatial and temporal dynamical heterogeneity show that the smaller species play an important role in facilitating particle rearrangements. The glass transition in our sample occurs at fg z 0.58, with characteristic signs of aging observed for all samples with f > fg.