Decoupling of rotation and translation at the colloidal glass transition

Abstract: Little is known about the coupling of rotation and translation in dense systems. Here, we report results of confocal fluorescence microscopy where simultaneous recording of translational and rotational particle trajectories from a bidisperse colloidal dispersion is achieved by spiking the samples with rotational probe particles. The latter consist of colloidal particles containing two fluorescently labelled cores suited for tracking the particle's orientation. A comparison of the experimental data with event driven Brownian simulations gives insight into the system's structure and dynamics close to the glass transition and sheds new light onto the translation-rotation coupling. The data show that with increasing volume fractions, translational dynamics slows down drastically, whereas rotational dynamics changes very little. We find convincing agreement between simulation and experiments, even though the simulations neglect far-field hydrodynamic interactions. An additional analysis of the glass transition following mode coupling theory works well for the structural dynamics but indicates a decoupling of the diffusion of the smaller particle species. The shear stress correlations do not decorrelate in the simulated glass states and are not affected by rotational motion.