Dynamical heterogeneity and the freezing transition in hard-sphere suspensions: Further analysis of the mean square displacement and the velocity autocorrelation function

The velocity autocorrelation function is derived from the mean-squared displacement measured on a colloidal suspension of particles with hard-sphere-like interactions. It decays to zero from below and follows a stretched exponential function of delay time for the thermodynamically stable suspension. For the metastable suspension a power-law decay emerges. The results are discussed in terms of the classical Lorentz gas and the model that describes diffusion confined to one dimension. With the aid of these models, the experimental results provide a characterization of the dynamical heterogeneities which are observed microscopically, and an explanation for the enhanced resistance to flow and diffusion usually found in undercooled fluids upon approaching the glass transition.