Two-step crystallization kinetics in colloidal hard-sphere systems

The crystallization kinetics of colloidal hard spheres was studied using a special Bragg spectrometer with high sensitivity. In contrast with the classical scenario we observe a two-step nucleation process: the number of crystallites increases slowly at early times, followed by a dramatic reduction at intermediate times, prior to undergoing a rapid increase at late times. We explain these results in terms of a polydispersity limited growth of crystallites, where the crystallization at early times is governed by local fractionation processes, leading to a long delay prior to final crystallization.