Crystallization time scales for polydisperse hard-sphere fluids

Abstract

We study the evolution of crystallization in dense mono- and polydisperse hard sphere fluids, initially quenched to an amorphous configuration. We use as signatures of crystallization both the decay of the reduced pressure Z and the increase in the local and global orientational order parameters Q[over ¯](6). For a given realization of the crystallization process these parameters show sudden changes, both large and small, separated by long periods of quiescence. However, averaging over a large number of realizations, a well-defined scenario for their evolution appears. We find an initial fast relaxation to a disordered state, followed by a period of slow variation, associated to the presence of nucleation events, followed by a fast change, composed of the growth of a few crystals with different orientations, and a final and slow coarsening in a domain-growth process. No clear scaling for this whole process was found. We also find that the transition to an stable glassy fluid is quite sharp as the polydispersity is increased, showing a probable first-order phase transition behavior. A well-defined boundary between crystallizing and permanently amorphous fluids should exist, at least for a region in packing fractions. We looked for segregation at large values of polydispersity, but no effects of this type were found.