Precursor-Mediated Crystallization Process in Suspensions of Hard Spheres

We report on a large scale computer simulation study of crystal nucleation in hard spheres. Through a combined analysis of real- and reciprocal-space data, a picture of a two-step crystallization process is supported: First, dense, amorphous clusters form which then act as precursors for the nucleation of well-ordered crystallites. This kind of crystallization process has been previously observed in systems that interact via potentials that have an attractive as well as a repulsive part, most prominently in protein solutions. In this context the effect has been attributed to the presence of metastable fluid-fluid demixing. Our simulations, however, show that a purely repulsive system (that has no metastable fluid-fluid coexistence) crystallizes via the same mechanism.