Crystallization of hard-sphere glasses

Abstract

We study by molecular dynamics the interplay between arrest and crystallization in hard spheres. For state points in the plane of volume fraction ($0.54\le phi\le 0.63$) and polydispersity ($0\le s\le 0.085$), we delineate states that spontaneously crystallize from those that do not. For noncrystallizing (or precrystallization) samples we find isodiffusivity lines consistent with an ideal glass transition at ${\varphi }_g\approx 0.585$, independent of $s$. Despite this, for $s<0.05$, crystallization occurs at $\varphi >{\varphi }_g$. This happens on time scales for which the system is aging, and a diffusive regime in the mean square displacement is not reached; by those criteria, the system is a glass. Hence, contrary to a widespread assumption in the colloid literature, the occurrence of spontaneous crystallization within a bulk amorphous state does not prove that this state was an ergodic fluid rather than a glass.

4 pages, 3 figures

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