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Crystallization of hard-sphere glasses |
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AbstractWe study by molecular dynamics the interplay between arrest and crystallization in hard spheres. For state points in the plane of volume fraction ($0.54 ≤ phi ≤ 0.63$) and polydispersity ($0 ≤ s ≤ 0.085$), 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 $φ_g ≈ 0.585$, independent of $s$. Despite this, for $s<0.05$, crystallization occurs at $φ > φ_g$. 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.
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