Crystallization and aging in hard-sphere glasses

C Valeriani, E Sanz, E Zaccarelli, W C K Poon, M E Cates, P N Pusey
2011 Journal of Physics: Condensed Matter  
We report new results from our programme of molecular dynamics simulation of hard-sphere systems, focusing on crystallization and glass formation at high concentrations. First we consider a much larger system than hitherto, N = 86 400 equal-sized particles. The results are similar to those obtained with a smaller system, studied previously, showing conventional nucleation and growth of crystals at concentrations near melting and crossing over to a spinodal-like regime at higher concentrations
more » ... er concentrations where the free energy barrier to nucleation appears to be negligible. Second, we investigate the dependence on the initial state of the system. We have devised a Monte Carlo 'constrained aging' method to move the particles in such a way that crystallization is discouraged. After a period of such aging, the standard molecular dynamics programme is run. For a system of N = 3200, we find that constrained aging encourages caging of the particles and slows crystallization somewhat. Nevertheless, both aged and unaged systems crystallize at volume fraction φ = 0.61 whereas neither system shows full crystallization in the duration of the simulation at φ = 0.62, a concentration still significantly below that of random close packing.
doi:10.1088/0953-8984/23/31/319501 fatcat:zh5okhb77nb77ixyoma33jopha