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Usually, supercooled liquids and glasses are thermodynamically unstableagainst crystallization. Classical nucleation theory (CNT) has been used todescribe the crystallization dynamics of supercooled liquids. However, recentstudies on overcompressed hard spheres show that their crystallization dynamicsare intermittent and mediated by avalanche-like rearrangements of particles,which largely differ from the CNT. These observations suggest that thecrystallization times of deeply supercooled liquids or glasses cannot bedescribed by the CNT, but this point has not yet been studied in detail. Inthis paper, we use molecular dynamics simulations to study the crystallizationdynamics of soft spheres just after an instantaneous quench. We show thatalthough the equilibrium relaxation time increases in a super-Arrhenius mannerwith decreasing temperature, the crystallization time shows an Arrheniustemperature dependence at very low temperatures. This is contrary to theconventional formula based on the CNT. Furthermore, the estimated energybarrier for the crystallization is surprisingly small compared to that for theequilibrium dynamics. By comparing the crystallization and aging dynamicsquantitatively, we show that a coupling between aging and crystallization isthe key for understanding the rapid crystallization of deeply supercooledliquids or glasses.

Arrhenius temperature dependence of the crystallization time of deeply supercooled liquids