One of the biggest unresolved problems in crystallization phenomena is the significant discrepancy in the nucleation rate between experiments and simulations even for the simplest liquid, i.e., the hard-sphere system.… Click to show full abstract
One of the biggest unresolved problems in crystallization phenomena is the significant discrepancy in the nucleation rate between experiments and simulations even for the simplest liquid, i.e., the hard-sphere system. A popular explanation for this discrepancy is the neglect of hydrodynamic interactions (HI) in simulation studies. By comparing simulations with and without HI, we show that the long-time diffusive dynamics of the colloids is slowed down more rapidly by hydrodynamic lubrication effects with increasing volume fraction. We find that the kinetics of both nucleation and growth are controlled by this long-time diffusion and that it is possible to account for most of the effects of HI by rescaling with this timescale. Therefore, we conclude that HI is not the primary cause of the accelerated nucleation rates observed in experiments.
               
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