Role of dynamic heterogeneities in crystal nucleation kinetics in an oxide supercooled liquid.

The temperature at which the classical critical nucleus size is equal to the average size of the cooperatively rearranging regions (CRR) in a supercooled liquid has been referred to as a "cross-over" temperature. We show, for the first time, using published nucleation rate, viscosity, and thermo-physical data, that the cross-over temperature for the lithium disilicate melt is significantly larger than the temperature of the kinetic spinodal and is equal or close to the temperature corresponding to the maximum in the experimentally observed nucleation rates. We suggest that the abnormal decrease in nucleation rates below the cross-over temperature is most likely because, in this regime, the CRR size controls the critical nucleus size and the nucleation rate. This finding links, for the first time, measured nucleation kinetics to the dynamic heterogeneities in a supercooled liquid.