Direct observation of liquid nucleus growth in homogeneous melting of colloidal crystals

Abstract

The growth behaviour of liquid nucleus is crucial for crystal melting, but its kinetics is difficult to predict and remains challenging in experiment. Here we directly observed the growth of individual liquid nuclei in homogeneous melting of three-dimensional superheated colloidal crystals with single-particle dynamics by video microscopy. The growth rate of nucleus at weak superheating is well fitted by generalizing the Wilson–Frenkel law of crystallization to melting and including the surface tension effects and non-spherical-shape effects. As the degree of superheating increases, the growth rate is enhanced by nucleus shape fluctuation, nuclei coalescence and multimer attachment. The results provide new guidance for the refinement of nucleation theory, especially for the poorly understood strong-superheating regime. The universal Lindemann parameter observed at the superheat limit and solid–liquid interfaces indicates a connection between homogeneous and heterogeneous melting.

Abstract

Monitoring crystal melting at a single-atom level is challenging because of the small spatial and temporal scales involved, especially for a bulk process. Wang et al. report the melting dynamics of a colloidal crystal with emphasis on the growth of critical nuclei upon different degrees of superheating.