In situ observation of colloidal monolayer nucleation driven by an alternating electric field

The nucleation of crystalline materials is a hotly debated subject in the physical sciences(1). Despite the emergence of several theories in recent decades(2-7), much confusion still surrounds the dynamic processes of nucleation(5-7). This has been due in part to the limitations of existing experimental evidence. Charged colloidal suspensions have been used as experimental model systems for the study of crystal nucleation and structural phase transitions(8-12), as their crystallization phase diagram is analogous to that of atomic and molecular systems, but they can be visualized using microscopy. Previously, three-dimensional imaging of colloidal nucleation dynamics was achieved using confocal microscopy(13). However, the limited temporal resolution of the confocal microscope is of concern when trying to capture real-time colloidal crystal nucleation events. Moreover, as the thermodynamic driving force has remained undefined, data on key factors such as the critical nuclei size are at best semiquantitative(13). Here we present real-time direct imaging and quantitative measurements of the pre- and post-nucleation processes of colloidal spheres, and the kinetics of nucleation driven by an alternating electric field, under well-defined thermodynamic driving forces. Our imaging approach could facilitate the observation of other rarely observed phenomena, such as defect and grain-boundary formation(14) and the effects of foreign particles during crystallization(15). Furthermore, it may prove useful in identifying optical and biological technologies based on colloids(16-21).