Interfacial undercooling in solidification of colloidal suspensions: Analyses with quantitative measurements

Interfacial undercooling in the complex solidification of colloidal suspensions is of significance and remains a puzzling problem. Two types of interfacial undercooling are supposed to be involved in the freezing of colloidal suspensions, i.e., solute constitutional supercooling (SCS) caused by additives in the solvent and particulate constitutional supercooling (PCS) caused by particles. However, quantitative identification of the interfacial undercooling in the solidification of colloidal suspensions, is still absent; thus, the question of which type of undercooling is dominant in this complex system remains unanswered. Here, we quantitatively measured the static and dynamic interface undercoolings of SCS and PCS in ideal and practical colloidal systems. We show that the interfacial undercooling primarily comes from SCS caused by the additives in the solvent, while PCS is minor. This finding implies that the thermodynamic effect of particles from the PCS is not the fundamental physical mechanism for pattern formation of cellular growth and lamellar structure in the solidification of colloidal suspensions, a general case of ice-templating method. Instead, the patterns in the ice-templating method can be controlled effectively by adjusting the additives.