Multiple Scenarios of Low-Temperature Nucleation in Simple Liquids.

Abstract

Usually, sufficient supercooling of a liquid is employed to bypass the free energy barrier and speed up crystallization. However, lowering the temperature T induces new issues competing with the crystallization, e.g., slow particle motion, geometric frustration, and the glass formation, which complicates our understanding of crystal growth. Here we systematically study the low-temperature nucleation kinetics discriminated by the maximum nucleation rate temperature T_{d} and the glass transition temperature T_{g}. At T_{d}, the ratio of the precursor and geometrically frustrated particles reaches the maximum. When T_{g}<T<T_{d}, nucleation kinetics is characterized by the subdiffusive slow particle motion, the high degrees of geometric frustration, and the saturation of precursors. In this regime, nucleation can proceed through the diffusionless-like ordering of precursors. Near T_{g}, there is a crossover regime, where geometrically frustrated particles percolate and the glass formation strongly slows down the nucleation. When T<T_{g}, diffusionless nucleation is obstructed due to the weak vibrational motion and the mechanical stability of the glassy state.