Multiple Scenarios of Low-Temperature Nucleation in Simple Liquids

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 Td and the glass transition temperature Tg. At Td, the ratio of the precursor and geometrically frustrated particles reaches the maximum. When Tg<T<Td, 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 Tg, there is a crossover regime, where geometrically frustrated particles percolate and the glass formation strongly slows down the nucleation. When T<Tg, diffusionless nucleation is obstructed due to the weak vibrational motion and the mechanical stability of the glassy state.