Crystal Nucleation and Growth in Liquids: Cooperative Atom Attachment and Detachment

Abstract: Classical theories of crystal nucleation and growth from the liquid assume activated processes that are interface limited, with the atoms individually joining the growing interface by jumps that occur at a rate that is determined by the diffusion coefficient in the liquid phase. These assumptions are in contradiction with the results of molecular dynamics studies that are presented here for supercooled Ni and Al20Ni60Zr20. Instead of diffusion-based attachment across the interface, atoms join the interface by making small changes so as to match the orientational order parameter of the nucleating crystal. Further, instead of joining individually multiple atoms join cooperatively, with the number of cooperative atoms increasing with decreasing temperature.