Imperfectly coordinated water molecules pave the way for homogeneous ice nucleation (2304.12665v2)

Abstract: Water freezing is ubiquitous on Earth, affecting many areas from biology to climate science and aviation technology. Probing the atomic structure in the homogeneous ice nucleation process from scratch is of great value but still experimentally unachievable. Theoretical simulations have found that ice originates from the low-mobile region with increasing abundance and persistence of tetrahedrally coordinated water molecules. However, a detailed microscopic picture of how the disordered hydrogen-bond network rearranges itself into an ordered network is still unclear. In this work, we use a deep neural network (DNN) model to "learn" the interatomic potential energy from quantum mechanical data, thereby allowing for large-scale and long molecular dynamics (MD) simulations with ab initio accuracy. The nucleation mechanism and dynamics at atomic resolution, represented by a total of 36 $\mu$s-long MD trajectories, are deeply affected by the structural and dynamical heterogeneity in supercooled water. We find that imperfectly coordinated (IC) water molecules with high mobility pave the way for hydrogen-bond network rearrangement, leading to the growth or shrinkage of the ice nucleus. The hydrogen-bond network formed by perfectly coordinated (PC) molecules stabilizes the nucleus, thus preventing it from vanishing and growing. Consequently, ice is born through competition and cooperation between IC and PC molecules. We anticipate that our picture of the microscopic mechanism of ice nucleation will provide new insights into many properties of water and other relevant materials.