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Kinetics of Stacking-Order Evolution during Heterogeneous Ice Formation
Xudan Huang1,2, Zifeng Yuan3, Chon-Hei Lo3
1Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China.
None:
The selection of stacking order in a broad range of close-packed polymorphic materials remains a challenging enigma. Using in situ cryogenic transmission electron microscopy, we uncover the atomistic mechanisms governing the vapor deposition growth of ice. We find that the heterogeneous ice nucleation and growth undergo recrystallization accompanied by bifurcation, reflecting a coherent epitaxial transition from a cubic-ice embryonic core to hexagonal-ice prismatic dendrites, with intermediate stacking-disordered layers serving as a dynamic fluctuating bridge. Supported by molecular dynamics simulations, these phenomena are attributed to a surface-constrained, symmetry-breaking crystallization preference aligned with the principle of minimizing free energy. Our results highlight the critical role of the combined effects of surface and symmetry in shaping ice crystallization, providing fresh insights into crystal growth mechanisms and guiding principles for the design of advanced materials.
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