Tracking cubic ice at molecular resolution

XD Huang and LF Wang and KY Liu and L Liao and HC Sun and JL Wang and XZ Tian and Z Xu and WL Wang and L Liu and Y Jiang and J Chen and EE Wang and XD Bai, NATURE, 617, 86-+ (2023).

DOI: 10.1038/s41586-023-05864-5

Ice is present everywhere on Earth and has an essential role in several areas, such as cloud physics, climate change and cryopreservation. The role of ice is determined by its formation behaviour and associated structure. However, these are not fully understood(1). In particular, there is a long-standing debate about whether water can freeze to form cubic ice-a currently undescribed phase in the phase space of ordinary hexagonal ice(2-6). The mainstream view inferred from a collection of laboratory data attributes this divergence to the inability to discern cubic ice from stacking-disordered ice-a mixture of cubic and hexagonal sequences(7-11). Using cryogenic transmission electron microscopy combined with low-dose imaging, we show here the preferential nucleation of cubic ice at low-temperature interfaces, resulting in two types of separate crystallization of cubic ice and hexagonal ice from water vapour deposition at 102 K. Moreover, we identify a series of cubic-ice defects, including two types of stacking disorder, revealing the structure evolution dynamics supported by molecular dynamics simulations. The realization of direct, real-space imaging of ice formation and its dynamic behaviour at the molecular level provides an opportunity for ice research at the molecular level using transmission electron microscopy, which may be extended to other hydrogen-bonding crystals.

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