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追踪立方冰的分子分辨率。

Tracking cubic ice at molecular resolution.

机构信息

Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, China.

School of Physical Sciences, University of Chinese Academy of Sciences, Chinese Academy of Sciences, Beijing, China.

出版信息

Nature. 2023 May;617(7959):86-91. doi: 10.1038/s41586-023-05864-5. Epub 2023 Mar 29.

Abstract

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. 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. 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. 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.

摘要

冰存在于地球的各个角落,在云物理学、气候变化和低温保存等多个领域发挥着重要作用。冰的作用取决于其形成行为和相关结构。然而,这些都还没有被完全理解。特别是,长期以来一直存在争议的是,水是否可以冻结形成立方冰——这是普通六方冰相空间中目前尚未描述的一个相。从一系列实验室数据推断出的主流观点认为,这种分歧归因于无法从堆积无序冰(立方和六方序列的混合物)中分辨出立方冰。我们使用低温传输电子显微镜结合低剂量成像技术,在这里展示了在低温界面上立方冰的优先成核,导致在 102 K 时从水蒸气沉积中立方冰和六方冰的两种类型的分离结晶。此外,我们还确定了一系列立方冰缺陷,包括两种类型的堆积无序,揭示了分子动力学模拟所支持的结构演化动力学。直接在分子水平上对冰形成及其动态行为进行实时成像的实现,为使用透射电子显微镜进行冰的分子水平研究提供了机会,这可能会扩展到其他氢键晶体。

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