Atomic imaging of the edge structure and growth of a two-dimensional hexagonal ice

• Published in: Nature (London) Vol. 577; no. 7788; pp. 60 - 63
• Main Authors: Ma, Runze, Cao, Duanyun, Zhu, Chongqin, Tian, Ye, Peng, Jinbo, Guo, Jing, Chen, Ji, Li, Xin-Zheng, Francisco, Joseph S., Zeng, Xiao Cheng, Xu, Li-Mei, Wang, En-Ge, Jiang, Ying
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 02-01-2020; Nature Publishing Group
• Subjects: 119/118; 639/301/357/1018; 639/638/440/950; 639/766/119/544; 639/766/930/328/968; 639/766/94; Atomic force microscopy; Crystallization; Crystals; Edge detection (Image processing); Fragility; Growth; Humanities and Social Sciences; Ice; Ice formation; Image reconstruction; Methods; Microscopy; Microscopy, Scanning Tunneling; multidisciplinary; Observations; Perturbation; Science; Science (multidisciplinary); Structure; Water chemistry; China
• ISSN: 0028-0836; 1476-4687
• DOI: 10.1038/s41586-019-1853-4

The formation and growth of water-ice layers on surfaces and of low-dimensional ice under confinement are frequent occurrences
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. This is exemplified by the extensive reporting of two-dimensional (2D) ice on metals
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, insulating surfaces
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, graphite and graphene
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and under strong confinement
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,
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–
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. Although structured water adlayers and 2D ice have been imaged, capturing the metastable or intermediate edge structures involved in the 2D ice growth, which could reveal the underlying growth mechanisms, is extremely challenging, owing to the fragility and short lifetime of those edge structures. Here we show that noncontact atomic-force microscopy with a CO-terminated tip (used previously to image interfacial water with minimal perturbation)
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, enables real-space imaging of the edge structures of 2D bilayer hexagonal ice grown on a Au(111) surface. We find that armchair-type edges coexist with the zigzag edges usually observed in 2D hexagonal crystals, and freeze these samples during growth to identify the intermediate edge structures. Combined with simulations, these experiments enable us to reconstruct the growth processes that, in the case of the zigzag edge, involve the addition of water molecules to the existing edge and a collective bridging mechanism. Armchair edge growth, by contrast, involves local seeding and edge reconstruction and thus contrasts with conventional views regarding the growth of bilayer hexagonal ices and 2D hexagonal matter in general.
Real-space imaging of the edge structures and growth of a two-dimensional ice on a gold substrate is achieved using noncontact atomic-force microscopy with a carbon monoxide tip.