Atomically engineering interlayer symmetry operations of two-dimensional crystals

Ziyi Han; Shengqiang Wu; Chun Huang; Fengyuan Xuan; Xiaocang Han; Yinfeng Long; Qing Zhang; Junxian Li; Yuan Meng; Lin Wang; Jiahuan Zhou; Wenping Hu; Jingsi Qiao; Dechao Geng; Xiaoxu Zhao

doi:10.1038/s41467-024-55130-z

Atomically engineering interlayer symmetry operations of two-dimensional crystals

Nat Commun. 2024 Dec 30;15(1):10835. doi: 10.1038/s41467-024-55130-z.

Authors

Ziyi Han^#^{1

2}, Shengqiang Wu^#¹, Chun Huang^#³, Fengyuan Xuan⁴, Xiaocang Han¹, Yinfeng Long⁵, Qing Zhang^{2

6

7}, Junxian Li¹, Yuan Meng¹, Lin Wang⁵, Jiahuan Zhou⁸, Wenping Hu^{2

6}, Jingsi Qiao³, Dechao Geng^{9

10

11}, Xiaoxu Zhao¹²

Affiliations

¹ School of Materials Science and Engineering, Peking University, Beijing, 100871, China.
² Key Laboratory of Organic Integrated Circuits, Ministry of Education & Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Tianjin University, Tianjin, 300072, China.
³ MIIT Key Laboratory for Low-Dimensional Quantum Structure and Devices & Advanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing, 100081, China.
⁴ Suzhou Laboratory, Suzhou, 215123, China.
⁵ School of Mechanical Engineering, Shanghai JiaoTong University, Shanghai, 200240, China.
⁶ Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin, 300072, China.
⁷ Beijing National Laboratory for Molecular Sciences, Beijing, 100190, China.
⁸ Wangxuan Institute of Computer Technology, Peking University, Beijing, China.
⁹ Key Laboratory of Organic Integrated Circuits, Ministry of Education & Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Tianjin University, Tianjin, 300072, China. gengdechao_1987@tju.edu.cn.
¹⁰ Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin, 300072, China. gengdechao_1987@tju.edu.cn.
¹¹ Beijing National Laboratory for Molecular Sciences, Beijing, 100190, China. gengdechao_1987@tju.edu.cn.
¹² School of Materials Science and Engineering, Peking University, Beijing, 100871, China. xiaoxuzhao@pku.edu.cn.

^# Contributed equally.

Abstract

Crystal symmetry, which governs the local atomic coordination and bonding environment, is one of the paramount constituents that intrinsically dictate materials' functionalities. However, engineering crystal symmetry is not straightforward due to the isotropically strong covalent/ionic bonds in crystals. Layered two-dimensional materials offer an ideal platform for crystal engineering because of the ease of interlayer symmetry operations. However, controlling the crystal symmetry remains challenging due to the ease of gliding perpendicular to the Z direction. Herein, we proposed a substrate-guided growth mechanism to atomically fabricate AB'-stacked SnSe₂ superlattices, containing alternating SnSe₂ slabs with periodic interlayer mirror and gliding symmetry operations, by chemical vapor deposition. Some higher-order phases such as 6 R, 12 R, and 18 C can be accessed, exhibiting modulated nonlinear optical responses suggested by first-principle calculations. Charge transfer from mica substrates stabilizes the high-order SnSe₂ phases. Our approach shows a promising strategy for realizing topological phases via stackingtronics.

Abstract

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