Interfacial epitaxy of multilayer rhombohedral transition-metal dichalcogenide single crystals

Author:

Qin Biao12ORCID,Ma Chaojie1ORCID,Guo Quanlin1ORCID,Li Xiuzhen3ORCID,Wei Wenya4ORCID,Ma Chenjun1ORCID,Wang Qinghe1ORCID,Liu Fang1ORCID,Zhao Mengze1,Xue Guodong1ORCID,Qi Jiajie1ORCID,Wu Muhong567ORCID,Hong Hao17ORCID,Du Luojun3ORCID,Zhao Qing1ORCID,Gao Peng5ORCID,Wang Xinqiang1ORCID,Wang Enge56ORCID,Zhang Guangyu36ORCID,Liu Can2ORCID,Liu Kaihui156ORCID

Affiliation:

1. State Key Laboratory for Mesoscopic Physics, Frontiers Science Centre for Nano-optoelectronics, School of Physics, Peking University, Beijing, China.

2. Key Laboratory of Quantum State Construction and Manipulation (Ministry of Education), Department of Physics, Renmin University of China, Beijing, China.

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

4. Guangdong Basic Research Center of Excellence for Structure and Fundamental Interactions of Matter, Guangdong Provincial Key Laboratory of Quantum Engineering and Quantum Materials, School of Physics, South China Normal University, Guangzhou, China.

5. International Centre for Quantum Materials, Collaborative Innovation Centre of Quantum Matter, Peking University, Beijing, China.

6. Songshan Lake Materials Laboratory, Dongguan, China.

7. Interdisciplinary Institute of Light-Element Quantum Materials and Research Centre for Light-Element Advanced Materials, Peking University, Beijing, China.

Abstract

Rhombohedral-stacked transition-metal dichalcogenides (3R-TMDs), which are distinct from their hexagonal counterparts, exhibit higher carrier mobility, sliding ferroelectricity, and coherently enhanced nonlinear optical responses. However, surface epitaxial growth of large multilayer 3R-TMD single crystals is difficult. We report an interfacial epitaxy methodology for their growth of several compositions, including molybdenum disulfide (MoS 2 ), molybdenum diselenide, tungsten disulfide, tungsten diselenide, niobium disulfide, niobium diselenide, and molybdenum sulfoselenide. Feeding of metals and chalcogens continuously to the interface between a single-crystal Ni substrate and grown layers ensured consistent 3R stacking sequence and controlled thickness from a few to 15,000 layers. Comprehensive characterizations confirmed the large-scale uniformity, high crystallinity, and phase purity of these films. The as-grown 3R-MoS 2 exhibited room-temperature mobilities up to 155 and 190 square centimeters per volt second for bi- and trilayers, respectively. Optical difference frequency generation with thick 3R-MoS 2 showed markedly enhanced nonlinear response under a quasi–phase matching condition (five orders of magnitude greater than monolayers).

Publisher

American Association for the Advancement of Science (AAAS)

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