Jinhua Hong†, ‡, §, Cong Wang†, §, Hongjun Liu‖, ‖‖§, Xibiao Ren‡, Jinglei Chen‖, Guanyong Wang††, Jinfeng Jia††, Maohai Xie‖, *, Chuanhong Jin‡, *, Wei Ji†, *, Jun Yuan‡,‡‡, Ze Zhang‡
†Beijing Key Laboratory of Optoelectronic Functional Materials & Micro-Nano Devices, Department of Physics, Renmin University of China, Beijing 100872, China
‡State Key Laboratory of Silicon Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, Zhejiang 310027, China.
‖Physics Department, The University of Hong Kong, Pokfulam Road, Hong Kong, ††Key Laboratory of Artificial Structures and Quantum Control (Ministry of Education), Department of Physics and Astronomy, Shanghai Jiaotong University, 800 Dongchuan Road, Shanghai 200240, China
‡‡Department of Physics, University of York, Heslington, York, YO10 5DD, United Kingdom
‖‖Institute of Functional Crystals, Tianjin University of Technology, Tianjin 300384, China.
§ These authors contributed equally to this work.
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DOI:10.1021/acs.nanolett.7b02600 Publication Date: Oct. 12, 2017
Interlayer rotation and stacking were recently demonstrated as effective strategies for tuning physical properties of various two-dimensional materials. The latter strategy was mostly realized in hetero-structures with continuously varied stacking orders, which obscure the revelation of the intrinsic role of a certain stacking order in its physical properties. Here, we introduce inversion-domain-boundaries into molecular-beam-epitaxy grown MoSe2homo-bilayers, which induce unusual fractional lattice translations to their surrounding domains, accounting for the observed diversity of large-area and uniform stacking sequences. Low-symmetric stacking orders were observed using transmission electron microscopy and detailed geometries were identified by density functional theory. A linear relation was also revealed between interlayer distance and stacking energy. These stacking sequences yield various energy alignments between the valence states at the Γand K points of the Brillion zone, showing stacking dependent bandgaps and valence band tail states in the measured scanning tunneling spectroscopy. These results may benefit the design of two-dimensional multilayers with manipulable stacking orders.