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July 4, 2024Science153 citations

Interfacial epitaxy of multilayer rhombohedral transition-metal dichalcogenide single crystals

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BQBiao QinCMChaojie MaQGQuanlin Guo

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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).

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Qin et al. (2024) studied this question.

synapsesocial.com/papers/68e615d4b6db6435875a8124https://doi.org/10.1126/science.ado6038
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