Reconfiguring nucleation for CVD growth of twisted bilayer MoS2 with a wide range of twist angles

Twisted bilayer (TB) transition metal dichalcogenides (TMDCs) beyond TB-graphene are considered an ideal platform for investigating condensed matter physics, due to the moiré superlattices-related peculiar band structures and distinct electronic properties. The growth of large-area and high-quality TB-TMDCs with wide twist angles would be significant for exploring twist angle-dependent physics and applications, but remains challenging to implement. Here, we propose a reconfiguring nucleation chemical vapor deposition (CVD) strategy for directly synthesizing TB-MoS 2 with twist angles from 0° to 120°. The twist angles-dependent Moiré periodicity can be clearly observed, and the interlayer coupling shows a strong relationship to the twist angles. Moreover, the yield of TB-MoS 2 in bilayer MoS 2 and density of TB-MoS 2 are significantly improved to 17.2% and 28.9 pieces/mm 2 by tailoring gas flow rate and molar ratio of NaCl to MoO 3 . The proposed reconfiguring nucleation approach opens an avenue for the precise growth of TB-TMDCs for both fundamental research and practical applications. Twisted bilayers of 2D semiconductors are being intensively investigated due to their emergent physical properties, but their controlled bottom-up synthesis remains challenging. Here, the authors report a confined-space chemical vapour deposition strategy to synthesize MoS 2 bilayers with twist angles ranging from 0° to 120°.