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-MoS₂ 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-MoS₂ in bilayer MoS₂ and density of TB-MoS₂ are significantly improved to 17.2% and 28.9 pieces/mm² by tailoring gas flow rate and molar ratio of NaCl to MoO₃. The proposed reconfiguring nucleation approach opens an avenue for the precise growth of TB-TMDCs for both fundamental research and practical applications.

由于莫尔超晶格相关的奇特能带结构和独特的电子特性，除 TB 石墨烯之外的扭曲双层 (TB) 过渡金属二硫属化物 (TMDC) 被认为是研究凝聚态物理的理想平台。具有宽扭转角的大面积、高质量 TB-TMDC 的生长对于探索扭转角相关的物理和应用具有重要意义，但实施起来仍然具有挑战性。在这里，我们提出了一种重新配置成核化学气相沉积（CVD）策略，用于直接合成扭转角从0°到120°的TB-MoS ₂ 。可以清楚地观察到与扭转角相关的莫尔周期性，并且层间耦合与扭转角显示出很强的关系。此外，通过调整气体流量和NaCl与MoO ₃的摩尔比，双层MoS ₂中TB-MoS ₂的产率和TB-MoS ₂的密度显着提高至17.2%和28.9个/mm ² 。所提出的重新配置成核方法为基础研究和实际应用的 TB-TMDC 的精确生长开辟了道路。