Epitaxial Growth of High‐Quality MoS ₂ via Sulfur Reflux CVD and Substrate Engineering

ABSTRACT MoS ₂ , as a representative transition metal dichalcogenide (TMDCs), shows a promising channel material for post‐silicon electronics due to its unique structural and electronic properties. However, the growth of high‐quality single‐crystalline MoS ₂ remains challenging. In this study, we present a reproducible method for the development of high‐quality single‐crystalline MoS ₂ films via a precursor reflux strategy on the C/M sapphire substrate. The epitaxial growth of single‐crystalline MoS ₂ with cm ² exhibits low defect density (sulfur vacancy concentration: 6.5 × 10 ¹² cm ^{− 2} ) and exceptional electrical performance, including a high on/off current ratio of 10⁹ and a field‐effect mobility of 105.2 cm ² V ⁻¹ s ⁻¹ . Uniform device performance across fabricated arrays confirms the homogeneity of the MoS ₂ film. Additionally, this method can be extended to grow other 2D TMDCs, such as 3R‐MoS ₂ and 3R‐WS ₂ . This work provides an innovative approach for the growth of high‐quality single‐crystalline MoS ₂ , thereby advancing its application in 2D electronics.