Robust growth of two-dimensional metal dichalcogenides and their alloys by active chalcogen monomer supply

The precise precursor supply is a precondition for controllable growth of two-dimensional (2D) transition metal dichalcogenides (TMDs). Although great efforts have been devoted to modulating the transition metal supply, few effective methods of chalcogen feeding control were developed. Here we report a strategy of using active chalcogen monomer supply to grow high-quality TMDs in a robust and controllable manner, e.g., MoS₂ monolayers perform representative photoluminescent circular helicity of ~92% and electronic mobility of ~42 cm²V^-1s^-1. Meanwhile, a uniform quaternary TMD alloy with three different anions, i.e., MoS_2(1-x-y)Se_2xTe_2y, was accomplished. Our mechanism study revealed that the active chalcogen monomers can bind and diffuse freely on a TMD surface, which enables the effective nucleation, reaction, vacancy healing and alloy formation during the growth. Our work offers a degree of freedom for the controllable synthesis of 2D compounds and their alloys, benefiting the development of high-end devices with desired 2D materials.