Chemically Tailored Growth of 2D Semiconductors via Hybrid Metal-Organic Chemical Vapor Deposition

Two-dimensional (2D) semiconducting transition-metal dichalcogenides (TMDCs) are an exciting platform for new excitonic physics and next-generation electronics, creating a strong demand to understand their growth, doping, and heterostructures. Despite significant progress in solid-source (SS-) and metal-organic chemical vapor deposition (MOCVD), further optimization is necessary to grow highly crystalline 2D TMDCs with controlled doping. Here, we report a hybrid MOCVD growth method that combines liquid-phase metal precursor deposition and vapor-phase organo-chalcogen delivery to leverage the advantages of both MOCVD and SS-CVD. Using our hybrid approach, we demonstrate WS_2 growth with tunable morphologies - from separated single-crystal domains to continuous monolayer films - on a variety of substrates, including sapphire, SiO_2, and Au. These WS_2 films exhibit narrow neutral exciton photoluminescence linewidths down to 33 meV and room-temperature mobility up to 34 - 36 cm^2V^-^1s^-^1). Through simple modifications to the liquid precursor composition, we demonstrate the growth of V-doped WS_2, MoxW_1_-_xS_2 alloys, and in-plane WS_2-MoS_2 heterostructures. This work presents an efficient approach for addressing a variety of TMDC synthesis needs on a laboratory scale.