High-Crystalline Monolayer Transition Metal Dichalcogenides Films for Wafer-Scale Electronics

Chemical vapor deposition (CVD) using liquid-phase precursors has emerged as a viable technique for synthesizing uniform large-area transition metal dichalcogenide (TMD) thin films. However, the liquid-phase precursor-assisted growth process typically suffers from small-sized grains and unreacted transition metal precursor remainders, resulting in lower-quality TMDs. Moreover, synthesizing large-area TMD films with a monolayer thickness is also quite challenging. Herein, we successfully synthesized high-quality large-area monolayer molybdenum diselenide (MoSe₂) with good uniformity via promoter-assisted liquid-phase CVD process using the transition metal-containing precursor homogeneously modified with an alkali metal halide. The formation of a reactive transition metal oxyhalide and reduction of the energy barrier of chalcogenization by the alkali metal promoted the growth rate of the TMDs along the in-plane direction, enabling the full coverage of the monolayer MoSe₂ film with negligible few-layer regions. Note that the fully selenized monolayer MoSe₂ with high crystallinity exhibited superior electrical transport characteristics compared with those reported in previous works using liquid-phase precursors. We further synthesized various other monolayer TMD films, including molybdenum disulfide, tungsten disulfide, and tungsten diselenide, to demonstrate the broad applicability of the proposed approach.