High‐Pressure Chemical Vapor Deposition Growth of Transition Metal Dichalcogenides With Minimized Sulfur Vacancies

Molybdenum disulfide (MoS 2 ), a prototypical two‐dimensional semiconductor, is regarded as a promising channel material for next‐generation nanoelectronics. However, its large‐area synthesis via chemical vapor deposition (CVD) remains plagued by high defect densities (10 12 –10 14 cm −2 ), particularly sulfur vacancies that act as deep traps and severely degrade carrier transport and optical performance. Here, we develop a high‐pressure CVD approach capable of operating at pressures up to 3800 torr while precisely regulating the sulfur partial pressure. The sulfur‐vacancy density in monolayer MoS 2 grown at 3800 torr is reduced to 8 × 10 11 cm −2 , the lowest value reported for CVD‐grown samples and comparable to that of mechanically exfoliated crystals. The elevated sulfur partial pressure effectively suppresses thermal desulfurization, yielding films with enhanced crystallinity, long‐range c ‐axis alignment, and uniform defect distribution. Corresponding MoS 2 field‐effect transistors exhibit a fivefold enhancement in carrier mobility and a reduced subthreshold swing, directly linked to the diminished trap density. These results identify growth pressure as a critical thermodynamic variable for point‐defect control and establish high‐pressure CVD as a robust and scalable platform for synthesizing high‐quality transition metal dichalcogenides for future electronic and optoelectronic applications.