Growth of Large-Area Homogeneous Monolayer Transition-Metal Disulfides via a Molten Liquid Intermediate Process

Growth of large-area, uniform, and high-quality monolayer transition-metal dichalcogenides (TMDs) for practical and industrial applications remains a long-standing challenge. The present study demonstrates a modified predeposited chemical vapor deposition (CVD) process by employing an annealing procedure before sulfurization, which helps in achieving large-area, highly uniform, and high-quality TMDs on various substrates. The annealing procedure resulted in a molten liquid state of the precursors in the CVD process, which not only facilitated a uniform redistribution of the precursor on the substrate (avoid the aggregation) because of the uniform redistribution of the liquid precursor on the substrate but more importantly avoided the undesired multilayer growth via the self-limited lateral supply precursors mechanism. A 2 in. uniform and continuous monolayer WS₂ film has been synthesized on the SiO₂/Si substrate. Moreover, uniform monolayer WS₂ single crystals can be prepared on more general and various substrates including sapphire, mica, quartz, and Si₃N₄ using the same growth procedure. Besides, this growth mechanism can be generalized to synthesize other monolayer TMDs such as MoS₂ and MoS₂/WS₂ heterostructures. Hence, the present method provides a generalized attractive strategy to grow large-area, uniform, single-layer two-dimensional (2D) materials. This study has significant implications in the advancement of batch production of various 2D-material-based devices for industrial and commercial applications.