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2D transition metal dichalcogenides (TMDs) for advanced logic transistor technologies are deposited by various modifications of the chemical vapor deposition (CVD) method using a wide variety of precursors. Being a major electrical performance limiter, the TMD crystal grain size strongly differs between the various CVD precursor chemistries from nano‐ to millimeter‐sized crystals. However, it remains unclear how the CVD precursor chemistry affects the nucleation density and resulting TMD crystal grain size. This work postulates guiding principles to design a CVD process for highly crystalline TMD deposition using a quantitative analytical model benchmarked against the literature. The TMD nucleation density reduces favorably under low supersaturation conditions where the metal precursor sorption on the starting surface is reversible and the corresponding metal precursor desorption rate exceeds the overall deposition rate. Such reversible precursor adsorption guarantees efficient long‐range gas‐phase lateral diffusion of precursor species in addition to short‐range surface diffusion, which vitally increases crystal grain size. The proposed model explains the large spread in experimentally observed TMD nucleation densities and crystal grain sizes for state‐of‐the‐art CVD chemistries. Ultimately, it empowers the reader to interpret and modulate precursor adsorption and diffusion reactions through designing CVD precursor chemistries. [ABSTRACT FROM AUTHOR]

Two-dimensional (2D) transition metal dichalcogenides are potential low dissipative semiconductor materials for nanoelectronic devices. Such applications require the deposition of these materials in their crystalline form and with controlled number of monolayers on large area substrates, preferably using deposition temperatures compatible with temperature sensitive structures. This paper presents a low temperature plasma-enhanced atomic layer deposition (PEALD) process for 2D WS2 based on a ternary reaction cycle consisting of consecutive WF6, H2 plasma, and H2S reactions. Strongly textured, nanocrystalline WS2 is grown at 300 °C. The composition and crystallinity of these layers depends on the PEALD process conditions, as understood by a model for the redox chemistry of this process. The H2 plasma is essential for the deposition of WS2 as it enables the reduction of -W6+Fx surface species. Nevertheless, the impact of subsurface reduction reactions needs to be minimized to obtain WS2 with well-controlled composition (S/W ratio of 2). [ABSTRACT FROM AUTHOR]