Understanding the growth mechanisms of 2D van der Waals (vdW) heterostructures is of great importance in exploring their functionalities and device applications. A custom-built system integrating physical vapor deposition and optical microscopy/Raman spectroscopy is employed to study the dynamic growth processes of 2D vdW heterostructures in situ. This allows the identification of a new growth mode with a distinctly different growth rate and morphology from those of the conventional linear growth mode. A model that explains the difference in morphologies and quantifies the growth rates of the two modes by taking the role of surface diffusion into account is proposed. A range of material combinations including CdI 2 /WS 2 , CdI 2 /MoS 2 , CdI 2 /WSe 2 , PbI 2 /WS 2 , PbI 2 /MoS 2 , PbI 2 /WSe 2 , and Bi 2 Se 3 /WS 2 is systematically investigated. These findings may be generalized to the synthesis of many other 2D heterostructures with controlled morphologies and physical properties, benefiting future device applications.

Two-dimensional transition-metal dichalcogenides (TMDs) have been one of the hottest focus of materials due to the most beneficial electronic and optoelectronic properties. Up to now, one of the big challenges is the synthesis of large-area layer-number-controlled single-crystal films. However, the poor understanding of the growth mechanism seriously hampers the progress of the scalable production of TMDs with precisely tunable thickness at an atomic scale. Here, the growth mechanisms in the vertical direction were systemically studied based on the density functional theory (DFT) calculation and an advanced chemical vapor deposition (CVD) growth. As a result, the U-type relation of the TMD layer number to the ratio of metal/chalcogenide is confirmed by the capability of ultrafine tuning of the experimental conditions in the CVD growth. In addition, high-quality uniform monolayer, bilayer, trilayer, and multilayer TMDs in a large area (8 cm2) were efficiently synthesized by applying this modified CVD. Although bilayer TMDs can be obtained at both high and low ratios of metal/chalcogenide based on the suggested mechanism, they demonstrate significantly different optical and electronic transport properties. The modified CVD strategy and the proposed mechanism should be helpful for synthesizing and large-area thickness-controlled TMDs and understanding their growth mechanism and could be used in integrated electronics and optoelectronics.

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