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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 CdI2/WS2, CdI2/MoS2, CdI2/WSe2, PbI2/WS2, PbI2/MoS2, PbI2/WSe2, and Bi2Se3/WS2 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.
A new growth mode of 2D van der Waals (vdW) heterostructures with distinctly different morphologies and growth rates from the conventional mode is observed using a custom‐built system integrating physical vapor deposition with in situ optical microscopy/Raman spectroscopy. A model to explain these two growth modes is proposed, which appears to be applicable to 2D vdW heterostructures in general.