General synthesis of mixed-dimensional van der Waals heterostructures with hexagonal symmetry

The combination of two-dimensional (2D) materials with non-2D materials (quantum dots, nanowires and bulk materials), i.e. mixed-dimensional van der Waals (md-vdW) heterostructures endow 2D materials with remarkable electronics properties. However, it remains a big challenge to synthesize md-vdW heterostructures because of the difference of crystal symmetry between 2D and non-2D materials. Meanwhile, it is difficult to initiate the nucleation due to the lack of chemical active sites on chemical inert surfaces of 2D materials. Herein, we design a general chemical vapor deposition method for synthesizing a broad class of md-vdW heterostructures with well-aligned hexagonal symmetry including MoS2/FeS, MoS2/CoS, MoS2/MnS, MoS2/ZnS, Mo(SxSe1–x)2/ZnSxSe1–x, Mo(SxSe1–x)2/CdSxSe1–x. Combining with DFT calculation, we find that the hexagonal symmetry and the centered clusters of MoS2 and Mo(SxSe1–x)2 nanoflakes are two crucial factors to launch the hexagonally oriented growth and nucleation of non-2D materials on 2D materials. Our discovery opens an opportunity for the versatile hetero-integration of 2D materials and allows systematic investigation of physical properties in a wide variety of md-vdW heterostructures.