Two-dimensional van der Waals heterostructures (vdWHs) have attracted considerable interest1,2,3,4. However, most vdWHs reported so far are created by an arduous micromechanical exfoliation and manual restacking process5, which—although versatile for proof-of-concept demonstrations6,7,8,9,10,11,12,13,14,15,16 and fundamental studies17,18,19,20,21,22,23,24,25,26,27,28,29,30—is clearly not scalable for practical technologies. Here we report a general synthetic strategy for two-dimensional vdWH arrays between metallic transition-metal dichalcogenides (m-TMDs) and semiconducting TMDs (s-TMDs). By selectively patterning nucleation sites on monolayer or bilayer s-TMDs, we precisely control the nucleation and growth of diverse m-TMDs with designable periodic arrangements and tunable lateral dimensions at the predesignated spatial locations, producing a series of vdWH arrays, including VSe2/WSe2, NiTe2/WSe2, CoTe2/WSe2, NbTe2/WSe2, VS2/WSe2, VSe2/MoS2 and VSe2/WS2. Systematic scanning transmission electron microscopy studies reveal nearly ideal vdW interfaces with widely tunable moiré superlattices. With the atomically clean vdW interface, we further show that the m-TMDs function as highly reliable synthetic vdW contacts for the underlying WSe2 with excellent device performance and yield, delivering a high ON-current density of up to 900 microamperes per micrometre in bilayer WSe2 transistors. This general synthesis of diverse two-dimensional vdWH arrays provides a versatile material platform for exploring exotic physics and promises a scalable pathway to high-performance devices.
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The authors at Hunan University acknowledge the support from National Natural Science Foundation of China (grant numbers 51991340, 51991343 and 51872086), and the Hunan Key Laboratory of Two-Dimensional Materials (grant number 2018TP1010). The planar TEM studies were conducted at the Center for Electron Microscopy at Tianjin University of Technology. The cross-sectional STEM experiments were conducted using the facilities in the Irvine Materials Research Institute (IMRI) at the University of California, Irvine. The work at University of California, Irvine was supported by the Department of Energy (DOE), Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under grant DE-SC0014430.
The authors declare no competing interests.
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Extended data figures and tables
a, Optical microscopy image of WSe2 with periodically patterned defects. b, AFM image of WSe2 with patterned defects. c, The height profile of the white circle region in b, exhibiting a depth of about 0.3 nm.
Raman spectra of VSe2 on SiO2/Si (a) and VSe2/WSe2 vertical heterostructure (b). c, Photoluminescence spectra of the bare WSe2 and the overlapping VSe2/WSe2 vertical heterostructure.
Atomic-resolution HAADF-STEM image of VSe2 (a) and the corresponding intensity profile of V (b). c, d, Atomic-resolution HAADF-STEM image of WSe2 (c) and the corresponding intensity profile of W (d).
Zoom-in view of four locations of moiré structures marked in Fig. 4c (i, ii, iii, i), showing three distinct atomic arrangements, corresponding to the single V atom arrangement (i), V stacking over Se (ii), and V stacking over W (iii). The two panels labelled ‘i’ are identical. The red, blue and yellow spheres correspond to V, W and Se, respectively.
Optical microscopy images of the NbTe2/WSe2 vdWH arrays (a) and the VS2/WSe2 vdWH arrays (b).
a, Typical photograph of highly oriented monolayer MoS2 continuous films grown on 2-inch sapphire wafer. b, c, Optical microscopy images of large-scale periodic VSe2/MoS2 vdWH arrays grown on continuous MoS2 thin films taken with ×10 magnification objective (b) and ×20 magnification objective (c). d–g, High-magnification optical microscopy images of periodic VSe2/MoS2 vdWH arrays collected in different regions of b, suggesting highly uniform growth of VSe2/MoS2 vdWH arrays.
a, Typical optical microscopy image of a VSe2/WS2 vdWH array. b, Raman spectra of the bare WS2 and the overlapping VSe2/WS2 vertical heterostructure. c, d, Raman intensity mapping image of VSe2/WSe2 vdWH arrays at resonant peaks of 353 cm−1 (WS2; c) and 206 cm−1 (VSe2; d). e, Photoluminescence spectra of the bare WS2 and the overlapping VSe2/WS2 vertical heterostructure. f, Photoluminescence intensity mapping image at 658 nm (WS2 emission).
Extended Data Fig. 8 Electrical characterization of a bilayer WSe2 transistors with synthetic vdW contacts.
a, b, Output (a) and transfer (b) curves of a typical device with synthetic VSe2 vdW contacts on 285-nm SiO2/Si. The channel length is about 2.0 μm.
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Li, J., Yang, X., Liu, Y. et al. General synthesis of two-dimensional van der Waals heterostructure arrays. Nature 579, 368–374 (2020). https://doi.org/10.1038/s41586-020-2098-y
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