We report a general synthetic strategy for highly robust growth of diverse lateral heterostructures, multiheterostructures, and superlattices from two-dimensional (2D) atomic crystals. A reverse flow during the temperature-swing stage in the sequential vapor deposition growth process allowed us to cool the existing 2D crystals to prevent undesired thermal degradation and uncontrolled homogeneous nucleation, thus enabling highly robust block-by-block epitaxial growth. Raman and photoluminescence mapping studies showed that a wide range of 2D heterostructures (such as WS-WSe and WS-MoSe), multiheterostructures (such as WS-WSe-MoS and WS-MoSe-WSe), and superlattices (such as WS-WSe-WS-WSe-WS) were readily prepared with precisely controlled spatial modulation. Transmission electron microscope studies showed clear chemical modulation with atomically sharp interfaces. Electrical transport studies of WSe-WS lateral junctions showed well-defined diode characteristics with a rectification ratio up to 10.

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Two-dimensional materials with intrinsic magnetism have recently drawn intense interest for both the fundamental studies and potential technological applications. However, the studies to date have been largely limited to mechanically exfoliated materials. Herein, an atmospheric pressure chemical vapor deposition route to ultrathin group VB metal telluride MTe (M = V, Nb, Ta) nanoplates with thickness as thin as 3 nm is reported. It is shown that the resulting nanoplates can be systematically evolved from mostly thicker hexagonal domains to thinner triangular domains with an increasing flow rate of the carrier gas. X-ray diffraction and transmission electron microscopy studies reveal MTe (M = V, Nb, Ta) nanoplates are high-quality single crystals. High-resolution scanning transmission electron microscope imaging reveals the VTe and NbTe nanoplates adopt the hexagonal 1T phase and the TaTe nanoplates show a monoclinic distorted 1T phase. Electronic transport studies show that MTe single crystals exhibit metallic behavior. Magnetic measurements show that VTe and NbTe exhibit ferromagnetism and TaTe shows paramagnetic behavior. The preparation of ultrathin few-layered MTe nanoplates will open up exciting opportunities for the burgeoning field of spintronics, sensors, and magneto-optoelectronics.

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The recent discovery of topological semimetals has stimulated extensive research interest due to their unique electronic properties and novel transport properties related to a chiral anomaly. However, the studies to date are largely limited to bulk crystals and exfoliated flakes. Here, we report the controllable synthesis of ultrathin two-dimensional (2D) platinum telluride (PtTe) nanosheets with tunable thickness and investigate the thickness-dependent electronic properties. We show that PtTe nanosheets can be readily grown, using a chemical vapor deposition approach, with a hexagonal or triangular geometry and a lateral dimension of up to 80 μm, and the thickness of the nanosheets can be systematically tailored from over 20 to 1.8 nm by reducing the growth temperature or increasing the flow rate of the carrier gas. X-ray-diffraction, transmission-electron microscopy, and electron-diffraction studies confirm that the resulting 2D nanosheets are high-quality single crystals. Raman spectroscopic studies show characteristics E and A vibration modes at ∼109 and ∼155 cm, with a systematic red shift with increasing nanosheet thickness. Electrical transport studies show the 2D PtTe nanosheets display an excellent conductivity up to 2.5 × 10 S m and show strong thickness-tunable electrical properties, with both the conductivity and its temperature dependence varying considerably with the thickness. Moreover, 2D PtTe nanosheets show an extraordinary breakdown current density up to 5.7 × 10 A/cm, the highest breakdown current density achieved in 2D metallic transition-metal dichalcogenides to date.

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Two-dimensional (2D) layered materials have stimulated extensive research interest for their unique thickness-dependent electronic and optical properties. However, the layer-number-dependent studies on 2D materials to date are largely limited to exfoliated flakes with relatively small lateral size and poor yield. The direct synthesis of 2D materials with a precise control of the number of atomic layers remains a substantial synthetic challenge. Here we report a systematic study of chemical vapor deposition synthesis of large-area atomically thin 2D nickel telluride (NiTe2) single crystals and investigate the thickness dependent electronic properties. By controlling the growth temperature, we show that the highly uniform NiTe2 single crystals can be synthesized with precisely tunable thickness varying from 1, 2, 3, . . . to multilayers with a standard deviation (∼0.3 nm) of less than the thickness of a monolayer layer NiTe2. Our studies further reveal a systematic evolution of single crystal domain size and nucleation density with the largest lateral domain size up to ∼440 μm. X-ray diffraction, transmission electron microscopy, and high resolution scanning transmission electron microscope studies demonstrate that the resulting 2D crystals are high quality single crystals and adopt hexagonal 1T phase. Electrical transport studies reveal that the 2D NiTe2 single crystals show a strong thickness-tunable electrical properties, with an excellent conductivity up to 7.8 × 105 S m–1 and extraordinary breakdown current density up to 4.7 × 107 A/cm2. The systematic study and robust synthesis of NiTe2 nanosheets defines a reliable chemical route to 2D single crystals with precisely tailored thickness and could enable the design of new device architectures based on thickness-tunable electrical properties.