Although polycrystalline hexagonal boron nitride (PC-hBN) has been realized, defects and grain boundaries still cause charge scatterings and trap sites, impeding high-performance electronics. Here, we report a method of synthesizing wafer-scale single-crystalline hBN (SC-hBN) monolayer films by chemical vapor deposition. The limited solubility of boron (B) and nitrogen (N) atoms in liquid gold promotes high diffusion of adatoms on the surface of liquid at high temperature to provoke the circular hBN grains. These further evolve into closely packed unimodal grains by means of self-collimation of B and N edges inherited by electrostatic interaction between grains, eventually forming an SC-hBN film on a wafer scale. This SC-hBN film also allows for the synthesis of wafer-scale graphene/hBN heterostructure and single-crystalline tungsten disulfide.

Although hexagonal boron nitride (h-BN) is a good candidate for gate-insulating materials by minimizing interaction from substrate, further applications to electronic devices with available two-dimensional semiconductors continue to be limited by flake size. While monolayer h-BN has been synthesized on Pt and Cu foil using chemical vapour deposition (CVD), multilayer h-BN is still absent. Here we use Fe foil and synthesize large-area multilayer h-BN film by CVD with a borazine precursor. These films reveal strong cathodoluminescence and high mechanical strength (Young's modulus: 1.16±0.1 TPa), reminiscent of formation of high-quality h-BN. The CVD-grown graphene on multilayer h-BN film yields a high carrier mobility of ∼24,000 cm2 V−1 s−1 at room temperature, higher than that (∼13,000 2 V−1 s−1) with exfoliated h-BN. By placing additional h-BN on a SiO2/Si substrate for a MoS2 (WSe2) field-effect transistor, the doping effect from gate oxide is minimized and furthermore the mobility is improved by four (150) times.

We report the synthesis of centimeter-scale monolayer WS2 on gold foil by chemical vapor deposition. The limited tungsten and sulfur solubility in gold foil allows monolayer WS2 film growth on gold surface. To ensure the coverage uniformity of monolayer WS2 film, the tungsten source-coated substrate was placed in parallel with Au foil under hydrogen sulfide atmosphere. The high growth temperature near 935 °C helps to increase a domain size up to 420 μm. Gold foil is reused for the repeatable growth after bubbling transfer. The WS2-based field effect transistor reveals an electron mobility of 20 cm(2) V(-1) s(-1) with high on-off ratio of ∼10(8) at room temperature, which is the highest reported value from previous reports of CVD-grown WS2 samples. The on-off ratio of integrated multiple FETs on the large area WS2 film on SiO2 (300 nm)/Si substrate shows within the same order, implying reasonable uniformity of WS2 FET device characteristics over a large area of 3 × 1.5 cm(2).

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High-quality and large-area molybdenum disulfide (MoS ) thin film is highly desirable for applications in large-area electronics. However, there remains a challenge in attaining MoS film of reasonable crystallinity due to the absence of appropriate choice and control of precursors, as well as choice of suitable growth substrates. Herein, a novel and facile route is reported for synthesizing few-layered MoS film with new precursors via chemical vapor deposition. Prior to growth, an aqueous solution of sodium molybdate as the molybdenum precursor is spun onto the growth substrate and dimethyl disulfide as the liquid sulfur precursor is supplied with a bubbling system during growth. To supplement the limiting effect of Mo (sodium molybdate), a supplementary Mo is supplied by dissolving molybdenum hexacarbonyl (Mo(CO) ) in the liquid sulfur precursor delivered by the bubbler. By precisely controlling the amounts of precursors and hydrogen flow, full coverage of MoS film is readily achievable in 20 min. Large-area MoS field effect transistors (FETs) fabricated with a conventional photolithography have a carrier mobility as high as 18.9 cm V s , which is the highest reported for bottom-gated MoS -FETs fabricated via photolithography with an on/off ratio of ≈10 at room temperature.

We report a facile method for the synthesis of large-area tungsten disulfide (WS) films by means of chemical vapor deposition (CVD). To promote WS film growth, the precursor solution, which includes pre-reduced tungsten suboxides, is prepared by using hydrazine as the strong reducing agent and spin-coated onto the growth substrate. Growth is then carried out in a CVD chamber vaporized with dimethyl disulfide as the sulfur precursor. Although only WS flakes are grown with unreduced tungsten precursors under a hydrogen atmosphere, WS films are readily attained on pre-reduced tungsten suboxide substrates without the need for further reduction by hydrogen, which is noted to induce discontinuity of the grown film. The result presents the coverage of WS to be proportional to the amount of reduced tungsten suboxides, which is revealed by X-ray photoelectron spectroscopy. Furthermore, it is found that the multilayer WS flakes grow along the grain boundary, which allows the analysis of the grain size of WS films by optical microscopy images only. WS field effect transistors are fabricated by conventional photolithography and show an average electron mobility of 0.4 cm V s and a high on/off ratio of 10 at room temperature.

We report on the synthesis of large-area molybdenum disulfide (MoS2) film on an insulating substrate by means of chemical vapor deposition. A single mixture of molybdenum hexacarbonyl (Mo(CO)6) and dimethyl disulfide (C2H6S2) was utilized as an organic liquid precursor for the synthesis of MoS2 film. Carbon impurities stemming from the dissociation of the organic precursor are effectively removed by water oxidation, and hydrogen gas, which is a by-product of the oxidation of carbon impurities, inhibits the formation of molybdenum oxides. The use of a liquid precursor assisted with water oxidation ensures high reproducibility and full-coverage of MoS2 film for large area, which is not typically achieved with solid precursors such as molybdenum oxide and sulfur powder. We believe that our approach will advance the synthesis of transition metal dichalcogenides.

Two-dimensional (2D) van der Waals (vdW) heterostructures exhibit novel physical and chemical properties, allowing the development of unprecedented electronic, optical, and electrochemical devices. However, the construction of wafer-scale vdW heterostructures for practical applications is still limited due to the lack of well-established growth and transfer techniques. Herein, we report a method for the fabrication of wafer-scale 2D vdW heterostructures with an ultraclean interface between layers via the aid of a freestanding viscoelastic polymer support layer (VEPSL). The low glass transition temperature (T g) and viscoelastic nature of the VEPSL ensure absolute conformal contact between 2D layers, enabling the easy pick-up of layers and attaching to other 2D layers. This eventually leads to the construction of random sequence 2D vdW heterostructures such as molybdenum disulfide/tungsten disulfide/molybdenum diselenide/tungsten diselenide/hexagonal boron nitride. Furthermore, the VEPSL allows the conformal transfer of 2D vdW heterostructures onto arbitrary substrates, irrespective of surface roughness. To demonstrate the significance of the ultraclean interface, the fabricated molybdenum disulfide/graphene heterostructure employed as an electrocatalyst yielded excellent results of 73.1 mV·dec–1 for the Tafel slope and 0.12 kΩ of charge transfer resistance, which are almost twice as low as that of the impurity-trapped heterostructure.