Bilayer two-dimensional (2D) van der Waals (vdW) materials are attracting increasing attention due to their predicted high quality electronic and optical properties. Here we demonstrate dense, selective growth of WSe2 bilayer flakes by chemical vapor deposition with the use of a 1:10 molar mixture of sodium cholate and sodium chloride as the growth promoter to control the local diffusion of W-containing species. A large fraction of the bilayer WSe2 flakes showed a 0 (AB) and 60 o (AA') twist between the two layers, while moiré 15 and 30 o -twist angles were also observed. Well-defined monolayer-bilayer junctions were formed in the as-grown bilayer WSe2 flakes, and these interfaces exhibited p-n diode rectification and an ambipolar transport characteristic. This work provides an efficient method for the layer-controlled growth of 2D materials, in particular, 2D transition metal dichalcogenides and promotes their applications in next-generation electronic and optoelectronic devices.

Research on 2D materials is one of the core themes of modern condensed matter physics. Prompted by the experimental isolation of graphene, much attention has been given to the unique optical, electronic, and structural properties of these materials. In the past few years, semiconducting transition metal dichalcogenides (TMDs) have attracted increasing interest due to properties such as direct band gaps and intrinsically broken inversion symmetry. Practical utilization of these properties demands large-area synthesis. While films of graphene have been by now synthesized on the order of square meters, analogous achievements are difficult for TMDs given the complexity of their growth kinetics. This article provides an overview of methods used to synthesize films of mono-and few-layer TMDs, comparing spatial and time scales for the different growth strategies. A special emphasis is placed on the unique applications enabled by such large-scale realization, in fields such as electronics and optics.

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Two-dimensional (2D) van der Waals superlattices comprised of two stacked monolayer materials have attracted significant interest as platforms for novel optoelectronic and structural behavior. Although studies are focused on superlattice fabrication, less effort has been given to the nanoscale patterning and structural modification of these systems. In this report, we demonstrate the localized layer-by-layer thinning and formation of nanopores/defects in 2D superlattices, such as stacked MoS2-WS2 van der Waals heterostructures and chemical vapor deposited bilayer WSe2, using aberration-corrected scanning transmission electron microscopy (STEM). Controlled electron beam irradiation is used to locally thin superlattices by removing the bottom layer of atoms, followed by defect formation through ablation of the second layer of atoms. The resulting defects exhibit atomically-sharp pore edges with tunable diameters down to 0.6 nm. Structural periodicities and focused STEM irradiation are also utilized to form close-packed nanopore arrays in superlattices with varying twist angles and commensurability. Applying these methods and mechanisms provides a forward approach in the atomic-scale patterning of stacked 2D nanodevices.

The large‐scale growth of semiconducting thin films on insulating substrates enables batch fabrication of atomically thin electronic and optoelectronic devices and circuits without film transfer. Here an efficient method to achieve rapid growth of large‐area monolayer MoSe2 films based on spin coating of Mo precursor and assisted by NaCl is reported. Uniform monolayer MoSe2 films up to a few inches in size are obtained within a short growth time of 5 min. The as‐grown monolayer MoSe2 films are of high quality with large grain size (up to 120 µm). Arrays of field‐effect transistors are fabricated from the MoSe2 films through a photolithographic process; the devices exhibit high carrier mobility of ≈27.6 cm2 V–1 s–1 and on/off ratios of ≈105. The findings provide insight into the batch production of uniform thin transition metal dichalcogenide films and promote their large‐scale applications.