Multilayered heterostructures of two-dimensional materials have recently attracted increased interest because of their unique electronic and optical properties. Here, we present chemical vapor deposition (CVD) growth of triangular crystals of monolayer MoS2 on single-crystalline hexagonal graphene domains which are also grown by CVD. We found that MoS2 grows selectively on the graphene domains rather than on the bare supporting SiO2 surface. Reflecting the heteroepitaxy of the growth process, the MoS2 domains grown on graphene present two preferred equivalent orientations. The interaction between the MoS2 and the graphene induced an upshift of the Raman G and 2D bands of the graphene, while significant photoluminescence quenching was observed for the monolayer MoS2. Furthermore, photoinduced current modulation along with an optical memory effect was demonstrated for the MoS2-graphene heterostructure. Our work highlights that heterostructures synthesized by CVD offer an effective interlayer van der Waals interaction which can be developed for large-area multilayer electronic and photonic devices.

The presence of grain boundaries in two-dimensional (2D) materials is known to greatly affect their physical, electrical, and chemical properties. Given the difficulty in growing perfect large single-crystals of 2D materials, revealing the presence and characteristics of grain boundaries becomes an important issue for practical applications. Here, we present a method to visualize the grain structure and boundaries of 2D materials by epitaxially growing transition metal dichalcogenides (TMDCs) over them. Triangular single-crystals of molybdenum disulfide (MoS2) epitaxially grown on the surface of graphene allowed us to determine the orientation and size of the graphene grains. Grain boundaries in the polycrystalline graphene were also visualized reflecting their higher chemical reactivity than the basal plane. The method was successfully applied to graphene field-effect transistors, revealing the actual grain structures of the graphene channels. Moreover, we demonstrate that this method can be extended to determine the grain structure of other 2D materials, such as tungsten disulfide (WS2). Our visualization method based on van der Waals epitaxy can offer a facile and large-scale labeling technique to investigate the grain structures of various 2D materials, and it will also contribute to understand the relationship between their grain structure and physical properties.

Heterostructures of two-dimensional (2D) layered materials have attracted growing interest due to their unique properties and possible applications in electronics, photonics, and energy. Reduction of the dimensionality from 2D to one-dimensional (1D), such as graphene nanoribbons (GNRs), is also interesting due to the electron confinement effect and unique edge effects. Here, we demonstrate a bottom-up approach to grow vertical heterostructures of MoS2 and GNRs by a two-step chemical vapor deposition (CVD) method. Single-layer GNRs were first grown by ambient pressure CVD on an epitaxial Cu(100) film, followed by the second CVD process to grow MoS2 over the GNRs. The MoS2 layer was found to grow preferentially on the GNR surface, while the coverage could be further tuned by adjusting the growth conditions. The MoS2/GNR nanostructures show clear photosensitivity to visible light with an optical response much higher than that of a 2D MoS2/graphene heterostructure. The ability to grow a novel 1D heterostructure of layered materials by a bottom-up CVD approach will open up a new avenue to expand the dimensionality of the material synthesis and applications.

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