Aligned growth of transition metal dichalcogenides and related two-dimensional (2D) materials is essential for the synthesis of high-quality 2D films due to effective stitching of merging grains. Here, we demonstrate the controlled growth of highly aligned molybdenum disulfide (MoS) on c-plane sapphire with two distinct orientations, which are highly controlled by tuning sulfur concentration. We found that the size of the aligned MoS grains is smaller and their photoluminescence is weaker as compared with those of the randomly oriented grains, signifying enhanced MoS-substrate interaction in the aligned grains. This interaction induces strain in the aligned MoS, which can be recognized from their high susceptibility to air oxidation. The surface-mediated MoS growth on sapphire was further developed to the rational synthesis of an in-plane MoS-graphene heterostructure connected with the predefined orientation. The in-plane epitaxy was observed by low-energy electron microscopy. Transmission electron microscopy and scanning transmission electron microscopy suggest the alignment of a zigzag edge of MoS parallel to a zigzag edge of the neighboring graphene. Moreover, better electrical contact to MoS was obtained by the monolayer graphene compared with a conventional metal electrode. Our findings deepen the understanding of the chemical vapor deposition growth of 2D materials and also contribute to the tailored synthesis as well as applications of advanced 2D heterostructures.

We demonstrate the synthesis of unique heterostructures consisting of SnS and WS (or SnS and MoS) by two-step chemical vapor deposition (CVD). After the first CVD growth of triangular WS (MoS) grains, the second CVD step was performed to grow square SnS grains on the same substrate. We found that these SnS grains can be grown at very low temperature with the substrate temperature of 200 °C. Most of the SnS grains nucleated from the side edges of WS (MoS) grains, resulting in the formation of partly stacked heterostructures with a large overlapping area. The SnS grains showed doped p-type transfer character with a hole mobility of 15 cm V s, while the WS and MoS grains displayed n-type character with a high on/off ratio of >10. The SnS-WS and SnS-MoS heterostructures exhibited clear rectifying behavior, signifying the formation of p-n junctions at their interfaces. This heterostructure growth combined with the low temperature SnS growth will provide a promising means to exploit two-dimensional heterostructures by avoiding possible damage to the first material.

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