The stacking of few layers of transition metal dichalcogenides (TMDs) and their heterostructures allows us to create new structures, observe new physical phenomena, and envision new applications. Moreover, the twist angle in few-layer TMDs can significantly impact their electrical and optical properties. Therefore, controlling the TMD material and obtaining different stacking orientations when synthesizing TMDs via chemical vapor deposition (CVD) is a powerful tool, which can add functionality to TMD-based optoelectronic devices. Here, we report on the synthesis of few-layer MoS[Formula: see text] and WS[Formula: see text] crystals, as well as their heterobilayer structures with [Formula: see text] and [Formula: see text] twist angles between layers via CVD. Raman and photoluminescence spectroscopies demonstrate the quality, crystallinity, and layer count of our grown samples, while second harmonic generation shows that adjacent layers grow with 0[Formula: see text] or 60[Formula: see text] twist angles, corresponding to two different crystal phases. Our study based on TMDs with different and multiple stacking configurations provides an alternative route for the development of future optoelectronic and nonlinear optical devices.
We report on second harmonic generation from MoS2/WS2 as-grown heterostructures. The two crystal structures naturally align with 0掳 and ^60. twist angles. While the former enhances, the latter decreases the nonlinearity from individual layers.
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