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Spectroscopic Visualization of Grain Boundaries of Monolayer Molybdenum Disulfide by Stacking Bilayers.

Polycrystalline growth of molybdenum disulfide (MoS2) using chemical vapor deposition (CVD) methods is subject to the formation of grain boundaries (GBs), which have a large effect on the electrical and optical properties of MoS2-based optoelectronic devices. The identification of grains and GBs of CVD-grown monolayer MoS2 has traditionally required atomic resolution microscopy or nonlinear optical imaging techniques. Here, we present a simple spectroscopic method for visualizing GBs of polycrystalline monolayer MoS2 using stacked bilayers and mapping their indirect photoluminescence (PL) peak positions and Raman peak intensities. We were able to distinguish a GB between two MoS2 grains with tilt angles as small as 6° in their grain orientations and, based on the inspection of several GBs, found a simple empirical rule to predict the location of the GBs. In addition, the large number of twist angle domains traced through our facile spectroscopic mapping technique allowed us to identify a continuous evolution of the coupled structural and optical properties of bilayer MoS2 in the vicinity of the 0° and 60° commensuration angles which were explained by elastic deformation model of the MoS2 membranes.