Polarization‐dependent anisotropic Raman response of CVD‐grown vertically stacked MoS2 layers

Abstract We report on the polarized Raman scattering results of vertically stacked few‐layer MoS 2 grown by chemical vapor deposition. Results of monolayer MoS 2 showed that the polarization‐angle‐resolved intensity profiles of both out‐of‐plane A 1g and in‐plane phonon modes followed the Raman polarization selection rules. In contrast, the polarization‐angle dependence of the phonon intensity in the multilayer region showed a deviation from the polarization selection rules, whereas that of the A 1g phonon intensity remained unchanged regardless of the layer number. Furthermore, the polarization anisotropy of the phonon intensity increased with an increase in layer number. The vertically stacked MoS 2 multilayers had oblique, deformed edge boundaries that were not parallel to the basal monolayer edge, suggesting the presence of slight interlayer twisting and/or sliding between neighboring layers. Therefore, we suggest that the polarization‐dependent anisotropic behavior of the phonon in the multilayer region is attributed to stacking disorder between MoS 2 layers.