Determination of Crystal Axes in Semimetallic T′‐MoTe₂ by Polarized Raman Spectroscopy

Distorted octahedral T′ phase of MoTe₂ has recently attracted significant interest due to its predicted topological states and novel charge transport properties. Here, we report a nondestructive method for determining the crystal orientation of few‐layer T′‐MoTe₂ flakes by polarized Raman spectroscopy. The experimentally observed Raman modes are assigned to eigenmodes of vibrations predicted by density functional theory calculations. Polarized Raman measurements reveal four distinct types of angle‐dependent intensity variations. From group theory, it can be deduced that the intensity of the B_g mode reaches a maximum in the configuration when the polarization vector of the incident light is either parallel or orthogonal to the metal–metal zigzag chain direction. The intensity variation of the B_g mode cannot be used to unambiguously determine the crystal orientation. Using electron diffraction analysis, it is demonstrated that the intensity of the A_g mode at around 162 cm⁻¹ reaches a maximum when the polarization vector of the incident light is parallel to the metal–metal chain direction in the configuration. Furthermore, a simple method is proposed for identifying crystal orientation in nonpolarized Raman spectroscopy.