Anomalous lattice vibrations of monolayer MoS₂ probed by ultraviolet Raman scattering

We present a comprehensive Raman scattering study of monolayer MoS2 with increasing laser excitation energies ranging from the near-infrared to the deep-ultraviolet. The Raman scattering intensities from the second-order phonon modes are revealed to be enhanced anomalously by only the ultraviolet excitation wavelength 354 nm. We demonstrate theoretically that such resonant behavior arises from a strong optical absorption that forms near the Γ point and ½ΓK of the band structure and an inter-valley resonant electronic scattering by the M-point phonons. These results advance our understanding of the double resonance Raman scattering process in low-dimensional semiconducting nanomaterials and provide a foundation for the technological development of monolayer MoS2 in the ultraviolet frequency range.