We have performed a comparative study of resonance Raman scattering in transition-metal dichalcogenides 2H-MX 2 semiconductors (M ¼ Mo, W; X ¼ S, Se) and single-layer MoS 2. Raman spectra were collected using excitation wavelengths 633 nm (1.96 eV), 594 nm (2.09 eV), 532 nm (2.33 eV), 514 nm (2.41 eV), and 488 nm (2.54 eV). In bulk-MoS 2 and WS 2 , the resonant energies appear to coincide with their exciton excitations. The resonance can be fine tuned by varying sample temperatures, which confirms its excitonic origin in both MoS 2 and WS 2. Temperature dependence of Raman intensities is analyzed in the context of resonance Raman theory, which agrees well with the existing absorption data. While in WSe 2 , the resonance has been observed in a wider range of excitations from 633 to 514 nm, which cannot be explained with its excitonic energies of 1.6 and 2.0 eV. It is considered that additional excitonic bands induced by band splitting are involved in the inter-band transitions and substantially extend the resonance energy range. The Raman resonance energy range remains unchanged in single-layer MoS 2 compared with that in the bulk sample. However, most phonon modes in single-layer MoS 2 are significantly broadened or strongly suppressed under resonance conditions. This change could be related to the modification of acoustic modes by the substrate. V
Photoluminescence (PL) and Raman spectra under uniaxial strain were measured in mono-and bi-layer MoSe 2 to comparatively investigate the evolution of excitonic gaps and Raman phonons with strain. We observed that the strain dependence of excitonic gaps shows a nearly linear behavior in both flakes. One percent of strain increase gives a reduction of ∼ 42 meV (∼ 35 meV) in A-exciton gap in monolayer (bilayer) MoSe 2 . The PL width remains little changed in monolayer MoSe 2 while it increases rapidly with strain in the bilayer case. We have made detailed discussions on the observed strain-modulated results and compared the difference between monolayer and bilayer cases. The hybridization between 4d orbits of Mo and 4p orbits of Se, which is controlled by the Se-Mo-Se bond angle under strain, can be employed to consistently explain the observations. The study may shed light into exciton physics in few-layer MoSe 2 and provides a basis for their applications.
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