We report on room-temperature Raman scattering measurements in few-layer crystals of exfoliated molybdenum ditelluride (MoTe2) performed with the use of 632.8 nm (1.96 eV) laser light excitation. In agreement with a recent study reported by G. Froehlicher et al 1 we observe a complex structure of the out-of-plane vibrational modes (A1g/A 1 ), which can be explained in terms of interlayer interactions between single atomic planes of MoTe2. In the case of low-energy shear and breathing modes of rigid interlayer vibrations, it is shown that their energy evolution with the number of layers can be well reproduced within a linear chain model with only the nearest neighbor interaction taken into account. Based on this model the corresponding in-plane and out-of-plane force constants are determined. We also show that the Raman scattering in MoTe2 measured using 514.5 nm (2.41 eV) laser light excitation results in much simpler spectra. We argue that the rich structure of the out-of-plane vibrational modes observed in Raman scattering spectra excited with the use of 632.8 nm laser light results from its resonance with the electronic transition at the M point of the MoTe2 first Brillouin zone.
The Raman scattering has been studied in heterostructures composed of a thin MoS2 flake and a 1-1.5 nm layer of thermally evaporated gold (Au). There have been Au nanoislands detected in the heterostructure. It has been found that their surface density and the average size depend on the MoS2 thickness. The Raman scattering spectrum in the heterostructure with a few monolayer MoS2 only weakly depends on the excitation (resonant vs. non-resonant) mode. The overall Raman spectrum corresponds to the total density of phonon states, which is characteristic for disordered systems. The disorder in the MoS2 layer is related to the mechanical strain induced in the MoS2 layer by the Au nanoislands. The strain results in the localization of phonon modes, which leads to the relaxation of the momentum conservation rule in the scattering process. The relaxation allows phonons from the whole MoS2 Brillouin zone to interact with electronic excitations. Our results show that the Au nanoislands resulted from thermal evaporation of a thin metal layer introduce substantial disorder into the crystalline structure of the thin MoS2 layers.
Temperature-dependent (5 K-300 K) Raman scattering study of A 1g /A′ 1 phonon modes in mono-layer (1L), bilayer (2L), trilayer (3L), and tetralayer (4L) MoTe 2 is reported. The temperature evolution of the modes' intensity critically depends on the flake thickness. In particular with λ = 632.8-nm light excitation, a strongly non-monotonic dependence of the A 1g mode intensity is observed in 2L MoTe 2 . The intensity decreases with decreasing temperature down to 220 K, and the A 1g mode almost completely vanishes from the Stokes scattering spectrum in the temperature range between 160 K and 220 K. The peak recovers at lower temperatures, and at T = 5 K, it becomes three times more intense that at room temperature. Similar non-monotonic intensity evolution is observed for the out-of-plane mode in 3L MoTe 2 in which tellurium atoms in all three layers vibrate in-phase. The intensity of the other out-of-plane Raman-active mode (with vibrations of tellurium atoms in the central layer shifted by 180° with respect to the vibrations in outer layers) only weakly depends on temperature. The observed quenching of the Raman scattering in 2L and 3L MoTe 2 is attributed to a destructive interference between the resonant and non-resonant contributions to the Raman scattering amplitude. The observed "antiresonance" is related to the electronic excitation at the M point of the Brillouin zone in few-layer MoTe 2 .
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