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.
We investigate the origin of emission lines apparent in the low-temperature photoluminescence spectra of n-doped WS 2 monolayer embedded in hexagonal BN layers using external magnetic fields and first-principles calculations. Apart from the neutral A exciton line, all observed emission lines are related to the negatively charged excitons. Consequently, we identify emissions due to both the bright (singlet and triplet) and dark (spin- and momentum-forbidden) negative trions as well as the phonon replicas of the latter optically inactive complexes. The semidark trions and negative biexcitons are distinguished. On the basis of their experimentally extracted and theoretically calculated g -factors, we identify three distinct families of emissions due to exciton complexes in WS 2 : bright, intravalley, and intervalley dark. The g -factors of the spin-split subbands in both the conduction and valence bands are also determined.
Low temperature and polarization resolved magneto-photoluminescence experiments are used to investigate the properties of dark excitons and dark trions in a monolayer of WS2 encapsulated in hexagonal BN (hBN). We...
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 .
The temperature effect on the Raman scattering efficiency is investigated in $$\varepsilon$$ ε -GaSe and $$\gamma$$ γ -InSe crystals. We found that varying the temperature over a broad range from 5 to 350 K permits to achieve both the resonant conditions and the antiresonance behaviour in Raman scattering of the studied materials. The resonant conditions of Raman scattering are observed at about 270 K under the 1.96 eV excitation for GaSe due to the energy proximity of the optical band gap. In the case of InSe, the resonant Raman spectra are apparent at about 50 and 270 K under correspondingly the 2.41 eV and 2.54 eV excitations as a result of the energy proximity of the so-called B transition. Interestingly, the observed resonances for both materials are followed by an antiresonance behaviour noticeable at higher temperatures than the detected resonances. The significant variations of phonon-modes intensities can be explained in terms of electron-phonon coupling and quantum interference of contributions from different points of the Brillouin zone.
We report a study of Raman scattering in few-layer MoTe2 focused on high-frequency out-of-plane vibrational modes near 291 cm−1 which are associated with the bulk-inactive mode. Our temperature-dependent measurements reveal a double peak structure of the feature related to these modes in the Raman scattering spectra of 4- and 5-layer MoTe2. In accordance with literature data, the doublet’s lower- and higher-energy components are ascribed to the Raman-active A1g/ vibrations involving, respectively, only the inner and surface layers. We demonstrate a strong enhancement of the inner mode’s intensity at low temperature for 1.91 eV and 1.96 eV laser light excitation which suggests a resonant character of the Raman scattering processes probed under such conditions. A resonance of the laser light with a singularity of the electronic density of states at the M point of the MoTe2 Brillouin zone is proposed to be responsible for the observed effects.
Resonant conditions of the Raman scattering in monolayer WS2 encapsulated in hexagonal BN are investigated using the Raman scattering excitation technique at low temperature (T = 5 K). The resonance of the detected signal with the neutral exciton leads to an extremely rich Raman scattering excitation spectrum, which displays also the Raman scattering features not reported so far. Moreover, the intensities of the observed phonon modes are strongly enhanced when the energy difference between the excitation laser and the neutral exciton emission (X 0) is equal to the corresponding phonon energy. The intensity profile of the out-of-plane A 1 phonon mode reflects the Lorentzian lineshape of the X 0 line with the linewidth of about 4 meV, which underlines the outgoing resonance conditions with the X 0 complex.
The dielectric environment of atomically thin monolayer (ML) of semiconducting transition metal dichalcogenides affects both the electronic bandgap and the excitonic binding energy in the ML. We investigate the effect of the environment on the in-plane magnetic field brightening of neutral and charged dark exciton emissions in the WSe2 ML. The monolayers placed in three dielectric environments are studied, in particular, the ML encapsulated in hexagonal BN (hBN) flakes, the ML deposited on a hBN layer, and the ML embedded between the hBN flake and SiO2/Si substrate. We observe that the brightening rates of the neutral and charged dark excitons depend on the dielectric environment, which may be related to the variation of the level of carrier concentration in the ML. Moreover, the surrounding media, characterized by different dielectric constants, weakly influence the relative energies of the neutral and charged dark excitons in reference to the bright ones.
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