Raman scattering and photoluminescence (PL) emission are used to investigate a single layer of tungsten disulfide (WS2) obtained by exfoliating n-type bulk crystals. Direct gap emission with both neutral and charged exciton recombination is observed in the low temperature PL spectra. The ratio between the trion and exciton emission can be tuned simply by varying the excitation power. Moreover, the intensity of the trion emission can be independently tuned using additional sub band gap laser excitation.
As defects frequently govern the properties of crystalline solids, the precise microscopic knowledge of defect atomic structure is of fundamental importance. We report a new class of point defects in single-layer transition metal dichalcogenides that can be created through 60° rotations of metal–chalcogen bonds in the trigonal prismatic lattice, with the simplest among them being a three-fold symmetric trefoil-like defect. The defects, which are inherently related to the crystal symmetry of transition metal dichalcogenides, can expand through sequential bond rotations, as evident from in situ scanning transmission electron microscopy experiments, and eventually form larger linear defects consisting of aligned 8–5–5–8 membered rings. First-principles calculations provide insights into the evolution of rotational defects and show that they give rise to p-type doping and local magnetic moments, but weakly affect mechanical characteristics of transition metal dichalcogenides. Thus, controllable introduction of rotational defects can be used to engineer the properties of these materials.
We report on detailed temperature dependent (T = 7-295 K) optical spectroscopy studies of WSe, WS, MoSe and MoS monolayers exfoliated onto the same SiO/Si substrate. In the high energy region of absorption type (reflectivity contrast-RC) and emission (photo-luminescence-PL) spectra of all the monolayers resonances related to the neutral and charged excitons (X and T) are detected in the entire measured temperature range. The optical amplitudes of excitons and trions strongly depend on the temperature and two dimensional carrier gas (2DCG) concentration. In the low energy PL spectra of WSe and WS we detect a group of lines (L) which dominates the spectra at low temperatures but rapidly quenches with the increase in the temperature. Interestingly, in the same energy range of the RC spectra recorded for WS, we observe an additional line (L ), which behaves in the same way as the L lines in the PL spectra. The optical amplitude of L and T resonances in the RC spectra strongly increases with the growth of the 2DCG concentration. On the base of these observations we identify the L resonance in the RC spectra as arising from the fine structure of the trion. We also propose that the line interpreted previously in PL spectra of WSe and WS as related to the biexciton emission is a superposition of the biexciton, trion and localized exciton emission. We find that with the temperature increase from 7-295 K the total PL intensity decreases moderately in WSe and WS, strongly in MoS and dramatically in MoSe.
Photon upconversion is an anti-Stokes process in which an absorption of a photon leads to a reemission of a photon at an energy higher than the excitation energy. The upconversion photoemission has been already demonstrated in rare earth atoms in glasses, semiconductor quantum wells, nanobelts, carbon nanotubes and atomically thin semiconductors. Here, we demonstrate a room temperature upconversion photoluminescence process in a monolayer semiconductor WS2, with energy gain up to 150 meV. We attribute this process to transitions involving trions and many phonons and free exciton complexes. These results are very promising for energy harvesting, laser refrigeration and optoelectronics at the nanoscale.
Achieving significant doping in GaAs/AlAs core/shell nanowires (NWs) is of considerable technological importance but remains a challenge due to the amphoteric behavior of the dopant atoms. Here we show that placing a narrow GaAs quantum well in the AlAs shell effectively getters residual carbon acceptors leading to an unintentional p-type doping. Magneto-optical studies of such a GaAs/AlAs core-multishell NW reveal quantum confined emission. Theoretical calculations of NW electronic structure confirm quantum confinement of carriers at the core/shell interface due to the presence of ionized carbon acceptors in the 1 nm GaAs layer in the shell. Microphotoluminescence in high magnetic field shows a clear signature of avoided crossings of the n = 0 Landau level emission line with the n = 2 Landau level TO phonon replica. The coupling is caused by the resonant hole-phonon interaction, which points to a large two-dimensional hole density in the structure.
Unlike monolayers of transition metal dichalcogenides such as MoS2, which possess high in-plane symmetry, layered ReS2 exhibits reduced in-plane crystal symmetry with a distorted 1 T structure. This unique symmetry leads to anisotropic optical properties, very promising for light polarization devices. Here, we report on low temperature polarization-resolved emission and absorption measurements of excitons in ReS2 from bulk to monolayer. In photoluminescence and reflectivity contrast spectra we distinguish two strongly polarized excitons X1 and X2 with dipole vectors along different crystal directions, which persist from bulk down to monolayer. Basing on the PL and RC spectra of bulk crystals we determine the energy of the ground and first four excited states of both excitons, which follow the usual hydrogenic Rydberg series of energy levels of 3D excitonic states (En = Ry*/n2). From the numerical fit we estimate that the energy gap is direct and equal to 1671.7 meV and binding energy of X1 and X2 is equal to 117.5 and 86.6 meV, respectively. In magneto-PL spectra of bulk ReS2 up to B = 10 T, the energy shift of all the states is below 2 meV. On reducing the crystal thickness from bulk to monolayer the ground state experience a strong blue shift.
We report on room temperature, polarization-resolved Raman scattering measurements on layered crystals of the series MoSxSe(2–x) (0 ≤ x ≤ 2) grown by chemical vapor transport technique. The results reveal two distinct sets of features related to the E2g1 and A1g modes of pure members of series. As composition x changes, the in-plane E2g1 mode shows two-mode behavior, whereas the out-of-plane A1g mode presents more complex evolution. The MoSe2-like branch reveals the splitting associated with the altering arrangement of S and Se atoms around Mo and the resulting changes in the dipole moment of the molecule. The X-ray diffraction measurements confirm that the samples are single-phase materials of 2H-type structure over the entire range of the sulfide composition x, while the scanning transmission electron microscopy imaging reveals a random arrangement of the S and Se atoms. Modified random-element-isodisplacement model is adopted to predict the behavior of the individual modes in the alloys. The model successfully confirms the two-mode behavior exhibited by the MoSxSe(2–x) series.
We have examined the influence of flake-substrate effects that affect one and few layers of MoS 2 in terms of their electrical and optical properties. In the measurements, we used SiO 2 /Si substrates with etched cavities and aluminum electrodes. Suspended areas are easily identifiable both on images depicting the topography and on the surface potential maps measured with the Kelvin probe force microscopy. Compared to the SiO 2 /Si supported material, surface potential decrease is observable at the membrane. The surface potential value of the flakes located on the electrodes is the lowest. PL measurements prove that single MoS 2 monolayer was obtained. Suspended regions are also correlated with maps obtained as a result of Raman spectroscopy.
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