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Register a new userMeasurement of the optical dielectric function of transition metal dichalcogenide monolayers: MoS2, MoSe2, WS2 and WSe2
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We report a determination of the complex in-plane dielectric function of monolayers of four transition metal dichalcogenides: MoS2, MoSe2, WS2 and WSe2, for photon energies from 1.5 - 3 eV. The results were obtained from reflection spectra using a Kramers-Kronig constrained variational analysis. From the dielectric functions, we obtain the absolute absorbance of the monolayers. We also provide a comparison of the dielectric function for the monolayers with the corresponding bulk materials.
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Excitons with binding energies of a few hundreds of meV control the optical properties of transition metal dichalcogenide monolayers. Knowledge of the fine structure of these excitons is therefore essential to understand the optoelectronic properties of these 2D materials. Here we measure the exciton fine structure of MoS2 and MoSe2 monolayers encapsulated in boron nitride by magneto-photoluminescence spectroscopy in magnetic fields up to 30 T. The experiments performed in transverse magnetic field reveal a brightening of the spin-forbidden dark excitons in MoS2 monolayer: we find that the dark excitons appear at 14 meV below the bright ones. Measurements performed in tilted magnetic field provide a conceivable description of the neutral exciton fine structure. The experimental results are in agreement with a model taking into account the effect of the exchange interaction on both the bright and dark exciton states as well as the interaction with the magnetic field.
Monolayer transition-metal dichalcogenides are direct gap semiconductors with great promise for optoelectronic devices. Although spatial correlation of electrons and holes plays a key role, there is little experimental information on such fundamental properties as exciton binding energies and band gaps. We report here an experimental determination of exciton excited states and binding energies for monolayer WS2 and WSe2. We observe peaks in the optical reflectivity/absorption spectra corresponding to the ground- and excited-state excitons (1s and 2s states). From these features, we determine lower bounds free of any model assumptions for the exciton binding energies as E2sA - E1sA of 0.83 eV and 0.79 eV for WS2 and WSe2, respectively, and for the corresponding band gaps Eg >= E2sA of 2.90 and 2.53 eV at 4K. Because the binding energies are large, the true band gap is substantially higher than the dominant spectral feature commonly observed with photoluminescence. This information is critical for emerging applications, and provides new insight into these novel monolayer semiconductors.
We report on the various types of Peierls like two dimensional structural modulations and relative phase stability of 2H and 1T poly-types in MoS2-ReS2 and WS2-ReS2 alloy system. Theoretical calculation predicts a polytype phase transition cross over at ~50 at.% of Mo and W in ReS2 in both monolayer and bulk form, respectively. Experimentally, two different types of structural modulations at 50% and a modulation corresponding to trimerization at 75% alloy composition is observed for MoS2-ReS2 and only one type of modulation is observed at 50% WS2-ReS2 alloy system. The 50% alloy system is found to be a suitable monolithic candidate for metal semiconductor transition with minute external perturbation. ReS2 is known to be in 2D Peierls distorted 1Td structure and forms a chain like superstructure. Incorporation of Mo and W atoms in the ReS2 lattice modifies the metal-metal hybridization between the cations and influences the structural modulation and electronic property of the system. The results offer yet another effective way to tune the electronic structure and poly-type phases of this class of materials other than intercalation, strain, and vertical stacking arrangement.
The optical selection rules for inter-band transitions in WSe2, WS2 and MoSe2 transition metal dichalcogenide monolayers are investigated by polarization-resolved photoluminescence experiments with a signal collection from the sample edge. These measurements reveal a strong polarization-dependence of the emission lines. We see clear signatures of the emitted light with the electric field oriented perpendicular to the monolayer plane, corresponding to an inter-band optical transition forbidden at normal incidence used in standard optical spectroscopy measurements. The experimental results are in agreement with the optical selection rules deduced from group theory analysis, highlighting the key role played by the different symmetries of the conduction and valence bands split by the spin-orbit interaction. These studies yield a direct determination on the bright-dark exciton splitting, for which we measure 40 $pm 1$ meV and 55 $pm 2$ meV for WSe2 and WS2 monolayer, respectively.
We have investigated the exciton dynamics in transition metal dichalcogenide mono-layers using time-resolved photoluminescence experiments performed with optimized time-resolution. For MoSe2 monolayers, we measure $tau_{rad}=1.8pm0.2$ ps that we interpret as the intrinsic radiative recombination time. Similar values are found for WSe2 mono-layers. Our detailed analysis suggests the following scenario: at low temperature (T $leq$ 50 K), the exciton oscillator strength is so large that the entire light can be emitted before the time required for the establishment of a thermalized exciton distribution. For higher lattice temperatures, the photoluminescence dynamics is characterized by two regimes with very different characteristic times. First the PL intensity drops drastically with a decay time in the range of the picosecond driven by the escape of excitons from the radiative window due to exciton- phonon interactions. Following this first non-thermal regime, a thermalized exciton population is established gradually yielding longer photoluminescence decay times in the nanosecond range. Both the exciton effective radiative recombination and non-radiative recombination channels including exciton-exciton annihilation control the latter. Finally the temperature dependence of the measured exciton and trion dynamics indicates that the two populations are not in thermodynamical equilibrium.
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