The strong light-matter interaction and the valley selective optical selection rules make monolayer (ML) MoS 2 an exciting 2D material for fundamental physics and optoelectronics applications. But, so far, optical transition linewidths even at low temperature are typically as large as a few tens of meV and contain homogeneous and inhomogeneous contributions. This prevented in-depth studies, in contrast to the bettercharacterized ML materials MoSe 2 and WSe 2 . In this work, we show that encapsulation of ML MoS 2 in hexagonal boron nitride can efficiently suppress the inhomogeneous contribution to the exciton linewidth, as we measure in photoluminescence and reflectivity a FWHM down to 2 meV at T ¼ 4 K. Narrow optical transition linewidths are also observed in encapsulated WS 2 , WSe 2 , and MoSe 2 MLs. This indicates that surface protection and substrate flatness are key ingredients for obtaining stable, high-quality samples. Among the new possibilities offered by the well-defined optical transitions, we measure the homogeneous broadening induced by the interaction with phonons in temperature-dependent experiments. We uncover new information on spin and valley physics and present the rotation of valley coherence in applied magnetic fields perpendicular to the ML.

We show that the light-matter interaction in monolayer WSe_{2} is strongly enhanced when the incoming electromagnetic wave is in resonance with the energy of the exciton states of strongly Coulomb bound electron-hole pairs below the electronic band gap. We perform second harmonic generation (SHG) spectroscopy as a function of laser energy and polarization at T=4  K. At the exciton resonance energies we record an enhancement by up to 3 orders of magnitude of the SHG efficiency, due to the unusual combination of electric dipole and magnetic dipole transitions. The energy and parity of the exciton states showing the strong resonance effects are identified in 1- and 2-photon photoluminescence excitation experiments, corroborated by first principles calculations. Targeting the identified exciton states in resonant 2-photon excitation allows us to maximize k-valley coherence and polarization.

In monolayer MoS2, optical transitions across the direct band gap are governed by chiral selection rules, allowing optical valley initialization. In time-resolved photoluminescence (PL) experiments, we find that both the polarization and emission dynamics do not change from 4 to 300 K within our time resolution. We measure a high polarization and show that under pulsed excitation the emission polarization significantly decreases with increasing laser power. We find a fast exciton emission decay time on the order of 4 ps. The absence of a clear PL polarization decay within our time resolution suggests that the initially injected polarization dominates the steady-state PL polarization. The observed decrease of the initial polarization with increasing pump photon energy hints at a possible ultrafast intervalley relaxation beyond the experimental ps time resolution. By compensating the temperature-induced change in band gap energy with the excitation laser energy, an emission polarization of 40% is recovered at 300 K, close to the maximum emission polarization for this sample at 4 K.

The optical selection rules for interband transitions in WSe_{2}, WS_{2}, and MoSe_{2} 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 interband 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 of the bright-dark exciton splitting, for which we measure 40±1  meV and 55±2  meV in WSe_{2} and WS_{2} monolayer, respectively.

We study the neutral exciton energy spectrum fine structure and its spin dephasing in transition metal dichalcogenides such as MoS2. The interaction of the mechanical exciton with its macroscopic longitudinal electric field is taken into account. The splitting between the longitudinal and transverse excitons is calculated by means of the both electrodynamical approach and k ·p perturbation theory. This long-range exciton exchange interaction can induce valley polarization decay. The estimated exciton spin dephasing time is in the picosecond range, in agreement with available experimental data.PACS numbers: 71.70.Gm,72.25.Rb,78.66.Li Introduction. Monolayers (MLs) of transition metal dichalcogenides, in particular, MoS 2 form a class of novel two-dimensional materials with interesting electronic and optical properties. The direct band gap in these systems is realized at the edges of the Brillouin zone at points K + and K − .1 Strikingly, each of the valleys can be excited by the radiation of given helicity only.2-4 Recent experiments have indeed revealed substantial optical orientation in ML MoS 2 related to selective excitation of the valleys by circularly polarized light.5-8 Strong spin-orbit coupling in this material lifts the spin degeneracy of electron and hole states even at K + and K − points of the Brillouin zone resulting in relatively slow spin relaxation of individual charge carriers, which requires their intervalley transfer.9-13 However recent time-resolved measurements revealed surprisingly short, in the picosecond range, transfer times between valleys.14,15 This could be due to excitonic effects which are strong in transition metal dichalcogenides 16,17 Although individual carrier spin flips are energetically forbidden, spin relaxation of electron-hole pairs can be fast enough owing to the exchange interaction between an electron and a hole forming an exciton, 18,19 in close analogy to exciton dephasing in quantum wells.

, Room-temperature defect-engineered spin filter based on a nonmagnetic semiconductor

We investigate exciton dynamics in 2H-WSe2 bilayers in time-resolved photoluminescence (PL) spectroscopy. Fast PL emission times are recorded for both the direct exciton with $\tau_{D}$ ~ 3 ps and the indirect optical transition with $\tau_{i}$ ~ 25 ps. For temperatures between 4 to 150 K $\tau_{i}$ remains constant. Following polarized laser excitation, we observe for the direct exciton transition at the K point of the Brillouin zone efficient optical orientation and alignment during the short emission time $\tau_{D}$. The evolution of the direct exciton polarization and intensity as a function of excitation laser energy is monitored in PL excitation (PLE) experiments.Comment: 4 pages, 3 figure

We combine linear and non-linear optical spectroscopy at 4 K with ab initio calculations to study the electronic bandstructure of MoSe2 monolayers. In 1-photon photoluminescence excitation (PLE) and reflectivity we measure a separation between the A-and B-exciton emission of 220 meV. In 2-photon PLE we detect for the A-and B-exciton the 2p state 180 meV above the respective 1s state. In second harmonic generation (SHG) spectroscopy we record an enhancement by more than 2 orders of magnitude of the SHG signal at resonances of the charged exciton and the 1s and 2p neutral A-and B-exciton. Our post-Density Functional Theory calculations show in the conduction band along the K − Γ direction a local minimum that is energetically and in k-space close to the global minimum at the K-point. This has a potentially strong impact on the polarization and energy of the excitonic states that govern the interband transitions and marks an important difference to MoS2 and WSe2 monolayers.