Splitting between Bright and Dark excitons in Transition Metal Dichalcogenide Monolayers

The optical properties of transition metal dichalcogenide monolayers such as the two-dimensional semiconductors MoS$_2$ and WSe$_2$ are dominated by excitons, Coulomb bound electron-hole pairs. The light emission yield depends on whether the electron-hole transitions are optically allowed (bright) or forbidden (dark). By solving the Bethe Salpeter Equation on top of $GW$ wave functions in density functional theory calculations, we determine the sign and amplitude of the splitting between bright and dark exciton states. We evaluate the influence of the spin-orbit coupling on the optical spectra and clearly demonstrate the strong impact of the intra-valley Coulomb exchange term on the dark-bright exciton fine structure splitting.Comment: 6 pages, 2 figure

Efficient dynamical nuclear polarization in quantum dots: Temperature dependence

We investigate in micro-photoluminescence experiments the dynamical nuclear polarization in individual InGaAs quantum dots. Experiments carried out in an applied magnetic field of 2T show that the nuclear polarization achieved through the optical pumping of electron spins is increasing with the sample temperature between 2K and 55K, reaching a maximum of about 50%. Analysing the dependence of the Overhauser shift on the spin polarization of the optically injected electron as a function of temperature enables us to identify the main reasons for this increase.Comment: 5 pages, 3 figure

Carrier and polarization dynamics in monolayer MoS2

In monolayer MoS2 optical transitions across the direct bandgap 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 4K to 300K 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 4ps. 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 bandgap energy with the excitation laser energy an emission polarization of 40% is recovered at 300K, close to the maximum emission polarization for this sample at 4K.Comment: 7 pages, 7 figures including supplementary materia

Electron spin quantum beats in positively charged quantum dots: nuclear field effects

We have studied the electron spin coherence in an ensemble of positively charged InAs/GaAs quantum dots. In a transverse magnetic field, we show that two main contributions must be taken into account to explain the damping of the circular polarization oscillations. The first one is due to the nuclear field fluctuations from dot to dot experienced by the electron spin. The second one is due to the dispersion of the transverse electron Lande g-factor, due to the inherent inhomogeneity of the system, and leads to a field dependent contribution to the damping. We have developed a model taking into account both contributions, which is in good agreement with the experimental data. This enables us to extract the pure contribution to dephasing due to the nuclei.Comment: 10 pages, 6 figure

Bistability of the Nuclear Polarisation created through optical pumping in InGaAs Quantum Dots

We show that optical pumping of electron spins in individual InGaAs quantum dots leads to strong nuclear polarisation that we measure via the Overhauser shift (OHS) in magneto-photoluminescence experiments between 0 and 4T. We find a strongly non-monotonous dependence of the OHS on the applied magnetic field, with a maximum nuclear polarisation of 40% for intermediate magnetic fields. We observe that the OHS is larger for nuclear fields anti-parallel to the external field than in the parallel configuration. A bistability in the dependence of the OHS on the spin polarization of the optically injected electrons is found. All our findings are qualitatively understood with a model based on a simple perturbative approach.Comment: Phys Rev B (in press

Spectrally narrow exciton luminescence from monolayer MoS2 exfoliated onto epitaxially grown hexagonal BN

The strong light-matter interaction in transition Metal dichalcogenides (TMDs) monolayers (MLs) is governed by robust excitons. Important progress has been made to control the dielectric environment surrounding the MLs, especially through hexagonal boron nitride (hBN) encapsulation, which drastically reduces the inhomogeneous contribution to the exciton linewidth. Most studies use exfoliated hBN from high quality flakes grown under high pressure. In this work, we show that hBN grown by molecular beam epitaxy (MBE) over a large surface area substrate has a similarly positive impact on the optical emission from TMD MLs. We deposit MoS$_2$ and MoSe$_2$ MLs on ultrathin hBN films (few MLs thick) grown on Ni/MgO(111) by MBE. Then we cover them with exfoliated hBN to finally obtain an encapsulated sample : exfoliated hBN/TMD ML/MBE hBN. We observe an improved optical quality of our samples compared to TMD MLs exfoliated directly on SiO$_2$ substrates. Our results suggest that hBN grown by MBE could be used as a flat and charge free substrate for fabricating TMD-based heterostructures on a larger scale.Comment: 5 pages, 3 figure

Robust optical emission polarization in MoS2 monolayers through selective valley excitation

We report polarization resolved photoluminescence from monolayer MoS2, a two-dimensional, non-centrosymmetric crystal with direct energy gaps at two different valleys in momentum space. The inherent chiral optical selectivity allows exciting one of these valleys and close to 90% polarized emission at 4K is observed with 40% polarization remaining at 300K. The high polarization degree of the emission remains unchanged in transverse magnetic fields up to 9T indicating robust, selective valley excitation.Comment: 5 pages, 3 figure

Exciton states in monolayer MoSe2 and MoTe2 probed by upconversion spectroscopy

Transitions metal dichalcogenides (TMDs) are direct semiconductors in the atomic monolayer (ML) limit with fascinating optical and spin-valley properties. The strong optical absorption of up to 20 % for a single ML is governed by excitons, electron-hole pairs bound by Coulomb attraction. Excited exciton states in MoSe$_2$ and MoTe$_2$ monolayers have so far been elusive due to their low oscillator strength and strong inhomogeneous broadening. Here we show that encapsulation in hexagonal boron nitride results in emission line width of the A:1$s$ exciton below 1.5 meV and 3 meV in our MoSe$_2$ and MoTe$_2$ monolayer samples, respectively. This allows us to investigate the excited exciton states by photoluminescence upconversion spectroscopy for both monolayer materials. The excitation laser is tuned into resonance with the A:1$s$ transition and we observe emission of excited exciton states up to 200 meV above the laser energy. We demonstrate bias control of the efficiency of this non-linear optical process. At the origin of upconversion our model calculations suggest an exciton-exciton (Auger) scattering mechanism specific to TMD MLs involving an excited conduction band thus generating high energy excitons with small wave-vectors. The optical transitions are further investigated by white light reflectivity, photoluminescence excitation and resonant Raman scattering confirming their origin as excited excitonic states in monolayer thin semiconductors.Comment: 14 pages, 7 figures, main text and appendi