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.
Optical interband transitions in monolayer transition metal dichalcogenides such as WSe 2 and MoS 2 are governed by chiral selection rules. This allows efficient optical initialization of an electron in a specific K-valley in momentum space. Here we probe the valley dynamics in monolayer WSe 2 by monitoring the emission and polarization dynamics of the well separated neutral excitons (bound electron hole pairs) and charged excitons (trions) in photoluminescence. The neutral exciton photoluminescence intensity decay time is about 4ps, whereas the trion emission occurs over several tens of ps. The trion polarization dynamics shows a partial, fast initial decay within tens of ps before reaching a stable polarization of ≈ 20%, for which a typical valley polarization decay time larger than 1ns can be inferred. This is a clear signature of stable, optically initialized valley polarization.
We have measured the carrier spin dynamics in p-doped InAs/GaAs quantum dots by pump-probe and time-resolved photoluminescence experiments. We obtained experimental evidence of the hyperfine interaction between hole and nuclear spins. In the absence of an external magnetic field, our calculations based on dipole-dipole coupling between the hole and the quantum dot nuclei lead to a hole-spin dephasing time for an ensemble of dots of 14 ns, in close agreement with experiments.
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.
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