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A three-order of magnitude increase in the optical second-harmonic emission of WSe${}_{2}$ monolayers is detected by tuning the exciting laser beam to the WSe${}_{2}$ exciton resonances.

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 ${\mathrm{MoS}}_{2}$, 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.

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.