Monolayer transition metal dichalcogenides offer the possibility of optical control of the valley degree of freedom. In order to asses the potential of these materials in applications, detailed knowledge of the valley dynamics is essential. In this w
ork, we apply low temperature time-resolved photoluminescence (PL) measurements to investigate exciton valley relaxation dynamics and, in particular, its behavior under strong excitation. At the lowest excitation powers the inter valley scattering time is $simeq 50$ ps, but shortens by more than a factor of two at the highest powers. We attribute this acceleration to either heating of the exciton system or the presence of a dense exciton gas, which could influence the exciton valley properties. Furthermore, we analyze the PL dynamics of excitons and trions. We find that the PL decays for all peaks are bi-exponential and approximately independent of the excitation power. We attribute the short decay to radiative recombination and escape to a reservoir of dark states. The long decay is ascribed to a transfer of excitons back from the reservoir. For the first time, we evaluate the exciton PL decay time of $simeq$ 10 ps. The latter process is valley-conserving and occurs on a timescale of $simeq$ 50 ps.
Optical spectroscopy in high magnetic fields $Bleq65$ T is used to reveal the very different nature of carriers in monolayer and bulk transition metal dichalcogenides. In monolayer WSe$_{2}$, the exciton emission shifts linearly with the magnetic fie
ld and exhibits a splitting which originates from the magnetic field induced valley splitting. The monolayer data can be described using a single particle picture with a Dirac-like Hamiltonian for massive Dirac fermions, with an additional term to phenomenologically include the valley splitting. In contrast, in bulk WSe$_{2}$ where the inversion symmetry is restored, transmission measurements show a distinctly excitonic behavior with absorption to the 1s and 2s states. Magnetic field induces a spin splitting together with a small diamagnetic shift and cyclotron like behavior at high fields, which is best described within the hydrogen model.
Resonant Raman spectra of single layer WS$_{2}$ flakes are presented. A second order Raman peak (2LA) appears under resonant excitation with a separation from the E$^{1}_{2g}$ mode of only $4$cm$^{-1}$. Depending on the intensity ratio and the respec
tive line widths of these two peaks, any analysis which neglects the presence of the 2LA mode can lead to an inaccurate estimation of the position of the E$^{1}_{2g}$ mode, leading to a potentially incorrect assignment for the number of layers. Our results show that the intensity of the 2LA mode strongly depends on the angle between the linear polarization of the excitation and detection, a parameter which is neglected in many Raman studies.
Raman scattering and photoluminescence (PL) emission are used to investigate a single layer of tungsten disulfide (WS$_{2}$) obtained by exfoliating n-type bulk crystals. Direct gap emission with both neutral and charged exciton recombination is obse
rved in the low temperature PL spectra. The ratio between the trion and exciton emission can be tuned simply by varying the excitation power. Moreover, the intensity of the trion emission can be independently tuned using additional sub band gap laser excitation.
Magneto-photoluminescence measurements of individual zinc-blende GaAs/AlAs core/shell nanowires are reported. At low temperature a strong emission line at 1.507 eV is observed under low power (nW) excitation. Measurements performed in high magnetic f
ield allowed us to detect in this emission several lines associated with excitons bound to defect pairs. Such lines were observed before in epitaxial GaAs of very high quality, as reported by Kunzel and Ploog. This demonstrates that the optical quality of our GaAs/AlAs core/shell nanowires is comparable to the best GaAs layers grown by molecular beam epitaxy. Moreover, strong free exciton emission is observed even at room temperature. The bright optical emission of our nanowires in room temperature should open the way for numerous optoelectronic device applications.
