We study the ground-state and finite-density optical response of molybdenum disulfide by solving the semiconductor Bloch equations, using ab initio band structures and Coulomb interaction matrix elements. Spectra for excited carrier densities up to 10(13) cm(-2) reveal a redshift of the excitonic ground-state absorption, whereas higher excitonic lines are found to disappear successively due to Coulomb-induced band gap shrinkage of more than 500 meV and binding-energy reduction. Strain-induced band variations lead to a redshift of the lowest exciton line by ∼110 meV/% and change the direct transition to indirect while maintaining the magnitude of the optical response.
We present measurements of first- and second-order coherence of quantum-dot micropillar lasers together with a semiconductor laser theory. Our results show a broad threshold region for the observed high-beta microcavities. The intensity jump is accompanied by both pronounced photon intensity fluctuations and strong coherence length changes. The investigations clearly visualize a smooth transition from spontaneous to predominantly stimulated emission which becomes harder to determine for high beta. In our theory, a microscopic approach is used to incorporate the semiconductor nature of quantum dots. The results are in agreement with the experimental intensity traces and the photon statistics measurements.
Lasers are recognized for coherent light emission, the onset of which is reflected in a change in the photon statistics. For many years, attempts have been made to directly measure correlations in the individual photon emission events of semiconductor lasers. Previously, the temporal decay of these correlations below or at the lasing threshold was considerably faster than could be measured with the time resolution provided by the Hanbury Brown/Twiss measurement set-up used. Here we demonstrate a measurement technique using a streak camera that overcomes this limitation and provides a record of the arrival times of individual photons. This allows us to investigate the dynamical evolution of correlations between the individual photon emission events. We apply our studies to micropillar lasers with semiconductor quantum dots as the active material, operating in the regime of cavity quantum electrodynamics. For laser resonators with a low cavity quality factor, Q, a smooth transition from photon bunching to uncorrelated emission with increasing pumping is observed; for high-Q resonators, we see a non-monotonic dependence around the threshold where quantum light emission can occur. We identify regimes of dynamical anti-bunching of photons in agreement with the predictions of a microscopic theory that includes semiconductor-specific effects.
We discuss the photoluminescence (PL) of semiconducting transition metal dichalcogenides on the basis of experiments and a microscopic theory. The latter connects ab initio calculations of the single-particle states and Coulomb matrix elements with a many-body description of optical emission spectra. For monolayer MoS2, we study the PL efficiency at the excitonic A and B transitions in terms of carrier populations in the band structure and provide a quantitative comparison to an (In)GaAs quantum well-structure. Suppression and enhancement of PL under biaxial strain is quantified in terms of changes in the local extrema of the conduction and valence bands. The large exciton binding energy in MoS2 enables two distinctly different excitation methods: above-band gap excitation and quasi-resonant excitation of excitonic resonances below the single-particle band gap. The latter case creates a nonequilibrium distribution of carriers predominantly in the K-valleys, which leads to strong emission from the A-exciton transition and a visible B-peak even if the band gap is indirect. For above-band gap excitation, we predict a strongly reduced emission intensity at comparable carrier densities and the absence of B-exciton emission. The results agree well with PL measurements performed on monolayer MoS2 at excitation wavelengths of 405 nm (above) and 532 nm (below the band gap).
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