We demonstrate a new method to realize the population inversion of a single quantum dot excited by a laser pulse tuned within the neutral exciton phonon sideband. In contrast to the conventional method of inverting a two-level system by performing coherent Rabi oscillation, the inversion is achieved by rapid thermalization of the optically dressed states via incoherent phonon-assisted relaxation. A maximum exciton population of is measured for a laser tuned 0.83 meV to higher energy. Furthermore, the phonon sideband is mapped using a two-color pump-probe technique, with its spectral form and magnitude in very good agreement with the result of path-integral calculations.
Two-dimensional (2D) compounds provide unique building blocks for novel layered devices and hybrid photonic structures. However, large surface-to-volume ratio in thin films enhances the significance of surface interactions and charging effects requiring new understanding. Here we use micro-photoluminescence (PL) and ultrasonic force microscopy to explore the influence of the dielectric environment on optical properties of a few monolayer MoS2 films. PL spectra for MoS2 films deposited on SiO2 substrates are found to vary widely. This film-to-film variation is suppressed by additional capping of MoS2 with SiO2 and SixNy, improving mechanical coupling of MoS2 with surrounding dielectrics. We show that the observed PL non-uniformities are related to strong variation in the local electron charging of MoS2 films. In completely encapsulated films, negative charging is enhanced leading to uniform optical properties. Observed great sensitivity of optical characteristics of 2D films to surface interactions has important implications for optoelectronics applications of layered materials.
The spin dynamics in chemically synthesized CdSe/CdS core/shell nanocrystals (NCs) are studied by polarization- and time-resolved photoluminescence (PL) techniques in high magnetic fields and at low temperatures. Analysis of the recombination dynamics shows that the emission of thin-shell NCs is contributed by neutral excitons, while for thick-shell NCs it is dominated by charged excitons (trions). The sign of the PL polarization unambiguously demonstrates that these trions are negatively charged. A theoretical model of the PL polarization in an ensemble of randomly oriented NCs describes well magnetic field and time dependences of the PL polarization degree and allows us to determine the hole factor in CdSe/CdS NCs, . From direct measurements of the spin relaxation rate dependences on magnetic field and temperature, we identify the mechanism of the negative trion spin relaxation as two-phonon-assisted Raman scattering between the hole spin sublevels mixed by the applied magnetic field.