By degenerate pump and test measurements, we determine the coherence time and the lifetime of excitons in CuCl quantum dots. We show the importance of the induced recombination of coherent exciton states, excited in microcrystallites by two-photon absorption.
We present new experimental results concerning the optical nonlinearities of CuCl microcrystallites embedded in a glass matrix. Using a "pump and probe" technique, the induced absorption is measured in the spectral range of the Z3 exciton. We observe two phenomena: first, a bleaching of the excitonic resonance accompanied by the generation of a new absorption band at higher photon energies when the test probes the sample during the pump pulse; secondly, a weak shift of the excitonic resonance towards higher photon energies when probing the sample during and after the pump excitation. We vary the intensity and the photon energy of the pump beam as well as the delay between the pump and the probe pulses. Thus we can show that the pump beam populates excitonic states, which leads to a complete bleaching of the excitonic absorption. In addition, excitons can be created at higher energies, inducing the new absorption band. Its energy depends on the number of states already occupied in the microcrystallites. The shift of the excitonic resonance, on the contrary, can be explained by the heating of the microcrystallites through this high population of excitons and its non radiative decay during and after the excitation pulse.
We present a thorough investigation of the different relaxation channels opened in a strongly interacting system of excitonic quasiparticles in CuCl for density regimes ranging up to 50 MW/cm2. A spectrally narrow pump beam consisting of 30-ps pulses is tuned around one-half the biexciton energy. It creates an initial distribution of biexcitons through resonant two-photon absorption. A spectrally broad probe beam made of pulses that also have 30-ps duration monitors the excitation-induced variation of the transmission spectrum of CuCl samples near the Z3 exciton resonance. Coherent processes corresponding to parametric emissions of various orders are observed. Absorption and gain bands that reflect the evolution of biexciton and exciton populations on their respective dispersion curves are followed as functions of the time delay between pump and probe pulses.
Biexciton and triexciton states in CuCl quantum dots were studied by means of time-resolved size-selective pump-and-probe technique. A clear induced absorption band is observed on the high-energy side of the excitation photon energy. The new induced absorption is assigned to the transition from the exciton ground state to one of the weakly correlated exciton pair states which were theoretically predicted to exist and to play an important role in nonlinear optical processes. Its pump energy dependence and temporal evolution strongly support this assignment. Under high-density or two-color excitation condition, a triexciton state in quantum dots is observed for the first time.
Abstract We investigated the influence of excitation processes of a biexciton on the generation of superfluorescence, which is pulsed radiation from coherently coupled two-level systems, from biexcitons in CuCl quantum dots. Two excitation processes of biexcitons were examined: resonant two-photon excitation of biexcitons, and resonant one-photon excitation of excitons. The excitation density dependence of the time-resolved photoluminescence was measured. The results showed that for one-photon excitation, a stronger peak intensity, longer delay time and wider pulse width were observed compared to resonant two-photon excitation. The high density of the excited dots in the one-photon excitation process results in the strong pulse, while an initial population of excitons results in a suppression of coherent coupling.
Picosecond relaxation processes of excitons, including dephasing processes, are systematically studied in CuCl, CdSe and GaAs/AlAs MQW (multi-quantum well structures) by observing time-resolved induced absorption, luminescence and non-degenerate four-wave mixing. By studying the transient induced absorption from the exciton (polariton) state to the excitonic molecule state, time-resolved energy distribution of excitons in CuCl is determined (Fig.1).1) Another technique, i.e. time-resolved luminescence measurement, is applied to excitons in CdSe and GaAs/AlAs MQW (Figs.2 and 3).2,3) By analyzing the above-mentioned experiments the distribution of excitons in the two-dimensional energy-time coordinates is successfully determined. Thus, energy relaxation processes of excitons are clearly visualized. Prior to energy relaxation, coherently generated excitons are considered to be dephased. Phase relaxation of excitons in CuCl is directly measured for the first time in the picosecond time domain by means of time-resolved non-degenerate four-wave mixing (Fig.4).4) These new techniques will be demonstrated and the dephasing as well as energy relaxation mechanism of excitons and excitonic polaritons will be discussed. In the above experiments characteristics of a picosecond tunable optical parametric oscillator pumped by a mode-locked Nd3+:YAG laser as well as a picosecond tunable dye laser synchronously pumped by a mode-locked ion laser are complementarily utilized.