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Physical Review Letters

Transient phase-space filling by resonantly excited exciton interactions in CuCl

R. Leonelli, J. C. Mathae, J. M. Hvam, F. Tomasini, J. B. Grün

Published Mar 30, 1987• 15 citations
Publisher

Abstract

We report time-resolved induced-absorption measurements near the ${\mathrm{Z}}_{3}$-exciton resonance in CuCl platelets which were excited at the biexciton resonance by laser pulses of 30-ps duration. We find that the excitons created through biexciton decay induce exponential tails on their absorption line. This effect can be explained in terms of exciton phase-space filling if quantum fluctuations in the local exciton density are taken into account.

DOI
10.1103/physrevlett.58.1363

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We report time-resolved induced-absorption measurements near the Z3{\mathrm{Z}}_{3}Z3​-exciton resonance in CuCl platelets which were excited at the biexciton resonance by laser pulses of 30-ps duration. We find that the excitons created through biexciton decay induce exponential tails on their absorption line. This effect can be explained in terms of exciton phase-space filling if quantum fluctuations in the local exciton density are taken into account.
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{\mathrm{cm}}^{2}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{\mathit{Z}}_{3}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.
Abstract The induced absorption due to exciton‐biexciton transitions is observed in CuCl with an experimental set‐up using two dye lasers. The shape of the absorption band is studied. The oscillator strength per exciton of this absorption is estimated and compared to theoretical evaluations. The excitation spectrum of this induced absorption is also measured and its features are tentatively explained by the existence of a superficial layer on the samples, where excitons have a very short lifetime.
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.
Abstract Using nanosecond laser pulses the time behaviour is investigated of degenerate four‐wave mixing close to the biexcitonic resonance in CuCl. The signal emission presents different time evolutions depending on excitation conditions. Its generation rate shows intensity changes and retardation effects. These effects are explained by an attenuation of the pump pulse through a time‐dependent nonlinear absorption and, at the resonance, by a loss of coherence related to collisions with bi‐excitons.
Abstract In CuCl at 1.7 K optical gain/absorption spectra are recorded in the spectral range of bound exciton and biexciton emission. Energy, effective temperature, and oscillator strength of biexcitons are determined. The observed kinetics indicates that the total pair density in the exciton‐biexciton system is pinned at about 1.6 × 1016 cm−3 for all excitation densities above 10 kW/cm2. At intense excitation, a Fano‐interference is observed between a discrete impurity absorption line and a continuum absorption tail. The latter is followed by a band of positive gain towards lower photon energies.