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Physical Review Letters

Polaritonic Stop-Band Transparency via Exciton-Biexciton Coupling in CuCl

Stefano Chesi, M. Artoni, Giuseppe Carlo La Rocca, F. Bassani, A. Mysyrowicz

Published Jul 29, 2003• 23 citations
Publisher

Abstract

Radiation is almost completely reflected within the exciton-polariton stop band of a semiconductor, as in the typical case of CuCl. We predict, however, that a coherently driven exciton-biexciton transition allows for the propagation of a probe light beam within the stop band. The phenomenon is reminiscent of electromagnetically induced transparency effects occurring in three-level atomic systems, except that it here involves delocalized electronic excitations in a crystalline structure via a frequency and wave-vector selective polaritonic mechanism. A well-developed transparency, favored by the narrow linewidth of the biexciton, is established within the stop band where a probe pulse may propagate with significant delays. The transparency window can be controlled via the pump beam detuning and intensity.

DOI
10.1103/physrevlett.91.057402

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Radiation is almost completely reflected within the exciton-polariton stop band of a semiconductor, as in the typical case of CuCl. We predict, however, that a coherently driven exciton-biexciton transition allows for the propagation of a probe light beam within the stop band. The phenomenon is reminiscent of electromagnetically induced transparency effects occurring in three-level atomic systems, except that it here involves delocalized electronic excitations in a crystalline structure via a frequency and wave-vector selective polaritonic mechanism. A well-developed transparency, favored by the narrow linewidth of the biexciton, is established within the stop band where a probe pulse may propagate with significant delays. The transparency window can be controlled via the pump beam detuning and intensity.
A coherently driven exciton–biexciton transition in CuCl enables one to propagate a probe light beam within the exciton-polariton stop-band where radiation is otherwise completely reflected. The stop-band transparency window can be controlled via the pump beam frequency and intensity. The phenomenon is reminiscent of quantum coherence effects occurring in three-level atomic systems, except that it here involves delocalized electronic excitations in a crystal via a frequency and wave-vector selective polaritonic mechanism. Both a free standing slab and a microcavity configuration are theoretically studied. (© 2004 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)
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.
We show that a laser beam, tuned in the transparency region of a direct-gap semiconductor, not only shifts but also splits the exciton levels. This splitting originates from the degeneracy of the valence band as the (${\ensuremath{\sigma}}_{+},{\ensuremath{\sigma}}_{\ensuremath{-}}$) parts of the light are not similarly coupled to the various exciton components. In the case of a fourfold-degenerate valence band, we find that, at large detuning, the shifts of the (2\ifmmode\times\else\texttimes\fi{}4) eightfold exciton are exactly the shifts of a (2+4) six-level atom. This is just the generalization of the simple band-structure case with one electron and one hole band in which the large detuning excitonic shift has the same value as that of the two-level (dressed) atom. We give the selection rules to observe the various shifted lines for typical pump-probe experiments. We also discuss the experimental conditions necessary to see an exciton red shift at the two-photon absorption threshold, when the molecular biexciton is stable.
The propagation of light in strongly coupled atomic media takes place through the formation of polaritons-hybrid quasiparticles resulting from a superposition of an atomic and a photonic excitation. Here we consider the propagation under the condition of electromagnetically induced transparency and show that a novel many-body phenomenon can appear due to strong, dissipative interactions between the polaritons. Upon increasing the photon-pump strength, we find a first-order transition between an opaque phase with strongly broadened polaritons and a transparent phase where a long-lived polariton branch with highly tunable occupation emerges. Across this nonequilibrium phase transition, the transparency window is reconstructed via nonlinear interference effects induced by the dissipative polariton interactions. Our predictions are based on a systematic diagrammatic expansion of the nonequilibrium Dyson equations which can be controlled, even in the nonperturbative regime of large single-atom cooperativities, provided the polariton interactions are sufficiently long-ranged. Such a regime can be reached in photonic crystal waveguides thanks to the tunability of interactions, allowing us to observe the interaction-induced transparency transition even at low polariton densities.
We study the relaxation dynamics of spin-polarized exciton-polaritons using a technique in a pump-probe configuration: According to their total angular momentum, exciton-polaritons can be excited by circularly polarized light of either σ+ or σ− helicities. In addition, a bound state of two excitons may exist to which the transition is only allowed when using two photons of opposite helicities. After excitation by a pump pulse of σ+ helicity, additional polaritons from a probe pulse of σ− helicity may be absorbed to excite biexcitons, while absorption of those with σ+ helicity becomes possible only after a spin-flip process. It is characterized by a time-constant τs, which can be determined by a time-resolved study of the induced transmission changes at the exciton–biexciton transition. We demonstrate this method using bulk CuCl, in which the biexciton binding energy is large and in which effects due to polariton propagation can be nicely evidenced. We thus identify a spectral region where the spin-flip process is dominating, which is situated just below the polariton bottleneck.