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AIP conference proceedings

Pump-probe spectroscopy of CuCl exciton-biexciton system in a slab: Aspect of EIT interpretation

Mamoru Sakaue, Kikuo Cho

Published Jan 1, 2007• 0 citations
Publisher

Abstract

Theory of pump‐probe process for weakly confined exciton‐biexciton system is revisited from the viewpoint of EIT proposed recently by Chesi et al. In order to clarify the reason why the EIT window does not come out sharp enough, we study a more detailed model of the dielectric function of a slab by renormalizing the transitions among the size quantized exciton‐biexciton levels. Numerical analysis shows that this model gives a better description of EIT behavior than that of “renormalized bulk dielectric function with generalized ABC’s” used by Chesi et al.

DOI
10.1063/1.2730216

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Theory of pump‐probe process for weakly confined exciton‐biexciton system is revisited from the viewpoint of EIT proposed recently by Chesi et al. In order to clarify the reason why the EIT window does not come out sharp enough, we study a more detailed model of the dielectric function of a slab by renormalizing the transitions among the size quantized exciton‐biexciton levels. Numerical analysis shows that this model gives a better description of EIT behavior than that of “renormalized bulk dielectric function with generalized ABC’s” used by Chesi et al.
As an application of the nonlocal theory of radiation matter interaction, pump-probe spectra for ultrathin (<500 Å) platelets of CuCl have been calculated for the pumping condition between exciton and biexciton levels. Typical aspects such as (1) pump induced absorption to biexciton states, and (2) optical Stark shift and resonant broadening of size quantized exciton levels can be seen in the calculated response spectra. The spatial variation of the light field inside the samples depends sensitively on the frequency and slab thickness, which is clearly reflected in the response spectra as quasi k -selection rule. For thicker samples the k -selection rule becomes more strictly valid, as expected.
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)
Abstract Infrared transient absorption (IRTA) spectra for excitons and biexcitons in CuCl bulk crystal have been measured by pump‐probe spectroscopy. The IRTA peak energy of the exciton agrees with the transition energy between Rydberg 1s to 2p states reported in one‐ and two‐photon absorption measurement. On the other hand, the IRTA peak energy of the biexcitons locates in energy higher than that of the excitons, which is reasonable by taking hydrogen molecule model into account. In addition, our results support the enhancement of the transition energy between 1s and 2p states in quantum dots compared to the bulk case. (© 2009 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)
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.