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Journal of the Physical Society of Japan

Nonlocal Theory of the Optical Stark Effect on the Size-Quantized Excitons in a Slab

Naoki Matsuura, Kikuo Cho

Published Feb 15, 1995• 7 citations
Publisher

Abstract

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.

DOI
10.1143/jpsj.64.651

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Nonlocal theory of the pump-probe spectroscopy for CuCl thin slabs under the pumping of exciton-biexciton transitions

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•Jul 25, 1995•0 citations
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.
We theoretically analyze a pump–probe experiment to detect the optical Stark effect on impurity-bound excitons taking the quantization of the pump field into account. A density matrix approach allows the calculation of the probe absorption spectra with high accuracy. For bound excitons with low inhomogeneous broadening of several tens of μeV, the photon statistics of the pump field has a considerable influence on the lineshape of the Stark-shifted resonance. The effect should be clearly observable for broad photon number distributions and low pump detuning.
We measured the transient reflection spectra induced by infrared light for a CuCl single crystal using pump-probe spectroscopy. A Stark shift of the 1 s exciton was observed using light with a near resonant energy between the 1 s and 2 p exciton levels. The amount of energy shift due to the Stark effect was obtained from the absorption spectra calculated using the Kramers–Kronig transform. We investigated the energy shift of 1 s excitons with respect to the excitation density. This is the first published report on the Stark effect of 1 s exciton associated with the internal energy levels of the excitons in CuCl crystal.
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.
The biexciton optical Stark-effect under resonant pumping between the exciton and biexciton levels is studied theoretically. The probabilities of biexciton two-photon absorption of a weak probe light and of one-photon biexciton-exciton transition are calculated. The optical Stark splitting manifests itself in two-photon biexciton absorption through two absorption peaks spaced 2 (Omega) apart. Omega is the Raby frequency. In the luminescence spectrum due to biexciton-exciton one-photon transition three luminescence maxima appear which are shifted with respect to the luminescence maximum in the case without pumping.