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Journal of Physics Conference Series

Observation of optical Stark effect between 1s - 2p exciton levels in CuCl single crystal

S Efumi, Yuki Uchibori, Jun Ishihara, Kensuke Miyajima

Published May 1, 2019• 3 citations
Publisher

Abstract

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.

DOI
10.1088/1742-6596/1220/1/012022

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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.
We measured the optical transitions due to the internal energy levels of an exciton and biexciton in a CuCl single crystal using pump-probe spectroscopy. The transient absorption bands due to the transitions from the 1s1s1s to 2p2p2p and from the 1s1s1s to 3p3p3p exciton states were observed at 3 K, which is consistent with their reported energies. Simultaneously, the transient absorption peak due to the biexciton was observed, which corresponds to a transition from the lowest state (composed of two 1s1s1s excitons) to higher states (composed of 1s1s1s and 2p2p2p excitons). The value of the observed biexciton peak energy was reasonable considering the hydrogen molecule orbitals and the electron-to-hole effective mass ratio. In addition, the transient absorption peaks were broadened at 77 K, because of the increase in the homogeneous width of the 2p2p2p exciton state. The transient absorption spectrum was almost completely determined by this width. Our findings are of importance with regard to the optical phenomena in the infrared region related to the quantum coherence of excitons and biexcitons in semiconductors.
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)
Large, nonlinear-optical phenomena are shown theoretically to be observable under nearly two-photon resonant pumping of the excitonic molecule (EM), e.g., in a CuCl crystal. When the exciton polariton (EP) is resonantly pumped into the EM, they are hybridized with each other and show optical Stark splitting. These splittings can be observed, respectively, as a sharp dip in the reflection spectrum and two-photon absorption spectrum due to the EM. We can also clarify how these splittings change into the blueshifts and redshifts of the EP and the EM as functions of the pump frequency and power. The generation of the phase-conjugated wave is shown also to be enhanced under two-photon resonant pumping of the EM. Some characteristics about pump-probe frequency and polarization dependences are also clarified. We have also derived the effective Hamiltonian of the exciton and the EM from the first-principles equation of motion for the exciton coupled with that of the EM. This Hamiltonian has made possible the theoretical analysis of these nonlinear-optical phenomena.
The optical Stark effect of excitons in semiconductors, where the exciton resonance is blue shifted by an off-resonance light beam, has been actively studied. Here we report on the observation of a very fast recovery of the exciton bleaching for an off-resonance excitation condition in a quantum well sample at room temperature. The good agreement between the experimental results and our numerical calculations of the time-resolved absorption spectra suggests a coherent transient population buildup and decay occurring on the time scale of the pump pulse.
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.