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Physical review. B./Physical review. B

Optical transitions from the lowest to higher exciton and biexciton Rydberg states in CuCl

Kensuke Miyajima, K. Sakaniwa, M. Sugawara

Published Nov 28, 2016• 4 citations
Publisher

Abstract

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 $1s$ to $2p$ and from the $1s$ to $3p$ 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 $1s$ excitons) to higher states (composed of $1s$ and $2p$ 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 $2p$ 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.

DOI
10.1103/physrevb.94.195209

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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)
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.
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Coherent optical control of individual particles has been demonstrated both for atoms and semiconductor quantum dots. Here we demonstrate the emergence of quantum coherent effects in semiconductor Rydberg excitons in bulk Cu_{2}O. Because of the spectral proximity between two adjacent Rydberg exciton states, a single-frequency laser may pump both resonances with little dissipation from the detuning. As a consequence, additional resonances appear in the absorption spectrum that correspond to dressed states consisting of two Rydberg exciton levels coupled to the excitonic vacuum, forming a V-type three-level system, but driven only by one laser light source. We show that the level of pure dephasing in this system is extremely low. These observations are a crucial step towards coherently controlled quantum technologies in a bulk semiconductor.
Exciton-biexciton coherent coupling effects are examined in semiconductor quantum dots. The exciton absorption spectrum is measured with the microphotoluminescence excitation technique in a single InGaAs quantum dot. The spectrum changes from a Lorenztian-type line shape to an unusual dip-shaped line shape with increasing excitation intensities in a higher exciton state where there is a large oscillator strength between the exciton and biexciton states. The intensity dependence of the dip energy width clearly indicates that coherent Rabi oscillation occurs between the exciton and biexciton states. The absorption properties with excitation light of different polarizations show that the dip-shaped spectra only appear when there is a large biexciton state population with linear polarization. A theoretical analysis undertaken with the density matrix method agrees well with experimental results. This agreement reveals that exciton-biexciton coherent interactions lead to unusual absorption spectra and contribute crucially to the optical properties of quantum dots. The exciton-biexciton coherent effects provide a scheme for controlling four distinguishable states, which can be applied to a demonstration of quantum gate operations.