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Physica status solidi. C, Conferences and critical reviews/Physica status solidi. C, Current topics in solid state physics

Infrared transient absorption spectra for excited transition of excitons and biexcitons in CuCl

Takaaki Yoshioka, Kensuke Miyajima, Masaaki Ashida, Tadashi Itoh

Published Oct 20, 2008• 2 citations
Publisher

Abstract

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)

DOI
10.1002/pssc.200879905

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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 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.
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.
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)
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Abstract We investigated the influence of excitation processes of a biexciton on the generation of superfluorescence, which is pulsed radiation from coherently coupled two-level systems, from biexcitons in CuCl quantum dots. Two excitation processes of biexcitons were examined: resonant two-photon excitation of biexcitons, and resonant one-photon excitation of excitons. The excitation density dependence of the time-resolved photoluminescence was measured. The results showed that for one-photon excitation, a stronger peak intensity, longer delay time and wider pulse width were observed compared to resonant two-photon excitation. The high density of the excited dots in the one-photon excitation process results in the strong pulse, while an initial population of excitons results in a suppression of coherent coupling.
A comprehensive investigation of the optical properties of excitonic molecules in CuCl films is presented and discussed. The experimental work includes resonant two-photon absorption (TPA), observations of the resonantly excited biexciton emission, and optical pump-and-probe studies. The collision broadening of the TPA implies a collision rate \ensuremath{\sim}${10}^{\ensuremath{-}12}$ sec for the biexcitons, which is sufficiently rapid to establish a quasithermal equilibrium for the particles on a time scale that is short in comparison with the biexciton lifetime and the duration of the laser pump pulse. The biexciton luminescence line shapes obtained with resonant $\stackrel{\ensuremath{\rightarrow}}{\mathrm{k}}=0$ two-photon excitation have been fitted using a Bose-Einstein thermal distribution of biexcitons. The chemical potential obtained from the fits goes to zero as the biexciton density is increased at a fixed lattice temperature or if the lattice temperature is decreased at fixed density. The sharp luminescence features that are observed at high densities and low temperatures with single-beam, two-photon excitation are interpreted as resulting from a Bose-Einstein---condensed state of the biexcitons at twice the wave vector of the laser pumping photons. Further evidence for a condensed state is obtained from optical-probe measurements in which a small number of probe biexcitons is injected into the sample, with and without the presence of a condensed state produced by an intense laser pump beam. The luminescence of these injected probe biexcitons is modified in the presence of the pump beam such that it exhibits the sharp features of the emission from the condensed state. Measurements of optical gain and stimulated emission in the presence of the pump beam show that the redistribution of the probe luminescence does not result from those processes, but must involve a preferential redistribution of the probe particles in momentum space via collisions. Such a redistribution is expected when additional particles are added to a condensed system of bosons.