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physica status solidi (b)

Biexciton resonant two‐photon absorption in CuCl

Vu Duy Phach, Albert Bivas, B. Hönerlage, J. B. Grün

Published Dec 1, 1977• 81 citations
Publisher

Abstract

Abstract In studying the two‐photon absorption (TPA) of the biexciton in CuCl by using two different light sources, interesting information is obtained. The biexciton ground‐state energy is determined accurately; its symmetry is experimentally verified; a value for the TPA coefficient is deduced and compared with a theoretical evaluation; a lineshape analysis enables us to discuss the damping constants of the exciton and biexciton states involved.

DOI
10.1002/pssb.2220840239

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Journal of the Optical Society of America B•Jan 1, 1984•0 citations
Abstract In studying the two‐photon absorption (TPA) of the biexciton in CuCl by using two different light sources, interesting information is obtained. The biexciton ground‐state energy is determined accurately; its symmetry is experimentally verified; a value for the TPA coefficient is deduced and compared with a theoretical evaluation; a lineshape analysis enables us to discuss the damping constants of the exciton and biexciton states involved.
Abstract LO‐phonon‐assisted two‐photon absorption of the first excited level of the excitonic molecule in CuCl is considered on the basis of the previously derived symmetry properties of this state. A giant cross‐section for this process is predicted mainly due to the “resonant” intermediate state Γ 1/5 of the single exciton. The process under consideration overcomes the difficulties of pure two‐photon absorption (TPA) of p‐type envelope states of the excitonic molecule as stated by Hanamura.
Abstract Two different theoretical models of the giant two‐photon absorption due to excitonic molecules (xx) are examined experimentally. The conventional model (Hanamura, 1973) follows the sequence: photon + photon → exciton + photon → xx, while the self‐consistent model (Ivanov and Haug, 1993) gives the other scenario of the two‐photon absorption: photon + photon → exciton + exciton → xx. Our high‐precision measurement of the frequency dependence of the two‐photon xx absorption coefficient in CuCl allows us to discriminate these two models and supports the new self‐consistent model.
Abstract Phonon‐assisted two‐photon absorption of biexcitonic levels in CuCl is considered including damping of the nearly resonant excitonic intermediate state. A pronounced structure of the line shape due to resonance effects, threshold effects, and structure in the Fourier transform of the envelope of the excitonic molecule is predicted. A detailed discussion of both temperature and damping effects is given. Large cross sections are predicted. The most favourable energetic range to observe the effects derived here is the low energy tail of the line, on the left of the Γ⅕ exeiton.
Abstract The induced absorption due to exciton‐biexciton transitions is observed in CuCl with an experimental set‐up using two dye lasers. The shape of the absorption band is studied. The oscillator strength per exciton of this absorption is estimated and compared to theoretical evaluations. The excitation spectrum of this induced absorption is also measured and its features are tentatively explained by the existence of a superficial layer on the samples, where excitons have a very short lifetime.
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