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Acta Physica Polonica A

Direct Two-Photon Creation of Excitonic Molecule in CuCl

W. Ungier, P. Janiszewski, Maciej Suffczynski

Published Oct 1, 2000• 1 citation
Publisher

Abstract

The probability of direct excitation of excitonic molecule in the two-photon absorption process is calculated with an Hylleraas-Ore type biexciton envelope, which is variationally optimized.In the second order of perturbation, because of the resonance effect, only the exciton .r5intermediate state is taken into account.The band structure at band extrema due to spin-orbit interaction is assumed.The transition probability of two-photon absorption is expressed by matrix element between the free exciton and the biexciton envelopes.The obtained probability of two-photon absorption in CuCl is about three orders of magnitude smaller when compared to that obtained by Hauamura.

DOI
10.12693/aphyspola.98.411

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The probability of direct excitation of excitonic molecule in the two-photon absorption process is calculated with an Hylleraas-Ore type biexciton envelope, which is variationally optimized.In the second order of perturbation, because of the resonance effect, only the exciton .r5intermediate state is taken into account.The band structure at band extrema due to spin-orbit interaction is assumed.The transition probability of two-photon absorption is expressed by matrix element between the free exciton and the biexciton envelopes.The obtained probability of two-photon absorption in CuCl is about three orders of magnitude smaller when compared to that obtained by Hauamura.
The absorption coefficient for the two-photon creation of biexciton is calculated for CuCl and wurtzite crystals. Because of the resonance effect only the intermediate lowest optically active excitonic states are taken into account. The absorption coefficient is expressed by a functional of the biexciton envelope. The numerical results are computed with the envelope function of Hylleraas-Ore type (modified and minimized by Brinkman et al). The obtained results for CuCI are in good agreement with absorption measurements published by Gale and Mysyrowicz.
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.
Line shapes of the giant two-photon absorption (GTA) band for the direct generation of excitonic molecules (EM) and the subsequent secondary emission of the EM resonantly generated have been studied in CuCl at various pump powers with the use of a high resolution spectroscopic method. The mutual collision of the EM, the rate of which is nearly proportional to their density, is found to be the main origin for causing the broadening of the GTA band, the decrease of the Raman yield and the rapid increase of the EM luminescence. The collision rate increases up to 10 12 /sec for the pump power of ∼1 MW/cm 2 . With the use of pump and probe method further evidence is obtained for the effectiveness of the mutual collision of the EM.
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.
Giant two-photon absorption spectrum for the direct generation of excitonic molecules is measured with using a frequency tunable dye laser, and absorption peak is found at 3.1870 eV. Emission spectrum with excitation at the giant two-photon absorption band depends on the spectral width, ΔΩ1\varDelta\varOmega_{1}ΔΩ1​, of excitation light. In the case of ΔΩ1=0.25\varDelta\varOmega_{1}{=}0.25ΔΩ1​=0.25 meV, the two-photon resonance Raman scattering is found to be predominant. The Raman process involves an excitonic molecule and a longitudinal exciton as the intermediate and final states, respectively. On the other hand, for the case of ΔΩ1=2.3\varDelta\varOmega_{1}{=}2.3ΔΩ1​=2.3 meV, the emission spectrum shows a very sharp line at 3.1649 eV, which has been previously ascribed to be due to the Bose-Einstein condensation of excitonic molecules. Discussions are made on the dependence of emission spectrum upon the energy band-width of excitation light.
Under the off-resonant excitation at the slightly higher energy side of the giant two-photon absorption band (GTA) for the direct generation of excitonic molecules (EM) in CuCl, new narrow emission bands designated as X T and X L have been found in the energy region of the M T and M L broad bands, respectively. Their photon energies increase with the decrease of the pump photon energy from the higher-energy side of the resonance and finally, at the on-resonant excitation, their bands merge into M T 0 and M L 0 bands, respectively, previously reported by Mita et al. Based on the detailed studies on these bands, it is found that there exists a certain kind of transverse relaxation process which acts on the EM just after their generation by the GTA and brings about the X emission as a hot luminescence.