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Nonlinear Optics

Observation of large coherent nonlinearity caused by exciton-exciton interaction at exciton resonance in ZnSe

Takanao Saiki, Kenneth J. Takeuchi, Makoto Kuwata‐Gonokami

Published Jan 1, 1992• 0 citations
Publisher

Abstract

Excitonic nonlinearity in wide-gap semiconductors has a strong possibility that we can realize efficient ultrafast optical interactions. Recently, we have observed very large third-order nonlinear phase shift in ZnSe layers grown by MBE on GaAs substrate [1], The third-order nonlinear susceptibility at exciton resonance is more than 10–2 esu at 10 K. Because of the biaxial strain, the valence band splits into a heavy- and a light-hole branches at Γ point [2]. To clarify the intrinsic nature of excitonic nonlinearity, the materials which are free from such strain are preferable. In this report, we present our experiments on excitonic nonlinearity using ZnSe homoepitaxial layers which are free from the strain effects [3], and discuss the origin of enhanced nonlinearity at exciton resonance in ZnSe.

DOI
10.1364/nlo.1992.tud18

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A detailed numerical study of the third-order nonlinear optical susceptibilities (χ(3)) of semiconductor quantum wells is presented. The dependence of χ(3) on material parameters (electron-hole mass ratio and exciton linewidths), on the light polarization configuration (co- and countercircularly polarized) and on the spectral configuration is discussed. The goal of this study is to map out the nonlinear phase shift per quantum well and a related figure of merit caused by quasi-resonant excitonic and biexcitonic nonlinearities induced by picosecond light pulses. The study is based on the dynamics-controlled truncation formalism and evaluated under the assumption that only 1s-heavy-hole excitons contribute to the nonlinearities. It includes all correlation effects (exciton–exciton scattering in the singlet and triplet channels and coherent biexciton formation in the singlet channel) that contribute within the coherent excitonic χ(3) regime.
This dissertation presents investigations of fundamental optical nonlinearities in semi-conductor microstructures. Two distinct effects are studied. In the first part the excitonic optical Stark effect in InGaAs and GaAs multiple quantum-well structures is investigated by means of pump-probe spectroscopy. For nonresonant excitation below the excitonic transition the direction of the shift of the resonance depends on the polarization of the pump and probe pulses. In particular, for anti-circular polarization a surprising red-shift is observed. For resonant excitation, induced absorption energetically above and below the exciton transition and bleaching of the resonance is found. Experiments using both resonant and nonresonant excitation reveal the importance of bound and unbound two-exciton states in absorption changes of the 1s heavy-hole exciton resonance. It is found that higher-order Coulomb contributions determine the intensity as well as the time dependence of the differential excitonic absorption. In addition, the influence of light-hole excitons is analyzed. It is shown that the direction of the optical Stark shift for nonresonant excitation depends also sensitively on the heavy-hole to light-hole splitting and the detuning of the pump pulse. For very high pump intensities and nonresonant excitation the absorption is split when a circularly polarized pump and a linearly polarized probe beam are used. For co-circular excitation traces of hyper-Raman gain are observed. In the second part of this dissertation, the nonlinear optical response of semiconductor microcavities in the nonperturbative regime is studied in resonant single-beam transmission and pump-probe experiments. In both types of experiment, a pronounced third transmission peak lying spectrally between the two normal modes is observed. Its dependence on the probe intensity, pump intensity, pump-probe delay, exciton-cavity detuning and pump detuning is investigated. For single-beam transmission, the energy of the third peak parallels the position of the cavity resonance. It is more pronounced for circularly polarized excitation and lasts longer than the two normal modes. For pump-probe experiments, the third peak increases with decreasing probe intensity and increasing pump intensity. Its energy is close to the low-energy side of the pump spectrum and virtually unaffected by the cavity-exciton detuning. The appearance of the third peak requires temporal overlap of pump and probe pulses. The origin of this complex nonlinearity is the quantum nature of light, which induces intraband polarizations in the presence of a coherent driving field and a finite carrier density. It is found that the coupling of the intraband polarizations via guided modes to the polarization of the fundamental longitudinal mode is responsible for the third transmission peak. A fully quantized theory reproduces the experimental observations.