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Physical review. B, Condensed matter

Nonlinear sum rules: The three-level and the anharmonic-oscillator models

Sandro Scandolo, F. Bassani

Published Jun 15, 1992• 22 citations
Publisher

Abstract

Recently derived sum rules for nonlinear optics are shown to be relevant to a number of experiments in atomic and solid-state physics. To interpret the experiments on atomic transitions and exciton transitions in solids, we analyze the three-level model and examine the modification of the optical spectrum induced on a probe light by the presence of an additional intense light beam. We show that the nonlinear sum rules explain the known experimental data and predict anomalous asymmetry in the nonlinear line shape. We also consider the cases of vibrational states of diatomic molecules and of optical modes of polar crystals and treat them with the model of the anharmonic oscillator. The nonlinear sum rules are shown to be obeyed, thus clarifying the processes of nonlinear absorption.

DOI
10.1103/physrevb.45.13257

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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.

•Jan 1, 2001•0 citations
Recently derived sum rules for nonlinear optics are shown to be relevant to a number of experiments in atomic and solid-state physics. To interpret the experiments on atomic transitions and exciton transitions in solids, we analyze the three-level model and examine the modification of the optical spectrum induced on a probe light by the presence of an additional intense light beam. We show that the nonlinear sum rules explain the known experimental data and predict anomalous asymmetry in the nonlinear line shape. We also consider the cases of vibrational states of diatomic molecules and of optical modes of polar crystals and treat them with the model of the anharmonic oscillator. The nonlinear sum rules are shown to be obeyed, thus clarifying the processes of nonlinear absorption.
Resonant interactions of a coherent field with an anharmonic oscillator are classified based on the established analogy with multiphoton interactions of light with atoms. It is shown that interference interactions in which the absorption of a single coherent field quantum induces a multiphoton transition in the anharmonic oscillator are superpositions of resonances of the “cascade” and “lambda-V” types, and a general description of these resonances is given. For the third- and fourth-order nonlinearities, the general expressions are applicable to a resonant process with the absorption of a single photon and the double excitation of the oscillator. Resonant processes of the second harmonic generation and “rectification” of radiation are predicted and described; experimental investigation of these processes will provide information about anharmonicity parameters in the proposed model.
The resonance absorption line shape from cold (T<100(T<100(T<100 $\ensuremath{\mu}$K) atomic cesium vapor has been investigated with a probe laser after switching off the magneto-optical trapping fields. An additional nonabsorbed laser field has been used to produce quantum interference in a three-level ladder scheme. Predicted but counterintuitive modifications of the natural absorption line shape have been directly observed including inhibition of resonance absorption. The validity of a nonlinear sum rule deduced from the causality principle has been satisfactorily tested.
Introduction We have already encountered situations in which light of one frequency falling on an atomic system gives rise to light of different frequencies (cf. Section 15.6). The atom may here be considered to play the role of a (noisy) nonlinear transducer for the incident field. Even stronger nonlinear effects arise when one is dealing with a large number of atoms, or a nonlinear medium . Under these circumstances it is sometimes permissible to ignore the atomic structure and to treat the medium as a continuum, as in Maxwell's electromagnetic theory. The subject of the interaction of the incident field with the nonlinear medium is usually known as nonlinear optics. The subject had its beginnings in an experiment in which a strong beam of red light (wavelength 6943 Å) from a ruby laser was allowed to fall on a quartz crystal, and a faint beam of blue light at a wavelength of 3472 Å, the first harmonic of the red, was produced (Franken, Hill, Peters and Weinreich, 1961). The development of the subject of nonlinear optics into a mature field is due largely to the work of Bloembergen and his collaborators. In the following we shall consider only a few simple illustrative examples of phenomena in nonlinear optics. More topics and more detail can be found in the books by Bloembergen and others (Bloembergen, 1965; Yariv, 1967, Chap. 21; Shen, 1984; Schubert and Wilhelmi, 1986; Butcher and Cotter, 1990; Boyd, 1992).
Light propagation through an ensemble of ultracold Rydberg atoms in an electromagnetically-induced-transparency (EIT) configuration is studied. In strongly interacting Rydberg EIT media, nonlinear optical effects lead to a nontrivial dependence of the degree of probe-beam attenuation on the medium density and on its initial intensity. We develop a Monte Carlo rate equation model that self-consistently includes the effect of the probe-beam attenuation to investigate the steady state of the Rydberg medium driven by two laser fields. We compare our results to recent experimental data and to results of other state-of-the-art models for light propagation in Rydberg EIT media. We find that for low probe field intensities, our results match the experimental data best if a density-dependent dephasing rate is included in the model. At higher probe intensities, our model deviates from other theoretical approaches, because it predicts a spectral asymmetry together with line broadening. These are likely due to off-resonant excitation channels, which, however, have not been observed in recent experiments. Atomic motion and coupling to additional Rydberg levels are discussed as possible origins for these deviations.
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.