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Soviet Journal of Quantum Electronics

Investigation of two- and three-photon atomic resonances in a strong nonmonochromatic field

V. I. Anikin, Sergei A. Akhmanov, Konstantin N. Drabovich, A. N. Dubovik

Published Sep 30, 1976• 10 citations
Publisher

Abstract

An experimental investigation was made of the dispersion of the cubic susceptibility of sodium vapor in the region of two- and three-photon resonances with the 3s-4s and 3s-7p transitions. A compensation of the contributions to the nonlinear susceptibility of two- and three-photon resonances was observed. A theory was developed for the generation of the third harmonic in a nonmonochromatic field under resonance conditions and this theory was found to be in good agreement with the experimental results. A reduction in the effective susceptibility occurred in a strong field and this was due to saturation and Stark shift of the levels.

DOI
10.1070/qe1976v006n09abeh011847

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An experimental investigation was made of the dispersion of the cubic susceptibility of sodium vapor in the region of two- and three-photon resonances with the 3s-4s and 3s-7p transitions. A compensation of the contributions to the nonlinear susceptibility of two- and three-photon resonances was observed. A theory was developed for the generation of the third harmonic in a nonmonochromatic field under resonance conditions and this theory was found to be in good agreement with the experimental results. A reduction in the effective susceptibility occurred in a strong field and this was due to saturation and Stark shift of the levels.
A study was made of the influence of autoionization-like resonances in the continuum, induced by strong optical radiation, on the nonlinear susceptibilities governing third harmonic generation and the optical activity of sodium vapor. It was demonstrated experimentally for the first time that it should be possible to study high-lying states of atoms and molecules by the method of nonlinear polarization spectroscopy of the fifth-order optical nonlinearity. The experimental results were compared with the theory. An analysis was made of the feasibility of using this effect for spectroscopy of the states in the continuum and for generation of short-wavelength radiation in gaseous media.
An expression is obtained for the nonlinear susceptibility governing the addition of frequencies under resonance conditions. Allowance is made for the Stark shift, changes in populations, and transient response of the medium. Analysis is made of the stimulated emission of the third harmonic as a result of two-photon resonance in parallel and focused beams. It is shown that the saturation effect limits seriously the conversion coefficient of a nonlinear medium of fixed length. Optimal intensities of the fundamental-frequency radiation are found. It is shown that when a beam is focused sharply in a nonlinear medium, the saturation effect and Stark shift make it possible to add frequencies in media with normal dispersion. The relationship between four-photon parametric effects and coherent resonant processes such as self-induced transparency is established for ultrashort pulses.
A theoretical analysis is made of the influence of the pump intensity on the nonlinear susceptibility of the third harmonic excited under conditions of two-photon resonance between the pump wave and the Doppler-broadened transition. Pumping by both traveling and standing waves is considered. For traveling wave pumping, an expression for the nonlinear harmonic susceptibility in an arbitrary field is derived and analyzed. The optimal detunings of twice the pump frequency relative to the two-photon transition frequency are determined. For standing wave pumping an expression for the nonlinear harmonic susceptibility is obtained from perturbation theory up to and including the third order. It is shown that an important factor in the reduction of the harmonic susceptibility is the saturation of the transition due to Doppler-free two-photon absorption of opposite traveling waves.
We present a theory of Stark splitting in doubly resonant three-photon ionization (three-level system) with nonmonochromatic fields. The asymmetry of the peaks of the resonance curve due to Stark splitting is shown to be reversed when the laser bandwidth is larger than the width of the atomic transitions of the resonant states. It is further shown that ionization as well as the probe field have a significant effect on the features of the splitting. Similar effects are found with monochromatic fields in the presence of an additional level near the initial level (four-level system). The results of the analysis are in general qualitative agreement with existing observations.