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Soviet Journal of Quantum Electronics

Induced autoionization-like resonances in nonlinear third- and fifth-order susceptibilities of sodium vapor

Stefan Dimov, Lubomir I. Pavlov, Yu. I. Geller, A. K. Popov

Published Aug 31, 1983• 4 citations
Publisher

Abstract

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.

DOI
10.1070/qe1983v013n08abeh004576

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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.
Efficient harmonic generation at laser-induced autoionizing state in continuum, were observed for the first time by our laboratory [1,2,3]. In this paper, nonlinear frequency mixing in alkali metal vapors at induced continuum structure in Na, are studied in detail. Besides, measurement of nonlinear optical susceptibility at induced autoionizing resonance, is performed. Tunable ultraviolet radiations by four-photon processes near induced resonances are obtained. Estimations of the real and imaginary parts of the nonlinearities, are estimated. We will specially note, that the resonant photoabsorption of ions is experimentally investigated since it gives information about the autoionizing states, which is impossible to obtain on the base only of the emission spectra. We use also laser inducing for obtaining of powerful radiation source in VUV. Thus, many actual problems as the selective impact on matter, laser photochemistry and laser isotope separation are connected directly with the induced autoionizing nonlinear resonances. The main interest is to control the spectral characteristics of continuum. The discrete level from the continuum structure leads to appearance of asymmetrical autoionizing resonance onto the background of the broad-band absorption line.
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.
The resonant self-induced optical activity (SIOA) in an atomic alkaline metal vapors has been investigated for the first time. Data on optical polarization rotation are presented and interpreted in terms of the resonance behavior of the third order susceptibility and finite elliptical polarization of real lasers. The limiting action of SIOA on the efficiency of resonance parametric generators and polarization spectroscopy is outlined. The observation of a nonlinear resonant self- induced of the laser beam polarization rotation in ruby crystal (Al2O3:Cr3+) at the laser transition are reported.
This paper investigates nonlinear processes in transitions to the continuum, and their manifestations in the photoabsorption, polarization, and angular distribution of the electrons, as well as in the nonlinear susceptibility in the case of frequency gases. Change of photoabsorption line shape by strong laser radiation upon transition to the continuum is examined. Conditions for the appearance of an induced autoionizing-like resonance in absorption are described, and allowance for the energy dependence of the matrix elements of the transitions to the continuum are examined. A discussion of narrow nonlinear resonances in ionization and recombination is presented. Induction of nonlinear resonances in a continuum when strong/radiation interacts with several close-lying discrete states is described. A presentation is given on the use of laser to induce nonlinear autoionizinglike resonances in a continuum to generate coherent radiation on the basis of frequency mixing in gases. Doppler broadening of nonlinear resonance is discussed. Phase modulation, frequency modulation and amplitude-phase modulation are outlined.