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Soviet Physics Uspekhi

Nonlinear effects in the emission and absorption spectra of gases in resonant optical fields

Igor M. Beterov, R. I. Sokolovskiǐ

Published Mar 31, 1973• 3 citations
Publisher

Abstract

The review systematizes the experimental material and reports the fundamental theoretical results on the study of nonlinear resonance effects in spectra of atomic systems situated in the radiation field of lasers. The theoretical part explains the topics of greatest importance and significance for understanding of the experimental studies: the Stark effect in an optical field; the nonequilibrium velocity distribution of the atoms; the shape of the spectral line for a transition adjacent to a transition combining with a strong field; the simultaneous manifestation of the Stark effect and of Doppler broadening in the form of a very sharp structure on the line contour; a brief mention of the influence of collisions, recoil, and other factors on the sharp structure in spectra. The experimental part reports the results of experiments on the observation of the Stark effect in the optical region of the spectrum, the fine structure of the profile of a Doppler-broadened line and its properties, namely the dependence on the observation direction, the anisotropy in the field of a standing wave, the polarization properties, etc. in spectra of spontaneous or stimulated emission, absorption, and generation.

DOI
10.1070/pu1973v016n03abeh005185

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The review systematizes the experimental material and reports the fundamental theoretical results on the study of nonlinear resonance effects in spectra of atomic systems situated in the radiation field of lasers. The theoretical part explains the topics of greatest importance and significance for understanding of the experimental studies: the Stark effect in an optical field; the nonequilibrium velocity distribution of the atoms; the shape of the spectral line for a transition adjacent to a transition combining with a strong field; the simultaneous manifestation of the Stark effect and of Doppler broadening in the form of a very sharp structure on the line contour; a brief mention of the influence of collisions, recoil, and other factors on the sharp structure in spectra. The experimental part reports the results of experiments on the observation of the Stark effect in the optical region of the spectrum, the fine structure of the profile of a Doppler-broadened line and its properties, namely the dependence on the observation direction, the anisotropy in the field of a standing wave, the polarization properties, etc. in spectra of spontaneous or stimulated emission, absorption, and generation.
Nonlinear effects in emission and absorption spectra of gaseous systems are considered. It is shown that level splitting can be detected spectroscopically even if it is below the Doppler width. Conditions for distinguishing interference effects from those due to nonequilibrium velocity distribution are determined. In the case of large Doppler broadening the correction for atomic motion is equivalent to the substitution of an "effective immobile atom" for the moving atom ensemble. The spectral manifestation of nonlinear effects is analyzed in detail. The influence of nonlinear interference effects on the generation characteristics in the presence of external field is investigated.
The review deals with resonance phenomena resulting from saturation of low-pressure-gas absorption lines by a coherent optical field, when the spectral lines are inhomogeneously broadened by the Doppler effect. Principal attention is paid to narrow resonances of width much smaller than the Doppler widths, which are produced upon saturation of the absorption by light waves under various experimental conditions (inside and outside the laser resonator, in traveling and standing waves, in spatially separated waves, etc.), owing to different effects (absorption saturation, mode interaction in the laser). Each of the phenomena is considered from both the theoretical and the experimental points of view. The phenomena considered serve as a basis of a new branch of optical spectroscopy, namely nonlinear laser spectroscopy of ultrahigh resolution.
The ground electronic state of even such simple atoms as those of alkali elements has the set of sublevels. These sublevels are hyperfine (HF) components and magnetic sublevels. The collisions with particles of nonmagnetic buffer gas or even with walls (when walls have proper coating) do not mix practically the populations of ground state HF sublevels, if the orbital moment of electrons in the ground state is equal to zero. Due to this reason these sublevels may be extremely long lived. Because of this, for instance, the so-called effects of optical orientation and optical pumping are apparent in atoms of alkali metals. The radiation can pump practically all the atoms (with which there is effective interaction) to a single HF component. In a situation in which optical pumping is a minor effect, the monochromatic absorption line consists of separate lines corresponding to intra-atomic transitions. The optical pumping is not significant, for example, if the radiation intensity is so low that now pumping between HF sublevels occurs in the time it takes the atom to traverse the light beam. Under the conditions of optical pumping and when other nonlinear effects are present, the absorption line profile can undergo considerable alteration. Many theoretical and experimental investigations have been done in the laser spectroscopy of resonant transitions of atoms (atoms of alkali metals) under the conditions of optical pumping within ground state HF structure. A characteristic feature of all such investigations is the velocity-selective excitation of absorbing atoms. Also, as a rule, the value of HF splitting is not very big in comparison to Doppler broadening in these experiments. Under such conditions, the absorption spectra consists of Doppler- broadened lines with nonlinear resonances, which emerge when two fields of different frequencies or different propagation directions are employed. When only one monochromatic traveling wave is employed, optical pumping leads to formation of a single smooth absorption line occupying a position between the resonant transitions frequencies associated with HF components. As HF splitting grows, the line profile remains smooth, its width is approximately equal to the size of the HF splitting. The strength of the optical pumping from one ground state HF component to another is greater for greater HF splitting in comparison to the Doppler width. In this regard, Cs and Rb are the most typical of the alkali atoms (the HF splitting exceeds the Doppler width by a factor close to 20). This is the qualitative picture of the absorption line profile (particularly for a monochromatic radiation) under the conditions of optical pumping between the HF sublevels of the electronic ground state, this qualitative picture had formed by now.
It is shown that, as a result of the atomic recoil associated with the absorption and emission of radiation, resonances can appear in nonlinear spectroscopy. The theory is illustrated by calculating the line shapes associated with nearly degenerate four-wave mixing and pump-probe spectroscopy when laser fields interact with an ensemble of two-level atoms. The recoil-induced resonances should be observable for atoms cooled below the Doppler limit of laser cooling, and the line shapes may provide a means for measuring the velocity distribution of these cooled atoms.
The features of resonance fluorescence and absorption of resonance laser radiation in atomic vapors in a superthin cell with thickness L of the order of a wavelength lambda are investigated theoretically. Taking into account the Fabry-Perot interference effect, it is found that the dependence of the fluorescence and absorption spectra on the ratio L/lambda is substantially different. Coherent spectral narrowing - the Dicke effect - when L=(2n+1)lambda/2 and broadening of the spectral line when L = n lambda (n is a whole number) are observed in the absorption spectra. This effect is absent in the spector of resonance fluorescence in extended media. It is also shown that the processes of saturation and optical pumping significantly alter the spectral line shape as the laser intensity increases; in particular, additional sub-Doppler dips appear at the frequency of the atomic transitions. Calculated curves are given for the D2 lines of ^85Rb atoms. © 2004 Optical Society of America