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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Spectral saturation resonances in gas near a solid surface

A. P. Kol'Chenko

Published Oct 21, 1998• 0 citations
Publisher

Abstract

The nonlinear spectral lineshape of gas absorption near the solid surface in the field of one travelling monochromatic wave is analyzed theoretically. A 'far' zone of distances to the surface, where coherent particle polarization is formed already after their collisions with surface but interparticle collisions in the gas are not yet significant, is considered. It is demonstrated that the narrow saturation sub-Doppler resonances may be appeared on the Doppler lineshape in this zone. These resonances having no analogues in the gas laser spectroscopy. A formation mechanism of such resonances is discussed.

DOI
10.1117/12.328248

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The nonlinear spectral lineshape of gas absorption near the solid surface in the field of one travelling monochromatic wave is analyzed theoretically. A 'far' zone of distances to the surface, where coherent particle polarization is formed already after their collisions with surface but interparticle collisions in the gas are not yet significant, is considered. It is demonstrated that the narrow saturation sub-Doppler resonances may be appeared on the Doppler lineshape in this zone. These resonances having no analogues in the gas laser spectroscopy. A formation mechanism of such resonances is discussed.
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.
A theoretical investigation is carried out through the interaction of the plane running monochromatic light wave, having an arbitrary intensity, with atoms (molecules) of a rarefied gas in the plane cell (at the normal incidence of the wave). Cases of closed and open resonance transitions from the non-degenerate ground (or metastable) quantum level are considered. Possible sub-Doppler resonances are analysed in the wave absorption, caused by the transient establishment of the optical coherence on the transition, Rabi oscillations between its levels, and optical pumping during the free flights of particles between the walls of the cell. Results of the previous works on given problems are generalized, which were obtained at definite restrictions on the wave intensity and cell length. Moreover, non-trivial sub-Doppler spectral structures, resulting as a consequence of the dependence of the absorption saturation on the transit relaxation of particles, have been established and investigated. Such structures may consist of a number of peaks and dips caused by Rabi oscillations between the transition levels. The results obtained can be used in sub-Doppler spectroscopy and for the stabilization of laser frequencies in thin gas cells.
Using the exact solution for a sine-driven two-level system we have calculated the nonlinear absorption coefficient of a gas of two-level molecules with homogeneous (hard collisions, spontaneous decay) and inhomogeneous (Doppler effect) broadening mechanisms. We have studied the dependence of the form of the absorption lines on relaxation parameters, on the strength of the electric field, and for various ratios between the homogeneous and inhomogeneous linewidths. We include considerations about saturation of the medium caused by the external field that gives rise to the so-called power broadening of the spectral lines. The dependence of the linewidth on the saturation parameters and on the relaxation parameters is determined. These parameters appear in the ratio of the purely homogeneous and purely inhomogeneous linewidths. Asymptotic behaviors of this linewidth for the homogeneous limit and for the inhomogeneous limit are also determined.
Abstract The nonlinear optical effect of free polarization decay (FPD) in an ultrathin gas cell, the inner thickness of which is less than or on the order of the wavelength of the exciting monochromatic laser radiation propagating orthogonally to the plane-parallel walls of this cell, is studied theoretically. The considered coherent FPD signal is emitted immediately after abrupt termination of this comparatively weak stationary radiation. The sub-Doppler resonances appearing at the central frequencies of the studied quantum transitions in the FPD intensity and energy spectra due to the transit-time relaxation of atoms in the gas cell are detected and studied. It is shown that these resonances and the FPD dynamics strongly depend on the ratio between the inner thickness of the gas cell and the wavelength of the exciting monochromatic radiation. The narrow high–contrast sub-Doppler resonances of FPD observed and studied in a linear optical regime can be used in atomic (molecular) high-resolution spectroscopy and as references for compact frequency standards.
The method of sub-Doppler spectroscopy is theoretically elaborated, which is based on the specific dynamics of a number of optically excited atomic particles (atoms or molecules) of a rarefied gas medium in a thin cell after the action of the resonance pulse of the monochromatic radiation. Corresponding calculations are carried out on the basis of density matrix equations for the resonance optical transition between Zeeman degenerate ground and excited quantum levels of particles in case of the linear polarization of the laser pulse at its normal incidence on the cell. The situation is considered when the radiative lifetime of the excited level is much more than the characteristic transit time of particles between nearest plane-parallel walls of the cell. Then the distribution of a number of excited particles versus the pulse frequency detuning narrows in the process of particles collisions with walls of the cell after action of the laser pulse. The factor of such a narrowing (in comparison with the Doppler broadening of the spectral line of the resonance transition) may be more than the ratio of the characteristic transverse size of the thin gas cell to its inner thickness. We discuss possible use of given sub-Doppler resonances (of the number of excited particles) in the high-resolution spectroscopy and also in high-selective processes of photo-ionization and photo-dissociation, especially, for isotope (or isomer) separation and detection of rare (in particular single) atoms or molecules of a gas medium.
We have studied theoretically nontrivial specific features of sub-Doppler resonances of saturated absorption in a multilayer gas cell with a rarefied gas medium, which is a compact analog of a large number of plane-parallel atomic beams. Spatially separated saturating and probing monochromatic laser beams that co- and counterpropagate (at the same frequency) in this cell have been considered. In this situation, the action of the light radiation of the saturating beam on the probing beam is determined by optically pumped atoms that fly between the beams under conditions that the longitudinal components of their velocities experience selection due to a specific geometry of the multilayer cell. Such a selection leads to a narrowing of the sub-Doppler resonance in the absorption of the probing beam and decreases the difference between the structures of this resonance for the cases of co- and counterpropagation of the saturating radiation. We have found that, in the considered multilayer cell, the effective width of the sub-Doppler resonance can be smaller (by a factor of about 1.5) than the extremely narrow characteristic width of the well-known Lamb dip in spectroscopy of saturated absorption in the standard gas cell. Results of this study can be used in atomic spectroscopy of ultrahigh resolution and for the laser-frequency stabilization.