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

Sub-Doppler spectroscopy based on optical pumping and transit relaxation of atoms in a thin gas cell

А. Ч. Измайлов

Published Jun 15, 2007• 7 citations
Publisher

Abstract

The paper is the review of methods, achievements, and possibilities of the recently elaborated and well tested high-resolution laser spectroscopy based on sub-Doppler absorption and polarization resonances (on centers of quantum transitions), which arise because of the optical pumping and specific transit relaxation of atoms (molecules) in a thin cell with a rarefied gas. Theoretical basis of this spectroscopy is presented. Experimental technique and results on the record of the sub-Doppler spectral structure of Cs and Rb atoms and on the frequency stabilization of diode lasers by given spectroscopy methods are discussed.

DOI
10.1117/12.752243

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The paper is the review of methods, achievements, and possibilities of the recently elaborated and well tested high-resolution laser spectroscopy based on sub-Doppler absorption and polarization resonances (on centers of quantum transitions), which arise because of the optical pumping and specific transit relaxation of atoms (molecules) in a thin cell with a rarefied gas. Theoretical basis of this spectroscopy is presented. Experimental technique and results on the record of the sub-Doppler spectral structure of Cs and Rb atoms and on the frequency stabilization of diode lasers by given spectroscopy methods are discussed.
This work continues a theoretical investigation of the capabilities of the well-known method based on using a monochromatic probe light beam in combination with optical pumping of atoms (molecules) of a rarefied-gas medium by a broadband radiation in a thin cell the diameter of which is much larger than its internal thickness. In contrast to calculations carried out in the previous publications on this method of spectroscopy, here, we consider the case of arbitrary values of pump intensity and thickness of a cylindrical gas cell. Thus, all the possible mechanisms and specificities of velocity selection of atoms in optically excited levels caused by transit-time relaxation of such atoms in gas cells of this kind are analyzed. Within the framework of this approach, sub-Doppler absorption resonances of the probe light beam corresponding to quantum transitions from the upper level excited by optical pumping are investigated. The obtained results can be used in high-resolution spectroscopy of atoms (molecules), as well as for laser-frequency stabilization to established narrow spectral resonances.
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.
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 degen- erate 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 par- ticles collisions with walls of the cell after action of the laser pulse. The factor of such a narrowing (in compar- ison 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.
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.
By analogy with the well-tested method of high-resolution spectroscopy in thin gas cells for the processes of optical pumping of atoms, this work shows the possibility of detecting narrow sub-Doppler optical resonances caused directly by straight photoionization of atoms (or molecules) in such cells. The structure of the established nontrivial resonances substantially depends on the probability of photoionization of atoms and dimensions of such a cell, the internal thickness of which is many times smaller than its diameter. Of particular interest is the broadening of the considered sub-Doppler resonances, which is determined directly by the photoionization cross section of atoms and the intensity of radiation causing ionization. Under certain conditions, such photoionization broadening can be measured experimentally with high accuracy, as a result of which it is possible to obtain new important information about ionization processes in atoms and molecules. Keywords: sub-Doppler resonances, photoionization of atoms, thin gas cell, transit-time relaxation of atoms.