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Журнал прикладной спектроскопии

ВНУТРИДОПЛЕРОВСКАЯ СПЕКТРОСКОПИЯ ВОЗБУЖДЕННЫХ АТОМОВ В МНОГОСЛОЙНОЙ ГАЗОВОЙ ЯЧЕЙКЕ

А. Ч. Измайлов

Published Mar 19, 2020• 0 citations
OpenAlex

Abstract

The possibilities of spectroscopy in a multilayer cell with a rarefied gas medium are theoretically investigated, when this cell can be used as a compact analogue of a large number of plane-parallel beams of atoms (or molecules) on the optically excited quantum level. Such a situation is realized, in particular, for metastable and also highly excited long-lived Rydberg states of atoms and molecules. The efficiency of the velocity selection of atoms (molecules) on a similar quantum level excited by broadband optical pumping, due to their characteristic transit and collisional relaxation in the cell under consideration, is established. As a result of this selection, narrow sub-Doppler resonances arise at the frequencies of optical transitions from a given level in the absorption of a probe monochromatic light beam.

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Theoretical research is carried out of excitation of atoms from the ground quantum level to a metastable state by the running monochromatic radiation in thin gas cell, whose inner thickness is much less than its radius. As a result, sub-Doppler resonances has been discovered and analyzed, which appear in the population of the metastable atomic level at scan of the radiation frequency because of light induced Rabi oscillation on the given optical transition and also transit relaxation of atoms in the considered cell with the rarefied gas. Such nontrivial resonances may be detected in atomic fluorescence by additional probe light beam. The method for direct measurement of the Rabi frequency on spectral intervals between established sub-Doppler resonances is proposed. Obtained results may be applied in atomic spectroscopy for precise determination of components of matrix elements of dipole moments and related Einstein coefficients and oscillator strengths of quantum transitions between ground and metastable atomic levels.

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The possibilities of spectroscopy in a multilayer cell with a rarefied gas medium are theoretically investigated, when this cell can be used as a compact analogue of a large number of plane-parallel beams of atoms (or molecules) on the optically excited quantum level. Such a situation is realized, in particular, for metastable and also highly excited long-lived Rydberg states of atoms and molecules. The efficiency of the velocity selection of atoms (molecules) on a similar quantum level excited by broadband optical pumping, due to their characteristic transit and collisional relaxation in the cell under consideration, is established. As a result of this selection, narrow sub-Doppler resonances arise at the frequencies of optical transitions from a given level in the absorption of a probe monochromatic light beam.
The excitation of atoms (molecules) of a rarefied gas by stationary broadband optical radiation in a thin cell, the inner thickness of which is many times smaller than its transverse size, is studied theoretically. The features of optical pumping and transit-time relaxation of atomic particles in such cells open new possibilities for ultra-high resolution spectroscopy. The conditions are analyzed under which narrow high-contrast sub-Doppler fluorescence resonances arise at the central frequencies of spontaneous transitions from optically excited atomic (molecular) quantum levels.
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.
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.
Abstract A method of sub-Doppler spectroscopy is proposed, based on the peculiarities of narrowing over time of the velocity distribution of optically excited atoms (molecules) of a rarefied gas medium in a thin cell after exposure to a sufficiently short pulse of broadband radiation. Recording of narrow sub-Doppler resonances at the central frequencies of quantum transitions from the atomic state excited by such a pump pulse is carried out by subsequent probe monochromatic light pulses. The optimal conditions for the implementation of this spectroscopy method occur when the radiation decay time of an optically excited atomic level exceeds the characteristic time of flight of atoms between the walls of the thin cell under consideration, the inner thickness of which is many times smaller than its transverse dimensions.
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.
Theoretical research is carried out of excitation of atoms from the ground quantum level to a metastable state by the running monochromatic radiation in thin gas cell, whose inner thickness is much less than its radius. As a result, sub-Doppler resonances has been discovered and analyzed, which appear in the population of the metastable atomic level at scan of the radiation frequency because of light induced Rabi oscillation on the given optical transition and also transit relaxation of atoms in the considered cell with the rarefied gas. Such nontrivial resonances may be detected in atomic fluorescence by additional probe light beam. The method for direct measurement of the Rabi frequency on spectral intervals between established sub-Doppler resonances is proposed. Obtained results may be applied in atomic spectroscopy for precise determination of components of matrix elements of dipole moments and related Einstein coefficients and oscillator strengths of quantum transitions between ground and metastable atomic levels.