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Журнал прикладной спектроскопии

Внутридоплеровская флуоресцентная спектроскопия в тонких газовых ячейках при накачке широкополосным излучением

А. С. Гасанова, Ч. О. Каджар, А. Ч. Измайлов

Published May 28, 2021• 0 citations
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Abstract

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.

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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 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.
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.
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 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 linear-optical effect of the free polarization decay (FPD) in an ultrathin gas cell, the internal thickness of which is less than or of the order of the wavelength of the exciting monochromatic laser radiation, transmitted orthogonally to the plane-parallel walls of this cell, is theoretically investigated. The considered coherent FPD signal is emitted immediately after an abrupt interruption of such a relatively weak stationary radiation. Sub-Doppler resonances arising at the central frequencies of the studied quantum transitions in the spectra of the intensity and energy of the FPD as a result of the transit-time relaxation of atoms in the gas cell are established and analyzed. A significant dependence of these resonances and the dynamics of the FPD on the ratio of the inner thickness of the ultrathin cell to the wavelength of the exciting monochromatic radiation is shown. The narrow, high-contrast sub-Doppler resonances of the FPD detected and investigated in the linear-optical regime can be used in ultrahigh-resolution atomic (molecular) spectroscopy, as well as references for compact frequency standards.
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.