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Laser Physics Letters

Rise of the sub-Doppler spectroscopy resolution in thin gas cells by the spatial separation of pumping and probe radiations

А. Ч. Измайлов

Published Oct 27, 2005• 6 citations
Publisher

Abstract

The present theoretical work shows the possible essential rise of the resolution of the well tested sub-Doppler laser spectroscopy method, based on the optical pumping and transit of atoms (molecules) in a thin gas cell, by means of the definite spatial separation of pumping and probe light beams.
DOI
10.1002/lapl.200510072

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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 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.
We experimentally demonstrate two methods that improve the resolution of sub-Doppler spectroscopy using a 1 mm thick vapor cell. The linewidths of the observed spectra are approximately 1 order of magnitude narrower than the Doppler width. The first method involves using a 1 mm thick cell filled with Rb atomic vapor and two spatially separated laser beams. By employing the same principle, we also demonstrate that it is possible to achieve the same resolution by using the pump and probe pulses of a single beam. The latter method enables us to construct a simple and robust optical setup for sub-Doppler spectroscopy.
New sub-Doppler resonances at central frequencies of atomic (molecular) transitions that appear in the spectrum of absorption of the probe optical radiation under the influence of optical pumping propagating in the orthogonal direction through a relatively narrow area of a cylindrical cell containing dilute gas medium are discovered and analyzed. These resonances are induced by specific optical pumping of atoms as they fly freely from the inner cell surface through the pumped region toward the probe optical beam. The obtained mathematical relations are used to investigate the dependence of the discussed resonances on the intensity and spatial distribution of the localized optical pumping. The proposed method could allow reducing the Doppler broadening of the detected spectral lines by the factor equal to the ratio of the effective width of the narrow pumped region to the cell radius. The obtained results may find application in high-resolution spectroscopy of atoms (molecules), as well as for laser-frequency stabilization by using the discovered sub- Doppler 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.
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.