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Annales de Physique

Velocity-selective optical pumping and collision effects

C.G. Aminoff

Published Jan 1, 1985• 2 citations
Publisher

Abstract

Optical pumping performed with a quasi monochromatic laser beam in an atomic gas introduces a redistribution of Zeeman populations selectively in a single velocity class. In the limit of low pumping intensity the rate theory is valid for a description of velocity-selective optical pumping (V.S.O.P.). Well-defined atomic observables (population, orientation, alignment) and their velocity-correlated collisional relaxation can be studied. Also, a modified scheme for the detection of second order effects of optical pumping allows one to observe light shift induced signals. In particular, V.S.O.P. and its combination with modulated pumping, magnetic depolarization (level crossing), and magnetic resonance techniques provide information about the atomic collision characteristics such as collision rates and kernels for velocity-changing collisions.

DOI
10.1051/anphys:01985001006099500

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In 1950, Professor Alfred Kastler described the way in which optical fields could be used to redistribute population among the Zeeman sublevels of a given atomic state. The « optical pumping » process discovered by Kastler continues to be a research topic of current interest. With developments in laser spectroscopy, it has become important to understand the interplay of optical pumping, transit-time and collisional effects to properly interpret experimental line shapes. A brief review of the current status of the theory is given, with special emphasis on what, as yet, appear to be unresolved problems. Velocity selective optical pumping and collision-induced resonances are discussed.

Annales de Physique•Jan 1, 1985•0 citations
Optical pumping performed with a quasi monochromatic laser beam in an atomic gas introduces a redistribution of Zeeman populations selectively in a single velocity class. In the limit of low pumping intensity the rate theory is valid for a description of velocity-selective optical pumping (V.S.O.P.). Well-defined atomic observables (population, orientation, alignment) and their velocity-correlated collisional relaxation can be studied. Also, a modified scheme for the detection of second order effects of optical pumping allows one to observe light shift induced signals. In particular, V.S.O.P. and its combination with modulated pumping, magnetic depolarization (level crossing), and magnetic resonance techniques provide information about the atomic collision characteristics such as collision rates and kernels for velocity-changing collisions.
We consider optical pumping with a quasi monochromatic tunable light beam, in the low intensity limit where a rate equation regime is obtained The velocity selective optical pumping (V.S.O.P.) introduces a correlation between atomic velocity and internal variables in the ground (or metastable) state. The aim of this article is to evaluate these atomic observables (orientation, alignment, population) as a function of velocity, using a phenomenological description of the relaxation effect of collisions. The V.S.O.P. line shapes, obtained by scanning the pumping beam frequency and using a counterpropagating detection beam with the same frequency, are given in various circumstances. The combination of V.S.O.P. with modulated pumping, magnetic resonance, and level crossing methods is considered; the corresponding line shapes can provide useful information on the relaxation characteristics, such as collision rates and kernels.
We describe a spectroscopic method combining saturated absorption and Zeeman optical pumping. A weak expanded monochromatic laser beam creates a velocity-correlated orientation in an atomic level without optical saturation. A polarization-modulated counterpropagating detection beam provides signals related to simple atomic observables. Combination with magnetic resonance techniques is described. We have applied this method to metastable states of Ne, with nuclear or electronic orientation. Effects of velocity-changing, depolarization (Kastler- or Dehmelt-type pumping) or metastability exchange collisions are discussed.
We report on a quantitative experimental investigation of velocity-changing collisions by means of velocity-selective optical pumping (VSOP). We have calculated the VSOP line shape for an atom with hyperfine structure with the use of two phenomenological kernels for the collision effects: the Keilson-Storer kernel, and a two-term kernel consisting of a broad Keilson-Storer part and a narrower Gaussian component. Corrections were included to account for the finite absorption in the sample and the backward reflection of the pumping beam. The experiments were carried out in sodium vapor with neon as the perturber gas. The D1{D}_{1}D1​ line of sodium was used for optical pumping, and the orientation of the ground state was detected. Free parameters of the theory were determined by fitting the predicted line shapes to experimental curves. The Keilson-Storer kernel proved unsatisfactory, but the two-term kernel reproduced well the observed line shapes over the entire collision profiles in the neon pressure range 0-57 mtorr. In an independent experiment using rapidly modulated VSOP we also measured directly the cross section of velocity-changing collisions: $\ensuremath{\sigma}=(1.13\ifmmode\pm\else\textpm\fi{}0.10)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}14}$ cm2{\mathrm{cm}}^{2}cm2. The large weight obtained for the narrow Gaussian from the fits, as well as the collision cross section which is three times as large as the cross section deduced from tabulated gas kinetic radii, may indicate the presence of collisions with relatively small velocity changes in addition to hard-sphere encounters.
We report new results on the effect of collisions on radio-frequency (rf) -laser double resonances in an atomic vapor under conditions of velocity-selective optical pumping. Our experiments are performed on Zeeman resonances in the 4${f}^{6}666{s}^{2}$ 7{\mathrm{}}^{7}7F1{F}_{1}F1​--4${f}^{6}$6s6p 7{\mathrm{}}^{7}7F0{F}_{0}F0​ transition in samarium vapor in the presence of rare-gas perturbers (He, Ne, Ar, Xe). The collisional relaxation of the rf-generated sublevel coherence is studied using Raman heterodyne detection; this recently introduced spectroscopic technique is capable of separately yielding signal contributions originating from optically resonant and off-resonant atoms. The corresponding measurements clearly reveal that velocity-changing collisions (VCC) can completely determine the characteristics of the rf-laser double-resonance signals. Our experimental findings on the linewidths and line shapes of the rf resonances are in satisfactory quantitative agreement with theoretical predictions that are based on a novel four-level density-matrix calculation; here a Keilson-Storer collision kernel is used to describe the velocity diffusion processes. The comparison of calculated and measured results also permits us to derive cross sections for VCC and depolarizing collisions; moreover, information on the spectrum of the velocity changes connected with alignment-preserving collisions can be obtained.
Reports the optogalvanic detection of observables induced by optical pumping in metastable states of neon. As with optical methods signals are obtained which are related to electronic and nuclear orientation or alignment. Many optical pumping experiments may thus be performed using optogalvanic techniques, including the Hanle effect and 'velocity selective optical pumping' described. Different mechanisms are discussed from which optogalvanic signals related to non-scalar observables may originate. Profiles obtained from frequency sweeps of two polarisation-modulated counterpropagating pump beams indicate the dominant mechanism is a second-order pumping effect which induces a modulated depletion of the metastable state. No effect has been observed arising from a variation of the Penning collision cross section when the two metastable colliding atoms are oriented. The analogy between signals produced by optogalvanic and optical methods are pointed out.
In 1950, Professor Alfred Kastler described the way in which optical fields could be used to redistribute population among the Zeeman sublevels of a given atomic state. The « optical pumping » process discovered by Kastler continues to be a research topic of current interest. With developments in laser spectroscopy, it has become important to understand the interplay of optical pumping, transit-time and collisional effects to properly interpret experimental line shapes. A brief review of the current status of the theory is given, with special emphasis on what, as yet, appear to be unresolved problems. Velocity selective optical pumping and collision-induced resonances are discussed.