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Physical Review A

Direct measurement of velocity-changing collision cross sections by laser optical pumping

Gregory M. Shimkaveg, W. W. Quivers, Ramachandra Rao Dasari, Michael S. Feld

Published Aug 1, 1993• 8 citations
Publisher

Abstract

We extend the theory of velocity-selective laser optical pumping in atomic vapors, allowing for arbitrarily rapid velocity-changing collisional rates. The results yield a simple relationship between the line-shape areas of narrow spectroscopic features present in optically pumped samples. This relationship gives directly the ground- and excited-state velocity-changing collision rates and cross sections. We use the results to analyze the data from a laser optical-pumping experiment in $^{6}\mathrm{Li}$ vapor perturbed by Ar buffer gas.

DOI
10.1103/physreva.48.1409

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Velocity-selective optical pumping and collision effects

C.G. Aminoff

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.

Annales de Physique•Jan 1, 1985•2 citations
We extend the theory of velocity-selective laser optical pumping in atomic vapors, allowing for arbitrarily rapid velocity-changing collisional rates. The results yield a simple relationship between the line-shape areas of narrow spectroscopic features present in optically pumped samples. This relationship gives directly the ground- and excited-state velocity-changing collision rates and cross sections. We use the results to analyze the data from a laser optical-pumping experiment in 6Li^{6}\mathrm{Li}6Li vapor perturbed by Ar buffer gas.
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 have observed that spectral lines obtained in sodium vapor can be strongly distroted when using two-photon spectroscopy with a resonant intermediate state. In some cases, the spectral lines appear to be split into two components. We demonstrate that these effects are due to velocity-selective optical pumping of the atomic ground state; the line shapes reflect the velocity distribution of atoms in the excited intermediate state. We have analyzed the effects using the time-dependent solutions of the rate equations which describe the time evolution of optical pumping for the various atomic velocity groups, and we obtain good agreement with experiment. Optical-pumping problems are often analyzed with the use of steady-state rate equations which incorporate phenomenological relaxation; such approaches are not capable of describing our observations. Velocity-changing collisions are shown to suppress the effects and they explain why these effects were not previously observed; the previous experiments were carried out with slight amounts of a buffer gas in the vapor cell. The effects reported here must be accounted for when carrying out laser-induced line-narrowing experiments in atoms or molecules that can be optically pumped; they can also be used as a new and more sensitive probe of optical pumping in vapors.
Optical pumping of the ground states of sodium can radically alter the shape of the laser-induced fluorescence excitation spectrum, complicating measurements of temperature, pressure, etc., which are based on these spectra. Modeling of the fluorescence using rate equations for the eight hyperfine states of the sodium D manifolds can be used to quantify the contribution to the ground state pumping of transitions among the hyperfine excited states induced by collisions with buffer gas atoms. This model is used here to determine, from the shape of experimental spectra, cross sections for $\ensuremath{\Delta}F$ transitions of the P3/2{P}_{3/2}P3/2​ state induced by collisions with helium and argon atoms, for a range of values assumed for the ${P}_{1/2}, \ensuremath{\Delta}F$ cross sections. The hyperfine cross sections measured using this method, which to our knowledge is novel, are compared with cross sections for transitions involving polarized magnetic substates mF{m}_{F}mF​ measured previously using polarization sensitive absorption. Also, fine-structure transition $(\ensuremath{\Delta}J)$ cross sections were measured in the pumped vapor, giving agreement with previous measurements made in the absence of pumping.
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.
Experiments have shown the novel combination of laser optical pumping and velocity-changing collisions (between active- and buffer-gas atoms) to be very effective in producing vapors with high atomic or nuclear polarizations. This paper presents a theory which has proven successful in analyzing these experiments. The theory predicts the amount of polarization attainable for particular experimental conditions and establishes the general criteria for optimum polarization. The theory is based on sets of coupled rate equations, which contain terms describing the pumping process (i.e., stimulated absorption or emission), radiative branching, relaxation, and velocity-changing collisions. The collision terms are written in the strong-collision approximation, which assumes that a single collision, on average, thermalizes the velocity distribution. Expressions are derived for the polarization and level populations.
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.