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Optics Letters

Frequency-dependent optical pumping in atomic Λ-systems

John E. Kitching, Leo W. Hollberg, Svenja A. Knappe, R. Wynands

Published Oct 1, 2001• 10 citations
Publisher

Abstract

We consider the effects of optical pumping on the conversion of laser-frequency modulation into intensity modulation by an atomic absorption line in a vapor of alkali atoms driven in a ?-configuration. It is found that, due to optical pumping in combination with the excited-state hyperfine structure, the absorption line shape is distorted substantially as the Fourier frequency of the FM is changed. The most significant effect of the distortion is a shift of the apparent line center, which depends on how the frequency of the modulation compares with the optical pumping rate. This shift has implications for locking lasers to atomic transitions and also for FM-AM noise conversion in atomic vapors.

DOI
10.1364/ol.26.001507

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Journal of the Optical Society of America B•May 1, 1995•13 citations
We consider the effects of optical pumping on the conversion of laser-frequency modulation into intensity modulation by an atomic absorption line in a vapor of alkali atoms driven in a ?-configuration. It is found that, due to optical pumping in combination with the excited-state hyperfine structure, the absorption line shape is distorted substantially as the Fourier frequency of the FM is changed. The most significant effect of the distortion is a shift of the apparent line center, which depends on how the frequency of the modulation compares with the optical pumping rate. This shift has implications for locking lasers to atomic transitions and also for FM-AM noise conversion in atomic vapors.
Optical pumping of an atomic vapor with low-power lasers often results in low pumping efficiency because of the narrow laser linewidth. Broadening of the laser spectrum by frequency modulation (FM) ensures the contribution of atoms from all velocity classes. We numerically evaluate the difference between the population enhancement for a vapor pumped with a modulated laser and that with a nonmodulated laser. The most efficient modulation scheme among those considered is FM with narrow-band Gaussian noise. The achieved optical pumping enhancement depends on laser linewidth and available power.
The ground electronic state of even such simple atoms as those of alkali elements has the set of sublevels. These sublevels are hyperfine (HF) components and magnetic sublevels. The collisions with particles of nonmagnetic buffer gas or even with walls (when walls have proper coating) do not mix practically the populations of ground state HF sublevels, if the orbital moment of electrons in the ground state is equal to zero. Due to this reason these sublevels may be extremely long lived. Because of this, for instance, the so-called effects of optical orientation and optical pumping are apparent in atoms of alkali metals. The radiation can pump practically all the atoms (with which there is effective interaction) to a single HF component. In a situation in which optical pumping is a minor effect, the monochromatic absorption line consists of separate lines corresponding to intra-atomic transitions. The optical pumping is not significant, for example, if the radiation intensity is so low that now pumping between HF sublevels occurs in the time it takes the atom to traverse the light beam. Under the conditions of optical pumping and when other nonlinear effects are present, the absorption line profile can undergo considerable alteration. Many theoretical and experimental investigations have been done in the laser spectroscopy of resonant transitions of atoms (atoms of alkali metals) under the conditions of optical pumping within ground state HF structure. A characteristic feature of all such investigations is the velocity-selective excitation of absorbing atoms. Also, as a rule, the value of HF splitting is not very big in comparison to Doppler broadening in these experiments. Under such conditions, the absorption spectra consists of Doppler- broadened lines with nonlinear resonances, which emerge when two fields of different frequencies or different propagation directions are employed. When only one monochromatic traveling wave is employed, optical pumping leads to formation of a single smooth absorption line occupying a position between the resonant transitions frequencies associated with HF components. As HF splitting grows, the line profile remains smooth, its width is approximately equal to the size of the HF splitting. The strength of the optical pumping from one ground state HF component to another is greater for greater HF splitting in comparison to the Doppler width. In this regard, Cs and Rb are the most typical of the alkali atoms (the HF splitting exceeds the Doppler width by a factor close to 20). This is the qualitative picture of the absorption line profile (particularly for a monochromatic radiation) under the conditions of optical pumping between the HF sublevels of the electronic ground state, this qualitative picture had formed by now.
Using a three-level model and semiclassical density matrix formalism, we show that optical pumping influences both line positions and amplitudes in Doppler-broadened alkali-atom D1 and D2 spectra for intensities much lower than the two-level atom saturation intensity. The influence on the D2 spectrum is particularly interesting due to the presence of closed hyperfine transitions unaffected by optical pumping. This effect is of importance for example when lasers are frequency stabilized using linear absorption or when the alkali-atom vapour pressure is determined using absorption measurements.
The features of resonance fluorescence and absorption of resonance laser radiation in atomic vapors in a superthin cell with thickness L of the order of a wavelength lambda are investigated theoretically. Taking into account the Fabry-Perot interference effect, it is found that the dependence of the fluorescence and absorption spectra on the ratio L/lambda is substantially different. Coherent spectral narrowing - the Dicke effect - when L=(2n+1)lambda/2 and broadening of the spectral line when L = n lambda (n is a whole number) are observed in the absorption spectra. This effect is absent in the spector of resonance fluorescence in extended media. It is also shown that the processes of saturation and optical pumping significantly alter the spectral line shape as the laser intensity increases; in particular, additional sub-Doppler dips appear at the frequency of the atomic transitions. Calculated curves are given for the D2 lines of ^85Rb atoms. © 2004 Optical Society of America
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.
Cs and Rb atomic vapors have been optically pumped in their ground states. The optical/rf-field configuration used allowed for the optical detection of magnetic resonance spectra with subkilohertz resolution by a pump–probe beam technique, in which the free-precessional motion of spins is recorded in the time domain. A six-level system serves as a model to describe the dependence of the observed spectra on the optical frequencies involved. With an intense laser beam applied during the free-precession period, Zeeman light-shift effects are observed. The spatial electric-field distribution of the laser beams and particle diffusion have to be taken into account to let us explain the observed magnetic resonance line shapes adequately.