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Physical Review A

Line-shape changes due to optical pumping of Na in buffer gas

Robert E. Walkup, Annie Spielfiedel, William D. Phillips, David E. Pritchard

Published Apr 1, 1981• 38 citations
Publisher

Abstract

We have observed a collapse of the Na hyperfine doublet into a single peak due to laser-induced optical pumping when the product of laser power and buffer gas pressure exceeds \ensuremath{\sim}0.1 mW Torr. The complex line shapes observed under these conditions have been quantitatively explained by a model which describes the laser-induced change in the population of the ground-state hyperfine levels and also includes pressure broadening and diffusion of atoms out of the laser beam. The line-shape distortion can occur at laser intensities ${10}^{3}$ below that required for radiative saturation, and must be considered in experiments involving the line shape or the population of the hyperfine levels.

DOI
10.1103/physreva.23.1869

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Distortion of on-resonance two-photon spectroscopic line shapes caused by velocity-selective optical pumping

John E. Bjorkholm, P. F. Liao, Alexander J. Wokaun

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.

Physical Review A•Nov 1, 1982•32 citations
We have observed a collapse of the Na hyperfine doublet into a single peak due to laser-induced optical pumping when the product of laser power and buffer gas pressure exceeds \ensuremath{\sim}0.1 mW Torr. The complex line shapes observed under these conditions have been quantitatively explained by a model which describes the laser-induced change in the population of the ground-state hyperfine levels and also includes pressure broadening and diffusion of atoms out of the laser beam. The line-shape distortion can occur at laser intensities 103{10}^{3}103 below that required for radiative saturation, and must be considered in experiments involving the line shape or the population of the hyperfine levels.
Detailed analysis of spectral line broadening and variations in relative intensities of hyperfine spectral components due to optical pumping is presented. Hyperfine levels of sodium 3p1/23{p}_{1/2}3p1/2​ and 3p3/23{p}_{3/2}3p3/2​ levels are selectively excited in a supersonic beam at various laser intensities under the conditions when optical pumping time is shorter than transit time of atoms through the laser beam. The excitation spectra exhibit significant line broadening at laser intensities well below the saturation intensity, and redistribution of intensities of hyperfine spectral components is observed, which in some cases is contradicting with intuitive expectations. Theoretical analysis of the dynamics of optical pumping shows that spectral line broadening sensitively depends on the branching coefficient of the laser-driven transition. Analytical expressions for branching ratio dependent critical Rabi frequency and critical laser intensity are derived, which give the threshold for onset of noticeable line broadening by optical pumping. The critical laser intensity has its smallest value for transitions with branching coefficient equal to 0.5, and it can be much smaller than the saturation intensity. Transitions with larger and smaller branching coefficients are relatively less affected. The theoretical excitation spectra were calculated numerically by solving density matrix equations of motion using the split propagation technique, and they well-reproduce the observed effects of line broadening and peak intensity variations. The calculations also show that presence of dark (i.e., not laser coupled) Zeeman sublevels in the lower state results in effective branching coefficients which vary with laser intensity and differ from those implied by the sum rules, and this can lead to peculiar changes in peak ratios of hyperfine components of the spectra.
Atomic coherence gives rise to a series of interesting phenomena in quantum optics.1 In this work we investigate coherence effects within the Na Dl line, demonstrating coherent trapping and lasing without inversion, and study the dependence of these phenomena on buffer gas pressure. Two pump laser beams (I, and I2) are tuned to the frequencies υ1 and υ2 that correspond to the 3S1/2 (F=1, 2) → 3P1/2 transition and are right circularly polarized. Pockels cells are used to turn on or/and off the beams within approximately one nanosecond. To demonstrate lasing without inversion, a weak pulse of left polarized light tuned to t)2 was used to create a small population in the upper level (3P1/2) and the amplification of I, was observed. We found a significant gain in the absence of population inversion, which was verified by a direct experimental observation. These results were observed as a function of buffer gas pressure. The atomic coherence effects are shown to disappear in the presence of a helium buffer gas at a pressure of ≈ 1 Torr; whereas, complete optical pumping is only achieved at helium buffer gas pressures >10 Torr.
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.
Collision-enhanced Hanle resonances in the 3 2S1/2^{2}S_{1/2}2S1/2​ electronic ground state of Na atoms have been studied in a phase-conjugate four-wave light-mixing geometry. Narrow resonances in zero magnetic field have been observed at very high inert-buffer-gas pressures, with a width of 21 mG, or less than 10 kHz, full width at half-maximum. The intensity and the width of these resonances has been studied as a function of buffer-gas pressure, of alkali-metal vapor pressure, of detuning from the D1{D}_{1}D1​ and D2{D}_{2}D2​ Na resonances, and of the intensity of the incident light beams. Saturation phenomena and power broadening are observed. The results are explained theoretically in terms of transversely pumped optical gratings. The equivalence of this description with collision-induced coherence gratings in the limit of low light intensities is demonstrated.
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 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.