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Physical Review Letters

Push-Pull Optical Pumping of Pure Superposition States

Yuan‐Yu Jau, E. Miron, Amber Post, Nicholas N. Kuzma, W. Happer

Published Oct 13, 2004• 174 citations
Publisher

Abstract

A new optical pumping method, "push-pull pumping," can produce very nearly pure, coherent superposition states between the initial and the final sublevels of the important field-independent 0-0 clock resonance of alkali-metal atoms. The key requirement for push-pull pumping is the use of D1 resonant light which alternates between left and right circular polarization at the Bohr frequency of the state. The new pumping method works for a wide range of conditions, including atomic beams with almost no collisions, and atoms in buffer gases with pressures of many atmospheres.

DOI
10.1103/physrevlett.93.160802

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A new optical pumping method, "push-pull pumping," can produce very nearly pure, coherent superposition states between the initial and the final sublevels of the important field-independent 0-0 clock resonance of alkali-metal atoms. The key requirement for push-pull pumping is the use of D1 resonant light which alternates between left and right circular polarization at the Bohr frequency of the state. The new pumping method works for a wide range of conditions, including atomic beams with almost no collisions, and atoms in buffer gases with pressures of many atmospheres.
A vapor of alkali-metal atoms in the external cavity of a semiconductor laser, pumped with a time-independent injection current, can cause the laser to self-modulate at the "field-independent 0-0 frequency" of the atoms. Push-pull optical pumping by the modulated light drives most of the atoms into a coherent superposition of the two atomic sublevels with an azimuthal quantum number m=0. The atoms modulate the optical loss of the cavity at the sharply defined 0-0 hyperfine frequency. As in a maser, the system is not driven by an external source of microwaves, but a very stable microwave signal can be recovered from the modulated light or from the modulated voltage drop across the laser diode. Potential applications for this new phenomenon include atomic clocks, the production of long-lived coherent atomic states, and the generation of coherent optical combs.
In this thesis, we present new studies of alkali-hyperfine resonances, new optical pumping of alkali-metal atoms, and the new measurements of binary spin-exchange cross-section between alkali-metal atoms and xenon atoms. We report a large light narrowing effect of the hyperfine end-resonance signals, which was predicted from our theory and observed in our experiments. By increasing the intensity of the circularly polarized pumping beam, alkali-metal atoms are optically pumped into a state of static polarization, and trapped into the hyperfine end-state. Spin exchange between alkali-metal atoms has minimal effect on the end-resonance of the highly spinpolarized atoms. This new result will possibly benefit the design of atomic clocks and magnetometer. We also studied the pressure dependence of the atomic-clock resonance linewidth and pointed out that the linewidth was overestimated by people in the community of atomic clock. Next, we present a series study of coherent population trapping (CPT), which is a promising technique with the same or better performance compared to the traditional microwave spectroscopy. For miniature atomic clocks, CPT method is thought to be particularly advantages. From our studies, we invented a new optical-pumping method, push-pull optical pumping, which can pump atoms into nearly pure 0-0 superposition state, the superposition state of the two ground-state hyperfine sublevels with azimuthal quantum number m = 0. We believe this new invention will bring a big advantage to CPT frequency standards, the quantum state preparation for cold atoms or hot vapor, etc. We also investigated the pressure dependence of CPT excitation and the line shape of the CPT resonance theo-
We report on preliminarily results of push-pull optical pumping (PPOP) on the D1-transition of cesium. PPOP is based on a coherent population trapping effect prepared with polarization-modulated bichromatic light coupling the two ground-state hyperfine levels, the light polarization being modulated at the microwave frequency. With a suitable choice of polarizations, a single specific coherent superposition (dark state) formed by the two mF= 0 sublevels can be prepared under optimal conditions. This increase the contrast of the clock reference signal without significant line-broadening.
A variation of the usual method of atomic orientation of alkali metal vapors by optical pumping is proposed. This variation consists of employing a single circularly polarized D1{D}_{1}D1​ line as pumping radiation, instead of a mixture of the two DDD lines. Under these conditions, one magnetic substate of the ground state is transparent to the pumping radiation. It is shown that for a sufficiently intense light source and relatively weak relaxation, the entire population of the vapor will tend to be pumped into this single state, resulting in nearly one-hundred percent atomic orientation. The pumping process is analyzed in detail for sodium vapor illuminated with $3{P}_{\frac{1}{2}}\ensuremath{-}3{S}_{\frac{1}{2}}$ radiation, and the time dependence of the populations of the eight magnetic sublevels of the ground state is computed. It is shown that in the steady state, the light absorption by the vapor is linear rather than exponential with distance. A simple method of measuring relaxation times based on this observation is suggested. The conditions under which the imprisonment of resonance radiation limits the size of the oriented sample are discussed, and it is suggested that the proposed technique will allow the alignment of larger samples than is possible by the usual method of optical pumping.
A compact source which produces atomic alkali-metal beams in individual hyperfine sublevels has been developed. The methods are demonstrated with 23Na^{23}\mathrm{Na}23Na atoms. Initially nearly all atoms are transferred into one hyperfine sublevel (∣F,mF〉=∣2,2〉|F, {m}_{F}〉=|2, 2〉∣F,mF​〉=∣2,2〉) by a double-resonance technique using laser optical pumping and rf transitions. Subsequently the other hyperfine sublevels can be populated selectively by an adiabatic high-frequency transition. The hyperfine sublevel populations are determined by laser-induced fluorescence spectroscopy in a magnetic field.