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Physical Review A

Enhancement of optically pumped spin orientation via spin-exchange collisions at low vapor density

Witold Chałupczak, R. M. Godun, Pawel Anielski, Adam M. Wojciechowski, Szymon Pustelny, Wojciech Gawlik

Published Apr 4, 2012• 37 citations
Publisher

Abstract

An effect is demonstrated where off-resonant optical pumping is enhanced by spin-exchange collisions, which enables a high degree of spin orientation to be obtained in alkali-metal atoms. The experiment with room-temperature cesium vapor employs radio-frequency spectroscopy under conditions of the nonlinear Zeeman effect that allow the populations of the individual Zeeman sublevels to be determined. The improved efficiency of atomic orientation leads to a significant reduction of population relaxation out of the state with maximum magnetic quantum number $m$ (stretched state), which is observed as a narrowing of radio-frequency resonances. Spin-exchange collisions play a crucial role in this effect although the applied atomic density $\ensuremath{\sim}$10${}^{11}$ cm${}^{\ensuremath{-}3}$ corresponds to collision rates not greater than several tens of Hz. A simplified theoretical model has been developed to reproduce the measurement results numerically.

DOI
10.1103/physreva.85.043402

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The effect of spin-exchange collisions on the state populations obtained in an optically pumped ${\mathrm{Na}}^{23}$ vapor is studied in the limit of low light intensity. These state populations and hence the intensity of the rf Zeeman transitions are found theoretically to depend strongly on the spin-exchange cross sections. The various Zeeman rf transitions are found experimentally to be very different in intensity and this is interpreted as being partially due to spin-exchange collisions. From the intensity of the rf transitions in a magnetic field large enough to separate the six Zeeman components and from the observed relaxation time a spin-exchange cross section for two sodium atoms of $\ensuremath{\pi}{{S}_{0}}^{2}=6\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}14}$ ${\mathrm{cm}}^{2}$ is found.

Physical Review•Dec 15, 1961•14 citations
An effect is demonstrated where off-resonant optical pumping is enhanced by spin-exchange collisions, which enables a high degree of spin orientation to be obtained in alkali-metal atoms. The experiment with room-temperature cesium vapor employs radio-frequency spectroscopy under conditions of the nonlinear Zeeman effect that allow the populations of the individual Zeeman sublevels to be determined. The improved efficiency of atomic orientation leads to a significant reduction of population relaxation out of the state with maximum magnetic quantum number mmm (stretched state), which is observed as a narrowing of radio-frequency resonances. Spin-exchange collisions play a crucial role in this effect although the applied atomic density \ensuremath∼\ensuremath{\sim}\ensuremath∼1011{}^{11}11 cm\ensuremath−3{}^{\ensuremath{-}3}\ensuremath−3 corresponds to collision rates not greater than several tens of Hz. A simplified theoretical model has been developed to reproduce the measurement results numerically.
Traditionally, atomic spin orientation is achieved by the transfer of angular momentum from polarized light to an atomic system. We demonstrate the mechanism of orientation generation in room-temperature caesium vapors that combines three elements: optical pumping, nonlinear spin dynamics, and spin-exchange collisions. Through the variation of the spin-exchange relaxation rate, the transition between an aligned and an oriented atomic sample is presented. The observation is performed by monitoring the atomic radio-frequency spectra. The measurement configuration discussed paves the way to simple and robust radio-frequency atomic magnetometers that are based on a single low-power laser diode that approach the performance of multilaser pump-probe systems.
The relaxation and generation of multipole orientations in a heavy-alkali-metal vapor in the presence of a weak static magnetic field are theoretically studied both for populations and for Zeeman coherences by taking into account the effects on the evolution of the atomic density matrix of the relaxation processes (by alkali-atom--buffer-gas, alkali-atom--alkali-atom with spin exchange and alkali-atom--cell-wall collisions) and of the optical pumping with any light polarization and spectral distribution. The dependence of the stationary-state multipole orientations on the pumping characteristic parameters is numerically analyzed. The detection process of these orientations is also studied.
Spin-exchange collisions often play a dominant role in the broadening of Zeeman resonances in an alkali-metal vapor. Contrary to intuitive expectations, at high alkali-metal densities this broadening can be completely eliminated by operating in a low magnetic field, allowing construction of ultrasensitive atomic magnetometers. We describe a detailed study of the Zeeman resonance frequencies and linewidths as a function of the magnetic field, alkali-metal density, and the degree of spin polarization of the atoms. Due to the nonlinear nature of the density matrix equations describing the spin-exchange collisions both the gyromagnetic ratio and the linewidth change as a function of the polarization. The results of experimental measurements are in excellent agreement with analytical and numerical solutions of the density matrix equations.
A new and unusual phenomenon which we call light narrowing is reported and discussed in this paper. We discovered this effect in dense, spin-polarized cesium vapor optically pumped with a cw blue dye laser beam tuned to the second resonance D1{D}_{1}D1​ line (4593 \AA{}). We observe a significant narrowing of the radio-frequency power-broadened magnetic resonance lines (linewidths narrow by as much as a factor of 2.5) when the intensity of the circularly polarized incident dye laser beam is increased by either focusing the beam or by the removal of attenuating filters from the focused beam. The magnetic resonance linewidths in spin-polarized cesium vapor were measured over a wide range of cesium number densities (5\ifmmode\times\else\texttimes\fi{}1012{10}^{12}1012 ${\mathrm{cm}}^{\ensuremath{-}3}$ \ensuremath{\le}[Cs]\ensuremath{\le}1\ifmmode\times\else\texttimes\fi{}1016{10}^{16}1016 ${\mathrm{cm}}^{\ensuremath{-}3}$). This corresponds to cesium spinexchange rates of 4.5\ifmmode\times\else\texttimes\fi{}103{10}^{3}103 to 9\ifmmode\times\else\texttimes\fi{}106{10}^{6}106 ${\mathrm{sec}}^{\ensuremath{-}1}$. For low cesium number densities (5\ifmmode\times\else\texttimes\fi{}1012{10}^{12}1012 [Cs]3\ifmmode\times\else\texttimes\fi{}1014{10}^{14}1014 ${\mathrm{cm}}^{\ensuremath{-}3}$) the light-narrowing effect is large (a factor of 2.5) and independent of [Cs]. In the region of 3\ifmmode\times\else\texttimes\fi{}1014{10}^{14}1014 to 1\ifmmode\times\else\texttimes\fi{}1015{10}^{15}1015 ${\mathrm{cm}}^{\ensuremath{-}3}$ in number densities, the light-narrowing effect decreases with increasing [Cs]. At high cesium number densities ([Cs]> 1\ifmmode\times\else\texttimes\fi{}1015{10}^{15}1015 ${\mathrm{cm}}^{\ensuremath{-}3}$) this light-narrowing effect almost completely disappears. In the limit of low-radio-frequency power the magnetic resonance linewidths for focused and unfocused dye laser beam are nearly the same. Experimental observations on this new effect are presented in detail. In the latter part of this paper a self-contained theoretical treatment of the light-narrowing effect is developed. Using Bloch equations in the presence of optical pumping, spin relaxation (diffusion, electron randomization), rapid spin exchange, and radio-frequency magnetic field, expressions for magnetic resonance line shapes are derived. In general, we find good agreement between our experimental results and the theory.
We observe very narrow (\ensuremath{\sim}200 Hz) magnetic resonance lines in alkali vapors with atomic densities much greater than usual and with cell dimensions much smaller than usual. The Zeeman resonance frequency is shifted downward by a large factor, but the spin-exchange broadening vanishes in the high-density limit. This new regime affords important new possibilities for investigating basic interactions in dense alkali vapors, and it also opens the way to miniaturized optically pumped devices.
The effect of spin-exchange collisions on the state populations obtained in an optically pumped Na23{\mathrm{Na}}^{23}Na23 vapor is studied in the limit of low light intensity. These state populations and hence the intensity of the rf Zeeman transitions are found theoretically to depend strongly on the spin-exchange cross sections. The various Zeeman rf transitions are found experimentally to be very different in intensity and this is interpreted as being partially due to spin-exchange collisions. From the intensity of the rf transitions in a magnetic field large enough to separate the six Zeeman components and from the observed relaxation time a spin-exchange cross section for two sodium atoms of $\ensuremath{\pi}{{S}_{0}}^{2}=6\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}14}$ cm2{\mathrm{cm}}^{2}cm2 is found.