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Physical Review A

Amplitude-modulated indirect pumping of spin orientation in low-density cesium vapor

R. Gartman, Witold Chałupczak

Published May 26, 2015• 13 citations
Publisher

Abstract

A recently demonstrated technique of continuous indirect pumping enables a high level of atomic spin polarization to be generated in thermal alkali-metal vapors, without compromising the coherence lifetime through power broadening from the pump laser. The indirect pumping process combines optical excitation and spin-exchange collisions. Here we describe the pumping process and the role of spin-exchange collisions for the case of amplitude-modulated optical excitation. We demonstrate that effective spin-exchange decoherence is modified by the measurement geometry and dynamics. Decoherence changes are studied through magneto-optical-rotation signals. The studies presented here are particularly important for optimizing the performance of an atomic magnetometer operating in the quantum nondemolition configuration in a nonzero-magnetic-field environment.

DOI
10.1103/physreva.91.053419

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A recently demonstrated technique of continuous indirect pumping enables a high level of atomic spin polarization to be generated in thermal alkali-metal vapors, without compromising the coherence lifetime through power broadening from the pump laser. The indirect pumping process combines optical excitation and spin-exchange collisions. Here we describe the pumping process and the role of spin-exchange collisions for the case of amplitude-modulated optical excitation. We demonstrate that effective spin-exchange decoherence is modified by the measurement geometry and dynamics. Decoherence changes are studied through magneto-optical-rotation signals. The studies presented here are particularly important for optimizing the performance of an atomic magnetometer operating in the quantum nondemolition configuration in a nonzero-magnetic-field environment.
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.
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 $\ensuremath{\sim}101010{}^{11}$ 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.
We present a detailed experimental and theoretical study on the relaxation of spin coherence due to the spin-exchange mechanism arising in the electronic ground states of alkali-metal vapor atoms. As opposed to the well-explored formation of a stretched state in a longitudinal geometry (magnetic field parallel to the laser propagation direction) we employ adapted hyperfine-selective optical pumping in order to suppress spin-exchange relaxation. By comparing measurements of the intrinsic relaxation rate of the spin coherence in the ground state of cesium atoms with detailed density-matrix simulations we show that the relaxation due to spin-exchange collisions can be reduced substantially even in a tilted magnetic field of geomagnetic strength, the major application case of scalar magnetic surveying. This explains the observed striking improvement in sensitivity and further deepens the understanding of the light-narrowed Mx{M}_{x}Mx​ magnetometer, which was presented recently. Additionally, new avenues for investigating the dynamics in alkali-metal atoms governed by the spin-exchange interaction and interacting with arbitrary external fields open up.
Spin-exchange collisions in hot vapors are generally regarded as a decoherence mechanism. In contrast, we show that linear and nonlinear spin-exchange coupling can lead to the generation of atomic coherence in a Bell-Bloom magnetometer. In particular, we theoretically and experimentally demonstrate that nonlinear spin-exchange coupling, acting in an analogous way to a wave-mixing mechanism, can create additional modes of coherent excitation which inherit the magnetic properties of the natural Larmor coherence. The generated coherences further couple via linear spin-exchange interaction, leading to an increase of the natural coherence lifetime of the system. Notably, the measurements are performed in a low-density caesium vapor and for nonzero magnetic field, outside the standard conditions for collisional coherence transfer. The strategies discussed are important for the development of spin-exchange coupling into a resource for an improved measurement platform based on room-temperature alkali-metal vapors.
A spin-exchange optical pumping experiment to study collisions between cesium atoms and quasifree electrons is reported. In this experiment, electrons in a weak magnetic field were polarized through spin-exchange collisions with optically pumped cesium atoms. The cesium-electron collisions were the principal source of the electron-resonance linewidth, and they also gave rise to a shift in the center frequency of the electron resonance. The magnitudes of the linewidth and frequency shift depend upon the two-body scattering amplitude for elastic collisions, the cesium polarization, and the cesium density. From measurements of the electron linewidth and the frequency shift, a value is derived for the electron-cesium spin-flip cross section. The spin-flip cross section at 20\ifmmode^\circ\else\textdegree\fi{}C is found to be approximately 3.5\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}14}$ cm2{\mathrm{cm}}^{2}cm2. The expressions for the linewidth and frequency shift due to spin-exchange collisions of electrons with alkali-metal atoms are generalized to cover the case where there is a spin-orbit interaction between the electron-alkali-metal-atom systems.
We theoretically investigate the magneto-optical rotation (MOR) effect in cesium atoms in the Voigt geometry, in which an off-resonance linearly polarized laser beam serves as both pump and probe. By calculating the detailed evolution of atomic multipole moments truncated to second-rank, alignment-to-orientation conversion (AOC) effects are observed in two hyperfine ground states. The mechanisms responsible for this effect are demonstrated. The tensor AC-Stark shift produced by the optical pumping generates a nonlinear effect, resulting in atomic alignment directly coupled to orientation, which enables spin orientation to be obtained. Simultaneously, spin-exchange collisions lead to atomic alignment and orientation transfer between two ground-state manifolds. Additionally, we present the analytical expression of atomic spin polarization described by atomic multipole moments, and the contributions of the AOC effect to the optical-rotation signals are discussed in different light power regimes. Our results can be helpful for guiding MOR experiments by refining and optimizing the parameters.