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Journal of the Optical Society of America

Optical Methods of Atomic Orientation and of Magnetic Resonance*

Alfred Kastler

Published Jun 1, 1957• 223 citations
Publisher

Abstract

In the optical excitation of atoms with polarized light, producing excited atoms, only some of the Zeeman sublevels of the excited state are actually reached, so that large differences of population can be built up between Zeeman sublevels or between hyperfine structure (hfs) levels. This property can be used to detect radio-frequency resonance in optically excited atomic states. These resonances produce a characteristic change in intensity or in the degree of polarization of the light re-emitted. Zeeman intervals, Stark effects, and hfs intervals can be measured in this manner. (The Stark constant of the 63P1 level of Hg and the electric quadrupole moments of the alkali atoms have been obtained in this way.)The technique of “optical pumping” gives a way to concentrate atoms in some of the Zeeman sublevels of one of the hfs levels of the ground state.Atomic orientation has been obtained with the Na atom, in an atomic beam and in the vapor in equilibrium with the metal. The orientation effects have been studied by detection of radio-frequency resonance signals in the ground state. Orientation can be increased many times by adding a variable pressure of a foreign gas to the pure Na vapor. Because of the coupling between nuclear spin and electron spin, nuclear orientation is produced at the same time as atomic orientation.

DOI
10.1364/josa.47.000460

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In the optical excitation of atoms with polarized light, producing excited atoms, only some of the Zeeman sublevels of the excited state are actually reached, so that large differences of population can be built up between Zeeman sublevels or between hyperfine structure (hfs) levels. This property can be used to detect radio-frequency resonance in optically excited atomic states. These resonances produce a characteristic change in intensity or in the degree of polarization of the light re-emitted. Zeeman intervals, Stark effects, and hfs intervals can be measured in this manner. (The Stark constant of the 63P1 level of Hg and the electric quadrupole moments of the alkali atoms have been obtained in this way.)The technique of “optical pumping” gives a way to concentrate atoms in some of the Zeeman sublevels of one of the hfs levels of the ground state.Atomic orientation has been obtained with the Na atom, in an atomic beam and in the vapor in equilibrium with the metal. The orientation effects have been studied by detection of radio-frequency resonance signals in the ground state. Orientation can be increased many times by adding a variable pressure of a foreign gas to the pure Na vapor. Because of the coupling between nuclear spin and electron spin, nuclear orientation is produced at the same time as atomic orientation.
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.
Optical orientation of Na atoms in a metal vapor with circularly polarized D1{D}_{1}D1​ resonance radiation results in a shift in the $2\mathrm{Na}\ensuremath{\leftrightarrow}\mathrm{Na}{}_{2}$ gas phase equilibrium in the direction that destroys dimers. Plane polarized D1{D}_{1}D1​ or D2{D}_{2}D2​ resonance radiation produces the opposite effect: an increase in equilibrium dimer density. The atom-dimer reaction can be controlled to favor either products or reactants by simply changing the polarization of the resonance light. Application of a radio-frequency field at the Na atomic Zeeman resonance frequency while optically pumping the atoms with circularly polarized D1{D}_{1}D1​ radiation also permits a magnetic resonance tuning control of either an increase or decrease in dimer density.
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.
Excitation of atoms in a vapor by polarized light produces unequal population of the magnetic sublevels of the excited state. The emitted optical resonance radiation is therefore partly polarized. The application of radiofrequency or microwave fields at a magnetic resonance frequency will induce transitions between sublevels of the excited state. The degree of polarization of the emitted optical resonance radiation is altered when the magnetic resonance condition is fulfilled. As suggested by Brossel and Kastler, this effect may be used to reveal the structure of the energy level. A detailed theory applicable to, and experiments on the 3P1^{3}P_{1}3P1​ state of all the isotopes of mercury are reported. The results obtained indicate that double resonance phenomena constitute a valuable new tool for investigating the structure of atomic energy levels. The mean life of the 3P1^{3}P_{1}3P1​ state is shown by observations on the resonance line widths to be 1.55\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}7}$ sec for all the isotopes. The ggg-factor of the 3P1^{3}P_{1}3P1​ state for isotopes with zero spin, measured in terms of the proton ggg-factor, is 1.4838\ifmmode\pm\else\textpm\fi{}0.0004.
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.
By D1{\mathit{D}}_{1}D1​-line optical pumping of alkali-metal atoms (Cs and Rb) in superfluid helium (He II), we could achieve large spin polarization of the atoms in the ground states, more than 50% for both electron and nuclear spins, especially for the Cs atoms. The alkali-metal atoms were implanted into He II by laser sputtering. We detected optically the magnetic resonances between the ground-state Zeeman sublevels, and found that the g values and hyperfine constants in He II were the same as in vacuum within the experimental error. We discuss possible applications of these spin-polarized atoms in He II.