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Optics and Spectroscopy

Interrelationship between the polarization moments of different parity upon optical pumping of atoms under magnetic resonance conditions: II. Theory

N. A. Dovator, A. I. Okunevich

Published May 1, 2007• 7 citations
Publisher

Abstract

The mutual coupling between the polarization moments with ranks of different parity is theoretically considered. The manifestation of this mutual coupling has been revealed previously in experiments on magnetic resonance of optically oriented cesium atoms. The two well-known types of the coupling between the polarization moments are considered: the field coupling of these moments that occur due to the breaking of the hyperfine coupling between the electronic and nuclear moments of the alkali atom by the magnetic field and the light coupling of the moments due to the absorption of the pumping light by polarized atoms. The experimentally observed similarity in the shape of resonance signals of alignment and orientation upon circularly polarized pumping can be explained by the fact that, for alkali atoms, the generation of alignment by light at the wavelength of the D 1 line is of low efficiency. Therefore, alignment arises mainly from orientation by means of either the field or the light coupling of polarization moments. For metastable 23 S 1 4He atoms, no influence of the orientation on the alignment was observed because, in these atoms, the field coupling between the polarization moments is absent and the light coupling is not displayed because the generation of alignment by the circularly polarized pumping light is more efficient than the creation of alignment from orientation by means of light coupling of polarization moments.

DOI
10.1134/s0030400x07050049

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Interrelationship between the polarization moments of different parity upon optical pumping of atoms under magnetic resonance conditions: III. Comparison of theory with experiment

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W. Franzen, A. G. Emslie

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 ${D}_{1}$ line as pumping radiation, instead of a mixture of the two $D$ 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.

Physical Review•Dec 15, 1957•88 citations
The mutual coupling between the polarization moments with ranks of different parity is theoretically considered. The manifestation of this mutual coupling has been revealed previously in experiments on magnetic resonance of optically oriented cesium atoms. The two well-known types of the coupling between the polarization moments are considered: the field coupling of these moments that occur due to the breaking of the hyperfine coupling between the electronic and nuclear moments of the alkali atom by the magnetic field and the light coupling of the moments due to the absorption of the pumping light by polarized atoms. The experimentally observed similarity in the shape of resonance signals of alignment and orientation upon circularly polarized pumping can be explained by the fact that, for alkali atoms, the generation of alignment by light at the wavelength of the D 1 line is of low efficiency. Therefore, alignment arises mainly from orientation by means of either the field or the light coupling of polarization moments. For metastable 23 S 1 4He atoms, no influence of the orientation on the alignment was observed because, in these atoms, the field coupling between the polarization moments is absent and the light coupling is not displayed because the generation of alignment by the circularly polarized pumping light is more efficient than the creation of alignment from orientation by means of light coupling of polarization moments.
The optical pumping of Cs atoms with light of the D 1 line under magnetic resonance conditions is numerically calculated. This calculation is done to check the suggestion that an unexpectedly strong influence of the polarization of the pumping light on the resonance signals of transverse alignment, which we observed experimentally, is caused by the coupling between orientation and alignment by means of the magnetic field and/or the pumping light. This suggestion has been confirmed: upon circularly polarized pumping, the shape of the signal line of transverse alignment proved to be similar, as well as in the experiment, to the shape of the signal line of transverse orientation and was sharply different from the shape of the line of alignment observed upon linearly polarized pumping. For metastable 23 S 1 4He atoms, in accordance with the experimental data, the calculated shape of the signal line of transverse alignment is found to be independent of the polarization of the pumping light. The calculations also confirm the possibility of a reverse effect: the influence of alignment on orientation, which manifests itself in the occurrence of orientation upon pumping with unpolarized light under magnetic resonance conditions. For Cs atoms exposed to a field of ∼0.6 Oe, the largest contribution to this effect is yielded by the field coupling of orientation and alignment, whereas, for metastable 23 S 1 4He atoms, the largest contribution is made by the light coupling of these polarization moments.
In an experiment with an optical pumping of 133Cs atoms in the 62 S 1/2 ground state, the line shape of the D 2f magnetic resonance signal for the transverse alignment component oscillating at a double frequency f of a radio-frequency (RF) magnetic field is found to strongly depend on the polarization of pumping radiation. On passage from a linearly polarized pumping light to a circularly polarized (CP) light with a sufficiently strong RF field the ordinary three-peak line with the highest central peak transforms into a two-peak line with a minimum at the center, so that the D 2f signal line resembles the M f signal line of a transverse orientation oscillating at the RF field frequency f. This suggests that the orientation (the first-rank polarization moment (PM)) arising upon CP pumping affects the alignment (the second-rank PM); i.e., the PMs of Cs atoms with different parities of their ranks become coupled. No influence of the polarization of a pumping radiation on the line shape of the D 2f signal is observed in a similar experiment with the 4He atoms in the 23 S 1 metastable state.
It has been demonstrated that optical pumping of alkali atoms (rubidium and cesium) results to a highly efficient indirect optical orientation of metastable He (2 3 S 1 ) atoms. However, in an attempt to perform the inverse experiment (i.e. to receive spin-polarization of alkali atoms upon optical pumping of metastable helium atoms) the result was quite unexpected: the magnetic resonance signal of Cs or Rb atoms was very weak (several hundred times weaker compared to conventional optical pumping of helium in the presence of cesium (rubidium)). We propose an explanation for the unusually small ratio of the magnetic resonance signals from Cs (Rb) and metastable He atoms under condition of optical orientation of He atoms. Except of Cs atoms we are the first to have observed magnetic resonance signals from atoms of 85 Rb and 87 Rb isotopes when using the indirect optical orientation in conditions of helium-rubidium gas discharge plasma. It is shown that the anomaly in the amplitude ratios of the observed MR signals can be explained by the unidirectional action of three different factors (the presence of a large nuclear spin of alkali atoms, depolarization of alkali atoms between collisions, and spin exchange between atoms of rubidium isotopes (for the He-Rb system).
The alignment-orientation process is exactly treated for an alkali-like atom with purely electronic couplings. Analytic expressions for the circular polarization of the optical emission are given for specific types of anisotropic excitation in terms of the magnetic field and the spin-orbit parameter. No advanced formalism is used. It is shown how the hyperfine interaction with the electron orbital motion operates in a manner very similar to the purely electronic spin-orbit coupling, again leading to orbital orientation and to circularly polarized optical emission. Detailed computed results for alignment-orientation conversion for neutral helium are summarized, as are the results of experiments which directly exhibit circularly polarized emission due to the alignment-orientation effect in gases.
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.
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.