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.
A novel coherent Raman effect induced by a laser and a radio-frequency (rf) field is used to detect cw and pulsed nuclear magnetic resonance (NMR) in ground and excited electronic states. The effect is illustrated in the impurity-ion solid
Pr3+: La
F3 at 1.6 K utilizing the
Pr3+ optical transition $^{3}H_{4}({\ensuremath{\Gamma}}_{1})\ensuremath{\rightarrow}^{1}D_{2}({\ensuremath{\Gamma}}_{1})$. The laser field of frequency ${\ensuremath{\omega}}_{E}$ and the rf field (${\ensuremath{\omega}}_{H}$) induce a light wave at the sum ${\ensuremath{\omega}}_{E}+{\ensuremath{\omega}}_{H}$ (anti-Stokes) and difference ${\ensuremath{\omega}}_{E}\ensuremath{-}{\ensuremath{\omega}}_{H}$ (Stokes) frequencies, generating an absorptive or dispersive heterodyne beat signal (${\ensuremath{\omega}}_{H}$) with the laser field at a photodetector. The theory of this effect is characterized in a new three-level perturbation calculation which requires, unlike the usual stimulated Raman effect, that all three transitions be electric- or magnetic-dipole allowed. Detailed predictions are confirmed by cw measurements of the
Pr3+: La
F3 hyperfine splittings where the optical heterodyne signals are shot-noise limited. The
Pr3+ nuclear quadrupole parameters are obtained for the
3H4 and
1D2 states where the line centers are determined with kilohertz precision. The corresponding wave functions show significant hyperfine-state mixing, as required for all three transitions to be dipole allowed. The cw line shapes are narrow (30-160 kHz), inhomogeneously broadened by nuclear magnetic interactions, and reveal either a Gaussian or an anomalous second-derivative---like line shape. The spin-echo measurements for the
3H4 and
1D2 hyperfine transitions yield homogeneous line shapes which are Lorentzian, and rather surprisingly, linewidths in the narrow range 10-20 kHz, a result which tests current line-broadening theories.