An ``amplitude model'' of the laser-rf double-resonance process has been quantitatively verified, providing a complete explanation of the anomalous line shapes observed in studies of
Na2 hyperfine structure. We find excellent agreement with new laser-rf double-resonance measurements in low-J'' rotational levels of the
X1${\ensuremath{\Sigma}}_{g}^{+}$(v''=0) ground state of
Na2 as well as with earlier data for J''=28. These results confirm the idea that absorption and stimulated-emission Rabi cycles in the presence of the laser field create coherence between the ground-state hyperfine levels when these levels are optically unresolved. A novel ground-state ``quantum beat'' experiment is proposed.
Level-crossing effects have been detected non-optically with the use of a Rabi-type atomic-beam method. The sodium beam was excited by intense linearly polarised radiation from a CW narrow-band dye laser. Several superimposed resonances were observed in the atomic-beam signal when scanning the magnetic field around zero. The two narrower resonances are interpreted as high-order non-linear effects. They arise from the coupling of laser-induced Zeeman coherences in the ground state (including a hexa-decapole moment) with the populations of the Zeeman sublevels.
Subnatural-width resonances due to coherent effects in optical pumping at hyperfine (hf) transitions of Rb are investigated using a linearly or circularly polarized single-frequency diode laser beam. The sign and amplitude of the resonances in the fluorescence are measured by scanning the laser frequency over the hf transitions of the Rb D 1 and D 2 lines. The fluorescence perpendicular to the laser beam is detected as a function of magnetic field parallel to the beam propagation and scanned around zero value. In the case of linear polarization of the field, dark resonances are observed for hf transitions with F g → F e = F g -1 and F g → F e = F g , and bright resonances are observed for transitions with F g → F e = F g + 1. This is in agreement with the recently developed theories. For all (except F g = 2→ F e = 3, 85 Rb, D 1 line) hf transitions the sign of the resonances reverses when the polarization of the field changes to circular. The amplitudes of the resonances correspond to the probability of the hf transitions and to the calculated loss rate of the population to the ground hf level not excited by the laser field. The observed narrow resonances (FWHM: few tens of kHz) and their sensitivity to weak magnetic fields are interesting for high-resolution spectroscopy and for development of simple and precise magnetometers.
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.
With use of a narrow-band laser, the free
NO2 molecule is prepared in a well-defined excited state under conditions that correspond to an optical-frequency--radiofrequency double-resonance experiment. We observe a resonant increase or decrease (dependent on the divergence of the light beam) of the total fluorescence intensity when the radiofrequency field is in resonance with the Zeeman splitting in the ground or excited state of the laser-induced transition. These resonances differ significantly from well-known optical-rf double-resonance signals and laser saturation effects. The resonances are, however, well described with use of a model which assumes an irreversible evolution in the free
NO2 molecule.
We present the results of an experimental as well as a theoretical study of nonlinear magneto-optical resonances in diatomic potassium molecules in the electronic ground state with large values of the angular momentum quantum number $J\ensuremath{\sim}100$. At zero magnetic field, the absorption transitions are suppressed because of population trapping in the ground state due to Zeeman coherences between magnetic sublevels of this state along with depopulation pumping. The destruction of such coherences in an external magnetic field was used to study the resonances in this work. K
2 molecules were formed in a glass cell filled with potassium metal at a temperature above 150 ${}^{\ensuremath{\circ}}$C. The cell was placed in an oven and was located in a homogeneous magnetic field B, which was scanned from 0 to 0.7 T.
Q-type and
R-type transitions were excited with a tunable, single-mode diode laser with a central wavelength of 660 nm. Well-pronounced nonlinear Hanle effect signals were observed in the intensities of the linearly polarized components of the laser-induced fluorescence (LIF) detected in the direction parallel to the B field with polarization vectors parallel (
Ipar) and perpendicular (
Iper) to the polarization vector of the exciting laser radiation, which was orthogonal to B. The intensities of the LIF components were detected for different experimental parameters, such as laser power density and vapor temperature, in order to compare them with numerical simulations that were based on the optical Bloch equations for the density matrix. We report good agreement of our measurements with numerical simulations. Narrow, subnatural linewidth dark resonances in
Iper(B) were detected and explained.