For pt.I see ibid., vol.9, p.357 (1976). A theory of the optical pumping of high-J molecule levels with a broad-band CW laser has previously been developed. The linewidth of the Hanle effect is analysed in the present paper for two particular cases in which an exact integration is possible. These cases are: (i) gT (where g is the Lande factor and T the lifetime) is the same for the two levels; and (ii) one of the Lande factors vanishes. In general, the Hanle resonance is power-broadened for high laser intensities. However, in the case of a zero Lande factor of the ground state, the theory predicts a radiative narrowing of the Hanle effect. It is shown that this most unusual feature is connected to the fact that, in the latter case, the physical observables of the resonance level may get the ground-state lifetime, when the transition is saturated.
The optical pumping of high J levels with a broad-band CW laser is studied theoretically. Exact non-perturbative solutions are obtained by means of a Fourier development of the response of the irradiated medium. This leads to such theoretical predictions as the depolarization of the fluorescence for high laser intensities, the power broadening of the Hanle effect and the appearance of a zero-field saturation resonance in the pi fluorescence. All these theoretical predictions are finally compared with recent experiments on the optical pumping of molecules especially Na 2 and I 2 .
In a previous paper, I have presented a general theory of the optical pumping of atoms by a polarized multimode-laser beam, in the presence of a magnetic field. Equations of motion, valid at arbitrary laser intensities for the density matrix of the atomic system, have been obtained. In this paper, these equations are exactly solved for a linearly $\ensuremath{\sigma}$-polarized laser and levels having small angular momenta. More precisely, I consider the laser transitions ${J}_{b}=1\ensuremath{\rightarrow}{J}_{a}=0$, ${J}_{b}=1\ensuremath{\rightarrow}{J}_{a}=1$, and ${J}_{b}=1\ensuremath{\rightarrow}{J}_{a}=2$. Two particular results are emphasized: (i) For $J=1\ensuremath{-}J=0$ and $J=1\ensuremath{-}J=1$ transitions and for the
J=2 level of a $J=1\ensuremath{-}J=2$ transition, the laser-induced Hanle effects keep a Lorentzian shape, independent of the laser intensity. For the $J=1\ensuremath{-}J=1$ transition, it is shown that the depolarizing relaxation processes play a leading part in the coupling induced by the laser between the transverse alignments of the two levels. On the other hand, the power broadenings of the Hanle effects are shown to be similar. For the
J=1 level of a $J=1\ensuremath{-}J=2$ transition, the Hanle-effect shape presents a departure from the Lorentzian one, owing to a coupling with the laser-induced hexadecapole moment in the
J=2 level. (ii) The populations of the levels exhibit a "zero-field saturation resonance" which is due to the coupling with the Zeeman coherences. These resonances, which reproduce the Hanle effects of the transition, can be observed on the $\ensuremath{\pi}$-polarized fluorescence from the levels. In general, these resonances appear as a saturation effect, i.e., they reduce the laser-induced fluorescence of the levels in zero magnetic field. However, for the ${J}_{b}=1\ensuremath{\rightarrow}{J}_{a}=2$ transition, the ${J}_{a}=2\ensuremath{\rightarrow}{J}_{f}=2 \ensuremath{\pi}$ fluorescence presents an anomalous behavior; the saturation resonance increases the zero-field laser-induced fluorescence. The theoretical study shows the prominent part played by the value of the
Jb=1 level lifetime in the interpretation of this anomaly. Other results, such as the laser-induced depolarization of the fluorescence, are also obtained. All the theoretical predictions have been experimentally checked and will be presented in forthcoming papers.
The optical Hanle effect (light-shift-induced zero-field level crossing) has been investigated theoretically and experimentally. In the case of a $J=0\ensuremath{\rightarrow}1\ensuremath{\rightarrow}0$ three-level system and of a $J=0\ensuremath{\rightarrow}1$ two-level system, the resonance line shape has been obtained using a nonlinear-response-function method. Approximate expressions, valid under the conditions for the observation of light shifts, are obtained and compared with exact calculations as well as with the corresponding expression for the magnetic Hanle effect. As concerns the weak laser beam which produces the coherent excitation of atomic substates, we have calculated the linear response in the limiting case of monochromatic and of broad-band excitation. The experimental investigation has been performed for the Ba resonance line using two cw dye lasers at $\ensuremath{\lambda}=5535$ \AA{} and an atomic beam. The absorption- and dispersion-shaped level crossing resonances have been observed, for narrow- and broad-band excitation, by varying the power of the strong nonresonant laser beam. We have checked that the line shapes are only dependent upon the reduced variable $\frac{{P}_{L}}{\ensuremath{\delta}}$ (
PL; beam power; $\ensuremath{\delta}$: frequency detuning). Using the theoretical expressions, we have tried to fit the experimental curves. Provided that the Gaussian distribution of the beams is taken into account, we have obtained a good agreement between theory and experiment for the whole set of experimental data.
The optical pumping of atoms by a multimode gas laser, in the presence of a magnetic field, is studied theoretically. The atoms are described by their density matrix, which is expanded on an irreducible tensorial set. The atomic relaxation is assumed to be isotropic. In order to avoid the usual perturbation theory, we use the so-called "Broad-Line approximation" (BLA). BLA is valid when the width of the "Bennett hole" created by one laser mode in the velocity distribution of the excited atoms is comparable to the spacing between modes; under these conditions, the atomic response does not depend on the velocity and the multimode laser irradiation is equivalent to a broad-line excitation. For the atomic system, BLA leads to a set of coupled equations which is valid at arbitrary intensities of the laser field and which depends on this field through a unique parameter, $\ensuremath{\gamma}$. This parameter can be understood as a laser-induced transition probability. In this article, we analyze the nonlinear effects which can be deduced from this theory, for any value of the angular momenta involved in the laser transition: Hanle-effect broadening, alignment coupling, saturation resonances on the populations are shown. The exact calculations, valid at arbitrary laser intensities for $J=1\ensuremath{\leftrightarrow}J=0$, $J=1\ensuremath{\leftrightarrow}J=1$, and $J=1\ensuremath{\leftrightarrow}J=2$ transitions, and the corresponding experimental results will be presented in forthcoming papers.
A quantum-statistical theory of optical Hanle effect is developed for arbitrary intensities and bandwidths of the pump field. The excited- and ground-state level shifts, caused by another light field with appropriate polarization, are directly included in the theory by using the method of time averaging. The laser fluctuations are taken into account exactly by using the phase-diffusion model of the pump laser. The analytical and numerical results for the fluorescence signals are presented for a variety of excitations. Our results in the limiting case reduce to those of Kaftandjian, Klein, and Hanle. Finally, the case of a very broadband excitation under saturation conditions is analyzed and the results for signals in various directions and the polarizations are obtained.