The optical-pumping cycle in the three-level system e,g,f (J e =1=J f , J g =0), irradiated by two monochromatic sigma -polarized laser light waves is analysed theoretically by the successive approximation (iteration) method up to fourth order. The solutions of the density-matrix evolution equations describe (i) in second order, the influence of the Zeeman structure of the e and f states on the saturation resonances in the intermediate level g (second-order population effect) and (ii) in fourth order, the influence of the Hanle effects and the saturation phenomena on the shape of the double-quantum Hanle resonances and on the two-photon transition probabilities.
The physics of the two-photon absorption process is investigated for a three-state system. The density-matrix equations for the two-photon interaction are solved in the steady-state limit assuming that the pump laser radiation is monochromatic. Collisional broadening, saturation, and Stark shifting of the two-photon resonance are investigated in detail by numerical solution of the steady-state density-matrix equations. Analytical expressions for the saturation intensity and the Stark shift are derived for the case where the single-photon transitions between the intermediate state and the initial and final states are far from resonance with the pump laser. For this case, it is found that the direction of the Stark shift is dependent on the relative magnitudes of the dipole-moment matrix elements for the single-photon transitions that couple the intermediate state with the initial and final states. Saturation and Stark shifting are also investigated for the case where the single-photon transitions between the intermediate state and the initial and final states are close to resonance with the pump laser.
The fluorescence light emitted by atoms (Ne) optically pumped with a multimode laser beam exhibits a resonance each time the Zeeman splitting is equal to the frequency difference between two modes. The experimental study shows that these resonances are very sensitive to the relative phase of modes and that their width is approximately equal to the Hanle effect width. A theoretical interpretation is given with the help of a perturbation calculation. Two phenomena produce resonances : 1) A Population Effect (PE) which is resonant when the σ + component of one mode and the σ- component of another interact with atoms of same velocity (hole crossing). The width of these resonances is 2 Γ'ab (natural width broadened by collisions). 2) A Zeeman Coherence Effect (ZCE) : the action of a pair of modes (ν, σ +) and (μ, σ-) produces (at 2nd order) transverse alignment modulated at the beat frequency ων — ω μ and resonant when the Zeeman splitting is equal to that frequency ; by interaction with a second pair of modes (λ, σ-) and (κ, σ+) (ων —ω μ + ωλ — ωκ = 0), this alignment produces unmodulated longitudinal quantities (4th order) which exhibit, as the magnetic field is scanned, a resonance whose width is close to that of the Hanle curve (Γ b(2)). In our experimental conditions (close modes : Γ'ab≳ Δω > Γ b(2)), the resonances of the first kind are not resolved and the observed resonances are only of the second type's which arevery sensitive to the phases of modes. We also discuss the possibility of using these resonances to measure Landé g factors.
The resonances of saturation which occur when the mode spacing is equal to the Zeeman splitting are theoretically studied for a mode spacing \ensuremath{\lesssim} the natural width broadened by collisions. Two kinds of resonances occur. The first set, due to a population effect (crossing of holes), is not resolved and is unobservable. The second set, due to a Zeeman coherence effect, is well resolved since the widths of the resonances are of the order of the Hanle-effect width. These resonances are very sensitive to the relative phases of the modes.
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.
Two-photon Hanle resonances were observed in a three-level atomic system interacting with two resonant light fields. The choice of suitable polarisation of the light beams and shape analysis of the resonances enabled one to distinguish the effects connected with two-photon coherent transitions from the effects due to stepwise transitions. The experiment was performed with Ne atoms simultaneously interacting with 632.8 nm and 3392 nm radiations from two He-Ne lasers. The mutual coupling of these lasers made it possible to observe the influence of the mutual correlation of both light fields on the two-photon Hanle effect.
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.