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Physical Review A

Theory of resonant Doppler-broadened backward four-wave mixing in the pump saturation regime

M. Ducloy, F. A. M. de Oliveira, Daniel Bloch

Published Sep 1, 1985• 47 citations
Publisher

Abstract

We analyze the properties of phase-conjugate (PC) emission via resonant, Doppler-broadened, backward four-wave mixing in the saturation regime, when both counterpropagating pump waves are arbitrarily intense. One considers two atomic situations, either a four-level system modeled as a pair of uncoupled transitions, or a three-level system. The first case leads to an analytical expression of the PC field, for arbitrary pump intensities, in the Doppler limit. The second case, in general, necessitates a numerical solution, except in the asymptotic regime when one pump is very intense compared to the other one. One finds that both cases lead to quite similar predictions: (i) two-peaked or four-peaked emission line shape, depending on the forward to backward pump intensity ratio; (ii) the maximum of PC reflectivity is obtained for infinite backward saturation, but for a fi-p nite value of the forward pump intensity; (iii) for backward saturation, the emission line shape is practically independent of the forward pump intensity. Finally, the theoretical analysis is extended to the case of a saturating probe and its effect on emission line shape and PC reflectivity, as well as its application to the properties of emission processes involving higher-order optical susceptibilities (degenerate multiwave mixing).

DOI
10.1103/physreva.32.1614

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We present a theoretical study of phase-conjugate (PC) emission by backward degenerate four-wave mixing (DFWM) processes in a resonant gas medium. In this study, high-intensity (pump) saturation and Doppler broadening are simultaneously taken into account. We develop a general formalism to deal with the saturation effects in the case of a three-level atom (with degenerate frequencies) and obtain analytical expressions of the PC field amplitude (after integration over the velocity distribution) under the following conditions: (1) the probe beam and one of the pump beams have intensities weak enough to be treated at the lowest perturbation order, whereas the other pump intensity is arbitrarily high; (2) the probe crosses the standing pump wave at grazing incidence. It is shown that the saturation induced by the forward pump (copropagating with the probe beam) leads to entirely different behavior of the nonlinear susceptibility from that induced by the backward pump (counterpropagating with the probe beam). This saturation anisotropy is specific to the inhomogeneous broadening of the gas medium, which is also responsible for the frequency splitting experimentally observed in the intensity line shape of the PC emission for large pump intensities. At saturation, this splitting is theoretically shown to be proportional to the Rabi frequency, with a proportionality coefficient critically dependent on the relaxation processes; in the case of a single-relaxation model, the splitting is equal to 1.5 times the Rabi frequency. The PC intensity line shape is demonstrated to be of dispersive origin in the case of backward saturation, whereas for forward saturation, narrow structures are predicted in both real and imaginary parts of the nonlinear susceptibility, also leading to the intensity line-shape splitting. One also finds that the reflectivity of PC mirrors based on resonant DFWM strongly depends on the origin of the saturation. For a saturating forward pump, the PC emission intensity tends toward zero with increasing pump intensities, and it reaches a finite (nonzero) limit in the case of backward saturation. Most of these predictions have been observed experimentally [ BlochD., Phys. Rev. Lett.49, 719 ( 1982)].

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Physical Review A•Dec 1, 1984•77 citations
We analyze the properties of phase-conjugate (PC) emission via resonant, Doppler-broadened, backward four-wave mixing in the saturation regime, when both counterpropagating pump waves are arbitrarily intense. One considers two atomic situations, either a four-level system modeled as a pair of uncoupled transitions, or a three-level system. The first case leads to an analytical expression of the PC field, for arbitrary pump intensities, in the Doppler limit. The second case, in general, necessitates a numerical solution, except in the asymptotic regime when one pump is very intense compared to the other one. One finds that both cases lead to quite similar predictions: (i) two-peaked or four-peaked emission line shape, depending on the forward to backward pump intensity ratio; (ii) the maximum of PC reflectivity is obtained for infinite backward saturation, but for a fi-p nite value of the forward pump intensity; (iii) for backward saturation, the emission line shape is practically independent of the forward pump intensity. Finally, the theoretical analysis is extended to the case of a saturating probe and its effect on emission line shape and PC reflectivity, as well as its application to the properties of emission processes involving higher-order optical susceptibilities (degenerate multiwave mixing).
We present a theoretical study of phase-conjugate (PC) emission by backward degenerate four-wave mixing (DFWM) processes in a resonant gas medium. In this study, high-intensity (pump) saturation and Doppler broadening are simultaneously taken into account. We develop a general formalism to deal with the saturation effects in the case of a three-level atom (with degenerate frequencies) and obtain analytical expressions of the PC field amplitude (after integration over the velocity distribution) under the following conditions: (1) the probe beam and one of the pump beams have intensities weak enough to be treated at the lowest perturbation order, whereas the other pump intensity is arbitrarily high; (2) the probe crosses the standing pump wave at grazing incidence. It is shown that the saturation induced by the forward pump (copropagating with the probe beam) leads to entirely different behavior of the nonlinear susceptibility from that induced by the backward pump (counterpropagating with the probe beam). This saturation anisotropy is specific to the inhomogeneous broadening of the gas medium, which is also responsible for the frequency splitting experimentally observed in the intensity line shape of the PC emission for large pump intensities. At saturation, this splitting is theoretically shown to be proportional to the Rabi frequency, with a proportionality coefficient critically dependent on the relaxation processes; in the case of a single-relaxation model, the splitting is equal to 1.5 times the Rabi frequency. The PC intensity line shape is demonstrated to be of dispersive origin in the case of backward saturation, whereas for forward saturation, narrow structures are predicted in both real and imaginary parts of the nonlinear susceptibility, also leading to the intensity line-shape splitting. One also finds that the reflectivity of PC mirrors based on resonant DFWM strongly depends on the origin of the saturation. For a saturating forward pump, the PC emission intensity tends toward zero with increasing pump intensities, and it reaches a finite (nonzero) limit in the case of backward saturation. Most of these predictions have been observed experimentally [ BlochD., Phys. Rev. Lett.49, 719 ( 1982)].
Nonlinear effects of sublevel coherence on resonant backward-degenerate four-wave mixing are analyzed in the saturation regime of an inhomogeneously broadened and optically thin gas medium, composed of \ensuremath{\Lambda}-type three-level atoms. No limitations are set to the pump-field intensities, and an analytical approach is presented in the Doppler limit and efficient transverse-optical-pumping regime. It is shown that coherent population trapping due to strong pump-field coupling has a negligible incidence in phase conjugation, while interference of two imbalanced coherent-population-injection channels determines the mixing process. Level-crossing emission resonances are found to exhibit particular line-shape characteristics: (1) an insensitivity to power shifts, (2) strong power-broadening accompanied by incomplete line splitting, or (3) field-induced line-broadening inhibition. The conditions under which these effects should be observable are identified, and their dependence on pump imbalance is remarked.
We present in this paper a theoretical study of the angular dependence of phase-conjugate emission via resonant degenerate four-wave mixing (FWM) in Doppler-broadened gas media. The nonlinear optical polarization is calculated through an expansion of the atomic density matrix up to the third order in the incident fields. One finds that, when the incident frequency is resonant for a single-photon transition, both strength and lineshape of the phase-conjugate emission strongly depend on the angle 0 between standing pump wave and probe wave. The emission intensity, maximum at grazing incidences, decreases rapidly by several orders of magnitude when 0 increases. Simultaneously the emission linewidth increases from homogeneous to Doppler width. Similar effects are predicted for nearly-degenerate FWM (different pump and probe frequencies). In particular, one shows that the bandwidth of the equivalent optical reflection filter undergoes a Doppler-broadening linearly increasing with sin θ. On the opposite, none of the above effects is predicted in two-photon-resonant FWM which does not exhibit any angular dependence.
The effect of an intense pump beam on the intensity of the phase-conjugated emission is studied in the case of a three-level atom. We first extend to the case of cross-polarized pump beams the dressed-atom model that we have presented previously [Phys. Rev. A 34, 4008 (1986)] for the case of two-level atoms. The range of validity of our theory is \ensuremath{\Gamma} (natural width) ${\ensuremath{\Omega}}_{1}$ (Rabi frequency of the intense pump) ku (Doppler width). We have studied the line shape in degenerate four-wave mixing, the influence of a static magnetic field, and the resonances that appear in nondegenerate four-wave mixing. Experiments are done in a neon discharge using cw dye lasers. The experimental results are in good agreement with the theoretical predictions. In degenerate four-wave mixing, we have shown that the saturating dip disappears when the weak beams have orthogonal polarizations. In the presence of a static magnetic field and in the nearly degenerate case, narrow resonances corresponding to transitions between energy levels of the dressed atom are observed. The intensity and the width of these resonances are in very good agreement with the predictions of the theoretical model.
In this paper, we present a detailed analysis of saturation effects in resonant degenerate four-wave mixing (phase conjugation) or multiwave mixing (high-order diffraction on an optically induced grating). The experiments are performed in a low-pressure Ne discharge in the Doppler-broadened regime, both on an "ideal" two- or three-level system (1s_{4}(J = 1) - 2p_{3}(J = 0)) or on a degenerate multi-level system (1s_{5}(J = 2) - 2p_{9}(J = 3)). The saturation effects appearing when both pump beams are intense are studied, and a very good agreement is found with the previously developed theory [8]. It is demonstrated that there is an absolute maximum to the phase-conjugate reflectivity, and various effects on the lineshape (splitting, linewidth, etc.) are investigated. The effects produced by the Gaussian nature of the incident beams are analyzed in order to interpret some of the discrepancies between theory and experiment. Several new theoretical results for high-order diffraction are also presented, and compared with the experiments. The possibility of dealing with the saturation effects in four-wave mixing when all three incident fields are saturating appears as a consequence of these studies on multiwave mixing. Notably discussed are the case of an intense diffracting field, and of intense grating fields, whose intensity may be unbalanced. Finally, the polarization selection rules for high-order diffraction experiments are established.
We present the theory of resonant backward degenerate four-wave mixing in gaseous media for Doppler-broadened degenerate two-level systems. The degeneracy of the atomic levels as well as the influence of the polarization of the incident fields are taken into account within the framework of a tensorial formalism. The amplitude, line shape, and polarization of the reemitted phase-conjugate field are calculated up to the third order in the incident fields. The velocity average is performed in the approximation of large Doppler linewidths. One considers in detail the influence of depolarizing relaxation processes and the effects of pump-probe angular separation. In particular, the importance of the residual Doppler effect (shortening of the lifetime of the optically induced gratings by the atomic motion) associated with the pump-probe angle is emphasized. We show that the polarization of the reemitted fields is governed by very simple laws as soon as the residual Doppler effect overcomes the lifetimes of the atomic levels. Phase-conjugate mirrors can be simply characterized by a linear dichroism (parallel pump polarizations) or a birefringence (cross-polarized pumps). Vectorial phase conjugation is also analyzed, in the case of counter-rotating circular polarizations of the pumps. Finally, the case of two-photon transition is studied and compared with the case of a resonant transition.