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Optics Letters

Saturation splitting of line shapes in noncollinear four-wave mixing in SF_6

O. Di Lorenzo-Filho, Paulo C. de Oliveira, J. R. Rios Leite

Published May 1, 1991• 4 citations
Publisher

Abstract

Phase-conjugate emission by resonant degenerate four-wave mixing with two counterpropagating weak pump beams and a noncollinear strong object beam was calculated for a Doppler-broadened two-level system. Singlepeak Doppler-free lines with small saturation broadening at a collinear configuration became split for a wide angle. The effect is demonstrated with the use of a CO(2) laser and SF(6). Conversely, calculated line shapes with Stark splitting in a collinear arrangement became single peaked for a wide angle.

DOI
10.1364/ol.16.000657

Related papers

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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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Claudio Lenz Cesar, J. W. R. Tabosa, Paulo C. de Oliveira +2 more

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Theory of degenerate four-wave mixing in resonant Doppler-broadened systems - I. Angular dependence of intensity and lineshape of phase-conjugate emission

M. Ducloy, Daniel Bloch

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.

Journal de physique•Jan 1, 1981•74 citations
Phase-conjugate emission by resonant degenerate four-wave mixing with two counterpropagating weak pump beams and a noncollinear strong object beam was calculated for a Doppler-broadened two-level system. Singlepeak Doppler-free lines with small saturation broadening at a collinear configuration became split for a wide angle. The effect is demonstrated with the use of a CO(2) laser and SF(6). Conversely, calculated line shapes with Stark splitting in a collinear arrangement became single peaked for a wide angle.
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)].
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 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.