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Applied Physics Letters

Saturation splitting of phase-conjugate line through resonant degenerate four-wave mixing in SF6

Jean-Luc Boulnois, Philippe Aubourg, A. Van Lerberghe, Govind Prasad Agrawal

Published Feb 1, 1983• 4 citations
Publisher

Abstract

Using the isolated P(33)A 12 one-photon resonance in SF6 the degenerate four-wave mixing spectrum is shown to exhibit line splitting below a critical pressure. The dependence of this saturation splitting on the gas pressure and the pump intensity is quantitatively studied.
DOI
10.1063/1.93900

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Optics Letters•Dec 1, 1988•13 citations
CW phase conjugation on the ν3 vibrational bands of SF6 and OsO4 is demonstrated as a means of investigation in high resolution spectroscopy through resonant degenerate four-wave mixing at 10.6 µm by using a stable low power CO2 laser operating on the P(18), P(16), P(12) lines respectively. Peak reflectivities of 3.8 10-3 are measured in SF6. They only reach 0.34 10-3 in OsO4. Phase conjugate spectra with 2 MHz, namely sub-Doppler resolutions, are compared with simultaneous recordings of the saturated-absorption spectra over a 80 MHz bandwidth. The saturation splitting encountered on a one-photon transition in SF6 is also analysed in terms of pressure broadening and pump imbalance.
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)].
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.
Degenerate-four-wave mixing (DFWM) is an important technique for the generation of phase-conjugate wave, to which much attention has been paid. In this paper. a tunalile CW CO2 1.aser is used as the pump sourse and gaseous SF6 as the nonlinear medium, the dependence of reflectivity of phase-conjugate wave generated by DFWM on the pump intensity, the pressure in SF6, the angle between the pump and probe beams as welt as the potarization of the optical fields etc, is investigated experimentatty and exptained theoretically. Peak reftectivity of 2.1x101 is abtained at P=4 Torr in the gaseous SF6. In the Doppler-free phase-conjugate spectrum of SF6 five absorption dips are observed and the spectral resolving power is measured to be about 3 MHz.