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Journal of the Optical Society of America

Nondegenerate four-wave mixing in a Doppler-broadened resonant medium

Joseph Nilsen, Amnon Yariv

Published Feb 1, 1981• 47 citations
Publisher

Abstract

Third-order susceptibilities are calculated for a Doppler-broadened two-level system. The dependence of four-wave mixing on the angle θ between the pump and signal fields is studied, and the reflection coefficient is shown to have a narrow field of view that is inversely proportional to the ratio of the Doppler width to the homogeneous linewidth. For the collinear geometry, θ = 0°, the frequency dependence of the nondegenerate case is analyzed and shown capable of yielding a real-time narrow-bandwidth optical filter whose bandwidth is limited by the homogeneous linewidth.

DOI
10.1364/josa.71.000180

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Journal of the Optical Society of America B•Jun 1, 1996•27 citations
Third-order susceptibilities are calculated for a Doppler-broadened two-level system. The dependence of four-wave mixing on the angle θ between the pump and signal fields is studied, and the reflection coefficient is shown to have a narrow field of view that is inversely proportional to the ratio of the Doppler width to the homogeneous linewidth. For the collinear geometry, θ = 0°, the frequency dependence of the nondegenerate case is analyzed and shown capable of yielding a real-time narrow-bandwidth optical filter whose bandwidth is limited by the homogeneous linewidth.
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 formulation of phase conjugation via nondegenerate four-wave mixing in a homogeneously broadened resonant medium is generalized to include saturating pump waves. An ultrahigh-Qoptical filter is predicted, showing both gain and a bandwidth less than the homogeneous linewidth of the atom. The dependence of the filter function on the ac Stark effect and on the use of asymmetric pump wave intensities is discussed. In addition, several new phenomena are shown which manifest themselves as a dip in the degenerate reflectivity at line center.
An analysis is made of nondegenerate four-wave interaction (FWI) in a resonant medium (two-level model) with Doppler line broadening allowing for nonlinear absorption of the weak radiation. The cubic approximation with respect to the field is used to derive expressions for the coefficients of parametric coupling and absorption of the mixed waves. The angular dependences of the reflection coefficient are studied for quasicollinear and orthogonal FWI geometries. It is shown that, as a result of the thermal motion of the particles, the dependence of the reflection coefficient on the angle θ between the interacting waves results in considerable limitation of the angular width of the reversed beams. This limitation is greater for degenerate FWI. In the case of nondegenerate FWI, as a result of the selective action of waves on groups of atoms having a specific velocity projection, the reversal efficiency may increase on increase in θ.
In this article, we analyse a new sensitive spectroscopic technique in which a sample cell is irradiated by a two-frequency pump beam (ω + Δ ± δ/2) and a counter-propagating probe beam (ω). The phase-conjugate fields re-emitted at frequencies ω ± δ, via four-wave mixing processes, are detected through their heterodyne beating with the probe field. The properties of the heterodyne beat signal are studied by means of a perturbation calculation of the nonlinear response of the medium, carried out to the third order in the incident fields. In resonant gas media, the emission lineshape exhibits a Doppler-free doublet structure [frequency splitting 3 δ/2 for single-photon resonances, and δ/2 for two-photon transitions]. By using a phase-sensitive detection of the beat signal, one can separately analyse real (dispersion) or imaginary parts (absorption) of the nonlinear susceptibility. For single-photon transitions, the signal phase shift is related to the atomic levels lifetime and allows one to study the relaxation dynamics in gas phase (like quenching collisions, velocity diffusion, etc...). This is particularly interesting for cross-over resonances, in which only the common level contributes. In three-level systems, one also predicts a selective resonant enhancement of the phase-conjugate emission through Raman-type two-photon processes. Most of these predictions have been experimentally verified.
Nondegenerate four-wave mixing (FWM) has been used for wavelength conversion of optical information.1 In such experiments, two beams F-P (frequency ω1) intersect in a nonlinear medium with a small crossing angle θ (≈ 10 mrad), while a third beam B {frequency ω2) is nearly counterpro- pagating to F [Fig. 1(a)]. This can be viewed as real-time holography with frequency conversion.1 However, the physics differ considerably when the medium is transparent at frequency ω1, as there is no optically induced grating. This occurs when FWM is based on resonant two-photon, ω1 + ω2, absorption (frequencies ω1 and ω2 being resonant with a cascade three-level system and ω1 coupling unpopulated excited states). One interesting feature is that the two-photon coherence is nearly Doppler-free and does not depend much on the θ angle.
The effect of Doppler broadening on degenerate four-wave mixing (DFWM) signal intensities in the regime of high pump and probe laser intensities is investigated theoretically. DFWM reflectivities are calculated by solving the time-dependent density-matrix equations for a two-level system interacting with three laser fields. The density-matrix equations are integrated directly in the time domain on a grid of spatial locations along the phase-matching axis; the DFWM signal level is then calculated by summation of the polarization contribution (with the appropriate phase factor) from each of the spatial grid points. For the case in which the Doppler and the collisional linewidths are comparable, the DFWM reflectivity is found to be inversely proportional to the factor 1 + (bΔωD/ΔωC)2, where ΔωD is the Doppler width, ΔωC is the collisional width, and b is weakly dependent on the pump and the probe laser powers. We developed an analytical expression for the reflectivity of a line that is both collision and Doppler broadened by dividing the widely used Abrams and Lind expression for homogeneous reflectivity Rhom by the factor 1 + (bΔωD/ΔωC)2. This modified reflectivity expression is found to give accurate results for the DFWM reflectivity over a wide range of values for the ratio of Doppler to collisional width. With this modified Abrams–Lind expression, strategies for quantitative DFWM concentration measurements in flames and plasmas are proposed and analyzed. We conclude that, by selection of the appropriate rotational transition, a DFWM reflectivity that is directly proportional to the square of the total species number density can be obtained over a wide range of temperature for constant-laser-intensity spatial profile mapping in flames.