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Physical Review A

Enhancement of phase-conjugate reflectivity using Zeeman coherence in highly degenerate molecular systems

Nandini Mukherjee

Published Jan 26, 2010• 2 citations
Publisher

Abstract

A comprehensive theoretical analysis is developed for the vectorial phase conjugation using resonant four-wave mixing (FWM) in a highly degenerate rotational vibrational molecular system. The dynamic Stark shifts, saturation, and Doppler broadening are included for a realistic analysis. It is shown that the electromagnetically induced multilevel coherence controls the nonlinear wave mixing yielding interesting results for the phase conjugate (PC) reflectivity. It turns out that the efficiency of the PC reflectivity is decided by the relative phase of the Zeeman coherence and the population grating. When these two contributions are aligned in phase by a small detuning of the pump frequency, a large PC reflectivity ($~$20%) is obtained with moderate pump intensity ($~$500 mW/cm${}^{2}$).

DOI
10.1103/physreva.81.013823

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Europhysics Letters (EPL)•Nov 15, 1986•30 citations
A comprehensive theoretical analysis is developed for the vectorial phase conjugation using resonant four-wave mixing (FWM) in a highly degenerate rotational vibrational molecular system. The dynamic Stark shifts, saturation, and Doppler broadening are included for a realistic analysis. It is shown that the electromagnetically induced multilevel coherence controls the nonlinear wave mixing yielding interesting results for the phase conjugate (PC) reflectivity. It turns out that the efficiency of the PC reflectivity is decided by the relative phase of the Zeeman coherence and the population grating. When these two contributions are aligned in phase by a small detuning of the pump frequency, a large PC reflectivity ( ~ 20%) is obtained with moderate pump intensity ( ~ 500 mW/cm2{}^{2}2).
The effect of Zeeman coherence on phase conjugation is investigated in the saturation regime by using a nonperturbative analysis of resonant degenerate four-wave mixing with orthogonally polarized pump beams in a A-type homogeneously broadened three-level system. The dependence of the phase-conjugation efficiency on phase-interrupting collisions and pump imbalance is particularly studied. Significant phase-conjugate reflectivities can be obtained at pump intensities much below those required for a two-level system.
Nondegenerate four-wave mixing on the j=0\ensuremath{\rightarrow}j=1 transition, in a ``V '' system, using orthogonal, circularly polarized pump beams is used to study theoretically the generation of the phase-conjugate signals. The efficiency of generation of the conjugate wave is studied as a function of the various system parameters such as pump-probe detuning, Zeeman splitting, pump-atom detuning, collisional parameters, and the intensities of the pump beams. The origin of the various resonances in the reflectivity is explained. For weak pump fields, some resonances are shown to have subnatural linewidths. In the degenerate case, the reflectivity as a function of pump-atom detuning has, in contrast to a two-level system, a doublet structure for moderate absorption-length parameters and field strengths. The reflectivity is shown to have additional resonances due to pump imbalance. The phase-conjugate signal is also shown to exhibit the pressure-induced extra resonances.
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)].
An analytic nonperturbative treatment of degenerate four-wave mixing is presented to study Zeeman-coherence effects in phase conjugation. The counterpropagating pump waves are taken to be orthogonally circularly polarized and interact with different Zeeman sublevels. The nonlinear medium is modeled in terms of a homogeneously broadened, folded three-level system. Particular attention is paid to the phase-conjugate spectrum obtained by varying the Larmor frequency associated with the Zeeman splitting. A level-crossing resonance is found to occur in the saturation regime and manifests itself as a narrow peak or dip depending on various level decay rates. Even for a purely absorptive system, the Zeeman coupling of the ground-state degenerate sublevels is shown to produce significant phase-conjugate reflectivities at pump intensities much lower than those required for a two-level system.
We demonstrate experimentally that phase-conjugation (PC) by resonant degenerate four-wave mixing in Na vapour can reach large efficiencies in the c.w. regime (reflectivity up to 250%). With PC reflectivity exceeding unity, a c.w. phase-conjugate laser oscillation is obtained, for the first time on a resonant gas medium. We show that large Na densities are required, as well as large frequency detunings of the intense incident beams. The PC oscillation is characterized through threshold effect, pump depletion, and polarization characteristics.