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Journal of the Optical Society of America B

Effects of population pulsations on backward, nearly degenerate four-wave mixing spectroscopy and optical phase conjugation

Duncan G. Steel, Stephen Colby Rand, J. T. Remillard, Jing Liu

Published Jan 1, 1988• 1 citation
Publisher

Abstract

We discuss the effects of population pulsations on the spectral response of backward nearly degenerate four-wave mixing (NDFWM). We include the effects of state-specific decay and spontaneous emission on both two-level and inverted-v-type three-level systems. We compare the results with experiments in both the gas phase and the condensed phase that show ultranarrow resonances. In addition, we examine the response in the presence of strong pump fields. We show that in a simple two-level system, the NDFWM response results in an ac-Stark splitting of the spectral response, whereas in a simple three-level system with decay to a metastable state, a single narrow resonance is observed, which broadens in the presence of strong pumps.

DOI
10.1364/josab.5.000171

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Journal of the Optical Society of America•May 1, 1983•67 citations
We discuss the effects of population pulsations on the spectral response of backward nearly degenerate four-wave mixing (NDFWM). We include the effects of state-specific decay and spontaneous emission on both two-level and inverted-v-type three-level systems. We compare the results with experiments in both the gas phase and the condensed phase that show ultranarrow resonances. In addition, we examine the response in the presence of strong pump fields. We show that in a simple two-level system, the NDFWM response results in an ac-Stark splitting of the spectral response, whereas in a simple three-level system with decay to a metastable state, a single narrow resonance is observed, which broadens in the presence of strong pumps.
The purpose of this research is to study the dynamic behavior of a resonant system using four-wave-mixing spectroscopy (FWM). From this study, we have obtained rich information about the FWM spectral response of systems which have different state-specific reservoir couplings. Atomic sodium (Na) is used as our model system. It is shown that the FWM spectral response depends strongly on how each level couples to the vacuum radiation field (through spontaneous emission). This effect is illustrated in the line shape obtained from a nearly degenerate FWM (NDFWM) experiment for a simple two-level system in Na. A narrow spike on top of a wide resonance is observed at zero pump-probe detuning (δ\deltaδ = 0) when the upper-state decay rate $\gamma\sb2$ to the reservoir is larger than the lower-state decay rate $\gamma\sb1$. The width of the spike is 2$\gamma\sb1$ and the width of the wide resonance is determined by the total upper-level decay rate (2$\gamma\sbsp{2}{\rm t}$). From the NDFWM spectrum, all the decay rates characterizing a two-level system may be measured directly. If magnetic substate degeneracy is included, the NDFWM line shape has contributions arising from orientation and alignment gratings, as well as from population gratings. For a two-level system closed with respect to population, the orientation or alignment gratings may contribute a narrow resonance at δ\deltaδ = 0 in the NDFWM response. These features are demonstrated for the first time by using NDFWM. Reservoir coupling can also occur through collisions with externally added gas. Collisions can cause a closed two-level system to become open, resulting in NDFWM spectra that show a narrow resonance at δ\deltaδ = 0 with a width below the residual Doppler width (Dicke narrowing). This is also the first time that Dicke narrowing has been observed in population terms. Finally, we present a calculation of the NDFWM response for strong degenerate pump fields and a weak probe field. We compare the differences between NDFWM spectra of closed two- and three-level systems in the presence of strong pumps.
The theory of nondegenerate four-wave mixing (NDFWM) in semiconductor lasers and amplifiers is presented with particular emphasis on the physical processes that lead to population pulsations. In the case of nearly degenerate four-wave mixing, modulation of the carrier density at the beat frequency Ω of the pump and probe waves creates a dynamic population grating whose effectiveness is governed by the spontaneous carrier lifetime τs. Such a grating affects both the gain and the refractive index of the probe wave. In particular, the probe gain exhibits features analogous to those observed in a detuned atomic system arising from the optical Stark effect. Both the gain grating and the index grating contribute to NDFWM, with the dominant contribution coming from the index grating. For detunings such that Ωτs ≫ 1, population pulsations correspond to modulation of the intraband population arising from spectral hole burning. Our results show that NDFWM is then limited by the phase-mismatch effects governed by the transit time τ rather than by the intraband population-relaxation time T1. Significant NDFWM is expected to occur for detunings up to about 300 GHz for typical transit-time values of 3 psec in semiconductor lasers.
The use of resonantly enhanced four-wave mixing to generate high reflectivity phase-conjugate waves is discussed. A physical understanding of the mechanisms underlying the nonlinear response for a simple two-level system is presented followed by a discussion of the complicating effects of pump absorption, pump depletion, unbalanced pumps, and thermal motion. Modifications of the theory to describe four-level behavior are presented and compared with experiments. The application of nearly degenerate four-wave mixing to narrow-band filtering complicated by the A. C. Stark effect is dis-cussed along with examples of experimental observations.
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 a theoretical description of the interaction of optical waves due to the resonant nonlinear response of an atomic system. We emphasize how the resonant nature of the nonlinear coupling is modified by the shifting of the atomic energy levels as a consequence of the dynamic Stark effect and show the equivalent role played by population pulsations in determining the nature of the nonlinear coupling. A general formalism is developed to treat these effects and is explicitly applied to several examples of current interest, including single-beam saturation spectroscopy, pump–probe saturation spectroscopy, modulation spectroscopy, degenerate four-wave mixing for phase conjugation, and instabilities in the beam propagation through resonant media.
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)].