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IEEE Journal of Quantum Electronics

Nearly degenerate four-wave mixing enhanced by the ac Stark effect

Donald J. Harter, Robert W. Boyd

Published Oct 1, 1980• 85 citations
Publisher

Abstract

A model is developed to describe nondegenerate four-wave mixing in a medium characterized by a single strong atomic resonance. The nonlinear response is calculated using the density-matrix formalism, and propagation effects are included by solving coupled-wave equations. This model predicts large resonant responses for signals detuned from the pump frequency by approximately the generalized Rabi frequency. Potential applications of the effects predicted by this model include construction of tunable bandpass filters and four-wave parametric oscillators.

DOI
10.1109/jqe.1980.1070374

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Physical Review A•Jan 1, 1988•7 citations
A model is developed to describe nondegenerate four-wave mixing in a medium characterized by a single strong atomic resonance. The nonlinear response is calculated using the density-matrix formalism, and propagation effects are included by solving coupled-wave equations. This model predicts large resonant responses for signals detuned from the pump frequency by approximately the generalized Rabi frequency. Potential applications of the effects predicted by this model include construction of tunable bandpass filters and four-wave parametric oscillators.
This thesis describes the theoretical solution and experimental verification of phase conjugation via nondegenerate four-wave mixing in resonant media. The theoretical work models the resonant medium as a two-level atomic system with the lower state of the system being the ground state of the atom. Working initially with an ensemble of stationary atoms, the density matrix equations are solved by third-order perturbation theory in the presence of the four applied electro-magnetic fields which are assumed to be nearly resonant with the atomic transition. Two of the applied fields are assumed to be non-depleted counterpropagating pump waves while the third wave is an incident signal wave. The fourth wave is the phase conjugate wave which is generated by the interaction of the three previous waves with the nonlinear medium. The solution of the density matrix equations gives the local polarization of the atom. The polarization is used in Maxwell's equations as a source term to solve for the propagation and generation of the signal wave and phase conjugate wave through the nonlinear medium. Studying the dependence of the phase conjugate signal on the various parameters such as frequency, we show how an ultrahigh-Q isotropically sensitive optical filter can be constructed using the phase conjugation process. In many cases the pump waves may saturate the resonant medium so we also present another solution to the density matrix equations which is correct to all orders in the amplitude of the pump waves since the third-order solution is correct only to first-order in each of the field amplitudes. In the saturated regime, we predict several new phenomena associated with degenerate four-wave mixing and also describe the ac Stark effect and how it modifies the frequency response of the filtering process. We also show how a narrow bandwidth optical filter with an efficiency greater than unity can be constructed. In many atomic systems the atoms are moving at significant velocities such that the Doppler linewidth of the system is larger than the homogeneous linewidth. The latter linewidth dominates the response of the ensemble of stationary atoms. To better understand this case the density matrix equations are solved to third-order by perturbation theory for an atom of velocity v. The solution for the polarization is then integrated over the velocity distribution of the macroscopic system which is assumed to be a gaussian distribution of velocities since that is an excellent model of many real systems. Using the Doppler broadened system, we explain how a tunable optical filter can be constructed whose bandwidth is limited by the homogeneous linewidth of the atom while the tuning range of the filter extends over the entire Doppler profile. Since it is a resonant system, sodium vapor is used as the nonlinear medium in our experiments. The relevant properties of sodium are discussed in great detail. In particular, the wavefunctions of the 3S and 3P states are analyzed and a discussion of how the 3S-3P transition models a two-level system is given. Using sodium as the nonlinear medium we demonstrate an ultrahigh-Q optical filter using phase conjugation via nondegenerate four-wave mixing as the filtering process. The filter has a FWHM bandwidth of 41 MHz and a maximum efficiency of 4 x 10-3. However, our theoretical work and other experimental work with sodium suggest that an efficient filter with both gain and a narrower bandwidth should be quite feasible.
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.
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.
We present a revision of the theory of finite laser bandwidth effects on degenerate four-wave mixing (DFWM) of Alber, Cooper, and Ewart (ACE) [Phys. Rev. A 31, 2344 (1985)]. The same model is used for intense, broad-bandwidth pump lasers interacting with a weak monochromatic probe in a medium composed of two-level atoms. The density-matrix equations describing the time evolution of the atomic polarization coupled to fluctuating fields are solved using an appropriate decorrelation approximation. A steady-state analytical solution is found for resonant and near-resonant DFWM, for intensities that do not saturate the medium. For more intense fields it is found to be necessary to form a more complicated set of differential equations for all products of the field and atomic density-matrix elements. The results show that as in the ACE theory, increasing the bandwidth b leads to an increased effective saturation intensity. However, we find the DFWM reflectivity scales as 1/b2{b}^{2}b2 when the probe is monochromatic and not 1/b as in the ACE theory. Furthermore, the saturation behavior of nonresonant DFWM is found to differ from the predictions of ACE. Atomic motion effects are shown to yield a Doppler-broadened line shape and also to affect the saturation behavior of the signal.
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 report on an ac-Stark-effect-enhanced wave-mixing experiment in I2{\mathrm{I}}_{2}I2​ vapor in which an output uv signal at frequency 2${\ensuremath{\omega}}_{1}$+${\ensuremath{\omega}}_{2}$ is maximized when the input frequencies ${\ensuremath{\omega}}_{1}$ and ${\ensuremath{\omega}}_{2}$ are both detuned in the same direction from the resonance frequencies of the free molecule. A theory based on a configuration interaction between the ``dressed molecular levels'' is presented to explain the strong enhancement of the uv signal under these conditions. The data presented demonstrate that tunable coherent radiation at ultraviolet and vacuum-ultraviolet frequencies can be generated by the wave-mixing process we describe.