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Phase Conjugation via Four-Wave Mixing in a Resonant Medium

Joseph Nilsen

Published Jan 1, 1982• 0 citations
Publisher

Abstract

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.

DOI
10.7907/rv9b-gv44.

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•Mar 1, 1980•2 citations
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.
We develop a semiclassical theory of the polarization properties of phase conjugation by two-photon resonant degenerate four-wave mixing. The theory includes the effects of saturation by the pump waves. We solve the density-matrix equations of motion in steady state for a nonlinear medium consisting of stationary atoms with a ground and excited state connected by two-photon transitions. As an illustration of the general results, we consider an S0{S}_{0}S0​\ensuremath{\rightarrow}S0{S}_{0}S0​ two-photon transition, which is known to lead to perfect polarization conjugation in the limit of third-order theory. We show that the fidelity of the polarization-conjugation process is degraded for excessively large pump intensities. The degradation can occur both due to transfer of population to the excited state and due to nonresonant Stark shifts. Theoretical results are compared to those of a recent experiment [Malcuit, Gauthier, and Boyd, Opt. Lett. 13, 663 (1988)].
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.
Part I of this thesis describes the theoretical and experimental aspects of a new area in coherent optics known as phase conjugate optics. By using nonlinear optical mixing techniques, the complex conjugate of an arbitrary incident monochromatic wave can be generated. In particular, the theory of the degenerate four-wave mixing technique is presented. Experimental observation of phase conjugate wave front generation in a liquid crystal material (MBBA) is described. The ability of the conjugate wave front to correct for phase aberration is demonstrated. The quantum mechanical origin of the nonlinear third order susceptibility responsible for the four-wave mixing process is illustrated in an atomic system. Because of a finite memory time of such an atomic system, the electromagnetic waves taking part in the mixing process need not occur simultaneously. The applications of the phase conjugation process to real-time information processing and the characteristics of a phase conjugate resonator are discussed in detail. The ability of an optical fiber to confine the propagation of electromagnetic waves over a long distance and within a small cross sectional area implies that large optical intensities can be maintained over a long " interaction length even at moderate incident optical power. Part II of this thesis describes some third order nonlinear optical phenomena that have been observed under this condition. Especially, phase conjugation by degenerate four-wave mixing in a fiber has been shown to require significantly less pumping power. The theoretical and experimental studies of four-wave mixing in a liquid-filled fiber are presented. Extensive experimental efforts have been devoted over the last few years to the study of stimulated Raman scattering and the oscillation of the Stokes radiation inside fibers. A detailed theoretical treatment will be given here to describe these effects. The analysis shows that pump depletion due to the nonlinear process is very important in describing the stimulated Raman scattering in low loss fibers and is the dominant saturation effect in a fiber Raman oscillator. Finally, the implications of nonlinear optical phenomena to fiber optic communication will be mentioned.
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 theoretical and experimental aspects as well as potential applications in the field of coherent optics known as Phase Conjugate Optics (PCO). By utilizing nonlinear optical techniques, real-time or wavefront reversal of an arbitrary incident electromagnetic field can be realized. The nonlinear optical interaction gives rise to what is referred to as the phase conjugate (of the incident monochromatic wave) by performing the operation of complex conjugation upon the incident wave's complex spatial amplitude in real time. This conjugate wave, which is also designated as being a wavefront, has the property of exactly retracing the path of the incident field. The ability of the conjugate wave to correct for inhomogeneous linear and nonlinear (intensity-dependent) aberrations as well as polarization distortions is proved. In particular, the theory of a degenerate four-wave nonlinear optical interaction as providing for the conjugator is presented. The effects of linear and nonlinear losses upon this interaction are discussed. The quantum mechanical origin of the third order nonlinear optical susceptibility responsible for the four-wave mixing process is analyzed for both single and two-photon allowed transitions in an atomic (or molecular) system. The analogies of four-wave mixing with that of real-time holography are discussed. The theory of conjugation via four-wave mixing in optical waveguides is presented. Several of the above characteristics of conjugate fields are verified experimentally where conjugate fields via degenerate four-wave mixing were observed both in the bulk and in waveguide geometries, using carbon disulfide as the nonlinear medium. Amplified time-reversed wavefront generation as well as a mirrorless optical parametric mode of oscillation have been observed, both in agreement with theoretical predictions. Potential applications of PCO are discussed in three different regimes: spatial-frequency, temporal-frequency, and spatial/temporal frequency domains. In the first category, the ability of PCO to correct for image modal dispersion in optical waveguides as well as the use of PCO to perform real-time coherent image processing and nonlinear microscopy is discussed. Temporal-frequency domain applications of PCO to be analyzed include the use of a nearly degenerate four-wave mixing process as a narrowband, wide field-of-view optical filter, capable of an amplified bandpass. The ability of a PCO interaction to renarrow (transform limited) optical pulses which have been temporally spread due to propagation through (group velocity) dispersive channels is analyzed. A potential application of PCO in the field of nonlinear laser spectroscopy is presented. Specifically, the scattering of a probe photon off a two-photon coherent state (created in a three-level atomic system) is shown to yield a conjugate replica. This conjugate replica is capable of providing sub-Doppler width resolution of the two-photon resonance. Further, in the transient regime, the optical free-induction decay of the conjugate wave is capable of yielding detailed spectral features of the three-level system such as the anharmonic contribution to a (nearly) harmonic potential. This technique, performed in the time domain, is known as [alpha]-beat spectroscopy. Finally, a detailed theoretical and experimental study is presented of a laser resonator in which one (or both) of the mirror(s) comprising the optical cavity is replaced by a conjugate mirror (PCM). This novel resonator, which is termed a conjugate resonator (PCR), combines many of the spatial- and temporal-frequency aspects of PCO interactions discussed above. The stability criterion, transverse and longitudinal mode spectra, and the PCR output energy, as well as the frequency locking features of the laser modes to the PCM are discussed.