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International Meeting on Instabilities and Dynamics of Lasers and Nonlinear Optical Systems

Four-wave-mixing Processes in Multiple-pump Multiphonon Systems: Effects of Coherence Length

Jui‐Teng Lin

Published Jan 1, 1985• 0 citations
Publisher

Abstract

The effects of four-way-mixing (4WM) and the generation of high-order Stokes (HOS) in a single pump single phonon system have been studied previously.1 In the present paper we shall develop a general theory which provides the equations of motion in a multiple pump multiphonon system which includes all pair field interactions via both Raman and 4WM. The effects of the coherence length of the pump pairs and of the 4WM on the generation of HOS will be investigated analytically and numerically. Pump depletion and the feedback effects due to the high-order processes will be included. The dephasing of the phonon modes will be derived via the phonon-phonon interaction in the Markovian approximation.2

DOI
10.1364/idlnos.1985.wd25

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The effects of four-way-mixing (4WM) and the generation of high-order Stokes (HOS) in a single pump single phonon system have been studied previously.1 In the present paper we shall develop a general theory which provides the equations of motion in a multiple pump multiphonon system which includes all pair field interactions via both Raman and 4WM. The effects of the coherence length of the pump pairs and of the 4WM on the generation of HOS will be investigated analytically and numerically. Pump depletion and the feedback effects due to the high-order processes will be included. The dephasing of the phonon modes will be derived via the phonon-phonon interaction in the Markovian approximation.2
A general theory of transient stimulated Raman scattering and the phase-matching diagrams are developed based on an interaction Hamiltonian which includes all the possible competing interaction channels. In a Raman system pumped by multiple crossing beams with multiple Stokes and anti-Stokes components, these channels are defined by the interactions among fields at different frequencies and/or k vectors of the pump pairs and Stokes and anti-Stokes fields. An ensemble-averaged equation of motion for the active phonon mode is derived within the Markovian approximation in which the phonon-phonon coupling (pressure effect) is reduced to an energy relaxation and a phase fluctuation. A complete set of transient coupled equations including phase modulation, Stark shift, medium (anharmonic) saturation, and all the possible four-wave-mixing channels is presented. In the transient regime, it is found that the effects of the Stark shift on the Raman efficiency are mainly governed by the input pump energy in contrast to the steady-state theory where the pump intensity plays the main role. Both analytic and numerical methods are developed in describing the nonlinear effects due to the energy feedback mechanism in the strong pump-depletion regime. Twelve possible four-wave-mixing channels are analyzed for nonlinear phase diagrams characterized by the angles among pump pairs, and Stokes and anti-Stokes fields. Finally, numerical examples are shown for the effects of the coherence lengths of high-order Stokes fields and pump pairs on the generation of low-order Stokes fields.
The delayed or time-domain four-wave-mixing experiment is treated in the regime of intense near-resonant pulses. The interaction with the radiation during both pump and probe pulses is considered to all powers of the electric field amplitude. Analytical results are obtained for an effective four-level system. These include the dependence of the coherence amplitudes on the ratio of the pump-field intensities when there is a large vibrational discrepancy between ground and excited electronic states and a general solution for the unitary time development during the probe pulse. For the first time, delayed coherent anti-Stokes Raman scattering is detected from highly dilute (10-ppm) guest molecules. Illustrative examples are presented for the system of pentacene in benzoic acid at low temperature. Vibronic-free induction decay and the effect of field inhomogeneity across the beam profile are found to be essential for understanding the observed intensity and spectral distribution of the signal beam in the region of optimum pulse intensity.
I study the coherent interaction of a three-level atom in the lambda configuration with pump, Stoke, and anti-Stokes laser fields. The pump laser field drives transitions from the two non-degenerate lower levels to the excited state which is highly detuned for either transition. This excited state is also coupled to each of the lower states by Stokes or anti-Stokes transitions so that this system may represent a model of four-wave mixing. Assuming large detunings, the excited state is adiabatically eliminated from obtaining an effective two-level system with Raman coupling between the levels. Optical Bloch equations are obtained for this effective two-level system, and phenomenological damping terms are added for collisional dephasing of the Raman transitions. The equations are solved for the steady-state as well as by the method of adiabatic following. From these solutions we obtain the polarization.
Four-wave coherent mixing models for two quasi-monochromatic pumping fields and pulses of a two-component Stokes field with an elliptic polarization and a duration on the order of the period of oscillations have been derived for a two-level medium with a forbidden dipole transition. It is shown that, under the unidirectional wave propagation conditions and in the absence of depletion of pumping, the system of Maxwell-Bloch equations can be reduced to a new completely integrable system of equations. Nonsoliton radiation dynamics of generation of Stokes field pulses is studied in the framework of the integrable reduction of this model. The apparatus for the inverse problem algorithm corresponding to the solvable problem is developed. An approximate asymptotic expression for the leading front of the pulse packet being generated is obtained for various initial and boundary conditions. The application of these results for describing parametric processes involving various types of waves is discussed.
The equations for plane-wave steady-state propagation of n fields interacting via four wave processes in a Raman medium have been known since at least 1962. Complete analytic solutions have only been found for the process of harmonic generation. However, solutions have been obtained in the gain regime assuming zero pump depletion. Assuming all fields satisfy the phase matching condition we have found general analytic solutions to these equations. The solutions are complete in that they describe both pump deletion and saturation. Some example problems will be studied.