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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Study of four-wave mixing based on excited state absorption

Xinxian Bao, Chunfei Li

Published Oct 25, 1996• 0 citations
Publisher

Abstract

Azo dye polymeric film were widely studied for real-time polarization holography and optical storage by degenerate four-wave mixing in the resonant absorption spectrum of the sample in the few past years. In this paper, we will report the experimental results of four-wave mixing based on excited-state absorption in ethyl orange doped in polyvinyl alcohol film. A He-Ne laser was used as the four-wave mixing source, and the excited light was an Ar+ beam. To explain the experimental results, a simplex four-level model of azo molecule polymeric system is built up. The dynamic process of phase conjugation signal by excited-state four- wave mixing is calculated through solving the rate equation of population in the excited-state. The theoretical analyses agree with the experimental results well. The excited-state optical storage mechanism of sample is discussed.

DOI
10.1117/12.255497

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Azo dye polymeric film were widely studied for real-time polarization holography and optical storage by degenerate four-wave mixing in the resonant absorption spectrum of the sample in the few past years. In this paper, we will report the experimental results of four-wave mixing based on excited-state absorption in ethyl orange doped in polyvinyl alcohol film. A He-Ne laser was used as the four-wave mixing source, and the excited light was an Ar+ beam. To explain the experimental results, a simplex four-level model of azo molecule polymeric system is built up. The dynamic process of phase conjugation signal by excited-state four- wave mixing is calculated through solving the rate equation of population in the excited-state. The theoretical analyses agree with the experimental results well. The excited-state optical storage mechanism of sample is discussed.
Four-wave mixing spectroscopy is presented as a convenient and effective optical method for the study of excited-state optical storage properties and nonlinear mechanisms in a dye-doped polymer film. The dynamic processes of optical storage properties and the efficiency of the diffraction grating are discussed. Backward-scattering four-wave mixing and forward-scattering four-wave mixing optical configurations are presented. A simple energy-level model is used to explain the excited-state optical storage mechanism, resulting from photo-induced excited-state population grating and trans-cis isomer grating.
The properties of polarization-dependent phase-conjugate (PC) reflectivities by degenerate four-wave mixing in saturable-dye-doped films are investigated on the basis of a four-level model including an excited-state absorption. Numerical calculations are carried out by taking account of the effect of molecular orientation as well as of pump propagation under the assumption that optically anisotropic dye molecules are rigidly fixed in a solid matrix without any positional and orientational order, in which a PC wave can be generated even in the case of a probe wave perpendicularly polarized to pump waves. Two cases of the polarization state are employed, where the polarization direction of the probe wave is either parallel or perpendicular to that of the parallel linearly polarized pump waves. Numerically calculating the PC reflectivities as a function of the pump intensity, we show how the polarization properties of the PC-reflectivity curves depend on saturation parameters, and clarify the influences of the molecular orientational and the pump propagation effect. The numerical results are compared with the experimental results obtained by using eosin-Y-doped polyvinyl alcohol films as saturable absorbers.
Phase conjugation by degenerate four-wave mixing in a saturable absorbing medium with a relatively long-lived excited state is analyzed; the analytical results are compared with experimental results. We propose a four-level model and take into account the effects of both excited-state absorption and pump propagation to explain the experimental results, which could not be explained by the models proposed previously. The numerical result predicts that the value of the phase-conjugate reflectivity as a function of the pump intensity is maximum at a certain absorbance (as absorbance increases) that is dependent on the cross section of the excited-state absorption. The present analysis explains most observations in the experiment, which was performed with a saturable-dye-doped polymer film as the saturable absorbing medium.
Studies on optical phase conjugation by degenerate four-wave mixing in aqueous rhodamine 6G solutions and in rhodamine 6G embedded in polyvinyl alcohol thin films are presented. The experiments were performed at 532 nm using picosecond pulses. Strong nonlinearities were observed in both media for three different polarization configurations of the incoming beams. The time dependence of the signals was also studied and was similar in both media. The decay kinetics in each case reflects the competition between two different processes: a fast one related to the relaxation of the anisotropic absorption and a slower one associated with the decay of the stable S1 state.
Degenerate four-wave mixing (DFWM) is a simple method to achieve phase conjugation. It uses the third-order nonlinearity of the electric susceptibility to produce changes in the optical properties of materials. A dynamic grating is then induced. Such gratings might be used as fast optical memories in optical computing. Our aim is to find media with large nonlinear susceptibilities and fast response time. We report phase conjugation of 532-nm laser radiation by DFWM in dye solutions. The time dependence of the conjugated wave is investigated experimentally and compared to theoretical predictions. We have also studied the influence of the solvents, dye concentration, and pump intensity on the phase conjugated signal. The results are compared with those predicted by three nonlinear mechanisms. Thermally induced refractive-index changes, Kerr effect, and saturable absorption are considered.
The properties of phase conjugate (PC) beams generated by an erythrosin/polyvinyl alcohol film are briefly reviewed along with demonstrations of PC interferometries, and an experimental study of the time dependence of the phase difference between saturable absorption and holographic components of the PC signal is reported. The results show that the phase difference between two components of PC signals changed temporally with a period of about nine minutes and reached 110 deg five minutes after the initiation of degenerate four-wave mixing at the pump beam intensity of 1 W/sq cm.