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

Excited-state optical storage study in a dye-doped film using four-wave mixing spectroscopy

Xinxian Bao, Chunfei Li, Hongjing Kan, Lu Dai, William M. Tong

Published Jan 23, 1997• 0 citations
Publisher

Abstract

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.

DOI
10.1117/12.264197

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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Sep 16, 2005•0 citations
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.
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.
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.
Summary form only given. Self-diffraction by four-wave-mixing (FWM) in a nonlinear medium such as liquid crystals and photorefractive materials can contribute to perform energy transfer between the two incident beams. FWM in a saturable gain media has received an intense attention in recent years. Owing to the amplification experienced by all the interaction beams, the high diffraction efficiency is expected. This paper presents the demonstration of transient self-diffraction by pico-second FWM in a saturable amplifier Rhodamine 6G polymer dye. In this work, we extend our previous study of FWM in an inverted polymer dye in the transient regime by using signal and pump lasers with pulse duration of much less than the population relaxation time (several nanoseconds) in the polymer dye. The polymer dye saturable amplifier is shown to be an excellent nonlinear material with high diffraction efficiency and fast response time. It has a potential for applications such as real-time holography, phase conjugation, pulse shaping, and all optical temporal-spatial conversion.
Optical phase conjugation through degenerate four-wave mixing is observed in 4-[4-(Dimethylamino)styryl]-1-docosyl pyridinium bromide (DASPB) dye-doped in Polymethyl methacrylate - metacrylic acid (PMMA-PA) polymer films under low-power, continuous-wave laser irradiation. A maximum phase conjugate efficiency of 0.42% has been obtained for probe beam intensity at 2.5 W/cm2. Phase conjugation is observed for both parallel- and orthogonally-polarized probe and pump beams. The maximum PC reflectivity is achieved when the angle between probe beam and forward pump beam is 8 degrees. The effects of dye concentration, inter beam angle between probe and forward pump beam on phase conjugation reflectivity are also studied. PC signal strength first increases and then decreases with time. PC reflectivity is also increased by increasing the intensity of the backward and forward pump beam. The polarization and intensity profile are verified to be preserved in the conjugate signal. The predominant phase conjugation signal is attributed due to the saturable absorption and two photon induced fluorescence property of the dye molecules.
This work presents theoretical and experimental studies of the energy efficiency of multiwave mixing in complex molecular media (dye solutions) exhibiting higher order nonlinearities. There is a great variety of such media, including the resonance ones revealing nonlinearities of higher orders due to the absorption saturation effect and transitions between different excited states of the molecules. However, the majority of previous studies of multiwave mixing have been performed in the resonant medium approximation disregarding the induced anisotropy effect. A new method for enhancement of multiwave mixing in solutions of laser dyes has been proposed and substantiated with the use of lasing as an additional light beam, whose absorption by the molecules in the excited states leads to the formation of thermal dynamic gratings resultant in the improved efficiency of the energy exchange. The theoretical models for the formation of nonlinear dynamic holograms adequately describing the control process over multiwave mixing by an independent light beam, the frequency of which is tuned into the induced absorption band from the molecules in the excited state, have been developed. Polarization multiwave mixing has been realized in Rhodamine-6G dye solution using nonlinearities up to the ninth order inclusive. It has been demonstrated that on orthogonal polarization of the hologram recording waves the diffraction efficiency is lowered by one-two orders, the diffracted wave polarization being dependent on the diffraction order (the polarization plane alignment is identical within the orders of the same evenness).