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IEEE Journal of Quantum Electronics

Dynamic gratings and four-wave phases conjugation in dye solutions

V. V. Kabanov, Alexander S. Rubanov

Published Jan 1, 1990• 8 citations
Publisher

Abstract

Four-wave phase conjugation in bleachable dye solutions modeled by two-, three-, and four-level schemes with Stokes-shifted absorption and emission bands is analyzed theoretically. The contribution of different types of dynamic gratings (resonance and thermal) to the formation of the conjugate wave, the influence of pump wave absorption, and the conditions for multistable reflectivity are considered. The conditions of the high reflectivity (R>1) caused by phase dynamic gratings have been determined.>

DOI
10.1109/3.62118

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Four-wave phase conjugation in bleachable dye solutions modeled by two-, three-, and four-level schemes with Stokes-shifted absorption and emission bands is analyzed theoretically. The contribution of different types of dynamic gratings (resonance and thermal) to the formation of the conjugate wave, the influence of pump wave absorption, and the conditions for multistable reflectivity are considered. The conditions of the high reflectivity (R>1) caused by phase dynamic gratings have been determined.>
In addition to results of earlier experiments where Bragg scattering from a distributed feedback dye laser is observed, in the experiment described here the occurrence of a phase conjugated reflected beam is demonstrated. It is shown that a distributed feedback laser can be used as a frequency selective reflector for a seperate dye laser. Some time ago Golub and Shuker investigated the feasibility of optical switching by Bragg scattering of a light beam from a spatially modulated gain grating. This grating formed the basis of a distributed feedback dye laser (DFDL) and the reflection was only visible if the DFDL was pumped above threshold. In that case reflectivities of more than 100% for small input signals could be obtained. Golub and Shuker emphasized that in their experiment phase conjugation could not occur. Their main argument was, that the probe beam and the pump beams had completely different origins. Consequently these beams had no constant phase relation, and hence degenerated four-wave mixing leading to phase conjugation was excluded.
We present a model to describe degenerate four-wave mixing in critical binary liquid mixtures and we analyze it through an experimental study of phase conjugation in critical microemulsions. The two concentration gratings related to the four-wave-mixing configuration give contributions to the conjugated signal which can be separated from their different formation and relaxation times. The model quantitatively describes the amplitude and the dynamics of the gratings and thus of the conjugate signal when one approaches the critical point. The theoretical predictions fit very well with the experimental data. Close to the critical point a 10% reflectivity has been obtained in this medium using a beam power of 1 W from a cw Ar+{\mathrm{Ar}}^{+}Ar+ laser. The limitations of these reflectivities at higher powers are discussed.
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.
We show that in order to describe completely the coherent coupling between the pump and probe pulses in a pump– probe measurement of transient absorption, the influence of induced phase gratings must be included. The importance of phase gratings is demonstrated experimentally for the case of a bleachable dye and analyzed in terms of transient four-wave mixing. These results are relevant to the interpretation of pump–probe measurements on all time scales performed with pulses from a single laser, particularly when the pulse duration is comparable with the material response time.
Two-frequency four-wave mixing in a dye is demonstrated, in which degenerate four-wave mixing is performed simultaneously within the absorption and emission frequency spectra, with two separate sets of beams. The coupling between the two bands gives rise to backward output waves at both frequencies, which are proportional to the phase conjugate of a single probe which can be at either of the two frequencies. Forward-propagating waves which are not conjugated are also generated at both frequencies. The frequency shifted outputs are tunable over the bandwidth of the spectrum in which they lie. A theoretical analysis is performed which is based on a four-level system model of the ground and first excited singlet states in a dye. Resulting are coupled equations, which are solved to yield the efficiencies of the various outputs. Experiments give results in good agreement with the theory.
Phase conjugation of backward-and forward-wave produced by degenerate four-wave mixing using a nearly resonantly enhanced nonlinearity in four-level organic dye solutions was investigated. The conversion efficiency of 22% had been obtained in a 2.5 X 10-5 - molar solution of Chlorophyll A in methylalcohol with a 5 mm interaction length and a pumping energy of ～ 8 mJ from SH of a Q-switched Nd: YAG. Degene-rate four-wave mixing by two-photon resonant-enhancement in the solution of rhodamine 6G in alcohol was studied. Measurements were performed which described the dependence of nonlinear reflectivities on the molar concentrations of the media and the intensities of the pumping and object waves. Phase conjugation characteristics of forward-wave in four-wave mixing process were theoretically analysed. Experiments have cofirmed the theoretical prediction. The method of quartet degenerate four-wave mixing had been ex-tended to the doublet degenerate case. Using this method image conversion from 1.06 μm to 5320 ? had been realized with a conversion efficiency of 25% in a 5 mm long satu-rable absorber made of organic dye 9740 solution in dichloroethane. Theoretical analy-sis showed that using a medium, which is a near resonant absorber for the infrared object wave but is transparent for the visible reconstruction wave, the conversion efficiency may be well in excess of unity.