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Quantum and Semiclassical Optics Journal of the European Optical Society Part B

Polarization of radiation amplified by dye solutions

V. A. Chernyavskii, L. G. Pikulik, K. I. Rudik, A. F. Grib

Published Jun 1, 1998• 5 citations
Publisher

Abstract

Experimental investigations of the change of polarization state of probing radiation on passing through anisotropically excited solutions of rhodamine 6G and 3,6-tetramethyldiamino- N -methylphthalimide in glycerol were carried out. These investigations allowed us to find the phase anisotropy in these molecular systems. The parameters of the polarization ellipse (the ratio of axes , orientation, direction of rotation) were determined. The main factors (the intensity and orientation of the polarization plane of the probing radiation) influencing these parameters were established. The differences between the refractive indices were designed with the help of the obtained parameters of the polarization ellipse. The spectral behaviour of the amplitude and phase anisotropy for the long-wavelength band of absorption and fluorescence was studied and described qualitatively. The features of the spectral behaviour of for the indicated solutions, which are modelled by different systems of energy levels of the active molecules, were established.

DOI
10.1088/1355-5111/10/3/004

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Experimental investigations of the change of polarization state of probing radiation on passing through anisotropically excited solutions of rhodamine 6G and 3,6-tetramethyldiamino- N -methylphthalimide in glycerol were carried out. These investigations allowed us to find the phase anisotropy in these molecular systems. The parameters of the polarization ellipse (the ratio of axes , orientation, direction of rotation) were determined. The main factors (the intensity and orientation of the polarization plane of the probing radiation) influencing these parameters were established. The differences between the refractive indices were designed with the help of the obtained parameters of the polarization ellipse. The spectral behaviour of the amplitude and phase anisotropy for the long-wavelength band of absorption and fluorescence was studied and described qualitatively. The features of the spectral behaviour of for the indicated solutions, which are modelled by different systems of energy levels of the active molecules, were established.
Experimental data on the amplification of polarized light in optical quantum amplifiers utilizing laserpumped dyes show that, in general, the polarization of the amplified light differs from that of the light being amplified. A theory is put forward whereby this effect is related to the anisotropy of the stimulated emission characteristic of complex organic molecules and is interpreted as a difference between the polarizations of the stimulated emission and stimulating radiation. The complex polarizability tensor is used as the main optical characteristic of complex molecules. The possibility of using the difference between the polarizations of the stimulated emission and stimulating radiation to produce light-amplifying polarizers and optical switches is indicated.
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).
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.
Emission spectra of concentrated (~10 18 –10 19 cm –3 ) ethanol solutions of Rhodamine C excited by high-power (~10 25 –10 26 cm –2 s –1 ) laser radiation were measured. The emission spectrum consists of two narrow bands (with half-widths of ~200–300 cm –1 ). The long-wavelength band was interpreted as cooperative spontaneous emission, and the short-wavelength band was assigned to the amplified spontaneous emission. The ratio of their intensities depends on the dye concentration and the pump power density. The ratio of band intensities is assumed to be determined by the dephasing rate of excited molecules responsible for cooperative spontaneous emission.
Many practical laser amplifiers exhibit anisotropic gain due to polarization of the pumping fields or to a fixed preferential alignment of the active dipoles. Several specific causes and consequences of gain anisotropy are discussed in detail. In the analysis, the emphasis is placed on dye-laser systems including arbitrary amplitudes, phases, and polarizations of the pump and signal fields. Analytical results are presented for a unidrectional molecular distribution, and it is found that the polarization states of the pump and signal fields change with distance in the amplifier.