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Soviet Journal of Quantum Electronics

Tensor description of anisotropy in light amplification by dye solutions

O. I. Yaroshenko, K. I. Rudik

Published Mar 31, 1981• 3 citations
Publisher

Abstract

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.

DOI
10.1070/qe1981v011n03abeh006330

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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.
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.
Introduction Previous discussions (see Section 10.4) suggested that stimulated emission can be used to generate optical gain, that is, to amplify radiation. The reader certainly has experience in the amplification of electronic signal. For example, radio receivers capture faint radio waves and turn them into a signal that is powerful enough to drive large speakers. This electronic amplification increases the amplitude of the signal while faithfully preserving its acoustic frequencies and modulation characteristics. Similarly, optical amplification is expected to increase the amplitude of an optical signal while preserving its frequency, its modulation characteristics, and its coherence. The latter requirement is of particular significance for optical radiation, where the coherence of naturally occurring radiation rarely exceeds one micrometer. Lasers are the primary source for coherent radiation. They depend on stimulated emission for amplification and for the generation of coherent radiation (the word laser is the acronym of Light Amplification by Stimulated Emission of Radiation). For amplification, an atomic system that is part of the laser medium must be prepared with a sufficiently large number of particles in the excited state. (The term atomic system is used here to describe all microscopic systems including molecules and free electrons.) Radiation passing through that excited medium encounters multiple events of stimulated emission, each event contributing one photon that is added coherently to the propagating beam. When the number of events of stimulated emission exceed all losses by absorption or scattering, the incident radiation is amplified.
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 mechanisms behind the amplification of light by stimulated emission are investigated using a semiclassical approach. The theory is developed in the plane wave mode picture so as to follow closely the correspondence with the usual quantized field treatment. It is shown that the interference between stimulating and stimulated fields is an essential process for producing the well-known first-order effects, and that interference between stimulated emission fields from different atoms in the sample determines the spatial distribution of the amplification when this is measured locally using a light detector without mode discrimination.
The phenomenon of stimulated Rayleigh-wing scattering in anisotropic molecular liquids is analyzed. Representative combinations of polarization for the incident and scattered light are considered. It is shown that in regions where the focused laser beam is intense, saturation occurs in the molecular response to external optical fields, in that perfect alignment of the individual liquid molecules in the optical fields is approached. Accordingly, the nonlinear amplification associated with the stimulated radiation is reduced. The results of the analysis qualitatively explain several important recent observations which are in conflict with previous theroretical predictions. For example, it is shown that the nonlinear gain is considerably greater when the incident light is circularly polarized (the stimulated radiation being circularly polarized in the reverse sense) than it is when the incident light is linearly polarized. Despite saturation, sufficient amplification exists in the former case to allow the efficient conversion of incident to stimulated Rayleigh light at moderate power levels.