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Soviet Journal of Quantum Electronics

Relationship between stimulated fluorescence and stimulated resonance Raman scattering of dyes in a resonator

A. Lau, Kurt Lenz, P. P. Kircheva, H.‐J. Weigmann, M Pfeiffer, W. Werncke

Published Dec 31, 1979• 2 citations
Publisher

Abstract

An investigation was made of the visibility of stimulated Raman lines under conditions of molecular resonance. A cell containing the medium under study was placed inside a resonator whose parameters were varied by changing the reflection coefficients of the mirrors or altering the length. The observed deterioration in the visibility of the Raman lines when the resonator Q factor was increased and its length was decreased could be explained qualitatively by a decrease in the nonlinear transmission of the dye for the pump radiation.

DOI
10.1070/qe1979v009n12abeh009907

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An investigation was made of the visibility of stimulated Raman lines under conditions of molecular resonance. A cell containing the medium under study was placed inside a resonator whose parameters were varied by changing the reflection coefficients of the mirrors or altering the length. The observed deterioration in the visibility of the Raman lines when the resonator Q factor was increased and its length was decreased could be explained qualitatively by a decrease in the nonlinear transmission of the dye for the pump radiation.
An analysis is made of nonlinear nonstationary equations describing dynamics of the stimulated Raman scattering in optical resonators excited by external nonmonochromatic radiation. The threshold of the excitation of the stimulated scattering by nonmonochromatic radiation is found and its dependence on the dispersion of the active medium is deduced. Solutions are obtained for steady-state oscillations in a resonator and their characteristics are investigated as a function of the spectrum of the exciting radiation and of the dispersion of the active medium.
Abstract The gain of the stimulated resonance RAMAN scattering (SRRS) and stimulated fluorescence is obtained by means of an analytical solution of the density matrix equation and MAXWELL's equations for laser‐ und STOKES‐radiation. The transient effects, which are caused by the population change of the molecule levels, and the influence of the resonance absorption on the pumping and the STOKES radiation are studied. The strong laser absorption yields a maximal gain, which shows, why the stimulated resonance RAMAN scattering could not be observed in many substances. As a result of our paper we give a possible interpretation of the experimentally observed relation between the stimulated fluorescence and the resonant RAMAN scattering.
A new variant of active Raman spectroscopy is proposed. Instead of two-frequency pumping, radiation in resonance with the scattering transition is used and a static electric field is applied simultaneously. This variant may have an advantage over the conventional method in the case of a large Stokes shift which is found, for example, in the Raman scattering due to electronic transitions. An analysis is made of the dynamics of the interacting waves and the optimal length of nonlinear medium to which a static electric field should be applied is determined.
A theoretical investigation is reported of the Raman scattering in the rf range by polar molecules. It is shown that an increase in the Stokes frequency ω s (from zero) results in an increase in the imaginary part of the susceptibility, which governs the spontaneous Raman scattering cross section and the stimulated Raman scattering increment. This increase in the susceptibility is faster than in the optical range by a factor of ω s 2 . The susceptibility maximum occurs at the Stokes frequency and its width is of the order of the width of the transition line at which the Raman scattering takes place. A further increase in the frequency reduces the resonant contribution to the Raman scattering, and the frequency dependences of the parameters of this contribution approach the dependences typical of the optical range. The influence of the saturation effects on the resonant Raman response is pointed out.
A model is developed for the description of stimulated Raman scattering. This model allows for changes in the level populations due to radiative transitions and it can be used also for an arbitrary detuning of the pump radiation from the center of a line of an atom in the active medium. A study is made of the conversion of wide-band laser radiation into a Stokes signal. It is shown that this conversion is quite efficient and the Stokes signal gain corresponds to coherent scattering. This result is related to the matching of the phases of the pump and Stokes signals. Numerical investigations carried out using this model under the experimental conditions described elsewhere give results in agreement with the experimental data.
An investigation was made of the influence of the geometric excitation conditions on the energy dependences of the stimulated scattering of focused laser pulses of ~ 10 −8 sec duration when the sharpness and depth of focusing were varied. The experimental results obtained in this study were interpreted theoretically on the basis of a quantum analysis of stimulated Raman scattering in a two-level system. The experimental relationships could be explained only if an allowance was made for the changes in the populations of the levels participating in the Raman transition. It was possible to select the experimental conditions so that reconstruction of the wavefront of the pump radiation was observed under stimulated scattering conditions in a wide energy range.