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Soviet Journal of Quantum Electronics

Influence of nuclear relaxation on stimulated emission from complex organic compounds

Yu. T. Mazurenko

Published Aug 31, 1979• 0 citations
Publisher

Abstract

An analysis is made of the dynamics of the electronic spectra of complex molecules associated with the nuclear motion, and of its manifestation on exposure of a molecule to high-power optical radiation. A model is proposed for the inhomogeneous broadening dynamics. This describes the random walk of the spectral frequency in the form of a Gauss-Markov random process and allows for the relaxation of the spectra which accompanies an electronic transition. Simple readily interpreted relationships, which describe the influence of nuclear relaxation on the stimulated emission frequency, are obtained.

DOI
10.1070/qe1979v009n08abeh009398

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An analysis is made of the dynamics of the electronic spectra of complex molecules associated with the nuclear motion, and of its manifestation on exposure of a molecule to high-power optical radiation. A model is proposed for the inhomogeneous broadening dynamics. This describes the random walk of the spectral frequency in the form of a Gauss-Markov random process and allows for the relaxation of the spectra which accompanies an electronic transition. Simple readily interpreted relationships, which describe the influence of nuclear relaxation on the stimulated emission frequency, are obtained.
An analysis is made of the intermolecular relaxation processes in activated solutions, which transform a two-level system of vibronic states of the activator molecules to a four-level system. It is shown that this alters considerably the main relationships in the theory of amplification and generation of light in activated solutions. More rigorous relationships obtained in the new model predict changes (in the course of pumping) not only of the intensity but generally also of the position and form of the absorption and luminescence spectra of such solutions, which should help in the interpretation of the known and new stimulated emission phenomena.
The correlation of inhomogeneous broadening at various frequency transitions in three-level systems is investigated, as is its effect on the intensity of a stimulated photon echo. It is shown that the correlation coefficient of inhomogeneous broadening at two different transitions and the response intensity of the stimulated photon echo depend on the parameter of the random interaction of an optical electron with a local field, as well as on the distribution width of additional frequency shifts owing to a partial fixation of transition energies. In this case, an insignificant variation of the correlation coefficient results in a considerable decrease in the response intensity.
The temporal dynamics of stimulated emission is studied, with particular emphasis on stimulated emission induced by x-ray pulses interacting with nuclei. In typical nuclear forward scattering experiments, the short incident x-ray pulse is accompanied by a huge number of off-resonant background photons. This prompts the question of whether stimulated emission can be observed in the delayed nuclear scattering signal which is emitted after the incident pulse has passed. We find that the stimulated photons essentially overlap with the stimulating pulse. To overcome this problem, we identify the reduction of the delayed scattered light intensity as an alternative signature for the stimulated emission. We further study a phase-sensitive variant of stimulated emission in the low-excitation regime, which provides convenient control parameters to facilitate the detection. Finally, we analyze the possibility of observing stimulated emission in nuclei driven by free electron lasers or synchrotron radiation sources.
Using a numerical solution of a system of equations for matrix elements of file-level model molecule density operator time dependencies of population on its states at different values of two irradiation pulses parameters (the pump pulse and the dump (or probe) pulse) and constants, determining rates of induced radiative transitions of the molecule, and radiative and nonradiative decays of the molecular states are calculated. The values of these constants were taken, in particular, close to these of the corresponding constants of molecules with intramolecular hydrogen bond as the 3-hydroxyflavone (3-HF) molecule. Values of irradiation pulses parameters are obtained, at which after enol-keto photoisomerization, induced by pump pulse, dump pulse induces molecular transition from excited electronic state in keto-form to ground state in this (ldquotautomericrdquo) form. This transition is accompanied by stimulated emission with a frequency of ldquotautomericrdquo fluorescence. Examples of periodic change of intensity of the stimulated emission are given, the frequency of oscillations of fluorescence intensity being proportional to dump pulse intensity.
The problem about fluorescence of organic molecules located in micropartical-cavity at two-photon absorption in the condition of laser pulse radiation influence taking into account stimulated transitions was theoretically investigated. The approach based on the metod of open-resonator theory with light fields expanded in series of quasinormal vibrational eigenmodes of a dielectric full sphere was used. For active molecules in microcavity the model of generalized two-level system noted with processes of two-photon absorption and emission, spontaneous and stimulated emissions on stokes frequencies was considered. The kinetic equations solution were obtained.