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Optics and Spectroscopy

Influence of intermolecular relaxation processes on the absorption and emission spectra of solutions with high-intensity optical excitation

Nikolay G Bakhshiev, Е. С. Воропай, V. A. Gaisenok, O. P. Girin, A. M. Sarzhevskii

Published Jun 1, 1981• 2 citations
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36-21

Elizaveta Smirnova, Natalia A. Lozing, M. G. Gladush +1 more

The current paper demonstrates theoretical analysis of two types of spectral curves for several configurations of system of two-level light emitters, considering the influence of local field and close environment inside a transparent medium. Probe field absorption spectra and resonant fluorescence spectra are calculated under excitation of a strong monochromatic cw laser. The sensitivity of absorption and emission optical spectroscopy method is compared for revealing the effects of the medium on individual emitters and their ensembles. Spectral curves were calculated for model emitters considering local field influence of a transparent dielectric medium and local electron-phonon interactions, which determined the response of the emitters to an external laser field and effective relaxation mechanisms. The calculation formalism is based on a semiclassical approach, while the relaxation processes associated with the phonon contribution are introduced phenomenologically with references to other studies.

Оптика и спектроскопия•Jan 1, 2022•0 citations
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.
An investigation is made of the influence of quantum interference processes accompanying radiative relaxation of excited states on the population dynamics, total intensity, and spectra of the resonance fluorescence of three-level V -type atoms. Analytic expressions are obtained for the total intensity and spectra of the resonance fluorescence taking into account the off-diagonal nature of the radiative relaxation operator. It is shown that quantum interference process can substantially alter the total spontaneous emission intensity of the atoms and the population dynamics of the atomic levels, as well as the resonance fluorescence spectra.
The current paper demonstrates theoretical analysis of two types of spectral curves for several configurations of system of two-level light emitters, considering the influence of local field and close environment inside a transparent medium. Probe field absorption spectra and resonant fluorescence spectra are calculated under excitation of a strong monochromatic cw laser. The sensitivity of absorption and emission optical spectroscopy method is compared for revealing the effects of the medium on individual emitters and their ensembles. Spectral curves were calculated for model emitters considering local field influence of a transparent dielectric medium and local electron-phonon interactions, which determined the response of the emitters to an external laser field and effective relaxation mechanisms. The calculation formalism is based on a semiclassical approach, while the relaxation processes associated with the phonon contribution are introduced phenomenologically with references to other studies.