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Optics and Spectroscopy

On the Theory of the Resonance Transformation of Light by Molecules with Consideration of Two Intermediate Energy Levels

Vitaly Morozov, P. P. Shorygin

Published Feb 1, 1966• 2 citations
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A mathematical modeling of the time evolution of the populations of the states of a five-level molecule during transformation of resonant monochromatic irradiation and spontaneous emission from the highest-energy state excited by a short pulse of light is performed. The formalism of the optical Bloch equations and quantum theory of radiation are applied a composite system consisting of a molecule and a quantized radiation field. The results of simulation of the evolution of the population of the states of the molecule in the case of spontaneous emission are similar for both of these two approaches, but differ significantly in the case of conversion by the molecule of monochromatic radiation. These differences are the greater, the higher the intensity of resonance Rayleigh scattering or (and) relaxed fluorescence, as a result of which the molecule returns to the initial ground state. An explanation of the nature of these differences is given.
In an optical radio-frequency double-resonance experiment on NO2{\mathrm{O}}_{2}O2​ optical saturation resonances are observed. These resonances appear superimposed on the normal magnetic resonance spectrum. With increasing laser light intensity they change the resonance spectrum considerably. We present a model to describe the observed saturation phenomena: The resonances are attributed to the interaction of two optical photons and at least one radio-frequency photon with the molecule. The theory shows that saturation resonances appear in the population and in the coherence of the dressed-molecule levels in agreement with the experimental results.
Dissociation probabilities, energy absorption, and ground-state populations are calculated numerically for interaction of a Morse oscillator with a resonant ultrashort (tp{\mathit{t}}_{\mathit{p}}tp​${10}^{\mathrm{\ensuremath{-}}12}$ sec) intense laser pulse as a function of intensity and pulse area in order to investigate the sensitivity of coherence phenomena to delocalization and chaos in molecule-radiation field systems. It is concluded that a zero-area pulse can reduce considerably energy absorbed by a molecule as well as dissociation probabilities for intensities below and near the chaotic region. It is found that the two-level model (describing the interaction of light resonant with the ground to first excited level transition) works well up to the intensity 1012{10}^{12}1012 W/cm2{\mathrm{cm}}^{2}cm2, above which transitions to higher levels must be considered.