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Soviet Journal of Quantum Electronics

Resonance fluorescence of bromine and Raman scattering of laser radiation by bromine in small pores

Nikolai V. Karlov, А. Н. Орлов, R. P. Petrov, Yu. N. Petrov, A M Prokhorov, M. A. Yakubova

Published May 31, 1981• 0 citations
Publisher

Abstract

An investigation was made of the fluorescence and Raman scattering spectra of molecular bromine adsorbed in glass with fine pores. The source of pump radiation was an argon laser. Molecules adsorbed in a monolayer participated only in the Raman scattering but not in the fluorescence. The nature of the scattering depended strongly on the surface coverage of the adsorbent with bromine.

DOI
10.1070/qe1981v011n05abeh006939

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The review deals with various variants of classification of the types of secondary emission of light by molecules; cases are distinguished in which the secondary emission occurs without additional processes that find their way between photon emission and absorption; the advisability of differentiating between the cases of resonance fluorescence and resonance scattering is noted. Reference is made to papers that have made contributions to the development of quantum-mechanical and classical theory of Raman scattering and to the development of the concepts of the relations between electron-vibrational absorption spectra, fluorescence spectra, and scattering excitation near and near and far resonance. Conditions are considered of excitation of the spectrum at different relations between the electronic-oscillator damping constant, the atom vibration frequency, the rotational frequencies, and the difference between the frequency of the incident light and the frequency of the electronic transition. The conditions for the excitation of typical light scattering, typical resonance fluorescence, and certain intermediate types, in which individual features of scattering are combined with certain features of fluorescence (phenomena of the transition type) are noted. The results of investigations of different models of the scattering centers, their advantages, shortcomings, and limits of applicability are compared. The most interesting results of the experimental investigations of resonant scattering of light by molecules and crystals are noted.
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The characteristics of stimulated Raman scattering in benzene and carbon disulfide introduced in pores of globular photonic crystals—opal matrices formed from close-packed balls (globules) of amorphous quartz (silica)—have been experimentally studied. Stimulated Raman scattering spectra have been excited by giant pulses of the second optical harmonic (532 nm) of a YAG laser. The spectra have been recorded in the direction of mirror reflection from the (111) growth surface of a globular photonic crystal at various angles of incidence (10°–70°) of laser radiation. It has been shown that the threshold of stimulated Raman scattering decreases sharply (by more than an order of magnitude) at a certain angle of mirror reflection and additional Stokes and anti-Stokes Raman satellites appear in the spectrum. The observed sharp decrease in the threshold of stimulated Raman scattering has been explained by an increase in the spectral density of the electromagnetic field in the surface region of the photonic crystal because of the approach of the spectral position of the stopband of the photonic crystal to the exciting line (532 nm) under variation of the angle of incidence of pump radiation on the (111) surface.
A theory for the resonance light scattering in a molecular system interacting with the heat bath is developed, taking into account the multilevel structure of the molecular system. An expression for the cross section of the resonance light scattering process is derived by using the Liouville operator method in the Markoff approximation; the cross section consists of three terms: resonance Raman scattering, resonance fluorescence, and their mixing. The mixing term vanishes in the limit of the zero vibrational dephasing constant. Analytical expressions for the resonance Raman scattering and resonance fluorescence cross sections are derived in the displaced harmonic oscillator model. Model calculations of the vibrational band structure in the resonance light scattering cross section are performed by using the expressions derived. Differences of the band intensity distribution in the resonance fluorescence from that in the resonance Raman scattering are illustrated.