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Soviet Journal of Quantum Electronics

Stimulated resonance Raman scattering (review)

Яков Семенович Бобович, A. V. Bortkevich

Published Mar 31, 1977• 6 citations
Publisher

Abstract

An analysis is made of some features of spontaneous resonance Raman scattering representing a noise signal which is amplified by a strong field in a nonlinear medium. A detailed review is made of the experimental results obtained in investigations of the spectra of stimulated preresonance and resonance Raman scattering in nonlasing and lasing systems. It is shown that, depending on the experimental conditions, these spectra may be due to transitions between vibrational levels of molecules which are in the ground or first excited electronic states. The example of several compounds is used to demonstrate the information which can be derived from such spectra. Possible practical applications of studies of such spectra are indicated. The physical basis of the theory of stimulated resonance Raman scattering is discussed and conclusions are drawn on the nature and mechanism of this Raman effect.

DOI
10.1070/qe1977v007n03abeh009442

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Soviet Journal of Quantum Electronics•Nov 30, 1979•1 citation
An analysis is made of some features of spontaneous resonance Raman scattering representing a noise signal which is amplified by a strong field in a nonlinear medium. A detailed review is made of the experimental results obtained in investigations of the spectra of stimulated preresonance and resonance Raman scattering in nonlasing and lasing systems. It is shown that, depending on the experimental conditions, these spectra may be due to transitions between vibrational levels of molecules which are in the ground or first excited electronic states. The example of several compounds is used to demonstrate the information which can be derived from such spectra. Possible practical applications of studies of such spectra are indicated. The physical basis of the theory of stimulated resonance Raman scattering is discussed and conclusions are drawn on the nature and mechanism of this Raman effect.
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.
Abstract A review of the theory of the stimulated resonance Raman scattering (SRRS) is given. The calculation of the gains for the SRRS with the ground level (SRRS I) or an excited one (SRRS II) as initial states shows that there are some restrictions for their appearance. Due to the strong resonance absorption of the pumping wave and the disturbing influence of stimulated fluorescence the SRRS I is not observable in a Franck‐Condon excitation and in an absorption of Lorentzian line shape. The SRRS II has a sufficiently large gain on the condition τel ≪vib (τel, τvib – transversal relaxation time of the electronic or vibronic transition). In case of a strong deviation of the wings of the absorption profile from the Lorentzian shape, however, the SRRS I is favoured rather than the two other processes. Another possibility to avoid the resonance absorption of the pumping wave exists for the transversal excitation of the SRRS. Thereby the limit of application of the SRRS may be extended to other substances which are no saturable absorbers. Apart from the saturable absorption and the transversal excitation the self‐induced transparency is the third possibility to generate SRRS of ultrashort light pulses.
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.
The passage of strong monochromatic laser radiation through a resonance medium consisting of three-level atoms is investigated. It is shown that if collisions are taken into account in the scattered waves the resonances at combination frequencies occur to first order in the laser field intensity. A numerical analysis of the dependence of the stimulated electronic Raman scattering (SERS) components' gain factors on the pump frequency is carried out. The dispersion curves of the SERS components' gain (absorption) factors for fixed values of pump frequency and intensity are plotted.
It is shown that, in strong optical fields (~109 W/cm2), Raman lines may be excited due to transitions with changes by 3 and 4 in the rotational quantum number, which are forbidden in the linear approximation. This lifting of forbiddenness for Raman scattering is due to four-photon processes in which a pump photon is absorbed and a Stokes photon is emitted in an elementary event. Under quasiresonance pumping, this type of stimulated Raman scattering may be observed due to rotational transitions. Estimate are made of the conditions for observation of the spontaneous and stimulated processes in specific media.