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Soviet Physics Uspekhi

RESONANCE STIMULATED RAMAN SCATTERING IN MOLECULAR SYSTEMS HAVING NORMAL AND INVERTED POPULATIONS OF ELECTRONIC STATES

Яков Семенович Бобович, A. V. Bortkevich

Published Jan 31, 1971• 10 citations
Publisher

Abstract

CONTENTS I. Introduction 1 II. Principal Physical Hypotheses and Formulas 2 III. Requirements Imposed on the Substances Being Studied. Processes Accompanying Resonance Stimulated Raman Scattering. Experimental Systems 7 IV. Quasiresonance Stimulated Raman Spectra of Unexcited Molecules 10 V. Resonance Stimulated Raman Scattering of Excited Molecules 13 VI. Conclusion 18 Bibliography 19

DOI
10.1070/pu1971v014n01abeh004433

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Stimulated resonance Raman scattering (review)

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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.

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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.

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Abstract The gain of the stimulated resonance RAMAN scattering (SRRS) and stimulated fluorescence is obtained by means of an analytical solution of the density matrix equation and MAXWELL's equations for laser‐ und STOKES‐radiation. The transient effects, which are caused by the population change of the molecule levels, and the influence of the resonance absorption on the pumping and the STOKES radiation are studied. The strong laser absorption yields a maximal gain, which shows, why the stimulated resonance RAMAN scattering could not be observed in many substances. As a result of our paper we give a possible interpretation of the experimentally observed relation between the stimulated fluorescence and the resonant RAMAN scattering.

Annalen der Physik•Jan 1, 1974•6 citations
CONTENTS I. Introduction 1 II. Principal Physical Hypotheses and Formulas 2 III. Requirements Imposed on the Substances Being Studied. Processes Accompanying Resonance Stimulated Raman Scattering. Experimental Systems 7 IV. Quasiresonance Stimulated Raman Spectra of Unexcited Molecules 10 V. Resonance Stimulated Raman Scattering of Excited Molecules 13 VI. Conclusion 18 Bibliography 19
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.
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.
Abstract Laser Stimulated Scattering and Multiphoton Excitation is the first book that comprehensively covers the following three major areas: (1) Quantum electrodynamic theory of stimulated scattering and multiphoton excitation processes; (2) Various stimulated scattering effects, including the early discovered stimulated Raman scattering (SRS) and stimulated Brillouin scattering (SBS), the later investigated stimulated Kerr scattering (SKS), and the recently developed stimulated Rayleigh–Bragg scattering (SRBS) and stimulated Mie scattering (SMS); (3) Multiphoton excitation-based nonlinear optical effects, photoelectric effects, atomic and molecular ionization effects, and molecular dissociation effects. Each chapter covers: (i) the concept and mechanism description, (ii) the necessary theoretical formulation, (iii) the experimental research achievements, and (iv) the scientific/technological applications. Laser Stimulated Scattering and Multiphoton Excitation is useful and suitable for academics, experts, and students working or interested in the areas of nonlinear optics, nonlinear photonics, laser spectroscopy, physical optics, physical chemistry, and optoelectronic engineering.
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.
Abstract The gain of the stimulated resonance RAMAN scattering (SRRS) and stimulated fluorescence is obtained by means of an analytical solution of the density matrix equation and MAXWELL's equations for laser‐ und STOKES‐radiation. The transient effects, which are caused by the population change of the molecule levels, and the influence of the resonance absorption on the pumping and the STOKES radiation are studied. The strong laser absorption yields a maximal gain, which shows, why the stimulated resonance RAMAN scattering could not be observed in many substances. As a result of our paper we give a possible interpretation of the experimentally observed relation between the stimulated fluorescence and the resonant RAMAN scattering.