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American Journal of Physics

The Stimulated Raman Effect

N. Bloembergen

Published Nov 1, 1967• 461 citations
Publisher

Abstract

This paper reviews the main experimental and theoretical developments in stimulated Raman scattering of light, which has been actively investigated since 1962. The effect cannot be discussed properly without paying attention to related nonlinear effects which include stimulated Brillouin and Rayleigh scattering, self-focusing of light, and modulation of the refractive index. The physical processes are emphasized and no encyclopedic survey of all the data and the research literature is attempted, but a brief historical account is added in the final section.

DOI
10.1119/1.1973774

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This paper reviews the main experimental and theoretical developments in stimulated Raman scattering of light, which has been actively investigated since 1962. The effect cannot be discussed properly without paying attention to related nonlinear effects which include stimulated Brillouin and Rayleigh scattering, self-focusing of light, and modulation of the refractive index. The physical processes are emphasized and no encyclopedic survey of all the data and the research literature is attempted, but a brief historical account is added in the final section.
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An investigation was made of the influence of different excitation conditions on the self-focusing of stimulated Raman-scattered light. It was found that the dimensions of self-focusing filaments and their number depended on the energy of the exciting radiation and the thickness of the scattering layer. In the situation in which self-focusing points were observed at both ends of a Dewar flask, the anti-Stokes scattering included (in addition to rings of class 1) scattering along the axis. Estimates were obtained of the self-focusing threshold power related to the Kerr effect and to the increase in the polarizability of molecules due to excitation. It was found that the first of these mechanisms could not give rise to self-focusing of the Raman-scattered light, whereas the threshold of the second mechanism was close to the excitation energy at which such self-focusing was observed.
We review the history and nature of stimulated scattering of optical beams and of the large phase-conjugate component often observed in stimulated backscattering, whether it be of Raman, Brillouin, Rayleigh, or other origin. We review the theory of the magnitude of the phase-conjugate component in stimulated backscattering of waves in a multimode optical guide (the usual experimental configuration) or in free focus. Wide applicability of stimulated backscattering for optical phase conjugation is found.
Polarization effects in stimulated Raman and stimulated Rayleigh scattering and self focusing are investigated from the viewpoint of the scattering of polarized photons by molecules. Both stimulated vibrational Raman scattering in liquids and stimulated rotational Raman scattering in gases are considered, and it is demonstrated that the polarization changes and relative power thresholds for different laser polarizations should be somewhat different to those predicted in other theories. For example, the ellipticity eta 0 of the stimulated rotational Raman photons in the forward direction from Delta J=+or-2 transitions in gaseous symmetric top molecules is given in terms of the initial ellipticity eta 1 by sin 2 eta 0 = - 5 / 7 sin 2 eta 1 , whereas conventional theories predict that eta 0 and eta 1 are equal in magnitude and opposite in sign. Furthermore it is shown that deviations from this relation could provide a measure of the degree of optical orientation of the molecules.
When a high-intensity laser beam passes through a transparent and homogeneous optical medium, the induced light scattering may manifest the properties of stimulated radiation characterized by threshold requirement, high directionality, and high brightness. This is the stimulated scattering of intense coherent light. Discoveries and studies of various types of stimulated scattering effects have provided a much deeper and more comprehensive understanding of interactions between the intense coherent light and matter. On the other hand, devices based on stimulated Raman scattering, stimulated Brillouin scattering, and stimulated spin-flip Raman scattering can be employed as highly efficient tunable frequency shifters of coherent light. Stimulated Kerr scattering can be used to generate a super-broadband coherent light and to investigate the molecular anisotropy of liquids. In addition, the recently developed stimulated Rayleigh–Bragg scattering and stimulated Mie scattering can significantly reduce the threshold requirement, and provide a highly efficient no-frequency-shift optical phase conjugation wave.
Selected topics related to the fundamentals of nonlinear optics are discussed. First, a brief description on the theory of nonlinear optical susceptibilities is given. Emphasis is on the basic properties, on the recently developed bond theory, and on the dispersion of nonlinear susceptibilities. Then the coupled wave approach is discussed. It is shown that the transverse resonant excitation in material can be treated as a material excitational wave, and most nonlinear optics problems can be understood as results of coupling between em waves or em and material excitational waves. A number of examples of current interest are presented. These include sum- and difference-frequency generation, Raman scattering by coherent excitation, stimulated Raman and stimulated polariton scattering, four-wave mixing, and vibrational relaxation measurements. Finally, the physical distinction between laser emission and resonant stimulated Raman scattering in an optically pumped three-level system are considered. A similar problem on the distinction of hot luminescence and resonant Raman scattering has recently attracted much attention. It is shown that the hot laser action is connected directly with the population inversion, while the resonant stimulated Raman scattering is connected with transverse excitation. The problem is, however, more complicated for a multi-level system. (auth)