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Physical Review

Saturation Effects in Stimulated Rayleigh-Wing Scattering

R. M. Herman

Published Dec 5, 1967• 16 citations
Publisher

Abstract

The phenomenon of stimulated Rayleigh-wing scattering in anisotropic molecular liquids is analyzed. Representative combinations of polarization for the incident and scattered light are considered. It is shown that in regions where the focused laser beam is intense, saturation occurs in the molecular response to external optical fields, in that perfect alignment of the individual liquid molecules in the optical fields is approached. Accordingly, the nonlinear amplification associated with the stimulated radiation is reduced. The results of the analysis qualitatively explain several important recent observations which are in conflict with previous theroretical predictions. For example, it is shown that the nonlinear gain is considerably greater when the incident light is circularly polarized (the stimulated radiation being circularly polarized in the reverse sense) than it is when the incident light is linearly polarized. Despite saturation, sufficient amplification exists in the former case to allow the efficient conversion of incident to stimulated Rayleigh light at moderate power levels.

DOI
10.1103/physrev.164.200

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Journal of the Optical Society of America B•Jan 1, 1995•8 citations
The phenomenon of stimulated Rayleigh-wing scattering in anisotropic molecular liquids is analyzed. Representative combinations of polarization for the incident and scattered light are considered. It is shown that in regions where the focused laser beam is intense, saturation occurs in the molecular response to external optical fields, in that perfect alignment of the individual liquid molecules in the optical fields is approached. Accordingly, the nonlinear amplification associated with the stimulated radiation is reduced. The results of the analysis qualitatively explain several important recent observations which are in conflict with previous theroretical predictions. For example, it is shown that the nonlinear gain is considerably greater when the incident light is circularly polarized (the stimulated radiation being circularly polarized in the reverse sense) than it is when the incident light is linearly polarized. Despite saturation, sufficient amplification exists in the former case to allow the efficient conversion of incident to stimulated Rayleigh light at moderate power levels.
A theoretical study of the polarization dependence of stimulated Rayleigh-wing scattering and the optical-frequency Kerr effect has been undertaken. When the incident light is circularly polarized, a striking difference in gain is found for the co- and counter-rotating senses of polarization of the scattered light---the former being suppressed and the latter being exceptionally favored. The analysis begins with a model for the Kerr effect, which involves the alignment of anisotropic molecules in an electric field, but the results can be immediately generalized to any light scattering process of tensor symmetry. The nonlinear problem of the propagation of an intense elliptically polarized light wave in a Kerr-active medium is shown to have a solution in which the vibrational ellipse undergoes self-precession and self-retardation. The stimulated scatterings or instabilities of such a self-precessing and self-retarding light wave are obtained for the backward and forward directions. Birefringence, optical activity, and linear and circular dichroisms are some of the phenomena which result, but the forward direction yields substantially different results from the backward direction because of Stokes-anti-Stokes coupling.
Stimulated scattering is a nonlinear process that often results in the generation of a backwardgoing signal. This signal is known to display several unique and interesting properties; perhaps the most notable is phase conjugation. Stimulated Rayleigh-wing scattering (SRWS)1'2 is the stimulated scattering process arising from the optical Kerr effect, and it possesses an extremely fast response time (2 ps in CS2). Under certain experimental conditions, SRWS is known to conjugate both the phase and polarization of an incident field.3 The optical Kerr effect also leads to an intensity-dependent refractive index and is often the dominant contribution to this effect. With a large nonlinear index change, several undesirable effects, such as self-focusing and filamentation,Stimulated scattering is a nonlinear process that often results in the generation of a backwardgoing signal. This signal is known to display several unique and interesting properties; perhaps the most notable is phase conjugation. Stimulated Rayleigh-wing scattering (SRWS)1'2 is the stimulated scattering process arising from the optical Kerr effect, and it possesses an extremely fast response time (2 ps in CS2). Under certain experimental conditions, SRWS is known to conjugate both the phase and polarization of an incident field.3 The optical Kerr effect also leads to an intensity-dependent refractive index and is often the dominant contribution to this effect. With a large nonlinear index change, several undesirable effects, such as self-focusing and filamentation, occur as an intense optical wave propagates through a nonlinear medium.4
The stimulated line of the Rayleigh wing (SLRW) was studied with circularly polarized light from a giant-pulse ruby laser focused into nitrobenzene. The dependence of the observed frequency shift at high input power on the distance of the focus from the entrance window reported previously was confirmed. At low power the shift is constant regardless of position, consistent with existing theory. For intermediate power a complex spectrum is observed. The simultaneous observation of self-focusing and the SLRW provided an impetus for the modification of the theory to include both phenomena. Experiments were performed to test the predicted absorption dependence. Experimental results indicate substantial agreement.
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.
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.
Backward stimulated Rayleigh-wing scattering as a result of simultaneous introduction of two beams, a pump and a probe, in CS2 has been observed. The dependence of this scattering on delay times, angle, and polarization states was measured. A novel phenomenon consisting of the geometric deviation of the scattered beam from its previous backward direction when a weak probe beam is added to the pump beam has been explained by consideration of the large bandwidth scattering in the spectrum. Frequency displacement and simultaneous amplification were observed.