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Journal of the Optical Society of America B

Stimulated Rayleigh-wing scattering with two-beam coupling in CS_2

Kokou D. Dorkenoo, D. Wang, Nguyen Phu Xuan, J. P. Lecoq, Roger A. Chevalier, Genevieve Rivoire

Published Jan 1, 1995• 8 citations
Publisher

Abstract

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.

DOI
10.1364/josab.12.000037

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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.
A frequency-unshifted and backward stimulated scattering can be efficiently generated in one-photon-absorption free but two-photon absorbing materials. Using a number of novel two-photon absorbing dye solutions as the scattering media and nanosecond pulsed laser as the pump beams, a highly directional backward stimulated scattering at the exact pump wavelength can be readily observed once the pump intensity is higher than a certain threshold level. The spectral and spatial structures as well as the temporal behavior and optical phase-conjugation property of this new type of backward stimulated scattering have been experimentally studied. This stimulated scattering phenomenon can be explained by using a model of two-photon-excitation enhanced standing-wave Bragg grating initially formed by the strong forward pump beam and much weaker backward Rayleigh scattering beam; the partial reflection of the pump beam from this grating provides an positive feedback to the initial backward Rayleigh scattering beam without suffering linear attenuation influence. Comparing to other known stimulated (Raman, Brillouin, Rayleigh-wing, and Kerr) scattering effects, the stimulated Rayleigh-Bragg scattering exhibits the advantages of no frequency-shift, low pump threshold, and low spectral linewidth requirement.
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
Two-beam coupling is demonstrated in CS2 and other transparent Kerr liquids by use of frequency chirped, picosecond 532-nm-wavelength pulses with several polarization combinations. As the temporal delay between pulses is varied within the coherence time, the first pulse always loses energy while the second pulse gains this energy. The transferred energy at a fixed delay varies linearly with irradiance. The results are consistent with energy transfer from transient refractive gratings that are due to stimulated Rayleigh-wing scattering.
The origin and mechanism of backward stimulated Rayleigh scattering in two-photon absorbing media are studied theoretically and experimentally. This type of stimulated scattering has the unusual features of no frequency shift and low pump threshold requirement compared to all other known stimulated scattering effects. This frequency-unshifted stimulated Rayleigh scattering effect can be well explained by a two-photon-excitation-enhanced Bragg grating reflection model. The reflection of the forward pump beam from this stationary Bragg grating may substantially enhance the backward Rayleigh scattering beam, providing a positive feedback mechanism without causing any frequency shift. A two-counterpropagating-beam-formed grating experiment in a two-photon absorbing dye solution is conducted. The measured dynamic behavior of Bragg grating formation and reflectivity properties are basically consistent with the predictions from the proposed model.
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 frequency-unshifted and backward stimulated Rayleigh scattering can be produced in a linearly transparent but two-photon absorbing medium. Using a novel two-photon active dye solution as the nonlinear medium pumped by 532-nm and ~10-ns laser pulses, a highly directional backward stimulated scattering at the pump wavelength can be readily observed. The experimental results on spectral structure, spatial and temporal behaviors, and output/input relationship of this new type of stimulated scattering are presented. To explain the observed phenomenon and its experimental behaviors, a physical model of feedback mechanism provided by a two-photon-excitation enhanced Bragg grating inside the scattering medium is proposed. Comparing to other types of stimulated scattering, the stimulated Rayleigh-Bragg scattering exhibits the advantages of no-frequency shift, low threshold, and low requirement for pump spectral line-width.