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Physical Review Letters

Stimulated Thermal Rayleigh Scattering in Gases

T. A. Wiggins, C. W. Cho, D. R. Dietz, N. D. Foltz

Published Apr 15, 1968• 35 citations
Publisher

Abstract

Stimulated thermal Rayleigh scattering that has been seen previously in absorbing liquids has been observed in gaseous nitrogen and carbon dioxide using small amounts of N${\mathrm{O}}_{2}$ and ${\mathrm{I}}_{2}$ to produce absorption. The anti-Stokes shift of half the half-intensity width of the incident light, thresholds, gain narrowing, and critical absorption coefficients were observed.

DOI
10.1103/physrevlett.20.831

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Physical Review•Dec 5, 1967•16 citations
Stimulated thermal Rayleigh scattering that has been seen previously in absorbing liquids has been observed in gaseous nitrogen and carbon dioxide using small amounts of NO2{\mathrm{O}}_{2}O2​ and I2{\mathrm{I}}_{2}I2​ to produce absorption. The anti-Stokes shift of half the half-intensity width of the incident light, thresholds, gain narrowing, and critical absorption coefficients were observed.
Using well defined input pulses the amplification by stimulated thermal Rayleigh scattering was investigated experimentally as a function of time (within the pulse), of absorption coefficient, and of interaction length. The frequency difference between the two interacting light pulses was varied with an accuracy better than Δν/ν = 10-8. Amplification was measured in the backward direction and at several degrees from the forward direction. The various experimental observations are in good agreement with theory. The possibility of determining material parameters in this amplifier system is discussed
The use of stimulated light scattering as a means for achieving optical control functions directed toward an optical computer is described. Stimulated thermal Rayleigh scattering is seen to be a preferred nonlinear optical mechanism when compared with the more familiar stimulated Raman and stimulated Brillouin scattering. It possesses the highest gain, the lowest threshold, and scattered radiation which is approximately the same frequency as the inducing radiation. Optical control functions such as optical bistable switching, optical amplification and optical limiting or clipping are described.
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.
Abstract : Preliminary experiments were conducted whose ultimate goal is to develop all-optical control functions useful in an all-optical or optical- electronic hybrid digital computer or for optical interconnects. Stimulated thermal Rayleigh scattering (STRS) based upon generator experiments was pursued for scattering angles of 90 deg and 180 deg (backscattering). A pulsed nitrogen laser pumped dye laser served as the radiation source and the interaction medium was a liquid to which an absorbing dye was added. STRS amplifier experiments were successful and gain was observed and studied parametrically using eosine dye in ethanol. The gain was found to increase (although the gain coefficient decreased) with increasing pump power and the gain was found to be a maximum at an absorption coefficient of about 2.6 per cm. The generator experiments did not lead to stimulated scattering due to the limited output power of the laser and its multi-longitudinal spectral mode content. These studies will be continued along with analytical modeling in order to characterize the interaction and to enable the optimization of the scattering process.
The use of stimulated light scattering as a means for achieving optical control functions directed toward an optical computer is described. Stimulated thermal Rayleigh scattering is seen to be a preferred nonlinear optical mechanism when compared with the more familiar stimulated Raman and stimulated Brillouin scattering. It possesses the highest gain, the lowest threshold, and scattered radiation that is approximately the same frequency as the inducing radiation. Optical control functions such as optical bistable switching, optical amplification, and optical limiting or clipping are described.
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.