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Physical Review A

Stimulated Rayleigh-Bragg scattering in two-photon absorbing media

Guang S. He, Changgui Lü, Qingdong Zheng, Paras N. Prasad, Petros Zerom, Robert W. Boyd, Marek J. Samoc

Published Jun 17, 2005• 25 citations
Publisher

Abstract

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.

DOI
10.1103/physreva.71.063810

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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.
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.
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.
We show that the backward-stimulated Rayleigh-Bragg scattering (SRBS) can be efficiently generated in a three-photon absorbing medium. Compared with all other known stimulated (such as Brillouin and Raman) scattering effects, the observed effect exhibits the following three features: (i) no frequency shift, (ii) a lower pump threshold, and (iii) no critical requirement for pump spectral linewidths within a range of Δv¯≤1cm−1. The specific nonlinear scattering medium is a three-photon absorbing chromophore solution (PRL-OT04 in chloroform), pumped by 1064nm laser pulses of nanoseconds duration but with three different spectral linewidths. The mechanism for generating backward SRBS in a three-photon active medium is the formation of a stationary Bragg grating enhanced by three-photon-absorption-associated refractive index changes. A superior optical phase-conjugation property of the backward SRBS beam has been experimentally demonstrated by employing two different optical setups. In both cases, a specially introduced aberration influence of 4-5 mrad can be basically removed by the backward SRBS beam that retains a much smaller beam divergence of ≤0.4 mrad.
This work reports the properties of stimulated Rayleigh–Bragg scattering (SRBS) from a two-photon absorbing CdSe–Cds–ZnS quantum-rods (QRs) solution in chloroform, excited by 1064-nm and$\sim$13-ns laser pulses. The two-photon absorbing capability of the scattering medium, as well as the pump threshold, spectral structure, and pulse waveforms of the backward stimulated scattering were measured. Comparing to a pure solvent or an organic dye-solution, the semiconductor QR system has many advantages such as the lower pump threshold, higher energy transfer efficiency, and better photo-physical and photo-chemical stability. The measured output/input characteristic curve shows that the backward SRBS can enhance the optical power limiting performance that is based on two-photon absorption, backward stimulated scattering, and other nonlinear absorption mechanisms. In addition, the backward SRBS beam from our sample medium exhibits a fairly good optical phase-conjugation capability, so that the distortion influence from an inserted aberrator can be automatically removed.
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.
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