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Journal of the Optical Society of America B

Purely refractive transient energy transfer by stimulated Rayleigh-wing scattering

Aristide C. Dogariu, Tiejun J. Xia, David J. Hagan, A. A. Said, Eric W. Van Stryland, N. Bloembergen

Published Apr 1, 1997• 61 citations
Publisher

Abstract

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.

DOI
10.1364/josab.14.000796

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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.
Femtosecond two-beam coupling is demonstrated in N,N′-dimethylformamide and dimethyl sulfoxide by using a time-resolved pump-probe system at a wavelength of 800 nm. As the temporal delay between pulses is varied within the coherence time, transient energy transfer from one pulse to another occurs. Because of the asymmetry of the normalized transmittance, two-photon absorption is considered in the two liquids. A theory based on two-beam coupling in perpendicular linear polarization is used to interpret the experimental results. Good agreement is obtained between the theory and experiment. Moreover, by introducing a valuable variable, the ratio of the relaxation times of the two Kerr liquids is directly characterized.
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.
We examine coherent energy transfer between two circularly polarized degenerate Gaussian laser beams whose pulsewidth is of the order of the medium response time. For this situation, energy transfer proceeds via a phase lag that arises from the finite response time of the nonlinear medium and the pulsed nature of the incident light beams. Locally, this phase lag is driven by the difference in the local intensities of the two laser beams. Previously, we studied the gain as a function of beam delay for the case of a linearly polarized probe and a circularly pump wave, with a large pump to probe intensity radio. Here, we focus on the situation where the beam intensities are equal, both beams are circularly polarized, and CS2 is the nonlinear medium. This polarization configuration allows us to examine more closely the orientational gratings formed by the two light beams as they propagate through the sample.
We have observed transient, coherent beam combination by degenerate two-wave mixing of frequency-doubled Nd:YAG picosecond laser pulses in carbon disulfide, using a circularly polarized pump wave and a linearly polarized probe beam. The important role of beam polarization is observed, and its part in energy transfer is discussed. A theory that treats polarization effects in transient two-wave mixing is presented, applied to the carbon disulfide experiments, and found to be in excellent agreement with the data.
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