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Physical Review Letters

Spectral Narrowing in Coherent Rayleigh-Brillouin Scattering

A. Manteghi, Nico J. Dam, A. S. Meijer, Astrid Silvia de Wijn, Willem van de Water

Published Oct 18, 2011• 12 citations
Publisher

Abstract

Coherent Rayleigh-Brillouin scattering is a four-wave mixing technique that provides information on various physical properties of the scattering medium in the spectral domain. Being based on density gratings generated by dipole forces, the method requires two pump beams of sufficient spectral width to span the full response bandwidth of the scattering medium. We provide experimental data on the scattered spectrum as a function of the coherence between the two pump beams and derive the corresponding pump beam spectrum. We argue that all experiments on coherent Rayleigh-Brillouin scattering to date, have, in fact, been performed in the incoherent regime and show that orders of magnitude in scattering efficiency are to be expected when the experiments are performed with bandwidth-limited picosecond laser pulses.

DOI
10.1103/physrevlett.107.173903

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Coherent Rayleigh-Brillouin scattering is a four-wave mixing technique that provides information on various physical properties of the scattering medium in the spectral domain. Being based on density gratings generated by dipole forces, the method requires two pump beams of sufficient spectral width to span the full response bandwidth of the scattering medium. We provide experimental data on the scattered spectrum as a function of the coherence between the two pump beams and derive the corresponding pump beam spectrum. We argue that all experiments on coherent Rayleigh-Brillouin scattering to date, have, in fact, been performed in the incoherent regime and show that orders of magnitude in scattering efficiency are to be expected when the experiments are performed with bandwidth-limited picosecond laser pulses.
We measure the spectrum of coherent Brillouin scattering (CBS) in a gas as a function of time and observe for the first time additional spectral sidebands and line shape narrowing of the Brillouin peak. We find that both effects result from the interference of the density modulation induced by the moving dipole force of the pump beams with the acoustic waves induced by their fast thermalization and are predicted by a hydrodynamic-light scattering model. These line shapes differ from both spontaneous and stimulated Brillouin scattering spectra and also from previous coherent Rayleigh-Brillouin measurements.
We present an experimental and theoretical study of the coherent Rayleigh-Brillouin scattering in gases in the kinetic regime. Gas density perturbation waves were generated by two crossing pump laser beams through optical dipole forces. A probe laser beam was then coherently scattered from the perturbation waves. The line shape of the scattered light was modeled using kinetic theory. The model takes into account the internal energy modes of the gas particles and is applicable to both molecular and atomic gases. We discuss the implication of coherent Rayleigh-Brillouin scattering on kinetic theory and photon matter interaction.
Steady-state stimulated Rayleigh-Brillouin gain spectroscopy and its application are reported. The stimulated gain, which is derived in terms of the spectral function of density fluctuations, is shown to approach, in the limit of zero density, the gain derived from the individual-particle picture of Rayleigh scattering. Using a pulsed pump laser, experimental gain spectra of pure SF6{\mathrm{SF}}_{6}SF6​, pure Ar, and a SF6{\mathrm{SF}}_{6}SF6​- and He-gas mixture are obtained and explained. Other associated coherent Rayleigh-Brillouin spectroscopies and the possibility of using a cw pump laser for higher spectral resolution are discussed.
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.
Single-shot coherent Rayleigh-Brillouin scattering (CRBS) is modeled using direct simulation Monte Carlo (DSMC). In CRBS, an optical lattice generated by the interference of two pump lasers traps the neutral particles via the dipole force. The gradient of refractive index due to the trapped particles of the gaseous media leads to coherent scattering of a probe beam, resulting in the CRBS signal. Additionally, using a chirped laser beam, CRBS signals can be obtained in a single laser shot, shortening the measurement time of the gas flow (on the order of 100 ns). The DSMC results of single-shot CRBS assuming Maxwellian velocity distribution functions (VDFs) show good agreement with experimental data, including argon, carbon dioxide, and xenon, for different gas pressures. One of the key observations obtained from the present simulations is that the CRBS signals become asymmetric when using a fast chirp rate due to finite time for collisionless trapping and collisional thermalization. Published by the American Physical Society 2024
Forced light scattering using broad-bandwidth incoherent pump light (${\ensuremath{\lambda}}_{\mathit{B}}$=508 nm, full width at half maximum \ensuremath{\Delta}${\ensuremath{\lambda}}_{\mathit{B}}$=13.8 nm), and narrow-bandwidth probe light is investigated experimentally and compared with self-diffraction. Forced light scattering improves the dynamic range of measurement by an order of magnitude compared to self-diffraction. A theoretical analysis of this scheme is presented. The technique is used to measure the dephasing kinetics of solutions of crystal violet and bis-(dimethylamino)heptamethine. Resulting from the relatively large autocorrelation time of 40 fs, the experimental signals show no influence from inhomogeneous broadening of the absorption bands; the dephasing kinetics can be characterized by a dephasing time T2{\mathit{T}}_{2}T2​\ensuremath{\approxeq}10 fs and an intrinsic correlation time ${\mathrm{\ensuremath{\tau}}}_{\mathit{C}}$\ensuremath{\approxeq}30 fs with a weak modulation (center frequencies ranging from 800 to 1200 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$), which is attributed to a coherent motion of the molecule (vibration). The dephasing kinetics of crystal violet shows a close agreement with the dephasing kinetics of malachite green previously reported for two-pulse photon echoes with ultrashort pulses [P. C. Becker et al., Phys. Rev. Lett. 63, 505 (1989)].