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Physical Review A

Coherent Rayleigh-Brillouin scattering in molecular gases

Xingguo Pan, Mikhail N. Shneider, Richard B. Miles

Published Mar 22, 2004• 144 citations
Publisher

Abstract

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.

DOI
10.1103/physreva.69.033814

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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.
Molecular nitrogen at 0.8 atm and 300 and 500 K and methane at 0.8 atm and 300 K were subjected to optical lattices formed by narrow-band 532-nm laser pulses with intensities on the optical axis near, but below, the gas ionization limit. A third pulse was introduced to experimentally probe the response, as a function of the lattice velocity, of the gas to the deep monochromatic potential wells formed by the lasers. Coherent Rayleigh-Brillouin scattering (CRBS) line shapes were recorded and compared to numerically predicted magnitudes of the density perturbations induced in the gas. Both experimental results and those from direct simulation Monte Carlo simulations show a deviation from previously published low-intensity CRBS line-shape models. The deviation indicates a trend, as a function of lattice velocity, similar to that relating to previously published energy and momentum transfer calculations for high-intensity lattices. Furthermore, the deviation indicates a maximum intensity at which current CRBS theory is valid.
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.
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.
The effect of mixing two high-power ruby-laser beams in several gases has been investigated by means of light scattering. Coherently scattered light has been observed with intensities of up to three orders of magnitude, exceeding that of incoherent Rayleigh scattered light. The dependence of the effect on laser power, gas density, and refractive index is described. It is shown that for higher pressures (\ensuremath{\sim} 100 Torr) a threshold power exists for the effect, and that saturation is observed with increasing pressure as well as increasing mixing beam power.
Equations of a semiclassical model of superradiant Rayleigh scattering of high-intensity short light pulses from a Bose-Einstein condensate of dilute atomic gases are solved numerically taking into account the excitation of atoms by coherent Rayleigh radiation and their recoil in the backward direction. The evolution of the populations of coherent atomic states with a particular momentum is studied, and the pulse shape and the structure of the spectrum of such scattering are found in relation to the laser beam intensity and the recoil kinetic energy of atoms.