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Physical Review Letters

Spectral Narrowing in Coherent Rayleigh Scattering

Henry T. Bookey, Mikhail N. Shneider, P. F. Barker

Published Sep 26, 2007• 18 citations
Publisher

Abstract

Spectral narrowing of the coherent Rayleigh scattering line shape in a room temperature ${\mathrm{CO}}_{2}$ gas ($2.5\ifmmode\times\else\texttimes\fi{}{10}^{23}\text{ }\text{ }{\mathrm{m}}^{\ensuremath{-}3}$) with intense fields in the ${10}^{15}\text{ }\text{ }\mathrm{W}\text{ }{\mathrm{m}}^{\ensuremath{-}2}$ range is observed. The line shape saturates to a width of approximately half that observed at low pump intensities and indicates a transition from scattering primarily from untrapped molecules to that from both trapped and untrapped molecules that are localized by the deep (60 K) optical potentials produced by the pump beams. At higher densities ($5\ifmmode\times\else\texttimes\fi{}{10}^{24}\text{ }\text{ }{\mathrm{m}}^{\ensuremath{-}3}$), collisions between the trapped and untrapped molecules broaden the spectral profile.

DOI
10.1103/physrevlett.99.133001

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We study the spectral profile of Rayleigh scattered light from molecular species trapped in optical lattices created by strong fields in the ${10}^{16}\text{ }\text{W}\text{ }{\text{m}}^{\ensuremath{-}2}$ range. We show that, for lattices with well depths on the order of 100 K, the motional sidebands imparted on spectra are shifted from the central Dicke-narrowed Rayleigh peak by hundreds of MHz. Our calculations for these short duration (30 ns) lattices show that these spectral features appear even in room temperature gases suggesting a new technique for measuring gas composition based on the frequency offset of the sidebands. Finally, we study the role of field-induced molecular alignment within the lattice and calculate its effect on the shape and position of the sidebands.
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.
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.
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 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.
We observe spectral hole burning in a room-temperature optical fiber pumped by a spectrally broadened pump beam. This beam drives the stimulated Brillouin process, creating an inhomogeneously broadened resonance in the material whose shape can be engineered by tailoring the beam's spectrum. A monochromatic saturating beam "burns" a narrow spectral hole that is approximately 10(4) times narrower than the inhomogeneous width of the resonance. This research paves the way toward agile optical information processing and storage using standard telecommunication components.