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Physica B+C

Collision and Doppler broadening of fluorescence and Raman scattering from atoms

Gerard Nienhuis, F. Schuller

Published Nov 1, 1977• 10 citations
Publisher
DOI
10.1016/0378-4363(77)90139-5

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We have observed collisional redistribution of laser light scattered by a three-level atom, thallium, in the presence of argon. The two observed spectral components correspond to Raman scattering and collision-induced fluorescence. We have seen the growth of both components from spontaneous to stimulated scattering as the laser intensity is increased. While the gain for the Raman component agrees with theory, the observed gain of the collision-induced fluorescence is over an order of magnitude lower than predicted.

Physical Review Letters•Nov 21, 1977•39 citations
The resonant scattering of monochromatic light in gases is analyzed. Explicit expressions for the differential cross section are obtained in the limits (Doppler width) \ensuremath{\gg} (natural width) \ensuremath{\gg} (collision width) and (collision width) \ensuremath{\gg} (natural width) \ensuremath{\gg} (Doppler width). In the former limit, the frequency distribution of scattered light is narrowed in the forward and backward directions, and has the full absorption width for right-angle scattering. In the collision-dominated limit, the cross section separates into a coherent and a fluorescent component. The motion of the atoms broadens the $\ensuremath{\delta}$ function distribution characterizing coherent scattering from a stationary target. The interference between light scattered by different atoms is assessed.
The influence of phase memory effects on the spectrum of resonance Raman scattering by three-level atoms with the Λ configuration of levels experiencing collisions with buffer gas atoms in a strong monochromatic radiation field is studied theoretically. Systems with a small Doppler broadening compared to the collision frequency (large buffer gas pressures) are analysed in the general case of an arbitrary change (from complete change to complete preservation) in the phase memory at any of three transitions in the Λ system. It is shown that in the absence of the collision relaxation of the low-frequency coherence at the transitions between two lower levels of the Λ system, the radiation scattering spectrum has a spectrally narrow component at the Raman frequency, which, despite the homogeneous broadening of the absorption line, exhibits a strongly pronounced anisotropy. In the direction, close to the propagation direction of exciting radiation, this line maximally narrows down. It is significant that upon optical pumping to the level unaffected by a strong field the resonance Raman spectrum noticeably differs from the spectrum in the case of the probe field. A simple expression is proposed for calculating the degree of the phase memory preservation in collisions from the relative amplitude of the Raman resonance.
We have observed collisional redistribution of laser light scattered by a three-level atom, thallium, in the presence of argon. The two observed spectral components correspond to Raman scattering and collision-induced fluorescence. We have seen the growth of both components from spontaneous to stimulated scattering as the laser intensity is increased. While the gain for the Raman component agrees with theory, the observed gain of the collision-induced fluorescence is over an order of magnitude lower than predicted.