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Physical Review Letters

Observation of Radiative Collisional Fluorescence.

J. C. White, G. Zdasiuk, J. F. Young, Stephen E. Harris

Published Feb 12, 1979• 4 citations
Publisher

Abstract

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DOI
10.1103/physrevlett.42.480

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We have measured the time-dependent fluorescence of the sodium DDD lines following pulsed excitation of one DDD line, in the presence of radiation trapping with optical depths k0L{k}_{0}Lk0​L of \ensuremath{\sim}10 to 2000. When collisional coupling of the 3P123{P}_{\frac{1}{2}}3P21​​ and 3P323{P}_{\frac{3}{2}}3P23​​ levels and different radiative-escape probabilities for each DDD line are taken into account, we obtain excellent agreement with Holstein's theory for the effective radiative decay rates in the Doppler region (${k}_{0}L\ensuremath{\sim}10\ensuremath{-}300$) and in the redistributed Lorentzian region (k0L>1000{k}_{0}L>1000k0​L>1000). For k0L{k}_{0}Lk0​L between these two regions, we observe an abrupt transition between the two limiting formulas. The buildup rate of the sensitized fluorescence signal also yields a $3{P}_{\frac{3}{2}}\ensuremath{\rightarrow}3{P}_{\frac{1}{2}}$ excitation transfer cross section in agreement with our previously reported cw measurement. Additionally, we have measured the dependence of the 3P3P3P fluorescence on laser power and beam diameter, and we explain the observed approach to saturation. We suggest that the previously reported "anomalous" approaches to saturation may be explained in terms of the laser beam burning through the optically thick vapor. Laser-beam spatial intensity variations and self-focusing also contribute to fluorescence signals that deviate from the usual single-atom saturation behavior.
The formal structure of the time dependence of the state of an atom in a perturber bath in an intense classical monochromatic radiation field is studied. The authors allow the cross sections of binary collisions to be affected by the radiation field. The result is used to derive an expression for the collision-broadened saturated fluorescence excitation spectrum and absorption rate in terms of a collisional relaxation operator. This operator can be related to the rate of collisionally aided radiative excitation.