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Physical Review Letters

Observation of Radiative Collisional Fluorescence

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

Published Dec 18, 1978• 23 citations
Publisher

Abstract

We report the observation of spontaneous radiative emission during the collision of two excited Ba atoms. The emission occurs at the sum energy of the excited atoms and is the emission analog of the laser-induced inelastic collision process. We measure a collision cross section for deexcitation by spontaneous radiative emission of 2.6\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}20}$ ${\mathrm{cm}}^{2}$.

DOI
10.1103/physrevlett.41.1709

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We report the observation of spontaneous radiative emission during the collision of two excited Ba atoms. The emission occurs at the sum energy of the excited atoms and is the emission analog of the laser-induced inelastic collision process. We measure a collision cross section for deexcitation by spontaneous radiative emission of 2.6\ifmmode\times\else\texttimes\fi{}10\ensuremath−20{10}^{\ensuremath{-}20}10\ensuremath−20 cm2{\mathrm{cm}}^{2}cm2.
Observations are made of dipole-quadrupole laser-induced inelastic collisions occurring during the collision of two Ba atoms. Results for both stimulated-absorption and spontaneous-emission experiments using the same collisional configuration are reported for the first time. In both experiments the interaction maximizes at the $R=\ensuremath{\infty}$ wavelength and has a full-width-at-half-maximum linewidth of \ensuremath{\sim}8 ${\mathrm{cm}}^{\ensuremath{-}1}$. These results bear on the study of the interatomic potentials for colliding atoms and permit the collisional energy transfer to states hitherto inaccessible to dipole-dipole collisions.
Energy-pooling collisions between low-lying excited states of Ba have been studied. We have used a CW dye laser to excite the level in Ba. Radiative decay and collisions with Ba or buffer-gas atoms (Ar, He) populate also the , and metastable levels. The spatial density distributions of these excited levels were measured by the absorption of lines from a Ba hollow-cathode lamp as a function of laser frequency. When the laser was on the exact atomic resonance we observed fluorescence from the , , , , , , and states populated by energy-pooling collisions of Ba( , ). By changing the buffer gas pressure the fluorescence intensity ratio between - and - transitions changes dramatically. This is found to be due to redistribution of population among metastable levels, both in magnitude and space. In addition, we have found that the and metastable levels are also populated when the laser is tuned to the blue from the 553.5 nm line under which conditions a pronounced red-shifted light cone (cone emission) is observed.
A theory is given of radiative collisions, i.e., of elementary events in which the emission of a photon occurs in the course of a collision. Special attention is paid to radiative collisions stimulated by a laser field. Simple but clear approaches formulated in the forties or fifties are described briefly. This theory applies, in particular, to collisions in a strong electromagnetic field which affect the collision dynamics. Chemical radiative collisions, i.e., chemical reactions stimulated by photons absorbed in the course of a collision, are reviewed. An analysis is made of several recent experiments in which the theoretically predicted effects were observed: these include the radiative-collisional transfer of excitation from atom to atom, nonlinear effects due to the influence of the field on the collision dynamics, and photosubstitution of one of the atoms in a halogen molecule with an inert gas atom.