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Journal of Physics B Atomic and Molecular Physics

Laser-induced energy transfer and radiative collisions

P. L. Knight

Published Apr 21, 1977• 24 citations
Publisher

Abstract

A theory of the dynamics of radiative collisions is presented in which the laser-induced energy transfer is described by a dipole-dipole interaction between non-identical atoms compounded with stimulated absorption to a further excited level of the acceptor during the collisional interaction.
DOI
10.1088/0022-3700/10/6/003

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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.
The authors introduce a model for radiative collisions which allows one to obtain a simple analytical expression for the transition probability. This model basically consists of an improvement to the Landau-Zener model, in order to obtain a more realistic representation of the Hamiltonian of the system throughout the collision. They apply the results to the problem of radiative collisions when the dipole-dipole interaction is responsible for the energy transfer and obtain an analytical expression for the cross section as a function of the frequency and intensity of the laser field. Their results are compared with experimental results and reasonable agreement is obtained.
The transfer of energy from the translational to the internal degrees of freedom or vice versa is analyzed for radiatively assisted inelastic collisions among atoms in a gas. For a specific atomic-level configuration, it is shown that the absorption of a laser photon may induce a transition between two levels that are displaced by the collisional interaction (a dipole-dipole potential in this treatment) if a fraction of the kinetic energy of the atomic relative motion is simultaneously absorbed. The process thus results in a cooling of the atomic kinetic temperature. In other level configurations, energy goes in the opposite direction, with a heating of the kinetic temperature. This mechanism is described by means of the Wigner-function formalism, which allows a passing to the quasiclassical limit for the atomic motion in a simple way.
The collision-induced absorption and emission coefficients for electric-dipole forbidden atomic transitions are calculated for weak radiation fields. The approximations used are valid for $\ensuremath{\hbar}\ensuremath{\omega}$ near $\ensuremath{\hbar}{\ensuremath{\omega}}_{0}$, the atomic energy differences. The example case of $S\ensuremath{-}D$ transitions induced by a spherically symmetric perturber (e.g., a noble-gas atom) is treated in detail and compared to measurements. The case of "radiative collisions," in which both colliding atoms change their state, is included in the theory and is also compared to experiment.
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.