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Two-state models of radiative collisions and related ionization effects. [Cs + Cs; Xe + Ar]

M. G. Payne, Howard C. Baker

Published Jan 1, 1981• 0 citations
OpenAlex

Abstract

A two-state model of processes of the type A(i) + B(i) + N h-bar ..omega.. ..-->.. A(F) + B(F) is presented. A general solution is given to the two-state model within the approximations of straight-line trajectories for the relative nuclear motion and dipole-dipole interatomic interaction. The processes Cs(6s/sub 1/2/) + Cs(6s/sub 1/2/) + 2 h-bar ..omega..(..omega.. approx. 11,455 cm/sup -1/) ..-->.. Cs(6P/sub 3/2/) + Cs(6s/sub 1/2/) and Xe(5p/sup 5/(/sup 2/P/sub 3/2/)6p(3/2)/sub 1/) + h-bar ..omega.. approx. 6177 A + Ar(3p/sup 6/) ..-->.. Xe(5p/sup 6/) + Ar (3p/sup 5/(/sup 2/P/sub 1/2/)4s(1/2)/sub 1/ are discussed as special cases.

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A two-state model of processes of the type A(i) + B(i) + N h-bar ..omega.. ..-->.. A(F) + B(F) is presented. A general solution is given to the two-state model within the approximations of straight-line trajectories for the relative nuclear motion and dipole-dipole interatomic interaction. The processes Cs(6s/sub 1/2/) + Cs(6s/sub 1/2/) + 2 h-bar ..omega..(..omega.. approx. 11,455 cm/sup -1/) ..-->.. Cs(6P/sub 3/2/) + Cs(6s/sub 1/2/) and Xe(5p/sup 5/(/sup 2/P/sub 3/2/)6p(3/2)/sub 1/) + h-bar ..omega.. approx. 6177 A + Ar(3p/sup 6/) ..-->.. Xe(5p/sup 6/) + Ar (3p/sup 5/(/sup 2/P/sub 1/2/)4s(1/2)/sub 1/ are discussed as special cases.
We report on the spectra of the long-range attractive molecular states of the Cs/sub 2/ dimer below the dissociation limits 6s+6p/sub 1/2/ and 6s+6p/sub 3/2/ which are accessible by molecular photoassociation of cold Cs atoms. For the states O/sub u//sup +/ and O/sub g//sup -/(6s+6p/sub 3/2/), we have performed trap-loss measurements, which are in good agreement with the theoretical calculations, performed in a perturbative approach. For the O/sub g//sup -/ and 1/sub u/(6s+6p/sub 3/2/) states, we observe, after spontaneous decay of the electronically excited molecules, the formation of translationally cold molecules. A rate of formation of cold molecules of the order of /spl sim/10/sup 6/ molecules per second is obtained in the case of the state O/sub g//sup $/.
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.
A theoretical treatment of the relaxation and transfer of atomic multipole moments due to interatomic collisions is presented, applicable to systems of emitters and perturbers with any angular momenta. Expressions are obtained for the rate constants, within the impact approximation, in terms of the elements of the scattering matrix evaluated as a function of impact parameter for an emitter-perturber collision. Processes in which the total electronic excitation energy is not conserved are excluded and collisions are assumed to occur isotropically. Explicit evaluation of rate constants has been carried out using the first-order dipole-dipole (resonance) interaction, assuming the classical straight line path approximation. Four special cases have been treated by numerical integration of the Schrodinger equation in the interaction representation. These are: J g (ground state angular momentum)=0, J e (excited state)=1; j g = 1 / 2 , J e = 1 / 2 ; J g = 1 / 2 , J e = 3 / 2 ; J g =1, J e =1. The ( 1 / 2 , 1 / 2 ) rate constants are shown to be simply related to those for the (0, 1) case. Within the context of the various approximations, numerical accuracy is expected to be better than 1%.
An experimental investigation of the Cs 6s {sup 2}S{sub 1/2}{yields}6p {sup 2}P{sub 3/2}{yields}10s {sup 2}S{sub 1/2} double-resonance two-photon polarization spectrum has been made. In the investigation, a linear polarization degree was measured to extract the alignment depolarization cross section in the cesium 6p {sup 2}P{sub 3/2} level due to collisions between ground-level argon and excited 6p {sup 2}P{sub 3/2} cesium atoms over the Zeeman coherences. The spectra show strong depolarization of the Cs 6p {sup 2}P{sub 3/2} level. The measured alignment depolarization cross section value of 186 (58) A{sup 2} is in good agreement with the experiment and theoretical predictions.