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Physical Review A

Depopulation of rubidium Rydberg states by CO molecules: An experimental and theoretical study

L. Petitjean, F. Gounand, P. R. Fournier

Published Jul 1, 1984• 31 citations
Publisher

Abstract

The quenching cross sections of highly excited Rb $ns(25\ensuremath{\le}n\ensuremath{\le}45)$ and Rb $nd(23\ensuremath{\le}n\ensuremath{\le}44)$ states by CO, a weak polar molecule, are measured, and these experimental data are compared to theoretical predictions where the main process responsible for the quenching is taken to be the Rydberg-electron-CO interaction. It is shown that the long-range Rydberg-electron-molecular-dipole interaction is often dominant leading mainly to $n$-changing and, to a lesser extent, to Rydberg ionization via quasiresonant molecular rotational transitions. It is also shown that the Rydberg-${e}^{\ensuremath{-}}$ ---molecular-quadrupole interaction is negligible and the short-range interaction leading to $l$-mixing processes is less efficient. The agreement between experimental and theoretical values is quite satisfactory.

DOI
10.1103/physreva.30.71

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The quenching cross sections of highly excited Rb ns(25\ensuremath≤n\ensuremath≤45)ns(25\ensuremath{\le}n\ensuremath{\le}45)ns(25\ensuremath≤n\ensuremath≤45) and Rb nd(23\ensuremath≤n\ensuremath≤44)nd(23\ensuremath{\le}n\ensuremath{\le}44)nd(23\ensuremath≤n\ensuremath≤44) states by CO, a weak polar molecule, are measured, and these experimental data are compared to theoretical predictions where the main process responsible for the quenching is taken to be the Rydberg-electron-CO interaction. It is shown that the long-range Rydberg-electron-molecular-dipole interaction is often dominant leading mainly to nnn-changing and, to a lesser extent, to Rydberg ionization via quasiresonant molecular rotational transitions. It is also shown that the Rydberg-e\ensuremath−{e}^{\ensuremath{-}}e\ensuremath− ---molecular-quadrupole interaction is negligible and the short-range interaction leading to lll-mixing processes is less efficient. The agreement between experimental and theoretical values is quite satisfactory.
The total depopulation cross sections by N2{\mathrm{N}}_{2}N2​ of high rubidium Rydberg states, $\mathrm{Rb}(\mathrm{ns}) (n=25\ensuremath{-}46)$ and $\mathrm{Rb}(\mathrm{nd}) (n=23\ensuremath{-}44)$, have been measured using time-resolved field ionization technique and compared to previous results obtained on the quenching of Rb(nl)\mathrm{Rb}(\mathrm{nl})Rb(nl) by CO. It is shown that the Rb(nl)\mathrm{Rb}(\mathrm{nl})Rb(nl) depopulation by N2{\mathrm{N}}_{2}N2​ is much less efficient than the Rb(nl)\mathrm{Rb}(\mathrm{nl})Rb(nl) depopulation by CO and leads mainly to the quasielastic process of angular momentum mixing via the short-range interaction between the quasifree Rydberg-state electron and the molecule. It is clearly demonstrated that the presence of a permanent dipole in CO changes the collisional processes drastically. The agreement between experimental and theoretical predictions based on the impulse approximation is quite satisfactory.
The cross sections for the quenching of highly excited Rb(nS) (32<or=n<or=45) and Rb(nD) (30<or=n<or=41) states have been measured for the different rare gases. In most cases studied, the quenching cross sections seem rather constant or slightly decreasing with n for a given series and a given rare gas. The experimental data are compared with the results of calculations using various theoretical approaches. It is shown that in this range of large n values the main process responsible for the quenching is the Rydberg-electron-rare-gas interaction, as previously stated for lower n values (10<or=n<or=20).
Total depopulation cross sections of Rb(ns) and Rb(nd) levels by collisions with NH3{\mathrm{NH}}_{3}NH3​ have been measured over a wide range of n values (24\ensuremath{\le}n\ensuremath{\le}49). The analysis of the n-dependent behavior of the cross sections reveals that NH3{\mathrm{NH}}_{3}NH3​ inversion can produce a very efficient l-mixing process via a quasiresonant mechanism. This behavior appears qualitatively well described by theoretical calculations based on the impulse approximation (IA). A quantitative comparison between theory and experiment appears difficult, but it seems that the IA should provide reasonable estimates (within a factor of 4), though its use for large dipole moment (1.47 D for NH3{\mathrm{NH}}_{3}NH3​) is questionable from a theoretical point of view.
Electron-transfer processes are studied in thermal collisions of Rydberg atoms with alkaline-earth Ca(4s 2), Sr(5s 2), and Ba(6s 2) atoms capable of forming negative ions with a weakly bound outermost p-electron. We consider the ion-pair formation and resonant quenching of highly excited atomic states caused by transitions between Rydberg covalent and ionic terms of a quasi-molecule produced in collisions of particles. The contributions of these reaction channels to the total depopulation cross section of Rydberg states of Rb(nl) and Ne(nl) atoms as functions of the principal quantum number n are compared for selectively excited nl-levels with l ≪ n and for states with large orbital quantum numbers l = n − 1, n − 2. It is shown that the contribution from resonant quenching dominates at small values of n, and the ion-pair formation process begins to dominate with increasing n. The values and positions of the maxima of cross sections for both processes strongly depend on the electron affinity of an alkaline-earth atom and on the orbital angular momentum l of a highly excited atom. It is shown that in the case of Rydberg atoms in states with large l ∼ n − 1, the rate constants of ion-pair formation and collisional quenching are considerably lower than those for nl-levels with l ≪ n.
Abstract The results of theoretical studies of the resonant quenching and ion-pair formation processes induced by collisions of Rydberg atoms with highly polar molecules possessing small electron affinities are reported. We elaborate an approach for describing collisional dynamics of both processes and demonstrate the predominant role of resonant quenching channel of reaction for the destruction of Rydberg states by electron-attaching molecules. The approach is based on the solution of the coupled differential equations for the transition amplitudes between the ionic and Rydberg covalent terms of a quasimolecule formed during a collision of particles. It takes into account the possibility of the dipole-bound anion decay in the Coulomb field of the positive ionic core and generalizes previous models of charge-transfer processes involving Rydberg atoms to the cases, when the multistate Landau–Zener approaches become inapplicable. Our calculations for Rb ( nl ) atom perturbed by C 2 H 4 SO 3 , CH 2 CHCN , CH 3 NO 2 , CH 3 CN , C 3 H 2 O 3 , and C 3 H 4 O 3 molecules show that the curves representing the dependence of the resonant quenching cross sections on the principal quantum number n are bell-shaped with the positions of maxima being shifted towards lower values of n and the peak values, σ max ( q ) , several times higher than those for the ion-pair formation, σ max
The cross sections for quasi-elastic and inelastic collisional processes between rubidium in non-hydrogenic Rydberg nS and nD states and helium have been measured. The quenching cross section of the Rydberg levels seems to behave similarly for different series, it first increases with n and then reaches a maximum, which is more or less shifted towards low n values, depending on the proximity of the highly degenerate hydrogenic neighbouring levels. The authors' experimental results and those previously obtained are in fair agreement (within a factor of 3 in the worst cases) with the values computed using a simple theoretical approach only taking into account the Rydberg electron-helium interaction.