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Physical Review A

Collisions of rubidium Rydberg-state atoms with ammonia

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

Published Jan 1, 1986• 20 citations
Publisher

Abstract

Total depopulation cross sections of Rb(ns) and Rb(nd) levels by collisions with ${\mathrm{NH}}_{3}$ 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 ${\mathrm{NH}}_{3}$ 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 ${\mathrm{NH}}_{3}$) is questionable from a theoretical point of view.

DOI
10.1103/physreva.33.143

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•Jan 1, 1980•0 citations
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.
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).
This paper reports the measurement of the depopulation cross sections of the Rb(ns) and Rb(nd) states by ND3{\mathrm{ND}}_{3}ND3​ (23\ensuremath{\le}n\ensuremath{\le}50). The experimental data are discussed with reference to previous work done on collisions between Rb(ns) and Rb(nd) states and NH3{\mathrm{NH}}_{3}NH3​.
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 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 nnn-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 lll-mixing processes is less efficient. The agreement between experimental and theoretical values is quite satisfactory.
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.
In thermal collisions between Xe(nf) Rydberg atoms and NH(,3) collisional depopulation of the nf state occurs through at least three distinct mechanisms: n-changing collisions, l-changing collisions, and ionizing collisions. Using selective field ionization, the total collisional depopulation rate constants k(,d) are measured for laser-excited Xe(nf) atoms in the n range of 22 to 39. The magnitudes of k(,d) are large, corresponding to reaction cross sections comparable to the geometric size of the Xe(nf) atom at n = 22. In the n range of 25 to 40, Xe('+) ion production provides an absolute measure of the rate constants for collisional ionization. Approximate rate constants for n-and l-changing collisions are also presented for the 31f state. In these experiments, one finds that the state-changing collision rate constants are fairly independent of n and are determined largely by the l-changing collisions. The collisional ionization rate constants measured are smaller than the state-changing rate constants and increase with increasing n, ranging between 0.2 and 4.6 x 10('-7) cm('3)/sec for n between 25 and 40. The present results are compared to those of recent theoretical calculations.