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Physical Review A

Collisional depopulation of rubidium Rydberg states by ND3

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

Published Feb 1, 1986• 9 citations
Publisher

Abstract

This paper reports the measurement of the depopulation cross sections of the Rb(ns) and Rb(nd) states by ${\mathrm{ND}}_{3}$ (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 ${\mathrm{NH}}_{3}$.

DOI
10.1103/physreva.33.1372

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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.
We have measured total cross sections for the collisional depopulation of high-lying nP\mathrm{nP}nP states ($12\ensuremath{\le}n\ensuremath{\le}22$) of rubidium induced by thermal collisions with ground-state rubidium or rare-gas atoms. It is observed that for $n\ensuremath{\ge}14$ the rubidium-rare-gas cross sections do not vary with the principal quantum number, contrary to previous hypotheses. Our results are discussed using the simple argument of quasifree behavior of the valence electron involving either an elastic-scattering or a binary-encounter approach. However, the disagreement observed between the experimental and the computed cross sections suggests that a three-body approach is generally needed for a good understanding of collisional processes involving highly excited states.
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.
This paper reports a study of collisions between Rb atoms in ns\mathrm{ns}ns, np\mathrm{np}np, and nd\mathrm{nd}nd states (27< n< 7027<~n<~7027< n< 70) and Xe. The experimental data show that collisions result in transitions from the initial level to states in adjacent high-lll manifolds and that, at the lower values of nnn, there are significant differences in the cross sections for such state-changing processes for ns\mathrm{ns}ns, np\mathrm{np}np, and nd\mathrm{nd}nd states. These differences are discussed with reference to the amount of energy transfer in the collisions, and the data are compared with recent Born-approximation calculations.
In thermal-energy collisions between sodium atoms in ns\mathrm{ns}ns or np\mathrm{np}np states (32< n< 5232<~n<~5232< n< 52) and xenon atoms, depopulation of the Rydberg states is observed to occur predominantly through state-changing reactions of the type $\mathrm{Na}(ns or np)+\mathrm{Xe}\ensuremath{\rightarrow}\mathrm{Na}(n\ensuremath{-}1, l>~2)+\mathrm{Xe}$. For the present range of nnn, the measured cross sections increase with nnn and lie between 1500 and 2600 A˚2{\mathrm{\AA{}}}^{2}A˚2 for ns\mathrm{ns}ns states and between 2000 and 4200 A˚2{\mathrm{\AA{}}}^{2}A˚2 for np\mathrm{np}np states. Implications of the data are discussed.