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Physical Review Letters

Energy Transfer in Charge Exchange Collisions between Slow Ions and Rydberg Atoms

D. S. Fisher, C. W. Fehrenbach, S. R. Lundeen, Eric A. Hessels, Brett D DePaola

Published Aug 31, 1998• 11 citations
Publisher

Abstract

Charge transfer collisions between slow ions and Rydberg atoms have been studied for ion charges $q\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}1--4$, using resonant laser excitation to detect specific energy states of the collision products. The data collected show a clear resonance in the capture cross section to a particular energy state as the binding energy of the Rydberg target is varied. The resonance position differs significantly from the predictions of the classical overbarrier model, and its width becomes very small (0.025 eV) at the lowest velocities studied.

DOI
10.1103/physrevlett.81.1817

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Charge transfer collisions between slow ions and Rydberg atoms have been studied for ion charges q=1−−4q\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}1--4q=1−−4, using resonant laser excitation to detect specific energy states of the collision products. The data collected show a clear resonance in the capture cross section to a particular energy state as the binding energy of the Rydberg target is varied. The resonance position differs significantly from the predictions of the classical overbarrier model, and its width becomes very small (0.025 eV) at the lowest velocities studied.
Charge-transfer collisions between slow multiply charged ions and highly excited Rydberg atoms have been studied to determine the details of the internal energy transfer accompanying charge exchange. The experiment uses lasers to define uniquely the binding energies of both initial and final states of the collision, thereby eliminating the ambiguity inherent in the selective field ionization method used for previous studies. The results clearly characterize the capture energetics over the range of ion charge q=1−−11q=1--11q=1−−11 and velocity v=0.031−−0.138a.u.v=0.031--0.138\mathrm{a}.\mathrm{u}.v=0.031−−0.138a.u. The measurements are in very good agreement with predictions of the classical trajectory Monte Carlo method, but not with predictions of other classical models.
New experimental results have been obtained in collisions of singly charged ions with Na Rydberg atoms. (a) The distribution of final n states populated by electron capture shows non-monotonic variations of width with incident energy over the range 60-2100 eV. (b) The total capture cross section for alkali ions on Rydberg targets shows peaks and dips over the same energy range, correlated with particular reduced velocities v and the polarization of the exciting laser. (c) {ell}-Changing collision of Na{sup +} on Na(nd) targets, n=26 and 28, at low v preferentially transfer multiple units {h_bar} of orbital angular momentum under single-collision conditions, despite very large impact parameters. (d) Inelastic impacts of Na{sup f+} on Na 36s and 30p states, perturbed by electric fields, populate a strongly field-dependent mixture of nearby Stark levels. A synopsis of recent progress will be given.
Low-energy collisions of Rydberg atom-ion systems are investigated theoretically. We present the parameter space associated with suitable approaches for the dynamics of Rydberg atom-ion collisions, i.e., quantum, Langevin, and classical exchange regimes, showing that for the lowest reachable temperatures a classical treatment is appropriate. A quasiclassical trajectory method is used to study charge exchange cross sections for ${\mathrm{Li}}^{*}\text{\ensuremath{-}}{\mathrm{Li}}^{+}$ and ${\mathrm{Li}}^{*}\text{\ensuremath{-}}{\mathrm{Cs}}^{+}$ at collision energies down to 1K1\phantom{\rule{0.28em}{0ex}}\mathrm{K}1K. For cold collisions we find the charge exchange cross section deviating from the n4{n}^{4}n4 geometric scaling. Furthermore, for low-energy collisions, we find both an influence of the ionic core repulsion as well as variations for two different models used for describing the electron-core potential.
The absolute cross section for the energy transfer between the nP Rydberg atom (n=35--60) and the ground-state (5S) atom of rubidium is measured to be 4.8\ifmmode\times\else\texttimes\fi{}102{10}^{2}102 A˚2{\r{}}^{2}˚2 for thermal collisions at 420 K. This value of the cross section is in agreement with the calculated value for resonant charge transfer at the relevant collision energy. It is concluded that the energy transfer process is essentially charge transfer between the Rydberg ion core and the ground-state atom, where the Rydberg electron stays as a spectator.
Charge transfer from high‐n atomic targets populates comparably excited states of ionic projectiles. This paper reviews a decade of accelerating experimental and theoretical progress in the field, which offers an unusual variety of challenges in the preparation of initial states and in the analysis of final states. Interesting dynamical questions at the interface of classical and quantum mechanics are posed by new experimental results. Rydberg atom phenomena are increasingly found to be important for other areas of atomic collision physics in all energy regimes.