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AIP conference proceedings

Collisions of Rydberg atoms with ions: A review of recent work on charge transfer from highly excited targets

Keith B. MacAdam

Published Jan 1, 1993• 0 citations
Publisher

Abstract

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.

DOI
10.1063/1.45237

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•Jan 1, 2009•0 citations
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.
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.
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.
Atoms in highly excited Rydberg states possess physical characteristics quite unlike those associated with atoms in the ground or low-lying excited states. In particular, they are physically very large and are only very weakly bound. In consequence, collisions can lead to a wide variety of reaction processes many of which are unique to Rydberg species and have very large collision cross sections. In collisions with neutral targets, Rydberg atoms behave not as an atom but rather as a pair of well-separated independent scatterers, namely the core ion and the excited Rydberg electron. In the present article we discuss many of the different reactions that can occur when Rydberg atoms collide with neutral targets, focusing principally on reactions that are dominated by (binary) Rydberg electron-target interactions and include collisions with molecules that attach free low-energy electrons and with polar targets. In certain situations, however, interactions involving the Rydberg core ion are important. This is illustrated using as an example the destruction of ultralong-range Rydberg molecules excited in a cold dense gas.
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.
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.
In this thesis, we examine the ponderomotive interaction between an applied optical field and a highly excited Rydberg electron. An atom in a Rydberg state is essentially composed of an electron loosely bound, at a relatively large radial separation, to a positive ionic core. As such, the ponderomotive interaction for the Rydberg electron is similar to the interaction with free charges, which has been studied in context of plasma physics, new particle accelerator techniques, ion trapping, and electron diffraction among others. We are focused on using the ponderomotive interaction with the Rydberg electron to exert control over both the center-of-mass and electronic states of translationally cold Rydberg atoms. These capabilities can be adapted as tools for application in many experiments in areas such as atomic spectroscopy and quantum information processing. Our theoretical investigations have provided a well-defined parameter space for our experimental work and have allowed us to develop experimental methods appropriate for studying Rydberg atoms in ponderomotive potentials. In dense gases of cold Rydberg atoms, rich dynamics stem from electric multipole interactions among the Rydberg atoms. For example, interatomic forces between Rydberg atoms cause state-changing collisions which can significantly increase the kinetic energy of the colliding atoms. In addition to the studies of Rydberg atoms in ponderomotive potentials, we discuss collisions of cold Rydberg atoms in which internal energy of the Rydberg atoms is converted into kinetic energy.