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Physical Review Letters

Double Rydberg States Formed in Stabilized Triple Electron Capture

Serge Martin, Jérôme Bernard, L. Chen, Alain Denis, Jean Desesquelles

Published Nov 18, 1996• 12 citations
Publisher

Abstract

Double Rydberg states were populated by triple electron capture in collisions of highly charged ions with atoms. The highest stabilization of states produced by triple capture at $v\ensuremath{\cong}0.2\mathrm{a}.\mathrm{u}.$ was found for binding energies of the projectile electrons near the limits of the $({2,n,n}^{\ensuremath{'}})$ and $({3,n,n}^{\ensuremath{'}})$ series. Population of triply excited double Rydberg states was confirmed by the emission of Rydberg transitions. Results are interpreted by two successive autotransfer into Rydberg states for $({3,n,n}^{\ensuremath{'}})$ states and of one-step two-electron autotransfer for $({2,n,n}^{\ensuremath{'}})$ states.

DOI
10.1103/physrevlett.77.4306

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Double Rydberg states were populated by triple electron capture in collisions of highly charged ions with atoms. The highest stabilization of states produced by triple capture at v\ensuremath≅0.2a.u.v\ensuremath{\cong}0.2\mathrm{a}.\mathrm{u}.v\ensuremath≅0.2a.u. was found for binding energies of the projectile electrons near the limits of the (2,n,n\ensuremath′)({2,n,n}^{\ensuremath{'}})(2,n,n\ensuremath′) and (3,n,n\ensuremath′)({3,n,n}^{\ensuremath{'}})(3,n,n\ensuremath′) series. Population of triply excited double Rydberg states was confirmed by the emission of Rydberg transitions. Results are interpreted by two successive autotransfer into Rydberg states for (3,n,n\ensuremath′)({3,n,n}^{\ensuremath{'}})(3,n,n\ensuremath′) states and of one-step two-electron autotransfer for (2,n,n\ensuremath′)({2,n,n}^{\ensuremath{'}})(2,n,n\ensuremath′) states.
A classical model of singly charged ion collisions with Rydberg atoms in linear Stark states directed toward the oncoming ion beam predicts a bimodal distribution of final states resulting from electron capture. At a reduced velocity $\stackrel{\ifmmode \tilde{}\else \~{}\fi{}}{v}{=v}_{\mathrm{ion}}{/v}_{\mathrm{Bohr}}=0.45,$ the calculated energy distribution of captured electrons peaks near the target binding energy Ei,{E}_{i},Ei​, but has a second peak at energies roughly Ei/4.{E}_{i}/4.Ei​/4. Analysis of the impact-parameter dependence of the capture probabilities indicates that the second peak arises from three-swap capture events. The decrease in binding energy of the captured electrons is attributed to excitation via united-atom rotational coupling.
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.
Scattering of K(np) Rydberg atoms by electron-attaching molecules can result in the formation of positive-negative ion pairs through electron transfer reactions. These reactions can involve the dissociation of a transient intermediate negative ion into a smaller negative ion and a neutral fragment, or they can result in the parent molecule forming a metastable negative ion, with the excess energy being distributed among its internal modes. For Rydberg atoms of intermediate n, it is possible for these ion pairs to orbit each other at large separation, weakly bound by their mutual electrostatic attraction, forming what are known as heavy-Rydberg states. Measurements of the binding energy and velocity distributions of the ion pairs are used to probe the dynamics of electron transfer reactions. The data are analyzed using a semiclassical Monte Carlo collision code to explore the lifetime of the intermediate, the nature of its dissociation, the distribution of the excess energy of reaction, and the branching ratio of the various reaction channels. Results obtained using a variety of attaching targets including CF3I, CCl4, SF6, CH2Br2, 1,1,1-C2Cl3F3, CCl3Br, Fe(CO)5, and CH3NO2 have demonstrated both the wide variety of different behaviors that can accompany electron capture as well as the different behaviors of the product ion-pair states themselves. Remarkably, despite previous work showing that it was possible for CH3NO2 to form long-lived valence-bound negative ions through Rydberg electron transfer, the present work showed that such collisions do not result in the formation of long-lived bound ion-pair states. Rather, the data show that collisions lead to very strong Rydberg atom scattering through formation of transient ion-pair states. These results are consistent with theoretical work that predicts significant collisional quenching of Rydberg atoms by highly polar molecules and highlight a new mechanism for Rydberg atom scattering.
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.
First Major Highlight: Collisional Stark Mixing at ultralow energies in Rydberg Plasmas. Atoms in high (n,l) states formed in cold Rydberg plasmas decay to the ground state in a succession of radiative transitions populating intermediate excited states. Which states are populated during cascading and with what probability can be obtained from known transition probabilities. Classical models simplify the calculation considerably, revealing the "trajectory" in nt space followed during the cascade, scaling rules and other aspects hidden within the quantal approach. Conserved Quantity (quantal analogue obscure): Quantal-Classical correspondence in radiative recombination and decay is directly demonstrated. Classical transition probabilities and radiative, recombination cross-section are in excellent agreement with quantal results. Cross section for three body collisional capture is formulated for arbitrary electron-energy distributions.