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Chinese Journal of Physics

Effective Elimination of Space Charge Effects in Ion-Beam Experiments

Michio Matsuzawa

Published Dec 1, 2013• 0 citations
Publisher

Abstract

An experimental method is proposed for the effective elimination of space-charge effects in ion-beam experiments based on collisions of high-Rydberg atoms with neutral species. One can effectively avoid the space-charge effects encountered in ion-beam experiments by the provision of an extra electron in a circular high-Rydberg state on the ion. This procedure is expected to achieve accurate probing of the interaction between the ion and the neutral species without space-charge effects at low energies.

DOI
10.6122/cjp.51.1184

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Cambridge University Press eBooks•Sep 15, 1994•0 citations
An experimental method is proposed for the effective elimination of space-charge effects in ion-beam experiments based on collisions of high-Rydberg atoms with neutral species. One can effectively avoid the space-charge effects encountered in ion-beam experiments by the provision of an extra electron in a circular high-Rydberg state on the ion. This procedure is expected to achieve accurate probing of the interaction between the ion and the neutral species without space-charge effects at low energies.
We have theoretically studied the conditions of the behavior of a high Rydberg electron as a spectator to an ion-molecule reaction in high Rydberg neutral collisions. Adoption of a circular high Rydberg atom in the initial channel of the high Rydberg neutral collisions ensures the behavior of the high Rydberg electron as the spectator to interaction between an ion core of the high Rydberg atom and an incoming neutral species; i.e., the ion-molecule reaction. This theoretical consideration leads to equivalence between the high Rydberg neutral collision and the ion-molecule reaction with high accuracy. This equivalence gives us a possibility of probing the ion-molecule reaction at low energies without space-charge effects encountered in ion-beam experiments.
Abstract Recently, a new method has been introduced to study ion-molecule reactions at very low collision energies, down to below k B ⋅ 1 K (Allmendinger et al 2016 ChemPhysChem 17 3596). To eliminate the acceleration of the ions by stray electric fields in the reaction volume, the reactions are observed within the orbit of a Rydberg electron with large principal quantum number n > 20. This electron is assumed not to influence the reaction taking place between the ion core and the neutral molecules. This assumption is tested here with the example of the He(n) + CO → C(n′) + O + He reaction, which is expected to be equivalent to the He+ + CO → C+ + O + He reaction, using a merged-beam approach enabling measurements of relative reaction rates for collision energies E coll in the range from 0 to about k B ⋅ 25 K with a collision-energy resolution of ∼k B ⋅ 200 mK at E coll = 0. In contrast to the other ion-molecule reactions studied so far with this method, the atomic ion product (C+) is in its electronic ground state and does not have rotational and vibrational degrees of freedom so that the corresponding Rydberg product [C(n′)] cannot decay by autoionization. Consequently, one can investigate whether the principal quantum number is effectively conserved, as would be expected in the spectator Rydberg-electron model. We measure the distribution of principal quantum numbers of the reactant He(n) and product C(n′) Rydberg atoms by pulsed-field ionization following initial preparation of He(n) in states with n values between 30 and 45 and observe that the principal quantum number of the Rydberg electron is conserved during the reaction. This observation indicates that the Rydberg electron is not affected by the reaction, from which we can conclude that it does not affect the reaction either. This conclusion is strengthened by measurements of the collision-energy-dependent reaction yields at n = 30, 35 and 40, which exhibit the same behavior, i.e. a marked decrease below E coll ≈ k B ⋅ 5 K.
List of contributors Preface 1. Rydberg atoms in astrophysics A. Dalgarno 2. Theoretical studies of hydrogen Rydberg atoms in electric fields R. J. Damburg and V. V. Kolosov 3. Rydberg atoms in strong fields D. Kleppner, Michael G. Littman and Myron L. Zimmerman 4. Spectroscopy of one- and two-electron Rydberg atoms C. Fabre and S. Haroche 5. Interaction of Rydberg atoms with blackbody radiation T. F. Gallagher 6. Theoretical approaches to low-energy collisions of Rydberg atoms with atoms and ions A. P. Hickman, R. E. Olson and J. Pascale 7. Experimental studies of the interaction of Rydberg atoms with atomic species at thermal energies F. Gounand and J. Berlande 8. Theoretical studies of collisions of Rydberg atoms with molecules Michio Matsuzawa 9. Experimental studies of thermal-energy collisions of Rydberg atoms with molecules F. B. Dunning and R. F. Stebbings 10. High-Rydberg molecules Robert S. Freund 11. Theory of Rydberg collisions with electrons, ions and neutrals M. R. Flannery 12. Experimental studies of the interactions of Rydberg atoms with charged particles J. -F. Delpech 13. Rydberg studies using fast beams Peter M. Koch Index.
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.
The large size and low binding energies, scaling as n 4 and n −2 , of Rydberg atoms make them nearly irresistible subjects for collision experiments. While one might expect collision cross sections to be enormous, by and large they are not. In fact, Rydberg atoms are quite transparent to most collision partners. Collisions involving Rydberg atoms can be broken into two general categories, collisions in which the collision partner, or perturber, interacts with the Rydberg atom as a whole, and those in which the perturber interacts separately with the ionic core and the Rydberg electron. The difference between these two categories is in essence a question of the range of the interaction between the perturber and the Rydberg atom relative to the size of the Rydberg atom. A few examples serve to clarify this point. A Rydberg atom interacting with a charged particle is a charge–dipole interaction with a 1/ R 2 interaction potential, and the resonant dipole–dipole interaction between two Rydberg atoms has a 1/ R 3 interaction potential. Here R is the internuclear separation of the Rydberg atom and the perturber. In both of these interactions the perturber interacts with the Rydberg atom as a whole. On the other hand when a Rydberg atom interacts with a N 2 molecule the longest range atom–molecule interaction is a dipole–induced dipole interaction with a potential varying as 1/ R 6 .