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Physical Review Letters

From 1 r to 1 r 2 Potentials: Electron Exchange between Rydberg Atoms and Polar Molecules

C. Desfrançois, Hassan Abdoul‐Carime, N. Khélifa, J. P. Schermann

Published Oct 31, 1994• 269 citations
Publisher

Abstract

Several new molecular anions, in their dipole-bound ground states, have been created by charge exchange between polar molecules and laser-excited Rydberg atoms. Measurement of electron-binding energies, by means of electric field detachment, as function of known molecular dipole moments gives the first experimental estimation of the minimum molecular dipole required to bind an electron.

DOI
10.1103/physrevlett.73.2436

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Several new molecular anions, in their dipole-bound ground states, have been created by charge exchange between polar molecules and laser-excited Rydberg atoms. Measurement of electron-binding energies, by means of electric field detachment, as function of known molecular dipole moments gives the first experimental estimation of the minimum molecular dipole required to bind an electron.
We describe two simple models for the determination of electron binding energies (Eb{\mathit{E}}_{\mathit{b}}Eb​) of several dipole-bound negative ions from field-detachment experiments and charge-transfer formation-rate-constant measurements in collisions between cold neutral molecules and Rydberg atoms. These models are able to correctly reproduce the experimental data, from which we deduce two compatible sets of Eb{\mathit{E}}_{\mathit{b}}Eb​ values. A curve-crossing model for calculating anion formation rate constants allows us to qualitatively understand the sharply peaked shapes of the experimental curves and to derive a simple quantitative law between Eb{\mathit{E}}_{\mathit{b}}Eb​ values and principal Rydberg quantum numbers at which anion formation rate constants are maximum.
Electron transfer collisions between state‐selected Rydberg atoms and polar closed‐shell molecules or molecular clusters is a very efficient way to create ground‐state dipole‐bound molecular anions. This process can be selective with respect to the total electric dipole moment of the neutral parent and is well understood in terms of a ionic‐covalent curve‐crossing model. It is also a very gentle and reversible way to ionize polar molecules or clusters, with minimal change of the neutral geometry. The application of Rydberg charge exchange to the isomeric selection of small size‐selected polar molecular clusters is discussed.
Rydberg molecule, formed by one or more Rydberg atoms, exhibits remarkable properties, including an exceptionally large spatial extent, rich rovibrational level structures, permanent electric dipole moments, and a pronounced sensitivity to external fields. Based on the underlying binding mechanisms, Rydberg molecules can be divided into three categories, the ground-Rydberg molecule that is bound via a low-energy electron-atom scattering interaction between ground atom and Rydberg electron, the Rydberg-Rydberg molecule that is bound via a long-range electrostatic interaction between Rydberg atoms, and the ion-Rydberg molecule that is bound via single- or multi-polar interactions between Rydberg atom and ion. This review focuses on recent theoretical and experimental advances in diatomic Rydberg molecules, covering their formation and binding mechanisms, potential energy curves, experimental observations, and spectroscopic properties, with the aim of providing a comprehensive overview of the current state and future prospects of this rapidly developing field.
Low-energy electron transfer in collisions between a Rydberg atom and a target molecule can result in the formation of negative ions. Depending as to the properties of the target molecule the electron may be bound in a localized molecular orbital (valence-bound) or bound by its dipole potential in a diffuse orbital located at the positive end of the dipole (dipole-bound). Here we examine the properties of valence-bound and dipole-bound negative ions created through electron transfer in collision with Rydberg atoms, in particular, their lifetimes, collisional properties and electric-field-induced detachment characteristics. Intercomparison of the various data also leads to new insights into electron attachment to molecules that can support both valence-bound and dipole-bound negative ion states.
The authors investigate long-range Cs2{}_{2}2​ molecules consisting of a ground-state and a Rydberg atom, and measure and calculate permanent molecular electric-dipole moments showing that the sign of the dipole moment is negative, reflecting a deficiency of Rydberg-electron density near the ground-state constituent
Resonant energy transfer (RET) between the equal parity 1s65s ^{3}S_{1} and 1s66s ^{3}S_{1} Rydberg levels in helium has been observed in low-temperature (∼80 mK) collisions with ammonia molecules that undergo inversion transitions in their X ^{1}A_{1} ground electronic state. This hybrid Rydberg-atom-polar-molecule resonant energy transfer represents a monopole-dipole energy exchange reaction that necessarily requires spatial overlap of the Rydberg-electron and molecular wave functions. Calculations that account explicitly for the charge-dipole interaction between the Rydberg electron and the molecule provide a quantitative explanation of the observations. Total parity is conserved in the reaction through the mixing of collisional angular momentum in the atom-molecule complex. This work opens opportunities to expand the toolbox for quantum science with charge-dipole-mediated energy exchange in hybrid atom-polar-molecule platforms.