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.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.

Physical Review LettersNov 18, 199612 citations

Rydberg states of molecules

Ch. Jungen

AIP conference proceedingsJan 1, 19951 citation

Near-zero-energy electron attachment to S F 6 using Rydberg excitation and two-color resonance-enhanced multiphoton ionization of NO

Irina Jana, Eric James Smoll, Jonathan H. Frank +1 more

We report the formation of $\mathrm{S}{\mathrm{F}}_{6}^{\ensuremath{-}}$ in a molecular beam containing coexpanded NO and $\mathrm{S}{\mathrm{F}}_{6}$ by direct electron transfer from laser-excited Rydberg states of NO, and electron attachment from ultracold plasma induced by Penning ionization or photoionization of NO. At short times of up to 2 \textmu{}s after laser excitation, we find that the dominant pathway for near-zero-energy electron attachment to $\mathrm{S}{\mathrm{F}}_{6}$ molecules forming $\mathrm{S}{\mathrm{F}}_{6}^{\ensuremath{-}}$ ions is from Rydberg electron transfer from excited Rydberg states, within a few $\mathrm{c}{\mathrm{m}}^{\ensuremath{-}1}$ of the Rydberg limit. $\mathrm{S}{\mathrm{F}}_{6}^{\ensuremath{-}}$ ion production occurs by electron transfer from NO Rydberg states with a principal quantum number $n\ensuremath{\ge}165$. At this principal quantum number threshold, the Rydberg reaction range is \ensuremath{\sim}15 \textmu{}m. For lower-lying Rydberg states of NO, no $\mathrm{S}{\mathrm{F}}_{6}^{\ensuremath{-}}$ ions are detected despite the efficiency of $\mathrm{S}{\mathrm{F}}_{6}$ as an electron scavenger of weakly bound electrons. We hypothesize that $\mathrm{S}{\mathrm{F}}_{6}^{\ensuremath{-}}$ anions formed in closer proximity to a $\mathrm{N}{\mathrm{O}}^{+}$ cation core may undergo efficient back-electron transfer.We report the formation of $\mathrm{S}{\mathrm{F}}_{6}^{\ensuremath{-}}$ in a molecular beam containing coexpanded NO and $\mathrm{S}{\mathrm{F}}_{6}$ by direct electron transfer from laser-excited Rydberg states of NO, and electron attachment from ultracold plasma induced by Penning ionization or photoionization of NO. At short times of up to 2 \textmu{}s after laser excitation, we find that the dominant pathway for near-zero-energy electron attachment to $\mathrm{S}{\mathrm{F}}_{6}$ molecules forming $\mathrm{S}{\mathrm{F}}_{6}^{\ensuremath{-}}$ ions is from Rydberg electron transfer from excited Rydberg states, within a few $\mathrm{c}{\mathrm{m}}^{\ensuremath{-}1}$ of the Rydberg limit. $\mathrm{S}{\mathrm{F}}_{6}^{\ensuremath{-}}$ ion production occurs by electron transfer from NO Rydberg states with a principal quantum number $n\ensuremath{\ge}165$. At this principal quantum number threshold, the Rydberg reaction range is \ensuremath{\sim}15 \textmu{}m. For lower-lying Rydberg states of NO, no $\mathrm{S}{\mathrm{F}}_{6}^{\ensuremath{-}}$ ions are detected despite the efficiency of $\mathrm{S}{\mathrm{F}}_{6}$ as an electron scavenger of weakly bound electrons. We hypothesize that $\mathrm{S}{\mathrm{F}}_{6}^{\ensuremath{-}}$ anions formed in closer proximity to a $\mathrm{N}{\mathrm{O}}^{+}$ cation core may undergo efficient back-electron transfer.

Physical Review AFeb 20, 20253 citations

Bound He Rydberg states

Thomas F. Gallagher

Cambridge University Press eBooksSep 15, 19940 citations

Theoretical approaches for doubly-excited Rydberg states in quasi-two-electron systems: two-electron dynamics far away from the nucleus

Matthieu Génévriez

We report on recent progress regarding the theoretical treatment of doubly-excited Rydberg states of atoms with two valence electrons. Building upon state-of-the-art techniques, we demonstrate that an approach based on configuration interaction with exterior complex scaling (CI-ECS) is capable of describing high Rydberg states (n∼100) and does not rely on the assumptions of R-matrix multichannel quantum-defect theory. We show that CI-ECS allows the simultaneous, accurate treatment of a range of doubly-excited Rydberg states broader than previously possible. The implementation of the method with numerical basis functions is explained in detail. As an example, CI-ECS calculations of the doubly-excited states of Mg and Sr are presented, and excellent agreement is found with available experimental data. The CI-ECS method opens new perspectives for studying collective two-electron dynamics in doubly-excited Rydberg states of alkaline-earth metal atoms, and is also of interest for the field of Rydberg-based quantum simulation.We report on recent progress regarding the theoretical treatment of doubly-excited Rydberg states of atoms with two valence electrons. Building upon state-of-the-art techniques, we demonstrate that an approach based on configuration interaction with exterior complex scaling (CI-ECS) is capable of describing high Rydberg states (n∼100) and does not rely on the assumptions of R-matrix multichannel quantum-defect theory. We show that CI-ECS allows the simultaneous, accurate treatment of a range of doubly-excited Rydberg states broader than previously possible. The implementation of the method with numerical basis functions is explained in detail. As an example, CI-ECS calculations of the doubly-excited states of Mg and Sr are presented, and excellent agreement is found with available experimental data. The CI-ECS method opens new perspectives for studying collective two-electron dynamics in doubly-excited Rydberg states of alkaline-earth metal atoms, and is also of interest for the field of Rydberg-based quantum simulation.

Molecular PhysicsDec 18, 20208 citations

We report the formation of $\mathrm{S}{\mathrm{F}}_{6}^{\ensuremath{-}}$ in a molecular beam containing coexpanded NO and

\mathrm{S}{\mathrm{F}}_{6}

by direct electron transfer from laser-excited Rydberg states of NO, and electron attachment from ultracold plasma induced by Penning ionization or photoionization of NO. At short times of up to 2 \textmu{}s after laser excitation, we find that the dominant pathway for near-zero-energy electron attachment to

\mathrm{S}{\mathrm{F}}_{6}

molecules forming $\mathrm{S}{\mathrm{F}}_{6}^{\ensuremath{-}}$ ions is from Rydberg electron transfer from excited Rydberg states, within a few $\mathrm{c}{\mathrm{m}}^{\ensuremath{-}1}$ of the Rydberg limit. $\mathrm{S}{\mathrm{F}}_{6}^{\ensuremath{-}}$ ion production occurs by electron transfer from NO Rydberg states with a principal quantum number $n\ensuremath{\ge}165$. At this principal quantum number threshold, the Rydberg reaction range is \ensuremath{\sim}15 \textmu{}m. For lower-lying Rydberg states of NO, no $\mathrm{S}{\mathrm{F}}_{6}^{\ensuremath{-}}$ ions are detected despite the efficiency of

\mathrm{S}{\mathrm{F}}_{6}

as an electron scavenger of weakly bound electrons. We hypothesize that $\mathrm{S}{\mathrm{F}}_{6}^{\ensuremath{-}}$ anions formed in closer proximity to a

\mathrm{N}{\mathrm{O}}^{+}

cation core may undergo efficient back-electron transfer.