Abstract
Nonvalence states of molecular anions play key roles in processes, such as electron mobility, in rare-gas liquids, radiation-induced damage to DNA, and the formation of anions in the interstellar medium. Recently, a class of nonvalence bound anion state has been predicted by theory in which correlation forces are predominantly responsible for binding the excess electron. We present a direct spectroscopic observation of this nonvalence correlation-bound state (CBS) in the para-toluquinone trimer cluster anion. Time-resolved photoelectron velocity map imaging shows that photodetachment of the CBS produces a narrow and highly anisotropic photoelectron distribution, consistent with detachment from an s-like orbital. The CBS is bound by ~50 meV and decays by vibration-mediated autodetachment with a lifetime of 700 ± 100 fs. These states are likely to be common in large and/or polarizable anions and clusters and may act as doorway states in electron attachment processes.
Original language | English |
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Article number | e1603106 |
Journal | Science Advances |
Volume | 3 |
Issue number | 5 |
DOIs | |
Publication status | Published - 19 May 2017 |
Profiles
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James Bull
- School of Chemistry, Pharmacy and Pharmacology - Associate Professor in Ultrafast Chemical Physics
- Centre for Photonics and Quantum Science - Member
- Chemistry of Light and Energy - Member
Person: Research Group Member, Academic, Teaching & Research