Observation and ultrafast dynamics of a nonvalence correlation-bound state of an anion

Bull, James N. ORCID: https://orcid.org/0000-0003-0953-1716 and Verlet, Jan R. R. (2017) Observation and ultrafast dynamics of a nonvalence correlation-bound state of an anion. Science Advances, 3 (5). ISSN 2375-2548

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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.

Item Type: Article
Uncontrolled Keywords: general ,/dk/atira/pure/subjectarea/asjc/1000
Faculty \ School: Faculty of Science > School of Chemistry
UEA Research Groups: Faculty of Science > Research Groups > Chemistry of Light and Energy
Faculty of Science > Research Groups > Centre for Photonics and Quantum Science
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Depositing User: LivePure Connector
Date Deposited: 04 Feb 2019 14:30
Last Modified: 09 Feb 2023 13:46
URI: https://ueaeprints.uea.ac.uk/id/eprint/69833
DOI: 10.1126/sciadv.1603106

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