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

Bull, James N. and Verlet, Jan R. R. (2017) 'Observation and ultrafast dynamics of a nonvalence correlation-bound state of an anion.', Science advances., 3 (5). e1603106.

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
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Available under License - Creative Commons Attribution Non-commercial.
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Status:Peer-reviewed
Publisher Web site:https://doi.org/10.1126/sciadv.1603106
Publisher statement:2017 © The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).
Date accepted:22 March 2017
Date deposited:05 July 2017
Date of first online publication:19 May 2017
Date first made open access:05 July 2017

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