James N. Bull
Observation and ultrafast dynamics of a nonvalence correlation-bound state of an anion
Bull, James N.; Verlet, Jan R.R.
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.
Citation
Bull, J. N., & Verlet, J. R. (2017). Observation and ultrafast dynamics of a nonvalence correlation-bound state of an anion. Science Advances, 3(5), Article e1603106. https://doi.org/10.1126/sciadv.1603106
Journal Article Type | Article |
---|---|
Acceptance Date | Mar 22, 2017 |
Online Publication Date | May 19, 2017 |
Publication Date | May 19, 2017 |
Deposit Date | Jun 30, 2017 |
Publicly Available Date | Jul 5, 2017 |
Journal | Science Advances |
Electronic ISSN | 2375-2548 |
Publisher | American Association for the Advancement of Science |
Peer Reviewed | Peer Reviewed |
Volume | 3 |
Issue | 5 |
Article Number | e1603106 |
DOI | https://doi.org/10.1126/sciadv.1603106 |
Public URL | https://durham-repository.worktribe.com/output/1375963 |
Related Public URLs | http://advances.sciencemag.org/content/advances/3/5/e1603106.full.pdf |
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Copyright 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).
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