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

Bull, James N.; Verlet, Jan R.R.

doi:10.1126/sciadv.1603106

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

Bull, James N.; Verlet, Jan R.R.

Authors

James N. Bull

Professor Jan Verlet j.r.r.verlet@durham.ac.uk
Professor

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
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
Related Public URLs	http://advances.sciencemag.org/content/advances/3/5/e1603106.full.pdf

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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).