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On the formation of anions: frequency-, angle-, and time-resolved photoelectron imaging of the menadione radical anion

Bull, James N.; West, Christopher W.; Verlet, Jan R.R.

On the formation of anions: frequency-, angle-, and time-resolved photoelectron imaging of the menadione radical anion Thumbnail


Authors

James N. Bull

Christopher W. West



Abstract

Frequency-, angle-, and time-resolved photoelectron imaging of gas-phase menadione (vitamin K3) radical anions was used to show that quasi-bound resonances of the anion can act as efficient doorway states to produce metastable ground electronic state anions on a sub-picosecond timescale. Several anion resonances have been experimentally observed and identified with the assistance of ab initio calculations, and ground state anion recovery was observed across the first 3 eV above threshold. Time-resolved measurements revealed the mechanism of electronic ground state anion formation, which first involves a cascade of very fast internal conversion processes to a bound electronic state that, in turn, decays by slower internal conversion to the ground state. Autodetachment processes from populated resonances are inefficient compared with electronic relaxation through internal conversion. The mechanistic understanding gained provides insight into the formation of radical anions in biological and astrochemical systems.

Citation

Bull, J. N., West, C. W., & Verlet, J. R. (2015). On the formation of anions: frequency-, angle-, and time-resolved photoelectron imaging of the menadione radical anion. Chemical Science, 6(2), 1578-1589. https://doi.org/10.1039/c4sc03491k

Journal Article Type Article
Acceptance Date Dec 17, 2014
Online Publication Date Dec 17, 2014
Publication Date Feb 1, 2015
Deposit Date Feb 18, 2015
Publicly Available Date Mar 28, 2024
Journal Chemical Science
Print ISSN 2041-6520
Electronic ISSN 2041-6539
Publisher Royal Society of Chemistry
Peer Reviewed Peer Reviewed
Volume 6
Issue 2
Pages 1578-1589
DOI https://doi.org/10.1039/c4sc03491k

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Copyright Statement
This article is licensed under a Creative Commons Attribution 3.0 Unported Licence.





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