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Ultrafast dynamics of temporary anions probed through the prism of photodetachment

Anstöter, C.S.; Bull, J.N.; Verlet, J.R.R.

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Authors

C.S. Anstöter

J.N. Bull



Abstract

The recently developed method of frequency-, angle-, and time-resolved photoelectron imaging (FAT-PI) applied to the study of the dynamics of resonances of open-shell anions is reviewed. The basic principles of the method and its experimental realisation are outlined. The dynamics of a number of radical quinone anions is then considered. Firstly, we show for para-benzoquinone how frequency- and angle-resolved photoelectron imaging provides finger-prints of the dynamics of resonances and then how time-resolved photoelectron imaging yields deep mechanistic insight into the relaxation dynamics of the resonances. The effect of chemical substitutions of the para-quinone electrophore on the dynamics of resonances is discussed. Increasing the conjugation leads to a greatly enhanced ability for resonances to decay to the ground electronic state of the radical anion. Using time-resolved photoelectron spectroscopy, it is shown that the dynamics are facilitated by a bound valence state of the anion. The addition of electron donating methoxy groups leads to a reduced ability to access the ground state compared to para-benzoquinone. Both time-resolved dynamics and calculations provide a rationale for these observations. We consider the benefits and limitations of FAT-PI and its complementarity to 2D electron spectroscopy.

Citation

Anstöter, C., Bull, J., & Verlet, J. (2016). Ultrafast dynamics of temporary anions probed through the prism of photodetachment. International Reviews in Physical Chemistry, 35(4), 509-538. https://doi.org/10.1080/0144235x.2016.1203522

Journal Article Type Article
Acceptance Date Jun 8, 2016
Online Publication Date Aug 8, 2016
Publication Date Oct 1, 2016
Deposit Date Oct 31, 2016
Publicly Available Date Mar 29, 2024
Journal International Reviews in Physical Chemistry
Print ISSN 0144-235X
Electronic ISSN 1366-591X
Publisher Taylor and Francis Group
Peer Reviewed Peer Reviewed
Volume 35
Issue 4
Pages 509-538
DOI https://doi.org/10.1080/0144235x.2016.1203522

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