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Excited states in electron-transfer reaction products : ultrafast relaxation dynamics of an isolated acceptor radical anion.

Horke, D.A. and Roberts, G.M. and Verlet, J.R.R. (2011) 'Excited states in electron-transfer reaction products : ultrafast relaxation dynamics of an isolated acceptor radical anion.', Journal of physical chemistry A., 115 (30). pp. 8369-8374.

Abstract

The spectroscopy and ultrafast relaxation dynamics of excited states of the radical anion of a representative charge-transfer acceptor molecule, 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane, have been studied in the gas phase using time-resolved photoelectron spectroscopy. The photoelectron spectra reveal that at least two anion excited states are bound. Time-resolved studies show that both excited states are very short-lived and internally convert to the anion ground state, with the lower energy state relaxing within 200 fs and a near-threshold valence-excited state relaxing on a 60 fs time scale. These excited states, and in particular the valence-excited state, present efficient pathways for electron-transfer reactions in the highly exergonic inverted region which commonly displays rates exceeding predictions from electron-transfer theory.

Item Type:Article
Full text:(AM) Accepted Manuscript
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Status:Peer-reviewed
Publisher Web site:http://dx.doi.org/10.1021/jp2038202
Publisher statement:This document is the Accepted Manuscript version of a Published Work that appeared in final form in The Journal of Physical Chemistry A, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see http://dx.doi.org/10.1021/jp2038202.
Date accepted:No date available
Date deposited:05 February 2016
Date of first online publication:August 2011
Date first made open access:No date available

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