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Ultrafast intersystem crossing in 9,10-anthraquinones and intramolecular charge separation in an anthraquinone-based dyad

Lookup NU author(s): Dr Ben Allen, James Rostron, Emeritus Professor Anthony Harriman

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Abstract

Femtosecond transient absorption spectroscopy was employed to determine quantitatively the ultrafast S1-T1 intersystem crossing in a 2-substituted 9,10-anthraquinone derivative (3), kisc = 2.5 × 1012 s-1. Notwithstanding this rapid process, photoexcitation of dyad 1 is followed by competition between intersystem crossing and intramolecular charge separation, the latter leading to a short-lived (2 ps) singlet charge-transfer (CT) state. The local triplet state itself undergoes slower charge separation to populate a relatively long-lived (130 ns) triplet CT state. An earlier report about the formation of an extremely long-lived CT state (>900 μs) in 1 was found to be erroneous and was related to the sacrificial photo-oxidation of the dimethylsulfoxide solvent used in that study. Finally, some important criteria have been formulated for future experimental validation of "unusually long-lived" CT states. © 2006 American Chemical Society.

Publication metadata

Author(s): Van Ramesdonk HJ, Bakker BH, Groeneveld MM, Verhoeven JW, Allen BD, Rostron JP, Harriman A

Publication type: Article

Publication status: Published

Journal: Journal of Physical Chemistry A

Year: 2006

Volume: 110

Issue: 49

Pages: 13145-13150

ISSN (print): 1089-5639

ISSN (electronic): 1520-5215

Publisher: American Chemical Society

URL: http://dx.doi.org/10.1021/jp0663098

DOI: 10.1021/jp0663098

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