Ultrafast Electron Transfer Dynamics in a Series of Porphyrin/Viologen Complexes: Involvement of Electronically Excited Radical Pair Products

The Journal of Physical Chemistry. B
Jonas Petersson, Leif Hammarström

Abstract

Ultrafast electron transfer was studied for a series of metalloporphyrin/bipyridinium complexes in aqueous solution, using laser excitation in the Soret or Q-bands of the porphyrin. Electron transfer occurred before electronic and vibrational relaxation of the initial excited state. This allowed for a thorough investigation of the dependence of electron transfer rate constants on the driving force and the nature of the product state. The driving force dependence showed that electron transfer from the S2 state occurred to an electronically excited radical pair state, and the present results provide the most direct evidence to date for the formation of such states in photoinduced electron transfer reactions. We also found that subsequent recombination of the radical pair produced vibrationally excited ground states; the excess energy of the radical pair generated from the initial state is not completely dissipated during the lifetime of the radical pair. The porphyrin/bipyridinium complexes where recombination lies deeper in the Marcus inverted region show less formation of unrelaxed ground states, contrary to what is expected from equilibrium electron transfer theories. Instead, the rate of the electron transfer, which competes ...Continue Reading

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Citations

Jan 4, 2017·The Journal of Physical Chemistry. B·Alexey E NazarovAnatoly I Ivanov
Feb 1, 2017·The Journal of Physical Chemistry. B·Puspal MukherjeePratik Sen
Apr 24, 2018·Photochemical & Photobiological Sciences : Official Journal of the European Photochemistry Association and the European Society for Photobiology·Valentina A MikhailovaAnatoly I Ivanov
Aug 6, 2020·The Journal of Chemical Physics·Nickolay B SiplivyAnatoly I Ivanov
Jul 3, 2020·The Journal of Chemical Physics·Christoph NançozEric Vauthey
Dec 14, 2016·Chemical Reviews·Tatu KumpulainenEric Vauthey
Nov 12, 2020·The Journal of Physical Chemistry. B·Serguei V FeskovAnatoly I Ivanov
Jan 14, 2016·The Journal of Physical Chemistry. C, Nanomaterials and Interfaces·Jesus Nieto-PescadorLars Gundlach
Sep 11, 2021·The Journal of Physical Chemistry. B·Clark ZahnKarsten Heyne

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