Challenges in distinguishing superexchange and hopping mechanisms of intramolecular charge transfer through fluorene oligomers

The Journal of Physical Chemistry. a
Randall H GoldsmithM R Wasielewski

Abstract

The temperature dependence of intramolecular charge separation in a series of donor-bridge-acceptor molecules having phenothiazine (PTZ) donors, 2,7-oligofluorene FL(n) (n = 1-4) bridges, and perylene-3,4:9,10-bis(dicarboximide) (PDI) acceptors was studied. Photoexcitation of PDI to its lowest excited singlet state results in oxidation of PTZ via the FL(n) bridge. In toluene, the temperature dependence of the charge separation rate constants for PTZ-FL(n)-PDI, (n = 1-4) is relatively weak and is successfully described by the semiclassical Marcus equation. The activation energies for charge separation suggest that bridge charge carrier injection is not the rate limiting step. The difficulty of using temperature and length dependence to differentiate hopping and superexchange is discussed, with difficulties in the latter topic explored via an extension of a kinetic model proposed by Bixon and Jortner.

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Citations

Aug 24, 2013·Analytical Chemistry·Chris H WohlgamuthJason D Slinker
Jul 31, 2010·Journal of the American Chemical Society·Thomas HinesNongjian Tao
Aug 10, 2010·Journal of the American Chemical Society·James R DiersDavid F Bocian
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Oct 10, 2009·The Journal of Chemical Physics·Keisuke Saito, Hitoshi Sumi
May 21, 2011·Journal of the American Chemical Society·Axel KahntBo Albinsson
Jul 17, 2015·The Journal of Chemical Physics·Michael Kilgour, Dvira Segal
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Sep 20, 2011·The Journal of Physical Chemistry. B·Alexander A Voityuk
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Feb 16, 2011·Journal of the American Chemical Society·Tomoaki Miura, Michael R Wasielewski
Mar 29, 2018·Journal of the American Chemical Society·Joseph A ChristensenMichael R Wasielewski

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