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Lookup NU author(s): Professor Andrew Benniston, Emeritus Professor Anthony Harriman
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Electronic energy transfer (EET) from a donor to an acceptor is an important mechanism that controls the light harvesting efficiency in a wide variety of systems, including artificial and natural photosynthesis and contemporary photovoltaic technologies. The detailed mechanism of BET at short distances or large angles between the donor and acceptor is poorly understood. Here the influence of the orientation between the donor and acceptor on EET is explored using a molecule with two nearly perpendicular chromophores. Very fast EET with a time constant of 120 fs is observed, which is at least 40 times faster than the time predicted by Coulombic coupling calculations. Depolarization of the emission signal indicates that the transition dipole rotates through ca. 64 degrees, indicating the near orthogonal nature of the EET event. The rate of EET is found to be similar to structural relaxation rates in the photoexcited oligothiophene donor alone, which suggests that this initial relaxation brings the dyad to a conical intersection where the excitation jumps to the acceptor.
Author(s): Hedley GJ, Ruseckas A, Benniston AC, Harriman A, Samuel IDW
Publication type: Article
Publication status: Published
Journal: Journal of Physical Chemistry A
Year: 2015
Volume: 119
Issue: 51
Pages: 12665-12671
Print publication date: 24/12/2015
Online publication date: 28/11/2015
Acceptance date: 27/11/2015
ISSN (print): 1089-5639
ISSN (electronic): 1520-5215
Publisher: American Chemical Society
URL: http://dx.doi.org/10.1021/acs.jpca.5b08640
DOI: 10.1021/acs.jpca.5b08640
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