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Singlet fission in a hexacene dimer: energetics dictate dynamics

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Abstract

Singlet fission (SF) is an exciton multiplication process with the potential to raise the efficiency limit of single junction solar cells from 33% to up to 45%. Most chromophores generally undergo SF as solid-state crystals. However, when such molecules are covalently coupled, the dimers can be used as model systems to study fundamental photophysical dynamics where a singlet exciton splits into two triplet excitons within individual molecules. Here we report the synthesis and photophysical characterization of singlet fission of a hexacene dimer. Comparing the hexacene dimer to analogous tetracene and pentacene dimers reveals that excess exoergicity slows down singlet fission, similar to what is observed in molecular crystals. Conversely, the lower triplet energy of hexacene results in an increase in the rate of triplet pair recombination, following the energy gap law for radiationless transitions. These results point to design rules for singlet fission chromophores: the energy gap between singlet and triplet pair should be minimal, and the gap between triplet pair and ground state should be large.

Graphical abstract: Singlet fission in a hexacene dimer: energetics dictate dynamics

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Supplementary files

Article information


Submitted
08 Oct 2019
Accepted
06 Dec 2019
First published
09 Dec 2019

This article is Open Access
All publication charges for this article have been paid for by the Royal Society of Chemistry

Chem. Sci., 2020, Advance Article
Article type
Edge Article

Singlet fission in a hexacene dimer: energetics dictate dynamics

S. N. Sanders, E. Kumarasamy, K. J. Fallon, M. Y. Sfeir and L. M. Campos, Chem. Sci., 2020, Advance Article , DOI: 10.1039/C9SC05066C

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