Please use this identifier to cite or link to this item: http://hdl.handle.net/2440/111309
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Type: Journal article
Title: Endothermic singlet fission is hindered by excimer formation
Author: Dover, C.
Gallaher, J.
Frazer, L.
Tapping, P.
Petty, A.
Crossley, M.
Anthony, J.
Kee, T.
Schmidt, T.
Citation: Nature Chemistry, 2018; 10(3):305-310
Publisher: Nature Publishing Group
Issue Date: 2018
ISSN: 1755-4330
1755-4349
Statement of
Responsibility: 
Cameron B. Dover, Joseph K. Gallaher, Laszlo Frazer, Patrick C. Tapping, Anthony J. Petty II, Maxwell J. Crossley, John E. Anthony, Tak W. Kee and Timothy W. Schmidt
Abstract: Singlet fission is a process whereby two triplet excitons can be produced from one photon, potentially increasing the efficiency of photovoltaic devices. Endothermic singlet fission is desired for a maximum energy-conversion efficiency, and such systems have been considered to form an excimer-like state with multiexcitonic character prior to the appearance of triplets. However, the role of the excimer as an intermediate has, until now, been unclear. Here we show, using 5,12-bis((triisopropylsilyl)ethynyl)tetracene in solution as a prototypical example, that, rather than acting as an intermediate, the excimer serves to trap excited states to the detriment of singlet-fission yield. We clearly demonstrate that singlet fission and its conjugate process, triplet-triplet annihilation, occur at a longer intermolecular distance than an excimer intermediate would impute. These results establish that an endothermic singlet-fission material must be designed to avoid excimer formation, thus allowing singlet fission to reach its full potential in enhancing photovoltaic energy conversion.
Keywords: Energy transfer; excited states; reaction kinetics and dynamics; light harvesting; optical spectroscopy
Rights: © 2018 Macmillan Publishers Limited, part of Springer Nature. All rights reserved.
RMID: 0030083205
DOI: 10.1038/nchem.2926
Grant ID: http://purl.org/au-research/grants/arc/FT130100177
http://purl.org/au-research/grants/arc/CE170100026
http://purl.org/au-research/grants/arc/DP160103797
http://purl.org/au-research/grants/arc/LE0989747
Appears in Collections:Chemistry publications

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