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|Title:||Endothermic singlet fission is hindered by excimer formation|
|Citation:||Nature Chemistry, 2018; 10(3):305-310|
|Publisher:||Nature Publishing Group|
|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.|
|Appears in Collections:||Aurora harvest 3|
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