2019
DOI: 10.1021/jacs.9b02302
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Annihilation Versus Excimer Formation by the Triplet Pair in Triplet–Triplet Annihilation Photon Upconversion

Abstract: The triplet pair is the key functional unit in triplet–triplet annihilation photon upconversion. The same molecular properties that stabilize the triplet pair also allow dimers to form on the singlet energy surface, creating an unwanted energy relaxation pathway. Here we show that excimer formation most likely is a consequence of a triplet dimer formed before the annihilation event. Polarity-dependent studies were performed to elucidate how to promote wanted emission pathways over excimer formation. Furthermor… Show more

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Cited by 85 publications
(102 citation statements)
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“…It has recently been suggested that a reason for strong excimer emission in perylene based TTA-UC is the formation of excimers on the triplet surfaces before the annihilation event. 40 The relationship between excimer formation and molecular structure can be explored from an energetic point of view (Note S1.6, ESI †). To this end, we analysed the potential energy surface for the interaction between a pair of perylene molecules within the framework of time-dependent density functional theory (TD-DFT).…”
Section: Energetics Of Annihilator Dimersmentioning
confidence: 99%
See 1 more Smart Citation
“…It has recently been suggested that a reason for strong excimer emission in perylene based TTA-UC is the formation of excimers on the triplet surfaces before the annihilation event. 40 The relationship between excimer formation and molecular structure can be explored from an energetic point of view (Note S1.6, ESI †). To this end, we analysed the potential energy surface for the interaction between a pair of perylene molecules within the framework of time-dependent density functional theory (TD-DFT).…”
Section: Energetics Of Annihilator Dimersmentioning
confidence: 99%
“…39 We have further suggested that another main reason for the surprisingly large amount of excimer emission in perylene based photon upconversion is due to a preassembly step on the triplet energy surface, already before the upconversion event. 40 Alkyl substitution offers the opportunity to manipulate the stacking interactions of perylene with minimal impact on the excited levels of the individual molecules. Indeed, perylene derivatives like tetra-tert-butylperylene show low excimer formation in TTA-UC, since the molecular aggregation is sterically hindered.…”
Section: Introductionmentioning
confidence: 99%
“…The controlled excimer formation reported by Börjesson et al. would also be useful to rationally switch the upconverted emission color …”
Section: Aggregation‐induced Ucmentioning
confidence: 97%
“…Improving the efficiency of optoelectronic devices by harvesting both triplet and singlet excitons is a contemporary area of research (Uoyama et al, 2012;Obolda et al, 2016;Noda et al, 2018;Liang et al, 2019;Northey et al, 2019). Various approaches such as triplet-triplet annihilation (TTA) (Yang et al, 2017;Pu et al, 2019;Ye et al, 2019), exciton-polaron interaction (EPI) (Kim et al, 2018), and thermally activated delayed fluorescence (TADF) (Uoyama et al, 2012) have been put forward for this application. This is because both TTA and EPI are bimolecular processes and it is very challenging to control these processes in devices.…”
Section: Introductionmentioning
confidence: 99%