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Published on: July 19, 2019
Perylene-derivative singlet exciton fission in water solution
Chloe Magne1, Simona Streckaite2, Roberto A Boto3
1Université Paris-Saclay, CEA, CNRS, Institute for Integrative Biology of the Cell (I2BC) Gif-sur-Yvette 91190 France manuel.llansola@i2bc.paris-saclay.fr.
Abstract:
We provide direct evidence of singlet fission occurring with water-soluble compounds. We show that perylene-3,4,9,10-tetracarboxylate forms dynamic dimers in aqueous solution, with lifetimes long enough to allow intermolecular processes such as singlet fission. As these are transient dimers rather than stable aggregates, they retain a significant degree of disorder. We performed a comprehensive analysis of such dynamic assemblies using time-resolved absorption and fluorescence spectroscopy, nuclear magnetic resonance spectroscopy, and theoretical modelling, allowing us to observe the characteristic signatures of singlet fission and develop a model to characterize the different species observed. Our findings reveal that structure fluctuations within perylene-3,4,9,10-tetracarboxylate associations are key in favoring either singlet fission or charge separation. The efficiency of triplet formation is higher than 100%, and the disordered system leads to triplets living in the nanosecond time range.
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