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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.
This study demonstrates singlet fission in water-soluble perylene derivatives. Dynamic, disordered dimers enable efficient triplet formation, exceeding 100% efficiency in aqueous solutions.
Area of Science:
- Photochemistry
- Materials Science
- Physical Chemistry
Background:
- Singlet fission (SF) is an efficient photophysical process for generating multiple excitons from a single photon.
- Water-soluble organic compounds are desirable for sustainable energy applications but often lack efficient SF pathways.
- Perylene derivatives are known SF chromophores, but their aggregation in solution can hinder SF efficiency.
Purpose of the Study:
- To provide direct evidence of singlet fission in water-soluble compounds.
- To investigate the role of dynamic dimer formation in enabling SF in aqueous solutions.
- To characterize the structure-dynamics-SF relationship in perylene associations.
Main Methods:
- Time-resolved absorption and fluorescence spectroscopy.
- Nuclear magnetic resonance (NMR) spectroscopy.
- Theoretical modeling and computational chemistry.
Main Results:
- Perylene-3,4,9,10-tetracarboxylate forms dynamic, disordered dimers in aqueous solution.
- These transient dimers exhibit lifetimes sufficient for intermolecular singlet fission.
- Triplet formation efficiency was observed to be greater than 100%, with triplet lifetimes in the nanosecond range.
Conclusions:
- Dynamic dimer formation in water-soluble perylene derivatives facilitates efficient singlet fission.
- Structural disorder within these transient associations is crucial for optimizing SF and charge separation.
- This work opens avenues for designing water-compatible materials for advanced photophysical applications.
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