51. Spontaneous exciton dissociation enables spin state interconversion in delayed fluorescence organic semiconductors
- Author
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Gillett, Alexander J., Tonnelé, Claire, Londi, Giacomo, Ricci, Gaetano, Catherin, Manon, Unson, Darcy M. L., Casanova, David, Castet, Frédéric, Olivier, Yoann, Chen, Weimin M., Zaborova, Elena, Evans, Emrys W., Drummond, Bluebell H., Conaghan, Patrick J., Cui, Lin-Song, Greenham, Neil C., Puttisong, Yuttapoom, Fages, Frédéric, Beljonne, David, and Friend, Richard H.
- Subjects
Physics - Applied Physics ,Condensed Matter - Materials Science - Abstract
Engineering a low singlet-triplet energy gap ({\Delta}EST) is necessary for efficient reverse intersystem crossing (rISC) in delayed fluorescence (DF) organic semiconductors, but results in a small radiative rate that limits performance in LEDs. Here, we study a model DF material, BF2, that exhibits a strong optical absorption (absorption coefficient =3.8x10^5 cm^-1) and a relatively large {\Delta}EST of 0.2 eV. In isolated BF2 molecules, intramolecular rISC is slow (260 {\mu}s), but in aggregated films, BF2 generates intermolecular CT (inter-CT) states on picosecond timescales. In contrast to the microsecond intramolecular rISC that is promoted by spin-orbit interactions in most isolated DF molecules, photoluminescence-detected magnetic resonance shows that these inter-CT states undergo rISC mediated by hyperfine interactions on a ~24 ns timescale and have an average electron-hole separation of >1.5 nm. Transfer back to the emissive singlet exciton then enables efficient DF and LED operation. Thus, access to these inter-CT states resolves the conflicting requirements of fast radiative emission and low {\Delta}EST., Comment: 102 pages, 4 main-text figures
- Published
- 2021
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