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- Congrave, Daniel G., et al.
(författare)
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Suppressing aggregation induced quenching in anthracene based conjugated polymers
- 2021
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Ingår i: Polymer Chemistry. - : Royal Society of Chemistry. - 1759-9954 .- 1759-9962. ; 12:12, s. 1830-1836
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Tidskriftsartikel (refereegranskat)abstract
- Anthracene is a highly valuable building block for luminescent conjugated polymers, particularly when a large singlet-triplet energy gap (Delta E-ST) is desired. Unfortunately, the extended pi system of anthracene imparts a strong tendency for polymer aggregation, resulting in detrimental effects on its solid state photophysics. A large decrease in photoluminescence quantum yield (PLQY, phi(F)) on going from solution to the solid state is especially common, represented in terms of a low phi(R) (phi(R) = phi(F film)/phi(F sol.)). Significant and undesirable red-shifting of fluorescence in the solid state is also typical due to processes such as excimer formation. In this work a series of alkylene-encapsulated conjugated anthracene polymers is developed to overcome these challenging problems. We demonstrate a promising material which displays a good solid state PLQY that is effectively unchanged compared to solution measurements (phi(R) similar to 1, phi(F film) similar to 40%), alongside an identical PL 0-0 transition wavelength in solution and thin film. Such a direct transfer of luminescence properties from solution to the solid state is remarkable for a conjugated polymer and completely unprecedented for one based on anthracene.
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- Gillett, Alexander J., et al.
(författare)
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Spontaneous exciton dissociation enables spin state interconversion in delayed fluorescence organic semiconductors
- 2021
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Ingår i: Nature Communications. - : Nature Portfolio. - 2041-1723. ; 12:1
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Tidskriftsartikel (refereegranskat)abstract
- Engineering a low singlet-triplet energy gap (Delta E-ST) 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 = 3.8 x 10(5) cm(-1)) and a relatively large Delta E-ST of 0.2 eV. In isolated BF2 molecules, intramolecular rISC is slow (delayed lifetime = 260 mu s), but in aggregated films, BF2 generates intermolecular charge transfer (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 similar to 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, which is possible even at low BF2 doping concentrations of 4 wt%, resolves the conflicting requirements of fast radiative emission and low Delta E-ST in organic DF emitters.
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