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Hot-exciton harvesting via through-space single-molecule based white-light emission and optical waveguides.


ABSTRACT: Through-space donor-alkyl bridge-acceptor (D-σ-A) luminogens are developed as new organic single-molecule white light emitters (OSMWLEs) involving multiple higher lying singlet (S n ) and triplet (T m ) states (hot-excitons). Experimental and theoretical results confirm the origin of white light emission due to the co-existence of prompt fluorescence from locally excited states, thermally activated delayed fluorescence (TADF), and fast/slow dual phosphorescence color mixing simultaneously. Notably, the fast phosphorescence was observed due to trace amounts of isomeric impurities from commercial carbazole, while H-/J-aggregation resulted in slow phosphorescence. Crystal structure-packing-property analysis revealed that the alkyl chain length induced supramolecular self-assembly greatly influenced the solid-state optical properties. Remarkably, the 1D-microrod crystals of OSMWLEs demonstrated the first examples of triplet harvesting waveguides by self-guiding the generated phosphorescence through light propagation along their longitudinal axis. This work thus highlights an uncommon design strategy to achieve multi-functional OSMWLEs with in-depth mechanistic insights and optical waveguiding applications making them a potentially new class of white emissive materials.

SUBMITTER: Barman D 

PROVIDER: S-EPMC9365089 | biostudies-literature | 2022 Aug

REPOSITORIES: biostudies-literature

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Hot-exciton harvesting <i>via</i> through-space single-molecule based white-light emission and optical waveguides.

Barman Debasish D   Annadhasan Mari M   Chandrasekar Rajadurai R   Iyer Parameswar Krishnan PK  

Chemical science 20220704 31


Through-space donor-alkyl bridge-acceptor (D-σ-A) luminogens are developed as new organic single-molecule white light emitters (OSMWLEs) involving multiple higher lying singlet (S <sub><i>n</i></sub> ) and triplet (T <sub><i>m</i></sub> ) states (hot-excitons). Experimental and theoretical results confirm the origin of white light emission due to the co-existence of prompt fluorescence from locally excited states, thermally activated delayed fluorescence (TADF), and fast/slow dual phosphorescenc  ...[more]

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