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Davydov splitting and singlet fission in excitonically coupled pentacene dimers

Singlet fission (SF) allows two charges to be generated from the absorption of a single photon and is, therefore, potentially transformative toward improving solar energy conversion. Key to the present study of SF is the design of pentacene dimers featuring a xanthene linker that strictly places two...

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Detalles Bibliográficos
Autores principales: Basel, Bettina Sabine, Hetzer, Constantin, Zirzlmeier, Johannes, Thiel, Dominik, Guldi, Rebecca, Hampel, Frank, Kahnt, Axel, Clark, Timothy, Guldi, Dirk Michael, Tykwinski, Rik R.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Royal Society of Chemistry 2019
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6461118/
https://www.ncbi.nlm.nih.gov/pubmed/31015927
http://dx.doi.org/10.1039/c9sc00384c
Descripción
Sumario:Singlet fission (SF) allows two charges to be generated from the absorption of a single photon and is, therefore, potentially transformative toward improving solar energy conversion. Key to the present study of SF is the design of pentacene dimers featuring a xanthene linker that strictly places two pentacene chromophores in a rigid arrangement and, in turn, enforces efficient, intramolecular π-overlap that mimics interactions typically found in condensed state (e.g., solids, films, etc.). Inter-chromophore communication ensures Davydov splitting, which plays an unprecedented role toward achieving SF in pentacene dimers. Transient absorption measurements document that intramolecular SF evolves upon excitation into the lower Davydov bands to form a correlated triplet pair at cryogenic temperature. At room temperature, the two spin-correlated triplets, one per pentacene moiety within the dimers, are electronically coupled to an excimer state. The presented results are transferable to a broad range of acene morphologies including aggregates, crystals, and films.