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Issue 13, 2019
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Davydov splitting and singlet fission in excitonically coupled pentacene dimers

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Abstract

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.

Graphical abstract: Davydov splitting and singlet fission in excitonically coupled pentacene dimers

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Supplementary files

Article information


Submitted
23 Jan 2019
Accepted
21 Feb 2019
First published
06 Mar 2019

This article is Open Access
All publication charges for this article have been paid for by the Royal Society of Chemistry

Chem. Sci., 2019,10, 3854-3863
Article type
Edge Article

Davydov splitting and singlet fission in excitonically coupled pentacene dimers

B. S. Basel, C. Hetzer, J. Zirzlmeier, D. Thiel, R. Guldi, F. Hampel, A. Kahnt, T. Clark, D. M. Guldi and R. R. Tykwinski, Chem. Sci., 2019, 10, 3854
DOI: 10.1039/C9SC00384C

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