Robust singlet fission in pentacene thin films with tuned charge transfer interactions

Singlet fission, the spin-allowed photophysical process converting an excited singlet state into two triplet states, has attracted significant attention for device applications. Research so far has focused mainly on the understanding of singlet fission in pure materials, yet blends offer the promise...

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Autores principales: Broch, K., Dieterle, J., Branchi, F., Hestand, N. J., Olivier, Y., Tamura, H., Cruz, C., Nichols, V. M., Hinderhofer, A., Beljonne, D., Spano, F. C., Cerullo, G., Bardeen, C. J., Schreiber, F.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2018
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5838205/
https://www.ncbi.nlm.nih.gov/pubmed/29507287
http://dx.doi.org/10.1038/s41467-018-03300-1
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author Broch, K.
Dieterle, J.
Branchi, F.
Hestand, N. J.
Olivier, Y.
Tamura, H.
Cruz, C.
Nichols, V. M.
Hinderhofer, A.
Beljonne, D.
Spano, F. C.
Cerullo, G.
Bardeen, C. J.
Schreiber, F.
author_facet Broch, K.
Dieterle, J.
Branchi, F.
Hestand, N. J.
Olivier, Y.
Tamura, H.
Cruz, C.
Nichols, V. M.
Hinderhofer, A.
Beljonne, D.
Spano, F. C.
Cerullo, G.
Bardeen, C. J.
Schreiber, F.
author_sort Broch, K.
collection PubMed
description Singlet fission, the spin-allowed photophysical process converting an excited singlet state into two triplet states, has attracted significant attention for device applications. Research so far has focused mainly on the understanding of singlet fission in pure materials, yet blends offer the promise of a controlled tuning of intermolecular interactions, impacting singlet fission efficiencies. Here we report a study of singlet fission in mixtures of pentacene with weakly interacting spacer molecules. Comparison of experimentally determined stationary optical properties and theoretical calculations indicates a reduction of charge-transfer interactions between pentacene molecules with increasing spacer molecule fraction. Theory predicts that the reduced interactions slow down singlet fission in these blends, but surprisingly we find that singlet fission occurs on a timescale comparable to that in pure crystalline pentacene. We explain the observed robustness of singlet fission in such mixed films by a mechanism of exciton diffusion to hot spots with closer intermolecular spacings.
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spelling pubmed-58382052018-03-08 Robust singlet fission in pentacene thin films with tuned charge transfer interactions Broch, K. Dieterle, J. Branchi, F. Hestand, N. J. Olivier, Y. Tamura, H. Cruz, C. Nichols, V. M. Hinderhofer, A. Beljonne, D. Spano, F. C. Cerullo, G. Bardeen, C. J. Schreiber, F. Nat Commun Article Singlet fission, the spin-allowed photophysical process converting an excited singlet state into two triplet states, has attracted significant attention for device applications. Research so far has focused mainly on the understanding of singlet fission in pure materials, yet blends offer the promise of a controlled tuning of intermolecular interactions, impacting singlet fission efficiencies. Here we report a study of singlet fission in mixtures of pentacene with weakly interacting spacer molecules. Comparison of experimentally determined stationary optical properties and theoretical calculations indicates a reduction of charge-transfer interactions between pentacene molecules with increasing spacer molecule fraction. Theory predicts that the reduced interactions slow down singlet fission in these blends, but surprisingly we find that singlet fission occurs on a timescale comparable to that in pure crystalline pentacene. We explain the observed robustness of singlet fission in such mixed films by a mechanism of exciton diffusion to hot spots with closer intermolecular spacings. Nature Publishing Group UK 2018-03-05 /pmc/articles/PMC5838205/ /pubmed/29507287 http://dx.doi.org/10.1038/s41467-018-03300-1 Text en © The Author(s) 2018 Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.
spellingShingle Article
Broch, K.
Dieterle, J.
Branchi, F.
Hestand, N. J.
Olivier, Y.
Tamura, H.
Cruz, C.
Nichols, V. M.
Hinderhofer, A.
Beljonne, D.
Spano, F. C.
Cerullo, G.
Bardeen, C. J.
Schreiber, F.
Robust singlet fission in pentacene thin films with tuned charge transfer interactions
title Robust singlet fission in pentacene thin films with tuned charge transfer interactions
title_full Robust singlet fission in pentacene thin films with tuned charge transfer interactions
title_fullStr Robust singlet fission in pentacene thin films with tuned charge transfer interactions
title_full_unstemmed Robust singlet fission in pentacene thin films with tuned charge transfer interactions
title_short Robust singlet fission in pentacene thin films with tuned charge transfer interactions
title_sort robust singlet fission in pentacene thin films with tuned charge transfer interactions
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5838205/
https://www.ncbi.nlm.nih.gov/pubmed/29507287
http://dx.doi.org/10.1038/s41467-018-03300-1
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