Abstract
Entanglement of states is one of the most surprising and counter-intuitive consequences of quantum mechanics, with potent applications in cryptography and computing. In organic materials, one particularly significant manifestation is the spin-entangled triplet-pair state, which mediates the spin-conserving fission of one spin-0 singlet exciton into two spin-1 triplet excitons. Despite long theoretical and experimental exploration, the nature of the triplet-pair state and inter-triplet interactions have proved elusive. Here we use a range of organic semiconductors that undergo singlet exciton fission to reveal the photophysical properties of entangled triplet-pair states. We find that the triplet pair is bound with respect to free triplets with an energy that is largely material independent (∼30 meV). During its lifetime, the component triplets behave cooperatively as a singlet and emit light through a Herzberg-Teller-type mechanism, resulting in vibronically structured photoluminescence. In photovoltaic blends, charge transfer can occur from the bound triplet pairs with >100% photon-to-charge conversion efficiency.
Document Type
Article
Publication Date
7-12-2017
Digital Object Identifier (DOI)
https://doi.org/10.1038/ncomms15953
Funding Information
We thank the G8 Research Councils Initiative on Multilateral Research Funding (EPSRC EP/K025651; US National Science Foundation CMM1-1255494; Japanese Society for the Promotion of Science). J.C. thanks the University of Sheffield for a VC fellowship. A.J.M., J.C. and S.L.B. thank EPSRC (EP/M025330, EP/M01083X and EP/M025330). The work in Mons is supported by BELSPO through the PAI P6/27 Functional Supramolecular Systems project and by the Belgian National Fund for Scientific Research FNRS/F.R.S. D.B. is a Research Director of FNRS.
Related Content
The data that support the findings shown in both the main figures and Supplementary Figures in this study are available with the identifier https://doi.org/10.17863/CAM.9032.
Repository Citation
Yong, Chaw Keong; Musser, Andrew J.; Bayliss, Sam L.; Lukman, Steven; Tamura, Hiroyuki; Bubnova, Olga; Hallani, Rawad; Meneau, Aurélie; Resel, Roland; Maruyama, Munetaka; Hotta, Shu; Herz, Laura M.; Beljonne, David; Anthony, John E.; Clark, Jenny; and Sirringhaus, Henning, "The Entangled Triplet Pair State in Acene and Heteroacene Materials" (2017). Chemistry Faculty Publications. 99.
https://uknowledge.uky.edu/chemistry_facpub/99
Supplementary Information
Notes/Citation Information
Published in Nature Communications, v. 8, article no. 15953, p. 1-12.
© The Author(s) 2017
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/