The entangled triplet pair state in acene and heteroacene materials

Chaw Keong Yong, Andrew J. Musser, Sam L. Bayliss, Steven Lukman, Hiroyuki Tamura, Olga Bubnova, Rawad K. Hallani, Aurélie Meneau, Roland Resel, Munetaka Maruyama, Shu Hotta, Laura M. Herz, David Beljonne, John E. Anthony, Jenny Clark, Henning Sirringhaus

Research output: Contribution to journalArticle

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.
Original languageEnglish
Article number15953
Number of pages12
JournalNature Communications
Volume8
DOIs
Publication statusPublished - 2017

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    Yong, C. K., Musser, A. J., Bayliss, S. L., Lukman, S., Tamura, H., Bubnova, O., ... Sirringhaus, H. (2017). The entangled triplet pair state in acene and heteroacene materials. Nature Communications , 8, [15953]. https://doi.org/10.1038/ncomms15953