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, Aurelie Meneau, Roland Resel, Munetaka Maruyama, Shu Hotta, Laura M. Herz, David Beljonne, John E. Anthony, Jenny Clark, Henning Sirringhaus

Research output: Contribution to journalArticlepeer-review

141 Scopus citations


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
JournalNature Communications
StatePublished - Jul 12 2017

Bibliographical note

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).

Publisher Copyright:
© The Author(s) 2017.

ASJC Scopus subject areas

  • Chemistry (all)
  • Biochemistry, Genetics and Molecular Biology (all)
  • General
  • Physics and Astronomy (all)


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