Emissive spin-0 triplet-pairs are a direct product of triplet–triplet annihilation in pentacene single crystals and anthradithiophene films

David G. Bossanyi, Maik Matthiesen, Shuangqing Wang, Joel A. Smith, Rachel C. Kilbride, James D. Shipp, Dimitri Chekulaev, Emma Holland, John E. Anthony, Jana Zaumseil, Andrew J. Musser, Jenny Clark

Research output: Contribution to journalArticlepeer-review

23 Scopus citations


Singlet fission and triplet–triplet annihilation represent two highly promising ways of increasing the efficiency of photovoltaic devices. Both processes are believed to be mediated by a biexcitonic triplet-pair state, 1(TT). Recently however, there has been debate over the role of 1(TT) in triplet–triplet annihilation. Here we use intensity-dependent, low-temperature photoluminescence measurements, combined with kinetic modelling, to show that distinct 1(TT) emission arises directly from triplet–triplet annihilation in high-quality pentacene single crystals and anthradithiophene (diF-TES-ADT) thin films. This work demonstrates that a real, emissive triplet-pair state acts as an intermediate in both singlet fission and triplet–triplet annihilation and that this is true for both endo- and exothermic singlet fission materials. [Figure not available: see fulltext.]

Original languageEnglish
Pages (from-to)163-171
Number of pages9
JournalNature Chemistry
Issue number2
StatePublished - Feb 2021

Bibliographical note

Funding Information:
D.G.B. and J.A.S. thank the EPSRC Centre for Doctoral Training in New and Sustainable Photovoltaics (EP/L01551X/1) for studentship support. J.Z. and M.M. acknowledge funding by the Deutsche Forschungsgemeinschaft via the Collaborative Research Center ‘N-Heteropolycycles as Functional Materials’ (SFB 1249, C06). J.D.S. thanks the Grantham Centre for Sustainable Futures for studentship support. J.E.A. and E.H. thank the US NSF (CHE-1609974) for support of material synthesis. J.C., A.J.M. and S.W. thank EPSRC for funding (EP/S002103/1 and EP/M025330/1). We thank EPSRC for a Capital Equipment award (EP/L022613/1 and EP/R042802/1), which provided the Lord Porter Laser Laboratory Facility used in this study. We further thank Xenocs for their ongoing support through the X-ray scattering user programme at the University of Sheffield and we thank the EPSRC for funding the purchase of this instrument. We thank R. Jayaprakash for assistance with the polarized absorption measurement. Finally, we thank P. Green and M.W.B. Wilson from the University of Toronto for providing us with inorganic semiconductor nanocrystals for triplet sensitization.

Publisher Copyright:
© 2020, The Author(s), under exclusive licence to Springer Nature Limited.

ASJC Scopus subject areas

  • Chemistry (all)
  • Chemical Engineering (all)


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