Activated singlet exciton fission in a semiconducting polymer

Andrew J. Musser, Mohammed Al-Hashimi, Margherita Maiuri, Daniele Brida, Martin Heeney, Giulio Cerullo, Richard H. Friend, Jenny Clark

Research output: Contribution to journalArticle

89 Citations (Scopus)

Abstract

Singlet exciton fission is a spin-allowed process to generate two triplet excitons from a single absorbed photon. This phenomenon offers great potential in organic photovoltaics, but the mechanism remains poorly understood. Most reports to date have addressed intermolecular fission within small-molecular crystals. However, through appropriate chemical design chromophores capable of intramolecular fission can also be produced. Here we directly observe sub-100 fs activated singlet fission in a semiconducting poly(thienylenevinylene). We demonstrate that fission proceeds directly from the initial 1Bu exciton, contrary to current models that involve the lower-lying 2Ag exciton. In solution, the generated triplet pairs rapidly recombine and decay through the 2Ag state. In films, exciton diffusion breaks this symmetry and we observe long-lived triplets which form charge-transfer states in photovoltaic blends.

Original languageEnglish
Pages (from-to)12747-12754
Number of pages8
JournalJournal of the American Chemical Society
Volume135
Issue number34
DOIs
Publication statusPublished - 28 Aug 2013
Externally publishedYes

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Semiconducting polymers
Excitons
Polymers
Molecular crystals
Crystal symmetry
Chromophores
Photons
Charge transfer
LDS 751

ASJC Scopus subject areas

  • Chemistry(all)
  • Catalysis
  • Biochemistry
  • Colloid and Surface Chemistry

Cite this

Musser, A. J., Al-Hashimi, M., Maiuri, M., Brida, D., Heeney, M., Cerullo, G., ... Clark, J. (2013). Activated singlet exciton fission in a semiconducting polymer. Journal of the American Chemical Society, 135(34), 12747-12754. https://doi.org/10.1021/ja405427j

Activated singlet exciton fission in a semiconducting polymer. / Musser, Andrew J.; Al-Hashimi, Mohammed; Maiuri, Margherita; Brida, Daniele; Heeney, Martin; Cerullo, Giulio; Friend, Richard H.; Clark, Jenny.

In: Journal of the American Chemical Society, Vol. 135, No. 34, 28.08.2013, p. 12747-12754.

Research output: Contribution to journalArticle

Musser, AJ, Al-Hashimi, M, Maiuri, M, Brida, D, Heeney, M, Cerullo, G, Friend, RH & Clark, J 2013, 'Activated singlet exciton fission in a semiconducting polymer', Journal of the American Chemical Society, vol. 135, no. 34, pp. 12747-12754. https://doi.org/10.1021/ja405427j
Musser, Andrew J. ; Al-Hashimi, Mohammed ; Maiuri, Margherita ; Brida, Daniele ; Heeney, Martin ; Cerullo, Giulio ; Friend, Richard H. ; Clark, Jenny. / Activated singlet exciton fission in a semiconducting polymer. In: Journal of the American Chemical Society. 2013 ; Vol. 135, No. 34. pp. 12747-12754.
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