Polaron Delocalization in Donor–Acceptor Polymers and its Impact on Organic Electrochemical Transistor Performance

Maximilian Moser*, Achilleas Savva, Karl Thorley, Bryan D. Paulsen, Tania Cecilia Hidalgo, David Ohayon, Hu Chen, Alexander Giovannitti, Adam Marks, Nicola Gasparini, Andrew Wadsworth, Jonathan Rivnay, Sahika Inal, Iain McCulloch

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

58 Scopus citations


Donor–acceptor (D-A) polymers are promising materials for organic electrochemical transistors (OECTs), as they minimize detrimental faradaic side-reactions during OECT operation, yet their steady-state OECT performance still lags far behind their all-donor counterparts. We report three D-A polymers based on the diketopyrrolopyrrole unit that afford OECT performances similar to those of all-donor polymers, hence representing a significant improvement to the previously developed D-A copolymers. In addition to improved OECT performance, DFT simulations of the polymers and their respective hole polarons also reveal a positive correlation between hole polaron delocalization and steady-state OECT performance, providing new insights into the design of OECT materials. Importantly, we demonstrate how polaron delocalization can be tuned directly at the molecular level by selection of the building blocks comprising the polymers’ conjugated backbone, thus paving the way for the development of even higher performing OECT polymers.

Original languageEnglish (US)
Pages (from-to)7777-7785
Number of pages9
JournalAngewandte Chemie - International Edition
Issue number14
StatePublished - Mar 29 2021


  • conjugated backbones
  • organic electrochemical transistors
  • polaron delocalization
  • polymers
  • semiconductors

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)


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