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

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

doi:10.1002/ange.202014078

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

Journal Article · Fri Feb 26 00:00:00 EST 2021 · Angewandte Chemie

DOI:https://doi.org/10.1002/ange.202014078· OSTI ID:1779992

^[1]; ^[2]; ^[3]; ^[4]; Hidalgo, Tania Cecilia ^[2]; ^[2]; ^[5]; ^[6]; ^[7]; ^[7]; ^[1]; ^[8]; ^[2]; ^[9]

University of Oxford Department of Chemistry Oxford OX1 3TA UK
King Abdullah University of Science and Technology (KAUST) Biological and Environmental Science and Engineering Division Thuwal 23955-6900 Saudi Arabia
University of Kentucky Department of Chemistry Lexington KY 40506-0055 USA
Northwestern University Department of Biomedical Engineering Chicago IL 60208 USA
King Abdullah University of Science and Technology (KAUST) Physical Science and Engineering Division Thuwal 23955-6900 Saudi Arabia
Stanford University TomKatCenter for Sustainable Energy Stanford CA 94305-4125 USA
Imperial College London Department of Chemistry and Center for Plastic Electronics London W12 0BZ UK
Northwestern University Department of Biomedical Engineering Chicago IL 60208 USA, Northwestern University Simpson Querrey Institute Chicago IL 60611 USA
University of Oxford Department of Chemistry Oxford OX1 3TA UK, King Abdullah University of Science and Technology (KAUST) Physical Science and Engineering Division Thuwal 23955-6900 Saudi Arabia

Abstract

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.

View Accepted Manuscript (Publisher)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1779992

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 14 Vol. 133; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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