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Polaron Delocalization in Donor–Acceptor Polymers and its Impact on Organic Electrochemical Transistor Performance
Author(s) -
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
Publication year - 2021
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.202014078
Subject(s) - delocalized electron , polaron , polymer , acceptor , conjugated system , conductive polymer , materials science , nanotechnology , rational design , chemistry , chemical physics , organic chemistry , physics , composite material , condensed matter physics , quantum mechanics , electron
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.