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.
| Original language | English (US) |
|---|---|
| Pages (from-to) | 7777-7785 |
| Number of pages | 9 |
| Journal | Angewandte Chemie - International Edition |
| Volume | 60 |
| Issue number | 14 |
| DOIs | |
| State | Published - Mar 29 2021 |
Funding
The authors acknowledge generous funding from KAUST. The research reported in this publication was sponsored by funding from King Abdullah University of Science and Technology Office of Sponsored Research (OSR) under awards no. OSR‐2018‐CARF/CCF‐3079, no. OSR‐2015‐CRG4‐2572 and OSR‐4106 CPF2019. We acknowledge EC FP7 Project SC2 (610115), EC H2020 (643791), and EPSRC Projects EP/G037515/1, EP/M005143/1, and EP/L016702/1. B.P. and J.R. gratefully acknowledge support from the National Science Foundation Grant No. NSF DMR‐1751308. The authors would like to thank Joseph Strzalka and Qingteng Zhang for beamline assistance. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE‐AC02‐06CH11357. A.G. acknowledges funding from the TomKat Center for Sustainable Energy at Stanford University. The authors acknowledge generous funding from KAUST. The research reported in this publication was sponsored by funding from King Abdullah University of Science and Technology Office of Sponsored Research (OSR) under awards no. OSR-2018-CARF/CCF-3079, no. OSR-2015-CRG4-2572 and OSR-4106 CPF2019. We acknowledge EC FP7 Project SC2 (610115), EC H2020 (643791), and EPSRC Projects EP/G037515/1, EP/M005143/1, and EP/L016702/1. B.P. and J.R. gratefully acknowledge support from the National Science Foundation Grant No. NSF DMR-1751308. The authors would like to thank Joseph Strzalka and Qingteng Zhang for beamline assistance. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. A.G. acknowledges funding from the TomKat Center for Sustainable Energy at Stanford University.
Keywords
- conjugated backbones
- organic electrochemical transistors
- polaron delocalization
- polymers
- semiconductors
ASJC Scopus subject areas
- Catalysis
- General Chemistry