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The Role of Long-Alkyl-Group Spacers in Glycolated Copolymers for High-Performance Organic Electrochemical Transistors.

Published version
Peer-reviewed

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Authors

Kim, Jingwan 
Pitsalidis, Charalampos  ORCID logo  https://orcid.org/0000-0003-3978-9865

Abstract

Semiconducting polymers with oligoethylene glycol (OEG) sidechains have attracted strong research interest for organic electrochemical transistor (OECT) applications. However, key molecular design rules for high-performance OECTs via efficient mixed electronic/ionic charge transport are still unclear. In this work, new glycolated copolymers (gDPP-TTT and gDPP-TTVTT) with diketopyrrolopyrrole (DPP) acceptor and thiophene (T) and vinylene (V) thiophene-based donor units are synthesized and characterized for accumulation mode OECTs, where a long-alkyl-group (C12 ) attached to the DPP unit acts as a spacer distancing the OEG groups from the polymer backbone. gDPP-TTVTT shows the highest OECT transconductance (61.9 S cm-1 ) and high operational stability, compared to gDPP-TTT and their alkylated counterparts. Surprisingly, gDPP-TTVTT also shows high electronic charge mobility in a field-effect transistor, suggesting efficient ion injection/diffusion without hindering its efficient electronic charge transport. The elongated donor unit (TTVTT) facilitates hole polaron formation to be more localized to the donor unit, leading to faster and easier polaron formation with less impact on polymer structure during OECT operation, as opposed to the TTT unit. This is supported by molecular dynamics simulation. These simultaneously high electronic and ionic charge-transport properties are achieved due to the long-alkyl-group spacer in amphipathic sidechains, providing an important molecular design rule for glycolated copolymers.

Description

Funder: UK Department for Business, Energy and Industrial Strategy


Funder: National Measurement System

Keywords

accumulation mode, amphipathic sidechains, conjugated polymers, long-alkyl-group spacers, organic electrochemical transistors

Journal Title

Adv Mater

Conference Name

Journal ISSN

0935-9648
1521-4095

Volume Title

Publisher

Wiley
Sponsorship
Engineering and Physical Sciences Research Council (EP/J021199/1)