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Cited 6 time in webofscience Cited 13 time in scopus
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The Role of Long-Alkyl-Group Spacers in Glycolated Copolymers for High-Performance Organic Electrochemical Transistorsopen access

Authors
Tan, EllasiaKim, JingwanStewart, KatherinePitsalidis, CharalamposKwon, SooncheolSiemons, NicholasKim, JehanJiang, YifeiFrost, Jarvist M.Pearce, DrewTyrrell, James E.Nelson, JennyOwens, Roisin M.Kim, Yun-HiKim, Ji-Seon
Issue Date
Jul-2022
Publisher
WILEY-V C H VERLAG GMBH
Keywords
accumulation mode; amphipathic sidechains; conjugated polymers; long-alkyl-group spacers; organic electrochemical transistors
Citation
ADVANCED MATERIALS, v.34, no.27
Indexed
SCIE
SCOPUS
Journal Title
ADVANCED MATERIALS
Volume
34
Number
27
URI
https://scholarworks.bwise.kr/gnu/handle/sw.gnu/1086
DOI
10.1002/adma.202202574
ISSN
0935-9648
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 (C-12) 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.
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