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The role of long-alkyl-group spacers in glycolated copolymers for high performance organic electrochemical transistors
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Title: | The role of long-alkyl-group spacers in glycolated copolymers for high performance organic electrochemical transistors |
Authors: | Tan, E Kim, J Stewart, K Pitsalidis, C Kwon, S Siemons, N Kim, J Jiang, Y Frost, JM Pearce, D Tyrrell, JE Nelson, J Owens, RM Kim, Y-H Kim, J-S |
Item Type: | Journal Article |
Abstract: | Semiconducting polymers with oligoethylene glycol 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. Herein, we synthesize and characterize new glycolated copolymers (gDPP-TTT and gDPP-TTVTT) with diketopyrrolopyrrole (DPP) acceptor and thiophene-based (TTT or TTVTT) donor units for accumulation mode OECTs, where a long-alkyl-group (C12 ) attached to DPP unit acts as a spacer distancing the oligoethylene glycol 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 field-effect transistor, suggesting efficient ion injection/diffusion without hindering its efficient electronic charge transport. The elongated donor unit (TTVTT) facilitates the hole polaron formation 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 (MD) simulation. We conclude that 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. This article is protected by copyright. All rights reserved. |
Issue Date: | 7-Jul-2022 |
Date of Acceptance: | 26-Apr-2022 |
URI: | http://hdl.handle.net/10044/1/96962 |
DOI: | 10.1002/adma.202202574 |
ISSN: | 0935-9648 |
Publisher: | Wiley |
Journal / Book Title: | Advanced Materials |
Volume: | 34 |
Issue: | 27 |
Copyright Statement: | © 2022 The Authors. Advanced Materials published by Wiley-VCH GmbH This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited. |
Sponsor/Funder: | Engineering and Physical Sciences Research Council Commission of the European Communities |
Funder's Grant Number: | EP/L016702/1 742708 |
Keywords: | Science & Technology Physical Sciences Technology Chemistry, Multidisciplinary Chemistry, Physical Nanoscience & Nanotechnology Materials Science, Multidisciplinary Physics, Applied Physics, Condensed Matter Chemistry Science & Technology - Other Topics Materials Science Physics accumulation mode amphipathic sidechains conjugated polymers long-alkyl-group spacers organic electrochemical transistors CONJUGATED POLYMERS SIDE-CHAINS MOBILITY GROMACS MODE TRANSCONDUCTANCE SEMICONDUCTORS BEHAVIOR DESIGN IMPACT accumulation mode amphipathic sidechains conjugated polymers long-alkyl-group spacers organic electrochemical transistors accumulation mode amphipathic sidechain conjugated polymer long-alkyl-group spacer organic electrochemical transistor (OECT) 02 Physical Sciences 03 Chemical Sciences 09 Engineering Nanoscience & Nanotechnology |
Publication Status: | Published |
Conference Place: | Germany |
Article Number: | ARTN 2202574 |
Online Publication Date: | 2022-04-26 |
Appears in Collections: | Physics Chemistry Experimental Solid State Grantham Institute for Climate Change Faculty of Natural Sciences |
This item is licensed under a Creative Commons License