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The role of long-alkyl-group spacers in glycolated copolymers for high performance organic electrochemical transistors

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 Creative Commons