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

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cam.issuedOnline2022-05-27
dc.contributor.authorTan, Ellasia
dc.contributor.authorKim, Jingwan
dc.contributor.authorStewart, Katherine
dc.contributor.authorPitsalidis, Charalampos
dc.contributor.authorKwon, Sooncheol
dc.contributor.authorSiemons, Nicholas
dc.contributor.authorKim, Jehan
dc.contributor.authorJiang, Yifei
dc.contributor.authorFrost, Jarvist M
dc.contributor.authorPearce, Drew
dc.contributor.authorTyrrell, James E
dc.contributor.authorNelson, Jenny
dc.contributor.authorOwens, Roisin M
dc.contributor.authorKim, Yun-Hi
dc.contributor.authorKim, Ji-Seon
dc.contributor.orcidTan, Ellasia [0000-0002-8225-9045]
dc.contributor.orcidStewart, Katherine [0000-0003-3227-982X]
dc.contributor.orcidPitsalidis, Charalampos [0000-0003-3978-9865]
dc.contributor.orcidKwon, Sooncheol [0000-0003-2799-9558]
dc.contributor.orcidSiemons, Nicholas [0000-0002-0755-3981]
dc.contributor.orcidKim, Jehan [0000-0003-3555-8015]
dc.contributor.orcidFrost, Jarvist M [0000-0003-1938-4430]
dc.contributor.orcidTyrrell, James E [0000-0002-4530-5284]
dc.contributor.orcidNelson, Jenny [0000-0003-1048-1330]
dc.contributor.orcidOwens, Roisin M [0000-0001-7856-2108]
dc.contributor.orcidKim, Yun-Hi [0000-0001-8856-4414]
dc.contributor.orcidKim, Ji-Seon [0000-0003-4715-3656]
dc.date.accessioned2022-05-27T10:00:16Z
dc.date.available2022-05-27T10:00:16Z
dc.date.issued2022-07
dc.date.submitted2022-03-20
dc.date.updated2022-05-27T10:00:16Z
dc.descriptionFunder: UK Department for Business, Energy and Industrial Strategy
dc.descriptionFunder: National Measurement System
dc.description.abstractSemiconducting 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.
dc.identifier.doi10.17863/CAM.84951
dc.identifier.eissn1521-4095
dc.identifier.issn0935-9648
dc.identifier.otheradma202202574
dc.identifier.urihttps://www.repository.cam.ac.uk/handle/1810/337539
dc.languageen
dc.language.isoeng
dc.publisherWiley
dc.publisher.urlhttp://dx.doi.org/10.1002/adma.202202574
dc.subjectaccumulation mode
dc.subjectamphipathic sidechains
dc.subjectconjugated polymers
dc.subjectlong-alkyl-group spacers
dc.subjectorganic electrochemical transistors
dc.titleThe Role of Long-Alkyl-Group Spacers in Glycolated Copolymers for High-Performance Organic Electrochemical Transistors.
dc.typeArticle
prism.publicationNameAdv Mater
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/J021199/1)
rioxxterms.licenseref.urihttp://creativecommons.org/licenses/by/4.0/
rioxxterms.versionVoR
rioxxterms.versionofrecord10.1002/adma.202202574

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