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Mechanical, Morphological, and Charge Transport Properties of NDI Polymers with Variable Built-in ?-Conjugation Lengths Probed by Simulation and Experiment
Northwestern Univ, IL 60208 USA; Northwestern Univ, IL 60208 USA; Univ Elect Sci & Technol China, Peoples R China; City Univ Hong Kong, Peoples R China.
Chalmers Univ Technol, Sweden.
Birla Inst Technol & Sci, India.
Northwestern Univ, IL 60208 USA; Northwestern Univ, IL 60208 USA.
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2024 (English)In: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, Vol. 34, no 4, article id 2310071Article in journal (Refereed) Published
Abstract [en]

Mechanically deformable polymeric semiconductors are a key material for fabricating flexible organic thin-film transistors (FOTFTs)-the building block of electronic circuits and wearable electronic devices. However, for many pi-conjugated polymers achieving mechanical deformability and efficient charge transport remains challenging. Here the effects of polymer backbone bending stiffness and film microstructure on mechanical flexibility and charge transport are investigated via experimental and computational methods for a series of electron-transporting naphthalene diimide (NDI) polymers having differing extents of pi-conjugation. The results show that replacing increasing amounts of the pi-conjugated comonomer dithienylvinylene (TVT) with the pi-nonconjugated comonomer dithienylethane (TET) in the backbone of the fully pi-conjugated polymeric semiconductor, PNDI-TVT100 (yielding polymeric series PNDI-TVTx, 100 >= x >= 0), lowers backbone rigidity, degree of texturing, and pi-pi stacking interactions between NDI moieties. Importantly, this comonomer substitution increases the mechanical robustness of PNDI-TVTx while retaining efficient charge transport. Thus, reducing the TVT content of PNDI-TVTx suppresses film crack formation and dramatically stabilizes the field-effect electron mobility upon bending (e.g., 2 mm over 2000 bending cycles). This work provides a route to tune pi-pi stacking in pi-conjugated polymers while simultaneously promoting mechanical flexibility and retaining good carrier mobility in FOTFTs.

Place, publisher, year, edition, pages
WILEY-V C H VERLAG GMBH , 2024. Vol. 34, no 4, article id 2310071
Keywords [en]
de-conjugation; flexible organic thin-film transistors; molecular dynamics simulation; pi-conjugated; pi-pi stacking
National Category
Condensed Matter Physics
Identifiers
URN: urn:nbn:se:liu:diva-198965DOI: 10.1002/adfm.202310071ISI: 001084821200001OAI: oai:DiVA.org:liu-198965DiVA, id: diva2:1809976
Note

Funding Agencies|D.Z., D.K., and S.G. contributed equally to this work. A.F. and T.J.M. gratefully acknowledge financial support by AFOSR grant FA9550-22-1-0423, Northwestern University MRSEC grant NSF DMR-1720139, U.S. Department of Commerce, National Institute of Standar [FA9550-22-1-0423]; AFOSR [DMR-1720139]; Northwestern University MRSEC grant NSF [70NANB19H005]; U.S. Department of Commerce, National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD) [DMR-1720139, ECCS-1542205]; Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF); State of Illinois; US DOE Office of Science [DE-AC02-06CH11357]; US DOE [DMR-2223922]; NSF [2016-05990]; Swedish Research Council (VR) [SRG/2021/002169]; SERB

Available from: 2023-11-06 Created: 2023-11-06 Last updated: 2024-10-01Bibliographically approved

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Zozoulenko, Igor

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