Issue 1, 2024

A skeletal randomization strategy for high-performance quinoidal-aromatic polymers

Abstract

Enhancing the solution-processability of conjugated polymers (CPs) without diminishing their thin-film crystallinity is crucial for optimizing charge transport in organic field-effect transistors (OFETs). However, this presents a classic “Goldilocks zone” dilemma, as conventional solubility-tuning methods for CPs typically yield an inverse correlation between solubility and crystallinity. To address this fundamental issue, a straightforward skeletal randomization strategy is implemented to construct a quinoid-donor conjugated polymer, PA4T-Ra, that contains para-azaquinodimethane (p-AQM) and oligothiophenes as repeat units. A systematic study is conducted to contrast its properties against polymer homologues constructed following conventional solubility-tuning strategies. An unusually concurrent improvement of solubility and crystallinity is realized in the random polymer PA4T-Ra, which shows moderate polymer chain aggregation, the highest crystallinity and the least lattice disorder. Consequently, PA4T-Ra-based OFETs, fabricated under ambient air conditions, deliver an excellent hole mobility of 3.11 cm2 V−1 s−1, which is about 30 times higher than that of the other homologues and ranks among the highest for quinoidal CPs. These findings debunk the prevalent assumption that a random polymer backbone sequence results in decreased crystallinity. The considerable advantages of the skeletal randomization strategy illuminate new possibilities for the control of polymer aggregation and future design of high-performance CPs, potentially accelerating the development and commercialization of organic electronics.

Graphical abstract: A skeletal randomization strategy for high-performance quinoidal-aromatic polymers

Supplementary files

Article information

Article type
Communication
Submitted
21 Jul 2023
Accepted
01 Nov 2023
First published
02 Nov 2023

Mater. Horiz., 2024,11, 283-296

A skeletal randomization strategy for high-performance quinoidal-aromatic polymers

Q. Zhou, C. Liu, J. Li, R. Xie, G. Zhang, X. Ge, Z. Zhang, L. Zhang, J. Chen, X. Gong, C. Yang, Y. Wang, Y. Liu and X. Liu, Mater. Horiz., 2024, 11, 283 DOI: 10.1039/D3MH01143G

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