Molecular-dipole oriented universal growth of conjugated polymers into semiconducting single-crystal thin films

Chunyan Zhao, Xilin Lai, Dawei Liu, Xinrui Guo, Jiamin Tian, Zuoyuan Dong, Shaochuan Luo, Dongshan Zhou, Lang Jiang (), Ru Huang and Ming He ()
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Chunyan Zhao: Peking University
Xilin Lai: Peking University
Dawei Liu: Chinese Academy of Sciences
Xinrui Guo: Peking University
Jiamin Tian: Shenzhen Pinghu Lab
Zuoyuan Dong: Peking University
Shaochuan Luo: Nanjing University
Dongshan Zhou: Nanjing University
Lang Jiang: Chinese Academy of Sciences
Ru Huang: Peking University
Ming He: Peking University

Nature Communications, 2025, vol. 16, issue 1, 1-9

Abstract: Abstract Precise control over crystallinity and morphology of conjugated polymers (CPs) is essential for progressing organic electronics. However, manufacturing single-crystal thin films of CPs presents substantial challenges due to their complex molecular structures, distorted chain conformations, and unbalanced crystallization kinetics. In this work, we demonstrate a universal nanoconfined molecular-dipole orientating strategy to craft high-quality single-crystal thin films for a variety of CPs, spanning from traditional thiophene- and theinothiophene-based homopolymers to diketopyrrolopyrrole- (i.e., p-type) and naphthalene-based (i.e., n-type) donor-acceptor copolymers. Central to this strategy is the synergetic manipulations of molecular dipoles, π-π stackings, and alkyl-alkyl interactions of CPs within our rationally-designed spatial-electrostatic confinement capacitor, which facilitates the rotation of conjugated backbones and the alignment of π-π stackings into microscale-sized single-crystal thin films. A minimal energetic disorder of 25 meV that below the thermal fluctuation energy kBT at room temperature, as well as an excellent transistor mobility of 15.5 cm2V−1s−1 are achieved, marking a significant step towards controllable growths of conjugated-polymer single-crystal thin films that hold a cornerstone for high-performance organic electronic devices.

Date: 2025
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DOI: 10.1038/s41467-025-56757-2

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