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Achieving ideal transistor characteristics in conjugated polymer semiconductors.

ABSTRACT: Organic thin-film transistors (OTFTs) with ideal behavior are highly desired, because nonideal devices may overestimate the intrinsic property and yield inferior performance in applications. In reality, most polymer OTFTs reported in the literature do not exhibit ideal characteristics. Supported by a structure-property relationship study of several low-disorder conjugated polymers, here, we present an empirical selection rule for polymer candidates for textbook-like OTFTs with high reliability factors (100% for ideal transistors). The successful candidates should have low energetic disorder along their backbones and form thin films with spatially uniform energetic landscapes. We demonstrate that these requirements are satisfied in the semicrystalline polymer PffBT4T-2DT, which exhibits a reliability factor (~100%) that is exceptionally high for polymer devices, rendering it an ideal candidate for OTFT applications. Our findings broaden the selection of polymer semiconductors with textbook-like OTFT characteristics and would shed light upon the molecular design criteria for next-generation polymer semiconductors.

SUBMITTER: Xiao M

PROVIDER: S-EPMC10413658 | biostudies-literature | 2023 Jun

REPOSITORIES: biostudies-literature

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Achieving ideal transistor characteristics in conjugated polymer semiconductors.

Xiao Mingfei M Ren Xinglong X Ji Kangyu K Chung Sein S Shi Xiaoyu X Han Jie J Yao Zefan Z Tao Xudong X Zelewski Szymon J SJ Nikolka Mark M Zhang Youcheng Y Zhang Zhilong Z Wang Zichen Z Jay Nathan N Jacobs Ian I Wu Weijing W Yu Han H Abdul Samad Yarjan Y Stranks Samuel D SD Kang Boseok B Cho Kilwon K Xie Jin J Yan He H Chen Shangshang S Sirringhaus Henning H

Science advances 20230602 22

Organic thin-film transistors (OTFTs) with ideal behavior are highly desired, because nonideal devices may overestimate the intrinsic property and yield inferior performance in applications. In reality, most polymer OTFTs reported in the literature do not exhibit ideal characteristics. Supported by a structure-property relationship study of several low-disorder conjugated polymers, here, we present an empirical selection rule for polymer candidates for textbook-like OTFTs with high reliability f ...[more]

PMID: 37267357

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Project description:The development of solution-processable n-type molecular semiconductors that exhibit high electron mobility (μe ≥ 0.5 cm2/(V·s)) under ambient conditions, along with high current modulation (Ion/Ioff ≥ 106-107) and near-zero turn on voltage (Von) characteristics, has lagged behind that of other semiconductors in organic field-effect transistors (OFETs). Here, we report the design, synthesis, physicochemical and optoelectronic characterizations, and OFET performances of a library of solution-processable, low-LUMO (-4.20 eV) 2,2'-(2,8-bis(3-alkylthiophen-2-yl)indeno[1,2-b]fluorene-6,12-diylidene)dimalononitrile small molecules, β,β'-Cn-TIFDMTs, having varied alkyl chain lengths (n = 8, 12, 16). An intriguing correlation is identified between the solid-isotropic liquid transition enthalpies and the solubilities, indicating that cohesive energetics, which are tuned by alkyl chains, play a pivotal role in determining solubility. The semiconductors were spin-coated under ambient conditions on densely packed (grafting densities of 0.19-0.45 chains/nm2) ultrathin (∼3.6-6.6 nm) polystyrene-brush surfaces. It is demonstrated that, on this polymer interlayer, thermally induced dispersive interactions occurring over a large number of methylene units between flexible alkyl chains (i.e., zipper effect) are critical to achieve a favorable thin-film crystallization with a proper microstructure and morphology for efficient charge transport. While C8 and C16 chains show a minimal zipper effect upon thermal annealing, C12 chains undergo an extended interdigitation involving ∼6 methylene units. This results in the formation of large crystallites having lamellar stacking ((100) coherence length ∼30 nm) in the out-of-plane direction and highly favorable in-plane π-interactions in a slipped-stacked arrangement. Uninterrupted microstructural integrity (i.e., no face-on (010)-oriented crystallites) was found to be critical to achieving high mobilities. The excellent crystallinity of the C12-substituted semiconductor thin film was also evident in the observed crystal lattice vibrations (phonons) at 58 cm-1 in low-frequency Raman scattering. Two-dimensional micrometer-sized (∼1-3 μm), sharp-edged plate-like grains lying parallel with the substrate plane were observed. OFETs fabricated by the current small molecules showed excellent n-channel behavior in ambient with μe values reaching ∼0.9 cm2/(V·s), Ion/Ioff ∼ 107-108, and Von ≈ 0 V. Our study not only demonstrates one of the highest performing n-channel OFET devices reported under ambient conditions via solution processing but also elucidates significant relationships among chemical structures, molecular properties, self-assembly from solution into a thin film, and semiconducting thin-film properties. The design rationales presented herein may open up new avenues for the development of high-electron-mobility novel electron-deficient indenofluorene and short-axis substituted donor-acceptor π-architectures via alkyl chain engineering and interface engineering.

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Achieving ideal transistor characteristics in conjugated polymer semiconductors.

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Achieving ideal transistor characteristics in conjugated polymer semiconductors.

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