Morphological and electrical control over conjugated polymers has a great potential for the fabrication of high-performance organic thin-film transistors (OTFTs). Herein, we employed a multifunctional polymeric additive, namely, PBTTT-b-HTPB, to optimize the molecular packing order of an isoindigo-based model polymer (IIDSiC8) and simultaneously regulate the minority carriers for boosted transport properties in OTFTs via facile solution processing. By detailed comparative study, we demonstrated that PBTTT-b-HTPB remarkably improved the crystallinity of IIDSiC8 by forming elongated fibers with higher molecular order in a thin film, which originated from the larger size ordered solution aggregates due to the presence of the insulating block. On the other hand, the p-type conjugated block of PBTTT worked as a hole trapping center, resulting in significantly increased electron density, reduced off-current, and optimal n-type performance. Benefiting from the collaborative morphological and electrical regulation, IIDSiC8/PBTTT-b-HTPB films displayed well-aligned ordered morphology and a high electron mobility up close to 7 cm² V^–1 s^–1 together with an on/off ratio of 10⁶ in bar-coated OTFTs. The high electron mobility is among the top performance values reported for isoindigo-based polymers. Our work has achieved simultaneous optimization of film microstructures and carrier transport characteristics of polymer semiconductors, providing opportunities for the production of OTFT devices with a superior performance.

中文翻译：

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通过多功能聚合物添加剂对高迁移率共轭聚合物进行协同形态和电学调控


对共轭聚合物的形态和电学控制在制造高性能有机薄膜晶体管 （OTFT） 方面具有巨大潜力。在此，我们采用了一种多功能聚合物添加剂，即 PBTTT-b-HTPB，来优化基于异靛蓝的模型聚合物 （IIDSiC8） 的分子堆积顺序，同时通过简单的溶液处理调节少数载体以增强 OTFT 中的传输性能。通过详细的比较研究，我们证明 PBTTT-b-HTPB 通过在薄膜中形成具有更高分子级的细长纤维来显着提高 IIDSiC8 的结晶度，这源于由于绝缘块的存在而产生的较大尺寸有序的溶液聚集体。另一方面，PBTTT 的 p 型共轭嵌段用作空穴捕获中心，从而显着增加电子密度、降低关断电流和优化 n 型性能。得益于协同形态和电学调节，IIDSiC8/PBTTT-b-HTPB 薄膜在条状涂层 OTFT 中表现出对齐良好的有序形态和高电子迁移率，最高可达 7 cm^{2 V–1} s^–1 以及 10⁶ 的开/关比。高电子迁移率是 isoindigo 基聚合物报告的最高性能值之一。我们的工作实现了聚合物半导体的薄膜微结构和载流子传输特性的同步优化，为生产具有卓越性能的 OTFT 器件提供了机会。