Liu Di, Zhao Yinghan, Zhang Jianqi, Wei Zhixiang, Liu Yunqi, Wang Yang
Laboratory of Molecular Materials and Devices, State Key Laboratory of Molecular Engineering of Polymers, Department of Materials Science, Fudan University, 2005, Songhu Road, Shanghai, 200438, China.
Laboratory of Advanced Materials, Fudan University, 2005 Songhu Road, Shanghai, 200438, China.
Angew Chem Int Ed Engl. 2024 Apr 22;63(17):e202400061. doi: 10.1002/anie.202400061. Epub 2024 Mar 20.
The lack of ambipolar polymers with balanced hole (μ) and electron mobilities (μ) >10 cm V s is the main bottleneck for developing organic integrated circuits. Herein, we show the design and synthesis of a π-extended selenium-containing acceptor-dimeric unit, namely benzo[c][1,2,5]selenadiazol-4-yl)ethane (BBSeE), to address this dilemma. In comparison to its sulfur-counterpart, BBSeE demonstrates enlarged co-planarity, selective noncovalent interactions, polarized Se-N bond, and higher electron affinity. The successful stannylation of BBSeE offers a great opportunity to access acceptor-acceptor copolymer pN-BBSeE, which shows a narrower band gap, lower-lying lowest unoccupied molecular orbital level (-4.05 eV), and a higher degree of backbone planarity. Consequently, the pN-BBSeE-based organic transistors display an ideally balanced ambipolar transporting property with μ and μ of 10.65 and 10.72 cm V s, respectively. To the best of our knowledge, the simultaneous μ/μ values >10.0 cm V s are the best performances ever reported for ambipolar polymers. In addition, pN-BBSeE shows an excellent shelf-storage stability, retaining over 85 % of the initial mobility values after two months storage. Our study demonstrates the π-extended acceptor-dimeric BBSeE is a promising acceptor building block for constructing high-performance ambipolar polymers applied in next-generation organic integrated circuit.
缺乏空穴迁移率（μh）和电子迁移率（μe）均大于10 cm² V⁻¹ s⁻¹的双极性聚合物是开发有机集成电路的主要瓶颈。在此，我们展示了一种π-扩展的含硒受体二聚体单元，即苯并[c][1,2,5]硒二唑-4-基）乙烷（BBSeE）的设计与合成，以解决这一困境。与含硫类似物相比，BBSeE表现出更大的共平面性、选择性非共价相互作用、极化的Se-N键和更高的电子亲和力。BBSeE的成功锡基化提供了一个获得受体-受体共聚物pN-BBSeE的绝佳机会，该共聚物显示出更窄的带隙、更低的最低未占据分子轨道能级（-4.05 eV）和更高的主链平面度。因此，基于pN-BBSeE的有机晶体管表现出理想的平衡双极性传输特性，μh和μe分别为10.65和10.72 cm² V⁻¹ s⁻¹。据我们所知，μh/μe值同时大于10.0 cm² V⁻¹ s⁻¹是双极性聚合物迄今报道的最佳性能。此外，pN-BBSeE表现出优异的货架储存稳定性，储存两个月后仍保留超过85%的初始迁移率值。我们的研究表明，π-扩展的受体二聚体BBSeE是构建应用于下一代有机集成电路的高性能双极性聚合物的有前途的受体构建单元。
