Tailoring Multiscale Crystalline Structures in Conjugated Polymers: Bridging Fundamental Insights and Applications in Organic Field-Effect Transistors

作者：Hao Zheng, Yanan Guo, Zhiqun Lin, Juan Peng · 发表于：Accounts of Materials Research · 年份：2025 · DOI：10.1021/accountsmr.5c00193 · 被引用次数：9 · 研究领域：Organic Electronics and Photovoltaics、Conducting polymers and applications、Perovskite Materials and Applications

Conspectus π-Conjugated polymers are a class of semirigid macromolecules composed of unsaturated building blocks, where π-electron delocalization along the polymer backbones imparts exceptional optoelectronic properties. The charge transport in these polymers depends on intrinsic molecular structures as well as microstructural features, such as chain conformation, polymorphism, crystal orientation, and phase separation across solid-state length scales. Despite significant advancements in synthetic methodologies and iterative molecular design, progress in controlling the crystallization behavior and microstructural formation of conjugated polymers remains relatively limited. This limitation arises primarily from the distinct rigid backbone and flexible side chains and weak, complex interactions. Therefore, effectively controlling the crystallization behavior of conjugated polymers is essential to unravel the intricate relationship between their microstructure and device performance and to enable their deployment in optoelectronic applications. In this Account, we highlight our recent efforts to control and elucidate the formation mechanisms of three important and representative microstructures across distinct levels: polymorphism (interchain packing), crystal orientation (lamellar packing), and multicomponent cocrystallization (multicomponent phase behavior), and to investigate their impact on charge-transport properties. Polymorphism is one of the most fundamental structural ...