共轭体系
基态
电阻率和电导率
开壳
壳体(结构)
聚合物
电导率
材料科学
自旋(空气动力学)
化学物理
化学
凝聚态物理
纳米技术
物理
原子物理学
物理化学
热力学
有机化学
复合材料
量子力学
作者
Houji Cai,Haoran Tang,Tianzuo Wang,Chenhui Xu,Jinxin Xie,Muyi Fu,Xi Luo,Zhengwei Hu,Jingjing Chang,Yunfeng Deng,Guangwu Li,Chunchen Liu,Fei Huang,Yong Cao
标识
DOI:10.1002/anie.202402375
摘要
Open-shell conjugated polymers with a high intrinsic conductivity and high-spin ground state hold considerable promise for applications in organic electronics and spintronics. Herein, two novel acceptor-acceptor (A-A) conjugated polymers based on a highly electron-deficient quinoidal benzodifurandione unit have been developed, namely DPP-BFDO-Th and DPP-BFDO. The incorporation of the quinoidal moiety into the polymers backbones enables deeply aligned lower-lying lowest unoccupied molecular orbital (LUMO) levels of below -4.0 eV. Notably, DPP-BFDO exhibits an exceptionally low LUMO (-4.63 eV) and a high-spin ground state characterized by strong diradical characters. Moreover, a self-doping through intermolecular charge-transfer is observed for DPP-BFDO, as evidenced by X-ray photoelectron spectroscopy (XPS) studies. The high carrier concentration in combination with a planar and linear conjugated backbone yields a remarkable electrical conductivity (σ) of 1.04 S cm-1 in the "undoped" native form, ranking among the highest values reported for n-type radical-based conjugated polymers. When employed as an n-type thermoelectric material, DPP-BFDO achieves a power factor of 12.59 μW m-1 K-2. Furthermore, upon n-doping, the σ could be improved to 65.68 S cm-1. This study underscores the great potential of electron-deficient quinoidal units in constructing dopant-free n-type conductive polymers with a high-spin ground state and exceptional intrinsic conductivity.
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