Linear conjugated polymers have attracted significant attention in organic electronics in recent decades. However, despite intrachain π-delocalization, interchain hopping is their transport bottleneck. In contrast, two-dimensional (2D) conjugated polymers, as represented by 2D π-conjugated covalent organic frameworks (2D c-COFs), can provide multiple conjugated strands to enhance the delocalization of charge carriers in space. Herein, we demonstrate the first example of thiophene-based 2D poly(arylene vinylene)s (PAVs, 2DPAV-BDT-BT and 2DPAV-BDT-BP, BDT=benzodithiophene, BT=bithiophene, BP=biphenyl) via Knoevenagel polycondensation. Compared with 2DPAV-BDT-BP, the fully thiophene-based 2DPAV-BDT-BT exhibits enhanced planarity and π-delocalization with a small band gap (1.62 eV) and large electronic band dispersion, as revealed by the optical absorption and density functional calculations. Remarkably, temperature-dependent terahertz spectroscopy discloses a unique band-like transport and outstanding room-temperature charge mobility for 2DPAV-BDT-BT (65 cm2 V−1 s−1), which far exceeds that of the linear PAVs, 2DPAV-BDT-BP, and the reported 2D c-COFs in the powder form. This work highlights the great potential of thiophene-based 2D PAVs as candidates for high-performance opto-electronics.
| Identifer | oai:union.ndltd.org:DRESDEN/oai:qucosa:de:qucosa:89226 |
| Date | 24 January 2024 |
| Creators | Liu, Yamei, Heng, Yu, Hongde, Liao, Zhongquan, Paasch, Silvia, Xu, Shunqi, Zhao, Ruyan, Brunner, Eike, Bonn, Mischa, Wang, Hai I., Heine, Thomas, Wang, Mingchao, Mai, Yiyong, Feng, Xinliang |
| Publisher | Wiley-VCH |
| Source Sets | Hochschulschriftenserver (HSSS) der SLUB Dresden |
| Language | English |
| Detected Language | English |
| Type | info:eu-repo/semantics/publishedVersion, doc-type:article, info:eu-repo/semantics/article, doc-type:Text |
| Rights | info:eu-repo/semantics/openAccess |
| Relation | 1433-7851, 1521-3773, e202305978, 10.1002/anie.202305978, info:eu-repo/grantAgreement/European Commission/H2020 | ERC | ERC-COG/819698//Development of Thiophene Based Conjugated Polymers in Two Dimensions/T2DCP, info:eu-repo/grantAgreement/Deutsche Forschungsgemeinschaft/Sonderforschungsbereiche/417590517//Chemie der synthetischen zweidimensionalen Materialien/SFB 1415, info:eu-repo/grantAgreement/European Commission/H2020 | RIA/899205//Proto-Opto-Electro-Mechanical Hybrid Systems for Generation-Next Bionic Devices/PROGENY, info:eu-repo/grantAgreement/European Commission/H2020 | SGA-RIA/881603//Graphene Flagship Core Project 3/GrapheneCore3, info:eu-repo/grantAgreement/European Commission/H2020 | RIA/101008701//Emerging Printed Electronics Research Infrastructure/EMERGE, info:eu-repo/grantAgreement/Deutsche Forschungsgemeinschaft/Excellenzcluster/194636624//Zentrum für Perspektiven in der Elektronik Dresden/EXC 1056 |
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