[en] Two-dimensional conjugated polymers (2DCPs), composed of multiple strands of linear conjugated polymers with extended in-plane π-conjugation, are emerging crystalline semiconducting polymers for organic (opto)electronics. They are represented by two-dimensional π-conjugated covalent organic frameworks, which typically suffer from poor π-conjugation and thus low charge carrier mobilities. Here we overcome this limitation by demonstrating two semiconducting phthalocyanine-based poly(benzimidazobenzophenanthroline)-ladder-type 2DCPs (2DCP-MPc, with M = Cu or Ni), which are constructed from octaaminophthalocyaninato metal(II) and naphthalenetetracarboxylic dianhydride by polycondensation under solvothermal conditions. The 2DCP-MPcs exhibit optical bandgaps of ~1.3 eV with highly delocalized π-electrons. Density functional theory calculations unveil strongly dispersive energy bands with small electron-hole reduced effective masses of ~0.15m0 for the layer-stacked 2DCP-MPcs. Terahertz spectroscopy reveals the band transport of Drude-type free carriers in 2DCP-MPcs with exceptionally high sum mobility of electrons and holes of ~970 cm2 V-1 s-1 at room temperature, surpassing that of the reported linear conjugated polymers and 2DCPs. This work highlights the critical role of effective conjugation in enhancing the charge transport properties of 2DCPs and the great potential of high-mobility 2DCPs for future (opto)electronics.
Disciplines :
Chemistry
Author, co-author :
Wang, Mingchao ; Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Dresden, Germany
Fu, Shuai ; Max Planck Institute for Polymer Research, Mainz, Germany
Petkov, Petko ; Faculty of Chemistry and Pharmacy, University of Sofia, Sofia, Bulgaria
Fu, Yubin ; Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Dresden, Germany ; Max Planck Institute of Microstructure Physics, Halle, Germany
Zhang, Zhitao ; Anhui Province Key Laboratory of Condensed Matter Physics at Extreme Conditions, High Magnetic Field Laboratory, HFIPS, Chinese Academy of Sciences, Hefei, China
Liu, Yannan ; Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Dresden, Germany ; Max Planck Institute of Microstructure Physics, Halle, Germany
Ma, Ji ; Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Dresden, Germany ; Max Planck Institute of Microstructure Physics, Halle, Germany
Chen, Guangbo ; Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Dresden, Germany
Gali, Sai Manoj ; Université de Mons - UMONS > Faculté des Science > Service de Chimie des matériaux nouveaux
Gao, Lei; Max Planck Institute for Polymer Research, Mainz, Germany
Lu, Yang; Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Dresden, Germany ; Max Planck Institute of Microstructure Physics, Halle, Germany
Paasch, Silvia ; Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Dresden, Germany
Zhong, Haixia; Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Dresden, Germany
Steinrück, Hans-Peter; Institute of Physical Chemistry II, Friedrich-Alexander-Universität Erlangen-Nürnberg, Erlangen, Germany
Cánovas, Enrique ; Max Planck Institute for Polymer Research, Mainz, Germany ; Instituto Madrileño de Estudios Avanzados en Nanociencia (IMDEA Nanociencia), Madrid, Spain
Brunner, Eike; Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Dresden, Germany
Beljonne, David ; Université de Mons - UMONS > Faculté des Science > Service de Chimie des matériaux nouveaux
Bonn, Mischa ; Max Planck Institute for Polymer Research, Mainz, Germany
Wang, Hai I ; Max Planck Institute for Polymer Research, Mainz, Germany. wanghai@mpip-mainz.mpg.de
Dong, Renhao ; Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Dresden, Germany. renhaodong@sdu.edu.cn ; Key Laboratory of Colloid and Interface Chemistry of the Ministry of Education, School of Chemistry and Chemical Engineering, Shandong University, Jinan, China. renhaodong@sdu.edu.cn
Feng, Xinliang ; Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, Dresden, Germany. xinliang.feng@tu-dresden.de ; Max Planck Institute of Microstructure Physics, Halle, Germany. xinliang.feng@tu-dresden.de
R400 - Institut de Recherche en Science et Ingénierie des Matériaux Complexys
Funding text :
This work was financially supported by ERC Grants (T2DCP, no. 819698; FC2DMOF, no. 852909), DFG projects (CRC 1415, no. 417590517; SPP 2248, RACOF-MMIS), EU Graphene Flagship (Core3, no. 881603) and Center for Advancing Electronics Dresden. S.F. acknowledges fellowship support from the Chinese Scholarship Council (CSC). We thank Dresden Center for Nanoanalysis (DCN) and P. Formanek (IPF, Dresden) for the use of facilities. A portion of this work was performed on the Steady High Magnetic Field Facilities, High Magnetic Field Laboratory, CAS. We appreciate C. Naisa, S. Xing, W. Niu, S. Park, J. Liu, Z. Zhang, P. Zhang, B. Zhang and S. Revueta for helpful discussions and measurements. M.W. specially acknowledges J. Cui. R.D. thanks Taishan Scholars Program of Shandong Province (tsqn201909047) and National Natural Science Foundation of China (22272092). E.C. acknowledges financial support from MCIN/AEI grant PID2019-107808RA-I00 and Comunidad de Madrid grants 2021-5A/AMB-20942 and P2018/NMT-451. P.S.P. and Y.F. acknowledge the Center for Information Services and High Performance Computing (ZIH) at TU Dresden for providing the high-performance computing resources. S.M.G. and D.B. thank support from Consortium des Equipements de Calcul Intensif−CECI (no. 2.5020.11) and Walloon Region (ZENOBE Tier-1 supercomputer, no. 1117545).This work was financially supported by ERC Grants (T2DCP, no. 819698; FC2DMOF, no. 852909), DFG projects (CRC 1415, no. 417590517; SPP 2248, RACOF-MMIS), EU Graphene Flagship (Core3, no. 881603) and Center for Advancing Electronics Dresden. S.F. acknowledges fellowship support from the Chinese Scholarship Council (CSC). We thank Dresden Center for Nanoanalysis (DCN) and P. Formanek (IPF, Dresden) for the use of facilities. A portion of this work was performed on the Steady High Magnetic Field Facilities, High Magnetic Field Laboratory, CAS. We appreciate C. Naisa, S. Xing, W. Niu, S. Park, J. Liu, Z. Zhang, P. Zhang, B. Zhang and S. Revueta for helpful discussions and measurements. M.W. specially acknowledges J. Cui. R.D. thanks Taishan Scholars Program of Shandong Province (tsqn201909047) and National Natural Science Foundation of China (22272092). E.C. acknowledges financial support from MCIN/AEI grant PID2019-107808RA-I00 and Comunidad de Madrid grants 2021-5A/AMB-20942 and P2018/NMT-451. P.S.P. and Y.F. acknowledge the Center for Information Services and High Performance Computing (ZIH) at TU Dresden for providing the high-performance computing resources. S.M.G. and D.B. thank support from Consortium des Equipements de Calcul Intensif−CECI (no. 2.5020.11) and Walloon Region (ZENOBE Tier-1 supercomputer, no. 1117545).
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