Abstract
Layered two-dimensional conjugated polymers (2D CPs), or 2D conjugated covalent organic frameworks, are promising semiconductor materials for (opto)electronics and photocatalysis, but their performance is often limited by insufficient in-plane conjugation and poor charge transport. Guided by density functional theory calculations, we report two donor-acceptor-type 2D poly(arylene vinylene)s constructed from thienyl-benzodithiophene and diketopyrrolopyrrole units. These materials are predicted to exhibit strongly dispersive energy bands with ultralow in-plane effective masses (0.036 − 0.159 m0), enabling intrinsic charge mobilities approaching 2000 cm2 V−1 s−1. Solid-state Aldol-type 2D polycondensation yields crystalline materials with optical band gaps as narrow as 1.0 eV. Terahertz spectroscopy reveals long charge carrier scattering times of 76 fs and a high room-temperature mobility of 310 cm2 V−1 s−1, surpassing previously reported linear and 2D CP powder samples. This work highlights donor-acceptor engineering as an effective strategy to enhance charge transport in 2D CPs.
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The data supporting the findings of this study are available within the paper and its Supplementary Information files. The data generated in this study are provided in the Supplementary Information/Source Data file. Source data are provided with this paper.
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Acknowledgements
This work was financially supported by National Natural Science Foundation of China (52572196), ERC Grant (T2DCP, No. 819698) and DFG projects (CRC 1415, No. 417590517; SPP 2248, RACOF-MMIS). We appreciate the Materials Processing and Analysis Center at Peking University, and the Analysis and Testing Center of School of Advanced Materials, Peking University Shenzhen Graduate School for assistance with materials characterization. We thank using facilities at the Dresden Center for Nanoanalysis (DCN). The authors acknowledge Mr. Wei Wang for help with conductivity measurement. The authors thank Mr. Tianhao Xue and Prof. Thomas Bein for the measurement of diffuse reflectance spectra. The authors also acknowledge the Centre for Information Services and High Performance Computing (ZIH) at TU Dresden for the provided computational resources.
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M.W., R.Z., and X.F. conceived and designed the project. R.Z. synthesized the monomers, prepared the 2D PAVs, and arranged the structural, compositional, and property characterizations. H.Y. and T.H. performed the theoretical calculations of the 2D PAVs. H.Z., L.G., H.-I.W., and M.B. conducted the THz experiments and data analysis. A.H.K. and E.B. conducted the solid-state NMR measurement. C.L., X.L., X.C., and D.P. contributed to the structural characterization of materials. Y.F. contributed to helpful discussions. A.W.-L. and Y.V. performed UPS. R.Z., M.W., and X.F. co-wrote the manuscript with contributions from all co-authors.
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Zhao, R., Yu, H., Zhang, H. et al. Diketopyrrolopyrrole-based two-dimensional poly(arylene vinylene)s with high charge carrier mobility. Nat Commun (2026). https://doi.org/10.1038/s41467-026-69061-4
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DOI: https://doi.org/10.1038/s41467-026-69061-4
