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<p>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 <i>m</i><sub>0</sub>), enabling intrinsic charge mobilities approaching 2000 cm<sup>2 </sup>V<sup>−1</sup> s<sup>−1</sup>. 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 cm<sup>2 </sup>V<sup>−1</sup> s<sup>−1</sup>, 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.</p>

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Diketopyrrolopyrrole-based two-dimensional poly(arylene vinylene)s with high charge carrier mobility

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年2月3日

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  • Ruyan Zhao,
  • Hongde Yu,
  • Heng Zhang,
  • Lei Gao,
  • Arafat Hossain Khan,
  • Congxue Liu,
  • Xiaodong Li,
  • Xingyuan Chu,
  • Yubin Fu,
  • Darius Pohl,
  • Angelika Wrzesińska-Lashkova,
  • Eike Brunner,
  • Yana Vaynzof,
  • Hai I. Wang,
  • Mischa Bonn,
  • Thomas Heine,
  • Mingchao Wang,
  • Xinliang Feng

摘要

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.