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<p>Balanced ambipolar transport in conjugated polymers requires simultaneous control over frontier orbital energies and solid-state packing-two parameters that are difficult to tune independently in conventional polymer systems. Here we report a composition-engineered copolymer platform that integrates thiophene-flanked diketopyrrolopyrrole (<b>TDPP</b>) with a double B←N coordinated DPP (<b>2BN-DPP</b>) unit. The strongly electron-withdrawing B←N motif lowers and stabilizes the LUMO while modulating the HOMO through intramolecular coordination, providing a chemically distinct route to tuning ambipolar transport. To efficiently explore the non-monotonic composition landscape, Bayesian optimization was employed as an experimental design tool, identifying the optimal <b>2BN-DPP:TDPP</b> ratio using only five synthesized polymers across two iterations. The resulting copolymer, <b>P4-4.13</b>, exhibits nearly identical hole and electron mobilities (∼0.92 cm<sup>2</sup> V<sup>−1</sup> s<sup>−1</sup>), with maxima exceeding 1 cm<sup>2</sup> V<sup>−1</sup> s<sup>−1</sup>, together with enhanced mechanical robustness and environmental stability. Spectroscopic and structural analyses reveal that B←N incorporation simultaneously tunes orbital energies and induces mixed <i>face-on/edge-on</i> packing, rationalizing the origin of balanced ambipolar transport. These results establish B←N coordination as a versatile acceptor motif and demonstrate a generalizable strategy for composition engineering in conjugated polymers.</p>

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Data-driven composition engineering of B←N coordinated diketopyrrolopyrrole polymers for balanced ambipolar transport

  • 期刊论文

  • 发表日期：

    2026年5月29日

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  • Jiulong Zhang,
  • Xiangrui Gong,
  • Jinqiu Meng,
  • Linghui Zhang,
  • Tianqiang Cui,
  • Ying Jiang,
  • Lang Jiang,
  • Baoxin Zhang,
  • Xiangfeng Shao,
  • Hao-Li Zhang,
  • Zitong Liu

摘要

Balanced ambipolar transport in conjugated polymers requires simultaneous control over frontier orbital energies and solid-state packing-two parameters that are difficult to tune independently in conventional polymer systems. Here we report a composition-engineered copolymer platform that integrates thiophene-flanked diketopyrrolopyrrole (TDPP) with a double B←N coordinated DPP (2BN-DPP) unit. The strongly electron-withdrawing B←N motif lowers and stabilizes the LUMO while modulating the HOMO through intramolecular coordination, providing a chemically distinct route to tuning ambipolar transport. To efficiently explore the non-monotonic composition landscape, Bayesian optimization was employed as an experimental design tool, identifying the optimal 2BN-DPP:TDPP ratio using only five synthesized polymers across two iterations. The resulting copolymer, P4-4.13, exhibits nearly identical hole and electron mobilities (∼0.92 cm2 V−1 s−1), with maxima exceeding 1 cm2 V−1 s−1, together with enhanced mechanical robustness and environmental stability. Spectroscopic and structural analyses reveal that B←N incorporation simultaneously tunes orbital energies and induces mixed face-on/edge-on packing, rationalizing the origin of balanced ambipolar transport. These results establish B←N coordination as a versatile acceptor motif and demonstrate a generalizable strategy for composition engineering in conjugated polymers.