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High-mobility semiconducting polymers with different spin ground states

Author

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  • Xiao-Xiang Chen

    (School of Materials Science and Engineering, Peking University
    Peking University)

  • Jia-Tong Li

    (School of Materials Science and Engineering, Peking University)

  • Yu-Hui Fang

    (Peking University)

  • Xin-Yu Deng

    (School of Materials Science and Engineering, Peking University)

  • Xue-Qing Wang

    (School of Materials Science and Engineering, Peking University)

  • Guangchao Liu

    (School of Materials Science and Engineering, Peking University)

  • Yunfei Wang

    (The University of Southern Mississippi)

  • Xiaodan Gu

    (The University of Southern Mississippi)

  • Shang-Da Jiang

    (South China University of Technology)

  • Ting Lei

    (School of Materials Science and Engineering, Peking University
    Peking University)

Abstract

Organic semiconductors with high-spin ground states are fascinating because they could enable fundamental understanding on the spin-related phenomenon in light element and provide opportunities for organic magnetic and quantum materials. Although high-spin ground states have been observed in some quinoidal type small molecules or doped organic semiconductors, semiconducting polymers with high-spin at their neutral ground state are rarely reported. Here we report three high-mobility semiconducting polymers with different spin ground states. We show that polymer building blocks with small singlet-triplet energy gap (ΔES-T) could enable small ΔES-T gap and increase the diradical character in copolymers. We demonstrate that the electronic structure, spin density, and solid-state interchain interactions in the high-spin polymers are crucial for their ground states. Polymers with a triplet ground state (S = 1) could exhibit doublet (S = 1/2) behavior due to different spin distributions and solid-state interchain spin-spin interactions. Besides, these polymers showed outstanding charge transport properties with high hole/electron mobilities and can be both n- and p-doped with superior conductivities. Our results demonstrate a rational approach to obtain high-mobility semiconducting polymers with different spin ground states.

Suggested Citation

  • Xiao-Xiang Chen & Jia-Tong Li & Yu-Hui Fang & Xin-Yu Deng & Xue-Qing Wang & Guangchao Liu & Yunfei Wang & Xiaodan Gu & Shang-Da Jiang & Ting Lei, 2022. "High-mobility semiconducting polymers with different spin ground states," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-29918-w
    DOI: 10.1038/s41467-022-29918-w
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