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High-mobility semiconducting polymers with different spin ground states

Xiao-Xiang Chen, Jia-Tong Li, Yu-Hui Fang, Xin-Yu Deng, Xue-Qing Wang, Guangchao Liu, Yunfei Wang, Xiaodan Gu, Shang-Da Jiang and Ting Lei ()
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Xiao-Xiang Chen: School of Materials Science and Engineering, 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

Nature Communications, 2022, vol. 13, issue 1, 1-9

Abstract: 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.

Date: 2022
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DOI: 10.1038/s41467-022-29918-w

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