High-mobility semiconducting polymers with different spin ground states

作者：Chen, Xiao-Xiang; Li, Jia-Tong; Fang, Yu-Hui; Deng, Xin-Yu; Wang, Xue-Qing; Liu, Guangchao; Wang, Yunfei; Gu, Xiaodan; Jiang, Shang-Da; Lei, Ting^*

来源：Nature Communications, 2022, 13(1): 2258.

DOI：10.1038/s41467-022-29918-w

• EXTENDED P-QUINODIMETHANES
• COHERENT CHARGE-TRANSPORT
• CONDUCTING POLYMERS
• AGGREGATION
• DESIGN
• PROPERTY
• DISORDER

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 (Delta ES-T) could enable small Delta ES-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. @@@ Semiconducting polymers with high-spin at their neutral ground state are rarely reported. Here the authors synthesize three semiconducting polymers with different spin ground states and high hole/electron mobility, by appropriate choice of the building blocks' singlet-triplet energy gap, spin distributions and solid-state interchain interactions.

• 单位
  北京大学