High-mobility semiconducting polymers with different spin ground states

• Published in: Nature communications Vol. 13; no. 1; p. 2258
• Main Authors: 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
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 26.04.2022; Nature Publishing Group; Nature Portfolio
• Subjects: 140/131; 140/58; 147/3; 639/301/1005/1007; 639/638/440/94; 639/638/455/954; Charge transport; Copolymers; Electron mobility; Electron spin; Electronic structure; Electronics industry; Electrons; Energy gap; Ground state; Humanities and Social Sciences; Mobility; multidisciplinary; Organic semiconductors; Polymers; Science; Science (multidisciplinary); Semiconductors; Solid state; Transport properties
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-022-29918-w

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 (Δ E S-T ) could enable small Δ E S-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.