%AChen, Xiao-Xiang%ALi, Jia-Tong%AFang, Yu-Hui%ADeng, Xin-Yu%AWang, Xue-Qing%ALiu, Guangchao%AWang, Yunfei%AGu, Xiaodan%AJiang, Shang-Da%ALei, Ting%BJournal Name: Nature Communications; Journal Volume: 13; Journal Issue: 1 %D2022%I %JJournal Name: Nature Communications; Journal Volume: 13; Journal Issue: 1 %K %MOSTI ID: 10335928 %PMedium: X %THigh-mobility semiconducting polymers with different spin ground states %XAbstract 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. %0Journal Article