Journal
NATURE COMMUNICATIONS
Volume 13, Issue 1, Pages -Publisher
NATURE PORTFOLIO
DOI: 10.1038/s41467-022-29918-w
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Funding
- National Natural Science Foundation of China [22075001, 92156019]
- NSF [OIA-1757220]
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This study reports three high-mobility semiconducting polymers with different spin ground states. The researchers demonstrate that polymer building blocks with small singlet-triplet energy gap could increase the diradical character in copolymers. The electronic structure, spin density, and solid-state interchain interactions are crucial for the ground states of the high-spin polymers.
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.
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