Aromaticity‐Induced Spin State Switching and High‐Spin States in Non‐Alternant Polyradicals

-systems, which has a commensurate effect on GS electronic structure and spin spectrum, usually leading to greater stabilization of open-shell character, is potentially useful for novel compounds with previously unrealized properties for organic electronics, spintronics, biosensors, single-molecule devices, etc. The proposed polyradicals, with one of its derivatives recently synthesized and characterized as a triplet GS diradical, are rationally designed to minimize strain and steric hindrance to make them synthetically accessible and thermodynamically stable, and can be kinetically stabilized by bulky protecting groups at exposed radical sites.