Excited High-Spin Quartet (S = 3/2) State of a Novel π-Conjugated Organic Spin System, Pyrene–Verdazyl Radical

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Abstract
The excited high-spin quartet (S = 3/2) state of the intramolecular triplet–radical pair between the excited triplet state of pyrene and a dangling verdazyl radical was reported. A novel verdazyl radical with the pyrene moiety was designed and synthesized. The time-resolved ESR spectrum and a DFT calculation show the photo-induced ferromagnetic spin alignment between the excited triplet state of the pyrene moiety and the dangling verdazyl radical. This is the first observation of the high-spin (S > 1) excited state of the π-conjugated pyrene–radical pair.

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