Abstract
A practical difficulty in constructing organic molecule-based ferrimagnetics is co-crystallization of two distinct molecules with different spin quantum numbers. Coulombic energy between cationic and anionic molecules in organic salts is a promising driving force for co-crystallization. We investigated magnetic properties of four kinds of phenoxide-substituted nitronyl nitroxide biradical salts; a potassium and a sodium salt of 2,4-bis(1-oxyl-3-oxido-4,4,5,5-tetramethyl-2-imidazolin-2-yl)-phenol ( 1a and 1b), and a potassium and a sodium salt of 4-methyl-2,6-bis(1-oxyl-3-oxido-4,4,5,5-tetramethyl-2-imidazolin-2-yl)-phenol ( 2a and 2b). For 1a and 2a, it was found from the analysis of magnetic susceptibility in the solid state and ESR spectra in diluted frozen solutions that the ground-state spin multiplicities changed from triplet ( S=1) into singlet ( S=0) on ionization. For 1b and 2b, magnetic susceptibility in the solid state suggested the weakening of their intramolecular ferromagnetic interaction or the conversion of the ground-state spin multiplicities into singlet.
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