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By David E. Lalond, John A. Ross

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This value plummeted on lowering the temperature as a result of intermolecular antiferromagnetic interactions, the Weiss constant being −19 K. To the best of our knowledge, no information concerning the conformation of the molecule in the solid is available, while in solution, EPR spectra suggest the presence of several conformers in accord with the complex conformational space available to this molecule as a result of its four torsional degrees of freedom. Trimethylenemethane (TMM) has proved to be another extremely efficient ferromagnetic coupler of unpaired electrons [84], and the preparation by Iwamura and colleagues of a bis-nitroxide with diphenylethylene spacers between the radical centers proved its worth [85].

Incorporation of a water molecule into one of the salts reduced dramatically these interactions, implying that the hydrogen bonds aid the transmission of exchange interactions. 2 Oligo-nitroxides In general, the unconjugated oligo-nitroxide radicals present little or no appreciable through-bond coupling of the free electrons in the molecule. 2 Unconjugated Nitroxides 11 is extremely small, all the spin density being located equally on the nitrogen and oxygen atoms [59]. The diester 5 has ferromagnetic interactions in the solid within planes [60] containing the radical moieties from different molecules, which interact antiferromagnetically between them [14].

Magnetic susceptibility data of the crystals indicated that the ground state is indeed a doublet, with dominant antiferromagnetic interactions between two pairs of neighboring free electrons which force the ferromagnetic alignment of the remaining pair. It was claimed as the “first demonstration of an organic triradical showing competing interactions” [79]. Ab initio calculations of model compounds showed an angular dependence of the magnetic interaction through the m-phenylene coupler, and correctly reproduced antiferromagnetic coupling when the NO group is highly twisted out of the plane of the benzene ring, implying disjoint molecular orbitals as the origin of this phenomenon [80].

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