The spin–spin and magnetic properties of two (nitronyl nitroxide)‐(di‐p‐anisylamine‐phenothiazine) diradical cation salts, (DAA‐PTZ)+‐NN⋅MBr4− (M=Ga, Fe), have been investigated. These diradical‐cation species were prepared by the cross‐coupling of iodophenothiazine DAA‐PTZ‐I with NN‐AuPPh3 followed by oxidation with the thianthrenium radical cation (TA+⋅MBr4−). These salts were found to be highly stable under aerobic conditions. For the GaBr4 salt, large ferromagnetic intramolecular and small antiferromagnetic intermolecular interactions (J1/kB=+320 K and J2/kB=−2 K, respectively) were observed. The magnetic property of the Fe3+ salt was analyzed by using a six‐spin model assuming identical intramolecular exchange interaction (J3/kB=+320 K) and the other exchange interactions (J4/kB=−7 K and J5/kB=−4 K). A significant color change was observed in the UV/Vis/NIR absorption spectra upon electrochemical oxidation of the doublet DAA‐PTZ‐NN to the triplet (DAA‐PTZ)+‐NN.
Only a few radical-substituted π-donor radical cations have been reported to date. In this note, 5-mesityl-5′′-(nitronyl nitroxide)-2,2′:5′,2′′-ter(3,4-ethylenedioxythiophene) (NN-TEDOT) was prepared and its electrochemical and chemical oxidations were examined. The NN-TEDOT radical cation was moderately stable and slowly decomposed.
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