Intramolecular high-spin correlation in a series of the successively generated polycationic species of Bindschedler's green-based arylamine, N,N,N',N',N'',N''-hexakis[4-(dimethylamino)phenyl]-1,3,5-benzenetriamine (1), has been investigated by continuous wave (CW) and pulsed EPR spectroscopy. Cyclic voltammetry shows multiredox behavior of 1 that can be reversibly oxidized from monocation to hexacation. Depending on the quantity of the added oxidant, the characteristic EPR spectra are observed for polycations of 1 in frozen solution. Unequivocal determination of the spin state at each oxidation stage of 1 is given by a pulsed EPR technique, that is, electron spin transient nutation spectroscopy.
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