The postulate of a limiting resonance structure involving low-spin iro
n(II) and an unpaired electron on a radical ligand for the spin-equili
bria iron(III) tris(dithiocarbamates), Fe(S2CNR2)3, is disproved as a
result of the observation of a structured line in the g = 2 region of
the EPR spectrum of Fe(S2COEt)3, ascribed to an impurity [Fe(NO)(S2COE
t)2]. A similar signal in the spectra of the dithiocarbamates is assig
ned to [Fe(NO)(S2CNR2)2]. Evidence for unequivocal assignment of signa
ls for separate isomers in the EPR spectra of a spin-equilibrium compo
und, Fe(Ph.CS.CH.CO.Ph)3, is presented.