Three new compounds based on the cationic complex [Fe(III)(3-R-salEen)(2)]+ (salEen stands for N-(2-ethylamino)ethyl)-salicylaldimine, R = H, CH(3)O) with the electroactive Ni(dmit)(2) species as a counterion (dmit stands for 1,3-dithia-2-thione-4,5-dithiolato) have been synthesized and structurally and magnetically characterized. Compound 1 ([Ni(dmit)(2)][Fe(3-OMe-salEen)(2)]. CH(3)OH) shows an apparent hysteresis loop, due to an irreversible desolvatation process. Compound 2 ([Ni(dmit)(2)](NO(3))[Fe(salEen)(2)](2)) exhibits a gradual and incomplete spin transition. Compound 3 ([Ni(dmit)(2)](5)[Fe(salEen)(2)](2), 6CH(3)CN) is a fractional oxidation state complex, which behaves like a semiconductor and exhibits a gradual but complete spin transition between 300 and 4 K.
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