The mononuclear complex of general formula [FeII(TIA)2(NCS)2] (1) and the heterotrinuclear complex of (Cu-Pc)2[Fe(TIA)2(NCS)2] (2), where TIA = N-o-tolyl-2-imidazolaldimine and Pc = phthalocyanine, have been synthesized. The X-ray crystal structure of 1 shows it to consist to two NCS groups in the cis position. The magnetic properties of the complexes have been measured down to 4.2 K and Mössbauer spectra have been recorded down to 20 K. In 1, the iron(II) is pure high-spin S = 2 (5T2) over the whole temperature range. In 2, a gradual spin crossover (5T2↔1A1) occurs below 298 K and the spin crossover is incomplete since it still presents a high-spin fraction about 0.35, even at 4.0 K.
