Abstract: | Two new azido-bridged Fe(III) Schiff base complexes, Fe(salen)N 3 ] and Fe(MeO-salen)N 3 ]·2H 2 O, salen = N , N '-bis-salicylaldehyde(ethylenediimine) and MeO-salen = N , N' -bis-3-methoxysalicylaldehyde(ethylenediimine)] have been synthesized, characterized and studied cryo-magnetically. A new isomeric form of the complex {Fe(salen) 2 O}] was obtained when attempts were made to grow single crystal of Fe(salen)N 3 ] from different solvents. The structure of Fe(salen)] 2 O has been determined by single crystal X-ray analysis. Magnetic susceptibility measurements show the presence of antiferromagnetic interactions in Fe(salen)N 3 ] and Fe(MeO-salen)N 3 ]·2H 2 O. The theoretical fit of the susceptibility data yielded values for the spin exchange parameters J = m 10 ( - 0.2) and m 13 ( - 0.3) cm m 1 , for Fe(salen)N 3 ] and Fe(MeO-salen)N 3 ]·2H 2 O, respectively. |