The reactions of [MnIII(L4a)Cl] or [MnIII(L4b)Cl] with [Pt(SCN)6]2− resulted in the formation of a 1D polymeric complex [{Mn(L4a)}2{μ-Pt(SCN)6}]n (1) and a trinuclear compound [{Mn(L4b)(H2O)}2{μ-Pt(SCN)6}] (2), where L4a and L4b are tetradentate dianionic Schiff base ligands, H2L4a = N,N′-ethylenebis(salicylimine) and H2L4b = N,N′-3-methylbenzenebis(3-ethoxysalicylimine). In compound 1, the adjacent [Mn(L4a)]+ subunits are bound together through the phenolic oxygen atoms, thus forming [{Mn(L4a)}2]2+ dimers with the shortest Mn⋯Mn distance of 3.2101(5) Å, while in compound 2, the intermolecular bifurcated O–H⋯O hydrogen bonds between the neighbouring molecules form [{Mn(L4b)(H2O)}2]2+ dimers, resulting in a supramolecular 1D chain structure. The Mn⋯Mn distance within the supramolecular dimer is 4.7007(9) Å, while the shortest Mn⋯Mn distance between the dimers is 9.2347(10) Å. The magnetic analyses comprising the zero-field splitting resulted in a ferromagnetic exchange interaction within the phenolato-bridged dimer in 1 (J = +1.73 cm−1, DMn = −2.65 cm−1) and the antiferromagnetic exchange interaction within the supramolecular dimer in 2 (J = −0.88 cm−1, DMn = −3.06 cm−1). The experimental findings regarding the dominant as well as negligible exchange pathways are in good agreement with the results from DFT calculations at the B3LYP/TZVP level of theory.
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