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Two Mn 4 single-molecule-magnet (SMM)based coordination polymers, {[Mn 4 O(salox) systems with dpp and NaN 3 in DMF/MeOH, respectively. Both compounds comprise a mixed-valence tetranuclear manganese core, [Mn II Mn III 3 O] 9+ , which serves as a building unit for subsequent assembly via oximate and azido ligands. The flexible dpp ligand links with a Mn 4 unit, leading to the formation of a one-dimensional helical structure in 1•0.5MeOH and a three-dimensional pcu network in 2•1.5Et 2 O. The magnetic data analysis shows that antiferromagnetic interactions within the Mn 4 units resulted in S = 3 / 2 and 7 / 2 ground states for 1•0.5MeOH and 2•1.5Et 2 O, respectively. Both compounds show SMM behavior, as evidenced by frequency-dependent out-of-phase signals in alternating-current magnetic susceptibility and magnetic hysteresis loop studies with an energy barrier of U eff = 37 K for 2•1.5Et 2 O.

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