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The heterobimetallic metallacrown (MC),(TMA)$_2${Mn(OAc)$_2$[12-MC$_{Mn(III)Cu(II)N(shi)}$-4](CH$_3$OH)}$\cdot$2.90CH$_3$OH,1, where TMA$^+$ is tetramethylammonium, $^-$OAc is acetate, and shi$^{3-}$ issalicylhydroximate, consists of a Mn$^{II}$ ion captured in the central cavityand alternating unambiguous and ordered manganese(III) and copper(II) sitesabout the MC ring, a first for the archetypal MC structure design.DC-magnetometry characterization and subsequent simulation with the SpinHamiltonian $$H =-J_1(\mathbf{s}_1+\mathbf{s}_3)\cdot\mathbf{s}_5-J_2(\mathbf{s}_2+\mathbf{s}_4)\cdot\mathbf{s}_5-J_3\sum_{i=1}^{4}\mathbf{s}_i\cdot\mathbf{s}_{i+1}+ d(s_{z,1}^2 + s_{z,3}^2) + \mu_B\sum_{j=1}^5 g_j\mathbf{s}_j\cdot\mathbf{B}$$indicates an S = 5/2 ground state and a sizable axial zero-field splitting onMn$^{III}$. AC-susceptibility measurements reveal that 1 displays slowmagnetization relaxation akin to single-molecule magnet (SMM) behavior.

Slow Magnetic Relaxation of a 12-Metallacrown-4 Complex with a Manganese(III)-Copper(II) Heterometallic Ring Motif