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Using ab initio calculations all the components of the magnetic anisotropy in a dinuclear [MnIIICuIICl(5‐Br‐sap)2(MeOH)] single‐molecule magnet (SMM) have been computed. These calculations reveal that apart from the single‐ion anisotropy, the exchange anisotropy also plays a crucial role in determining the sign as well as the magnitude of the cluster anisotropy. Developed magneto‐structural correlations...
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