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A record anisotropy barrier (319 cm−1) for all d‐f complexes was observed for a unique FeII‐DyIII‐FeII single‐molecule magnet (SMM), which possesses two asymmetric and distorted FeII ions and one quasi‐D5h DyIII ion. The frozen magnetization of the DyIII ion leads to the decreased FeII relaxation rates evident in the Mössbauer spectrum. Ab initio calculations suggest that tunneling is interrupted...
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