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Dysprosium(III) ions are promising candidates for the design of single‐ion magnets (SIMs) as they show an intrinsic strong magnetic anisotropy. However, time‐demanding multireference methods are usually necessary to reproduce low‐lying magnetic states. In this work, we present an improved wave function‐based semiempirical ligand‐field (LF) theory approach to obtain magnetochemical properties of dysprosium(III)‐based...
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