161Dy Time‐Domain Synchrotron Mössbauer Spectroscopy for Investigating Single‐Molecule Magnets Incorporating Dy Ions

A new point of view: The magnetic hyperfine field at the ¹⁶¹Dy nucleus in Dy‐containing compounds can be determined by ¹⁶¹Dy time‐domain synchrotron Mössbauer spectroscopy. This quantity is influenced by the polarization of the s electrons at the ¹⁶¹Dy nucleus via metal–ligand interactions. The effect of different ligands in Dy‐containing single‐molecule magnets can now directly be explored from the viewpoint of the lanthanide ion.

Abstract

Time‐domain synchrotron Mössbauer spectroscopy (SMS) based on the Mössbauer effect of ¹⁶¹Dy has been used to investigate the magnetic properties of a Dy^III‐based single‐molecule magnet (SMM). The magnetic hyperfine field of [Dy(Cy₃PO)₂(H₂O)₅]Br₃⋅2 (Cy₃PO)⋅2 H₂O⋅2 EtOH is with B ₀=582.3(5) T significantly larger than that of the free‐ion Dy^III with a ⁶H_15/2 ground state. This difference is attributed to the influence of the coordinating ligands on the Fermi contact interaction between the s and 4f electrons of the Dy^III ion. This study demonstrates that ¹⁶¹Dy SMS is an effective local probe of the influence of the coordinating ligands on the magnetic structure of Dy‐containing compounds.

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