Abstract
Metal-metal bonding interactions can engender outstanding magnetic properties in bulk materials and molecules, and examples abound for the transition metals. Extending this paradigm to the lanthanides, herein we report mixed-valence dilanthanide complexes (CpiPr5)2Ln2I3 (Ln is Gd, Tb, or Dy; CpiPr5, pentaisopropylcyclopentadienyl), which feature a singly occupied lanthanide-lanthanide σ-bonding orbital of parentage, as determined by structural, spectroscopic, and computational analyses. Valence delocalization, wherein the d electron is equally shared by the two lanthanide centers, imparts strong parallel alignment of the σ-bonding and f electrons on both lanthanides according to Hund’s rules. The combination of a well-isolated high-spin ground state and large magnetic anisotropy in (CpiPr5)2Dy2I3 gives rise to an enormous coercive magnetic field with a lower bound of 14 tesla at temperatures as high as 60 kelvin.
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