Research Article

A linear cobalt(II) complex with maximal orbital angular momentum from a non-Aufbau ground state

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Science  15 Nov 2018:
eaat7319
DOI: 10.1126/science.aat7319

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Abstract

Orbital angular momentum is a prerequisite for magnetic anisotropy, although in transition metal complexes it is typically quenched by the ligand field. Here, by reducing the basicity of the carbon donor atoms in a pair of alkyl ligands, we synthesize a cobalt(II) dialkyl complex, Co(C(SiMe2ONaphthyl)3)2, wherein the ligand field is sufficiently weak that interelectron repulsion and spin-orbit coupling play a dominant role in determining the electronic ground state. Assignment of a non-Aufbau (dx2–y2, dxy)3(dxz, dyz)3(dz2)1 electron configuration is supported by dc magnetic susceptibility data, experimental charge density maps, and ab initio calculations. Variable-field far-infrared spectroscopy and ac magnetic susceptibility measurements further reveal slow magnetic relaxation via a 450 cm−1 magnetic excited state.

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