Orbital angular momentum is a prerequisite for magnetic anisotropy, although in transition metal complexes it is typically quenched by the ligand field. By reducing the basicity of the carbon donor atoms in a pair of alkyl ligands, we synthesized a cobalt(II) dialkyl complex, Co(C(SiMe2ONaph)3)2 (where Me is methyl and Naph is a naphthyl group), 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 (d x 2 -y 2 , d xy )3(d xz , d yz )3(d z 2 )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-wave number magnetic excited state.

Department of Chemical and Biomolecular Engineering University of California Berkeley CA 94720 USA

Department of Chemistry and Centre for Materials Crystallography Aarhus University DK 8000 Aarhus C Denmark

Department of Chemistry University of California Berkeley CA 94720 USA

Institut für Physikalische Chemie and Center for Integrated Quantum Science and Technology Universität Stuttgart Pfaffenwaldring 55 70569 Stuttgart Germany

Institute of General and Inorganic Chemistry Bulgarian Academy of Sciences Academy Georgi Bontchev Sofia 1113 Bulgaria

Institute of Physics Charles University Ke Karlovu 5 12116 Praha 2 Czech Republic

Materials Sciences Division Lawrence Berkeley National Laboratory Berkeley CA 94720 USA

Max Planck Insitut für Kohlenforschung Mülheim an der Ruhr D 45470 Germany

Univ Grenoble Alpes Laboratoire National des Champs Magnétiques Intenses CNRS UGA UPS INSA EMFL 25 rue des Martyrs 38042 Grenoble France

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