A linear cobalt(II) complex with maximal orbital angular momentum from a non-Aufbau ground state
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(SiMe ONaph) ) (whe...
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| Veröffentlicht in: | Science (American Association for the Advancement of Science) Jg. 362; H. 6421 |
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| Hauptverfasser: | , , , , , , , , , |
| Format: | Journal Article |
| Sprache: | Englisch |
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21.12.2018
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| ISSN: | 1095-9203, 1095-9203 |
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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. By reducing the basicity of the carbon donor atoms in a pair of alkyl ligands, we synthesized a cobalt(II) dialkyl complex, Co(C(SiMe
ONaph)
)
(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
, d
)
(d
, d
)
(d
)
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. |
|---|---|
| AbstractList | 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.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. 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(SiMe ONaph) ) (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 , d ) (d , d ) (d ) 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. |
| Author | van Slageren, Joris Bunting, Philip C Atanasov, Mihail Perfetti, Mauro Overgaard, Jacob Neese, Frank Crassee, Iris Orlita, Milan Damgaard-Møller, Emil Long, Jeffrey R |
| Author_xml | – sequence: 1 givenname: Philip C orcidid: 0000-0002-6059-2680 surname: Bunting fullname: Bunting, Philip C organization: Department of Chemistry, University of California, Berkeley, CA 94720, USA – sequence: 2 givenname: Mihail orcidid: 0000-0003-4178-2187 surname: Atanasov fullname: Atanasov, Mihail organization: Institute of General and Inorganic Chemistry, Bulgarian Academy of Sciences, Academy Georgi Bontchev, Sofia 1113, Bulgaria – sequence: 3 givenname: Emil surname: Damgaard-Møller fullname: Damgaard-Møller, Emil organization: Department of Chemistry and Centre for Materials Crystallography, Aarhus University, DK-8000 Aarhus C, Denmark – sequence: 4 givenname: Mauro orcidid: 0000-0001-5649-0449 surname: Perfetti fullname: Perfetti, Mauro organization: Institut für Physikalische Chemie and Center for Integrated Quantum Science and Technology (IQST), Universität Stuttgart, Pfaffenwaldring 55, 70569 Stuttgart, Germany – sequence: 5 givenname: Iris orcidid: 0000-0002-1288-9236 surname: Crassee fullname: Crassee, Iris organization: Univ. Grenoble Alpes, Laboratoire National des Champs Magnétiques Intenses, CNRS-UGA-UPS-INSA-EMFL, 25 rue des Martyrs, 38042 Grenoble, France – sequence: 6 givenname: Milan orcidid: 0000-0002-9633-507X surname: Orlita fullname: Orlita, Milan organization: Institute of Physics, Charles University, Ke Karlovu 5, 12116 Praha 2, Czech Republic – sequence: 7 givenname: Jacob surname: Overgaard fullname: Overgaard, Jacob organization: Department of Chemistry and Centre for Materials Crystallography, Aarhus University, DK-8000 Aarhus C, Denmark – sequence: 8 givenname: Joris orcidid: 0000-0002-0855-8960 surname: van Slageren fullname: van Slageren, Joris organization: Institut für Physikalische Chemie and Center for Integrated Quantum Science and Technology (IQST), Universität Stuttgart, Pfaffenwaldring 55, 70569 Stuttgart, Germany – sequence: 9 givenname: Frank surname: Neese fullname: Neese, Frank organization: Max-Planck-Insitut für Kohlenforschung, Mülheim an der Ruhr D-45470, Germany – sequence: 10 givenname: Jeffrey R surname: Long fullname: Long, Jeffrey R email: jrlong@berkeley.edu organization: Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/30442763$$D View this record in MEDLINE/PubMed |
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| ContentType | Journal Article |
| Copyright | Copyright © 2018 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. |
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