Electronic structure of mononuclear and radical-bridged dinuclear cobalt(II) single-molecule magnets

Metal-organic compounds that feature magnetic bistability have been proposed as bits for magnetic storage, but progress has been slow. Four-coordinate cobalt(II) complexes feature high inversion barriers of the magnetic moment, but they lack magnetic bistability. Developing radical-bridged polynucle...

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Veröffentlicht in:Nature communications Jg. 16; H. 1; S. 2157 - 18
Hauptverfasser: Hunger, David, Netz, Julia, Suhr, Simon, Thirunavukkuarasu, Komalavalli, Engelkamp, Hans, Fåk, Björn, Albold, Uta, Beerhues, Julia, Frey, Wolfgang, Hartenbach, Ingo, Schulze, Michael, Wernsdorfer, Wolfgang, Sarkar, Biprajit, Köhn, Andreas, van Slageren, Joris
Format: Journal Article
Sprache:Englisch
Veröffentlicht: London Nature Publishing Group UK 04.03.2025
Nature Publishing Group
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Schlagworte:
639/638/298/920
639/638/563/758
639/638/911/406/939
639/766/119/997
Cobalt
Cobalt compounds
Data storage
Electronic structure
Electrons
Humanities and Social Sciences
Magnetic measurement
Magnetic moments
Magnetic properties
Magnetic storage
Magnets
multidisciplinary
Organic compounds
Organometallic compounds
Science
Science (multidisciplinary)
Spectroscopy
Spin-orbit interactions
ISSN:2041-1723, 2041-1723
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Zusammenfassung:Metal-organic compounds that feature magnetic bistability have been proposed as bits for magnetic storage, but progress has been slow. Four-coordinate cobalt(II) complexes feature high inversion barriers of the magnetic moment, but they lack magnetic bistability. Developing radical-bridged polynuclear systems is a promising strategy to encounter this; however detailed investigations of such species are scarce. We report an air-stable radical-bridged dinuclear cobalt(II) complex, studied by a combination of magnetometry and spectroscopy. Fits of the data give D  = −113 cm −1 for the zero-field splitting (ZFS) and J  = 390 cm −1 for the metal–radical exchange. Ab initio investigations reveal first-order spin–orbit coupling of the quasi-degenerate d x 2 − y 2 and d x y orbitals to be at the heart of the large ZFS. The corresponding transitions are spectroscopically observed, as are transitions related to the exchange coupling. Finally, signatures of spin-phonon coupling are observed and theoretically analyzed. Furthermore, we demonstrate that the spectral features are not predominantly spin excitations, but largely vibrational in character. Four-coordinate cobalt(II) complexes possess high energy barriers toward inversion of the magnetic moment, but not the magnetic bistability needed for magnetic data storage. Here, the authors report an air-stable radical-bridged binuclear cobalt(II) complex with improved magnetic properties.
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ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-025-57210-0