Air-stable redox-active nanomagnets with lanthanide spins radical-bridged by a metal–metal bond

Fupin Liu (), Georgios Velkos, Denis S. Krylov, Lukas Spree, Michal Zalibera, Rajyavardhan Ray, Nataliya A. Samoylova, Chia-Hsiang Chen, Marco Rosenkranz, Sandra Schiemenz, Frank Ziegs, Konstantin Nenkov, Aram Kostanyan, Thomas Greber, Anja U. B. Wolter, Manuel Richter, Bernd Büchner, Stanislav M. Avdoshenko () and Alexey A. Popov ()
Additional contact information
Fupin Liu: Leibniz Institute for Solid State and Materials Research (IFW Dresden)
Georgios Velkos: Leibniz Institute for Solid State and Materials Research (IFW Dresden)
Denis S. Krylov: Leibniz Institute for Solid State and Materials Research (IFW Dresden)
Lukas Spree: Leibniz Institute for Solid State and Materials Research (IFW Dresden)
Michal Zalibera: Slovak University of Technology
Rajyavardhan Ray: Leibniz Institute for Solid State and Materials Research (IFW Dresden)
Nataliya A. Samoylova: Leibniz Institute for Solid State and Materials Research (IFW Dresden)
Chia-Hsiang Chen: Leibniz Institute for Solid State and Materials Research (IFW Dresden)
Marco Rosenkranz: Leibniz Institute for Solid State and Materials Research (IFW Dresden)
Sandra Schiemenz: Leibniz Institute for Solid State and Materials Research (IFW Dresden)
Frank Ziegs: Leibniz Institute for Solid State and Materials Research (IFW Dresden)
Konstantin Nenkov: Leibniz Institute for Solid State and Materials Research (IFW Dresden)
Aram Kostanyan: Physik-Institut der Universität Zürich
Thomas Greber: Physik-Institut der Universität Zürich
Anja U. B. Wolter: Leibniz Institute for Solid State and Materials Research (IFW Dresden)
Manuel Richter: Leibniz Institute for Solid State and Materials Research (IFW Dresden)
Bernd Büchner: Leibniz Institute for Solid State and Materials Research (IFW Dresden)
Stanislav M. Avdoshenko: Leibniz Institute for Solid State and Materials Research (IFW Dresden)
Alexey A. Popov: Leibniz Institute for Solid State and Materials Research (IFW Dresden)

Nature Communications, 2019, vol. 10, issue 1, 1-11

Abstract: Abstract Engineering intramolecular exchange interactions between magnetic metal atoms is a ubiquitous strategy for designing molecular magnets. For lanthanides, the localized nature of 4f electrons usually results in weak exchange coupling. Mediating magnetic interactions between lanthanide ions via radical bridges is a fruitful strategy towards stronger coupling. In this work we explore the limiting case when the role of a radical bridge is played by a single unpaired electron. We synthesize an array of air-stable Ln2@C80(CH2Ph) dimetallofullerenes (Ln2 = Y2, Gd2, Tb2, Dy2, Ho2, Er2, TbY, TbGd) featuring a covalent lanthanide-lanthanide bond. The lanthanide spins are glued together by very strong exchange interactions between 4f moments and a single electron residing on the metal–metal bonding orbital. Tb2@C80(CH2Ph) shows a gigantic coercivity of 8.2 Tesla at 5 K and a high 100-s blocking temperature of magnetization of 25.2 K. The Ln-Ln bonding orbital in Ln2@C80(CH2Ph) is redox active, enabling electrochemical tuning of the magnetism.

Date: 2019
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DOI: 10.1038/s41467-019-08513-6

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