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Magnetic hysteresis and strong ferromagnetic coupling of sulfur-bridged Dy ions in clusterfullerene Dy2S@C82


Krylov, Denis; Velkos, Georgios; Chen, Chia-Hsiang; Büchner, Bernd; Kostanyan, Aram; Greber, Thomas; Avdoshenko, Stanislav M; Popov, Alexey A (2020). Magnetic hysteresis and strong ferromagnetic coupling of sulfur-bridged Dy ions in clusterfullerene Dy2S@C82. Inorganic Chemistry Frontiers, 7(19):3521-3532.

Abstract

Two isomers of metallofullerene Dy2S@C82 with sulfur-bridged Dy ions exhibit broad magnetic hysteresis with sharp steps at sub-Kelvin temperature. Analysis of the level crossing events for different orientations of a magnetic field showed that even in powder samples, the hysteresis steps caused by quantum tunneling of magnetization can provide precise information on the strength of intramolecular Dy⋯Dy interactions. A comparison of different methods to determine the energy difference between ferromagnetic and antiferromagnetic states showed that sub-Kelvin hysteresis gives the most robust and reliable values. The ground state in Dy2S@C82 has ferromagnetic coupling of Dy magnetic moments, whereas the state with antiferromagnetic coupling in Cs and C3v cage isomers is 10.7 and 5.1 cm−1 higher, respectively. The value for the Cs isomer is among the highest found in metallofullerenes and is considerably larger than that reported in non-fullerene dinuclear molecular magnets. Magnetization relaxation times measured in zero magnetic field at sub-Kelvin temperatures tend to level off near 900 and 3200 s in Cs and C3v isomers. These times correspond to the quantum tunneling relaxation mechanism, in which the whole magnetic moment of the Dy2S@C82 molecule flips at once as a single entity.

Abstract

Two isomers of metallofullerene Dy2S@C82 with sulfur-bridged Dy ions exhibit broad magnetic hysteresis with sharp steps at sub-Kelvin temperature. Analysis of the level crossing events for different orientations of a magnetic field showed that even in powder samples, the hysteresis steps caused by quantum tunneling of magnetization can provide precise information on the strength of intramolecular Dy⋯Dy interactions. A comparison of different methods to determine the energy difference between ferromagnetic and antiferromagnetic states showed that sub-Kelvin hysteresis gives the most robust and reliable values. The ground state in Dy2S@C82 has ferromagnetic coupling of Dy magnetic moments, whereas the state with antiferromagnetic coupling in Cs and C3v cage isomers is 10.7 and 5.1 cm−1 higher, respectively. The value for the Cs isomer is among the highest found in metallofullerenes and is considerably larger than that reported in non-fullerene dinuclear molecular magnets. Magnetization relaxation times measured in zero magnetic field at sub-Kelvin temperatures tend to level off near 900 and 3200 s in Cs and C3v isomers. These times correspond to the quantum tunneling relaxation mechanism, in which the whole magnetic moment of the Dy2S@C82 molecule flips at once as a single entity.

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Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Physics Institute
Dewey Decimal Classification:530 Physics
Scopus Subject Areas:Physical Sciences > Inorganic Chemistry
Language:English
Date:1 January 2020
Deposited On:08 Feb 2021 16:41
Last Modified:10 Feb 2021 16:04
Publisher:Royal Society of Chemistry
ISSN:2052-1553
OA Status:Hybrid
Publisher DOI:https://doi.org/10.1039/d0qi00771d
Project Information:
  • : FunderH2020
  • : Grant ID648295
  • : Project TitleGraM3 - Surface-grafted metallofullerene molecular magnets with controllable alignment of magnetic moments
  • : FunderH2020
  • : Grant ID748635
  • : Project TitleSamSD - Theoretical insides in endohedral metallofullerene based Self-Assembled Monolayers: Statics and Dynamics.
  • : FunderSNSF
  • : Grant ID200021L_147201
  • : Project TitleNitride Cluster Fullerene Spin Shuttles: The role of cluster composition for single molecule magnet behavior

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