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Single‐Molecule Magnets DyM2N@C80 and Dy2MN@C80 (M=Sc, Lu): The Impact of Diamagnetic Metals on Dy3+ Magnetic Anisotropy, Dy⋅⋅⋅Dy Coupling, and Mixing of Molecular and Lattice Vibrations


Spree, Lukas; Schlesier, Christin; Kostanyan, Aram; Westerström, Rasmus; Greber, Thomas; Büchner, Bernd; Avdoshenko, Stanislav M; Popov, Alexey A (2020). Single‐Molecule Magnets DyM2N@C80 and Dy2MN@C80 (M=Sc, Lu): The Impact of Diamagnetic Metals on Dy3+ Magnetic Anisotropy, Dy⋅⋅⋅Dy Coupling, and Mixing of Molecular and Lattice Vibrations. Chemistry - A European Journal, 26(11):2436-2449.

Abstract

The substitution of scandium in fullerene single‐molecule magnets (SMMs) DySc2N@C80 and Dy2ScN@C80 by lutetium has been studied to explore the influence of the diamagnetic metal on the SMM performance of dysprosium nitride clusterfullerenes. The use of lutetium led to an improved SMM performance of DyLu2N@C80, which shows a higher blocking temperature of magnetization (TB=9.5 K), longer relaxation times, and broader hysteresis than DySc2N@C80 (TB=6.9 K). At the same time, Dy2LuN@C80 was found to have a similar blocking temperature of magnetization to Dy2ScN@C80 (TB=8 K), but substantially different interactions between the magnetic moments of the dysprosium ions in the Dy2MN clusters. Surprisingly, although the intramolecular dipolar interactions in Dy2LuN@C80 and Dy2ScN@C80 are of similar strength, the exchange interactions in Dy2LuN@C80 are close to zero. Analysis of the low‐frequency molecular and lattice vibrations showed strong mixing of the lattice modes and endohedral cluster librations in k‐space. This mixing simplifies the spin–lattice relaxation by conserving the momentum during the spin flip and helping to distribute the moment and energy further into the lattice.

Abstract

The substitution of scandium in fullerene single‐molecule magnets (SMMs) DySc2N@C80 and Dy2ScN@C80 by lutetium has been studied to explore the influence of the diamagnetic metal on the SMM performance of dysprosium nitride clusterfullerenes. The use of lutetium led to an improved SMM performance of DyLu2N@C80, which shows a higher blocking temperature of magnetization (TB=9.5 K), longer relaxation times, and broader hysteresis than DySc2N@C80 (TB=6.9 K). At the same time, Dy2LuN@C80 was found to have a similar blocking temperature of magnetization to Dy2ScN@C80 (TB=8 K), but substantially different interactions between the magnetic moments of the dysprosium ions in the Dy2MN clusters. Surprisingly, although the intramolecular dipolar interactions in Dy2LuN@C80 and Dy2ScN@C80 are of similar strength, the exchange interactions in Dy2LuN@C80 are close to zero. Analysis of the low‐frequency molecular and lattice vibrations showed strong mixing of the lattice modes and endohedral cluster librations in k‐space. This mixing simplifies the spin–lattice relaxation by conserving the momentum during the spin flip and helping to distribute the moment and energy further into the lattice.

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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 > Catalysis
Physical Sciences > Organic Chemistry
Uncontrolled Keywords:General Chemistry
Language:English
Date:21 February 2020
Deposited On:14 Apr 2020 14:09
Last Modified:29 Jul 2020 15:01
Publisher:Wiley-VCH Verlag
ISSN:0947-6539
OA Status:Hybrid
Publisher DOI:https://doi.org/10.1002/chem.201904879
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 ID206021_150784
  • : Project TitleAn AC Sub-Kelvin Magnetometer at the University of Zürich Irchel (ASKUZI)
  • : FunderSNSF
  • : Grant ID200021L_147201
  • : Project TitleNitride Cluster Fullerene Spin Shuttles: The role of cluster composition for single molecule magnet behavior

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