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Single-Molecule Magnets DyM2N@C80and 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 LU ; Greber, Thomas ; Büchner, Bernd ; Avdoshenko, S. M. and Popov, A (2020) In Chemistry: A European Journal 26(11). p.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... (More)
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. (Less)
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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Chemistry: A European Journal
volume
26
issue
11
pages
14 pages
publisher
Wiley-VCH Verlag
external identifiers
  • scopus:85079064061
  • pmid:31774196
ISSN
1521-3765
DOI
10.1002/chem.201904879
language
English
LU publication?
yes
id
d8a206b8-0e02-4b37-a297-e82a6c1b4493
date added to LUP
2020-05-06 13:00:51
date last changed
2020-10-07 06:58:19
@article{d8a206b8-0e02-4b37-a297-e82a6c1b4493,
  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.},
  author       = {Spree, Lukas and Schlesier, Christin and Kostanyan, Aram and Westerström, Rasmus and Greber, Thomas and Büchner, Bernd and Avdoshenko, S. M. and Popov, A},
  issn         = {1521-3765},
  language     = {eng},
  number       = {11},
  pages        = {2436--2449},
  publisher    = {Wiley-VCH Verlag},
  series       = {Chemistry: A European Journal},
  title        = {Single-Molecule Magnets DyM2N@C80and Dy2MN@C80(M=Sc, Lu): The Impact of Diamagnetic Metals on Dy3++Magnetic Anisotropy, Dy···Dy Coupling, and Mixing of Molecular and Lattice Vibrations},
  url          = {http://dx.doi.org/10.1002/chem.201904879},
  doi          = {10.1002/chem.201904879},
  volume       = {26},
  year         = {2020},
}