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. 2017 Jul 11;53(56):7901-7904.
doi: 10.1039/c7cc03580b.

Record-high thermal barrier of the relaxation of magnetization in the nitride clusterfullerene Dy2ScN@C80-Ih

D S Krylov  1 , F Liu  1 , S M Avdoshenko  1 , L Spree  1 , B Weise  1 , A Waske  1 , A U B Wolter  1 , B Büchner  1 , A A Popov  1
Affiliations

Record-high thermal barrier of the relaxation of magnetization in the nitride clusterfullerene Dy2ScN@C80-Ih

D S Krylov et al. Chem Commun (Camb). .

Abstract

The Dy-Sc nitride clusterfullerene Dy2ScN@C80-Ih exhibits slow relaxation of magnetization up to 76 K. Above 60 K, thermally-activated relaxation proceeds via the fifth-excited Kramers doublet with the energy of 1735 ± 21 K, which is the highest barrier ever reported for dinuclear lanthanide single molecule magnets.

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Figures

Fig. 1
Fig. 1
(a) Single-crystal X-ray structure of Dy2ScN@C80-Ih(7)⋅NiII(OEP)·2C6H6. Solvent molecules are omitted for clarity, only the main site of the cluster is shown (fractional occupancy 0.69). (b) Two sites of the Dy2ScN cluster in the structure, the main site (Dy1, Dy2, and Sc1) is shown with solid bonds to N1, minor site (Dy3, Dy4, and Sc2) with dash-line bonds to N1, only one nitrogen site N1 is refined. All displacement parameters are shown at the 30% probability level.
Fig. 2
Fig. 2
Magnetization curves of Dy2ScN@C80 measured at 1.8–7 K (sweep rate of 2.9 mT s−1). At 8 K (not shown) the hysteresis is closed. The inset shows the blocking temperature of magnetization (TB) as the peak in the susceptibility of zero-field cooled (ZFC) sample as opposed to the field-cooled (FC) sample.
Fig. 3
Fig. 3
Relaxation times of the magnetization of Dy2ScN@C80. Green dots denote the values from dc measurements in zero field; two in-field points (red crosses) are also shown. AC values are measured with MPMS XL (7–50 K; open, magenta, and blue dots) and with PPMS (brown dots, 52–76 K). Magenta and blue dots denote long and short times from double-τ fits of the ac data, respectively, open dots – for single-τ fits.
Fig. 4
Fig. 4
AC-susceptibility measurements of Dy2ScN@C80 at selected temperatures: (a) χ″ and (b) Cole–Cole plots. Dots are experimental points, lines are fits to the points with generalized Debye model with either one or two relaxation times. The inset in (a) shows the fitting of the 20 K data with double-τ and single-τ models.
Fig. 5
Fig. 5
The energies of single-ion CF states of Dy1 and Dy2 as computed ab initio at the CASSCF/RASSI level. Red lines visualize transition probabilities computed from transverse components of the g-tensor (the thicker the line – the higher the probability).
See this image and copyright information in PMC

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