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Magnetization relaxation in the single-ion magnet DySc2N@C80: quantum tunneling, magnetic dilution, and unconventional temperature dependence.

ABSTRACT: Relaxation of magnetization in endohedral metallofullerenes DySc2N@C80 is studied at different temperatures, in different magnetic fields, and in different molecular arrangements. Magnetization behavior and relaxation are analyzed for powder sample, and for DySc2N@C80 diluted in non-magnetic fullerene Lu3N@C80, adsorbed in voids of a metal-organic framework, and dispersed in a polymer. The magnetic field dependence and zero-field relaxation are also studied for single-crystals of DySc2N@C80 co-crystallized with Ni(ii) octaethylporphyrin, as well as for the single crystal diluted with Lu3N@C80. Landau-Zener theory is applied to analyze quantum tunneling of magnetization in the crystals. The field dependence of relaxation rates revealed a dramatic dependence of the zero-field tunneling resonance width on the dilution and is explained with the help of an analysis of dipolar field distributions. AC magnetometry is used then to get access to the relaxation of magnetization in a broader temperature range, from 2 to 87 K. Finally, a theoretical framework describing the spin dynamics with dissipation is proposed to study magnetization relaxation phenomena in single molecule magnets.

SUBMITTER: Krylov DS

PROVIDER: S-EPMC5933001 | biostudies-literature | 2018 May

REPOSITORIES: biostudies-literature

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Magnetization relaxation in the single-ion magnet DySc2N@C80: quantum tunneling, magnetic dilution, and unconventional temperature dependence.

Krylov D S DS Liu F F Brandenburg A A Spree L L Bon V V Kaskel S S Wolter A U B AUB Büchner B B Avdoshenko S M SM Popov A A AA

Physical chemistry chemical physics : PCCP 20180419 17

Relaxation of magnetization in endohedral metallofullerenes DySc2N@C80 is studied at different temperatures, in different magnetic fields, and in different molecular arrangements. Magnetization behavior and relaxation are analyzed for powder sample, and for DySc2N@C80 diluted in non-magnetic fullerene Lu3N@C80, adsorbed in voids of a metal-organic framework, and dispersed in a polymer. The magnetic field dependence and zero-field ...[more]

PMID: 29671443

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Project description:The syntheses and properties of four magnetically-supramolecular oligomers of triangular Mn3 units are reported: dimeric [Mn6O2(O2CMe)8(CH3OH)2(pdpd)2] (3) and [Mn6O2(O2CMe)8(py)2(pdpd)2](ClO4)2 (4), and tetrameric [Mn12O4(O2CR)12(pdpd)6](ClO4)4 (R = Me (5), t Bu (6)). They were all obtained employing 3-phenyl-1,5-di(pyridin-2-yl)pentane-1,5-dione dioxime (pdpdH2), either in direct synthesis reactions involving oxidation of MnII salts or in metathesis reactions with the preformed complex [Mn3O(O2CMe)6(py)3](ClO4) (1); complex 6 was then obtained by carboxylate substitution on complex 5. Complexes 3 and 4 contain two [MnIII2MnII(μ3-O)]6+ and [MnIII3(μ3-O)]7+ units, respectively, linked by two pdpd2- groups. Complexes 5 and 6 contain four [MnIII3(μ3-O)]7+ units linked by six pdpd2- groups into a rectangular tetramer [MnIII3]4. Solid-state dc magnetic susceptibility studies showed that the Mn3 subunits in 3 and 4 have a ground-state spin of S = 3/2 and S = 2, respectively, while the Mn3 subunits in 5 and 6 possess an S = 6 ground state. Complexes 5 and 6 exhibit frequency-dependent out-of-phase (χ''M) ac susceptibility signals indicating 5 and 6 to be tetramers of Mn3 single-molecule magnets (SMMs). High-frequency EPR studies of a microcrystalline powder sample of 5·2CH2Cl2 provided precise spin Hamiltonian parameters of D = -0.33 cm-1, |E| = 0.03 cm-1, B04 = -8.0 × 10-5 cm-1, and g = 2.0. Magnetization vs. dc field sweeps on a single crystal of 5·xCH2Cl2 gave hysteresis loops below 1 K that exhibit exchange-biased quantum tunneling of magnetization (QTM) steps with a bias field of 0.19 T. Simulation of the loops determined that each Mn3 unit is exchange-coupled to the two neighbors linked to it by the pdpd2- linkers, with an antiferromagnetic inter-Mn3 exchange interaction of J/kB = -0.011 K (Ĥ = -2Jŝi ·ŝj convention). The work demonstrates a rational approach to synthesizing magnetically-supramolecular aggregates of SMMs as potential multi-qubit systems for quantum computing.

Dataset Information

Magnetization relaxation in the single-ion magnet DySc2N@C80: quantum tunneling, magnetic dilution, and unconventional temperature dependence.

Publications

Magnetization relaxation in the single-ion magnet DySc<sub>2</sub>N@C<sub>80</sub>: quantum tunneling, magnetic dilution, and unconventional temperature dependence.

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