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- ItemSingle Molecule Magnetism with Strong Magnetic Anisotropy and Enhanced Dy∙∙∙Dy Coupling in Three Isomers of Dy-Oxide Clusterfullerene Dy2O@C82(Chichester : John Wiley and Sons Ltd, 2019) Yang, W.; Velkos, G.; Liu, F.; Sudarkova, S.M.; Wang, Y.; Zhuang, J.; Zhang, H.; Li, X.; Zhang, X.; Büchner, B.; Avdoshenko, S.M.; Popov, A.A.; Chen, N.A new class of single-molecule magnets (SMMs) based on Dy-oxide clusterfullerenes is synthesized. Three isomers of Dy2O@C82 with Cs(6), C3v(8), and C2v(9) cage symmetries are characterized by single-crystal X-ray diffraction, which shows that the endohedral Dy−(µ2-O)−Dy cluster has bent shape with very short Dy−O bonds. Dy2O@C82 isomers show SMM behavior with broad magnetic hysteresis, but the temperature and magnetization relaxation depend strongly on the fullerene cage. The short Dy−O distances and the large negative charge of the oxide ion in Dy2O@C82 result in the very strong magnetic anisotropy of Dy ions. Their magnetic moments are aligned along the Dy−O bonds and are antiferromagnetically (AFM) coupled. At low temperatures, relaxation of magnetization in Dy2O@C82 proceeds via the ferromagnetically (FM)-coupled excited state, giving Arrhenius behavior with the effective barriers equal to the AFM-FM energy difference. The AFM-FM energy differences of 5.4–12.9 cm−1 in Dy2O@C82 are considerably larger than in SMMs with {Dy2O2} bridges, and the Dy∙∙∙Dy exchange coupling in Dy2O@C82 is the strongest among all dinuclear Dy SMMs with diamagnetic bridges. Dy-oxide clusterfullerenes provide a playground for the further tuning of molecular magnetism via variation of the size and shape of the fullerene cage.
- ItemMagnetic anisotropy of endohedral lanthanide ions: paramagnetic NMR study of MSc2N@C80-Ih with M running through the whole 4f row(Cambridge : RSC, 2015) Zhang, Y.; Krylov, D.; Rosenkranz, M.; Schiemenz, S.; Popov, A. A.Paramagnetic and variable temperature 13C and 45Sc nuclear magnetic resonance studies are performed for nitride clusterfullerenes MSc2N@C80 with icosahedral Ih(7) carbon cage, where M runs through all lanthanides forming nitride clusters. The influence of the endohedral lanthanide ions on the NMR spectral pattern is carefully followed, and dramatic differences are found in peak positions and line widths. Thus, 13C lines broaden from 0.01–0.02 ppm in diamagnetic MSc2N@C80 molecules (M = La, Y, Lu) to several ppm in TbSc2N@C80 and DySc2N@C80. Direction of the paramagnetic shift depends on the shape of the 4f electron density in corresponding lanthanide ions. In TmSc2N@C80 and ErSc2N@C80 with prolate 4f-density of lanthanide ions, 13C signals are shifted down-field, whereas 45Sc peaks are shifted up-field versus diamagnetic values. In all other MSc2N@C80 molecules lanthanide ions have oblate-shaped 4f electron density, and the lanthanide-induced shift is negative for 13C and positive for 45Sc peaks. Analysis of the pseudocontact and contact contributions to chemical shifts revealed that the pseudocontact term dominates both in 13C and 45Sc NMR spectra, although contact shifts for 13C signals are also considerable. Point charge computations of the ligand field splitting are performed to explain experimental results, and showed reasonable agreement with experimental pseudocontact shifts. Nitrogen atom bearing large negative charge and located close to the lanthanide ion results in large magnetic anisotropy of lanthanide ions in nitride clusterfullerenes with quasi-uniaxial ligand field.
- ItemTopological boundaries between helical domains as a nucleation source of skyrmions in the bulk cubic helimagnet Cu2OSeO3(College Park, MD : APS, 2022) Leonov, A.O.; Pappas, C.Cu2OSeO3 represents a unique example in the family of B20 cubic helimagnets with a tilted spiral and a low-temperature skyrmion phase arising for magnetic fields applied along the easy crystallographic (100) axes. Although the stabilization mechanism of these phases can be accounted for by cubic magnetic anisotropy, the skyrmion nucleation process is still an open question, since the stability region of the skyrmion phase displays strongly hysteretic behavior with different phase boundaries for increasing and decreasing magnetic fields. Here, we address this important point using micromagnetic simulations and come to the conclusion that skyrmion nucleation is underpinned by the reorientation of spiral domains occurring near the critical magnetic fields of the phase diagrams: HC1, the critical field of the transition between the helical and conical/tiled spiral phase, and HC2, the critical field between the conical/tiled spiral and the homogenous phase. By studying a wide variety of cases we show that domain walls may have a 3D structure. Moreover, they can carry a finite topological charge stemming from half-skyrmions (merons) also permitting along-the-field and perpendicular-to-the-field orientation. Thus, domain walls may be envisioned as nucleation source of skyrmions that can form thermodynamically stable and metastable lattices as well as skyrmion networks with misaligned skyrmion tubes. The results of numerical simulations are discussed in view of recent experimental data on chiral magnets, in particular, for the bulk cubic helimagnet Cu2OSeO3.
- ItemResearch Update: Magnetoionic control of magnetization and anisotropy in layered oxide/metal heterostructures(New York : American Institute of Physics, 2016) Duschek, K.; Pohl, D.; Fähler, S.; Nielsch, K.; Leistner, K.Electric field control of magnetization and anisotropy in layered structures with perpendicular magnetic anisotropy is expected to increase the versatility of spintronic devices. As a model system for reversible voltage induced changes of magnetism by magnetoionic effects, we present several oxide/metal heterostructures polarized in an electrolyte. Room temperature magnetization of Fe-O/Fe layers can be changed by 64% when applying only a few volts in 1M KOH. In a next step, the bottom interface of the in-plane magnetized Fe layer is functionalized by an L10 FePt(001) underlayer exhibiting perpendicular magnetic anisotropy. During subsequent electrocrystallization and electrooxidation, well defined epitaxial Fe3O4/Fe/FePt heterostructures evolve. The application of different voltages leads to a thickness change of the Fe layer sandwiched between Fe-O and FePt. At the point of transition between rigid magnet and exchange spring magnet regime for the Fe/FePt bilayer, this induces a large variation of magnetic anisotropy.
- ItemSpin-glass state and reversed magnetic anisotropy induced by Cr doping in the Kitaev magnet α-RuCl3(College Park, MD : American Physical Society, 2019) Bastien, G.; Roslova, M.; Haghighi, M.H.; Mehlawat, K.; Hunger, J.; Isaeva, A.; Doert, T.; Vojta, M.; Büchner, B.; Wolter, A.U.B.Magnetic properties of the substitution series Ru1-xCrxCl3 were investigated to determine the evolution from the anisotropic Kitaev magnet α-RuCl3 with Jeff=1/2 magnetic Ru3+ ions to the isotropic Heisenberg magnet CrCl3 with S=3/2 magnetic Cr3+ ions. Magnetization measurements on single crystals revealed a reversal of the magnetic anisotropy under doping, which we argue to arise from the competition between anisotropic Kitaev and off-diagonal interactions on the Ru-Ru links and approximately isotropic Cr-Ru and isotropic Cr-Cr interactions. In addition, combined magnetization, ac susceptibility, and specific-heat measurements clearly show the destabilization of the long-range magnetic order of α-RuCl3 in favor of a spin-glass state of Ru1-xCrxCl3 for a low doping of x≤0.1. The corresponding freezing temperature as a function of Cr content shows a broad maximum around x ≤ 0.45.