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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.
- ItemGrowth of PdCoO2 films with controlled termination by molecular-beam epitaxy and determination of their electronic structure by angle-resolved photoemission spectroscopy(Melville, NY : AIP Publ., 2022) Song, Qi; Sun, Jiaxin; Parzyck, Christopher T.; Miao, Ludi; Xu, Qing; Hensling, Felix V. E.; Barone, Matthew R.; Hu, Cheng; Kim, Jinkwon; Faeth, Brendan D.; Paik, Hanjong; King, Phil D. C.; Shen, Kyle M.; Schlom, Darrell G.Utilizing the powerful combination of molecular-beam epitaxy (MBE) and angle-resolved photoemission spectroscopy (ARPES), we produce and study the effect of different terminating layers on the electronic structure of the metallic delafossite PdCoO2. Attempts to introduce unpaired electrons and synthesize new antiferromagnetic metals akin to the isostructural compound PdCrO2 have been made by replacing cobalt with iron in PdCoO2 films grown by MBE. Using ARPES, we observe similar bulk bands in these PdCoO2 films with Pd-, CoO2-, and FeO2-termination. Nevertheless, Pd- and CoO2-terminated films show a reduced intensity of surface states. Additionally, we are able to epitaxially stabilize PdFexCo1-xO2 films that show an anomaly in the derivative of the electrical resistance with respect to temperature at 20 K, but do not display pronounced magnetic order.
- ItemSpin Hall effect emerging from a noncollinear magnetic lattice without spin-orbit coupling(Bristol : Institute of Physics Publishing, 2018) Zhang, Y.; Železný, J.; Sun, Y.; Van Den Brink, J.; Yan, B.The spin Hall effect (SHE), which converts a charge current into a transverse spin current, has long been believed to be a phenomenon induced by spin-orbit coupling. Here, we identify an alternative mechanism to realize the intrinsic SHE through a noncollinear magnetic structure that breaks the spin rotation symmetry. No spin-orbit coupling is needed even when the scalar spin chirality vanishes, different from the case of the topological Hall effect and topological SHE reported previously. In known noncollinear antiferromagnetic compounds Mn3X (X = Ga, Ge, and Sn), for example, we indeed obtain large spin Hall conductivities based on ab initio calculations.
- ItemElectronic structure and magnetic properties of the spin-1/2 Heisenberg system CuSe2O5(Milton Park : Taylor & Francis, 2009) Janson, O.; Schnelle, W.; Schmidt, M.; Prots, Yu; Drechsler, S.-L.; Filatov, S.K.; Rosner, H.A microscopic magnetic model for the spin-1/2 Heisenberg chain compound CuSe2O5 is developed based on the results of a joint experimental and theoretical study. Magnetic susceptibility and specific heat data give evidence for quasi-one-dimensional (1D) magnetism with leading antiferromagnetic (AFM) couplings and an AFM ordering temperature of 17 K. For microscopic insight, full-potential density functional theory (DFT) calculations within the local density approximation (LDA) were performed. Using the resulting band structure, a consistent set of transfer integrals for an effective one-band tight-binding model was obtained. Electronic correlations were treated on a mean-field level starting from LDA (LSDA+U method) and on a model level (Hubbard model). With excellent agreement between experiment and theory, we find that only two couplings in CuSe2O5 are relevant: the nearest-neighbour intra-chain interaction of 165 K and a non-frustrated inter-chain (IC) coupling of 20 K. From a comparison with structurally related systems (Sr2Cu(PO4)2, Bi2CuO4), general implications for a magnetic ordering in presence of IC frustration are made.
- ItemDomain wall asymmetries in Ni81Fe19/NiO: Proof of variable anisotropics in exchange bias systems(Milton Park : Taylor & Francis, 2009) McCord, Jeffrey; Schäfer, RudolfMultiple changes in the internal structure of magnetic domain walls due to alterations of the interfacial coupling across the ferromagnetic/antiferromagnetic interface are reported for Ni81Fe19/NiO exchange coupled films. Depending on the antiferromagnetically induced anisotropy, three different types of domain walls are observed. Cross-tie domain wall structures of decreased vortex to anti-vortex spacing develop with the addition of a thin antiferromagnetic layer. For exchange biased samples strong asymmetries in domain wall structure occur for the ascending and descending branch of the magnetization loop. For the descending branch a symmetric 180° Néel wall develops, whereas a folded cross-tie domain wall structure forms during magnetization reversal along the ascending loop branch. The novel type of 'zig-zagged' cross-tie wall is characterized by cross-ties reaching differently into the surrounding domain areas. The wall alterations indicate the existence of bi-modal coupling strengths in exchange coupled systems, which is in accordance with models of exchange bias that assume pinned and unpinned spins at the ferromagnetic/antiferromagnetic interface.
- ItemTopological Electronic Structure and Intrinsic Magnetization in MnBi4Te7: A Bi2Te3 Derivative with a Periodic Mn Sublattice(College Park, MD : American Physical Society, 2019) Vidal, R.C.; Zeugner, A.; Facio, J.I.; Ray, R.; Haghighi, M.H.; Wolter, A.U.B.; Corredor, Bohorquez, L.T.; Caglieris, F.; Moser, S.; Figgemeier, T.; Peixoto, T.R.F.; Vasili, H.B.; Valvidares, M.; Jung, S.; Cacho, C.; Alfonsov, A.; Mehlawat, K.; Kataev, V.; Hess, C.; Richter, M.; Büchner, B.; Van Den Brink, J.; Ruck, M.; Reinert, F.; Bentmann, H.; Isaeva, A.Combinations of nontrivial band topology and long-range magnetic order hold promise for realizations of novel spintronic phenomena, such as the quantum anomalous Hall effect and the topological magnetoelectric effect. Following theoretical advances, material candidates are emerging. Yet, so far a compound that combines a band-inverted electronic structure with an intrinsic net magnetization remains unrealized. MnBi2Te4 has been established as the first antiferromagnetic topological insulator and constitutes the progenitor of a modular (Bi2Te3)n(MnBi2Te4) series. Here, for n=1, we confirm a nonstoichiometric composition proximate to MnBi4Te7. We establish an antiferromagnetic state below 13 K followed by a state with a net magnetization and ferromagnetic-like hysteresis below 5 K. Angle-resolved photoemission experiments and density-functional calculations reveal a topologically nontrivial surface state on the MnBi4Te7(0001) surface, analogous to the nonmagnetic parent compound Bi2Te3. Our results establish MnBi4Te7 as the first band-inverted compound with intrinsic net magnetization providing a versatile platform for the realization of magnetic topological states of matter.
- ItemVoltage control of magnetic order in RKKY coupled multilayers(Washington, DC [u.a.] : Assoc., 2023) Kossak, Alexander E.; Huang, Mantao; Reddy, Pooja; Wolf, Daniel; Beach, Geoffrey S. D.In the field of antiferromagnetic (AFM) spintronics, there is a substantial effort present to make AFMs viable active components for efficient and fast devices. Typically, this is done by manipulating the AFM Néel vector. Here, we establish a method of enabling AFM active components by directly controlling the magnetic order. We show that magneto-ionic gating of hydrogen enables dynamic control of the Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction in solid-state synthetic AFM multilayer devices. Using a gate voltage, we tune the RKKY interaction to drive continuous transitions from AFM to FM and vice versa. The switching is submillisecond at room temperature and fully reversible. We validate the utility of this method by demonstrating that magneto-ionic gating of the RKKY interaction allows for 180° field-free deterministic switching. This dynamic method of controlling a fundamental exchange interaction can engender the manipulation of a broader array of spin textures, e.g., chiral domain walls and skyrmions.