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- ItemEngineering Kitaev exchange in stacked iridate layers: Impact of inter-layer species on in-plane magnetism(Cambridge : Royal Society of Chemistry, 2019) Yadav, R.; Eldeeb, M.S.; Ray, R.; Aswartham, S.; Sturza, M.I.; Nishimoto, S.; Van Den Brink, J.; Hozoi, L.Novel functionalities may be achieved in oxide electronics by appropriate stacking of planar oxide layers of different metallic species, MOp and M′Oq. The simplest mechanism allowing the tailoring of the electronic states and physical properties of such heterostructures is of electrostatic nature - charge imbalance between the M and M′ cations. Here we clarify the effect of interlayer electrostatics on the anisotropic Kitaev exchange in H3LiIr2O6, a recently proposed realization of the Kitaev spin liquid. By quantum chemical calculations, we show that the precise position of H+ cations between magnetically active [LiIr2O6]3- honeycomb-like layers has a strong impact on the magnitude of Kitaev interactions. In particular, it is found that stacking with straight interlayer O-H-O links is detrimental to in-plane Kitaev exchange since coordination by a single H-ion of the O ligand implies an axial Coulomb potential at the O site and unfavorable polarization of the O 2p orbitals mediating the Ir-Ir interactions. Our results therefore provide valuable guidelines for the rational design of Kitaev quantum magnets, indicating unprecedented Kitaev interactions of ≈40 meV if the linear interlayer linkage is removed.
- ItemAir-stable redox-active nanomagnets with lanthanide spins radical-bridged by a metal–metal bond(London : Nature Publishing Group, 2019) Liu, F.; Velkos, G.; Krylov, D.S.; Spree, L.; Zalibera, M.; Ray, R.; Samoylova, N.A.; Chen, C.-H.; Rosenkranz, M.; Schiemenz, S.; Ziegs, F.; Nenkov, K.; Kostanyan, A.; Greber, T.; Wolter, A.U.B.; Richter, M.; Büchner, B.; Avdoshenko, S.M.; Popov, A.A.Engineering intramolecular exchange interactions between magnetic metal atoms is a ubiquitous strategy for designing molecular magnets. For lanthanides, the localized nature of 4f electrons usually results in weak exchange coupling. Mediating magnetic interactions between lanthanide ions via radical bridges is a fruitful strategy towards stronger coupling. In this work we explore the limiting case when the role of a radical bridge is played by a single unpaired electron. We synthesize an array of air-stable Ln 2 @C 80 (CH 2 Ph) dimetallofullerenes (Ln 2 = Y 2 , Gd 2 , Tb 2 , Dy 2 , Ho 2 , Er 2 , TbY, TbGd) featuring a covalent lanthanide-lanthanide bond. The lanthanide spins are glued together by very strong exchange interactions between 4f moments and a single electron residing on the metal–metal bonding orbital. Tb 2 @C 80 (CH 2 Ph) shows a gigantic coercivity of 8.2 Tesla at 5 K and a high 100-s blocking temperature of magnetization of 25.2 K. The Ln-Ln bonding orbital in Ln 2 @C 80 (CH 2 Ph) is redox active, enabling electrochemical tuning of the magnetism.
- ItemPressure-induced dimerization and valence bond crystal formation in the Kitaev-Heisenberg magnet α-RuCl3(College Park, MD : American Physical Society, 2018) Bastien, G.; Garbarino, G.; Yadav, R.; Martinez-Casado, F.J.; Beltrán, Rodríguez, R.; Stahl, Q.; Kusch, M.; Limandri, S.P.; Ray, R.; Lampen-Kelley, P.; Mandrus, D.G.; Nagler, S.E.; Roslova, M.; Isaeva, A.; Doert, T.; Hozoi, L.; Wolter, A.U.B.; Büchner, B.; Geck, J.; Van Den Brink, J.Magnetization and high-resolution x-ray diffraction measurements of the Kitaev-Heisenberg material α-RuCl3 reveal a pressure-induced crystallographic and magnetic phase transition at a hydrostatic pressure of p∼0.2 GPa. This structural transition into a triclinic phase is characterized by a very strong dimerization of the Ru-Ru bonds, accompanied by a collapse of the magnetic susceptibility. Ab initio quantum-chemistry calculations disclose a pressure-induced enhancement of the direct 4d-4d bonding on particular Ru-Ru links, causing a sharp increase of the antiferromagnetic exchange interactions. These combined experimental and computational data show that the Kitaev spin-liquid phase in α-RuCl3 strongly competes with the crystallization of spin singlets into a valence bond solid.
- 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.