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    Single 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.
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    Spectromicroscopic measurements of electronic structure variations in atomically thin WSe2
    (2020) Klaproth, T.; Habenicht, C.; Schuster, R.; Büchner, B.; Knupfer, M.; Koitzsch, A.
    Atomically thin transition metal dichalcogenides (TMDCs) are promising candidates for implementation in next generation semiconducting devices, for which laterally homogeneous behavior is needed. Here, we study the electronic structure of atomically thin exfoliated WSe2, a prototypical TMDC with large spin–orbit coupling, by photoemission electron microscopy, electron energy-loss spectroscopy, and density functional theory. We resolve the inhomogeneities of the doping level by the varying energy positions of the valence band. There appear to be different types of inhomogeneities that respond differently to electron doping, introduced by potassium intercalation. In addition, we find that the doping process itself is more complex than previously anticipated and entails a distinct orbital and thickness dependence that needs to be considered for effective band engineering. In particular, the density of selenium vs tungsten states depends on the doping level, which leads to changes in the optical response beyond increased dielectric screening. Our work gives insight into the inhomogeneity of the electron structure of WSe2 and the effects of electron doping, provides microscopic understanding thereof, and improves the basis for property engineering of 2D materials.
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    Impact of Mn-Pn intermixing on magnetic properties of an intrinsic magnetic topological insulator: the µSR perspective
    (Bristol : IOP Publ., 2023) Sahoo, M.; Salman, Z.; Allodi, G.; Isaeva, A.; Folkers, L.; Wolter, A.U.B.; Büchner, B.; De Renzi, R.
    We investigated the magnetic properties of polycrystalline samples of the intrinsic magnetic topological insulators MnPn2Te4, with pnictogen Pn = Sb, Bi, by bulk magnetization and μSR. DC susceptibility detects the onset of magnetic ordering at TN = 27 K and 24 K and a field dependence of the macroscopic magnetization compatible with ferri- (or ferro-) and atiferro- magnetic ordering, respectively. Weak transverse field (wTF) Muon Spin Rotation (μSR) confirms the homogeneous bulk nature of magnetic ordering at the same two distinct transition temperatures. Zero Field (ZF) μSR shows that the Sb based material displays a broader distribution of internal field at the muon, in accordance with a larger deviation from the stoichiomectric composition and a higher degree of positional disorder (Mn at the Pn(6c) site), which however does not affect significantly the sharpness of the thermodynamic transition, as detected by the muon magnetic volume fraction and the observability of a critical divergence in the longitudinal and transverse muon relaxation rates.
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    Two-dimensional ferromagnetic extension of a topological insulator
    (College Park, MD : APS, 2023) Kagerer, P.; Fornari, C. I.; Buchberger, S.; Tschirner, T.; Veyrat, L.; Kamp, M.; Tcakaev, A. V.; Zabolotnyy, V.; Morelhão, S. L.; Geldiyev, B.; Müller, S.; Fedorov, A.; Rienks, E.; Gargiani, P.; Valvidares, M.; Folkers, L. C.; Isaeva, A.; Büchner, B.; Hinkov, V.; Claessen, R.; Bentmann, H.; Reinert, F.
    Inducing a magnetic gap at the Dirac point of the topological surface state (TSS) in a three-dimensional (3D) topological insulator (TI) is a route to dissipationless charge and spin currents. Ideally, magnetic order is present only at the surface, as through proximity of a ferromagnetic (FM) layer. However, experimental evidence of such a proximity-induced Dirac mass gap is missing, likely due to an insufficient overlap of TSS and the FM subsystem. Here, we take a different approach, namely ferromagnetic extension (FME), using a thin film of the 3D TI Bi2Te3, interfaced with a monolayer of the lattice-matched van der Waals ferromagnet MnBi2Te4. Robust 2D ferromagnetism with out-of-plane anisotropy and a critical temperature of Tc≈15 K is demonstrated by x-ray magnetic dichroism and electrical transport measurements. Using angle-resolved photoelectron spectroscopy, we observe the opening of a sizable magnetic gap in the 2D FM phase, while the surface remains gapless in the paramagnetic phase above Tc. Ferromagnetic extension paves the way to explore the interplay of strictly 2D magnetism and topological surface states, providing perspectives for realizing robust quantum anomalous Hall and chiral Majorana states.
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    Strong effects of uniaxial pressure and short-range correlations in Cr2Ge2Te6
    (College Park, MD : APS, 2022) Spachmann, S.; Elghandour, A.; Selter, S.; Büchner, B.; Aswartham, S.; Klingeler, R.
    Cr2Ge2Te6 is a quasi-two-dimensional semiconducting van der Waals ferromagnet down to the bilayer with great potential for technological applications. Engineering the critical temperature to achieve room-temperature applications is one of the critical next steps on this path. Here, we report high-resolution capacitance dilatometry studies on Cr2Ge2Te6 single crystals which directly prove significant magnetoelastic coupling and provide quantitative values of the large uniaxial pressure effects on long-range magnetic order (∂TC/∂pc=24.7 K/GPa and ∂TC/∂pab=−15.6 K/GPa) derived from thermodynamic relations. Moderate in-plane strain is thus sufficient to strongly enhance ferromagnetism in Cr2Ge2Te6 up to room temperature. Moreover, unambiguous signs of short-range magnetic order up to 200 K are found.
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    Tuning the interplay between nematicity and spin fluctuations in Na1-x Li x FeAs superconductors
    (London : Nature Publishing Group, 2018) Baek, S.-H.; Bhoi, D.; Nam, W.; Lee, B.; Efremov, D.V.; Büchner, B.; Kim, K.H.
    Strong interplay of spin and charge/orbital degrees of freedom is the fundamental characteristic of the iron-based superconductors (FeSCs), which leads to the emergence of a nematic state as a rule in the vicinity of the antiferromagnetic state. Despite intense debate for many years, however, whether nematicity is driven by spin or orbital fluctuations remains unsettled. Here, by use of transport, magnetization, and 75As nuclear magnetic resonance (NMR) measurements, we show a striking transformation of the relationship between nematicity and spin fluctuations (SFs) in Na1-x Li x FeAs; For x ≤ 0.02, the nematic transition promotes SFs. In contrast, for x ≥ 0.03, the system undergoes a non-magnetic phase transition at a temperature T 0 into a distinct nematic state that suppresses SFs. Such a drastic change of the spin fluctuation spectrum associated with nematicity by small doping is highly unusual, and provides insights into the origin and nature of nematicity in FeSCs.
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    Spectral field mapping in plasmonic nanostructures with nanometer resolution
    (London : Nature Publishing Group, 2018) Krehl, J.; Guzzinati, G.; Schultz, J.; Potapov, P.; Pohl, D.; Martin, J.; Verbeeck, J.; Fery, A.; Büchner, B.; Lubk, A.
    Plasmonic nanostructures and -devices are rapidly transforming light manipulation technology by allowing to modify and enhance optical fields on sub-wavelength scales. Advances in this field rely heavily on the development of new characterization methods for the fundamental nanoscale interactions. However, the direct and quantitative mapping of transient electric and magnetic fields characterizing the plasmonic coupling has been proven elusive to date. Here we demonstrate how to directly measure the inelastic momentum transfer of surface plasmon modes via the energy-loss filtered deflection of a focused electron beam in a transmission electron microscope. By scanning the beam over the sample we obtain a spatially and spectrally resolved deflection map and we further show how this deflection is related quantitatively to the spectral component of the induced electric and magnetic fields pertaining to the mode. In some regards this technique is an extension to the established differential phase contrast into the dynamic regime. © 2018, The Author(s).
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    Fe1-xNix alloy nanoparticles encapsulated inside carbon nanotubes: Controlled synthesis, structure and magnetic properties
    (Basel : MDPI AG, 2018) Ghunaim, R.; Damm, C.; Wolf, D.; Lubk, A.; Büchner, B.; Mertig, M.; Hampel, S.
    In the present work, different synthesis procedures have been demonstrated to fill carbon nanotubes (CNTs) with Fe1-xNix alloy nanoparticles (x = 0.33, 0.5). CNTs act as templates for the encapsulation of magnetic nanoparticles, and provide a protective shield against oxidation as well as prevent nanoparticles agglomeration. By variation of the reaction parameters, the purity of the samples, degree of filling, the composition and size of filling nanoparticles have been tailored and therefore the magnetic properties. The samples were analyzed by scanning electron microscopy (SEM), transmission electron microscopy (TEM), Bright-field (BF) TEM tomography, X-ray powder diffraction, superconducting quantum interference device (SQUID) and thermogravimetric analysis (TGA). The Fe1-x Nix-filled CNTs show a huge enhancement in the coercive fields compared to the corresponding bulk materials, which make them excellent candidates for several applications such as magnetic storage devices.
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    Single molecule magnet with an unpaired electron trapped between two lanthanide ions inside a fullerene
    (London : Nature Publishing Group, 2017) Liu, F.; Krylov, D.S.; Spree, L.; Avdoshenko, S.M.; Samoylova, N.A.; Rosenkranz, M.; Kostanyan, A.; Greber, T.; Wolter, A.U.B.; Büchner, B.; Popov, A.A.
    Increasing the temperature at which molecules behave as single-molecule magnets is a serious challenge in molecular magnetism. One of the ways to address this problem is to create the molecules with strongly coupled lanthanide ions. In this work, endohedral metallofullerenes Y 2 @C 80 and Dy 2 @C 80 are obtained in the form of air-stable benzyl monoadducts. Both feature an unpaired electron trapped between metal ions, thus forming a single-electron metal-metal bond. Giant exchange interactions between lanthanide ions and the unpaired electron result in single-molecule magnetism of Dy 2 @C 80 (CH 2 Ph) with a record-high 100 s blocking temperature of 18 K. All magnetic moments in Dy 2 @C 80 (CH 2 Ph) are parallel and couple ferromagnetically to form a single spin unit of 21 μ B with a dysprosium-electron exchange constant of 32 cm -1. The barrier of the magnetization reversal of 613 K is assigned to the state in which the spin of one Dy centre is flipped.
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    Possible experimental realization of a basic Z 2 topological semimetal in GaGeTe
    (College Park, MD : American Institute of Physics, 2019) Haubold, E.; Fedorov, A.; Pielnhofer, F.; Rusinov, I.P.; Menshchikova, T.V.; Duppel, V.; Friedrich, D.; Weihrich, R.; Pfitzner, A.; Zeugner, A.; Isaeva, A.; Thirupathaiah, S.; Kushnirenko, Y.; Rienks, E.; Kim, T.; Chulkov, E.V.; Büchner, B.; Borisenko, S.
    We report experimental and theoretical evidence that GaGeTe is a basic Z2 topological semimetal with three types of charge carriers: bulk-originated electrons and holes as well as surface state electrons. This electronic situation is qualitatively similar to the classic 3D topological insulator Bi2Se3, but important differences account for an unprecedented transport scenario in GaGeTe. High-resolution angle-resolved photoemission spectroscopy combined with advanced band structure calculations show a small indirect energy gap caused by a peculiar band inversion at the T-point of the Brillouin zone in GaGeTe. An energy overlap of the valence and conduction bands brings both electron and holelike carriers to the Fermi level, while the momentum gap between the corresponding dispersions remains finite. We argue that peculiarities of the electronic spectrum of GaGeTe have a fundamental importance for the physics of topological matter and may boost the material's application potential.