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Now showing 1 - 10 of 45
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    Saturation of the anomalous Hall effect at high magnetic fields in altermagnetic RuO2
    (Melville, NY : AIP Publ., 2023) Tschirner, Teresa; Keßler, Philipp; Gonzalez Betancourt, Ruben Dario; Kotte, Tommy; Kriegner, Dominik; Büchner, Bernd; Dufouleur, Joseph; Kamp, Martin; Jovic, Vedran; Smejkal, Libor; Sinova, Jairo; Claessen, Ralph; Jungwirth, Tomas; Moser, Simon; Reichlova, Helena; Veyrat, Louis
    Observations of the anomalous Hall effect in RuO2 and MnTe have demonstrated unconventional time-reversal symmetry breaking in the electronic structure of a recently identified new class of compensated collinear magnets, dubbed altermagnets. While in MnTe, the unconventional anomalous Hall signal accompanied by a vanishing magnetization is observable at remanence, the anomalous Hall effect in RuO2 is excluded by symmetry for the Néel vector pointing along the zero-field [001] easy-axis. Guided by a symmetry analysis and ab initio calculations, a field-induced reorientation of the Néel vector from the easy-axis toward the [110] hard-axis was used to demonstrate the anomalous Hall signal in this altermagnet. We confirm the existence of an anomalous Hall effect in our RuO2 thin-film samples, whose set of magnetic and magneto-transport characteristics is consistent with the earlier report. By performing our measurements at extreme magnetic fields up to 68 T, we reach saturation of the anomalous Hall signal at a field Hc ≃ 55 T that was inaccessible in earlier studies but is consistent with the expected Néel-vector reorientation field.
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    Magnetic Hysteresis at 10 K in Single Molecule Magnet Self‐Assembled on Gold
    (Weinheim : Wiley-VCH, 2021) Chen, Chia-Hsiang; Spree, Lukas; Koutsouflakis, Emmanouil; Krylov, Denis S.; Liu, Fupin; Brandenburg, Ariane; Velkos, Georgios; Schimmel, Sebastian; Avdoshenko, Stanislav M.; Federov, Alexander; Weschke, Eugen; Choueikani, Fadi; Ohresser, Philippe; Dreiser, Jan; Büchner, Bernd; Popov, Alexey A.
    Tremendous progress in the development of single molecule magnets (SMMs) raises the question of their device integration. On this route, understanding the properties of low‐dimensional assemblies of SMMs, in particular in contact with electrodes, is a necessary but difficult step. Here, it is shown that fullerene SMM self‐assembled on metal substrate from solution retains magnetic hysteresis up to 10 K. Fullerene‐SMM DySc2N@C80 and Dy2ScN@C80 are derivatized to introduce a thioacetate group, which is used to graft SMMs on gold. Magnetic properties of grafted SMMs are studied by X‐ray magnetic circular dichroism and compared to the films of nonderivatized fullerenes prepared by sublimation. In self‐assembled films, the magnetic moments of the Dy ions are preferentially aligned parallel to the surface, which is different from the disordered orientation of endohedral clusters in nonfunctionalized fullerenes. Whereas chemical derivatization reduces the blocking temperature of magnetization and narrows the hysteresis of Dy2ScN@C80, for DySc2N@C80 equally broad hysteresis is observed as in the fullerene multilayer. Magnetic bistability in the DySc2N@C80 grafted on gold is sustained up to 10 K. This study demonstrates that self‐assembly of fullerene‐SMM derivatives offers a facile solution‐based procedure for the preparation of functional magnetic sub‐monolayers with excellent SMM performance.
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    Intermixing-Driven Surface and Bulk Ferromagnetism in the Quantum Anomalous Hall Candidate MnBi6Te10
    (Weinheim : Wiley-VCH, 2023) Tcakaev, Abdul‐Vakhab; Rubrecht, Bastian; Facio, Jorge I.; Zabolotnyy, Volodymyr B.; Corredor, Laura T.; Folkers, Laura C.; Kochetkova, Ekaterina; Peixoto, Thiago R. F.; Kagerer, Philipp; Heinze, Simon; Bentmann, Hendrik; Green, Robert J.; Gargiani, Pierluigi; Valvidares, Manuel; Weschke, Eugen; Haverkort, Maurits W.; Reinert, Friedrich; van den Brink, Jeroen; Büchner, Bernd; Wolter, Anja U. B.; Isaeva, Anna; Hinkov, Vladimir
    The recent realizations of the quantum anomalous Hall effect (QAHE) in MnBi2Te4 and MnBi4Te7 benchmark the (MnBi2Te4)(Bi2Te3)n family as a promising hotbed for further QAHE improvements. The family owes its potential to its ferromagnetically (FM) ordered MnBi2Te4 septuple layers (SLs). However, the QAHE realization is complicated in MnBi2Te4 and MnBi4Te7 due to the substantial antiferromagnetic (AFM) coupling between the SLs. An FM state, advantageous for the QAHE, can be stabilized by interlacing the SLs with an increasing number n of Bi2Te3 quintuple layers (QLs). However, the mechanisms driving the FM state and the number of necessary QLs are not understood, and the surface magnetism remains obscure. Here, robust FM properties in MnBi6Te10 (n = 2) with Tc ≈ 12 K are demonstrated and their origin is established in the Mn/Bi intermixing phenomenon by a combined experimental and theoretical study. The measurements reveal a magnetically intact surface with a large magnetic moment, and with FM properties similar to the bulk. This investigation thus consolidates the MnBi6Te10 system as perspective for the QAHE at elevated temperatures.
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    Robust Single Molecule Magnet Monolayers on Graphene and Graphite with Magnetic Hysteresis up to 28 K
    (Weinheim : Wiley-VCH, 2021) Spree, Lukas; Liu, Fupin; Neu, Volker; Rosenkranz, Marco; Velkos, Georgios; Wang, Yaofeng; Schiemenz, Sandra; Dreiser, Jan; Gargiani, Pierluigi; Valvidares, Manuel; Chen, Chia-Hsiang; Büchner, Bernd; Avdoshenko, Stanislav M.; Popov, Alexey A.
    The chemical functionalization of fullerene single molecule magnet Tb2@C80(CH2Ph) enables the facile preparation of robust monolayers on graphene and highly oriented pyrolytic graphite from solution without impairing their magnetic properties. Monolayers of endohedral fullerene functionalized with pyrene exhibit magnetic bistability up to a temperature of 28 K. The use of pyrene terminated linker molecules opens the way to devise integration of spin carrying units encapsulated by fullerene cages on graphitic substrates, be it single-molecule magnets or qubit candidates. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH
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    Substrate-Independent Magnetic Bistability in Monolayers of the Single-Molecule Magnet Dy2ScN@C80 on Metals and Insulators
    (Weinheim : Wiley-VCH, 2020) Krylov, Denis S.; Schimmel, Sebastian; Dubrovin, Vasilii; Liu, Fupin; Nguyen, T.T. Nhung; Spree, Lukas; Chen, Chia-Hsiang; Velkos, Georgios; Bulbucan, Claudiu; Westerström, Rasmus; Studniarek, Michał; Dreiser, Jan; Hess, Christian; Büchner, Bernd; Avdoshenko, Stanislav M.; Popov, Alexey A.
    Magnetic hysteresis is demonstrated for monolayers of the single-molecule magnet (SMM) Dy2ScN@C80 deposited on Au(111), Ag(100), and MgO|Ag(100) surfaces by vacuum sublimation. The topography and electronic structure of Dy2ScN@C80 adsorbed on Au(111) were studied by STM. X-ray magnetic CD studies show that the Dy2ScN@C80 monolayers exhibit similarly broad magnetic hysteresis independent on the substrate used, but the orientation of the Dy2ScN cluster depends strongly on the surface. DFT calculations show that the extent of the electronic interaction of the fullerene molecules with the surface is increasing dramatically from MgO to Au(111) and Ag(100). However, the charge redistribution at the fullerene-surface interface is fully absorbed by the carbon cage, leaving the state of the endohedral cluster intact. This Faraday cage effect of the fullerene preserves the magnetic bistability of fullerene-SMMs on conducting substrates and facilitates their application in molecular spintronics. © 2019 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.
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    Tailoring Plasmonics of Au@Ag Nanoparticles by Silica Encapsulation
    (Weinheim : Wiley-VCH, 2021) Schultz, Johannes; Kirner, Felizitas; Potapov, Pavel; Büchner, Bernd; Lubk, Axel; Sturm, Elena V.
    Hybrid metallic nanoparticles (NPs) encapsulated in oxide shells are currently intensely studied for plasmonic applications in sensing, medicine, catalysis, and photovoltaics. Here, a method for the synthesis of Au@Ag@SiO2 cubes with a uniform silica shell of variable and adjustable thickness in the nanometer range is introduced and their excellent, highly reproducible, and tunable optical response is demonstrated. Varying the silica shell thickness, the excitation energies of the single NP plasmon modes can be tuned in a broad spectral range between 2.55 and 3.25 eV. Most importantly, a strong coherent coupling of the surface plasmons is revealed at the silver–silica interface with Mie resonances at the silica–vacuum interface leading to a significant field enhancement at the encapsulated NP surface in the range of 100% at shell thicknesses t ≃ 20 nm. Consequently, the synthesis method and the field enhancement open pathways to a widespread use of silver NPs in plasmonic applications including photonic crystals and may be transferred to other non-precious metals. © 2021 The Authors. Advanced Optical Materials published by Wiley-VCH GmbH
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    Exciton dispersion in para-quaterphenyl: Significant molecular interactions beyond Coulomb coupling
    (New York, NY : American Inst. of Physics, 2021) Graf, Lukas; Krupskaya, Yulia; Büchner, Bernd; Knupfer, Martin
    We have experimentally determined the momentum dependence of the electronic excitation spectra of para-quaterphenyl single crystals. The parallel arrangement of para-quaterphenyl molecules results in a strong Coulomb coupling of the molecular excitons. Such crystals have been considered to be a very good realization of the Frenkel exciton model, including the formation of H-type aggregates. Our data reveal an unexpected exciton dispersion of the upper Davydov component, which cannot be rationalized in terms of inter-molecular Coulomb coupling of the excitons. A significant reduction of the nearest neighbor coupling due to additional charge-transfer processes is able to provide an explanation of the data. Furthermore, the spectral onset of the excitation spectrum, which represents a heavy exciton resulting from exciton-phonon coupling, also shows a clear dispersion, which had been unknown so far. Finally, an optically forbidden excitation about 1 eV above the excitation onset is observed. © 2021 Author(s).
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    Crystal Growth of the Quasi-2D Quarternary Compound AgCrP2S6 by Chemical Vapor Transport
    (2021) Selter, Sebastian; Shemerliuk, Yuliia; Büchner, Bernd; Aswartham, Saicharan
    We report optimized crystal growth conditions for the quarternary compound AgCrP2S6 by chemical vapor transport. Compositional and structural characterization of the obtained crystals were carried out by means of energy-dispersive X-ray spectroscopy and powder X-ray diffraction. AgCrP2S6 is structurally closely related to the M2P2S6 family, which contains several compounds that are under investigation as 2D magnets. As-grown crystals exhibit a plate-like, layered morphology as well as a hexagonal habitus. AgCrP2S6 crystallizes in monoclinic symmetry in the space group P2/a (No. 13). The successful growth of large high-quality single crystals paves the way for further investigations of low dimensional magnetism and its anisotropies in the future and may further allow for the manufacturing of few-layer (or even monolayer) samples by exfoliation.
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    TSFZ Growth of Eu-Substituted Large-Size LSCO Crystals
    (Basel : MDPI, 2022) Voloshyna, Olesia; Romaka, Vitaliy V.; Karmakar, Koushik ;Seiro, Silvia; Maljuk, Andrey; Büchner, Bernd
    The travelling solvent floating zone (TSFZ) growth of Eu-substituted LSCO (La1.81−xEuxSr0.19CuO4, with nominal x = 0 ÷ 0.4) single crystals was systematically explored for the first time. The substitution of La with Eu considerably decreased the decomposition temperature. Optimal growth parameters were found to be: oxygen pressure 9.0–9.5 bars; Eu-free CuO-poor solvent (66 mol% CuO) with a molar ratio of La2O3:SrCO3:CuO = 4:4.5:16.5 and growth rate 0.6 mm/hour. The obtained single crystals were characterized with optical polarized microscopy, X-ray diffraction and energy-dispersive X-ray spectroscopy analysis. The solubility of Eu in LSCO appeared to be limited to x~0.36–0.38 under the used conditions. The substitution of La3+ with smaller Eu3+ ions led to a structural transition from tetragonal with space group I4/mmm for La1.81Sr0.19CuO4 (x = 0) to orthorhombic with space group Fmmm for La1.81−xSr0.19EuxCuO4 (x = 0.2, 0.3, 0.4), and to a substantial shrinking of the c-axis from 13.2446 Å (x = 0.0) to 13.1257 Å (x = 0.4). Such structural changes were accompanied by a dramatic decrease in the superconducting critical temperature, Tc, from 29.5 K for x = 0 to 13.8 K for 0.2. For x ≥ 0.3, no superconductivity was detected down to 4 K.
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    Flux Growth and Characterization of Bulk InVO4 Crystals
    (Basel : MDPI, 2023) Voloshyna, Olesia; Gorbunov, Mikhail V.; Mikhailova, Daria; Maljuk, Andrey; Seiro, Silvia; Büchner, Bernd
    The flux growth of InVO4 bulk single crystals has been explored for the first time. The reported eutectic composition at a ratio of V2O5:InVO4 = 1:1 could not be used as a self-flux since no sign of melting was observed up to 1100 °C. Crystals of InVO4 of typical size 0.5 × 1 × 7 mm3 were obtained using copper pyrovanadate (Cu2V2O7) as a flux, using Pt crucibles. X-ray powder diffraction confirmed the orthorhombic Cmcm structure. Rests of the flux material were observed on the sample surface, with occasional traces of Pt indicating some level of reaction with the crucible. X-ray absorption spectroscopy showed that oxidation states of indium and vanadium ions are +3 and +5, respectively. The size and high quality of the obtained InVO4 crystals makes them excellent candidates for further study of their physical properties.