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- ItemPhononic-magnetic dichotomy of the thermal Hall effect in the Kitaev material Na2 Co2 TeO6(College Park, MD : APS, 2023) Gillig, Matthias; Hong, Xiaochen; Wellm, Christoph; Kataev, Vladislav; Yao, Weiliang; Li, Yuan; Büchner, Bernd; Hess, ChristianThe quest for a half-quantized thermal Hall effect of a Kitaev system represents an important tool to probe topological edge currents of emergent Majorana fermions. Pertinent experimental findings for α-RuCl3 are, however, strongly debated, and it has been argued that the thermal Hall signal stems from phonons or magnons rather than from Majorana fermions. Here, we investigate the thermal Hall effect of the Kitaev candidate material Na2Co2TeO6, and we show that the measured signal emerges from at least two components, phonons and magnetic excitations. This dichotomy results from our discovery that the longitudinal and transversal heat conductivities share clear phononic signatures, while the transversal signal changes sign upon entering the low-temperature, magnetically ordered phase. Our results demonstrate that uncovering a genuinely quantized magnetic thermal Hall effect in Kitaev topological quantum spin liquids such as α-RuCl3 and Na2Co2TeO6 requires disentangling phonon vs magnetic contributions, including potentially fractionalized excitations such as the expected Majorana fermions.
- ItemStrong surface termination dependence of the electronic structure of polar superconductor LaFeAsO revealed by nano-ARPES([London] : IOP, 2022) Jung, Sung Won; Rhodes, Luke C; Watson, Matthew D; Evtushinsky, Daniil V; Cacho, Cephise; Aswartham, Saicharan; Kappenberger, Rhea; Wurmehl, Sabine; Büchner, Bernd; Kim, Timur KThe electronic structures of the iron-based superconductors have been intensively studied by using angle-resolved photoemission spectroscopy (ARPES). A considerable amount of research has been focused on the LaFeAsO family, showing the highest transition temperatures, where previous ARPES studies have found much larger Fermi surfaces than bulk theoretical calculations would predict. The discrepancy has been attributed to the presence of termination-dependent surface states. Here, using photoemission spectroscopy with a sub-micron focused beam spot (nano-ARPES) we have successfully measured the electronic structures of both the LaO and FeAs terminations in LaFeAsO. Our data reveal very different band dispersions and core-level spectra for different surface terminations, showing that previous macro-focus ARPES measurements were incomplete. Our results give direct evidence for the surface-driven electronic structure reconstruction in LaFeAsO, including formation of the termination-dependent surface states at the Fermi level. This experimental technique, which we have shown to be very powerful when applied to this prototypical compound, can now be used to study various materials with different surface terminations.
- ItemPhonon thermal transport shaped by strong spin-phonon scattering in a Kitaev material Na2Co2TeO6([London] : Nature Publishing Group, 2024) Hong, Xiaochen; Gillig, Matthias; Yao, Weiliang; Janssen, Lukas; Kocsis, Vilmos; Gass, Sebastian; Li, Yuan; Wolter, Anja U. B.; Büchner, Bernd; Hess, ChristianThe report of a half-quantized thermal Hall effect and oscillatory structures in the magnetothermal conductivity in the Kitaev material α-RuCl3 have sparked a strong debate on whether it is generated by Majorana fermion edge currents, spinon Fermi surface, or whether other more conventional mechanisms are at its origin. Here, we report low temperature thermal conductivity (κ) of another candidate Kitaev material, Na2Co2TeO6. The application of a magnetic field (B) along different principal axes of the crystal reveals a strong directional-dependent B impact on κ, while no evidence for mobile quasiparticles except phonons can be concluded at any field. Instead, severely scattered phonon transport prevails across the B−T phase diagram, revealing cascades of phase transitions for all B directions. Our results thus cast doubt on recent proposals for significant itinerant magnetic excitations in Na2Co2TeO6, and emphasize the importance of discriminating true spin liquid transport properties from scattered phonons in candidate materials.
- ItemSixfold fermion near the Fermi level in cubic PtBi2(Amsterdam : SciPost Foundation, 2021) Thirupathaiah, Setti; Kushnirenko, Yevhen; Koepernik, Klaus; Piening, Boy Roman; Büchner, Bernd; Aswartham, Saicharan; van den Brink, Jeroen; Borisenko, Sergey; Fulga, Ion CosmaWe show that the cubic compound PtBi2, is a topological semimetal hosting a sixfold band touching point in close proximity to the Fermi level. Using angle-resolved photoemission spectroscopy, we map the bandstructure of the system, which is in good agreement with results from density functional theory. Further, by employing a low energy effective Hamiltonian valid close to the crossing point, we study the effect of a magnetic field on the sixfold fermion. The latter splits into a total of twenty Weyl cones for a Zeeman field oriented in the diagonal, [111] direction. Our results mark cubic PtBi2, as an ideal candidate to study the transport properties of gapless topological systems beyond Dirac and Weyl semimetals.
- ItemSubstrate-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.
- ItemSynthesis and Physical Properties of Iridium-Based Sulfide Ca1−xIr4S6(S2) [x = 0.23–0.33](Basel : MDPI, 2022) Vogl, Michael; Valldor, Martin; Piening, Roman Boy; Efremov, Dmitri V.; Büchner, Bernd; Aswartham, SaicharanWe present the synthesis and characterization of the iridium-based sulfide Ca1−xIr4S6(S2). Quality and phase analysis were conducted by means of energy-dispersive X-ray spectroscopy (EDXS) and powder X-ray diffraction (XRD) techniques. Structure analysis reveals a monoclinic symmetry with the space group C 1 2/m 1 (No. 12), with the lattice constants a = 15.030 (3) Å, b = 3.5747 (5) Å and c = 10.4572 (18) Å. Both X-ray diffraction and EDXS suggest an off-stoichiometry of calcium, leading to the empirical composition Ca1−xIr4.0S6(S2) [x = 0.23–0.33]. Transport measurements show metallic behavior of the compound in the whole range of measured temperatures. Magnetic measurements down to 1.8 K show no long range order, and Curie–Weiss analysis yields θCW = −31.4 K, suggesting that the compound undergoes a magnetic state with short range magnetic correlations. We supplement our study with calculations of the band structure in the framework of the density functional theory.
- ItemRobust 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
- ItemSaturation 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, LouisObservations 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.
- ItemSimultaneous magnetic field and field gradient mapping of hexagonal MnNiGa by quantitative magnetic force microscopy(London : Springer Nature, 2023) Freitag, Norbert H.; Reiche, Christopher F.; Neu, Volker; Devi, Parul; Burkhardt, Ulrich; Felser, Claudia; Wolf, Daniel; Lubk, Axel; Büchner, Bernd; Mühl, ThomasMagnetic force microscopy (MFM) is a scanning microscopy technique that is commonly employed to probe the sample’s magnetostatic stray fields via their interaction with a magnetic probe tip. In this work, a quantitative, single-pass MFM technique is presented that maps one magnetic stray-field component and its spatial derivative at the same time. This technique uses a special cantilever design and a special high-aspect-ratio magnetic interaction tip that approximates a monopole-like moment. Experimental details, such as the control scheme, the sensor design, which enables simultaneous force and force gradient measurements, as well as the potential and limits of the monopole description of the tip moment are thoroughly discussed. To demonstrate the merit of this technique for studying complex magnetic samples it is applied to the examination of polycrystalline MnNiGa bulk samples. In these experiments, the focus lies on mapping and analyzing the stray-field distribution of individual bubble-like magnetization patterns in a centrosymmetric [001] MnNiGa phase. The experimental data is compared to calculated and simulated stray-field distributions of 3D magnetization textures, and, furthermore, bubble dimensions including diameters are evaluated. The results indicate that the magnetic bubbles have a significant spatial extent in depth and a buried bubble top base.
- ItemUnusual spin pseudogap behavior in the spin web lattice Cu3TeO6 probed by 125Te nuclear magnetic resonance(College Park, MD : APS, 2021) Baek, Seung-Ho; Yeo, Hyeon Woo; Park, Jena; Choi, Kwang-Yong; Büchner, BerndWe present a 125Te nuclear magnetic resonance (NMR) study in the three-dimensional spin web lattice Cu3TeO6 which harbors topological magnons. The 125Te NMR spectra and the Knight-shift K as a function of temperature show a drastic change at TS∼40K much lower than the Néel ordering temperature TN∼61K, providing evidence for the first-order structural phase transition within the magnetically ordered state. Most remarkably, the temperature dependence of the spin-lattice relaxation rate T−11 unravels spin-gap-like magnetic excitations, which sharply sets in at T∗∼75K, the temperature well above TN. The spin-gap behavior may be understood by weakly dispersive optical magnon branches of high-energy spin excitations originating from the unique corner-sharing Cu hexagon spin-1/2 network with low coordination number.