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- ItemSpectromicroscopic 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.
- ItemAll-on-Chip Concurrent Measurements of the Static Magnetization and of the Electron Spin Resonance with Microcantilevers(Wien [u.a.] : Springer, 2021) Alfonsov, A.; Büchner, B.; Kataev, V.A large variety of the samples of novel magnetic materials, which are of high interest due to their exotic properties, are only available in very small sizes. In some cases, it is not possible to synthesize large single crystals; in other cases, the small size itself is the key prerequisite to manifest a specifically interesting property of the material. The smallness of a sample rises a problem of the detection of the static magnetic response and of the electron spin resonance (ESR) signal. To overcome this problem, we propose to use a cantilever-based (torque-detected) setup with the capability of a simultaneous measurement of ESR and static magnetization. This setup offers a high sensitivity and the ability to acquire along with the ESR signal the components of the magnetization tensor in a single experimental run. Here, we present the working principle of this setup, as well as the estimate of its sensitivity from the measurements on the standard Co Tutton salt sample. © 2021, The Author(s).
- ItemImpact 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.
- ItemTwo-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.
- ItemStrong 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.
- ItemSeparate tuning of nematicity and spin fluctuations to unravel the origin of superconductivity in FeSe(London : Nature Publishing Group, 2020) Baek, S.-H.; Ok, J.M.; Kim, J.S.; Aswartham, S.; Morozov, I.; Chareev, D.; Urata, T.; Tanigaki, K.; Tanabe, Y.; Büchner, B.; Efremov, D.V.The interplay of orbital and spin degrees of freedom is the fundamental characteristic in numerous condensed matter phenomena, including high-temperature superconductivity, quantum spin liquids, and topological semimetals. In iron-based superconductors (FeSCs), this causes superconductivity to emerge in the vicinity of two other instabilities: nematic and magnetic. Unveiling the mutual relationship among nematic order, spin fluctuations, and superconductivity has been a major challenge for research in FeSCs, but it is still controversial. Here, by carrying out 77Se nuclear magnetic resonance (NMR) measurements on FeSe single crystals, doped by cobalt and sulfur that serve as control parameters, we demonstrate that the superconducting transition temperature Tc increases in proportion to the strength of spin fluctuations, while it is independent of the nematic transition temperature Tnem. Our observation therefore directly implies that superconductivity in FeSe is essentially driven by spin fluctuations in the intermediate coupling regime, while nematic fluctuations have a marginal impact on Tc.
- ItemIntertwined electronic and magnetic structure of the van-der-Waals antiferromagnet Fe2P2S6([London] : Nature Publishing Group, 2023) Koitzsch, A.; Klaproth, T.; Selter, S.; Shemerliuk, Y.; Aswartham, S.; Janson, O.; Büchner, B.; Knupfer, M.Many unusual and promising properties have been reported recently for the transition metal trichalcogenides of the type MPS3 (M = V, Mn, Fe, Ni..), such as maintaining magnetic order to the atomically thin limit, ultra-sharp many-body excitons, metal-insulator transitions and, especially for Fe2P2S6, giant linear dichroism among others. Here we conduct a detailed investigation of the electronic structure of Fe2P2S6 using angle-resolved photoemission spectroscopy, q-dependent electron energy loss spectroscopy, optical spectroscopies and density functional theory. Fe2P2S6 is a Mott insulator with a gap of E gap ≈ 1.4 eV and zigzag antiferromagnetism below T N = 119 K. The low energy excitations are dominated by Fe 3d states. Large and sign-changing linear dichroism is observed. We provide a microscopic mechanism explaining key properties of the linear dichroism based on the correlated character of the electronic structure, thereby elucidating the nature of the spin-charge coupling in Fe2P2S6 and related materials.
- ItemStrain derivative of thermoelectric properties as a sensitive probe for nematicity([London] : Nature Publishing Group, 2021) Caglieris, F.; Wuttke, C.; Hong, C.; Sykora, S.; Kappenberger, R.; Aswartham, S.; Wurmehl, S.; Büchner, B.; Hess, C.The nematic instability is an undebatable ingredient of the physics of iron-based superconductors. Yet, its origin remains enigmatic as it involves a fermiology with an intricate interplay of lattice-, orbital-, and spin degrees of freedom. It is well known that thermoelectric transport is an excellent probe for revealing even subtle signatures of instabilities and pertinent fluctuations. In this paper, we report a strong response of the thermoelectric transport properties of two underdoped 1111 iron-based superconductors to a vanishingly small strain. By introducing the strain derivative of the Seebeck and the Nernst coefficients, we provide a description of the nematic order parameter, proving the existence of an anisotropic Peltier-tensor beside an anisotropic conductivity tensor. Our measurements reveal that the transport nematic phenomenology is the result of the combined effect of both an anisotropic scattering time and Fermi surface distortions, pointing out that in a realistic description, abreast of the spin fluctuations also the orbital character is a fundamental ingredient. In addition, we show that nematic fluctuations universally relax in a Curie–Weiss fashion above TS in all the elasto-transport measurements and we provide evidences that nematicity must be band selective.
- ItemKramers doublets, phonons, crystal-field excitations, and their coupling in Nd2ZnIrO6(College Park, ML : American Physical Society, 2020) Singh, Birender; Vogl, M.; Wurmehl, S.; Aswartham, S.; Büchner, B.; Kumar, PradeepWe report comprehensive Raman-scattering measurements on a single crystal of double-perovskite Nd2ZnIrO6 in a temperature range of 4–330 K, spanning a broad spectral range from 20 to 5500cm−1. The paper focuses on lattice vibrations and electronic transitions involving Kramers doublets of the rare-earth Nd3+ ion with local C1 site symmetry. Temperature evolution of these quasiparticle excitations has allowed us to ascertain the intricate coupling between lattice and electronic degrees of freedom in Nd2ZnIrO6. Strong coupling between phonons and crystal-field excitation is observed via renormalization of the self-energy parameter of the phonons, i.e., peak frequency and linewidth. The phonon frequency shows abrupt hardening and linewidth narrowing below ∼100 K for the majority of the observed first-order phonons. We observed splitting of the lowest Kramers doublets of ground state (4I9/2) multiplets, i.e., lifting of the Kramers degeneracy, prominently at low temperature (below ∼100 K), attributed to the Nd-Nd/Ir exchange interactions and the intricate coupling with the lattice degrees of freedom. The observed splitting is of the order of ∼2–3 meV and is consistent with the estimated value. We also observed a large number of high-energy modes, 46 in total, attributed to the intraconfigurational transitions between 4f3 levels of Nd3+ coupled to the phonons reflected in their anomalous temperature evolution.
- ItemKitaev magnetism and fractionalized excitations in double perovskite Sm2ZnIrO6(College Park, ML : American Physical Society, 2020) Singh, Birender; Vogl, M.; Wurmehl, S.; Aswartham, S.; Büchner, B.; Kumar, PradeepThe quest for Kitaev spin liquids in particular three-dimensional solids is a long sought goal in condensed matter physics, as these states may give rise to exotic new types of quasiparticle excitations carrying fractional quantum numbers, namely Majorana fermionic excitations. Here we report the experimental signature of this characteristic feature of the Kitaev spin liquid via Raman measurements. Sm2ZnIrO6 is a strongly spin-orbit-coupled Mott insulator where Jeff=1/2 controls the physics, which provides striking evidence for this characteristic feature of the Kitaev spin liquid. As the temperature is lowered, we find that the spin excitations form a continuum in contrast to the conventional sharp modes expected in ordered antiferromagnets. Our observation of a broad magnetic continuum and anomalous renormalization of the phonon self-energy parameters shows the existence of fractionalization excitations in the double-perovskite structure, as theoretically conjectured in a Kitaev-Heisenberg geometrically frustrated double-perovskite system.