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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.
- ItemShape-adaptive single-molecule magnetism and hysteresis up to 14 K in oxide clusterfullerenes Dy2O@C72 and Dy2O@C74 with fused pentagon pairs and flexible Dy-(μ2-O)-Dy angle(Cambridge : Royal Society of Chemistry, 2020) Velkos, G.; Yang, W.; Yao, Y.-R.; Sudarkova, S.M.; Liu, X.; Büchner, B.; Avdoshenko, S.M.; Chen, N.; Popov, A.A.Dysprosium oxide clusterfullerenes Dy2O@Cs(10528)-C72 and Dy2O@C2(13333)-C74 are synthesized and characterized by single-crystal X-ray diffraction. Carbon cages of both molecules feature two adjacent pentagon pairs. These pentalene units determine positions of endohedral Dy ions hence the shape of the Dy2O cluster, which is bent in Dy2O@C72 but linear in Dy2O@C74. Both compounds show slow relaxation of magnetization and magnetic hysteresis. Nearly complete cancelation of ferromagnetic dipolar and antiferromagnetic exchange Dy⋯Dy interactions leads to unusual magnetic properties. Dy2O@C74 exhibits zero-field quantum tunneling of magnetization and magnetic hysteresis up to 14 K, the highest temperature among Dy-clusterfullerenes.
- 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).
- 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.
- 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.
- ItemSystematic investigations of annealing and functionalization of carbon nanotube yarns(Basel : MDPI AG, 2020) Scholz, M.; Hayashi, Y.; Eckert, V.; Khavrus, V.; Leonhardt, A.; Büchner, B.; Mertig, M.; Hampel, S.Carbon nanotube yarns (CNY) are a novel carbonaceous material and have received a great deal of interest since the beginning of the 21st century. CNY are of particular interest due to their useful heat conducting, electrical conducting, and mechanical properties. The electrical conductivity of carbon nanotube yarns can also be influenced by functionalization and annealing. A systematical study of this post synthetic treatment will assist in understanding what factors influences the conductivity of these materials. In this investigation, it is shown that the electrical conductivity can be increased by a factor of 2 and 5.5 through functionalization with acids and high temperature annealing respectively. The scale of the enhancement is dependent on the reducing of intertube space in case of functionalization. For annealing, not only is the highly graphitic structure of the carbon nanotubes (CNT) important, but it is also shown to influence the residual amorphous carbon in the structure. The promising results of this study can help to utilize CNY as a replacement for common materials in the field of electrical wiring.
- 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.
- ItemCharge-transfer energy in iridates: A hard x-ray photoelectron spectroscopy study(College Park, ML : American Physical Society, 2020) Takegami, D.; Kasinathan, D.; Wolff, K.K.; Altendorf, S.G.; Chang, C.F.; Hoefer, K.; Melendez-Sans, A.; Utsumi, Y.; Meneghin, F.; Ha, T.D.; Yen, C.H.; Chen, K.; Kuo, C.Y.; Liao, Y.F.; Tsuei, K.D.; Morrow, R.; Wurmehl, S.; Büchner, B.; Prasad, B.E.; Jansen, M.; Komarek, A.C.; Hansmann, P.; Tjeng, L.H.We have investigated the electronic structure of iridates in the double perovskite crystal structure containing either Ir4+ or Ir5+ using hard x-ray photoelectron spectroscopy. The experimental valence band spectra can be well reproduced using tight-binding calculations including only the Ir 5d, O 2p, and O 2s orbitals with parameters based on the downfolding of the density-functional band structure results. We found that, regardless of the A and B cations, the A2BIrO6 iridates have essentially zero O 2p to Ir 5d charge-transfer energies. Hence double perovskite iridates turn out to be extremely covalent systems with the consequence being that the magnetic exchange interactions become very long ranged, thereby hampering the materialization of the long-sought Kitaev physics. Nevertheless, it still would be possible to realize a spin-liquid system using the iridates with a proper tuning of the various competing exchange interactions.
- ItemCoupling of lattice, spin, and intraconfigurational excitations of Eu3+ in Eu2ZnIrO6(Washington, DC : American Association for the Advancement of Science, 2020) Singh, Birender; Vogl, M.; Wurmehl, S.; Aswartham, S.; Büchner, B.; Kumar, PradeepIn Eu2ZnIrO6, effectively two atoms are active; i.e., Ir is magnetically active, which results in complex magnetic ordering within the Ir sublattice at low temperature. On the other hand, although Eu is a Van Vleck paramagnet, it is active in the electronic channels involving 4f6 crystal-field split levels. Phonons, quanta of lattice vibration involving vibration of atoms in the unit cell, are intimately coupled with both magnetic and electronic degrees of freedom (DOF). Here, we report a comprehensive study focusing on the phonons as well as intraconfigurational excitations in double-perovskite Eu2ZnIrO6. Our studies reveal strong coupling of phonons with the underlying magnetic DOF reflected in the renormalization of the phonon self-energy parameters well above the spin-solid phase (TN∼12K) until temperature as high as ∼3TN evidences broken spin rotational symmetry deep into the paramagnetic phase. In particular, all the observed first-order phonon modes show softening of varying degree below ∼3TN, and low-frequency phonons become sharper, while the high-frequency phonons show broadening attributed to the additional available magnetic damping channels. We also observed a large number of high-energy modes, 39 in total, attributed to the electronic transitions between 4f levels of the rare-earth Eu3+ ion and these modes shows anomalous temperature evolution as well as mixing of the crystal-field split levels attributed to the strong coupling of electronic and lattice DOF.