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- 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.
- ItemLaser-Assisted Floating Zone Growth of BaFe2S3 Large-Sized Ferromagnetic-Impurity-Free Single Crystals(Basel : MDPI, 2021) Amigó, Maria Lourdes; Maljuk, Andrey; Manna, Kaustuv; Stahl, Quirin; Felser, Claudia; Hess, Christian; Wolter, Anja U.B.; Geck, Jochen; Seiro, Silvia; Büchner, BerndThe quasi-one-dimensional antiferromagnetic insulator BaFe2S3 becomes superconducting under a hydrostatic pressure of ∼10 GPa. Single crystals of this compound are usually obtained by melting and further slow cooling of BaS or Ba, Fe, and S, and are small and needle-shaped (few mm long and 50–200 μm wide). A notable sample dependence on the antiferromagnetic transition temperature, transport behavior, and presence of superconductivity has been reported. In this work, we introduce a novel approach for the growth of high-quality single crystals of BaFe2S3 based on a laser-assisted floating zone method that yields large samples free of ferromagnetic impurities. We present the characterization of these crystals and the comparison with samples obtained using the procedure reported in the literature.
- ItemMg3(Bi,Sb)2 single crystals towards high thermoelectric performance(Cambridge : RSC Publ., 2020) Pan, Yu; Yao, Mengyu; Hong, Xiaochen; Zhu, Yifan; Fan, Fengren; Imasato, Kazuki; He, Yangkun; Hess, Christian; Fink, Jörg; Yang, Jiong; Büchner, Bernd; Fu, Chenguang; Snyder, G. Jeffrey; Felser, ClaudiaThe rapid growth of the thermoelectric cooler market makes the development of novel room temperature thermoelectric materials of great importance. Ternary n-type Mg3(Bi,Sb)2 alloys are promising alternatives to the state-of-the-art Bi2(Te,Se)3 alloys but grain boundary resistance is the most important limitation. n-type Mg3(Bi,Sb)2 single crystals with negligible grain boundaries are expected to have particularly high zT but have rarely been realized due to the demanding Mg-rich growth conditions required. Here, we report, for the first time, the thermoelectric properties of n-type Mg3(Bi,Sb)2 alloyed single crystals grown by a one-step Mg-flux method using sealed tantalum tubes. High weighted mobility ∼140 cm2 V−1 s−1 and a high zT of 0.82 at 315 K are achieved in Y-doped Mg3Bi1.25Sb0.75 single crystals. Through both experimental angle-resolved photoemission spectroscopy and theoretical calculations, we denote the origin of the high thermoelectric performance from a point of view of band widening effect and electronegativity, as well as the necessity to form high Bi/Sb ratio ternary Mg3(Bi,Sb)2 alloys. The present work paves the way for further development of Mg3(Bi,Sb)2 for near room temperature thermoelectric applications.
- ItemThermoelectric Properties of Novel Semimetals: A Case Study of YbMnSb2(Weinheim : Wiley-VCH, 2020) Pan, Yu; Fan, Feng-Ren; Hong, Xiaochen; He, Bin; Le, Congcong; Schnelle, Walter; He, Yangkun; Imasato, Kazuki; Borrmann, Horst; Hess, Christian; Büchner, Bernd; Sun, Yan; Fu, Chenguang; Snyder, G. Jeffrey; Felser, ClaudiaThe emerging class of topological materials provides a platform to engineer exotic electronic structures for a variety of applications. As complex band structures and Fermi surfaces can directly benefit thermoelectric performance it is important to identify the role of featured topological bands in thermoelectrics particularly when there are coexisting classic regular bands. In this work, the contribution of Dirac bands to thermoelectric performance and their ability to concurrently achieve large thermopower and low resistivity in novel semimetals is investigated. By examining the YbMnSb2 nodal line semimetal as an example, the Dirac bands appear to provide a low resistivity along the direction in which they are highly dispersive. Moreover, because of the regular-band-provided density of states, a large Seebeck coefficient over 160 µV K−1 at 300 K is achieved in both directions, which is very high for a semimetal with high carrier concentration. The combined highly dispersive Dirac and regular bands lead to ten times increase in power factor, reaching a value of 2.1 mW m−1 K−2 at 300 K. The present work highlights the potential of such novel semimetals for unusual electronic transport properties and guides strategies towards high thermoelectric performance. © 2020 The Authors. Advanced Materials published by Wiley-VCH GmbH
- ItemElastoresistivity of Heavily Hole-Doped 122 Iron Pnictide Superconductors(Lausanne : Frontiers Media, 2022) Hong, Xiaochen; Sykora, Steffen; Caglieris, Federico; Behnami, Mahdi; Morozov, Igor; Aswartham, Saicharan; Grinenko, Vadim; Kihou, Kunihiro; Lee, Chul-Ho; Büchner, Bernd; Hess, ChristianNematicity in heavily hole-doped iron pnictide superconductors remains controversial. Sizeable nematic fluctuations and even nematic orders far from magnetic instability were declared in RbFe2As2 and its sister compounds. Here, we report a systematic elastoresistance study of a series of isovalent- and electron-doped KFe2As2 crystals. We found divergent elastoresistance on cooling for all the crystals along their [110] direction. The amplitude of elastoresistivity diverges if K is substituted with larger ions or if the system is driven toward a Lifshitz transition. However, we conclude that none of them necessarily indicates an independent nematic critical point. Instead, the increased nematicity can be associated with another electronic criticality. In particular, we propose a mechanism for how elastoresistivity is enhanced at a Lifshitz transition.
- 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.
- ItemDisorder-induced coupling of Weyl nodes in WTe2(2020) Sykora, Steffen; Schoop, Johannes; Graf, Lukas; Shipunov, Grigory; Morozov, Igor V.; Aswartham, Saicharan; Büchner, Bernd; Hess, Christian; Giraud, Romain; Dufouleur, JosephThe finite coupling between Weyl nodes due to residual disorder is investigated by magnetotransport studies in WTe2. The anisotropic scattering of quasiparticles is evidenced from classical and quantum transport measurements. A theoretical approach using the real band structure is developed in order to calculate the dependence of the scattering anisotropy with the correlation length of the disorder. A comparison between theory and experiments reveals a short correlation length in WTe2 (ξ∼5 nm). This result implies a significant coupling between Weyl nodes and other bands. Our study thus shows that a finite intercone scattering rate always exists in weakly disordered type-II Weyl semimetals, such as WTe2, which strongly suppresses topologically nontrivial properties.
- ItemEvidence for a percolative Mott insulator-metal transition in doped Sr2IrO4(College Park, MD : APS, 2021) Sun, Zhixiang; Guevara, Jose M.; Sykora, Steffen; Pärschke, Ekaterina M.; Manna, Kaustuv; Maljuk, Andrey; Wurmehl, Sabine; van den Brink, Jeroen; Büchner, Bernd; Hess, ChristianDespite many efforts to rationalize the strongly correlated electronic ground states in doped Mott insulators, the nature of the doping-induced insulator-to-metal transition is still a subject under intensive investigation. Here, we probe the nanoscale electronic structure of the Mott insulator Sr2IrO4−δ with low-temperature scanning tunneling microscopy and find an enhanced local density of states (LDOS) inside the Mott gap at the location of individual defects which we interpret as defects at apical oxygen sites. A chiral behavior in the topography for those defects has been observed. We also visualize the local enhanced conductance arising from the overlapping of defect states which induces finite LDOS inside of the Mott gap. By combining these findings with the typical spatial extension of isolated defects of about 2 nm, our results indicate that the insulator-to-metal transition in Sr2IrO4−δ could be percolative in nature.
- 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.