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- 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.
- ItemIntermixing-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, VladimirThe 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.
- ItemTSFZ Growth of Eu-Substituted Large-Size LSCO Crystals(Basel : MDPI, 2022) Voloshyna, Olesia; Romaka, Vitaliy V.; Karmakar, Koushik ;Seiro, Silvia; Maljuk, Andrey; Büchner, BerndThe 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.
- ItemFlux Growth and Characterization of Bulk InVO4 Crystals(Basel : MDPI, 2023) Voloshyna, Olesia; Gorbunov, Mikhail V.; Mikhailova, Daria; Maljuk, Andrey; Seiro, Silvia; Büchner, BerndThe 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.
- ItemFloating Zone Growth of Pure and Pb-Doped Bi-2201 Crystals(Basel : MDPI, 2024) Roslova, Maria; Büchner, Bernd; Maljuk, AndreyIn this review, we summarize recent progress in crystal growth and understanding of the influence of crystal structure on superconductivity in pure and Pb-doped Bi2Sr2CuOy (Bi-2201) materials belonging to the overdoped region of high-temperature cuprate superconductors. The crystal growth of Bi-2201 superconductors faces challenges due to intricate materials chemistry and the lack of knowledge of corresponding phase diagrams. Historically, a crucible-free floating zone method emerged as the most promising growth approach for these materials, resulting in high-quality single crystals. This review outlines the described methods in the literature and the authors’ synthesis endeavors encompassing Pb-doped Bi-2201 crystals, provides a detailed structural characterization of as-grown and post-growth annealed samples, and highlights optimal growth conditions that yield large-size, single-phase, and compositionally homogeneous Bi-2201 single crystals.
- ItemCovalency versus magnetic axiality in Nd molecular magnets: Nd-photoluminescence, strong ligand-field, and unprecedented nephelauxetic effect in fullerenes NdM2N@C80 (M = Sc, Lu, Y)(Cambridge : RSC, 2023) Yang, Wei; Rosenkranz, Marco; Velkos, Georgios; Ziegs, Frank; Dubrovin, Vasilii; Schiemenz, Sandra; Spree, Lukas; de Souza Barbosa, Matheus Felipe; Guillemard, Charles; Valvidares, Manuel; Büchner, Bernd; Liu, Fupin; Avdoshenko, Stanislav M.; Popov, Alexey A.Nd-based nitride clusterfullerenes NdM2N@C80 with rare-earth metals of different sizes (M = Sc, Y, Lu) were synthesized to elucidate the influence of the cluster composition, shape and internal strain on the structural and magnetic properties. Single crystal X-ray diffraction revealed a very short Nd-N bond length in NdSc2N@C80. For Lu and Y analogs, the further shortening of the Nd-N bond and pyramidalization of the NdM2N cluster are predicted by DFT calculations as a result of the increased cluster size and a strain caused by the limited size of the fullerene cage. The short distance between Nd and nitride ions leads to a very large ligand-field splitting of Nd3+ of 1100-1200 cm−1, while the variation of the NdM2N cluster composition and concomitant internal strain results in the noticeable modulation of the splitting, which could be directly assessed from the well-resolved fine structure in the Nd-based photoluminescence spectra of NdM2N@C80 clusterfullerenes. Photoluminescence measurements also revealed an unprecedentedly strong nephelauxetic effect, pointing to a high degree of covalency. The latter appears detrimental to the magnetic axiality despite the strong ligand field. As a result, the ground magnetic state has considerable transversal components of the pseudospin g-tensor, and the slow magnetic relaxation of NdSc2N@C80 could be observed by AC magnetometry only in the presence of a magnetic field. A combination of the well-resolved magneto-optical states and slow relaxation of magnetization suggests that Nd clusterfullerenes can be useful building blocks for magneto-photonic quantum technologies.
- ItemCurcumin and Graphene Oxide Incorporated into Alginate Hydrogels as Versatile Devices for the Local Treatment of Squamous Cell Carcinoma(Basel : MDPI, 2022) Madeo, Lorenzo Francesco; Sarogni, Patrizia; Cirillo, Giuseppe; Vittorio, Orazio; Voliani, Valerio; Curcio, Manuela; Shai-Hee, Tyler; Büchner, Bernd; Mertig, Michael; Hampel, SilkeWith the aim of preparing hybrid hydrogels suitable for use as patches for the local treatment of squamous cell carcinoma (SCC)-affected areas, curcumin (CUR) was loaded onto graphene oxide (GO) nanosheets, which were then blended into an alginate hydrogel that was crosslinked by means of calcium ions. The homogeneous incorporation of GO within the polymer network, which was confirmed through morphological investigations, improved the stability of the hybrid system compared to blank hydrogels. The weight loss in the 100–170 °C temperature range was reduced from 30% to 20%, and the degradation of alginate chains shifted to higher temperatures. Moreover, GO enhanced the stability in water media by counteracting the de-crosslinking process of the polymer network. Cell viability assays showed that the loading of CUR (2.5% and 5% by weight) was able to reduce the intrinsic toxicity of GO towards healthy cells, while higher amounts were ineffective due to the antioxidant/prooxidant paradox. Interestingly, the CUR-loaded systems were found to possess a strong cytotoxic effect in SCC cancer cells, and the sustained CUR release (~50% after 96 h) allowed long-term anticancer efficiency to be hypothesized.
- ItemSuppression of nematicity by tensile strain in multilayer FeSe/SrTiO3 films(College Park, MD : APS, 2023) Lou, Rui; Suvorov, Oleksandr; Grafe, Hans-Joachim; Kuibarov, Andrii; Krivenkov, Maxim; Rader, Oliver; Büchner, Bernd; Borisenko, Sergey; Fedorov, AlexanderThe nematicity in multilayer FeSe/SrTiO3 films has been previously suggested to be enhanced with decreasing film thickness. Motivated by this, there have been many discussions about the competing relation between nematicity and superconductivity. However, the criterion for determining the nematicity strength in FeSe remains highly debated. The understanding of nematicity as well as its relation to superconductivity in FeSe films is therefore still controversial. Here, we fabricate multilayer FeSe/SrTiO3 films using molecular beam epitaxy and study the nematic properties by combining angle-resolved photoemission spectroscopy, Se77 nuclear magnetic resonance, and scanning tunneling microscopy experiments. We unambiguously demonstrate that, near the interface, the nematic order is suppressed by the SrTiO3-induced tensile strain; in the bulk region further away from the interface, the strength of nematicity recovers to the bulk value. Our results not only solve the recent controversy about the nematicity in multilayer FeSe films, but also offer valuable insights into the relationship between nematicity and superconductivity.
- ItemTunable positions of Weyl nodes via magnetism and pressure in the ferromagnetic Weyl semimetal CeAlSi([London] : Nature Publishing Group UK, 2024) Cheng, Erjian; Yan, Limin; Shi, Xianbiao; Lou, Rui; Fedorov, Alexander; Behnami, Mahdi; Yuan, Jian; Yang, Pengtao; Wang, Bosen; Cheng, Jin-Guang; Xu, Yuanji; Xu, Yang; Xia, Wei; Pavlovskii, Nikolai; Peets, Darren C.; Zhao, Weiwei; Wan, Yimin; Burkhardt, Ulrich; Guo, Yanfeng; Li, Shiyan; Felser, Claudia; Yang, Wenge; Büchner, BerndThe noncentrosymmetric ferromagnetic Weyl semimetal CeAlSi with simultaneous space-inversion and time-reversal symmetry breaking provides a unique platform for exploring novel topological states. Here, by employing multiple experimental techniques, we demonstrate that ferromagnetism and pressure can serve as efficient parameters to tune the positions of Weyl nodes in CeAlSi. At ambient pressure, a magnetism-facilitated anomalous Hall/Nernst effect (AHE/ANE) is uncovered. Angle-resolved photoemission spectroscopy (ARPES) measurements demonstrated that the Weyl nodes with opposite chirality are moving away from each other upon entering the ferromagnetic phase. Under pressure, by tracing the pressure evolution of AHE and band structure, we demonstrate that pressure could also serve as a pivotal knob to tune the positions of Weyl nodes. Moreover, multiple pressure-induced phase transitions are also revealed. These findings indicate that CeAlSi provides a unique and tunable platform for exploring exotic topological physics and electron correlations, as well as catering to potential applications, such as spintronics.
- ItemChirality coupling in topological magnetic textures with multiple magnetochiral parameters([London] : Nature Publishing Group UK, 2023) Volkov, Oleksii M.; Wolf, Daniel; Pylypovskyi, Oleksandr V.; Kákay, Attila; Sheka, Denis D.; Büchner, Bernd; Fassbender, Jürgen; Lubk, Axel; Makarov, DenysChiral effects originate from the lack of inversion symmetry within the lattice unit cell or sample’s shape. Being mapped onto magnetic ordering, chirality enables topologically non-trivial textures with a given handedness. Here, we demonstrate the existence of a static 3D texture characterized by two magnetochiral parameters being magnetic helicity of the vortex and geometrical chirality of the core string itself in geometrically curved asymmetric permalloy cap with a size of 80 nm and a vortex ground state. We experimentally validate the nonlocal chiral symmetry breaking effect in this object, which leads to the geometric deformation of the vortex string into a helix with curvature 3 μm−1 and torsion 11 μm−1. The geometric chirality of the vortex string is determined by the magnetic helicity of the vortex texture, constituting coupling of two chiral parameters within the same texture. Beyond the vortex state, we anticipate that complex curvilinear objects hosting 3D magnetic textures like curved skyrmion tubes and hopfions can be characterized by multiple coupled magnetochiral parameters, that influence their statics and field- or current-driven dynamics for spin-orbitronics and magnonics.
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