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, Louis

Observations 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.

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.

2022, Naselli, Gabriele, Moghaddam, Ali G., Di Napoli, Solange, Vildosola, Verónica, Fulga, Ion Cosma, van den Brink, Jeroen, Facio, Jorge I.

We analyze the electronic structure of topological surface states in the family of magnetic topological insulators MnBi2nTe3n+1. We show that, at natural-cleavage surfaces, the Dirac cone warping changes its symmetry from hexagonal to trigonal at the magnetic ordering temperature. In particular, an energy splitting develops between the surface states of the same band index but opposite surface momenta upon formation of the long-range magnetic order. As a consequence, measurements of such energy splittings constitute a simple protocol to detect the magnetic ordering via the surface electronic structure, alternative to the detection of the surface magnetic gap. Interestingly, while the latter signals a nonzero surface magnetization, the trigonal warping predicted here is, in addition, sensitive to the direction of the surface magnetic flux. Our results may be particularly useful when the Dirac point is buried in the projection of the bulk states, caused by certain terminations of the crystal or in hole-doped systems, since in both situations the surface magnetic gap itself is not accessible in photoemission experiments.

2022, Galstian, I.Y., Tsapko, Y.A., Makarenko, O.V., Yampolskiy, A.L., Tarusin, Y.V., Len, E.G.

Using the methods of angular correlation of annihilation radiation (ACAR), attenuation of electromagnetic radiation in 1.5–2.2 GHz frequency range, and optical ellipsometry, it was shown that in composites of polytetrafluoroethylene (PTFE) + multi-walled carbon nanotubes (MWCNTs), a 2% decrease in the probability of annihilation of positrons in free volumes in PTFE leads to changes in other parameters of electronic structure of composites by 8–29%. Polytetrafluoroethylene is transparent to electromagnetic radiation, but after the addition of 10 wt.% or more of MWCNTs, the composites demonstrate 200–410-fold decrease in the electromagnetic radiation intensity when the radiation passes through a specimen with a thickness of ≈2 mm. It was found that the average radius of the free volumes and the probability of annihilation of positrons are determined by the defect and electronic structures of the polymer matrix only. The Fermi angle and the probability of positrons annihilation with free electrons are determined by the analogous structures of MWCNTs only. Since the electronic characteristics of the atoms and defects in the polymer matrix (at least outside the interphase) do not change, the changes in the other ACAR parameters are mainly due to changes in the imperfect MWCNTs’ atomic and electronic structures. The average radius of free volumes reaches its maximum value in the composite with 10 wt.% MWCNTs. It was found that in a specimen with 10 wt.% MWCNTs, the highest density of free electrons is observed due to charge transfer from free volumes to MWCNTs, and the highest electron density is observed on defects. A disorder of MWCNTs and their branched conductive network can form the ‘tails’ of electronic density of states in a band gap. Thus, composite with 10 wt.% MWCNTs has the highest absorption coefficient for electromagnetic radiation.

2021, Jin, Fei, Xin, Jinpeng, Guan, Runnan, Xie, Xiao-Ming, Chen, Muqing, Zhang, Qianyan, Popov, Alexey A., Xie, Su-Yuan, Yang, Shangfeng

Trimetallic carbide clusterfullerenes (TCCFs) encapsulating a quinary M3C2 cluster represent a special family of endohedral fullerenes with an open-shell electronic configuration. Herein, a novel TCCF based on a medium-sized rare earth metal, dysprosium (Dy), is synthesized for the first time. The molecular structure of Dy3C2@Ih(7)-C80 determined by single crystal X-ray diffraction shows that the encapsulated Dy3C2 cluster adopts a bat ray configuration, in which the acetylide unit C2 is elevated above the Dy3 plane by ∼1.66 Å, while Dy–Dy distances are ∼3.4 Å. DFT computational analysis of the electronic structure reveals that the endohedral cluster has an unusual formal charge distribution of (Dy3)8+(C2)2−@C806− and features an unprecedented three-center single-electron Dy–Dy–Dy bond, which has never been reported for lanthanide compounds. Moreover, this electronic structure is different from that of the analogous Sc3C2@Ih(7)-C80 with a (Sc3)9+(C2)3−@C806− charge distribution and no metal–metal bonding.

2018, Liu, Z., Lou, R., Guo, P., Wang, Q., Sun, S., Li, C., Thirupathaiah, S., Fedorov, A., Shen, D., Liu, K., Lei, H., Wang, S.

The topological nodal-line semimetal state, serving as a fertile ground for various topological quantum phases, where a topological insulator, Dirac semimetal, or Weyl semimetal can be realized when the certain protecting symmetry is broken, has only been experimentally studied in very few materials. In contrast to discrete nodes, nodal lines with rich topological configurations can lead to more unusual transport phenomena. Utilizing angle-resolved photoemission spectroscopy and first-principles calculations, here, we provide compelling evidence of nodal-line fermions in centrosymmetric semimetal TiB2 with a negligible spin-orbit coupling effect. With the band crossings just below the Fermi energy, two groups of Dirac nodal rings are clearly observed without any interference from other bands, one surrounding the Brillouin zone (BZ) corner in the horizontal mirror plane σh and the other surrounding the BZ center in the vertical mirror plane σv. The linear dispersions forming Dirac nodal rings are as wide as 2 eV. We further observe that the two groups of nodal rings link together along the Γ-K direction, composing a nodal-link configuration. The simple electronic structure with Dirac nodal links mainly constituting the Fermi surfaces suggests TiB2 as a remarkable platform for studying and applying the novel physical properties related to nodal-line fermions.

2016, Koitzsch, A., Heming, N., Knupfer, M., Büchner, B., Portnichenko, P.Y., Dukhnenko, A.V., Shitsevalova, N.Y., Filipov, V.B., Lev, L.L.

Some heavy fermion materials show so-called hidden-order phases which are invisible to many characterization techniques and whose microscopic origin remained controversial for decades. Among such hidden-order compounds, CeB6 is of model character due to its simple electronic configuration and crystal structure. Apart from more conventional antiferromagnetism, it shows an elusive phase at low temperatures, which is commonly associated with multipolar order. Here we show that this phase roots in a Fermi surface instability. This conclusion is based on a full 3D tomographic sampling of the electronic structure by angle-resolved photoemission and comparison with inelastic neutron scattering data. The hidden order is mediated by itinerant electrons. Our measurements will serve as a paradigm for the investigation of hidden-order phases in f-electron systems, but also generally for situations where the itinerant electrons drive orbital or spin order.

2020, Katukuri, Vamshi M., Bogdanov, Nikolay A., Weser, Oskar, Van den Brink, Jeroen, Alavi, Ali

The large antiferromagnetic exchange coupling in the parent high-Tc cuprate superconductors is believed to play a crucial role in pairing the superconducting carriers. The recent observation of superconductivity in hole-doped infinite-layer (IL-) NdNiO2 brings to the fore the relevance of magnetic coupling in high-Tc superconductors, particularly because no magnetic ordering is observed in the undoped IL-NdNiO2, unlike in parent copper oxides. Here, we investigate the electronic structure and the nature of magnetic exchange in IL-NdNiO2 using state-of-the-art many-body quantum chemistry methods. From a systematic comparison of the electronic and magnetic properties with isostructural cuprate IL-CaCuO2, we find that the on-site dynamical correlations are significantly stronger in IL-NdNiO2 compared to the cuprate analog. These dynamical correlations play a critical role in the magnetic exchange resulting in an unexpectedly large antiferromagnetic nearest-neighbor isotropic J of 77 meV between the Ni1+ ions within the ab plane. While we find many similarities in the electronic structure between the nickelate and the cuprate, the role of electronic correlations is profoundly different in the two. We further discuss the implications of our findings in understanding the origin of superconductivity in nickelates. © 2020 authors.

2020, Kern, Felix, Linck, Martin, Wolf, Daniel, Alem, Nasim, Arora, Himani, Gemming, Sibylle, Erbe, Artur, Zettl, Alex, Büchner, Bernd, Lubk, Axel

The reduced dimensionality in two-dimensional materials leads to a wealth of unusual properties, which are currently explored for both fundamental and applied sciences. In order to study the crystal structure, edge states, the formation of defects and grain boundaries, or the impact of adsorbates, high-resolution microscopy techniques are indispensable. Here we report on the development of an electron holography (EH) transmission electron microscopy (TEM) technique, which facilitates high spatial resolution by an automatic correction of geometric aberrations. Distinguished features of EH beyond conventional TEM imaging are gap-free spatial information signal transfer and higher dose efficiency for certain spatial frequency bands as well as direct access to the projected electrostatic potential of the two-dimensional material. We demonstrate these features with the example of h-BN, for which we measure the electrostatic potential as a function of layer number down to the monolayer limit and obtain evidence for a systematic increase of the potential at the zig-zag edges.

2014, Zhu, L.-F., Friák, M., Udyansky, A., Ma, D., Schlieter, A., Kühn, U., Eckert, J., Neugebauer, J.

We employ density functional theory (DFT) to calculate pressure dependences of selected thermodynamic, structural and elastic properties as well as electronic structure characteristics of equiatomic B2 FeTi. We predict ground-state single-crystalline Young's modulus and its two-dimensional counterpart, the area modulus, together with homogenized polycrystalline elastic parameters. Regarding the electronic structure of FeTi, we analyze the band structure and electronic density of states. Employing (i) an analytical dynamical matrix parametrized in terms of elastic constants and lattice parameters in combination with (ii) the quasiharmonic approximation we then obtained free energies, the thermal expansion coefficient, heat capacities at constant pressure and volume, as well as isothermal bulk moduli at finite temperatures. Experimental measurements of thermal expansion coefficient complement our theoretical investigation and confirm our theoretical predictions. It is worth mentioning that, as often detected in other intermetallics, some materials properties of FeTi strongly differ from the average of the corresponding values found in elemental Fe and Ti. These findings can have important implications for future materials design of new intermetallic materials.