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We show that in manganese-doped topological insulator bismuth telluride layers, Mn atoms are incorporated predominantly as interstitials in the van der Waals gaps between the quintuple layers and not substitutionally on Bi sites within the quintuple layers. The structural properties of epitaxial layers with Mn concentration of up to 13% are studied by high-resolution x-ray diffraction, evidencing a shrinking of both the in-plane and out-of plane lattice parameters with increasing Mn content. Ferromagnetism sets in for Mn contents around 3% and the Curie temperatures rises up to 15 K for a Mn concentration of 9%. The easy magnetization axis is along the c-axis perpendicular to the (0001) epilayer plane. Angle-resolved photoemission spectroscopy reveals that the Fermi level is situated in the conduction band and no evidence for a gap opening at the topological surface state with the Dirac cone dispersion is found within the experimental resolution at temperatures close to the Curie temperature. From the detailed analysis of the extended x-ray absorption fine-structure experiments (EXAFS) performed at the MnK-edge, we demonstrate that the Mn atoms occupy interstitial positions within the van der Waals gap and are surrounded octahedrally by Te atoms of the adjacent quintuple layers.

Magnetic topological insulators are narrow-gap semiconductor materials that combine non-trivial band topology and magnetic order 1 . Unlike their nonmagnetic counterparts, magnetic topological insulators may have some of the surfaces gapped, which enables a number of exotic phenomena that have potential applications in spintronics 1 , such as the quantum anomalous Hall effect 2 and chiral Majorana fermions 3 . So far, magnetic topological insulators have only been created by means of doping nonmagnetic topological insulators with 3 d transition-metal elements; however, such an approach leads to strongly inhomogeneous magnetic 4 and electronic 5 properties of these materials, restricting the observation of important effects to very low temperatures 2 , 3 . An intrinsic magnetic topological insulator—a stoichiometric well ordered magnetic compound—could be an ideal solution to these problems, but no such material has been observed so far. Here we predict by ab initio calculations and further confirm using various experimental techniques the realization of an antiferromagnetic topological insulator in the layered van der Waals compound MnBi 2 Te 4 . The antiferromagnetic ordering  that MnBi 2 Te 4  shows makes it invariant with respect to the combination of the time-reversal and primitive-lattice translation symmetries, giving rise to a ℤ 2 topological classification; ℤ 2  = 1 for MnBi 2 Te 4 , confirming its topologically nontrivial nature. Our experiments indicate that the symmetry-breaking (0001) surface of MnBi 2 Te 4 exhibits a large bandgap in the topological surface state. We expect this property to eventually enable the observation of a number of fundamental phenomena, among them quantized magnetoelectric coupling 6 – 8 and axion electrodynamics 9 , 10 . Other exotic phenomena could become accessible at much higher temperatures than those reached so far, such as the quantum anomalous Hall effect 2 and chiral Majorana fermions 3 . An intrinsic antiferromagnetic topological insulator, MnBi 2 Te 4 , is theoretically predicted and then realized experimentally, with implications for the study of exotic quantum phenomena.

Modification of the gap at the Dirac point (DP) in axion antiferromagnetic topological insulator MnBi 2 Te 4 and its electronic and spin structure have been studied by angle- and spin-resolved photoemission spectroscopy (ARPES) under laser excitation at various temperatures (9–35 K), light polarizations and photon energies. We have distinguished both large (60–70 meV) and reduced ( < 20 meV ) gaps at the DP in the ARPES dispersions, which remain open above the Neél temperature ( T N = 24.5 K ). We propose that the gap above T N remains open due to a short-range magnetic field generated by chiral spin fluctuations. Spin-resolved ARPES, XMCD and circular dichroism ARPES measurements show a surface ferromagnetic ordering for the “large gap” sample and apparently significantly reduced effective magnetic moment for the “reduced gap” sample. These observations can be explained by a shift of the Dirac cone (DC) state localization towards the second Mn layer due to structural disturbance and surface relaxation effects, where DC state is influenced by compensated opposite magnetic moments. As we have shown by means of ab-initio calculations surface structural modification can result in a significant modulation of the DP gap.

A new kind of magnetically-doped antiferromagnetic (AFM) topological insulators (TIs) with stoichiometry Bi 1.09 Gd 0.06 Sb 0.85 Te 3 has been studied by angle-resolved photoemission spectroscopy (ARPES), superconducting magnetometry (SQUID) and X-ray magnetic circular dichroism (XMCD) with analysis of its electronic structure and surface-derived magnetic properties at different temperatures. This TI is characterized by the location of the Dirac gap at the Fermi level (E F ) and a bulk AFM coupling below the Neel temperature (4–8 K). At temperatures higher than the bulk AFM/PM transition, a surface magnetic layer is proposed to develop, where the coupling between the magnetic moments located at magnetic impurities (Gd) is mediated by the Topological Surface State (TSS) via surface Dirac-fermion-mediated magnetic coupling. This hypothesis is supported by a gap opening at the Dirac point (DP) indicated by the surface-sensitive ARPES, a weak hysteresis loop measured by SQUID at temperatures between 30 and 100 K, XMCD measurements demonstrating a surface magnetic moment at 70 K and a temperature dependence of the electrical resistance exhibiting a mid-gap semiconducting behavior up to temperatures of 100–130 K, which correlates with the temperature dependence of the surface magnetization and confirms the conclusion that only TSS are located at the E F . The increase of the TSS’s spectral weight during resonant ARPES at a photon energy corresponding to the Gd 4 d -4 f edge support the hypothesis of a magnetic coupling between the Gd ions via the TSS and corresponding magnetic moment transfer at elevated temperatures. Finally, the observed out-of-plane and in-plane magnetization induced by synchrotron radiation (SR) due to non-equal depopulation of the TSS with opposite momentum, as seen through change in the Dirac gap value and the k ∥ -shift of the Dirac cone (DC) states, can be an indicator of the modification of the surface magnetic coupling mediated by the TSS.

The energy gap was revealed in the Dirac cone of the BiSbTeSe2 topological insulator after the submonolayer deposition of a ferromagnetic metal. As a ferromagnet, cobalt and manganese were used. Such way of the energy gap opening is novel in comparison to the bulk ferromagnetic doping of topological insulators.

We studied the electronic structure of EuNi2P2, which exhibits both heavy-fermion and mixed-valence behaviors, using angle-resolved photoemission spectroscopy. Multiple Ni 3d bands were observed near the Fermi energy, and one of them forms a hole-like Fermi surface around the X point of the Brillouin zone. We also found that the spectral weight of the Ni 3d states is rapidly enhanced with decreasing temperature, which is consistent with the temperature dependence of the mean valence of Eu ions. Our results thus demonstrate hybridization between the Ni 3d and Eu 4f electrons in EuNi2P2.

Modification of the gap at the Dirac point (DP) in axion antiferromagnetic topological insulator and its electronic and spin structure have been studied by angle- and spin-resolved photoemission spectroscopy (ARPES) under laser excitation at various temperatures (9-35 K), light polarizations and photon energies. We have distinguished both large (60-70 meV) and reduced ( ) gaps at the DP in the ARPES dispersions, which remain open above the Neél temperature ( ). We propose that the gap above remains open due to a short-range magnetic field generated by chiral spin fluctuations. Spin-resolved ARPES, XMCD and circular dichroism ARPES measurements show a surface ferromagnetic ordering for the \"large gap\" sample and apparently significantly reduced effective magnetic moment for the \"reduced gap\" sample. These observations can be explained by a shift of the Dirac cone (DC) state localization towards the second Mn layer due to structural disturbance and surface relaxation effects, where DC state is influenced by compensated opposite magnetic moments. As we have shown by means of ab-initio calculations surface structural modification can result in a significant modulation of the DP gap.

Modification of the gap at the Dirac point (DP) in axion antiferromagnetic topological insulator$${\\hbox {MnBi}}_2 {\\hbox {Te}}_4$$MnBi 2 Te 4 and its electronic and spin structure have been studied by angle- and spin-resolved photoemission spectroscopy (ARPES) under laser excitation at various temperatures (9–35 K), light polarizations and photon energies. We have distinguished both large (60–70 meV) and reduced ($$<20~ \\hbox {meV}$$< 20 meV ) gaps at the DP in the ARPES dispersions, which remain open above the Neél temperature ($$T_{\\mathrm{N}} = 24.5~ \\hbox {K}$$T N = 24.5 K ). We propose that the gap above$$T_{\\mathrm{N}}$$T N remains open due to a short-range magnetic field generated by chiral spin fluctuations. Spin-resolved ARPES, XMCD and circular dichroism ARPES measurements show a surface ferromagnetic ordering for the “large gap” sample and apparently significantly reduced effective magnetic moment for the “reduced gap” sample. These observations can be explained by a shift of the Dirac cone (DC) state localization towards the second Mn layer due to structural disturbance and surface relaxation effects, where DC state is influenced by compensated opposite magnetic moments. As we have shown by means of ab-initio calculations surface structural modification can result in a significant modulation of the DP gap.

Atomic scale engineering of two-dimensional materials could create devices with rich physical and chemical properties. External periodic potentials can enable the manipulation of the electronic band structures of materials. A prototypical system is 3x3-silicene/Ag(111), which has substrate-induced periodic modulations. Recent angle-resolved photoemission spectroscopy measurements revealed six Dirac cone pairs at the Brillouin zone boundary of Ag(111), but their origin remains unclear [Proc. Natl. Acad. Sci. USA 113, 14656 (2016)]. We used linear dichroism angle-resolved photoemission spectroscopy, the tight-binding model, and first-principles calculations to reveal that these Dirac cones mainly derive from the original cones at the K (K') points of free-standing silicene. The Dirac cones of free-standing silicene are split by external periodic potentials that originate from the substrate-overlayer interaction. Our results not only confirm the origin of the Dirac cones in the 3x3-silicene/Ag(111) system, but also provide a powerful route to manipulate the electronic structures of two-dimensional materials.