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Register a new userOrbital Complexity in Intrinsic Magnetic Topological Insulators MnBi$_4$Te$_7$ and MnBi$_6$Te$_{10}$
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Using angle-resolved photoelectron spectroscopy (ARPES), we investigate the surface electronic structure of the magnetic van der Waals compounds MnBi$_4$Te$_7$ and MnBi$_6$Te$_{10}$, the $n=$~1 and 2 members of a modular (Bi$_2$Te$_3$)$_n$(MnBi$_2$Te$_4$) series, which have attracted recent interest as intrinsic magnetic topological insulators. Combining circular dichroic, spin-resolved and photon-energy-dependent ARPES measurements with calculations based on density functional theory, we unveil complex momentum-dependent orbital and spin textures in the surface electronic structure and disentangle topological from trivial surface bands. We find that the Dirac-cone dispersion of the topologial surface state is strongly perturbed by hybridization with valence-band states for Bi$_2$Te$_3$-terminated surfaces but remains preserved for MnBi$_2$Te$_4$-terminated surfaces. Our results firmly establish the topologically non-trivial nature of these magnetic van der Waals materials and indicate that the possibility of realizing a quantized anomalous Hall conductivity depends on surface termination.
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The search for materials to support the Quantum Anomalous Hall Effect (QAHE) have recently centered on intrinsic magnetic topological insulators (MTIs) including MnBi$_2$Te$_4$ or heterostructures made up of MnBi$_2$Te$_4$ and Bi$_2$Te$_3$. While MnBi$_2$Te$_4$ is itself a MTI, most recent ARPES experiments indicate that the surface states on this material lack the mass gap that is expected from the magnetism-induced time-reversal symmetry breaking (TRSB), with the absence of this mass gap likely due to surface magnetic disorder. Here, utilizing small-spot ARPES scanned across the surfaces of MnBi$_4$Te$_7$ and MnBi$_6$Te$_{10}$, we show the presence of large mass gaps (~ 100 meV scale) on both of these materials when the MnBi$_2$Te$_4$ surfaces are buried below one layer of Bi$_2$Te$_3$ that apparently protects the magnetic order, but not when the MnBi$_2$Te$_4$ surfaces are exposed at the surface or are buried below two Bi$_2$Te$_3$ layers. This makes both MnBi$_4$Te$_7$ and MnBi$_6$Te$_{10}$ excellent candidates for supporting the QAHE, especially if bulk devices can be fabricated with a single continuous Bi$_2$Te$_3$ layer at the surface.
A striking feature of time reversal symmetry (TRS) protected topological insulators (TIs) is that they are characterized by a half integer quantum Hall effect on the boundary when the surface states are gapped by time reversal breaking perturbations. While time reversal symmetry (TRS) protected TIs have become increasingly under control, magnetic analogs are still largely unexplored territories with novel rich structures. In particular, topological magnetic insulators can also host a quantized axion term in the presence of lattice symmetries. Since these symmetries are naturally broken on the boundary, the surface states can develop a gap without external manipulation. In this work, we combine theoretical analysis, density functional calculations and experimental evidence to reveal intrinsic axion insulating behavior in MnBi6Te10. The quantized axion term arises from the simplest possible mechanism in the antiferromagnetic regime where it is protected by inversion symmetry and a fractional translation symmetry. The anticipated gapping of the Dirac surface state at the edge is subsequently experimentally established using Angle Resolved Spectroscopy. As a result, this system provides the magnetic analogue of the simplest TRS protected TI with a single, gapped Dirac cone at the surface.
Engineering magnetic orders in topological insulators is critical to the realization of topological quantum phenomena such as the axion insulator state and the quantum anomalous Hall insulator state. Here we establish MnBi$_6$Te$_{10}$ as a tunable topological material platform where ferromagnetism and antiferromagnetism can be selectively obtained. We conduct a comprehensive measurement of ferromagnetic MnBi$_6$Te$_{10}$ bulk crystals via laser-based angle-resolved photoemission spectroscopy, and compare the results with those from their antiferromagnetic counterparts. For ferromagnetic MnBi$_6$Te$_{10}$, we observe a magnetically driven broken-symmetry gap of 15 meV at the topological surface state on the MnBi$_2$Te$_4$ termination, which disappears when the temperature is raised above the Curie temperature. In contrast, antiferromagnetic MnBi$_6$Te$_{10}$ exhibits gapless topological surface states on all terminations. We consider disorder in the form of Mn migration from MnBi$_2$Te$_4$ layers to the neighboring Bi$_2$Te$_3$ layers as a possible driving force for the delicate ferromagnetism. Our spectroscopic study establishes MnBi$_6$Te$_{10}$ as the first bulk MnBi$_{2n}$Te$_{3n+1}$ compound to host tunable topological orders due to its highly variable electronic and magnetic structures.
The interplay of magnetism and topology is a key research subject in condensed matter physics and material science, which offers great opportunities to explore emerging new physics, like the quantum anomalous Hall (QAH) effect, axion electrodynamics and Majorana fermions. However, these exotic physical effects have rarely been realized in experiment, due to the lacking of suitable working materials. Here we predict that van der Waals layered MnBi$_2$Te$_4$-family materials show two-dimensional (2D) ferromagnetism in the single layer and three-dimensional (3D) $A$-type antiferromagnetism in the bulk, which could serve as a next-generation material platform for the state-of-art research. Remarkably, we predict extremely rich topological quantum effects with outstanding features in an experimentally available material MnBi$_2$Te$_4$, including a 3D antiferromagnetic topological insulator with the long-sought topological axion states, the type-II magnetic Weyl semimetal (WSM) with simply one pair of Weyl points, and the high-temperature intrinsic QAH effect. These striking predictions, if proved experimentally, could profoundly transform future research and technology of topological quantum physics.
The unoccupied part of the band structure in the magnetic topological insulator MnBi$_2$Te$_4$ is studied by first-principles calculations. We find a second, unoccupied topological surface state with similar electronic structure to the celebrated occupied topological surface state. This state is energetically located approximate $1.6$ eV above the occupied Dirac surface state around $Gamma$ point, which permit it to be directly observed by the two-photon angle-resolved photoemission spectroscopy. We propose a unified effective model for the occupied and unoccupied surface states. Due to the direct optical coupling between these two surface states, we further propose two optical effects to detect the unoccupied surface state. One is the polar Kerr effect in odd layer from nonvanishing ac Hall conductance $sigma_{xy}(omega)$, and the other is higher-order terahertz-sideband generation in even layer, where the non-vanishining Berry curvature of the unoccupied surface state is directly observed from the giant Faraday rotation of optical emission.
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