MnBi$_8$Te$_{13}$ is an intrinsic ferromagnetic (FM) topological insulator with different complex surface terminations. Resolving the electronic structures of different termination surfaces and manipulation of the electronic state are important. Here, by using micrometer spot time- and angle-resolved photoemission spectroscopy ($μ$-TrARPES), we resolve the electronic structures and reveal the ultrafast dynamics upon photoexcitation. Photoinduced filling of the surface state hybridization gap is observed for the Bi$_2$Te$_3$ quintuple layer directly above MnBi$_2$Te$_4$ accompanied by a nontrivial shift of the surface state, suggesting light-tunable interlayer interaction. Relaxation of photoexcited electrons and holes is observed within 1-2 ps. Our work reveals photoexcitation as a potential control knob for tailoring the interlayer interaction and surface state of MnBi$_8$Te$_{13}$.
Anomalous Hall effect (AHE) is an important transport signature revealing topological properties of magnetic materials and their spin textures. Recently, antiferromagnetic MnBi2Te4 has been demonstrated to be an intrinsic magnetic topological insulator that exhibits quantum AHE in exfoliated nanoflakes. However, its complicated AHE behaviors may offer an opportunity for the unexplored correlation between magnetism and band structure. Here, we show the Berry curvature dominated intrinsic AHE in wafer-scale MnBi2Te4 thin films. By utilizing a high-dielectric SrTiO3 as the back-gate, we unveil an…
In the newly discovered magnetic topological insulator MnBi$_2$Te$_4$, both axion insulator state and quantized anomalous Hall effect (QAHE) have been observed by tuning the magnetic structure. The related (MnBi$_2$Te$_4$)$_m$(Bi$_2$Te$_3$)$_n$ heterostructures with increased tuning knobs, are predicted to be a more versatile platform for exotic topological states. Here, we report angle-resolved photoemission spectroscopy (ARPES) studies on a series of the heterostructures (MnBi$_2$Te$_4$, MnBi$_4$Te$_7$ and MnBi$_6$Te$_{10}$). A universal gapless Dirac cone is observed at the MnBi$_2$Te$_4$ t…
Tailoring magnetic orders in topological insulators is critical to the realization of topological quantum phenomena. An outstanding challenge is to find a material where atomic defects lead to tunable magnetic orders while maintaining a nontrivial topology. Here, by combining magnetization measurements, angle-resolved photoemission spectroscopy, and transmission electron microscopy, we reveal disorder-enabled, tunable magnetic ground states in MnBi$_6$Te$_{10}$. In the ferromagnetic phase, an energy gap of 15 meV is resolved at the Dirac point on the MnBi$_2$Te$_4$ termination. In contrast, an…
Manipulating the interlayer magnetic coupling in van der Waals magnetic materials and heterostructures is the key to tailoring their magnetic and electronic properties for various electronic applications and fundamental studies in condensed matter physics. By utilizing the MnBi2Te4-family compounds and their heterostructures as a model system, we systematically studied the dependence of the sign and strength of interlayer magnetic coupling on constituent elements by using first-principles calculations. It was found that the coupling is a long-range superexchange interaction mediated by the cha…
Shubnikov-de Hass oscillations are directly observed in undoped antiferromagnetic topological insulator MnBi2Te4. With increasing magnetic fields, the oscillation period decreases gradually in the magnetic transition from canted antiferromagnetism to ferromagnetism and then saturates in high magnetic fields, indicating the field-induced evolution of the band structure. From the analysis of the high-field oscillations, a nontrivial Berry phase and a small effective mass are extracted, in agreement with the predicted Weyl semimetal phase in ferromagnetic MnBi2Te4. Furthermore, rotating the magne…
The recently discovered antiferromagnetic topological insulator MnBi$_2$Te$_4$ hosts a variety of exotic topological quantum phases such as the axion insulator and Chern insulator states. Here we report systematic gate voltage dependent magneto transport studies in six septuple-layer MnBi$_2$Te$_4$. In p-type carrier regime, we observe positive linear magnetoresistance when MnBi$_2$Te$_4$ is polarized in the ferromagnetic state by an out-of-plane magnetic field. Whereas in n-type regime, distinct negative magnetoresistance behaviors are observed. The magnetoresistance in both regimes is highly…
The recent discovered intrinsic magnetic topological insulator MnBi2Te4 have been met with unusual success in hosting emergent phenomena such as the quantum anomalous Hall effect and the axion insulator states. However, the surface-bulk correspondence of the Mn-Bi-Te family, composed by the superlattice-like MnBi2Te4/(Bi2Te3)n (n = 0, 1, 2, 3 ...) layered structure, remains intriguing but elusive. Here, by using scanning tunneling microscopy (STM) and angle-resolved photoemission spectroscopy (ARPES) techniques, we unambiguously assign the two distinct surface states of MnBi4Te7 (n = 1) to the…
Despite the rapid progress in understanding the first intrinsic magnetic topological insulator MnBi$_2$Te$_4$, its electronic structure remains a topic under debates. Here we perform a thorough spectroscopic investigation into the electronic structure of MnBi$_2$Te$_4$ via laser-based angle-resolved photoemission spectroscopy. Through quantitative analysis, we estimate an upper bound of 3 meV for the gap size of the topological surface state. Furthermore, our circular dichroism measurements reveal band chiralities for both the topological surface state and quasi-2D bands, which can be well rep…
Natural superlattice structures $\rm{(MnBi_2Te_4)(Bi_2Te_3)}$$_n$ ($n$ = 1, 2,...), in which magnetic $\rm{MnBi_2Te_4}$ layers are separated by nonmagnetic $\rm{Bi_2Te_3}$ layers, hold band topology, magnetism and reduced interlayer coupling, providing a promising platform for the realization of exotic topological quantum states. However, their magnetism in the two-dimensional limit, which is crucial for further exploration of quantum phenomena, remains elusive. Here, complex ferromagnetic (FM)-antiferromagnetic (AFM) coexisting ground states that persist up to the 2-septuple layers (SLs) limi…
The layered antiferromagnetic MnBi2Te4 films have been proposed to be an intrinsic quantum anomalous Hall (QAH) insulator with a large gap. To realize this proposal, it is crucial to open a magnetic gap of surface states. However, recent experiments have observed gapless surface states, indicating the absence of out-of-plane surface magnetism, and thus the quantized Hall resistance can only be achieved at the magnetic field above 6 T. In this work, we propose to induce out-of-plane surface magnetism of MnBi2Te4 films via the magnetic proximity with magnetic insulator CrI3. Our calculations hav…
The layered MnBi2nTe3n+1 family represents the first intrinsic antiferromagnetic topological insulator (AFM TI, protected by a combination symmetry ) ever discovered, providing an ideal platform to explore novel physics such as quantum anomalous Hall effect at elevated temperature and axion electrodynamics. Recent angle-resolved photoemission spectroscopy (ARPES) experiments on this family have revealed that all terminations exhibit (nearly) gapless topological surface states (TSSs) within the AFM state, violating the definition of the AFM TI, as the surfaces being studied should be -breaking …
Recently, natural van der Waals heterostructures of (MnBi2Te4)m(Bi2Te3)n have been theoretically predicted and experimentally shown to host tunable magnetic properties and topologically nontrivial surface states. In this work, we systematically investigate both the structural and electronic responses of MnBi2Te4 and MnBi4Te7 to external pressure. In addition to the suppression of antiferromagnetic order, MnBi2Te4 is found to undergo a metal-semiconductor-metal transition upon compression. The resistivity of MnBi4Te7 changes dramatically under high pressure and a non-monotonic evolution of \r{h…
The recent discovery of antiferromagnetic (AFM) topological insulator (TI) MnBi$_2$Te$_4$ has triggered great research efforts on exploring novel magnetic topological physics. Based on first-principles calculations, we find that the manipulation of magnetic orientation and order not only significantly affects material symmetries and orbital hybridizations, but also results in variant new magnetic topological phases in MnBi$_2$Te$_4$. We thus predict a series of unusual topological quantum phase transitions that are magnetically controllable in the material, including phase transitions from AFM…
The layered van der Waals (vdW) material MnBi$_2$Te$_4$ is an intrinsic magnetic topological insulator with various topological phases such as quantum anomalous Hall effect (QAHE) and axion states. However, both the zero-field and high-temperature QAHE are not easy to realize. It is theoretically proposed that the exchange bias can be introduced in the MnBi2Te4/ferromagnetic (FM) insulator heterostructures and thus opens the surface states gap, making it easier to realize the zero-field or high-temperature QAHE. Here we report the electrically tunable exchange bias in the van der Waals MnBi$_2…
Using angle-resolved photoelectron spectroscopy (ARPES), we investigate the surface electronic structure of the magnetic van der Waals compounds MnBi$_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 disent…
Optical study of the charge dynamics evolution in the topological insulators MnBi$_2$Te$_4$ and Mn(Bi$_{0.74}$Sb$_{0.26}$)$_2$Te$_4$ under high pressure
Tuning topological and magnetic properties of materials by applying an electric field is widely used in spintronics. In this work, we find a topological phase transition from topologically trivial to nontrivial states at an external electric field of about 0.1 V/A in MnBi$_2$Te$_4$ monolayer that is a topologically trivial ferromagnetic semiconductor. It is shown that when electric field increases from 0 to 0.15 V/A, the magnetic anisotropy energy (MAE) increases from about 0.1 to 6.3 meV, and the Curie temperature Tc increases from 13 to about 61 K. The increased MAE mainly comes from the enh…
Quantum states of matter combining non-trivial topology and magnetism attract a lot of attention nowadays; the special focus is on magnetic topological insulators (MTIs) featuring quantum anomalous Hall and axion insulator phases. Feasibility of many novel phenomena that \emph{intrinsic} magnetic TIs may host depends crucially on our ability to engineer and efficiently tune their electronic and magnetic structures. Here, using angle- and spin-resolved photoemission spectroscopy along with \emph{ab initio} calculations we report on a large family of intrinsic magnetic TIs in the homologous seri…
We use high-resolution, tunable angle-resolved photoemission spectroscopy (ARPES) and density functional theory (DFT) calculations to study the electronic properties of single crystals of MnBi2Te4, a material that was predicted to be the first intrinsic antiferromagnetic (AFM) topological insulator. We observe both bulk and surface bands in the electronic spectra, in reasonable agreement with the DFT calculations results. In striking contrast to the earlier literatures showing a full gap opening between two surface band manifolds along (0001) direction, we observed a gapless Dirac cone remain …
We present an approach to monitor and control the strength of the hybridization between electronic states of graphene and metal surfaces. Inspecting the distribution of the $π$ band in a high-quality graphene layer synthesized on Ni(111) by angle-resolved photoemission, we observe a new "kink" feature which indicates a strong hybridization between $π$ and \textit{d} states of graphene and nickel, respectively. Upon deposition and gradual intercalation of potassium atoms into the graphene/Ni(111) interface, the "kink" feature becomes less pronounced pointing at potassium mediated attenuation of…
Applying electric or magnetic fields is widely used to not only create and manipulate topological states but also facilitate their observations in experiments. In this work, we show by first-principles calculations and topological analysis that the time-reversal (TR) symmetry-broken quantum spin Hall (QSH) state emerges in a two-dimensional ferromagnetic MnBi$_4$Te$_7$ monolayer. This TR-symmetry broken QSH phase possesses a highly tunable nontrivial band gap under an external electric field (or tuning interlayer distance). Furthermore, based on the Wannier-function-based tight-binding approac…
We propose MnBi$_{2n}$Te$_{3n+1}$ as a magnetically tunable platform for realizing various symmetry-protected higher-order topology. Its canted antiferromagnetic phase can host exotic topological surface states with a Möbius twist that are protected by nonsymmorphic symmetry. Moreover, opposite surfaces hosting Möbius fermions are connected by one-dimensional chiral hinge modes, which offers the first material candidate of a higher-order topological Möbius insulator. We uncover a general mechanism to feasibly induce this exotic physics by applying a small in-plane magnetic field to the antifer…
We theoretically study magnon-phonon hybrid excitations (magnon-polarons) in two-dimensional antiferromagnets on a honeycomb lattice. With an in-plane Dzyaloshinskii-Moriya interaction (DMI) allowed from mirror symmetry breaking from phonons, we find non-trivial Berry curvature around the anti-crossing rings among magnon and both optical and acoustic phonon bands, which gives rise to finite Chern numbers. We show that the Chern numbers of the magnon-polaron bands can be manipulated by changing the magnetic field direction or strength. We evaluate the thermal Hall conductivity reflecting the no…
Van der Waals magnets are uniquely positioned at the intersection between two-dimensional materials, antiferromagnetic spintronics, and magnonics. The interlayer exchange interaction in these materials enables antiferromagnetic resonances to be accessed at GHz frequencies. Consequently, these layered antiferromagnets are intriguing materials out of which quantum hybrid magnonic devices can be fashioned. Here, we use both a modified macrospin model and micromagnetic simulations to demonstrate a comprehensive antiferromagnetic resonance spectra in van der Waals magnets near the ultrathin (monola…
In magnetic topological insulators (TIs), the interplay between magnetic order and nontrivial topology can induce fascinating topological quantum phenomena, such as the quantum anomalous Hall effect, chiral Majorana fermions and axion electrodynamics. Recently, a great deal of attention has been focused on the intrinsic magnetic TIs, where disorder effects can be eliminated to a large extent, which is expected to facilitate the emergence of topological quantum phenomena. In despite of intensive efforts, experimental evidence of the topological surface states (SSs) remains elusive. Here, by com…
The quantum anomalous Hall effect (QAHE) has unique advantages in topotronic applications, but it is still challenging to realize the QAHE with tunable magnetic and topological properties for building functional devices. Through systematic first-principles calculations, we predict that the in-plane magnetization induced QAHE with Chern numbers C = $\pm$1 and the out-of-plane magnetization induced QAHE with high Chern numbers C = $\pm$3 can be realized in a single material candidate, which is composed of van der Waals (vdW) coupled Bi and MnBi$_2$Te$_4$ monolayers. The switching between differe…
Topological materials featuring exotic band structures, unconventional current flow patterns, and emergent organizing principles offer attractive platforms for the development of next-generation transformative quantum electronic technologies. The family of MnBi2Te4 (Bi2Te3)n materials is naturally relevant in this context due to their nontrivial band topology, tunable magnetism, and recently discovered extraordinary quantum transport behaviors. Despite numerous pioneering studies, to date, the local magnetic properties of MnBi2Te4 (Bi2Te3)n remain an open question, hindering a comprehensive un…
Magnetic topological insulators (MnBi$_2$Te$_4$)(Bi$_2$Te$_3$)$_n$ ($n=0,1,2,3$) are promising to realize exotic topological states such as the quantum anomalous Hall effect (QAHE) and axion insulator (AI), where the Bi$_2$Te$_3$ layer introduces versatility to engineer electronic and magnetic properties. However, whether surface states on the Bi$_2$Te$_3$ terminated facet are gapless or gapped is debated, and its consequences in thin-film properties are rarely discussed. In this work, we find that the Bi$_2$Te$_3$ terminated facets are gapless for $n \ge 1$ compounds by calculations. Despite …
Orbital-Selective Engineering of Strain-Tunable Chern Insulators in Momentum Space
Key Laboratory of Magnetism and Magnetic Functional Materials (Lanzhou University), Ministry of Education（磁性功能材料教育部重点实验室（兰州大学））；Henan Institute of Technology（河南工学院）；School of Physics Science and Technology, Lanzhou University（兰州大学物理科学与技术学院）
The ability to fine-tune band gap and band inversion in topological materials is highly desirable for the development of novel functional devices. Here we propose that the electronic properties of a free-standing nanomembrane of topological crystalline insulator (TCI) SnTe and Pb$_{1-x}$Sn$_x$(Se,Te) are highly tunable by engineering elastic strain and controlling membrane thickness, resulting in tunable band gap and giant piezoconductivity. Membrane thickness governs the hybridization of topological electronic states on opposite surfaces, while elastic strain can further modulate the hybridiz…
We have investigated the structural and electronic properties of phosphorescent planar platinum(II) complexes at the interface of Au(111) with submolecular resolution using combined scanning tunneling microscopy and spectroscopy as well as density functional theory. Our analysis shows that molecule-substrate coupling and lateral intermolecular interactions are weak. While the ligand orbitals remain essentially unchanged upon contact to the substrate, we found modified electronic behavior at the Pt atom due to local hybridization and charge transfer to the substrate. Thus, this novel class of p…
As one of paradigmatic phenomena in condensed matter physics, the quantum anomalous Hall effect (QAHE) in stoichiometric Chern insulators has drawn great interest for years. By using model Hamiltonian analysis and first-principle calculations, we establish a topological phase diagram and map on it with different two-dimensional configurations, which is taken from the recently-grown magnetic topological insulators MnBi4Te7 and MnBi6Te10 with superlattice-like stacking patterns. These configurations manifest various topological phases, including quantum spin Hall effect with and without time-rev…
Hybrid magnonic systems host a variety of characteristic quantum phenomena such as the magnetically-induced transparency (MIT) and Purcell effect, which are considered useful for future coherent quantum information processing. In this work, we experimentally demonstrate a tunable MIT effect in the Y3Fe5O12(YIG)/Permalloy(Py) magnon-magnon coupled system via changing the magnetic field orientations. By probing the magneto-optic effects of Py and YIG, we identify clear features of MIT spectra induced by the mode hybridization between the uniform mode of Py and the perpendicular standing spin-wav…
Moiré interlayer exciton in transition metal dichalcogenide heterobilayer features a permanent electric dipole that enables the electrostatic control of its flow, and optical dipole that is spatially varying in the moiré landscape. We show the hybridization of moiré interlayer exciton with photons in a planar 2D cavity leads to two types of moiré polaritons that exhibit distinct forms of topological transport phenomena including the spin/valley Hall and polarization Hall effects, which feature remarkable electrical tunability through the control of exciton-cavity detuning by the interlayer bia…
Bulk photovoltaic (BPV) effect, a second order nonlinear process that generates static current under light irradiation, requires centrosymmetric broken systems as its application platform. In order to realize measurable BPV photocurrent in spatially centrosymmetric materials, various schemes such as chemical doping, structural deformation, or electric bias have been developed. In the current work, we suggest that magnetic proximity effect via van der Waals interfacial interaction, a contact-free strategy, also breaks the centrosymmetry and generate large BPV photocurrents. Using the Bi2Te3 qui…
Nonlinear photocurrent in time-reversal invariant noncentrosymmetric systems have attracted substantial interest. Here we propose two new types of second-order nonlinear direct photocurrent as the counterpart of normal shift photocurrent (NSC) and normal injection photocurrent (NIC), namely magnetic shift photocurrent (MSC) and magnetic injection photocurrent (MIC) in time-reversal symmetry and inversion symmetry broken system. We show that MSC is mainly governed by shift vector and interband Berry curvature, and MIC is dominated by absorption strength and asymmetry of the group velocity diffe…
The recent discovery of natural biaxial hyperbolicity in van der Waals crystals, such as $α$-MoO$_3$, has opened up new avenues for mid-IR nanophotonics due to their deep subwavelength phonon-polaritons. However, a significant challenge is the lack of active tunability of these hyperbolic phonon polaritons. In this work, we investigate heterostructures of graphene and $α$-MoO$_3$ for actively tunable hybrid plasmon phonon polariton modes via electrostatic gating in the mid-infrared spectral region. We observe a unique propagation direction dependent hybridization of graphene plasmon polaritons…
We show that the tunable hybridization between two lateral quantum dots connected to non-magnetic current leads in a `hanging-dot' configuration that can be used to implement a bipolar spin filter. The competition between Zeeman, exchange interaction, and interdot tunneling (molecular hybridization) yields a singlet-triplet transition of the double dot {\it ground state} that allows spin filtering in Coulomb blockade experiments. Its generic nature should make it broadly useful as a robust bidirectional spin polarizer.
Direct, tunable coupling between individually assembled graphene layers is a next step towards designer two-dimensional (2D) crystal systems, with relevance for fundamental studies and technological applications. Here we describe the fabrication and characterization of large-area (> cm^2), coupled bilayer graphene on SiO2/Si substrates. Stacking two graphene films leads to direct electronic interactions between layers, where the resulting film properties are determined by the local twist angle. Polycrystalline bilayer films have a "stained-glass window" appearance explained by the emergence of…
Hybridization of semiconducting and magnetic materials into a single heterostructure is believed to be potentially applicable to the design of novel functional spintronic devices. In the present work we report epitaxial stabilization of four magnetically ordered iron oxide phases (Fe3O4, γ-Fe2O3, α-Fe2O3 and most exotic metastable ε-Fe2O3) in the form of nanometer sized single crystalline films on GaN(0001) surface. The epitaxial growth of as many as four distinctly different iron oxide phases is demonstrated within the same single-target Laser MBE technological process on a GaN semiconductor …
Tunable 2D Electron- and 2D Hole States Observed at Fe/SrTiO$_3$ Interfaces
Universität Konstanz（康斯坦茨大学）；Technische Universität Dortmund（多特蒙德工业大学）；Forschungszentrum Jülich GmbH（于利希研究中心有限公司）；Paul Scherrer Institute（保罗谢尔研究所）；Ruhr-Universität Bochum（波鸿鲁尔大学）
