Haiming Deng, Zhiyi Chen, Agnieszka Wolos, Marcin Konczykowski, Kamil Sobczak, Joanna Sitnicka, Irina V. Fedorchenko, Jolanta Borysiuk, Tristan Heider, Lukasz Plucinski, Kyungwha Park, Alexandru B. Georgescu, Jennifer Cano, Lia Krusin-Elbaum
The quantum anomalous Hall effect is a fundamental transport response of a topologically non-trivial system in zero magnetic field. Its physical origin relies on the intrinsically inverted electronic band structure and ferromagnetism, and its most consequential manifestation is the dissipation-free flow of chiral charge currents at the edges that can potentially transform future quantum electronics. Here we report a previously unknown Berry-curvature-driven anomalous Hall regime ('Q-window') at above-Kelvin temperatures in the magnetic topological bulk crystals where through growth Mn ions self-organize into a period-ordered MnBi$_2$Te$_4$/Bi$_2$Te$_3$ superlattice. Robust ferromagnetism of the MnBi$_2$Te$_4$ monolayers opens a large surface gap, and anomalous Hall conductance reaches an $e^2/h$ quantization plateau when the Fermi level is tuned into this gap within a Q-window in which the anomalous Hall conductance from the bulk is to a high precision zero. The quantization in this new regime is not obstructed by the bulk conduction channels and thus should be present in a broad family of topological magnets.
Magnetic topological quantum materials (TQMs) provide a fertile ground for the emergence of fascinating topological magneto-electric effects. Recently, the discovery of intrinsic antiferromagnetic (AFM) topological insulator MnBi2Te4 that could realize quantized anomalous Hall effect and axion insulator phase ignited intensive study on this family of TQM compounds. Here, we investigated the AFM compound MnBi4Te7 where Bi2Te3 and MnBi2Te4 layers alternate to form a superlattice. Using spatial- and angle-resolved photoemission spectroscopy, we identified ubiquitous (albeit termination dependent)…
The magnetic structures of MnBi2Te4(Bi2Te3)n can be manipulated by tuning the interlayer coupling via the number of Bi2Te3 spacer layers n, while the intralayer ferromagnetic (FM) exchange coupling is considered too robust to control. By applying hydrostatic pressure up to 3.5 GPa, we discover opposite responses of magnetic properties for n = 1 and 2. MnBi4Te7 stays at A-type antiferromagnetic (AFM) phase with a decreasing Néel temperature and an increasing saturation field. In sharp contrast, MnBi6Te10 experiences a phase transition from A-type AFM to a quasi-two-dimensional FM state with a s…
MnBi$_{2}$Te$_{4}/$(Bi$_{2}$Te$_{3}$)$_{n}$ materials system has recently generated strong interest as a natural platform for realization of the quantum anomalous Hall (QAH) state. The system is magnetically much better ordered than substitutionally doped materials, however, the detrimental effects of certain disorders are becoming increasingly acknowledged. Here, from compiling structural, compositional, and magnetic metrics of disorder in ferromagnetic MnBi$_{2}$Te$_{4}/$(Bi$_{2}$Te$_{3}$)$_{n}$ it is found that migration of Mn between MnBi$_{2}$T$e_{4}$ septuple layers (SLs) and otherwise n…
In a magnetic topological insulator, nontrivial band topology conspires with magnetic order to produce exotic states of matter that are best exemplified by quantum anomalous Hall (QAH) insulators and axion insulators. Up till now, such magnetic topological insulators are obtained by doping topological insulators with magnetic atoms. The random magnetic dopants, however, inevitably introduce disorders that hinder further exploration of quantum effects in the material. Here, we resolve this dilemma by probing quantum transport in MnBi$_2$Te$_4$ thin flake - a topological insulator with intrinsic…
Magnetic topological insulators (MTIs) have received a lot of attention due to the existence of various quantum phenomena such as quantum anomalous Hall effect (QAHE) and topological magnetoelectric effect, etc. The intrinsic superlattice-like layered MTIs, MnBi2Te4/(Bi2Te3)n, have been extensively investigated mainly through the transport measurements, while the direct investigation of their superlattice-sensitive magnetic behaviors is relatively rare. Here, we report a microscopic real-space investigation of magnetic phase behaviors in MnBi4Te7 using cryogenic magnetic force microscopy (MFM)…
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 interlayer antiferromagnetic coupling hinders the observation of quantum anomalous Hall effect in magnetic topological insulator MnBi$_2$Te$_4$. We demonstrate that interlayer \textit{ferromagnetism} can be established by utilizing the \textit{p}-doping method in MnBi$_2$Te$_4$ multilayers. In two septuple-layers system, the interlayer ferromagnetic coupling appears by doping nonmagnetic elements (e.g., N, P, As, Na, Mg, K, and Ca), due to the redistribution of orbital occupations of Mn. We further find that Mg and Ca elements are the most suitable candidates because of their low formation…
Quantum anomalous Hall effect (QAHE) has been experimentally realized in magnetically-doped topological insulators or intrinsic magnetic topological insulator MnBi$_2$Te$_4$ by applying an external magnetic field. However, either the low observation temperature or the unexpected external magnetic field (tuning all MnBi$_2$Te$_4$ layers to be ferromagnetic) still hinders further application of QAHE. Here, we theoretically demonstrate that proper stacking of MnBi$_2$Te$_4$ and Sb$_2$Te$_3$ layers is able to produce intrinsically ferromagnetic van der Waals heterostructures to realize the high-te…
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…
Layer-polarized anomalous Hall effect (LP-AHE) is an attractive phenomenon in condensed-matter physics from the standpoints of both fundamental interest and device applications. The current LP-AHE research is based on the extrinsic paradigm of using external electric fields, in which the generation and control of LP-AHE are not straightforward. Here, we propose a novel mechanism that realizes intrinsic LP-AHE in bilayer lattices, through the mediation of sliding physics and Berry curvature. Moreover, this mechanism could render the LP-AHE in a controllable and reversable fashion. We analyze th…
Intrinsic magnetic topological insulators offer low disorder and large magnetic bandgaps for robust magnetic topological phases operating at higher temperatures. By controlling the layer thickness, emergent phenomena such as the Quantum Anomalous Hall (QAH) effect and axion insulator phases have been realised. These observations occur at temperatures significantly lower than the Neel temperature of bulk MnBi2Te4, and measurement of the magnetic energy gap at the Dirac point in ultra-thin MnBi2Te4 has yet to be achieved. Critical to achieving the promise of this system is a direct measurement o…
Using density functional theory and Monte Carlo calculations, we study the thickness dependence of the magnetic and electronic properties of a van der Waals interlayer antiferromagnet in the two-dimensional limit. Considering $\mathrm{MnBi_2Te_4}$ as a model material, we find it to demonstrate a remarkable set of thickness-dependent magnetic and topological transitions. While a single septuple layer block of $\mathrm{MnBi_2Te_4}$ is a topologically trivial ferromagnet, the thicker films made of an odd (even) number of blocks are uncompensated (compensated) interlayer antiferromagnets, which sh…
Intrinsic Even-Odd Thickness-Driven Anomalous Hall in Epitaxial MnBi2Te4 Thin Films
Oak Ridge National Laboratory（橡树岭国家实验室）；Pennsylvania State University（宾夕法尼亚州立大学）；Los Alamos National Laboratory（洛斯阿拉莫斯国家实验室）；Argonne National Laboratory（阿贡国家实验室）；University of Pennsylvania（宾夕法尼亚大学）
Understanding the effects of interfacial modification to the functional properties of magnetic topological insulator thin films is crucial for developing novel technological applications from spintronics to quantum computing. Here, we report that a large electronic and magnetic response is induced in the intrinsic magnetic topological insulator MnBi2Te4 by controlling the propagation of surface oxidation. We show that the formation of the surface oxide layer is confined to the top 1-2 unit cells but drives large changes in the overall magnetic response. Specifically, we observe a dramatic reve…
$\mathrm{MnBi_2Te_4}$ has recently been established as an intrinsic antiferromagnetic (AFM) topological insulator and predicted to be an ideal platform to realize quantum anomalous Hall (QAH) insulator and axion insulator states. We performed comprehensive studies on the structure, nontrivial surface state and magnetotransport properties of this material. Our results reveal an intrinsic anomalous Hall effect arising from a non-collinear spin structure for the magnetic field parallel to the $c$-axis. We also observed remarkable negative magnetoresistance under arbitrary field orientation below …
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 intrinsic antiferromagnetic (AFM) interlayer coupling in two-dimensional magnetic topological insulator MnBi$_2$Te$_4$ places a restriction on realizing stable quantum anomalous Hall effect (QAHE) [Y. Deng et al., Science 367, 895 (2020)]. Through density functional theory calculations, we demonstrate the possibility of tuning the AFM coupling to the ferromagnetic coupling in MnBi$_2$Te$_4$ films by alloying about 50% V with Mn. As a result, QAHE can be achieved without alternation with the even or odd septuple layers. This provides a practical strategy to get robust QAHE in ultrathin MnBi…
The intrinsic antiferromagnetic topological insulator MnBi2Te4 provides an ideal platform for exploring exotic topological quantum phenomena. Recently, the Chern insulator and axion insulator phases have been realized in few-layer MnBi2Te4 devices at low magnetic field regime. However, the fate of MnBi2Te4 in high magnetic field has never been explored in experiment. In this work, we report transport studies of exfoliated MnBi2Te4 flakes in pulsed magnetic fields up to 61.5 T. In the high-field limit, the Chern insulator phase with Chern number C = -1 evolves into a robust zero Hall resistance…
Observation of the quantum anomalous Hall effect (QAHE) in MnBi$_2$Te$_4$ flakes is one of the most exciting results in the study of the intrinsic magnetic topological insulator MnBi$_2$Te$_4$ and related compounds. This fascinating result is yet to be reproduced two years after its first report. The quality of starting MnBi$_2$Te$_4$ single crystals is believed to be the key factor. An interesting and important question to address is what is the right quality to enable the QAHE. In this perspective, we present possible approaches to tuning the magnetic and topological properties of MnBi$_2$Te…
Ultrathin films of intrinsic magnetic topological insulator MnBi2Te4 exhibit fascinating quantum properties such as quantum anomalous Hall effect and axion insulator state. In this work, we systematically investigate the evolution of the electronic structure of MnBi2Te4 thin films. With increasing film thickness, the electronic structure changes from an insulator-type with a large energy gap to one with in-gap topological surface states, which is, however, still drastically different from the bulk material. By surface doping of alkali-metal atoms, a Rashba split band gradually emerges and hybr…
The recent realizations of the quantum anomalous Hall effect (QAHE) in MnBi$_2$Te$_4$ and MnBi$_4$Te$_7$ benchmark the (MnBi$_2$Te$_4$)(Bi$_2$Te$_3$)$_n$ family as a promising hotbed for further QAHE improvements. The family owes its potential to its ferromagnetically (FM) ordered MnBi$_2$Te$_4$ septuple layers (SL). However, the QAHE realization is complicated in MnBi$_2$Te$_4$ and MnBi$_4$Te$_7$ due to the substantial antiferromagnetic (AFM) coupling between the SL. An FM state, advantageous for the QAHE, can be stabilized by interlacing the SL with an increasing number $n$ of Bi$_2$Te$_3$ l…
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…
The combination of topology and magnetism is attractive to produce exotic quantum matters, such as the quantum anomalous Hall state, axion insulators and the magnetic Weyl semimetals. MnBi2Te4, as an intrinsic magnetic topological insulator, provides a platform for the realization of various topological phases. Here we report the intermediate Hall steps in the magnetic hysteresis of MnBi2Te4, where four distinguishable magnetic memory states at zero magnetic field are revealed. The gate and temperature dependence of the magnetic intermediate states indicates the noncollinear spin structure in …
A central theme in condensed matter physics is to create and understand the exotic states of matter by incorporating magnetism into topological materials. One prime example is the quantum anomalous Hall (QAH) state. Recently, MnBi2Te4 has been demonstrated to be an intrinsic magnetic topological insulator and the QAH effect was observed in exfoliated MnBi2Te4 flakes. Here, we used molecular beam epitaxy (MBE) to grow MnBi2Te4 films with thickness down to 1 septuple layer (SL) and performed thickness-dependent transport measurements. We observed a non-square hysteresis loop in the antiferromagn…
We study the critical properties of the in-plane magnetic field-induced quantum anomalous Hall (QAH) plateau transition in axion insulators. Take even septuple layer film MnBi$_2$Te$_4$ as a concrete example, we find the mirror symmetry breaking from in-plane field could induce axion insulator to QAH insulator transition, which belongs to generic integer quantum Hall plateau transition. The chiral Majorana fermion does not necessarily emerge at the QAH plateau transition in MnBi$_2$Te$_4$ due to strong exchange field, but may be quite feasible in its descendent materials MnBi$_4$Te$_7$ and MnB…
As the first intrinsic antiferromagnetic topological insulator, MnBi$_2$Te$_4$ has provided a platform to investigate the interplay of band topology and magnetism as well as the emergent phenomena arising from such an interplay. Here we report the chemical-vapor-transport (CVT) growth and characterization of MnBi$_2$Te$_4$, as well as the observation of the field-induced quantized Hall conductance in 6-layer devices. Through comparative studies between our CVT-grown and flux-grown MnBi$_2$Te$_4$ via magnetic, transport, scanning tunneling microscopy, and angle-resolved photoemission spectrosco…
Three-dimensional (3D) compensated MnBi2Te4 is antiferromagnetic, but undergoes a spin-flop transition at intermediate fields, resulting in a canted phase before saturation. In this work, we experimentally show that the anomalous Hall effect (AHE) in MnBi2Te4 originates from a topological response that is sensitive to the perpendicular magnetic moment and to its canting angle. Synthesis by molecular beam epitaxy allows us to obtain a large-area quasi-3D 24-layer MnBi2Te4 with near-perfect compensation that hosts the phase diagram observed in bulk which we utilize to probe the AHE. This AHE is …
The topological Hall effect (THE), induced by the Berry curvature, which originates from non-zero scalar spin chirality, is an important feature for mesoscopic topological structures, such as skyrmions. However, the THE might also arise from other microscopic non-coplanar spin structures in the lattice. Thus, the origin of the THE inevitably needs to be determined to fully understand skyrmions and find new host materials. Here, we examine the Hall effect in both bulk- and micron-sized lamellar samples of MnBi. The sample size affects the temperature and field range in which the THE is detectab…
The I-Mn-V antiferromagnet, NaMnBi, develops a very large positive magnetoresistance (MR) up to 10,000% at 2 K and 9 T in crystals showing a semiconductor-to-metal transition (SMT). In the absence of an SMT, a modest (20%) MR is achieved. Here, we show that upon cooling below the magnetic transition, a spatial modulation appears giving rise to new Bragg peaks due to charge and defect ordering in a checkerboard pattern, with two kinds of modulation vectors, $q_1$=($\frac23$, 0, 1) and $q_2$=($\frac23, \frac13, \frac12$). This constitutes a superlattice transition ($T_s$) that lowers the symmetr…
We report temperature and magnetic field dependence of the thermal transport properties in single crystals of (Sr/Ca)MnBi$_2$ with linear energy dispersion. In SrMnBi$_2$ thermopower is positive, indicating hole-type carriers and the magnetic field enhances the thermopower significantly. The maximum change of thermopower is about 1600% in 9 T field and at 10 K. A negative thermopower is observed in CaMnBi$_2$ with dominant electron-type carriers and, in contrast, the magnetic field suppresses the absolute value of thermopower. First-principle band structure shows that the chemical potential is…
Breaking time reversal symmetry in a topological insulator may lead to quantum anomalous Hall effect and axion insulator phase. MnBi4Te7 is a recently discovered antiferromagnetic topological insulator with TN ~12.5 K, which is constituted of alternatively stacked magnetic layer (MnBi2Te4) and non-magnetic layer (Bi2Te3). By means of scanning tunneling spectroscopy, we clearly observe the electronic state present at a step edge of a magnetic MnBi2Te4 layer but absent at non-magnetic Bi2Te3 layers at 4.5 K. Furthermore, we find that as the temperature rises above TN, the edge state vanishes, wh…
Based on the ab initio calculations, we study the electronic structure of the BiTeI/MnBi2Te4 heterostructure interface composed of the anti-ferromagnetic topological insulator MnBi$_2$Te$_4$ and the polar semiconductor trilayer BiTeI. We found significant difference in electronic properties at different types of contact between substrate and the overlayer. While the case of Te-Te interface forms natural expansion of the substrate, when Dirac cone state locates mostly in the polar overlayer region and undergoes slight exchange splitting, Te-I contact is the source of four-band state contributed…
Fermi level dependence of magnetism and magnetotransport in the magnetic topological insulators Bi$_{2}$Te$_{3}$ and BiSbTe$_{3}$ containing self-organized MnBi$_{2}$Te$_{4}$ septuple layers
The observation of quantized anomalous Hall conductance in the forced ferromagnetic state of MnBi2Te4 thin flakes has attracted much attentions. However, strong magnetic field is needed to fully polarize the magnetic moments due to the large antiferromagnetic interlayer exchange coupling. Here, we reported the magnetic and electrical transport properties of the magnetic van der Waals MnBi2Te4(Bi2Te3)n (n=1,2) single crystals, in which the interlayer antiferromagnetic exchange coupling is greatly suppressed with the increase of the separation layers Bi2Te3. MnBi4Te7 and MnBi6Te10 show weak anti…
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…
Axion, first postulated as a hypothetical particle in high-energy physics, is now extended to describe a novel topological magnetoelectric effect derived from the Chern-Simons theory in condensed matter systems. The recent discovered intrinsic magnetic topological insulators MnBi2Te4 and its derivatives have attracted great attention because of their potential as a material platform to realize such a quantized axion field. Since the magnetic exchange gap can bring the half-quantized anomalous Hall effect at the surface, an axion insulator manifests as quantum anomalous Hall and zero Hall plate…
The metastable layered compound MnBi2Te4 is the first experimentally realized intrinsic antiferromagnetic topological insulator, predicted to host the quantum anomalous Hall effect at high temperatures upon exfoliation to atomically thin layers. While its magnetic ordering and topological properties have generated intensive interest, the mechanism behind its metastability and the ideal crystal synthesis conditions have remained elusive. Here, using a combined first-principles-based approach that considers lattice, charge, and spin degrees of freedom, we investigate the metastability of MnBi2Te…
Recently, intrinsic antiferromagnetic topological insulator MnBi2Te4 has drawn intense research interest and leads to plenty of significant progress in physics and materials science by hosting quantum anomalous Hall effect, axion insulator state, and other quantum phases. An essential ingredient to realize these quantum states is the magnetic gap in the topological surface states induced by the out-of-plane ferromagnetism on the surface of MnBi2Te4. However, the experimental observations of the surface gap remain controversial. Here, we report the observation of the surface gap via the point c…
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…
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…
A new kind of intrinsic magnetic topological insulators (MTI) MnBi2Te4 family have shed light on the observation of novel topological quantum effect such as quantum anomalous Hall effect (QAHE). However, the strong anti-ferromagnetic (AFM) coupling and high carrier concentration in the bulk hinder the practical applications. In closely related materials MnBi4Te7 and MnBi6Te10, the interlayer magnetic coupling is greatly suppressed by Bi2Te3 layer intercalation. However, AFM is still the ground state in these compounds. Here by magnetic and transport measurements, we demonstrate that Sb substit…
The intrinsic magnetic layered topological insulator MnBi2Te4 with nontrivial topological properties and magnetic order has become a promising system for exploring exotic quantum phenomena such as quantum anomalous Hall effect. However, the layer-dependent magnetism of MnBi2Te4, which is fundamental and crucial for further exploration of quantum phenomena in this system, remains elusive. Here, we use polar reflective magnetic circular dichroism spectroscopy, combined with theoretical calculations, to obtain an in-depth understanding of the layer-dependent magnetic properties in MnBi2Te4. The m…
