Two-dimensional van der Waals MnBi$_{2n}$Te$_{3n+1}$ (n = 1, 2, 3, 4) compounds have been recently found to be intrinsic magnetic topological insulators rendering quantum anomalous Hall effect and diverse topological states. Here, we summarize and compare the crystal and magnetic structures of this family, and discuss the effects of chemical composition on their magnetism. We found that a considerable fraction of Bi occupies at the Mn sites in MnBi$_{2n}$Te$_{3n+1}$ (n = 1, 2, 3, 4) while Mn is no detectable at the non-magnetic atomic sites within the resolution of neutron diffraction experiments. The occupancy of Mn monotonically decreases with the increase of n. The polarized neutron diffraction on the representative MnBi$_{4}$Te$_{7}$ reveals that its magnetization density is exclusively accumulated at the Mn site, in good agreement with the results from the unpolarized neutron diffraction. The defects of Bi at the Mn site naturally explain the continuously reduced saturated magnetic moments from n = 1 to n = 4. The experimentally estimated critical exponents of all the compounds generally suggest a three-dimensional character of magnetism. Our work provides material-specified structural parameters that may be useful for band structure calculations to understand the observed topological surface states and for designing quantum magnetic materials through chemical doping.
Magnetic topological insulators (TI) provide an important material platform to explore quantum phenomena such as quantized anomalous Hall (QAH) effect and Majorana modes, etc. Their successful material realization is thus essential for our fundamental understanding and potential technical revolutions. By realizing a bulk van der Waals material MnBi4Te7 with alternating septuple [MnBi2Te4] and quintuple [Bi2Te3] layers, we show that it is ferromagnetic in plane but antiferromagnetic along the c axis with an out-of-plane saturation field of ~ 0.22 T at 2 K. Our angle-resolved photoemission spect…
Surface magnetism and its correlation with the electronic structure are critical to understand the gapless topological surface state in the intrinsic magnetic topological insulator MnBi$_2$Te$_4$. Here, using static and time resolved angle-resolved photoemission spectroscopy (ARPES), we find a significant ARPES intensity change together with a gap opening on a Rashba-like conduction band. Comparison with a model simulation strongly indicates that the surface magnetism on cleaved MnBi$_2$Te$_4$ is the same as its bulk state. The coexistence of surface ferromagnetism and a gapless TSS uncovers t…
Using single crystal neutron diffraction, we present a systematic investigation of the crystal structure and magnetism of van der Waals topological insulators MnBi$_2$Te$_4$ and MnBi$_4$Te$_7$, where rich topological quantum states have been recently predicted and observed. Structural refinements reveal that considerable Bi atoms occupied on the Mn sites in both materials, distinct from the previously reported antisite disorder. We show unambiguously that MnBi$_{2}$Te$_{4}$ orders antiferromagnetically below 24 K featured by a magnetic symmetry $R_I$-${3c}$ while MnBi$_{4}$Te$_{7}$ is antiferr…
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…
The interplay between topology and magnetism is essential for realizing novel topological states including the axion insulator, the magnetic Weyl semimetal, etc. An intrinsically ferromagnetic topological material with only the topological bands at the charge neutrality energy has so far remained elusive. By rationally designing the natural heterostructure consisting of [MnBi2Te4] septuple layers and [Bi2Te3] quintuple layers, we report MnBi8Te13 as the first intrinsic ferromagnetic topological material with clean low-energy band structure. Based on the thermodynamic, transport and neutron dif…
The fine control of magnetism and electronic structure is crucial since the interplay between magnetism and band topology can lead to various novel magnetic topological states including axion insulators, magnetic Weyl semimetals and Chern insulators etc. Through crystal growth, transport, thermodynamic, neutron diffraction measurements, we show that with Sb-doping, the newly-discovered intrinsic antiferromagnetic topological insulator MnBi4Te7 evolves from antiferro-magnetic to ferromagnetic and then ferrimagnetic. We attribute this to the formation of Mn(Bi,Sb) antisites upon doping, which re…
Here we present microscopic evidence of the persistence of uniaxial A-type antiferromagnetic order to the surface layers of MnBi$_2$Te$_4$ single crystals using magnetic force microscopy. Our results reveal termination-dependent magnetic contrast across both surface step edges and domain walls, which can be screened by thin layers of soft magnetism. The robust surface A-type order is further corroborated by the observation of termination-dependent surface spin-flop transitions, which have been theoretically proposed decades ago. Our results not only provide key ingredients for understanding th…
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…
Intrinsic magnetic topological insulators from MnBi2Te4 family promise realization of axion insulator, a theoretically predicted state of matter capable to mutually convert electric and magnetic signals, and whose properties are reminiscent of cosmological axion dark matter. Here we report the first experimental realization of room-temperature axionic single-spin switch in topological metamaterial MnBi2Te3. The metamaterial was in situ created in the scanning tunneling microscopy (STM) experiment by removing Te atomic layer from MnBi2Te4 surface using STM tip. Room temperature STM study of MnB…
The MnBi$_{2}$Te$_{4}$ family has attracted significant attention due to its rich topological states such as the quantum anomalous Hall (QAH) insulator state, the axion insulator state, and the magnetic Weyl semimetal state. Nevertheless, the intrinsic antiferromagnetic (AFM) interlayer coupling in MnBi$_{2}$Te$_{4}$ partly hinders the realization of "high-temperature" QAH effect. Here, by using first-principles electronic structure calculations, we design a new class of materials Mn\emph{X}$_{2}$\emph{B}$_{2}$\emph{T}$_{6}$ (\emph{X}=Ge, Sn, or Pb; \emph{B}=Sb or Bi; \emph{T}=Se or Te) based …
Here we report the evolution of structural, magnetic and transport properties in MnBi$_{2-x}$Sb$_x$Te$_4$ (0$\leq x \leq$2) single crystals. MnSb$_2$Te$_4$, isostructural to MnBi$_2$Te$_4$, has the lattice parameters of \textit{a}=4.2445(3)$Å$ and \textit{c}=40.869(5)$Å$, respectively. With increasing Sb content in MnBi$_{2-x}$Sb$_x$Te$_4$, the \textit{a}-lattice decreases linearly following the Vegards law while the \textit{c}-lattice shows little compositional dependence. The \textit{a}-lattice contraction occurs by reducing Mn-Te-Mn bond angle while Mn-Te bond length remains nearly constant…
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 …
The layered van der Waals antiferromagnet MnBi$_2$Te$_4$ has been predicted to combine the band ordering of archetypical topological insulators such as Bi$_2$Te$_3$ with the magnetism of Mn, making this material a viable candidate for the realization of various magnetic topological states. We have systematically investigated the surface electronic structure of MnBi$_2$Te$_4$(0001) single crystals by use of spin- and angle-resolved photoelectron spectroscopy experiments. In line with theoretical predictions, the results reveal a surface state in the bulk band gap and they provide evidence for t…
MnBi2Te4(MBT) is a promising van der Waals layered antiferromagnetic (AF) topological insulator that combines a topologically non-trivial inverted Bi-Te band gap with ferromagnetic (FM) layers of Mn ions. We perform inelastic neutron scattering (INS) on co-aligned single crystals to study the magnetic interactions in MBT. Consistent with previous work, we find that the AF interlayer exchange coupling and uniaxial magnetic anisotropy have comparable strength, which supports metamagnetic transitions that allow access to different magnetic symmetries in applied fields. Modelling of the two-dimens…
Magnetism in topological materials creates phases exhibiting quantized transport phenomena with applications in spintronics and quantum information. The emergence of such phases relies on strong interaction between localized spins and itinerant states comprising the topological bands, and the subsequent formation of an exchange gap. However, this interaction has never been measured in any intrinsic magnetic topological material. Using a multimodal approach, this exchange interaction is measured in MnBi2Te4, the first realized intrinsic magnetic topological insulator. Interrogating nonequilibri…
The realization of magnetic frustration in a metallic van der Waals (vdW) coupled material has been sought as a promising platform to explore novel phenomena both in bulk matter and in exfoliated devices. However, a suitable material platform has been lacking so far. Here, we demonstrate that CeSiI hosts itinerant electrons coexisting with exotic magnetism. In CeSiI, the magnetic cerium atoms form a triangular bilayer structure sandwiched by van der Waals stacked iodine layers. From resistivity and magnetometry measurements, we confirm the coexistence of itinerant electrons with magnetism with…
Magnetic insulators are a key resource for next-generation spintronic and topological devices. The family of layered metal halides promises ultrathin insulating multiferroics, spin liquids, and ferromagnets, but new characterization methods are required to unlock their potential. Here, we report tunneling through the layered magnetic insulator CrI3 as a function of temperature and applied magnetic field. We electrically detect the magnetic ground state and inter-layer coupling and observe a field-induced metamagnetic transition. The metamagnetic transition results in magnetoresistances of 95%,…
The magnetic van der Waals crystals MnBi2Te4/(Bi2Te3)n have drawn significant attention due to their rich topological properties and the tunability by external magnetic field. Although the MnBi2Te4/(Bi2Te3)n family have been intensively studied in the past few years, their close relatives, the MnSb2Te4/(Sb2Te3)n family, remain much less explored. In this work, combining magnetotransport measurements, angle-resolved photoemission spectroscopy, and first principles calculations, we find that MnSb4Te7, the n = 1 member of the MnSb2Te4/(Sb2Te3)n family, is a magnetic topological system with versat…
CeTe3 is a unique platform to investigate the itinerant magnetism in a van der Waals (vdW) coupled metal. Despite chemical pressure being a promising route to boost quantum fluctuation in this system, a systematic study on the chemical pressure effect on Ce3+(4f1) states is absent. Here, we report on the successful growth of a series of Se doped single crystals of CeTe3. We found a fluctuation driven exotic magnetic rotation from the usual easy-axis ordering to an unusual hard-axis ordering. Unlike in localized magnetic systems, near-critical magnetism can increase itinerancy hand-in-hand with…
Emergent 3D Fermiology and Magnetism in an Intercalated Van der Waals System
University of L’Aquila（拉奎拉大学）；CNR-SPIN L’Aquila（意大利国家研究委员会自旋物理研究所拉奎拉分部）；Univ Rennes, CNRS, Institut des Sciences Chimiques de Rennes-UMR6226（雷恩大学，法国国家科学研究中心，雷恩化学科学研究所）；Synchrotron SOLEIL（索莱尔同步辐射中心）；CNR-Istituto di Struttura della Materia (CNR-ISM)（意大利国家研究委员会物质结构研究所）；Swiss Light Source, Paul Scherrer Institute（瑞士光源，保罗谢勒研究所）；Deutsches Elektronen-Synchrotron DESY（德国电子同步辐射中心）；MAX IV Laboratory, Lund University（隆德大学马克四实验室）
The relativistic Dirac equation covers the fundamentals of electronic phenomena in solids and as such it effectively describes the electronic states of the topological insulators like Bi$_2$Se$_3$ and Bi$_2$Te$_3$. Topological insulators feature gapless surface states and, moreover, magnetic doping and resultant ferromagnetic ordering break time-reversal symmetry to realize quantum anomalous Hall and Chern insulators. Here we focus on the bulk and investigate the mutual coupling of electronic and magnetic properties of Dirac electrons. Without carrier doping, spiral magnetic orders cause a fer…
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…
As the first intrinsic antiferromagnetic (AFM) topological insulator (TI), MnBi$_2$Te$_4$ has provided a material platform to realize various emergent phenomena arising from the interplay of magnetism and band topology. Here by investigating (Mn$_{1-x}$Pb$_x$)Bi$_2$Te$_4$ $(0\leq x \leq 0.82)$ single crystals via the x-ray, electrical transport, magnetometry and neutron measurements, chemical analysis, external pressure, and first-principles calculations, we reveal the magnetic dilution effect on the magnetism and band topology in MnBi$_2$Te$_4$. With increasing $x$, both lattice parameters $a…
The antiferromagnetic topological insulator has attracted lots of attention recently, as its intrinsic magnetism and topological property makes it a potential material to realize the quantum anomalous Hall effect (QAHE) at relative high temperature. Until now, only MnBi$_2$Te$_4$ is predicted and grown successfully. The other MB$_2$T$_4$-family materials predicted (MB$_2$T$_4$:M=transition-metal or rare-earth element, B=Bi or Sb, T=Te, Se, or S) with not only antiferromagnetic topological property but also rich and exotic topological quantum states and dynamically stable (or metastable) struct…
Metal thio(seleno)phosphates MPX$_3$ have attracted considerable attentions with wide spanned band gaps and rich magnetic properties. In this series, two neighboring members MnPS$_3$ and NiPS$_3$ differ in magnetic atoms, magnetic easy axes, spin anisotropy, as well as nearest-neighbor magnetic interactions. The competition between these components may cause intriguing physical phenomena. In this article, the evolution of magnetism of Mn$_{1-x}$Ni$_x$PS$_3$ series is reported. Despite the incompatible antiferromagnetic orders of two end members, the antiferromagnetism persists as the ground st…
The Mn(Bi$_{1-x}$Sb$_x$)$_2$Te$_4$ series is purported to span from antiferromagnetic (AF) topological insulator at x = 0 to a trivial AF insulator at x = 1. Here we report on neutron diffraction and inelastic neutron scattering studies of the magnetic interactions across this series. All compounds measured possess ferromagnetic (FM) triangular layers and we find a crossover from AF to FM interlayer coupling near x = 1 for our samples. The large spin gap at x = 0 closes rapidly and the average FM exchange interactions within the triangular layer increase with Sb substitution. Similar to a prev…
We have grown a series of nickel substituted single crystals of the layered ferromagnet (FM) Fe$_3$GeTe$_2$. The large single crystalline samples of (Fe$_{1-x}$Ni$_x$)$_3$GeTe$_2$ with $x = 0-0.84$ were characterized with single crystal X-ray diffraction, magnetic susceptibility, electrical resistance and muon spin spectroscopy. We find Fe can be continuously substituted with Ni with only minor structural variation. In addition, FM order is suppressed from $T_\mathrm{C}=212$~K for $x=0$ down to $T_\mathrm{C}=50$~K for $x=0.3$, which is accompanied with a strong suppression of saturated and eff…
The interplay between a multitude of electronic, spin, and lattice degrees of freedom underlies the complex phase diagrams of quantum materials. Layer stacking in van der Waals (vdW) heterostructures is responsible for exotic electronic and magnetic properties, which inspires stacking control of two-dimensional magnetism. Beyond the interplay between stacking order and interlayer magnetism, we discover a spin-shear coupling mechanism in which a subtle shear of the atomic layers can have a profound effect on the intralayer magnetic order in a family of vdW antiferromagnets. Using time-resolved …
Recently, the MnBi$_2$Te$_4$ material has been proposed as the first intrinsic antiferromagnetic topological insulator (AFMTI), where the interplay between magnetism and topology induces several fascinating topological phases, such as the quantum anomalous Hall effect, Majorana fermions, and axion electrodynamics. However, an exactly solvable model being capable to capture the essential physics of the interplay between magnetism and topology is still absent. Here, inspired by the the Ising-like nature [B. Li \textit{et al.} Phys. Rev. Lett. \textbf{124}, 167204 (2020)] and the topological prop…
Comparing with the widely known transitional metal based van der Waals (vdW) materials, rare-earth based ones are rarely explored in the research of intrinsic two-dimensional (2D) magnetism. In this work, we report the physical properties of DyOCl, a rare-earth based vdW magnetic insulator with direct band gap of $\sim 5.72~eV$. The magnetic order of bulk DyOCl is determined by neutron scattering as the $A$-type antiferromagnetic structure below the Néel temperature $T_N=10~$K. The large magnetic moment near 10.1 $ μ_{B} $/Dy lies parallel to the $a$-axis with strong uniaxial magnetic anisotro…
Recent developments in twisted and lattice-mismatched bilayers have revealed a rich phase space of van der Waals systems and generated excitement. Among these systems are heterobilayers which can offer new opportunities to control van der Waals systems with strong in plane correlations such as spin-orbit-assisted Mott insulator $α$-RuCl$_3$. Nevertheless, a theoretical $\textit{ab initio}$ framework for mismatched heterobilayers without even approximate periodicity is sorely lacking. We propose a general strategy for calculating electronic properties of such systems, mismatched interface theor…
