The antiferromagnetic (AF) compound MnBi$_{2}$Te$_{4}$ is suggested to be the first realization of an antiferromagnetic (AF) topological insulator. Here we report on inelastic neutron scattering studies of the magnetic interactions in MnBi$_{2}$Te$_{4}$ that possess ferromagnetic (FM) triangular layers with AF interlayer coupling. The spin waves display a large spin gap and pairwise exchange interactions within the triangular layer are frustrated due to large next-nearest neighbor AF exchange. The degree of frustration suggests proximity to a variety of magnetic phases, potentially including skyrmion phases, that could be accessed in chemically tuned compounds or upon the application of symmetry-breaking fields.
We report measurements on Ti$_4$MnBi$_2$, where a crystal structure involving linear chains of Mn ions suggests one-dimensional magnetic character. The electrical resistivity is metallic, consistent with the results of electronic structure calculations that find a robust Fermi surface albeit with moderate electronic correlations. Curie-Weiss fit to the magnetic susceptibility finds that the Mn moments are in the low-spin $S = 1/2$ configuration. Neutron diffraction measurements detect weak antiferromagnetic order within the Mn chains, with further evidence for the small staggered moment coming…
MnBi$_4$Te$_{7}$ and MnBi$_6$Te$_{10}$ are two members with n=2 and 3 in the family of MnBi$_{2n}$Te$_{3n+1}$ where the n=1 member, MnBi$_2$Te$_{4}$, has been intensively investigated as the first intrinsic antiferromagnetic topological insulator. Here we report the A-type antiferromagnetic order in these two compounds by measuring magnetic properties, electrical and thermal transport, specific heat, and single crystal neutron diffraction. Both compounds order into an A-type antiferromagnetic structure as does MnBi$_2$Te$_{4}$ with ferromagnetic planes coupled antiferromagnetically along the c…
The discovery of an intrinsic antiferromagnetic topological insulator (AFM-TI) in MnBi$_2$Te$_4$ has attracted intense attention, most of which lies on its electrical properties. In this paper, we report electronic, thermal, and thermoelectric transport studies of this newly found AFM-TI. The temperature and magnetic field dependence of its resistivity, thermal conductivity, and Seebeck coefficient indicate strong coupling between charge, lattice, and spin degrees of freedom in this system. Furthermore, MnBi$_2$Te$_4$ exhibits a large anomalous Nernst signal, which is associated with non-zero …
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…
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 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 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…
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 first principles calculations of the dynamic susceptibility in strained and doped ferromagnetic MnBi using time-dependent density functional theory. In spite of being a metal, MnBi exhibits signatures of strong correlation and a proper description in the framework of density functional theory requires Hubbard corrections to the Mn $d$-orbitals. To permit calculations of the dynamic susceptibility with Hubbard corrections applied to the ground state electronic structure, we use a consistent rescaling of the exchange-correlation kernel maintaining the delicate balance between the magn…
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…
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…
MnBi2Te4 has attracted tremendous research interest recently as the first intrinsic antiferromagnetic (AF) topological insulator. It undergoes a long-range AF order at TN = 24 K accompanied with a cusp-like anomaly in the metallic resistivity. Here, we studied the effect of hydrostatic pressure on its electrical transport properties up to 12.5 GPa by using a cubic anvil cell apparatus. We find that TN determined from the resistivity anomaly first increases slightly with pressure and then decreases until vanished completely at ~7 GPa. Intriguingly, its resistivity rho(T) is enhanced gradually b…
The square Bi layers in $A$MnBi$_2$ ($A =$ Sr, Ca) host Dirac fermions which coexist with antiferromagnetic order on the Mn sublattice below $T_\mathrm{N} = 290\,$K (Sr) and $270\,$K (Ca). We have measured the spin-wave dispersion in these materials by triple-axis neutron spectroscopy. The spectra show pronounced spin gaps of 10.2(2)$\,$meV (Sr) and 8.3(8)$\,$meV (Ca) and extend to a maximum energy transfer of 61 - 63$\,$meV. The observed spectra can be accurately reproduced by linear spin-wave theory from an Heisenberg effective spin Hamiltonian. Detailed global fits of the full magnon disper…
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…
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…
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…
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…
Combinations of non-trivial band topology and long-range magnetic order hold promise for realizations of novel spintronic phenomena, such as the quantum anomalous Hall effect and the topological magnetoelectric effect. Following theoretical advances material candidates are emerging. Yet, a compound with a band-inverted electronic structure and an intrinsic net magnetization remains unrealized. MnBi$_2$Te$_4$ is a candidate for the first antiferromagnetic topological insulator and the progenitor of a modular (Bi$_2$Te$_3$)$_n$(MnBi$_2$Te$_4$) series. For $n$ = 1, we confirm a non-stoichiometric…
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…
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 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 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…
Millimeter-sized MnBi$_2$Te$_4$ single crystals are grown out of Bi-Te flux and characterized by measuring magnetic and transport properties, scanning tunneling microscope (STM) and spectroscopy (STS). The magnetic structure of MnBi$_2$Te$_4$ below T$_N$ is determined by powder and single crystal neutron diffraction measurements. Below T$_N$=24\,K, Mn$^{2+}$ moments order ferromagnetically in the \textit{ab} plane but antiferromagnetically along the crystallographic \textit{c} axis. The ordered moment is 4.04(13) $μ_{B}$/Mn at 10\,K and aligned along the crystallographic \textit{c}-axis. The e…
Angle dependent field-driven reorientation transitions in uniaxial antiferromagnet MnBi$_2$Te$_4$ single crystal
Center for Quantum Materials & Devices and College of Physics, Chongqing University（重庆大学量子材料与器件中心及物理学院）；Low Temperature Physics Laboratory, College of Physics, Chongqing University（重庆大学物理学院低温物理实验室）
Magnetic topological insulators (TIs) with nontrivial topological electronic structure and broken time-reversal symmetry exhibit various exotic topological quantum phenomena. The realization of such exotic phenomena at high temperature is one of central topics in this area. We reveal that MnBi6Te10 is a magnetic TI with an antiferromagnetic ground state below 10.8 K whose nontrivial topology is manifested by Dirac-like surface states. The ferromagnetic axion insulator state with Z4 = 2 emerges once spins polarized at field as low as 0.1 T, accompanied with saturated anomalous Hall resistivity …
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 …
We measured the magnetic susceptibilities of Cu$_6$Ge$_6$O$_{18}$-xH$_2$O ($x = 0 \sim 6$). Susceptibility above the antiferromagnetic (AF) transition temperature ($T_{\rm N}$) agrees with susceptibility of the one-dimensional Heisenberg $S = 1/2$ model with competing AF interactions. From the estimated ratio between nearest-neighbor and next-nearest-neighbor AF exchange interactions, the spin system is probably located near a boundary between spin systems with gapless and gapped magnetic excitation. The value of $T_{\rm N}/T_{\rm max}$, where $T_{\rm max}$ is temperature at which the suscepti…
The high-temperature ferromagnet MnBi continues to receive attention as a candidate to replace rare-earth-containing permanent magnets in applications above room temperature. This is due to a high Curie temperature, large magnetic moments, and a coercivity that increases with temperature. The synthesis of MnBi also allows for crystals that are free of interstitial Mn, enabling more direct access to the key interactions underlying the physical properties of binary Mn-based ferromagnets. In this work, we use inelastic neutron scattering to measure the spin waves of MnBi in order to characterize …
We present a detailed study of magnetism in LuFe2O4, combining magnetization measurements with neutron and soft x-ray diffraction. The magnetic phase diagram in the vicinity of T_N involves a metamagnetic transition separating an antiferro- and a ferrimagnetic phase. For both phases the spin structure is refined by neutron diffraction. Observed diffuse magnetic scattering far above T_N is explained in terms of near degeneracy of the magnetic phases.
We investigate the Heisenberg model on a decorated square (Fisher) lattice in the presence of first-neighbor $J_{1}$, second-neighbor $J_{2}$, and third-neighbor $J_{3}$ exchange couplings, with antiferromagnetic $J_{1}$. The classical ground-state phase diagram obtained within a Luttinger-Tisza framework is spanned by two antiferromagnetically ordered phases, and an infinitely degenerate antiferromagnetic chain phase. Employing classical Monte Carlo simulations we show that thermal fluctuations fail to lift the degeneracy of the antiferromagnetic chain phase. Interestingly, the spin-wave spec…
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…
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…
Due to the interaction between topological defects of an order parameter and underlying fermions, the defects can possess induced fermion numbers, leading to several exotic phenomena of fundamental importance to both condensed matter and high energy physics. One of the intriguing outcome of induced fermion number is the presence of fluctuating competing orders inside the core of topological defect. In this regard, the interaction between fermions and skyrmion excitations of antiferromagnetic phase can have important consequence for understanding the global phase diagrams of many condensed matt…
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…
In RBaCo_{2}O_{5+x} compounds (R is rare earth), a ferromagnetic-antiferromagnetic competition is accompanied by a giant magnetoresistance. We study the magnetization of detwinned GdBaCo_{2}O_{5.5} single crystals, and find a remarkable uniaxial anisotropy of Co^{3+} spins which is tightly linked with the chain oxygen ordering in GdO_{0.5} planes. Reflecting the underlying oxygen order, CoO_2 planes also develop a spin-state order consisting of Co^{3+} ions in alternating rows of S=1 and S=0 states. The magnetic structure appears to be composed of weakly coupled ferromagnetic ladders with Isin…
We present a detailed investigation of the magnetic properties of complex vanadium phosphates M(VO)2(PO4)2 (M = Ca, Sr) by means of magnetization, specific heat, 31P NMR measurements, and band structure calculations. Experimental data evidence the presence of ferro- and antiferromagnetic interactions in M(VO)2(PO4)2 resulting in a nearly vanishing Curie-Weiss temperature θ_{CW} < 1 K that contrasts with the maximum of magnetic susceptibility at 3 K. Specific heat and NMR measurements also reveal weak exchange couplings with the thermodynamic energy scale J_c = 10-15 K. Additionally, the reduce…
We study the onset of spin-density wave order in itinerant electron systems via a two-dimensional lattice model amenable to numerically exact, sign-problem-free determinantal quantum Monte Carlo simulations. The finite-temperature phase diagram of the model reveals a dome-shaped $d$-wave superconducting phase near the magnetic quantum phase transition. Above the critical superconducting temperature, we observe an extended fluctuation regime, which manifests itself in the opening of a gap in the electronic density of states and an enhanced diamagnetic response. While charge density wave fluctua…
We study the phase diagram of an effective model of competing nematic and antiferromagnetic orders of interacting electrons on the Bernal-stacked honeycomb bilayer, as relevant for bilayer graphene. In the noninteracting limit, the model features a semimetallic ground state with quadratic band touching points at the Fermi level. Taking the effects of short-range interactions into account, we demonstrate the existence of an extended region in the mean-field phase diagram characterized by coexisting nematic and antiferromagnetic orders. By means of a renormalization group approach, we reveal tha…
It has long been known that two-dimensional metals with antiferromagnetic exchange interactions have a weak-coupling instability to the superconductivity of spin-singlet, d-wave electron pairs. We examine additional possible instabilities in the spin-singlet particle-hole channel, and study their interplay with superconductivity. We perform an unrestricted Hartree-Fock-BCS analysis of bond order parameters in a single band model on the square lattice with nearest-neighbor exchange and repulsion, while neglecting on-site interactions. The dominant particle-hole instability is found to be an inc…
In quantum spin systems, singlet phases often develop in the vicinity of an antiferromagnetic order. Typical settings for such problems arise when itinerant fermions are also present. In this work, we develop a theoretical framework for addressing such competing orders in an itinerant system, described by Dirac fermions strongly coupled to an O(3) nonlinear sigma model. We focus on two spatial dimensions, where upon disordering the antiferromagnetic order by quantum fluctuations the singular tunneling events also known as (anti)hedgehogs can nucleate competing singlet orders in the paramagneti…
