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At least 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Defect-driven ferrimagnetism and hidden magnetization in MnBi 2 Te 4

MnBi 2 Te 4 (MBT) materials are promising antiferromagnetic topological insulators in which field-driven ferromagnetism is predicted to cause a transition between axion insulator and Weyl semimetallic states. However, the presence of antiferromagnetic coupling between Mn/Bi antisite defects and the main Mn layer can reduce the low-field magnetization, and it has been shown that such defects are more prevalent in the structurally identical magnetic insulator MnSb 2 Te 4 (MST). We use high-field magnetization measurements to show that the magnetization of MBT and MST occur in stages and full saturation requires fields of ~60 T. As a consequence, the low-field magnetization plateau state in MBT, where many determinations of the quantum anomalous Hall state are studied, actually consists of ferrimagnetic septuple blocks containing both uniform and staggered magnetization components.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Dynamical piezomagnetic effect in time-reversal-invariant Weyl semimetals with axionic charge density waves

Charge density waves (CDWs) in Weyl semimetals (WSMs) have been shown to induce an exotic axionic insulating phase in which the sliding mode (phason) of the CDW acts as a dynamical axion field, giving rise to a large positive magnetoconductance. In this work, we predict that dynamical strain can induce a bulk orbital magnetization in time-reversal (TR)-invariant WSMs that are gapped by a CDW. Here, we term this effect the “dynamical piezomagnetic effect” (DPME). Unlike in J. Gooth et al., the DPME introduced in this work occurs in a bulk-constant (i.e., static and spatially homogeneous in the bulk) CDW, and does not rely on fluctuations, such as a phason. By studying the low-energy effective theory and a minimal tight-binding (TB) model, we find that the DPME originates from an effective valley axion field that couples the electromagnetic gauge field with a strain-induced pseudogauge field. In particular, whereas the piezoelectric effects studied in previous works are characterized by 2D Berry curvature, the DPME represents the first example of a fundamentally 3D strain effect originating from the Chern-Simons 3-form. We further find that the DPME has a discontinuous change at a critical value of the phase of the CDW order parameter. We demonstrate that, when there is a jump in the DPME, the surface of the system undergoes a topological quantum phase transition (TQPT), while the bulk remains gapped. Hence, the DPME provides a bulk signature of the boundary TQPT in a TR-invariant Weyl CDW.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Layer Hall effect in a 2D topological axion antiferromagnet

While ferromagnets have been known and exploited for millennia, antiferromagnets (AFMs) were only discovered in the 1930s. The elusive nature indicates AFMs' unique properties: At large scale, due to the absence of global magnetization, AFMs may appear to behave like any non-magnetic material; However, such a seemingly mundane macroscopic magnetic property is highly nontrivial at microscopic level, where opposite spin alignment within the AFM unit cell forms a rich internal structure. In topological AFMs, such an internal structure leads to a new possibility, where topology and Berry phase can acquire distinct spatial textures. Here, we study this exciting possibility in an AFM Axion insulator, even-layered MnBi 2 Te 4 flakes, where spatial degrees of freedom correspond to different layers. Remarkably, we report the observation of a new type of Hall effect, the layer Hall effect, where electrons from the top and bottom layers spontaneously deflect in opposite directions. Specifically, under no net electric field, even-layered MnBi 2 Te 4 shows no anomalous Hall effect (AHE); However, applying an electric field isolates the response from one layer and leads to the surprising emergence of a large layer-polarized AHE (~50e 2 /h). Such a layer Hall effect uncovers a highly rare layer-locked Berry curvature, which serves as a unique character of the space-time PT-symmetric AFM topological insulator state. Moreover, we found that the layer-locked Berry curvature can be manipulated by the Axion field, E∙B, which drives the system between the opposite AFM states. Our results achieve previously unavailable pathways to detect and manipulate the rich internal spatial structure of fully-compensated topological AFMs. The layer-locked Berry curvature represents a first step towards spatial engineering of Berry phase, such as through layer-specific moiré potential.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Even–Odd Layer-Dependent Exchange Bias Effect in MnBi 2 Te 4 Chern Insulator Devices

Magnetic topological materials with coexisting magnetism and nontrivial band structures exhibit many novel quantum phenomena, including the quantum anomalous Hall effect, the axion insulator state, and the Weyl semimetal phase. As a stoichiometric layered antiferromagnetic topological insulator, thin films of MnBi 2 Te 4 show fascinating even–odd layer-dependent physics. Here, in this work, we fabricate a series of thin-flake MnBi 2 Te 4 devices using stencil masks and observe the Chern insulator state at high magnetic fields. Upon magnetic field training, a large exchange bias effect is observed in odd but not in even septuple layer (SL) devices. Through theoretical calculations, we attribute the even–odd layer-dependent exchange bias effect to the contrasting surface and bulk magnetic properties of MnBi 2 Te 4 devices. Our findings reveal the microscopic magnetic configuration of MnBi 2 Te 4 thin flakes and highlight the challenges in replicating the zero magnetic field quantum anomalous Hall effect in odd SL MnBi 2 Te 4 devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Metamagnetism of few-layer topological antiferromagnets

MnBi 2 Te 4 (MBT) materials are a promising class of antiferromagnetic topological insulators whose films provide access to novel and technologically important topological phases, including quantum anomalous Hall states and axion insulators. MBT device behavior is expected to be sensitive to the various collinear and noncollinear magnetic phases that are accessible in applied magnetic fields. Here, we use classical Monte Carlo simulations and electronic structure models to calculate the ground state magnetic phase diagram as well as topological and optical properties for few-layer films with up to six septuple layers. Using magnetic interaction parameters appropriate for MBT, we find that it is possible to prepare a variety of different magnetic stacking sequences, some of which have sufficient symmetry to disallow nonreciprocal optical response and Hall transport coefficients. Other stacking arrangements do yield large Faraday and Kerr signals, even when the ground state Chern number vanishes.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Recent progress in MnBi2 n Te3 n +1 intrinsic magnetic topological insulators: crystal growth, magnetism and chemical disorder

ABSTRACT The search for magnetic topological materials has been at the forefront of condensed matter research for their potential to host exotic states such as axion insulators, magnetic Weyl semimetals, Chern insulators, etc. To date, the MnBi2nTe3n+1 family is the only group of materials showcasing van der Waals-layered structures, intrinsic magnetism and non-trivial band topology without trivial bands at the Fermi level. The interplay between magnetism and band topology in this family has led to the proposal of various topological phenomena, including the quantum anomalous Hall effect, quantum spin Hall effect and quantum magnetoelectric effect. Among these, the quantum anomalous Hall effect has been experimentally observed at record-high temperatures, highlighting the unprecedented potential of this family of materials in fundamental science and technological innovation. In this paper, we provide a comprehensive review of the research progress in this intrinsic magnetic topological insulator family, with a focus on single-crystal growth, characterization of chemical disorder, manipulation of magnetism through chemical substitution and external pressure, and important questions that remain to be conclusively answered.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Anti-site defect-induced disorder in compensated topological magnet MnBi2-xSbxTe4

Abstract The gapped Dirac-like surface states of compensated magnetic topological insulator MnBi 2-x Sb x Te 4 (MBST) are a promising host for exotic quantum phenomena such as the quantum anomalous Hall effect and axion insulating state. However, it has become clear that atomic defects undermine the stabilization of such quantum phases as they lead to spatial variations in the surface state gap and doping levels. The large number of possible defect configurations in MBST make studying the influence of individual defects virtually impossible. Here, we present a statistical analysis of the nanoscale effect of defects in MBST with x =0.64, by scanning tunnelling microscopy/spectroscopy. We identify (Bi,Sb) Mn anti-site defects to be the main source of the observed doping fluctuations, leading towards the formation of nanoscale charge puddles and effectively closing the transport gap. Our findings will guide further optimization of this material system via defect engineering, to enable exploitation of its promising properties.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Spin Texture Control and Magnetic Gap Engineering in a Ferromagnetic Insulator–Topological Insulator Sandwiched Heterostructure

Quantum materials that combine magnetism with topological order are emerging as key platforms for next-generation spintronics and low-energy electronics. They enable the realization of emergent quantum phenomena, such as the quantum anomalous Hall effect and axion insulator states. The ferromagnetic insulator (FMI)/topological insulator (TI)/FMI sandwich structure of a single-septuple layer (1SL) MnBi 2 Te 4 /four-quintuple layer (4QL) Bi 2 Te 3 /1SL MnBi 2 Te 4 holds great potential to achieve such desirable quantum phenomena at an elevated temperature, owing to its large Dirac point band gap and high Curie temperature. Here, for this work, spin- and angle-resolved photoemission spectroscopy (spin-ARPES) is employed to directly verify that the band gap arises from broken time-reversal symmetry via proximity-driven magnetization. This study demonstrates direct control of the spin state via external magnetic fields and unambiguously confirms the exchange interaction as the gap-opening mechanism. The robust magnetic gap and controllable spin texture make this heterostructure a suitable candidate for spintronic applications and magnetic topological quantum phases.

exchange gap↗
DOE OSTI2020

Colossal magnetoresistance in a nonsymmorphic antiferromagnetic insulator

Here we investigate antiferromagnetic Eu 5 In 2 Sb 6 , a nonsymmorphic Zintl phase. Our electrical transport data show that Eu 5 In 2 Sb 6 is remarkably insulating and exhibits an exceptionally large negative magnetoresistance, which is consistent with the presence of magnetic polarons. From ab initio calculations, the paramagnetic state of Eu 5 In 2 Sb 6 is a topologically nontrivial semimetal within the generalized gradient approximation (GGA), whereas an insulating state with trivial topological indices is obtained using a modified Becke–Johnson potential. Notably, GGA + U calculations suggest that the antiferromagnetic phase of Eu 5 In 2 Sb 6 may host an axion insulating state. Our results provide important feedback for theories of topological classification and highlight the potential of realizing clean magnetic narrow-gap semiconductors in Zintl materials.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Crossover from 2D Ferromagnetic Insulator to Wide Band Gap Quantum Anomalous Hall Insulator in Ultrathin MnBi 2 Te 4

Intrinsic magnetic topological insulators offer low disorder and large magnetic band gaps 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 realized. Furthermore, these observations occur at temperatures significantly lower than the Néel temperature of bulk MnBi 2 Te 4 , and measurement of the magnetic energy gap at the Dirac point in ultrathin MnBi 2 Te 4 has yet to be achieved. Critical to achieving the promise of this system is a direct measurement of the layer-dependent energy gap and verification of a temperature-dependent topological phase transition from a large band gap QAH insulator to a gapless TI paramagnetic phase. Here we utilize temperature-dependent angle-resolved photoemission spectroscopy to study epitaxial ultrathin MnBi 2 Te 4 . We directly observe a layer-dependent crossover from a 2D ferromagnetic insulator with a band gap greater than 780 meV in one septuple layer (1 SL) to a QAH insulator with a large energy gap (>70 meV) at 8 K in 3 and 5 SL MnBi 2 Te 4 . The QAH gap is confirmed to be magnetic in origin, as it becomes gapless with increasing temperature above 8 K.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Nanoscale Control of Intrinsic Magnetic Topological Insulator MnBi 2 Te 4 Using Molecular Beam Epitaxy: Implications for Defect Control

Intrinsic magnetic topological insulators have emerged as a promising platform to study the interplay between the topological surface states and ferromagnetism. This unique interplay can give rise to a variety of exotic quantum phenomena, including the quantum anomalous Hall effect and axion insulating states. Here, in this study, utilizing molecular beam epitaxy (MBE), we present a comprehensive study of the growth of MnBi 2 Te 4 thin films on Si (111), epitaxial graphene, and highly ordered pyrolytic graphite substrates. By combining a suite of in situ characterization techniques, we obtain critical insights into the nanoscale control of MnBi 2 Te 4 epitaxial growth. First, we extract the free energy landscape for the epitaxial relationship as a function of the in-plane angular distribution. Then, by employing an optimized layer-by-layer growth, we determine the chemical potential and Dirac point of the thin film at different thicknesses and how this quantity is manifested by the dopant compensation from different antisite defects. Overall, these results establish a foundation for understanding the growth kinetics of MnBi 2 Te 4 and pave the way for future applications of MBE-grown thin films in emerging topological quantum materials.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Axion optical induction of antiferromagnetic order

Using circularly polarized light to control quantum matter is a highly intriguing topic in physics, chemistry and biology. Previous studies have demonstrated helicity-dependent optical control of chirality and magnetization, with important implications in asymmetric synthesis in chemistry; homochirality in biomolecules; and ferromagnetic spintronics. We report the surprising observation of helicity-dependent optical control of fully compensated antiferromagnetic order in two-dimensional even-layered MnBi 2 Te 4 , a topological axion insulator with neither chirality nor magnetization. Furthermore, to understand this control, we study an antiferromagnetic circular dichroism, which appears only in reflection but is absent in transmission. We show that the optical control and circular dichroism both arise from the optical axion electrodynamics. Our axion induction provides the possibility to optically control a family of PT-symmetric antiferromagnets (P, inversion; T, time-reversal) such as Cr 2 O 3 , even-layered CrI3 and possibly the pseudo-gap state in cuprates. In MnBi 2 Te 4 , this further opens the door for optical writing of a dissipationless circuit formed by topological edge states.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Recent progress of MnBi 2 Te 4 epitaxial thin films as a platform for realising the quantum anomalous Hall effect

Since the first realisation of the quantum anomalous Hall effect (QAHE) in a dilute magnetic-doped topological insulator thin film in 2013, the quantisation temperature has been limited to less than 1 K due to magnetic disorder in dilute magnetic systems. With magnetic moments ordered into the crystal lattice, the intrinsic magnetic topological insulator MnBi 2 Te 4 has the potential to eliminate or significantly reduce magnetic disorder and improve the quantisation temperature. Surprisingly, to date, the QAHE has yet to be observed in molecular beam epitaxy (MBE)-grown MnBi 2 Te 4 thin films at zero magnetic field, and what leads to the difficulty in quantisation is still an active research area. Although bulk MnBi 2 Te 4 and exfoliated flakes have been well studied, revealing both the QAHE and axion insulator phases, experimental progress on MBE thin films has been slower. Furthermore, understanding how the breakdown of the QAHE occurs in MnBi 2 Te 4 thin films and finding solutions that will enable mass-produced millimetre-size QAHE devices operating at elevated temperatures are required. In this mini-review, we will summarise recent studies on the electronic and magnetic properties of MBE MnBi 2 Te 4 thin films and discuss mechanisms that could explain the failure of the QAHE from the aspects of defects, electronic structure, magnetic order, and consequences of their delicate interplay. Finally, we propose several strategies for realising the QAHE at elevated temperatures in MnBi 2 Te 4 thin films.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Multimodal Approach Reveals the Symmetry-Breaking Pathway to the Broken Helix in EuIn 2 ⁢As 2

Understanding and manipulating emergent phases, which are themes at the forefront of quantum-materials research, rely on identifying their underlying symmetries. This general principle has been particularly prominent in materials with coupled electronic and magnetic degrees of freedom, in which magnetic order influences the electronic band structure and can lead to exotic topological effects. However, identifying symmetry of a magnetically ordered phase can pose a challenge, particularly in the presence of small domains. Here we introduce a multimodal approach for determining magnetic structures, which combines symmetry-sensitive optical probes, scattering, and group-theoretical analysis. We apply it to EuIn 2 ⁢As 2 , a material that has received attention as a candidate axion insulator. While first-principles calculations predict this state on the assumption of a simple collinear antiferromagnetic structure, subsequent neutron-scattering measurements reveal a much more intricate magnetic ground state characterized by two coexisting magnetic wave vectors reached by successive thermal phase transitions. The proposed high- and low-temperature phases are a spin helix and a state with interpenetrating helical and Néel antiferromagnetic order termed a “broken helix,” respectively. Employing a multimodal approach, we identify the magnetic structure associated with these two phases of EuIn 2 ⁢As 2 . We find that the higher-temperature phase is characterized by a variation of the magnetic moment amplitude from layer to layer, with the moment vanishing entirely in every third Eu layer. The lower-temperature structure is similar to the broken helix, with one important difference: Because of local strain, the relative orientation of the magnetic structure and the lattice is not fixed. Consequently, the symmetry required to protect the axion phase is not generically protected in EuIn 2 ⁢As 2 , but we show that it can be restored if the magnetic structure is tuned with uniaxial strain. Finally, we present a spin Hamiltonian that identifies the spin interactions that account for the complex magnetic order in EuIn 2 ⁢As 2 . Our work highlights the importance of a multimodal approach in determining the symmetry of complex order parameters.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Topological Antiferromagnetic Van der Waals Phase in Topological Insulator/Ferromagnet Heterostructures Synthesized by a CMOS-Compatible Sputtering Technique

Breaking time-reversal symmetry by introducing magnetic order, thereby opening a gap in the topological surface state bands, is essential for realizing useful topological properties such as the quantum anomalous Hall and axion insulator states. In this work, a novel topological antiferromagnetic (AFM) phase is created at the interface of a sputtered, c-axis-oriented, topological insulator/ferromagnet heterostructure—Bi 2 Te 3 /Ni 80 Fe 20 because of diffusion of Ni in Bi 2 Te 3 (Ni-Bi 2 Te 3 ). The AFM property of the Ni-Bi2Te3 interfacial layer is established by observation of spontaneous exchange bias in the magnetic hysteresis loop and compensated moments in the depth profile of the magnetization using polarized neutron reflectometry. Analysis of the structural and chemical properties of the Ni-Bi2Te3 layer is carried out using selected-area electron diffraction, electron energy loss spectroscopy, and X-ray photoelectron spectroscopy. These studies, in parallel with first-principles calculations, indicate a solid-state chemical reaction that leads to the formation of Ni=Te bonds and the presence of topological antiferromagnetic (AFM) compound NiBi 2 Te 4 in the Ni-Bi 2 Te 3 interface layer. The Neél temperature of the Ni-Bi 2 Te 3 layer is ≈ 63 K, which is higher than that of typical magnetic topological insulators (MTIs). The presented results provide a pathway toward industrial complementary metal-oxide-semiconductor (CMOS)-process-compatible sputtered-MTI heterostructures, leading to novel materials for topological quantum devices.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Chirality locking charge density waves in a chiral crystal

In Weyl semimetals, charge density wave (CDW) order can spontaneously break the chiral symmetry, gap out the Weyl nodes, and drive the material into the axion insulating phase. Investigations have however been limited since CDWs are rarely seen in Weyl semimetals. Here, using scanning tunneling microscopy/spectroscopy (STM/S), we report the discovery of a novel unidirectional CDW order on the (001) surface of chiral crystal CoSi – a unique Weyl semimetal with unconventional chiral fermions. The CDW is incommensurate with both lattice momentum and crystalline symmetry directions, and exhibits an intra unit cell π phase shift in the layer stacking direction. The tunneling spectrum shows a particle-hole asymmetric V-shaped energy gap around the Fermi level that modulates spatially with the CDW wave vector. Combined with first-principle calculations, we identify that the CDW is locked to the crystal chirality and is related by a mirror reflection between the two enantiomers of the chiral crystal. Our findings reveal a novel correlated topological quantum state in chiral CoSi crystals and raise the potential for exploring the unprecedented physical behaviors of unconventional chiral fermions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Magnetotransport of Sm 2 Ir 2 O 7 across the pressure-induced quantum-critical phase boundary

Rare-earth pyrochlore iridates host two interlocking magnetic sublattices of corner-sharing tetrahedra and can harbour a unique combination of frustrated moments, exotic excitations and highly correlated electrons. They are also the first systems predicted to display both topological Weyl semimetal and axion insulator phases. We have measured the transport and magnetotransport properties of single-crystal Sm 2 Ir 2 O 7 up to and beyond the pressure-induced quantum critical point for all-in-all-out (AIAO) Ir order at p c = 63 kbar previously identified by resonant X-ray scattering and close to which Weyl semimetallic behavior has been previously predicted. Our findings overturn the accepted expectation that the suppression of AIAO order should lead to metallic conduction persisting down to zero temperature. Instead, the resistivity-minimum temperature, which tracks the decrease in the AIAO ordering temperature for pressures up to 30 kbar, begins to increase under further application of pressure, pointing to the presence of a second as-yet unidentified mechanism leading to non-metallic behavior. The magnetotransport does track the suppression of Ir magnetism, however, with a strong hysteresis observed only within the AIAO phase boundary, similar to that found for Ho 2 Ir 2 O 7 and attributed to plastic deformation of Ir domains. Around pc we find the emergence of a new type of electronic phase, characterized by a negative magnetoresistance with small hysteresis at the lowest temperatures, and hysteresis-free positive magnetoresistance above approximately 5K. The temperature dependence of our low-temperature transport data are found to be best described by a model consistent with a Weyl semimetal across the entire pressure range.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Coupled order parameters and photoinduced domain walls in the charge density wave of (TaSe 4 ) 2 I

The charge density wave in (TaSe 4 ) 2 I has drawn much attention recently as a controversial candidate for an axion insulator where the CDW breaks the chiral symmetry of the Weyl semimetal. Here we use ultrafast x-ray scattering to study the collective modes of this CDW. By measuring several diffraction peaks we find that the order parameter involves coupled optical and acoustic modes. For strong near-infrared excitation, the dynamics of the x-ray diffraction show evidence of photoinduced inversion of both components of the CDW order parameter, and associated domain walls. These results demonstrate the potential of ultrafast methods to induce topological defects through highly nonequilibrium dynamics. In (TaSe 4 ) 2 I these defects should lead to exotic electronic states due to the nontrivial topology of the band structure.

36 MATERIALS SCIENCE↗