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Single crystal growth, chemical defects, magnetic and transport properties of antiferromagnetic topological insulators ( Ge 1 – δ – x Mn x ) 2 Bi 2 Te 5 ( x ≤ 0.47 , 0.11 ≤ δ ≤ 0.20 )

Magnetic topological insulators provide a platform for emergent phenomena arising from the interplay between magnetism and band topology. Here we report the single crystal growth, crystal structure, magnetic and transport properties, as well as the neutron scattering studies of topological insulator series (Ge 1–δ–x Mn x ) 2 ⁢Bi 2 ⁢Te 5 (x ≤ 0.47, 0.11 ≤ δ ≤ 0.20). Upon doping up to x = 0.47, the lattice parameter c decreases by 0.8%, while the lattice parameter a remains nearly unchanged. Significant Ge vacancies and Ge/Bi site mixing are revealed via elemental analysis as well as refinements of the neutron and x-ray diffraction data, resulting in holes dominating the charge transport. At x = 0.47, below 10.8 K, a bilayer A-type antiferromagnetic ordered state emerges, featuring an ordered moment of 3.0(3) μ B /Mn at 5 K, with the c axis as the easy axis. Magnetization data unveils a much stronger effective interlayer antiferromagnetic exchange interaction and a much smaller uniaxial anisotropy compared to MnBi 2 ⁢Te 4 . We attribute the former to the shorter nearest-neighbor Mn-Mn interlayer superexchange path and the latter to the smaller ligand-field splitting in (Ge 1–δ–x ⁢Mn x ) 2 ⁢Bi 2 ⁢Te 5 . Finally, our study demonstrates that this series of materials holds promise for the investigation of the layer Hall effect and quantum metric nonlinear Hall effect.

36 MATERIALS SCIENCE

Coexistence of ferromagnetism and antiferromagnetic dimers in topological insulators

The addition of magnetic impurities in topological insulators (TIs) can drive ferromagnetic order that leads to quantum anomalous Hall transport well below the Curie temperature. The fragility of the quantized regime has been ascribed to the random nature of the magnetic moment distribution. Here, we refine this hypothesis by using inelastic neutron scattering and density-functional theory calculations to show that two antagonistic components define the magnetism in Mn-substituted SnTe, thereby limiting the effectiveness of dilute magnetic TIs. One component is strongly bound antiferromagnetic dimers that compete with ferromagnetic order. In conclusion, the other component consists of undimerized moments where ferromagnetic order develops via long-range interactions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND

Photogalvanic Effects in Surface States of Topological Insulators under Perpendicular Magnetic Fields

We present a theoretical study of the nonlinear magneto-optical shift conductivity in the surface states of the prototypical topological insulator Bi$_2$Se$_3$ under a perpendicular quantizing magnetic field. By describing the electronic states as Landau levels and using a perturbative approach, we derive the microscopic expression for the shift conductivity $\sigma^{(2);\alpha\beta\gamma}(-\omega,\omega)$, where $\alpha,\beta,\gamma=\pm$ stand for the circular polarization of light and $\omega$ is the light frequency; the spectra are further decomposed into contributions from the interband and intraband optical transitions, for which the selection rules are identified. Considering that the system possesses $C_3$ point group of symmetry, the nonzero components of the conductivity tensor are $\sigma^{(2);-++}=[\sigma^{(2);+--}]^\ast$. Therefore, a pure circularly polarized light generates zero shift current. In the clean limit, the conductivities are nonzero only for discrete photon energies because of the discrete Landau levels and energy conservation, and they become Lorentzian lineshapes with the inclusion of damping, which relaxes the condition of energy conservation. The dependence of the spectra on the damping parameters, the magnetic fields, and the chemical potentials is investigated in detail. Our results reveal that the shift current is highly tunable by the chemical potential and the magnetic field. Furthermore, these results underscore the potential of topological insulators for tunable, strong nonlinear magneto-optical applications.

Landau level

Detecting axion dynamics on the surface of magnetic topological insulators

Axions, initially proposed to solve the strong CP problem, have recently gained attention in condensed matter physics, particularly in topological insulators. However, detecting axion dynamics has proven challenging, with no experimental confirmations to date. In this paper, we identify the surface of magnetic topological insulators as an ideal platform for observing axion dynamics. The vanishing bulk gap at the surface allows for order O(1) variations in the axion field, making the detection of axionlike phenomena more feasible. In contrast, these phenomena are strongly suppressed in the bulk due to the small magnetic exchange gap. We investigate two-photon decay as a signature of axion dynamics and calculate the branching ratio using a perturbative approach. Our findings reveal that the photon flux emitted from the surface is in plane and orders of magnitude larger than that from the bulk, making it detectable with modern microwave technology. We also discuss potential material platforms for detecting axion two-photon decay and strategies to enhance the signal-to-noise ratio.

Gao, Zhi-Qiang

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

Creating and Probing Large Gap 2D Topological Insulators for Quantum Computing (Final Report)

Research under this award focused on experimental and theoretical efforts in developing and characterizing 2D topological insulators (TIs). Key areas of investigation included materials synthesis, device fabrication and characterization, and theoretical advancements. The team synthesized ZrTe 5 , a material with potential for TI phases. Additionally, the team pursued the synthesis of elemental thin films like Indene and Bismuthene, known for their large TI gaps. Indene was successfully stabilized on SiC. Another approach involved stacking and twisting transition metal dichalcogenides (TMDs) to engineer desired TI band structures. On the theoretical front, advancements made under this award predicted remarkable topological properties in twisted WSe2 bilayers, motivating experimental efforts to realize these states. Regarding device fabrication and characterization, significant progress was made in reducing contact resistance, crucial for reliable transport measurements. Contactless Pulsed Tunneling Spectroscopy (CPTS) was employed to study the electronic properties of WTe 2 and WSe 2 . However, challenges in device fabrication and electrode material selection hampered efforts to obtain desired spectra. Ancillary work, utilizing pulsed electrical methods, on the study of sliding ferroelectrics yielded impactful results demonstrating high speed operation and lack of degradation of devices after many billions of cycles.

77 NANOSCIENCE AND NANOTECHNOLOGY

Pressure-induced changes in structure, magnetic order and superconductivity in the ferromagnetic topological insulator MnBi 8 Te 13

Introducing superconductivity (SC) in an intrinsic magnetic topological system remains a significant challenge in modern condensed matter physics. Here, we show that SC can be induced by applying high pressure to a promising ambient-pressure magnetic topological insulator candidate, MnBi 8 Te 13 . Using electrical transport, magnetic susceptibility, and synchrotron x-ray diffraction, we construct a detailed temperature - pressure phase diagram. The ambient-pressure ferromagnetic order is progressively suppressed and replaced by an antiferromagnetic state. Above 16.6 GPa, bulk SC emerges with a critical temperature up to 6.8 K. This pressure-induced SC may co-exist with another AFM dome. In contrast, the related compounds with higher magnetic ion (Mn) concentration show no SC, highlighting the crucial role of Mn concentration in stabilizing SC. The observation of pressure-induced FM-AFM-SC transitions in MnBi 8 Te 13 not only establishes it as a rare Mn-based SC but also provides a platform to study the interplay between magnetism, SC, and potentially nontrivial band topology in correlated magnetic materials.

Huyan, S. [Ames Laboratory, and Iowa State Univ.,

Atomic-Scale Characterization of Dilute Dopants in Topological Insulators via STEM–EDS Using Registration and Cell Averaging Techniques

Magnetic dopants in three-dimensional topological insulators (TIs) offer a promising avenue for realizing the quantum anomalous Hall effect (QAHE) without the necessity for an external magnetic field. Understanding the relationship between site occupancy of magnetic dopant elements and their effect on macroscopic property is crucial for controlling the QAHE. By combining atomic-scale energy-dispersive X-ray spectroscopy (EDS) maps obtained by aberration-corrected scanning transmission electron microscopy (AC-STEM) and novel data processing methodologies, including semi-automatic lattice averaging and frame registration, we have determined the substitutional sites of Mn atoms within the 1.2% Mn-doped Sb 2 Te 3 crystal. More importantly, the methodology developed in this study extends beyond Mn-doped Sb 2 Te 3 to other quantum materials, traditional semiconductors, and even electron irradiation sensitive materials.

36 MATERIALS SCIENCE

Epitaxial 2D Magnet and Topological Insulator Heterostructures

I will discuss our latest advances on the epitaxial growth of 2D van der Waals (vdW) magnets and their integration with topological insulators (TI). This work is motivated by the realization of topological phases such as the quantum anomalous Hall effect and highly efficient spin-orbit torque produced by TIs. Our initial studies of MnSe2 growth on Bi2Se3 showed a tendency for the interdiffusion of Mn into the Bi2Se3. This ultimately led to the synthesis of MnBi2Se4 (MBS), a new magnetic TI. Interestingly, the vdW phase is not the thermodynamically stable phase and bulk crystals do not exist, so the epitaxial stabilization of MBS creates the opportunity to explore the magnetic and topological properties of this material. We find that MBS is a layered antiferromagnet, similar to MnBi2Te4, but a difference is that the magnetic moments lie in the plane of the film. Angle resolved photoemission experiments show the presence of a topological surface state with Dirac dispersion. For bilayers of 2D magnets and TIs, we have developed FGT films on Bi2Te3. We first optimized FGT by studying its growth on Ge(111) substrates, where we find that kinetic considerations play a major role. Using cross-sectional scanning transmission electron microscopy and scanning tunneling microscopy, we optimize the FGT films to have atomically smooth surfaces and abrupt interfaces with the Ge(111). Subsequently, we have developed the growth of FGT on Bi2Te3 for the integration of 2D magnets with Tis. Interestingly, we observe room temperature ferromagnetism in FGT/Bi2Te3 heterostructures by varying the growth conditions.

Kawakami, Roland

Unique optical excitations in topological insulators (Final Technical Report)

The overall objective of this research is to understand how light interacts with topological insulator (TI) films and layered structures. Unlike normal materials, the electrons in TI films are trapped at the top and bottom surfaces of the film. These electrons have unusual properties, including low mass and high velocity. Light shining on these trapped electrons will excite electron density waves, called plasmons, which inherit the unusual properties of the electrons. This project aims to understand how these plasmons interact with each other and how the plasmon properties change as the film dimensions change. By controlling the physical properties of the films, the optical response of the film can also be controlled. In addition to single TI films, the project will also investigate the properties of stacks of TI films layered with normal insulating films. Stacking these materials results in multiple layers of trapped electrons whose plasmons can interact in ever more complex ways. After these interactions are understood, we can begin to engineer complex TI structures to obtain designer optical phenomena in the far-infrared and THz, wavelength ranges of interest for environmental monitoring and chemical sensing. This research directly addresses DOE Grand Challenges, including understanding how properties of matter emerge from complex electronic correlations and learning how to control these properties as well as the mission of the Basic Energy Sciences program to understand and control matter at the electronic/atomic level.

36 MATERIALS SCIENCE

Distinguishing surface and bulk electromagnetism via their dynamics in an intrinsic magnetic topological insulator

The indirect exchange interaction between local magnetic moments via surface electrons has been long predicted to bolster the surface ferromagnetism in magnetic topological insulators (MTIs), which facilitates the quantum anomalous Hall effect. This unconventional effect is critical to determining the operating temperatures of future topotronic devices. However, the experimental confirmation of this mechanism remains elusive, especially in intrinsic MTIs. Here, we combine time-resolved photoemission spectroscopy with time-resolved magneto-optical Kerr effect measurements to elucidate the unique electromagnetism at the surface of an intrinsic MTI MnBi 2 Te 4 . Theoretical modeling based on 2D Ruderman-Kittel-Kasuya-Yosida interactions captures the initial quenching of a surface-rooted exchange gap within a factor of two but overestimates the bulk demagnetization by one order of magnitude. This mechanism directly explains the sizable gap in the quasi-2D electronic state and the nonzero residual magnetization in even-layer MnBi 2 Te 4 . Furthermore, it leads to efficient light-induced demagnetization comparable to state-of-the-art magnetophotonic crystals, promising an effective manipulation of magnetism and topological orders for future topotronics.

74 ATOMIC AND MOLECULAR PHYSICS

Giant spin transport anisotropy in magnetic topological insulators

Here, we report on exceptionally long spin transport and giant spin lifetime anisotropy in the gapped surface states of three-dimensional (3D) magnetic topological insulators (MTIs). We examine the properties of these states using the three-dimensional Fu-Kane-Mele Hamiltonian model in the presence of a magnetic exchange field. The corresponding spin textures of surface states, which are well reproduced by an effective two-band model, hint at a considerable enhancement of the lifetime of out-of-plane spins compared to in-plane spins. This is confirmed by large-scale spin transport simulations for 3D MTIs with disorder. The energy dependence of the spin lifetime anisotropy arises directly from the nontrivial spin texture of the surface states, and is correlated with the onset of the quantum anomalous Hall phase. Our findings suggest different spin filtering capabilities of the gapped surface MTI states, which could be explored by nonlocal spin valve measurements.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND

Reconstructing the Wave Function of Magnetic Topological Insulators MnBi 2 ⁢Te 4 and MnBi 4 ⁢Te 7 Using Spin-Resolved Photoemission

Despite their importance for exotic quantum effects, the surface electronic structure of magnetic topological insulators MnBi 2 ⁢Te 4 and MnBi 4 ⁢Te 7 remains poorly understood. Using high-efficiency spin- and angle-resolved photoemission spectroscopy, we directly image the spin-polarization and orbital character of the surface states in both compounds and map our observations onto a model wave function to describe the complex spin-orbital texture, which solidifies our understanding of the surface band structure by establishing the single-band nature of the most prominent states. Most importantly, our analysis reveals a new mechanism for reducing the magnetic gap of the topological surface states based on the orbital composition of the wave function.

Han, Xue [SLAC National Accelerator Laboratory (SL

Superconducting diode effect in two-dimensional topological insulator edges and Josephson junctions

The superconducting diode effect—the dependence of critical current on its direction—can arise from the simultaneous breaking of inversion and time-reversal symmetry in a superconductor and has gained interest for its potential applications in superconducting electronics. In this Letter, we study the effect in a two-dimensional topological insulator (2D TI) in both a uniform geometry as well as in a long Josephson junction. We show that in the presence of Zeeman fields, a circulating edge current enables a large non-reciprocity of the critical current. We find a maximum diode efficiency of 1 for the uniform 2D TI and (2−1)2≈0.17 for the long Josephson junction.

Physics

Tracing terahertz plasmon polaritons with a tunable-by-design dispersion in topological insulator metaelements

Abstract Collective oscillations of massless charge carriers in two-dimensional materials—Dirac plasmon polaritons (DPPs)—are of paramount importance for engineering nanophotonic devices with tunable optical response. However, tailoring the optical properties of DPPs in a nanomaterial is a very challenging task, particularly at terahertz (THz) frequencies, where the DPP momentum is more than one order of magnitude larger than that of the free-space photons, and DDP attenuation is high. Here, we conceive and demonstrate a strategy to tune the DPP dispersion in topological insulator metamaterials. We engineer laterally coupled linear metaelements, fabricated from epitaxial Bi 2 Se 3, with selected coupling distances with the purpose to tune their wavevector, by geometry. We launch and directly map the propagation of DPPs confined within coupled meta-atoms via phase-sensitive scattering-type scanning near-field nanoscopy. We demonstrate that the DPP wavelength can be tuned by varying the metaelements coupling distance, resulting in up to a 20% increase of the polariton wavevector Re(k p ) in dimers and triplets with a 1 μm spacing, with reduced losses and a >50% increase of the polariton attenuation length.

Optics

Enhanced ferromagnetism in monolayer Cr 2 Te 3 via topological insulator coupling

Exchange-coupled interfaces are pivotal in exploiting two-dimensional (2D) ferromagnetism. Due to the extraordinary correlations among charge, spin, orbital and lattice degrees of freedom, layered magnetic transition metal chalcogenides (TMCs) bode well for exotic topological phenomena. Here we report the realization of wafer-scale Cr 2 Te 3 down to monolayer (ML) on insulating SrTiO 3 (111) and/or Al 2 O 3 (001) substrates using molecular beam epitaxy. Robust ferromagnetism persists in the 2D limit. In particular, the Curie temperature T C of 2 ML Cr 2 Te 3 increases from 100 K to ∼120 K when proximitized to topological insulator (TI) (Bi,Sb) 2 Te 3 , with substantially boosted magnetization as observed via polarized neutron reflectometry. Our experiments and theory strongly indicate that the Bloembergen–Rowland interaction is likely universal underlying T C enhancement in TI-coupled magnetic heterostructures. The topological-surface-enhanced magnetism in 2D TMC enables further exchange coupling physics and quantum hybrid studies, including paving the way to realize interface-modulated topological electronics.

36 MATERIALS SCIENCE

Possible evidence of excitonic condensation in a topological insulator

The transient excitonic condensate is a nonequilibrium electron-hole Bardeen-Cooper-Schrieffer state in a photoexcited semiconductor and semimetal, where electron-hole pairs undergo a phase transition and condense into a single coherent quantum state. Despite numerous experimental works to realize the predicted excitonic condensation phase, experimental evidence still remains elusive. This is largely due to the absence of direct measurements of a material's transient momentum-dependent electronic structure and the excitonic state in the condensation regime. Here, using time and angle-resolved photoemission spectroscopy, we find direct evidence of a transient excitonic condensate in the spin-polarized spatially indirect excitonic topological states in Bi2Te3. Accompanying the formation of the excitonic topological states by photoexcitation, we reveal a splitting of the hole's and electron's quasi-equilibrium chemical potential followed by the band flattening and backbending of the transient topological surface state. Moreover, within the same momentum range, we report a reshaping of the bulk valence band in the form of a Mexican-hat-like Bogoliubov dispersion-hallmarks of the excitonic condensation, followed by the opening of an energy gap at the Fermi level. The fluence and temperature dependence of these renormalization effects are reminiscent of excitonic condensation within Bardeen-Cooper-Schrieffer (BCS)-like behavior. These results, together with theoretical simulation, point to the possible formation of a transient excitonic condensate and provide opportunities to manipulate topologically protected Bose condensates with light.

ARPES