Magneto-optical Effects of an Artificially Layered Ferromagnetic Topological Insulator with a TC of 160 K.

Magnetic topological insulators are a fertile platform for studying the interplay between magnetism and topology. The unique electronic band structure can induce exotic transport and optical properties. However, a comprehensive optical study at both near-infrared and terahertz frequencies has been lacking. Here, we report magneto-optical effects from a heterostructure of a Cr-incorporated topological insulator, CBST. By measuring the magneto-optical Kerr effect, we observe a high temperature ferromagnetic transition (160 K) in the CBST film. We also use time-domain terahertz polarimetry to reveal a terahertz Faraday rotation of 1.5 mrad and a terahertz Kerr rotation of 3.6 mrad at 2 K. The calculated terahertz Hall conductance is 0.42 e2/h. Our work shows the optical responses of an artificially layered magnetic topological insulator, paving the way toward a high-temperature quantum anomalous Hall effect via heterostructure engineering.

Enhanced Quantum Anomalous Hall Effect with an Active Capping Layer.

The quantum anomalous Hall effect (QAHE) was discovered a decade ago but is still not utilized beyond a handful of research groups, due to numerous limitations such as extremely low temperature, electric-field-effect gating requirement, small sample sizes, and environmental aging effect. Here, we present a robust platform that provides effective solutions to these problems. Specifically, on this platform, we observe QAH signatures at record-high temperatures, with a Hall conductance of 1.00 e2/h at 2.0 K, 0.98 e2/h at 4.2 K, and 0.92 e2/h at 10 K, on centimeter-scale substrates, without electric-field-effect gating. The key ingredient is an active CrOx capping layer, which substantially boosts the ferromagnetism while suppressing environmental degradation. With this development, QAHE will now be accessible to much broader applications than before.

Emergent Magnetism with Continuous Control in the Ultrahigh-Conductivity Layered Oxide PdCoO2.

The current challenge to realizing continuously tunable magnetism lies in our inability to systematically change properties, such as valence, spin, and orbital degrees of freedom, as well as crystallographic geometry. Here, we demonstrate that ferromagnetism can be externally turned on with the application of low-energy helium implantation and can be subsequently erased and returned to the pristine state via annealing. This high level of continuous control is made possible by targeting magnetic metastability in the ultrahigh-conductivity, nonmagnetic layered oxide PdCoO2 where local lattice distortions generated by helium implantation induce the emergence of a net moment on the surrounding transition metal octahedral sites. These highly localized moments communicate through the itinerant metal states, which trigger the onset of percolated long-range ferromagnetism. The ability to continuously tune competing interactions enables tailoring precise magnetic and magnetotransport responses in an ultrahigh-conductivity film and will be critical to applications across spintronics.

Spatial Interactions in Hydrogenated Perovskite Nickelate Synaptic Networks.

A key aspect of how the brain learns and enables decision-making processes is through synaptic interactions. Electrical transmission and communication in a network of synapses are modulated by extracellular fields generated by ionic chemical gradients. Emulating such spatial interactions in synthetic networks can be of potential use for neuromorphic learning and the hardware implementation of artificial intelligence. Here, we demonstrate that in a network of hydrogen-doped perovskite nickelate devices, electric bias across a single junction can tune the coupling strength between the neighboring cells. Electrical transport measurements and spatially resolved diffraction and nanoprobe X-ray and scanning microwave impedance spectroscopic studies suggest that graded proton distribution in the inhomogeneous medium of hydrogen-doped nickelate film enables this behavior. We further demonstrate signal integration through the coupling of various junctions.

Superconducting Fourfold Fe(Te,Se) Film on Sixfold Magnetic MnTe via Hybrid Symmetry Epitaxy.

Epitaxial Fe(Te,Se) thin films have been grown on various substrates but never been grown on magnetic layers. Here we report the epitaxial growth of fourfold Fe(Te,Se) film on a sixfold antiferromagnetic insulator, MnTe. The Fe(Te,Se)/MnTe heterostructure shows a clear superconducting transition at around 11 K, and the critical magnetic field measurement suggests the origin of the superconductivity to be bulk-like. Structural characterizations suggest that the uniaxial lattice match between Fe(Te,Se) and MnTe allows a hybrid symmetry epitaxy mode, which was recently discovered between Fe(Te,Se) and Bi2Te3. Furthermore, the Te/Fe flux ratio during deposition of the Fe(Te,Se) layer is found to be critical for its superconductivity. Now that superconducting Fe(Te,Se) can be grown on two related hexagonal platforms, Bi2Te3 and MnTe, this result opens a new possibility of combining topological superconductivity of Fe(Te,Se) with the rich physics in the intrinsic magnetic topological materials (MnTe)n(Bi2Te3)m family.

Spacer-Layer-Tunable Magnetism and High-Field Topological Hall Effect in Topological Insulator Heterostructures.

Controlling magnetic order in magnetic topological insulators (MTIs) is a key to developing spintronic applications with MTIs and is commonly achieved by changing the magnetic doping concentration, which inevitably affects the spin-orbit coupling strength and the topological properties. Here, we demonstrate tunable magnetic properties in topological heterostructures over a wide range, from a ferromagnetic phase with a Curie temperature of around 100 K all the way to a paramagnetic phase, while keeping the overall chemical composition the same, by controlling the thickness of nonmagnetic spacer layers between two atomically thin magnetic layers. This work showcases that spacer-layer control is a powerful tool to manipulate magneto-topological functionalities in MTI heterostructures. Furthermore, the interaction between the MTI and the Cr2O3 buffer layers also leads to a robust topological Hall effect surviving up to a record-high 6 T of magnetic field, shedding light on the critical role of interfacial layers in thin-film topological materials.

Hybrid Symmetry Epitaxy of the Superconducting Fe(Te,Se) Film on a Topological Insulator.

It is challenging to grow an epitaxial 4-fold compound superconductor (SC) on a 6-fold topological insulator (TI) platform due to the stringent lattice-matching requirement. Here, we demonstrate that Fe(Te,Se) can grow epitaxially on a TI (Bi2Te3) layer due to accidental, uniaxial lattice match, which is dubbed as "hybrid symmetry epitaxy". This new growth mode is critical to stabilizing robust superconductivity with TC as high as 13 K. Furthermore, the superconductivity in this FeTe1-xSex/Bi2Te3 system survives in the Te-rich phase with Se content as low as x = 0.03 but vanishes at Se content above x = 0.56, exhibiting a phase diagram that is quite different from that of the conventional Fe(Te,Se) systems. This unique heterostructure platform that can be formed in both TI-on-SC and SC-on-TI sequences opens a route to unprecedented topological heterostructures.

Electron-Hole Asymmetry of Surface States in Topological Insulator Sb2Te3 Thin Films Revealed by Magneto-Infrared Spectroscopy.

When surface states (SSs) form in topological insulators (TIs), they inherit the properties of bulk bands, including the electron-hole (e-h) asymmetry but with much more profound impacts. Here via combining magneto-infrared spectroscopy with theoretical analysis, we show that e-h asymmetry significantly modifies the SS electronic structures when interplaying with the quantum confinement effect. Compared with the case without e-h asymmetry, the SSs now bear not only a band asymmetry, such as that in the bulk, but also a shift of the Dirac point relative to the bulk bands and a reduction of the hybridization gap of up to 70%. Our results signify the importance of e-h asymmetry in the band engineering of TIs in the thin-film limit.

Ferromagnetic Anomalous Hall Effect in Cr-Doped Bi2Se3 Thin Films via Surface-State Engineering.

The anomalous Hall effect (AHE) is a nonlinear Hall effect appearing in magnetic conductors, boosted by internal magnetism beyond what is expected from the ordinary Hall effect. With the recent discovery of the quantized version of the AHE, the quantum anomalous Hall effect (QAHE), in Cr- or V-doped topological insulator (TI) (Sb,Bi)2Te3 thin films, the AHE in magnetic TIs has been attracting significant interest. However, one of the puzzles in this system has been that while Cr- or V-doped (Sb,Bi)2Te3 and V-doped Bi2Se3 exhibit AHE, Cr-doped Bi2Se3 has failed to exhibit even ferromagnetic AHE, the expected predecessor to the QAHE, though it is the first material predicted to exhibit the QAHE. Here, we have successfully implemented ferromagnetic AHE in Cr-doped Bi2Se3 thin films by utilizing a surface state engineering scheme. Surprisingly, the observed ferromagnetic AHE in the Cr-doped Bi2Se3 thin films exhibited only a positive slope regardless of the carrier type. We show that this sign problem can be explained by the intrinsic Berry curvature of the system as calculated from a tight-binding model combined with a first-principles method.

Engineering Topological Superlattices and Phase Diagrams.

The search for new topological materials and states of matter is presently at the forefront of quantum materials research. One powerful approach to novel topological phases beyond the thermodynamic space is to combine different topological/functional materials into a single materials platform in the form of superlattices. However, despite some previous efforts there has been a significant gap between theories and experiments in this direction. Here, we provide the first detailed set of experimentally verifiable phase diagrams of topological superlattices composed of archetypal topological insulator, Bi2Se3, and normal insulator, In2Se3, by combining molecular-level materials control, low-temperature magnetotransport measurements, and field theoretical calculations. We show how the electronic properties of topological superlattices evolve with unit-layer thicknesses and utilize the weak antilocalization effect as a tool to gain quantitative insights into the evolution of conducting channels within each set of heterostructures. This orchestrated study opens the door to the possibility of creating a variety of artificial-topological-phases by combining topological materials with various other functional building blocks such as superconductors and magnetic materials.

Record High-Proximity-Induced Anomalous Hall Effect in (BixSb1-x)2Te3 Thin Film Grown on CrGeTe3 Substrate.

Quantum anomalous Hall effect (QAHE) can only be realized at extremely low temperatures in magnetically doped topological insulators (TIs) due to limitations inherent with the doping process. In an effort to boost the quantization temperature of QAHE, the magnetic proximity effect in magnetic insulator/TI heterostructures has been extensively investigated. However, the observed anomalous Hall resistance has never been more than several ohms, presumably owing to the interfacial disorders caused by the structural and chemical mismatch. Here, we show that, by growing (BixSb1-x)2Te3 (BST) thin films on structurally and chemically well-matched, ferromagnetic-insulating CrGeTe3 (CGT) substrates, the proximity-induced anomalous Hall resistance can be enhanced by more than an order of magnitude. This sheds light on the importance of structural and chemical matches for magnetic insulator/TI proximity systems.

Solution to the Hole-Doping Problem and Tunable Quantum Hall Effect in Bi2Se3 Thin Films.

Bi2Se3, one of the most widely studied topological insulators (TIs), is naturally electron-doped due to n-type native defects. However, many years of efforts to achieve p-type Bi2Se3 thin films have failed so far. Here, we provide a solution to this long-standing problem, showing that the main culprit has been the high density of interfacial defects. By suppressing these defects through an interfacial engineering scheme, we have successfully implemented p-type Bi2Se3 thin films down to the thinnest topological regime. On this platform, we present the first tunable quantum Hall effect (QHE) study in Bi2Se3 thin films and reveal not only significantly asymmetric QHE signatures across the Dirac point but also the presence of competing anomalous states near the zeroth Landau level. The availability of doping tunable Bi2Se3 thin films will now make it possible to implement various topological quantum devices, previously inaccessible.

Control over Electron-Phonon Interaction by Dirac Plasmon Engineering in the Bi2Se3 Topological Insulator.

Understanding the mutual interaction between electronic excitations and lattice vibrations is key for understanding electronic transport and optoelectronic phenomena. Dynamic manipulation of such interaction is elusive because it requires varying the material composition on the atomic level. In turn, recent studies on topological insulators (TIs) have revealed the coexistence of a strong phonon resonance and topologically protected Dirac plasmon, both in the terahertz (THz) frequency range. Here, using these intrinsic characteristics of TIs, we demonstrate a new methodology for controlling electron-phonon interaction by lithographically engineered Dirac surface plasmons in the Bi2Se3 TI. Through a series of time-domain and time-resolved ultrafast THz measurements, we show that, when the Dirac plasmon energy is less than the TI phonon energy, the electron-phonon coupling is trivial, exhibiting phonon broadening associated with Landau damping. In contrast, when the Dirac plasmon energy exceeds that of the phonon resonance, we observe suppressed electron-phonon interaction leading to unexpected phonon stiffening. Time-dependent analysis of the Dirac plasmon behavior, phonon broadening, and phonon stiffening reveals a transition between the distinct dynamics corresponding to the two regimes as the Dirac plasmon resonance moves across the TI phonon resonance, which demonstrates the capability of Dirac plasmon control. Our results suggest that the engineering of Dirac plasmons provides a new alternative for controlling the dynamic interaction between Dirac carriers and phonons.

Infrared Spectroscopy of the Topological Surface States of Bi_{2}Se_{3} by Use of the Berreman Effect.

The Berreman effect (BE) allows one to study the electrodynamics of ultrathin conducting films at the surface of dielectrics by use of grazing-angle infrared spectroscopy and polarized radiation. Here, we first apply the BE to the two-dimensional electron system (2DES) at the interface between a high-purity film of the topological insulator Bi_{2}Se_{3} and its sapphire substrate. We determine for the 2DES a charge density n_{s}=(8±1)×10^{12} cm^{-2}, a thickness d=0.6±0.2 nm, and a mobility µ^{IR}=290±30 cm^{2}/V s. Within errors, all of these parameters result in being independent of temperature between 300 and 10 K. These findings consistently indicate that the 2DES is formed by topological surface states, whose infrared response is then directly observed here.

Finite-Size and Composition-Driven Topological Phase Transition in (Bi1-xInx)2Se3 Thin Films.

In a topological insulator (TI), if its spin-orbit coupling (SOC) strength is gradually reduced, the TI eventually transforms into a trivial insulator beyond a critical point of SOC, at which point the bulk gap closes: this is the standard description of the topological phase transition (TPT). However, this description of TPT, driven solely by the SOC (or something equivalent) and followed by closing and reopening of the bulk band gap, is valid only for infinite-size samples, and little is known how TPT occurs for finite-size samples. Here, using both systematic transport measurements on interface-engineered (Bi1-xInx)2Se3 thin films and theoretical simulations (with animations in the Supporting Information), we show that description of TPT in finite-size samples needs to be substantially modified from the conventional picture of TPT due to surface-state hybridization and bulk confinement effects. We also show that the finite-size TPT is composed of two separate transitions, topological-normal transition (TNT) and metal-insulator transition (MIT), by providing a detailed phase diagram in the two-dimensional phase space of sample size and SOC strength.

Resonance effects in thickness-dependent ultrafast carrier and phonon dynamics of topological insulator Bi2Se3.

Resonance effects in the thickness-dependent ultrafast carrier and phonon dynamics of topological insulator Bi2Se3 are found irrespective of the kind of substrate by measuring thickness-dependent abrupt changes of pump-probe differential-reflectivity signals (ΔR/R) from Bi2Se3 thin films on four different substrates of poly- and single-crystalline (sc-) ZnO, sc-GaN and SiO2. The absolute peak intensity of the ΔR/R is maximized at ∼t C (6 ∼ 9 quintuple layers), which is not directly related to but is very close to the critical thickness below which the energy gap opens. The intensities of the two phonon modes deduced from the oscillatory behaviors superimposed on the ΔR/R profiles are also peaked at ∼t C for the four kinds of substrates, consistent with the thickness-dependent Raman-scattering behaviors. These resonant effects and others are discussed based on possible physical mechanisms including the effects of three-dimensional carrier depletion and intersurface coupling.

Record Surface State Mobility and Quantum Hall Effect in Topological Insulator Thin Films via Interface Engineering.

Material defects remain as the main bottleneck to the progress of topological insulators (TIs). In particular, efforts to achieve thin TI samples with dominant surface transport have always led to increased defects and degraded mobilities, thus making it difficult to probe the quantum regime of the topological surface states. Here, by utilizing a novel buffer layer scheme composed of an In2Se3/(Bi0.5In0.5)2Se3 heterostructure, we introduce a quantum generation of Bi2Se3 films with an order of magnitude enhanced mobilities than before. This scheme has led to the first observation of the quantum Hall effect in Bi2Se3.

Topological Surface States Originated Spin-Orbit Torques in Bi(2)Se(3).

The three dimensional topological insulator bismuth selenide (Bi(2)Se(3)) is expected to possess strong spin-orbit coupling and spin-textured topological surface states and, thus, exhibit a high charge to spin current conversion efficiency. We evaluate spin-orbit torques in Bi(2)Se(3)/Co(40)Fe(40)B(20) devices at different temperatures by spin torque ferromagnetic resonance measurements. As the temperature decreases, the spin-orbit torque ratio increases from ∼0.047 at 300 K to ∼0.42 below 50 K. Moreover, we observe a significant out-of-plane torque at low temperatures. Detailed analysis indicates that the origin of the observed spin-orbit torques is topological surface states in Bi(2)Se(3). Our results suggest that topological insulators with strong spin-orbit coupling could be promising candidates as highly efficient spin current sources for exploring the next generation of spintronic applications.

Transferring MBE-grown topological insulator films to arbitrary substrates and metal-insulator transition via Dirac gap.

Mechanical exfoliation of bulk crystals has been widely used to obtain thin topological insulator (TI) flakes for device fabrication. However, such a process produces only microsized flakes that are highly irregular in shape and thickness. In this work, we developed a process to transfer the entire area of TI Bi2Se3 thin films grown epitaxially on Al2O3 and SiO2 to arbitrary substrates, maintaining their pristine morphology and crystallinity. Transport measurements show that these transferred films have lower carrier concentrations and comparable or higher mobilities than before the transfer. Furthermore, using this process we demonstrated a clear metal-insulator transition in an ultrathin Bi2Se3 film by gate-tuning its Fermi level into the hybridization gap formed at the Dirac point. The ability to transfer large area TI films to any substrate will facilitate fabrication of TI heterostructure devices, which will help explore exotic phenomena such as Majorana fermions and topological magnetoelectricity.