Tuning Displacement Fields in a Two-Dimensional Topological Insulator Using Nanopatterned Gates.

Epitaxial heterostructures with topological insulators enable novel quantum phases and practical device applications. Their topological electronic states are sensitive to the microscopic parameters, including structural inversion asymmetry (SIA), which is an inherent feature of many real heterostructures. Controlling SIA is challenging, because it requires the ability to tune the displacement field across the topological film. Here, using nanopatterned gates, we demonstrate a tunable displacement field in a heterostructure of the two-dimensional topological insulator cadmium arsenide. Transport studies in magnetic fields reveal an extreme sensitivity of the band inversion to SIA. We show that a relatively small displacement field (∼50 mV/nm) converts the crossing of the two zeroth Landau levels in magnetic field to an avoided crossing, signaling a change to trivial band order. This work demonstrates a universal methodology for tuning electronic states in topological thin films.

Anomalous Hall Transport by Optically Injected Isospin Degree of Freedom in Dirac Semimetal Thin Film.

Chirality of massless fermions emerging in condensed matter is a key to understand their characteristic behavior as well as to exploit their functionality. However, the chiral nature of massless fermions in Dirac semimetals has remained elusive, due to equivalent occupation of carriers with the opposite chirality in thermal equilibrium. Here, we show that the isospin degree of freedom, which labels the chirality of massless carriers from a crystallographic point of view, can be injected by circularly polarized light. Terahertz Faraday rotation spectroscopy successfully detects the anomalous Hall conductivity by a light-induced isospin polarization in a three-dimensional Dirac semimetal, Cd3As2. Spectral analysis of the Hall conductivity reveals a long scattering time and a long decay time, which are characteristic of the isospin. The long-lived, robust, and reversible character of the isospin promises a potential application of Dirac semimetals in future information technology.

Edge Channel Transmission through a Quantum Point Contact in the Two-Dimensional Topological Insulator Cadmium Arsenide.

Cadmium arsenide (Cd3As2) thin films feature a two-dimensional topological insulator (2D TI) phase for certain thicknesses, which theoretically hosts a set of counterpropagating helical edge states that are characteristic of a quantum spin Hall (QSH) insulator. In devices containing electrostatically defined junctions and for magnetic fields below a critical value, chiral edge modes of the quantum Hall effect can coexist with QSH-like edge modes. In this work, we use a quantum point contact (QPC) device to characterize edge modes in the 2D TI phase of Cd3As2 and to understand how they can be controllably transmitted, which is important for use in future quantum interference devices. We investigate equilibration among both types of modes and find non-spin-selective equilibration. We also demonstrate the effect of the magnetic field on suppressing equilibration. We discuss the potential role of QSH-like modes in a transmission pathway that precludes full pinch-off.

Zeeman Field-Induced Two-Dimensional Weyl Semimetal Phase in Cadmium Arsenide.

We report a topological phase transition in quantum-confined cadmium arsenide (Cd_{3}As_{2}) thin films under an in-plane Zeeman field when the Fermi level is tuned into the topological gap via an electric field. Symmetry considerations in this case predict the appearance of a two-dimensional Weyl semimetal (2D WSM), with a pair of Weyl nodes of opposite chirality at charge neutrality that are protected by space-time inversion (C_{2}T) symmetry. We show that the 2D WSM phase displays unique transport signatures, including saturated resistivities on the order of h/e^{2} that persist over a range of in-plane magnetic fields. Moreover, applying a small out-of-plane magnetic field, while keeping the in-plane field within the stability range of the 2D WSM phase, gives rise to a well-developed odd integer quantum Hall effect, characteristic of degenerate, massive Weyl fermions. A minimal four-band k·p model of Cd_{3}As_{2}, which incorporates first-principles effective g factors, qualitatively explains our findings.

Two-Dimensional Topological Insulator State in Cadmium Arsenide Thin Films.

Two-dimensional topological insulators (2D TIs) are a highly desired quantum phase but few materials have demonstrated clear signatures of a 2D TI state. It has been predicted that 2D TIs can be created from thin films of three-dimensional TIs by reducing the film thickness until the surface states hybridize. Here, we employ this technique to report the first observation of a 2D TI state in epitaxial thin films of cadmium arsenide, a prototype Dirac semimetal in bulk form. Using magnetotransport measurements with electrostatic gating, we observe a Landau level spectrum and quantum Hall effect that are in excellent agreement with those of an ideal 2D TI. Specifically, we observe a crossing of the zeroth Landau levels at a critical magnetic field. We show that the film thickness can be used to tune the critical magnetic field. Moreover, a larger change in film thickness causes a transition from a 2D TI to a 2D trivial insulator, just as predicted by theory. The high degree of tunability available in epitaxial cadmium arsenide heterostructures can thus be used to fine-tune the 2D TI, which is essential for future topological devices.

Disentangling the Competing Mechanisms of Light-Induced Anomalous Hall Conductivity in Three-Dimensional Dirac Semimetal.

We experimentally elucidate the origin of the anomalous Hall conductivity in a three-dimensional Dirac semimetal, Cd_{3}As_{2}, driven by circularly polarized light. Using time-resolved terahertz Faraday rotation spectroscopy, we determine the transient Hall conductivity spectrum with special attention to its sign. Our results clearly show the dominance of direct photocurrent generation assisted by the terahertz electric field. The contribution from the Floquet-Weyl nodes is found to be minor when the driving light is in resonance with interband transitions. We develop a generally applicable classification of microscopic mechanisms of light-induced anomalous Hall conductivity.

Tracking Ultrafast Change of Multiterahertz Broadband Response Functions in a Photoexcited Dirac Semimetal Cd3As2 Thin Film.

The electromagnetic response of Dirac semimetals in the infrared and terahertz frequency ranges is attracting growing interest for potential applications in optoelectronics and nonlinear optics. The interplay between the free-carrier response and interband transitions in the gapless, linear dispersion relation plays a key role in enabling novel functionalities. Here we investigate ultrafast dynamics in thin films of a photoexcited Dirac semimetal Cd3As2 by probing the broadband response functions as complex quantities in the multiterahertz region (10-45 THz, 40-180 meV, or 7-30 µm), which covers the crossover between the inter- and intraband response. We resolve dynamics of the photoexcited nonthermal electrons, which merge with originally existing carriers to form a single thermalized electron gas and how it is facilitated by high-density excitation. We also demonstrate that a large reduction of the refractive index by 80% dominates the nonequilibrium infrared response, which can be utilized for designing ultrafast switches in active optoelectronics.

Stimulated Rayleigh Scattering Enhanced by a Longitudinal Plasma Mode in a Periodically Driven Dirac Semimetal Cd_{3}As_{2}.

Using broadband (12-45 THz) multi-terahertz spectroscopy, we show that stimulated Rayleigh scattering dominates the transient optical conductivity of cadmium arsenide, a Dirac semimetal, under an optical driving field at 30 THz. The characteristic dispersive line shape with net optical gain is accounted for by optical transitions between light-induced Floquet subbands, strikingly enhanced by the longitudinal plasma mode. Stimulated Rayleigh scattering with an unprecedentedly large refractive index change may pave the way for slow light generation in conductive solids at room temperature.

Polar Nanodomains in a Ferroelectric Superconductor.

The mechanisms by which itinerant carriers compete with polar crystal distortions are a key unresolved issue for polar superconductors, which offer new routes to unconventional Cooper pairing. Strained, doped SrTiO3 films undergo successive ferroelectric and superconducting transitions, making them ideal candidates to elucidate the nature of this competition. Here, we reveal these interactions using scanning transmission electron microscopy studies of the evolution of polar nanodomains as a function of doping. These nanodomains are a precursor to the ferroelectric phase and a measure of long-range Coulomb interactions. With increasing doping, the magnitude of the polar displacements, the nanodomain size, and the Curie temperature are systematically suppressed. In addition, we show that disorder caused by the dopant atoms themselves presents a second contribution to the destabilization of the ferroelectric state. The results provide evidence for two distinct mechanisms that suppress the polar transition with doping in a ferroelectric superconductor.

Order-Disorder Ferroelectric Transition of Strained SrTiO_{3}.

SrTiO_{3} is an incipient ferroelectric that is believed to exhibit a prototype displacive, soft mode ferroelectric transition when subjected to mechanical stress or alloying. We use high-angle annular dark-field imaging in scanning transmission electron microscopy to reveal local polar regions in the room-temperature, paraelectric phase of strained SrTiO_{3} films, which undergo a ferroelectric transition at low temperatures. These films contain nanometer-sized domains in which the Ti columns are displaced. In contrast, these nanodomains are absent in unstrained films, which do not become ferroelectric. The results show that the ferroelectric transition of strained SrTiO_{3} is an order-disorder transition. We discuss the impact of the results on the nature of the ferroelectric transition of SrTiO_{3}.

Efficient Terahertz Harmonic Generation with Coherent Acceleration of Electrons in the Dirac Semimetal Cd_{3}As_{2}.

We report strong terahertz (∼10^{12} Hz) high harmonic generation at room temperature in thin films of Cd_{3}As_{2}, a three-dimensional Dirac semimetal. Third harmonics are detectable with a tabletop light source and can be as strong as 100 V/cm by applying a fundamental field of 6.5 kV/cm inside the film, demonstrating an unprecedented efficiency for terahertz frequency conversion. Our time-resolved terahertz spectroscopy and calculations also clarify the microscopic mechanism of the nonlinearity originating in the coherent acceleration of Dirac electrons in momentum space. Our results provide clear insights for nonlinear currents of Dirac electrons driven by the terahertz field under the influence of scattering, paving the way toward novel devices for high-speed electronics and photonics based on topological semimetals.

Non-Fermi liquids in oxide heterostructures.

Understanding the anomalous transport properties of strongly correlated materials is one of the most formidable challenges in condensed matter physics. For example, one encounters metal-insulator transitions, deviations from Landau Fermi liquid behavior, longitudinal and Hall scattering rate separation, a pseudogap phase, and bad metal behavior. These properties have been studied extensively in bulk materials, such as the unconventional superconductors and heavy fermion systems. Oxide heterostructures have recently emerged as new platforms to probe, control, and understand strong correlation phenomena. This article focuses on unconventional transport phenomena in oxide thin film systems. We use specific systems as examples, namely charge carriers in SrTiO3 layers and interfaces with SrTiO3, and strained rare earth nickelate thin films. While doped SrTiO3 layers appear to be a well behaved, though complex, electron gas or Fermi liquid, the rare earth nickelates are a highly correlated electron system that may be classified as a non-Fermi liquid. We discuss insights into the underlying physics that can be gained from studying the emergence of non-Fermi liquid behavior as a function of the heterostructure parameters. We also discuss the role of lattice symmetry and disorder in phenomena such as metal-insulator transitions in strongly correlated heterostructures.

Observation of the Quantum Hall Effect in Confined Films of the Three-Dimensional Dirac Semimetal Cd_{3}As_{2}.

The magnetotransport properties of epitaxial films of Cd_{3}As_{2}, a paradigm three-dimensional Dirac semimetal, are investigated. We show that an energy gap opens in the bulk electronic states of sufficiently thin films and, at low temperatures, carriers residing in surface states dominate the electrical transport. The carriers in these states are sufficiently mobile to give rise to a quantized Hall effect. The sharp quantization demonstrates surface transport that is virtually free of parasitic bulk conduction and paves the way for novel quantum transport studies in this class of topological materials. Our results also demonstrate that heterostructuring approaches can be used to study and engineer quantum states in topological semimetals.

Novel Metal-Insulator Transition at the SmTiO_{3}/SrTiO_{3} Interface.

We report on a metal-insulator transition (MIT) that is observed in an electron system at the SmTiO_{3}/SrTiO_{3} interface. This MIT is characterized by an abrupt transition at a critical temperature, below which the resistance changes by more than an order of magnitude. The temperature of the transition systematically depends on the carrier density, which is tuned from ∼1×10^{14} to 3×10^{14} cm^{-2} by changing the SmTiO_{3} thickness. An analysis of the transport properties shows non-Fermi-liquid behavior and mass enhancement as the carrier density is lowered. We compare the MIT characteristics with those of known MITs in other material systems and show that they are distinctly different in several aspects. We tentatively conclude that both long-range Coulomb interactions and the fixed charge at the polar interface are likely to play a role in this MIT. The strong dependence on the carrier density makes this MIT of interest for field-tunable devices.

Response of the Lattice across the Filling-Controlled Mott Metal-Insulator Transition of a Rare Earth Titanate.

The lattice response of a prototype Mott insulator, SmTiO_{3}, to hole doping is investigated with atomic-scale spatial resolution. SmTiO_{3} films are doped with Sr on the Sm site with concentrations that span the insulating and metallic sides of the filling-controlled Mott metal-insulator transition (MIT). The GdFeO_{3}-type distortions are investigated using an atomic resolution scanning transmission electron microscopy technique that can resolve small lattice distortions with picometer precision. We show that these distortions are gradually and uniformly reduced as the Sr concentration is increased without any phase separation. Significant distortions persist into the metallic state. The results present a new picture of the physics of this prototype filling-controlled MIT, which is discussed.

Probing the Metal-Insulator Transition in BaTiO_{3} by Electrostatic Doping.

The metal-to-insulator transition in BaTiO_{3} is investigated using electrostatic doping, which avoids effects from disorder and strain that would accompany chemical doping. SmTiO_{3}/BaTiO_{3}/SrTiO_{3} heterostructures are doped with a constant sheet carrier density of 3×10^{14} cm^{-2} that is introduced via the polar SmTiO_{3}/BaTiO_{3} interface. Below a critical BaTiO_{3} thickness, the structures exhibit metallic behavior with high carrier mobilities at low temperatures, similar to SmTiO_{3}/SrTiO_{3} interfaces. Above this thickness, data indicate that the BaTiO_{3} layer becomes ferroelectric. The BaTiO_{3} lattice parameters increase to a value consistent with a strained, tetragonal unit cell, the structures are insulating below ∼125 K, and the mobility drops by more than an order of magnitude, indicating self-trapping of carriers. The results shed light on the interplay between charge carriers and ferroelectricity.

Pseudogaps and Emergence of Coherence in Two-Dimensional Electron Liquids in SrTiO_{3}.

Using tunneling spectroscopy, we show that pseudogaps emerge in strongly correlated, two-dimensional electron liquids in SrTiO_{3} quantum wells that are tuned near a quantum critical point. Coherence peaks emerge at low temperatures in quantum wells embedded in antiferromagnetic SmTiO_{3} that remain itinerant to the lowest thickness. Quantum wells embedded in ferrimagnetic GdTiO_{3} that become ferromagnetic at low temperatures show no indication of quasiparticle coherence. They undergo a symmetry-lowering metal-to-insulator transition at the lowest thicknesses that coincides with a vanishing single-particle density of states (DOS) around the Fermi level. Both types of quantum wells show a power-law depletion of the DOS at high energies. The results show that the different pseudogap behaviors are closely correlated with the type of magnetism in the proximity of the quantum wells and thus provide insights into the microscopic mechanisms.

Extraordinary Thermoelectric Properties of Topological Surface States in Quantum-Confined Cd3As2 Thin Films.

Topological insulators and semimetals have been shown to possess intriguing thermoelectric properties promising for energy harvesting and cooling applications. However, thermoelectric transport associated with the Fermi arc topological surface states on topological Dirac semimetals remains less explored. This work systematically examines thermoelectric transport in a series of topological Dirac semimetal Cd3As2 thin films grown by molecular beam epitaxy. Surprisingly, significantly enhanced Seebeck effect and anomalous Nernst effect are found at cryogenic temperatures when the Cd3As2 layer is thin. In particular, a peak Seebeck coefficient of nearly 500 µV K-1 and a corresponding thermoelectric power factor over 30 mW K-2 m-1 are observed at 5 K in a 25-nm-thick sample. Combining angle-dependent quantum oscillation analysis, magnetothermoelectric measurement, transport modeling, and first-principles simulation, the contributions from bulk and surface conducting channels are isolated and the unusual thermoelectric properties are attributed to the topological surface states. The analysis showcases the rich thermoelectric transport physics in quantum-confined topological Dirac semimetal thin films and suggests new routes to achieving high thermoelectric performance at cryogenic temperatures.

Symmetry lowering in extreme-electron-density perovskite quantum wells.

We report on structural distortions in extreme-electron density (∼6×10(14) cm(-2)) confined quantum wells of SrTiO3 embedded in GdTiO3. Sr-column displacements are measured using high-angle annular dark-field imaging in scanning transmission electron microscopy. Using thick SrTiO3 layers as a reference, orthorhombic-like Sr-site displacements are observed when SrTiO3 quantum wells are thinner than 4 SrO layers, in precise agreement with an experimentally observed metal-to-insulator transition. It is shown that the structural displacements are absent in thicker quantum wells, even in the immediate proximity to the orthorhombic GdTiO3. The results are discussed in the context of strong electron correlations in this system.