In-Plane Anisotropy of Electrical Transport in Y0.85Tb0.15Ba2Cu3O7-x Films.

We fabricated high-quality c-axis-oriented epitaxial YBa2Cu3O7-x films with 15% of the yttrium atoms replaced by terbium (YTBCO) and studied their electrical properties. The Tb substitution reduced the charge carrier density, resulting in increased resistivity and decreased critical current density compared to pure YBa2Cu3O7-x films. The electrical properties of the YTBCO films showed an in-plane anisotropy in both the superconducting and normal states that, together with the XRD data, provided evidence for, at least, a partially twin-free film. Unexpectedly, the resistive transition of the bridges also demonstrated the in-plane anisotropy that could be explained within the framework of Tinkham's model of resistive transition and the Berezinskii-Kosterlitz-Thouless (BKT) model, depending on the sample parameters. Measurements of the differential resistance in the temperature range of the resistive transition confirmed the occurrence of the BKT transition in the YTBCO bridges. Therefore, we consider the YTBCO films to be a promising platform for both the fabrication of devices with high kinetic inductance and fundamental research on the BKT transition in cuprate superconductors.

Aharonov-Bohm Interference and Phase-Coherent Surface-State Transport in Topological Insulator Rings.

We present low-temperature magnetotransport measurements on selectively grown Sb2Te3-based topological insulator ring structures. These devices display clear Aharonov-Bohm oscillations in the conductance originating from phase-coherent transport around the ring. The temperature dependence of the oscillation amplitude indicates that the Aharonov-Bohm oscillations originate from ballistic transport along the ring arms. We attribute these oscillations to the topological surface states. Further insight into the phase coherence is gained by comparing with similar Aharonov-Bohm-type oscillations in topological insulator nanoribbons exposed to an axial magnetic field. Here, quasi-ballistic phase-coherent transport is confirmed for closed-loop topological surface states in the transverse direction enclosing the nanoribbon. In contrast, the appearance of universal conductance fluctuations indicates phase-coherent transport in the diffusive regime, which is attributed to bulk carrier transport. Thus, it appears that even in the presence of diffusive p-type charge carriers in Aharonov-Bohm ring structures, phase-coherent quasi-ballistic transport of topological surface states is maintained over long distances.

Phase-Selective Epitaxy of Trigonal and Orthorhombic Bismuth Thin Films on Si (111).

Over the past three decades, the growth of Bi thin films has been extensively explored due to their potential applications in various fields such as thermoelectrics, ferroelectrics, and recently for topological and neuromorphic applications, too. Despite significant research efforts in these areas, achieving reliable and controllable growth of high-quality Bi thin-film allotropes has remained a challenge. Previous studies have reported the growth of trigonal and orthorhombic phases on various substrates yielding low-quality epilayers characterized by surface morphology. In this study, we present a systematic growth investigation, enabling the high-quality growth of Bi epilayers on Bi-terminated Si (111) 1 × 1 surfaces using molecular beam epitaxy. Our work yields a phase map that demonstrates the realization of trigonal, orthorhombic, and pseudocubic thin-film allotropes of Bi. In-depth characterization through X-ray diffraction (XRD) techniques and scanning transmission electron microscopy (STEM) analysis provides a comprehensive understanding of phase segregation, phase stability, phase transformation, and phase-dependent thickness limitations in various Bi thin-film allotropes. Our study provides recipes for the realization of high-quality Bi thin films with desired phases, offering opportunities for the scalable refinement of Bi into quantum and neuromorphic devices and for revisiting technological proposals for this versatile material platform from the past 30 years.

Supercurrent in Bi4Te3 Topological Material-Based Three-Terminal Junctions.

In this paper, in an in situ prepared three-terminal Josephson junction based on the topological insulator Bi4Te3 and the superconductor Nb the transport properties are studied. The differential resistance maps as a function of two bias currents reveal extended areas of Josephson supercurrent, including coupling effects between adjacent superconducting electrodes. The observed dynamics for the coupling of the junctions is interpreted using a numerical simulation of a similar geometry based on a resistively and capacitively shunted Josephson junction model. The temperature dependency indicates that the device behaves similar to prior experiments with single Josephson junctions comprising topological insulators' weak links. Irradiating radio frequencies to the junction, we find a spectrum of integer Shapiro steps and an additional fractional step, which is interpreted with a skewed current-phase relationship. In a perpendicular magnetic field, we observe Fraunhofer-like interference patterns in the switching currents.

Selective Area Epitaxy of Quasi-1-Dimensional Topological Nanostructures and Networks.

Quasi-one-dimensional (1D) topological insulators hold the potential of forming the basis of novel devices in spintronics and quantum computing. While exposure to ambient conditions and conventional fabrication processes are an obstacle to their technological integration, ultra-high vacuum lithography techniques, such as selective area epitaxy (SAE), provide all the necessary ingredients for their refinement into scalable device architectures. In this work, high-quality SAE of quasi-1D topological insulators on templated Si substrates is demonstrated. After identifying the narrow temperature window for selectivity, the flexibility and scalability of this approach is revealed. Compared to planar growth of macroscopic thin films, selectively grown regions are observed to experience enhanced growth rates in the nanostructured templates. Based on these results, a growth model is deduced, which relates device geometry to effective growth rates. After validating the model experimentally for various three-dimensional topological insulators (3D TIs), the crystal quality of selectively grown nanostructures is optimized by tuning the effective growth rates to 5 nm/h. The high quality of selectively grown nanostructures is confirmed through detailed structural characterization via atomically resolved scanning transmission electron microscopy (STEM).

Integration of Topological Insulator Josephson Junctions in Superconducting Qubit Circuits.

The integration of semiconductor Josephson junctions (JJs) in superconducting quantum circuits provides a versatile platform for hybrid qubits and offers a powerful way to probe exotic quasiparticle excitations. Recent proposals for using circuit quantum electrodynamics (cQED) to detect topological superconductivity motivate the integration of novel topological materials in such circuits. Here, we report on the realization of superconducting transmon qubits implemented with (Bi0.06Sb0.94)2Te3 topological insulator (TI) JJs using ultrahigh vacuum fabrication techniques. Microwave losses on our substrates, which host monolithically integrated hardmasks used for the selective area growth of TI nanostructures, imply microsecond limits to relaxation times and, thus, their compatibility with strong-coupling cQED. We use the cavity-qubit interaction to show that the Josephson energy of TI-based transmons scales with their JJ dimensions and demonstrate qubit control as well as temporal quantum coherence. Our results pave the way for advanced investigations of topological materials in both novel Josephson and topological qubits.

Reappearance of first Shapiro step in narrow topological Josephson junctions.

In Josephson junctions, a supercurrent across a nonsuperconducting weak link is carried by electron-hole bound states. Because of the helical spin texture of nondegenerate topological surface states, gapless bound states are established in junctions with topological weak link. These have a characteristic 4π-periodic current phase relation (CΦR) that leads to twice the conventional Shapiro step separation voltage in radio frequency-dependent measurements. In this context, we identify an attenuated first Shapiro step in (Bi0.06Sb0.94)2Te3 (BST) Josephson junctions with AlO x capping layer. We further investigate junctions on narrow, selectively deposited BST nanoribbons, where surface charges are confined to the perimeter of the nanoribbon. Within these junctions, previously identified signatures of gapless bound states are absent. Because of confinement, transverse momentum sub-bands are quantized and a topological gap opening is observed. Surface states within these quantized sub-bands are spin degenerate, which evokes bound states of conventional 2π-periodic CΦR within the BST nanoribbon weak link.

Probing embedded topological modes in bulk-like GeTe-Sb2Te3 heterostructures.

The interface between topological and normal insulators hosts metallic states that appear due to the change in band topology. While topological states at a surface, i.e., a topological insulator-air/vacuum interface, have been studied intensely, topological states at a solid-solid interface have been less explored. Here we combine experiment and theory to study such embedded topological states (ETSs) in heterostructures of GeTe (normal insulator) and [Formula: see text] [Formula: see text] (topological insulator). We analyse their dependence on the interface and their confinement characteristics. First, to characterise the heterostructures, we evaluate the GeTe-Sb[Formula: see text]Te[Formula: see text] band offset using X-ray photoemission spectroscopy, and chart the elemental composition using atom probe tomography. We then use first-principles to independently calculate the band offset and also parametrise the band structure within a four-band continuum model. Our analysis reveals, strikingly, that under realistic conditions, the interfacial topological modes are delocalised over many lattice spacings. In addition, the first-principles calculations indicate that the ETSs are relatively robust to disorder and this may have practical ramifications. Our study provides insights into how to manipulate topological modes in heterostructures and also provides a basis for recent experimental findings [Nguyen et al. Sci. Rep. 6, 27716 (2016)] where ETSs were seen to couple over thick layers.

Phase-coherent loops in selectively-grown topological insulator nanoribbons.

We succeeded in the fabrication of topological insulator (Bi0.57Sb0.43)2Te3 Hall bars as well as nanoribbons by means of selective-area growth using molecular beam epitaxy. By performing magnetotransport measurements at low temperatures information on the phase-coherence of the electrons is gained by analyzing the weak-antilocalization effect. Furthermore, from measurements on nanoribbons at different magnetic field tilt angles an angular dependence of the phase-coherence length is extracted, which is attributed to transport anisotropy and geometrical factors. For the nanoribbon structures universal conductance fluctuations were observed. By performing a Fourier transform of the fluctuation pattern a series of distinct phase-coherent closed-loop trajectories are identified. The corresponding enclosed areas can be explained in terms of nanoribbon dimensions and phase-coherence length. In addition, from measurements at different magnetic field tilt angles we can deduce that the area enclosed by the loops are predominately oriented parallel to the quintuple layers.

Room temperature in-situ measurement of the spin voltage of a BiSbTe3 thin film.

One of the hallmarks of topological insulators (TIs), the intrinsic spin polarisation in the topologically protected surface states, is investigated at room temperature in-situ by means of four-probe scanning tunnelling microscopy (STM) for a BiSbTe3 thin film. To achieve the required precision of tip positions for measuring a spin signal, a precise positioning method employing STM scans of the local topography with each individual tip is demonstrated. From the transport measurements, the spin polarisation in the topological surface states (TSS) is estimated as p ~ 0.3 - 0.6, which is close to the theoretical limit.

Tantalum(v) 1,3-propanediolate ß-diketonate solution as a precursor to sol-gel derived, metal oxide thin films.

Tantalum oxide is ubiquitous in everyday life, from capacitors in electronics to ion conductors for electrochromic windows and electrochemical storage devices. Investigations into sol-gel deposition of tantalum oxide, and its sister niobium oxide, has accelerated since the 1980s and continues to this day. The aim of this study is to synthesize a near UV sensitive, air stable, and low toxicity tantalum sol-gel precursor solution for metal oxide thin films - these attributes promise to reduce manufacturing costs and allow for facile mass production. By utilizing 1D and 2D nuclear magnetic resonance, this study shows that by removing ethanol from the precursor solution at a relatively low temperature and pressure, decomposition of the photosensitive complex can be minimized while obtaining a precursor solution with sufficient stability for storage and processing in the atmosphere. The solution described herein is further modified for inkjet printing, where multiple material characterization techniques demonstrate that the solution can be utilized in low temperature, photochemical solution deposition of tantalum oxide, which is likely amorphous. Tested substrates include amorphous silica, crystalline silicon wafer, and gold/titanium/PET foil. The hope is that these results may spark future investigations into electronic, optical, and biomedical device fabrication with tantalum oxide, and potentially niobium oxide, based films using the proposed synthesis method.

Correction: Tantalum(v) 1,3-propanediolate ß-diketonate solution as a precursor to sol-gel derived, metal oxide thin films.

[This corrects the article DOI: 10.1039/D0RA02558E.].

Selective area growth and stencil lithography for in situ fabricated quantum devices.

The interplay of Dirac physics and induced superconductivity at the interface of a 3D topological insulator (TI) with an s-wave superconductor (S) provides a new platform for topologically protected quantum computation based on elusive Majorana modes. To employ such S-TI hybrid devices in future topological quantum computation architectures, a process is required that allows for device fabrication under ultrahigh vacuum conditions. Here, we report on the selective area growth of (Bi,Sb)2Te3 TI thin films and stencil lithography of superconductive Nb for a full in situ fabrication of S-TI hybrid devices via molecular-beam epitaxy. A dielectric capping layer was deposited as a final step to protect the delicate surfaces of the S-TI hybrids at ambient conditions. Transport experiments in as-prepared Josephson junctions show highly transparent S-TI interfaces and a missing first Shapiro step, which indicates the presence of Majorana bound states. To move from single junctions towards complex circuitry for future topological quantum computation architectures, we monolithically integrated two aligned hardmasks to the substrate prior to growth. The presented process provides new possibilities to deliberately combine delicate quantum materials in situ at the nanoscale.

Influence of Te-Doping on Catalyst-Free VS InAs Nanowires.

We report on the growth of Te-doped catalyst-free InAs nanowires by molecular beam epitaxy on silicon (111) substrates. Changes in the wire morphology, i.e. a decrease in length and an increase in diameter have been observed with rising doping level. Crystal structure analysis based on transmission electron microscopy as well as X-ray diffraction reveals an enhancement of the zinc blende/(wurtzite+zinc blende) segment ratio if Te is provided during the growth process. Furthermore, electrical two-point measurements show that increased Te-doping causes a gain in conductivity. Two comparable growth series, differing only in As-partial pressure by about 1 × 10-5 Torr while keeping all other parameters constant, were analyzed for different Te-doping levels. Their comparison suggests that the crystal structure is strongly affected and the conductivity gain is more distinct for wires grown at a comparably higher As-partial pressure.

Phase-coherent transport in selectively grown topological insulator nanodots.

Oxidized Si(111) substrates were pre-structured by electron beam lithography and used as a substrate for the selective growth of three-dimensional topological insulators (TI) by molecular beam epitaxy. The patterned holes were filled up by the TI, i.e. Sb2Te3 and Bi2Te3, to form nanodots. Scanning electron microscopy and focused ion beam cross-sectioning was utilized to determine the morphology and depth profile of the nanodots. The magnetotransport measurements revealed universal conductance fluctuations originating from electron interference in phase-coherent loops. We find that these loops are oriented preferentially within the quintuple layers of the TI with only a small perpendicular contribution. Furthermore, we found clear indications of an conductivity anisotropy between different crystal orientations.

Nanoscale Near-Field Tomography of Surface States on (Bi0.5Sb0.5)2Te3.

Three-dimensional topological insulators (TIs) have attracted tremendous interest for their possibility to host massless Dirac Fermions in topologically protected surface states (TSSs), which may enable new kinds of high-speed electronics. However, recent reports have outlined the importance of band bending effects within these materials, which results in an additional two-dimensional electron gas (2DEG) with finite mass at the surface. TI surfaces are also known to be highly inhomogeneous on the nanoscale, which is masked in conventional far-field studies. Here, we use near-field microscopy in the mid-infrared spectral range to probe the local surface properties of custom-tailored (Bi0.5Sb0.5)2Te3 structures with nanometer precision in all three spatial dimensions. Applying nanotomography and nanospectroscopy, we reveal a few-nanometer-thick layer of high surface conductivity and retrieve its local dielectric function without assuming any model for the spectral response. This allows us to directly distinguish between different types of surface states. An intersubband transition within the massive 2DEG formed by quantum confinement in the bent conduction band manifests itself as a sharp, surface-bound, Lorentzian-shaped resonance. An additional broadband background in the imaginary part of the dielectric function may be caused by the TSS. Tracing the intersubband resonance with nanometer spatial precision, we observe changes of its frequency, likely originating from local variations of doping or/and the mixing ratio between Bi and Sb. Our results highlight the importance of studying the surfaces of these novel materials on the nanoscale to directly access the local optical and electronic properties via the dielectric function.

Oxide removal and stabilization of bismuth thin films through chemically bound thiol layers.

Bismuth has been identified as a material of interest for electronic applications due to its extremely high electron mobility and quantum confinement effects observed at nanoscale dimensions. However, it is also the case that Bi nanostructures are readily oxidised in ambient air, necessitating additional capping steps to prevent surface re-oxidation, thus limiting the processing potential of this material. This article describes an oxide removal and surface stabilization method performed on molecular beam epitaxy (MBE) grown bismuth thin-films using ambient air wet-chemistry. Alkanethiol molecules were used to dissolve the readily formed bismuth oxides through a catalytic reaction; the bare surface was then reacted with the free thiols to form an organic layer which showed resistance to complete reoxidation for up to 10 days.

Electrical resistance of individual defects at a topological insulator surface.

Three-dimensional topological insulators host surface states with linear dispersion, which manifest as a Dirac cone. Nanoscale transport measurements provide direct access to the transport properties of the Dirac cone in real space and allow the detailed investigation of charge carrier scattering. Here we use scanning tunnelling potentiometry to analyse the resistance of different kinds of defects at the surface of a (Bi0.53Sb0.47)2Te3 topological insulator thin film. We find the largest localized voltage drop to be located at domain boundaries in the topological insulator film, with a resistivity about four times higher than that of a step edge. Furthermore, we resolve resistivity dipoles located around nanoscale voids in the sample surface. The influence of such defects on the resistance of the topological surface state is analysed by means of a resistor network model. The effect resulting from the voids is found to be small compared with the other defects.

Bi1Te1 is a dual topological insulator.

New three-dimensional (3D) topological phases can emerge in superlattices containing constituents of known two-dimensional topologies. Here we demonstrate that stoichiometric Bi1Te1, which is a natural superlattice of alternating two Bi2Te3 quintuple layers and one Bi bilayer, is a dual 3D topological insulator where a weak topological insulator phase and topological crystalline insulator phase appear simultaneously. By density functional theory, we find indices (0;001) and a non-zero mirror Chern number. We have synthesized Bi1Te1 by molecular beam epitaxy and found evidence for its topological crystalline and weak topological character by spin- and angle-resolved photoemission spectroscopy. The dual topology opens the possibility to gap the differently protected metallic surface states on different surfaces independently by breaking the respective symmetries, for example, by magnetic field on one surface and by strain on another surface.

Ultrafast photocurrents at the surface of the three-dimensional topological insulator Bi2Se3.

Three-dimensional topological insulators are fascinating materials with insulating bulk yet metallic surfaces that host highly mobile charge carriers with locked spin and momentum. Remarkably, surface currents with tunable direction and magnitude can be launched with tailored light beams. To better understand the underlying mechanisms, the current dynamics need to be resolved on the timescale of elementary scattering events (∼10 fs). Here, we excite and measure photocurrents in the model topological insulator Bi2Se3 with a time resolution of 20 fs by sampling the concomitantly emitted broadband terahertz (THz) electromagnetic field from 0.3 to 40 THz. Strikingly, the surface current response is dominated by an ultrafast charge transfer along the Se-Bi bonds. In contrast, photon-helicity-dependent photocurrents are found to be orders of magnitude smaller than expected from generation scenarios based on asymmetric depopulation of the Dirac cone. Our findings are of direct relevance for broadband optoelectronic devices based on topological-insulator surface currents.