Broadband Photodetection of Centimeter-Scale T-Phase Gallium Telluride Grown by Molecular Beam Epitaxy.

Two-dimensional (2D) semiconductors have recently attracted considerable attention due to their promising applications in future integrated electronic and optoelectronic devices. Large-scale synthesis of high-quality 2D semiconductors is an increasingly essential requirement for practical applications, such as sensing, imaging, and communications. In this work, homogeneous 2D GaTe films on a centimeter scale are epitaxially grown on fluorphlogopite mica substrates by molecular beam epitaxy (MBE). The epitaxial GaTe thin films showed an atomically 2D layered lattice structure with a T phase, which has not been discovered in the GaTe geometric isomer. Furthermore, semiconducting behavior and high mobility above room temperature were found in T-GaTe epitaxial films, which are essential for application in semiconducting devices. The T-GaTe-based photodetectors demonstrated respectable photodetection performance with a responsivity of 13 mA/W and a fast response speed. By introducing monolayer graphene as the substrate, we successfully realized high-quality GaTe/graphene heterostructures. The performance has been significantly improved, such as the responsivity was enhanced more than 20 times. These results highlight a feasible scheme for exploring the crystal phase of 2D GaTe and realizing the controlled growth of GaTe films on large substrates, which could promote the development of broadband, high-performance, and large-scale photodetection applications.

Role of topological surface states and mirror symmetry in topological crystalline insulator SnTe as an efficient electrocatalyst.

The surface orientation dependence on the hydrogen evolution reaction (HER) performance of topological crystalline insulator (TCI) SnTe thin films is studied. Their intrinsic activities are determined by linear sweep voltammetry and cyclic voltammetry measurements. It is found that SnTe (001) and (111) surfaces exhibit intrinsic activities significantly larger than the (211) surface. Density functional theory calculations reveal that pure (001) and (111) surfaces are not good electrocatalysts, while those with Sn vacancies or partially oxidized surfaces, with the latter as evidenced by X-ray photoelectron spectroscopy, have high activity. The calculated overall performance of the (001) and (111) surfaces with robust topological surface states (TSSs) is better than that of the lowly symmetric (211) surface with fragile or without TSSs, which is further supported by their measured weak antilocalization strength. The high HER activity of SnTe (001) and (111) is attributed to the enhanced charge transfer between H atoms and TSSs. We also address the effect of possible surface facets and the contrast of the HER activity of the available active sites among the three samples. Our study demonstrates that the TSSs and mirror symmetry of TCIs expedite their HER activity.

Superconductivity in Single-Quintuple-Layer Bi2Te3 Grown on Epitaxial FeTe.

How an interfacial superconductivity emerges during the nucleation and epitaxy is of great importance not only for unveiling the physical insights but also for finding a feasible way to tune the superconductivity via interfacial engineering. In this work, we report the nanoscale creation of a robust and relatively homogeneous interfacial superconductivity (TC ≈ 13 K) on the epitaxial FeTe surface, by van der Waals epitaxy of single-quintuple-layer topological insulator Bi2Te3. Our study suggests that the superconductivity in the Bi2Te3/FeTe heterostructure is generated at the interface and that the superconductivity at the interface does not enhance or weaken with the increase of the Bi2Te3 thickness beyond 1 quintuple layer (QL). The observation of the topological surface states crossing Fermi energy in the Bi2Te3/FeTe heterostructure with the average Bi2Te3 thickness of about 20 QL provides further evidence that this heterostructure may potentially host Majorana zero modes.

Studies on the origin of the interfacial superconductivity of Sb2Te3/Fe1+yTe heterostructures.

The recent discovery of the interfacial superconductivity (SC) of the Bi2Te3/Fe1+yTe heterostructure has attracted extensive studies due to its potential as a novel platform for trapping and controlling Majorana fermions. Here we present studies of another topological insulator (TI)/Fe1+yTe heterostructure, Sb2Te3/Fe1+yTe, which also has an interfacial 2-dimensional SC. The results of transport measurements support that reduction of the excess Fe concentration of the Fe1+yTe layer not only increases the fluctuation of its antiferromagnetic (AFM) order but also enhances the quality of the SC of this heterostructure system. On the other hand, the interfacial SC of this heterostructure was found to have a wider-ranging TI-layer thickness dependence than that of the Bi2Te3/Fe1+yTe heterostructure, which is believed to be attributed to the much higher bulk conductivity of Sb2Te3 that enhances indirect coupling between its top and bottom topological surface states (TSSs). Our results provide evidence of the interplay among the AFM order, itinerant carries from the TSSs, and the induced interfacial SC of the TI/Fe1+yTe heterostructure system.

Formation of Fe-Te Nanostructures during in Situ Fe Heavy Doping of Bi2Te3.

To study the in situ doping effect upon monotonically increasing dopant concentration, a Bi2Te3 layer doped with Fe up to ~6.9% along the growth direction was fabricated by the molecular beam epitaxy (MBE) technique. Its resistance versus temperature curve displays a superconductivity transition at about 12.3 K. Detailed structural and chemical analysis via X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and energy-dispersive X-ray spectroscopy (EDS) reveal that this layer consists of two types of unexpected Fe-Te nanostructures: one is FeTe thin layer formed near the surface, and the other is FeTe2 nanorod embedded in the Bi2Te3 layer. Based on the results of further electrical and magnetotransport studies, it is likely that the observed superconductivity originates from the interface between the FeTe nanostructure and the neighboring Bi2Te3 layer. We have addressed the formation mechanisms of the observed nanostructures, which is attributed to the strong reaction between Fe and Te atoms during the growth process. The findings of this study also provide an unusual approach to synthesizing nanostructures via heavy doping if the dopant element is strongly reactive with an element in the host matrix.

Pressure induced topological phase transition in layered Bi2S3.

A large bulk band gap and tunable Dirac carriers are desired for practical device applications of topological insulators. However, most known topological insulators are narrow gap materials and the manipulation of their Dirac surface states is limited by residual bulk charge carriers originating from intrinsic defects. In this study, via density functional theory based first-principles calculations, we predict that a layered hexagonal structure of Bi2S3 is stable, and it becomes a topological insulator under a moderate compressive pressure of about 5.3 GPa. Interestingly, we find that the strength of the spin-orbit interaction in Bi2S3 can be effectively enhanced by the applied pressure. This leads to an increased inverted band gap with pressure, which can reach 0.4 eV with a pressure of 13.7 GPa. Compared to Bi2Se3, intrinsic defects are suppressed in Bi2S3 under both cation- and anion-poor growth conditions. Our calculations predict a new Bi-based topological insulator, and also shed light on control over spin-orbit interactions in Bi2S3 and tuning of its topological properties.

Large-area epitaxial growth of MoSe2 via an incandescent molybdenum source.

We have developed an incandescent Mo source to fabricate large-area single-crystalline MoSe2 thin films. The as-grown MoSe2 thin films were characterized using transmission electron microscopy, energy dispersive x-ray spectroscopy, atomic force microscopy, Raman spectroscopy, photoluminescence (PL), reflection high energy electron diffraction (RHEED) and angular resolved photoemission spectroscopy (ARPES). A new Raman characteristic peak at 1591 cm-1 was identified. Results from Raman spectroscopy, PL, RHEED and ARPES studies consistently reveal that large-area single crystalline mono-layer of MoSe2 could be achieved by this technique. This technique enjoys several advantages over conventional approaches and could be extended to the growth of other two-dimensional layered materials containing a low-vapor-pressure element.

Self-Assembled Formation of Well-Aligned Cu-Te Nano-Rods on Heavily Cu-Doped ZnTe Thin Films.

Cu doping of ZnTe, which is an important semiconductor for various optoelectronic applications, has been successfully achieved previously by several techniques. However, besides its electrical transport characteristics, other physical and chemical properties of heavily Cu-doped ZnTe have not been reported. We found an interesting self-assembled formation of crystalline well-aligned Cu-Te nano-rods near the surface of heavily Cu-doped ZnTe thin films grown via the molecular beam epitaxy technique. A phenomenological growth model is presented based on the observed crystallographic morphology and measured chemical composition of the nano-rods using various imaging and chemical analysis techniques. When substitutional doping reaches its limit, the extra Cu atoms favor an up-migration toward the surface, leading to a one-dimensional surface modulation and formation of Cu-Te nano-rods, which explain unusual observations on the reflection high energy electron diffraction patterns and apparent resistivity of these thin films. This study provides an insight into some unexpected chemical reactions involved in the heavily Cu-doped ZnTe thin films, which may be applied to other material systems that contain a dopant having strong reactivity with the host matrix.

Robust two-dimensional superconductivity and vortex system in Bi2Te3/FeTe heterostructures.

The discovery of two-dimensional superconductivity in Bi2Te3/FeTe heterostructures provides a new platform for the search of Majorana fermions in condensed matter systems. Since Majorana fermions are expected to reside at the core of the vortices, a close examination of the vortex dynamics in superconducting interface is of paramount importance. Here, we report the robustness of the interfacial superconductivity and 2D vortex dynamics in four as-grown and aged Bi2Te3/FeTe heterostructure with different Bi2Te3 epilayer thickness (3, 5, 7, 14 nm). After two years' air exposure, superconductivity remains robust even when the thickness of Bi2Te3 epilayer is down to 3 nm. Meanwhile, a new feature at ~13 K is induced in the aged samples, and the high field studies reveal its relevance to superconductivity. The resistance of all as-grown and aged heterostructures, just below the superconducting transition temperature follows the Arrhenius relation, indicating the thermally activated flux flow behavior at the interface of Bi2Te3 and FeTe. Moreover, the activation energy exhibits a logarithmic dependence on the magnetic field, providing a compelling evidence for the 2D vortex dynamics in this novel system. The weak disorder associated with aging-induced Te vacancies is possibly responsible for these observed phenomena.

Anisotropic magnetic responses of a 2D-superconducting Bi2Te3/FeTe heterostructure.

We have investigated the anisotropic magnetic responses of a 2D-superconducting Bi2Te3/FeTe heterostructure. Cross-sectional STEM imaging revealed that the excess Fe atoms in the FeTe layer occupy specific interstitial sites. They were found to show strong anisotropic magnetic responses under a magnetic field either perpendicular or parallel to the sample surface. Under perpendicular magnetic fields within 1000 Oe, conventional paramagnetic Meissner effect, superconducting diamagnetism, and anomalous enhancement of magnetization successively occur as the magnetic field increases. In contrast, under parallel magnetic fields, superconducting diamagnetism was not observed explicitly in the magnetization measurements and the anomalous enhancement of magnetization appears only for fields higher than 1000 Oe. The observed strong magnetic anisotropy provides further evidence that the induced superconductivity at the interface of the Bi2Te3/FeTe heterostucture has a 2D nature.

Tunable interaction-induced localization of surface electrons in antidot nanostructured Bi2Te3 thin films.

Recently, a logarithmic decrease of conductivity has been observed in topological insulators at low temperatures, implying a tendency of localization of surface electrons. Here, we report quantum transport experiments on the topological insulator Bi2Te3 thin films with arrayed antidot nanostructures. With increasing density of the antidots, a systematic decrease is observed in the slope of the logarithmic temperature-dependent conductivity curves, indicating the electron-electron interaction can be tuned by the antidots. Meanwhile, the weak antilocalization effect revealed in magnetoconductivity exhibits an enhanced dominance of electron-electron interaction among decoherence mechanisms. The observation can be understood from an antidot-induced reduction of the effective dielectric constant, which controls the interactions between the surface electrons. Our results clarify the indispensable role of the electron-electron interaction in the localization of surface electrons and indicate the localization of surface electrons in an interacting topological insulator.

Two-dimensional superconductivity at the interface of a Bi2Te3/FeTe heterostructure.

The realization of superconductivity at the interface between a topological insulator and an iron-chalcogenide compound is highly attractive for exploring several recent theoretical predictions involving these two new classes of materials. Here we report transport measurements on a Bi2Te3/FeTe heterostructure fabricated via van der Waals epitaxy, which demonstrate superconductivity at the interface, which is induced by the Bi2Te3 epilayer with thickness even down to one quintuple layer, though there is no clear-cut evidence that the observed superconductivity is induced by the topological surface states. The two-dimensional nature of the observed superconductivity with the highest transition temperature around 12 K was verified by the existence of a Berezinsky-Kosterlitz-Thouless transition and the diverging ratio of in-plane to out-plane upper critical field on approaching the superconducting transition temperature. With the combination of interface superconductivity and Dirac surface states of Bi2Te3, the heterostructure studied in this work provides a novel platform for realizing Majorana fermions.

Growth, reaction and nanowire formation of Fe on the ZnS(1 0 0) surface.

The growth and reaction of Fe on a ZnS(1 0 0) substrate are studied in situ and with high lateral resolution using low energy electron microscopy (LEEM), micro low energy electron diffraction ( µLEED), x-ray photoemission electron microscopy (XPEEM), microprobe x-ray photoelectron spectroscopy ( µXPS) and x-ray magnetic circular dichroism PEEM (XMCDPEEM) for complementary structural, chemical, and magnetic characterization. Initially, a two-dimensional (Fe, Zn)S reaction layer forms with thickness that depends on growth temperature. Further growth results in the formation of a variety of three-dimensional crystals, most of them strongly elongated in the form of 'nanowires' of two distinct types, labeled as A and B. Type A nanowires are oriented near the ZnS[1 1 0] direction and are composed of Fe. Type B nanowires are oriented predominantly along directions a few degrees off the ZnS[0 0 1] direction and are identified as Greigite (Fe3S4). Both types of nanowires are magnetic with Curie temperatures above 450 °C. The understanding of the reactive growth mechanism in this system that is provided by these investigations may help to develop growth methods for other elemental and transition metal chalcogenide nanostructures on ZnS and possibly on other II-VI semiconductor surfaces.

Surface reactivity enhancement on a Pd/Bi2Te3 heterostructure through robust topological surface states.

We present a study of the surface reactivity of a Pd/Bi2Te3 thin film heterostructure. The topological surface states from Bi2Te3, being delocalized and robust owing to their topological natures, were found to act as an effective electron bath that significantly enhances the surface reactivity of palladium in the presence of two oxidizing agents, oxygen and tellurium respectively, which is consistent with a theoretical calculation. The surface reactivity of the adsorbed tellurium on this heterostructure is also intensified possibly benefitted from the effective transfer of the bath electrons. A partially inserted iron ferromagnetic layer at the interface of this heterostructure was found to play two competing roles arising from the higher-lying d-band center of the Pd/Fe bilayer and the interaction between the ferromagnetism and the surface spin texture of Bi2Te3 on the surface reactivity and their characteristics also demonstrate that the electron bath effect is long-lasting against accumulated thickness of adsorbates.

ZnSe nanotrenches: formation mechanism and its role as a 1D template.

High-resolution transmission electron microscopy was used to characterize the microstructures of ZnSe nanotrenches induced by mobile Au-alloy droplets. The contact side interfaces between the AuZnδ alloy droplets and the ZnSe as well as the four side walls of the resulting <011>-oriented nanotrenches were found all belong to the {111} plane family, with the front and back walls being the {111}A planes while the other two side walls being the {111}B planes. These findings offer a deeper understanding on the formation mechanism of the nanotrenches. Pure Au nanodashes were formed upon further deposition of Au on the nanotrenches.PACS: 61.46.Df, Structure of nanocrystals and nanoparticles. 81.16.Rf, Micro and nanoscale pattern formation. 68.37.Og, High resolution transmission electron microscopy.

Impurity effect on weak antilocalization in the topological insulator Bi2Te3.

We study the weak antilocalization (WAL) effect in topological insulator Bi(2)Te(3) thin films at low temperatures. The two-dimensional WAL effect associated with surface carriers is revealed in the tilted magnetic field dependence of magnetoconductance. Our data demonstrate that the observed WAL is robust against deposition of nonmagnetic Au impurities on the surface of the thin films, but it is quenched by the deposition of magnetic Fe impurities which destroy the π Berry phase of the topological surface states. The magnetoconductance data of a 5 nm Bi(2)Te(3) film suggests that a crossover from symplectic to unitary classes is observed with the deposition of Fe impurities.