Using high-resolution angle-resolved photoemission spectroscopy, the electronic structure near the Fermi level and the topological property of the Bi(111) films grown on the Bi$_2$Te$_3$(111) substrate were studied. Very different from the bulk Bi, we found another surface band near the $\bar{M}$ point besides the two well-known surface bands on the Bi(111) surface. With this new surface band, the bulk valence band and the bulk conduction band of Bi can be connected by the surface states. Our band mapping revealed odd number of Fermi crossings of the surface bands, which provided a direct experimental signature that Bi(111) thin films of a certain thickness on the Bi$_2$Te$_3$(111) substrate can be topologically nontrivial in three dimension.
The historic de Haas van Alphen effect observed in the late 1950s in CSIR-NPL by J.S. Dhillon and D. Shoenberg in pure bismuth and zinc metal is revisited in this article hrough a single crystalline phase of bismuth crystal, which is observed in terms of resistivity as predicted by Shubnikov de Haas oscillations. The occurrence of oscillations in the transverse magnetic field confirms the presence of the Fermi surface. The single crystal of bismuth is grown through solid-state reaction under an optimized heat treatment whose purity and structural phase are confirmed through XRD, SEM, and EDAX.
We report the growth of self-assembled Bi2Se3 quantum dots (QDs) by molecular beam epitaxy on GaAs substrates using the droplet epitaxy technique. The QD formation occurs after anneal of Bismuth droplets under Selenium flux. Characterization by atomic force microscopy, scanning electron microscopy, X-ray diffraction, high-resolution transmission electron microscopy and X-ray reflectance spectroscopy is presented. The quantum dots are crystalline, with hexagonal shape, and have average dimensions of 12 nm height (12 quintuple layers) and 46 nm width, and a density of $8.5 \cdot 10^9 cm^{-2}$. T…
While first-principles calculations with different levels of sophistication predict a topologically trivial $Z_2$ state for bulk bismuth, some photoemission experiments show surface states consistent with the interpretation of bismuth being in a topologically non-trivial $Z_2$ state. We resolve this contradiction between theory and experiment by showing, based on quasiparticle self-consistent $GW$ calculations, that the experimental surface states interpreted as supporting a non-trivial phase are actually consistent with a trivial $Z_2$ invariant. We identify this contradiction as the result o…
Bismuth has been the key element in the discovery and development of topological insulator materials. Previous theoretical studies indicated that Bi is topologically trivial and it can transform into the topological phase by alloying with Sb. However, recent high-resolution angle-resolved photoemission spectroscopy (ARPES) measurements strongly suggested a topological band structure in pure Bi. To address this issue, we study the band structure of Bi and Sb films by ARPES and first-principles calculations. By tuning tight binding parameters, we show that Bi quantum films in topologically trivi…
Bulk and surface electronic structures, calculated using density functional theory and a tight-binding model Hamiltonian, reveal the existence of two topologically invariant (TI) surface states in the family of cubic Bi perovskites (ABiO$_3$; A = Na, K, Rb, Cs, Mg, Ca, Sr and Ba). The two TI states, one lying in the valence band (TI-V) and other lying in the conduction band (TI-C) are formed out of bonding and antibonding states of the Bi-$\{$s,p$\}$ - O-$\{$p$\}$ coordinated covalent interaction. Below a certain critical thickness of the film, which varies with A, TI states of top and bottom …
We have investigated the Faraday rotation of in-plane magnetized bismuth - substituted ferrite garnet films grown by liquid phase epitaxy on (100) oriented gadolinium gallium garnet substrates. The Faraday spectra were measured for photon energies between 1.7 - 2.6 eV. To interprete the spectra, we use a model based on two electric dipole transitions, one tetrahedral and one octahedral. Furthermore, the Faraday rotation sensitivity was measured at 2.3 eV, and found to be in good agreement with the theoretical predicitions. In particular, we find that the sensitivity increases linearly with the…
We explore the Bi-surfactant-directed self-assembly and structure of InAs quantum dots grown on GaAs(110) by molecular beam epitaxy. The addition of a Bi flux during InAs deposition changes the InAs growth mode from two-dimensional (2D) Frank-van der Merwe to Stranski-Krastanov, resulting in the formation of three-dimensional (3D) InAs islands on the surface. Furthermore, exposing static InAs 2D layers to Bi induces a rearrangement of the strained layer into 3D islands. We explore the effect of varying the InAs thickness and Bi flux for these two growth approaches, observing a critical thickne…
Here, we report a combined experimental-theoretical study showing that collective application of rare earth doping on A-site and epitaxial strain to ferroelectric bismuth titanate does not lead to a very large c-axis polarization as reported previously. Further first principles calculations based on the examination of polarization tensor suggest that simultaneous Bi and Ti site doping could result in moderate polarization along c-axis of bismuth titanate which is typically a preferential axis of film growth and thus enabling c axis oriented films to have appreciable polarization. This approach…
We report electrical conductance measurements of Bi nanocontacts created by repeated tip-surface indentation using a scanning tunneling microscope at temperatures of 4 K and 300 K. As a function of the elongation of the nanocontact we measure robust, tens of nanometers long plateaus of conductance G0 = 2e^2/h at room temperature. This observation can be accounted for by the mechanical exfoliation of a Bi(111) bilayer, a predicted QSH insulator, in the retracing process following a tip-surface contact. The formation of the bilayer is further supported by the additional observation of conductanc…
By means of first-principles calculations, we predict a new 2D QSH insulator in the porous allotrope of Bismuth monolayer, bismuthylene, its dynamics stability being confirmed by phonon spectrum and molecular dynamics simulations. The analyses of electronic structures reveal that it is a native QSH state with a gap much as large as 0.29 eV at the Γ point, which is larger than the buckled (0.2 eV) and flattened (0.2 eV) bismuth, Bi4Br4 (0.18 eV), as well as stanene (0.1 eV), also more stable energetically than these systems. Interestingly, the bismuthylene has tunable band gaps and nontrivial b…
We report visible light detection with in-plane BiFeO3 (BFO) thin films grown on pre-patterned inter-digital electrodes. In-plane configured BFO film displayed photocurrents with a 40:1 photo-to-dark-current ratio and improved photo-sensing ability for >15000 s (4 hrs) under small bias voltage (42V). Nearly sixty percent of the photo-induced charge carriers decay in 1.0 s and follow a double-exponential decay model. At 373 K the effect of light does not significantly increase the dark current, probably due to reduced mobility. Sub-bandgap weak monochromatic light (1 mw/cm2) shows one fold incr…
Spin- and Angle-resolved Photoelectron Spectroscopy Study of the Quantum Spin Hall Insulator Bismuthene and its Precursor Phase
Chemnitz University of Technology（开姆尼茨工业大学）；Research Center for Materials, Architectures and Integration of Nanomembranes (MAIN)（纳米膜材料、架构与集成研究中心）；MAX IV Laboratory（MAX IV 实验室）；Lund University（隆德大学）
Here we study the kinetics of liquefaction and solidification of thin bismuth films grown on the insulating substrate by the pulsed laser deposited (PLD) and molecular beam epitaxy (MBE) and investigated by in situ electron and X-ray diffraction. By PLD, we can grow films similar to those obtained using MBE, studied by ex-situ AFM, KPFM, XRR, and XRD. The liquefaction-solidification transition is monitored in real-time by RHEED and synchrotron XRD, resulting in a dewetting phenomenon and the formation of spherical droplets which size depends on the initial film thickness. Studying this phase t…
Using wide-band (0.5-6.5 eV) spectroscopic ellipsometry we study ultrathin [Bi(0.6-2.5 nm)-FeNi(0.8,1.2 nm)]N multilayer films grown by rf sputtering deposition, where the FeNi layer has a nanoisland structure and its morphology and magnetic properties change with decreasing the nominal layer thickness. From the multilayer model simulations of the ellipsometric angles, Psi(omega) and Delta(omega), the complex (pseudo)dielectric function spectra of the Bi layer were extracted. The obtained results demonstrate that the Bi layer can possess the surface metallic conductivity, which is strongly aff…
Optical band gap properties of high-quality few-layer topological insulator Bi2Se3 thin films grown with magnetron sputtering are investigated using broadband absorption spectroscopy. We provide direct optical evidence of a rigid blue-shift to up to 0.5 eV in the band gap of Bi2Se3 as it approaches the two-dimensional limit. The onset of this behavior is most significant below six quintuple layers. The blue shift is very robust and is observed in both protected (capped) and exposed (uncapped) thin films. Our results are consistent with observations that finite-size effects have profound impact…
The mathematical field of topology has become a framework to describe the low-energy electronic structure of crystalline solids. A typical feature of a bulk insulating three-dimensional topological crystal are conducting two-dimensional surface states. This constitutes the topological bulk-boundary correspondence. Here, we establish that the electronic structure of bismuth, an element consistently described as bulk topologically trivial, is in fact topological and follows a generalized bulk-boundary correspondence of higher-order: not the surfaces of the crystal, but its hinges host topologica…
Binary bismuth chalcogenides Bi$_2$Se$_3$, Bi$_2$Te$_3$, and related materials are currently being extensively investigated as the reference topological insulators (TIs) due to their simple surface-state band dispersion (single Dirac cone) and relatively large bulk band gaps. Nanostructures of TIs are of particular interest as an increased surface-to-volume ratio enhances the contribution of surfaces states, meaning they are promising candidates for potential device applications. So far, the vast majority of research efforts have focused on the low-energy (0001) surfaces, which correspond to n…
Some meta-stable polymorphs of bismuth monolayer (bismuthene) can host topologically nontrivial phases. However, it remains unclear if these polymorphs can become stable through interaction with a substrate, whether their topological properties are preserved, and how to design an optimal substrate to make the topological phase more robust. Using first-principles techniques we demonstrate that bismuthene polymorphs can become stable over silicon carbide (SiC), silicon (Si), silicon dioxide (SiO2) and that the proximity interaction in the heterostructures has a significant effect on the electron…
We study the electrical transport properties of ensembles of bismuth telluride (Bi2Te3) nanoplates grown by solution based chemical synthesis. Devices consisting of Bi2Te3 nanoplates are fabricated by surface treatment after dropping the solution on the structured gold plates and the temperature dependence of resistance shows a nonmetallic behavior. Symmetric tunneling behavior in I-V was observed in both our experimental results and theoretical calculation of surface conductance based on a simple Hamiltonian, which excludes carrier-carrier interactions. Here, we present two devices: one showi…
We have investigated the transport properties of topological insulator Bi2Se3 thin films grown using magnetron sputtering with an emphasis on understanding the behavior as a function of thickness. We show that thickness has a strong influence on all aspects of transport as the two-dimensional limit is approached. Bulk resistivity and Hall mobility show disproportionately large changes below 6 quintuple layer which we directly correlate to an increase in the bulk band gap of few-layer Bi2Se3, an effect that is concomitant with surface gap opening. A tendency to crossover from a metallic to an i…
The impedance behavior of pre-oxidized iron in liquid lead-bismuth eutectic (LBE) at 200 oC is studied using electrochemical impedance spectroscopy. The structures and resistance of oxide grown on iron oxidized in air at different temperatures and durations are compared. The results show that the resistance of the oxide film increases with increasing oxidizing temperature, due to the formation of a thicker scale and fewer defects. At the same temperature (600 oC), increasing the oxidation time can also reduce the defect concentration in the oxide film and improve the impedance of the oxide sca…
Quantum Spin Hall (QSH) insulators with a large topologically nontrivial bulk gap are crucial for future applications of the QSH effect. Among these, group III-V monolayers and their halides with chair structure (regular hexagonal framework, RHF) were widely studied. Using first-principles calculations, we propose a new structure model for the functionalized group III-V monolayers, which consist of rectangular GaBi-X2 (X=I, Br, Cl) monolayers with a distorted hexagonal framework (DHF). These structures have a much lower energy than the GaBi-X2 monolayers with chair structure. Remarkably, the D…
Hetero-epitaxial films based on bismuth telluride with excess of Te were grown by hat wall technique at the surface of the mica (muscovite). Galvanomagnetic properties of the thin films were measured, and quantum oscillations of the magnetoresistance were found at the temperatures below 10 K in the magnetic field from 6 to 14 T. From analysis of magnetoresistance oscillations the main surface state parameters of the films were determined. Expementally obtained Landau level index shift and its temperature dependence are consistent with Berry phase specific for topological Dirac surface states. …
Two-dimensional (2D) bismuth oxyselenide (Bi2O2Se) with high electron mobility is advantageous in future high-performance and flexible electronic and optoelectronic devices. However, transfer of thin Bi2O2Se flakes is rather challenging, restricting measurements of its mechanical properties and application exploration in flexible devices. Here, we develop a reliable and effective polydimethylsiloxane (PDMS)-mediated method that allows transferring thin Bi2O2Se flakes from grown substrates onto target substrates like micro-electro-mechanical system substrates. The high fidelity of the transferr…
Bi(0001) films with thicknesses up to several bilayers (BLs) are grown on Se-terminated Bi$_2$Se$_3$(0001) surfaces, and low energy electron diffraction (LEED), low energy ion scattering (LEIS) and atomic force microscopy (AFM) are used to investigate the surface composition, topography and atomic structure. For a single deposited Bi BL, the lattice constant matches that of the substrate and the Bi atoms adjacent to the uppermost Se atoms are located at fcc-like sites. When a 2nd Bi bilayer is deposited, it is incommensurate with the substrate. As the thickness of the deposited Bi film increas…
We study the possibility of pressure-induced transitions from a normal semiconductor to a topological insulator (TI) in bismuth tellurohalides using density functional theory and tight-binding method. In BiTeI this transition is realized through the formation of an intermediate phase, a Weyl semimetal, that leads to modification of surface state dispersions. In the topologically trivial phase, the surface states exhibit a Bychkov-Rashba type dispersion. The Weyl semimetal phase exists in a narrow pressure interval of 0.2 GPa. After the Weyl semimetal--TI transition occurs, the surface electron…
The major breakthroughs in the understanding of topological materials over the past decade were all triggered by the discovery of the Z$_2$ topological insulator (TI). In three dimensions (3D), the TI is classified as either "strong" or "weak", and experimental confirmations of the strong topological insulator (STI) rapidly followed the theoretical predictions. In contrast, the weak topological insulator has so far eluded experimental verification, since the topological surface states emerge only on particular side surfaces which are typically undetectable in real 3D crystals. Here we provide …
Monoclinic scheelite bismuth vanadate (BiVO4) is a promising photoanode for water splitting yet the PEC performance is limited due to its relatively higher (2.4 eV) band gap. Here, we successfully decreased its the band gap to 1.72 eV by controlled antimony alloying. Low bandgap antimony alloyed bismuth vanadium oxide (Sb:BiVO4) thin film was prepared by RF sputtering of high purity homemade target, fabricated by solid-state reaction using a mixture of Sb2O3, Bi2O3, and V2O5 powders with desired stoichiometric ratios. Several growth parameters, powder crystallography, post-deposition effects, …
Combining angle-resolved photoemission spectroscopy and magneto-transport measurements, we systematically investigated the possible origin of the extreme magnetoresistance in Pr/Sm mono-antimonides/bismuthides (PrSb, SmSb, PrBi, SmBi). Our photoemission measurements reveal that the bulk band inversion and surface states are absent (present) in Pr/Sm antimonides (bismuthides), implying that topological surface states are unlikely to play an important role for the observed extreme magnetoresistance. We found that the electron-hole compensation is well satisfied in all these compounds and the bul…
A two-dimensional (2D) Weyl semimetal featuring a spin-polarized linear band dispersion and a nodal Fermi surface is a new topological phase of matter. It is a solid-state realization of Weyl fermions in an intrinsic 2D system. The nontrivial topology of 2D Weyl cones guarantees the existence of a new form of topologically protected boundary states, Fermi string edge states. In this work, we report the realization of a 2D Weyl semimetal in monolayer-thick epitaxial bismuthene grown on SnS(Se) substrate. The intrinsic band gap of bismuthene is eliminated by the space-inversion-symmetry-breaking…
The interface between a solid and vacuum can become electronically distinct from the bulk. This feature, encountered in the case of quantum Hall effect, has a manifestation in insulators with topologically protected metallic surface states. Non-trivial Berry curvature of the Bloch waves or periodically driven perturbation are known to generate it. Here, by studying the angle-dependent magnetoresistance in prismatic bismuth crystals of different shapes, we detect a robust surface contribution to electric conductivity when the magnetic field is aligned parallel to a two-dimensional boundary betw…
In order to determine the role of non-thermal transport of hot carriers which is decisive for the dissipation of energy in condensed matter we performed time-resolved broadband femtosecond transient reflectivity measurements on $7-197 \mathrm{nm}$ thick Bi(111) films epitaxially grown on Si(111). We monitored the behavior of the Fourier amplitude and the central frequency of the coherent $A_\mathrm{1g}$ phonon mode as function of the incident fluence, film thickness, and probe wavelength in the range of $580 -700 \mathrm{nm}$. The frequency redshift that follows photoexcitation was used as a r…
We report ab initio calculations showing that a single one-dimensional extended defect can originate topologically-protected metallic states in the bulk of two-dimensional topological insulators. We find that a narrow extended defect composed of periodic units consisting of one octogonal and two pentagonal rings embedded in the hexagonal bulk of a bismuth bilayer introduces two pairs of one-dimensional Dirac-fermion states with opposite spin-momentum locking. Although both Dirac pairs are localized along the extended-defect core, their interactions are screened due to the trivial topological n…
Highly sensitive and fast photodetector devices with CdSe quantum nanowires as active elements have been developed exploiting the advantages of electro- and wet-chemical routes. Bismuth nanoparticles electrochemically synthesized directly onto interdigitating platinum electrodes serve as catalysts in the following solution-liquid-solid synthesis of quantum nanowires directly on immersed substrates under mild conditions at low temperature. This fast and simple preparation process leads to a photodetector device with a film of nanowires of limited thickness bridging the electrode gaps, in which …
Topological insulators (TIs) like Bi$_2$Se$_3$ are a class of material with topologically protected surface states in which spin-momentum locking may enable spin-polarized and defect-tolerant transport. In this work, we achieved the epitaxial growth of Bi$_2$Se$_3$ thin films on germanium, which is a key material for microelectronics. Germanium also exhibits interesting properties with respect to the electron spin such as a spin diffusion length of several micrometers at room temperature. By growing Bi$_2$Se$_3$ on germanium, we aim at combining the long spin diffusion length of Ge with the sp…
Topologically protected chiral skyrmion is an intriguing spin texture, which has attracted much attention because of fundamental research and future spintronic applications. MnSi with the non-centrosymmetric structure is well-known material hosting skyrmion phase. To date, preparation of MnSi crystals has been investigated by using special instruments with ultrahigh vacuum chamber. Here, we introduce a facile way to grow MnSi films on sapphire, which is in relatively low vacuum environment of conventional magnetron sputtering. Magnetotransport properties including Hall resistivity measurements…
Topological insulator (TI) materials are exciting candidates for integration into next-generation memory and logic devices because of their potential for efficient, low-energy-consumption switching of magnetization. Specifically, the family of bismuth chalcogenides offers efficient spin-to-charge conversion because of its large spin-orbit coupling and spin-momentum locking of surface states. However, a major obstacle to realizing the promise of TIs is the thin-film materials' quality, which lags behind that of epitaxially grown semiconductors. In contrast to the latter systems, the Bi-chalcoge…
Ultrathin bismuth-yttrium iron garnet films with tunable magnetic anisotropy
ETH Zurich（苏黎世联邦理工学院）；Université Grenoble Alpes, CNRS, Institut Néel（格勒诺布尔阿尔卑斯大学，法国国家科学研究中心，内耳研究所）；Kyoto University（京都大学）；University of Konstanz（康斯坦茨大学）；Instituto de Nanociencia y Materiales de Aragón, CSIC（阿拉贡纳米科学与材料研究所，西班牙国家研究委员会）；Universidad de Zaragoza（萨拉戈萨大学）
Stanene has been predicted to be a two-dimensional topological insulator (2DTI). Its low-buckled atomic geometry and the enhanced spin-orbit coupling are expected to cause a prominent quantum spin hall (QSH) effect. However, most of the experimentally grown stanene to date displays a metallic state without a real gap, possibly due to the chemical coupling with the substrate and the stress applied by the substrate. Here,we demonstrate an efficient way of tuning the atomic buckling in stanene to open a topologically nontrivial energy gap. Via tuning the growth kinetics, we obtain not only the lo…
InAs-based two-dimensional electron systems grown on lattice mismatched InP substrates offer a robust platform for the pursuit of topologically protected quantum computing. We investigated strained composite quantum wells of In$_{0.75}$Ga$_{0.25}$As/InAs/In$_{0.75}$Ga$_{0.25}$As with In$_{0.75}$Al$_{0.25}$As barriers. By optimizing the widths of the In$_{0.75}$Ga$_{0.25}$As layers, the In$_{0.75}$Al$_{0.25}$As barrier, and the InAs quantum well we demonstrate mobility in excess of $1 \times 10^{6}\,$cm$^{2}/$Vs. Mobility vs. density data indicates that scattering is dominated by a residual thr…
We theoretically study the magnon spin thermal transport using a strong coupling approach in pyrochlore iridate trilayer thin films grown along the [111] direction. As a result of the Dzyaloshinskii-Moriya interaction (DMI), the spin configuration of the ground state is an all-in/all-out ordering on neighboring tetrahedra of the pyrochlore lattice. In such a state, the system has an inversion symmetry and a Nernst-type thermal spin current response is well defined. We calculate the temperature dependence of the magnon Nernst response with respect to the magnon band topology controlled by the s…
Bismuth selenide Bi$_2$Se$_3$ was grown by molecular beam epitaxy while carrier density and mobility were measured directly \emph{in situ} as a function of film thickness. Carrier density shows high interface n-doping (1.5 x 10$^{13}$ cm$^{-2}$) at the onset of film conduction, and bulk dopant density of $\sim$5 x 10$^{18}$ cm$^{-3}$, roughly independent of growth temperature profile. Mobility depends more strongly on the growth temperature and is related to the crystalline quality of the samples quantified by \emph{ex-situ} AFM measurements. These results indicate that Bi$_2$Se$_3$ as prepare…
We report on the structural and electronic properties of a single bismuth layer intercalated underneath a graphene layer grown on an Ir(111) single crystal. Scanning tunneling microscopy (STM) reveals a hexagonal surface structure and a dislocation network upon Bi intercalation, which we attribute to a $\sqrt{3}\times\sqrt{3}R30°$ Bi structure on the underlying Ir(111) surface. Ab-initio calculations show that this Bi structure is the most energetically favorable, and also illustrate that STM measurements are most sensitive to C atoms in close proximity to intercalated Bi atoms. Additionally, …
Extremely large non-saturating magnetoresistance has recently been reported for a large number of both topologically trivial and non-trivial materials. Different mechanisms have been proposed to explain the observed magnetotransport properties, yet without arriving to definitive conclusions or portraying a global picture. In this work, we investigate the transverse magnetoresistance of materials by combining the Fermi surfaces calculated from first principles with the Boltzmann transport theory approach relying on the semiclassical model and the relaxation time approximation. We first consider…
Stanene, the two-dimensional monolayer form of tin, has been predicted to be a 2D topological insulator due to its large spin--orbit interaction. However, a clear experimental demonstration of stanene's topologically nontrivial properties has eluded observation, in part because of the difficulty of choosing a substrate on which stanene will remain topologically nontrivial. In this paper, we present first-principles density functional theory (DFT) calculations of epitaxial monolayer stanene grown on the (0001) surface of alumina, Al$_{2}$O$_{3}$, as well as free-standing decorated stanene under…
The growth and characterization of Bismuth (Bi) substituted YIG (Bi-YIG, Bi0.1Y2.9Fe5O12) thin films are reported. Pulsed laser deposited (PLD) films with thicknesses ranging from 20 to 150 nm were grown on Gadolinium Gallium Garnet substrates. Two substrate orientations of (100) and (111) were considered. The enhanced distribution of Bi3+ ions at dodecahedral site along (111) is observed to lead to an increment in lattice constant from 12.379 angstrom in (100) to 12.415 angstrom in (111) oriented films. Atomic force microscopy images showed decreasing roughness with increasing film thickness.…
