We report the magneto-conductivity analysis of Bi2Se3 single crystal at different temperatures in a magnetic field range of 14Tesla. The single crystals are grown by the self-flux method and characterized through X-ray diffraction, Scanning Electron Microscopy, and Raman Spectroscopy. The single crystals show magnetoresistance (MR) of around 380 percent at a magnetic field of 14T and a temperature of 5K. The Hikami Larkin Nagaoka (HLN) equation has been used to fit the magneto-conductivity (MC) data. However, the HLN fitted curve deviates at higher magnetic fields above 1 Tesla, suggesting that the role of surface driven conductivity suppresses with an increasing magnetic field. This article proposes a speculative model comprising of surface-driven HLN and added quantum diffusive and bulk carriers driven classical terms. The model successfully explains the MC of the Bi2Se3 single crystal at various temperatures (5 to 200K) and applied magnetic fields (up to 14Tesla).
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…
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…
Ultrathin (~3 quintuple layer) field-effect transistors (FETs) of topological insulator Bi2Se3 are prepared by mechanical exfoliation on 300nm SiO2/Si susbtrates. Temperature- and gate-voltage dependent conductance measurements show that ultrathin Bi2Se3 FETs are n-type, and have a clear OFF state at negative gate voltage, with activated temperature-dependent conductance and energy barriers up to 250 meV.
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…
Bismuth Selenide (Bi2Se3) is a topological insulator exhibiting helical spin polarization and strong spin-orbit coupling. The spin-orbit coupling links the charge current to spin current via the spin Hall effect (SHE). We demonstrate a Bi2Se3 spin detector by injecting the pure spin current from a magnetic permalloy layer to a Bi2Se3 thin film and detect the inverse SHE in Bi2Se3. The spin Hall angle of Bi2Se3 is found to be 0.0093 and the spin diffusion length in Bi2Se3 to be 6.2 nm at room temperature. Our results suggest that topological insulators with strong spin-orbit coupling can be use…
We adopted and extended an efficient Grüneisen formalism to study the phonon anharmonicity and linear thermal expansion coefficients (TECs) of trigonal bismuth selenide (Bi$_2$Se$_3$) and antimony telluride (Sb$_2$Te$_3$). Anharmonicity of the systems is studied via extensive calculation of Grüneisen parameters that exploit symmetry-preserving deformations. Consistent with experimental findings, a large anisotropy between the TECs in the $a$ and $c$ directions is found. The larger anharmonicity inherent in Sb$_2$Te$_3$, as compared to Bi$_2$Se$_3$ is offset by the volumetric effect, resulting …
Cumulative X-ray Damage in Bismuth Selenide Examined by Simultaneous TXM and XRD
Stanford University（斯坦福大学）；SLAC National Accelerator Laboratory（SLAC国家加速器实验室）；PULSE Institute（脉冲研究所）；Lawrence Livermore National Laboratory（劳伦斯利弗莫尔国家实验室）；Pohang Accelerator Laboratory（浦项加速器实验室）；Pohang University of Science and Technology（浦项科技大学）；European Radiation Synchrotron Facility（欧洲辐射同步辐射装置）；Nevada National Security Site（内华达国家安全区）；Sogang University（西江大学）
We report that Bi$_2$Se$_3$ thin films can be epitaxially grown on SrTiO$_{3}$ substrates, which allow for very large tunablity in carrier density with a back-gate. The observed low field magnetoconductivity due to weak anti-localization (WAL) has a very weak gate-voltage dependence unless the electron density is reduced to very low values. Such a transition in WAL is correlated with unusual changes in longitudinal and Hall resistivities. Our results suggest much suppressed bulk conductivity at large negative gate-voltages and a possible role of surface states in the WAL phenomena. This work m…
Impact collision ion scattering spectroscopy (ICISS), which is a variation of low energy ion scattering (LEIS) that employs large scattering angles, is performed on Bi2Se3 surfaces prepared by ion bombardment and annealing (IBA). ICISS angular scans are collected experimentally and simulated numerically along the [120] and [-1 -2 0] azimuths, and the match of the positions of the flux peaks shows that the top three atomic layers are bulk-terminated. A newly observed feature is identified as a minimum in the multiple scattering background when the ion beam incidence is along a low index directi…
$\require{mhchem}$Topological superconductivity is of great contemporary interest and has been proposed in doped $\ce{Bi2Se3}$ in which electron-donating atoms such as Cu, Sr or Nb have been intercalated into the $\ce{Bi2Se3}$ structure. For $\ce{Nb_{x}Bi2Se3}$, with $\text{T}_\text{c} \sim 3 \ \text{K}$, it is assumed in the literature that Nb is inserted in the van der Waals gap. However, in this work an alternative origin for the superconductivity in Nb-doped $\ce{Bi2Se3}$ is established. In contrast to previous reports, it is deduced that Nb intercalation in $\ce{Bi2Se3}$ does not take pla…
We report the discovery of a temperature induced phase transition between the αand βstructures of antimonene. When antimony is deposited at room temperature on bismuth selenide, it forms domains of α-antimonene having different orientations with respect to the substrate. During a mild annealing, the βphase grows and prevails over the αphase, eventually forming a single domain that perfectly matches the surface lattice structure of bismuth selenide. First principles thermodynamics calculations of this van der Waals heterostructure explain the different temperature-dependent stability of the two…
Inspired by the recent first-principles calculations showing the high thermoelectric performance of layered pnictogen chalcogenides, we experimentally characterise the crystal structure and high-temperature transport properties of the layered antimony selenides REOSbSe2 (RE = La, Ce). The crystal structure of REOSbSe2 was the tetragonal P4/nmm space group, consisting of alternate stacks of SbSe2 and REO layers. These two compounds were n-type semiconductors. The optical band gaps of LaOSbSe2 and CeOSbSe2 were evaluated to be 1.0 and 0.6 eV, respectively. The room-temperature thermal conductivi…
The possibility to control the magnetic properties of a material with an electric field at room temperature is highly desirable for modern applications. Moreover, a coupling between magnetic and electric orders within a single material presenting a wide range of exceptional physical properties, such as bismuth iron garnet (BIG), may lead to great advances in the field of spintronic applications. In particular, the combination of the magnetoelectric (ME) coupling with the low damping of spin waves in BIG can allow the control and manipulation of spin waves by an electric field in magnonic devic…
Here, we examine the influence of surface chemical reactivity toward ambient gases on the performance of nanodevices based on two-dimensional materials "beyond graphene" and novel topological phases of matter. While surface oxidation in ambient conditions was observed for silicene and phosphorene with subsequent reduction of the mobility of charge carriers, nanodevices with active channels of indium selenide, bismuth chalcogenides and transition-metal dichalcogenides are stable in air. However, air-exposed indium selenide suffers of p-type doping due to water decomposition on Se vacancies, whe…
Bismuth chalcogenides and lead telluride/selenide alloys exhibit exceptional thermoelectric properties which could be harnessed for power generation and device applications. Since phonons play a significant role in achieving these desired properties, quantifying the interaction between phonons and electrons, which is encoded in the Eliashberg function of a material, is of immense importance. However, its precise extraction has in part been limited due to the lack of local experimental probes. Here we construct a method to directly extract the Eliashberg function using Landau level spectroscopy…
University of Duisburg-Essen（杜伊斯堡-埃森大学）；European Organization for Nuclear Research (CERN)（欧洲核子研究组织（CERN））；Universidade de Aveiro（阿威罗大学）；Institute for Research in Fundamental Sciences (IPM)（基础科学研究所（IPM））
In this paper, we first review fundamental aspects of magnetoresistance in multi-valley systems based on the semiclassical theory. Then we will review experimental evidence and theoretical understanding of magnetoresistance in an archetypal multi-valley system, where the electric conductivity is set by the sum of the contributions of different valleys. Bulk bismuth has three valleys with an extremely anisotropic effective mass. As a consequence, the magnetoconductivity in each valley is extremely sensitive to the orientation of the magnetic field. Therefore, a rotating magnetic field plays the…
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. …
Bismuth ferrite (BiFeO3) is one of the most promising multiferroics with a sufficiently high ferroelectric (FE) and antiferromagnetic transition temperatures, and magnetoelectric (ME) coupling coefficient at room temperature, and thus it is highly sensitive to the impact of cross-influence of applied electric and magnetic fields. According to the urgent demands of nanotechnology miniaturization for ultra-high density data storage in advanced nonvolatile memory cells, it is very important to reduce the sizes of multiferroic nanoparticles in the self-assembled arrays without serious deterioratio…
Bismuth Selenide is a two-dimensional topological insulator material composed of stacked quintuple layers (QL). The layers are held together by a weak van der Waals force that enables surface preparation by cleaving. Low energy ion scattering experiments (LEIS) show that Bi2Se3 cleaved under ultra-high vacuum (UHV) has a Se-terminated structure that is consistent with cleaving between QLs. Comparison of experimental data to molecular dynamics simulations confirms the Se-termination and provides an estimate of the surface relaxation.
We analyze the coupling between the ferroelectric and magnetic order parameters in the magnetoelectric multiferroic BiFeO_3 using density functional theory within the local spin density approximation and the LSDA+U method. We show that weak ferromagnetism of the Dzyaloshinskii-Moriya type occurs in this material, and we analyze the coupling between the resulting magnetization and the structural distortions. We explore the possibility of electric-field-induced magnetization reversal and show that, although it is unlikely to be realized in BiFeO_3, it is not in general impossible. Finally we out…
We present an extensive study of angle-dependent transverse magnetoresistance in bismuth, with a magnetic field perpendicular to the applied electric current and rotating in three distinct crystallographic planes. The observed angular oscillations are confronted with the expectations of semi-classic transport theory for a multi-valley system with anisotropic mobility and the agreement allows us to quantify the components of the mobility tensor for both electrons and holes. A quadratic temperature dependence is resolved. As Hartman argued long ago, this indicates that inelastic resistivity in b…
Thermoelectric (TE) materials research plays a vital role in heat-to-electrical energy conversion and refrigeration applications. Bismuth-antimony (Bi-Sb) alloy is a promising material for thermoelectric cooling. Herein, a high figure of merit, ZT, near 0.6 at cryogenic temperatures (100-150K) has been achieved in melt-spun n-type Bi85Sb15 bulk samples consisting of micron-size grains. The achieved ZT is nearly 50 percents higher than polycrystalline averaged single crystal ZT of ~0.4, and it is also significantly higher than ZT of less than ~0.3 measured below 150K in Bi-Te alloys commonly us…
We report on van der Waals epitaxial growth, materials characterization and magnetotransport experiments in crystalline nanosheets of Bismuth Telluro-Sulfide (BTS). Highly layered, good-quality crystalline nanosheets of BTS are obtained on SiO$_2$ and muscovite mica. Weak-antilocalization (WAL), electron-electron interaction-driven insulating ground state and universal conductance fluctuations are observed in magnetotransport experiments on BTS devices. Temperature, thickness and magnetic field dependence of the transport data indicate the presence of two-dimensional surface states along with …
Three dimensional topological insulator bismuth selenide (Bi2Se3) 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 Bi2Se3/Co40Fe40B20 devices at different temperatures by spin torque ferromagnetic resonance measurements. As 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 …
We use a magnetothermal resistance method to measure the lattice thermal conductivity of a single crystal of Bi$_2$Te$_3$ from 5 to 60 K. We apply a large transverse magnetic field to suppress the electronic thermal conduction while measuring thermal conductivity and electrical resistivity. The lattice thermal conductivity is then calculated by extrapolating the thermal conductivity versus electrical conductivity curve to a zero electrical conductivity value. Our results show that the measured phonon thermal conductivity follows the $e^{(Δ_{min}/T)}$ temperature dependence and the Lorenz ratio…
Metallic Bi2Te3 crystalline sheets with the room-temperature resistivity of above 10 mΩ cm were prepared and their magnetoresistive transport was measured in a field of up to 9 Tesla. The Shubnikov de Haas oscillations were identified from the secondly-derived magnetoresistance curves. While changing the angle between the field and normal axis of the sheets, we find that the oscillation periods present a cosine dependence on the angle. This indicates a two-dimensional transport due to the surface state. The work reveals a resolvable surface contribution to the overall conduction even in a meta…
For the first time, magnetoresistive properties of the single crystal of HgSe with a low electron concentration were studied in wide range of temperature and magnetic field. Some fundamental parameters of spectrum and scattering of electrons were experimentally determined. Two important features of magnetic transport were found - strong transverse magnetoresistance (MR) and negative longitudinal MR, which can indicate the existence of the topological phase of the Weyl semimetal (WSM) in HgSe. Taking this hypothesis into account we suggest a modified band diagram of the mercury selenide at low …
The semiclassical transport theory is especially powerful for investigating galvanomagnetic effects. Generally, the semiclassical theory is applicable only in weak fields because it does not consider Landau quantization. Herein, we extend the conventional semiclassical theory by considering Landau quantization through the field dependence of carrier density in semimetals. The extended semiclassical theory is applicable even in strong fields, where Landau quantization is noticeable. Using this new approach, we explain the qualitative change in the angular dependence of transverse magnetoresista…
Field driven Metal-Insulator transition in rhombohedral Bismuth and Arsenic crystals
CSIR-National Physical Laboratory（印度国家物理实验室）；Academy of Scientific and Innovative Research (AcSIR)（科学与创新研究学院）；Institute of Mathematical Sciences（数学科学研究所）
We report results of investigation of the low-frequency excess noise in device channels made from topological insulators - a new class of materials with a bulk insulating gap and conducting surface states. The thin-film bismuth selenide samples were prepared by the "graphene-like" mechanical exfoliation from bulk crystals. The fabricated four-contact devices had linear current - voltage characteristics in the low-bias regime. The current fluctuations had the noise spectral density proportional to 1/f for the frequency f below 10 kHz. The noise spectral density followed the quadratic dependence…
Hot wall technique was used to grow block single crystal films of Bi_2Te_3 and solid solutions of Bi_(0.5)Sb_(1.5)Te_3 on mica (muscovite) substrates. X-ray diffraction studies demonstrated that the crystalline c-axis in the films was normal to the substrate plane. Seebeck coefficient, electrical conductivity and magnetoresistivity tensor components were measured at various orientations of magnetic and electric fields in the temperature interval 77-300 K and magnetic field up to 14 T. Scattering mechanism of charge carriers in the films were studied using temperature dependences of the degener…
Bismuth Selenide (Bi2Se3) is a topological insulator with a two-dimensional layered structure that enables clean and well-ordered surfaces to be prepared by cleaving. Although some studies have demonstrated that the cleaved surface is terminated with Se, as expected from the bulk crystal structure, other reports have indicated either a Bi- or mixed-termination. Low energy ion scattering (LEIS), low energy electron diffraction (LEED) and x-ray photoelectron spectroscopy (XPS) are used here to compare surfaces prepared by ex situ cleaving, in situ cleaving, and ion bombardment and annealing (IBA…
Bismuth chalcogenides are the most studied 3D topological insulators. As a rule, at low temperatures thin films of these materials demonstrate positive magnetoresistance due to weak antilocalization. Weak antilocalization should lead to resistivity decrease at low temperatures; in experiments, however, resistivity grows as temperature decreases. From transport measurements for several thin films (with various carrier density, thickness, and carrier mobility), and by using purely phenomenological approach, with no microscopic theory, we show that the low temperature growth of the resistivity is…
Metal and magnetic overlayers alter the surface of the topological insulator (TI) bismuth selenide (Bi$_2$Se$_3$) through proximity effects but also by changing the composition and chemical structure of the Bi$_2$Se$_3$ sub-surface. The interface between Bi$_2$Se$_3$ and Mn metal or manganese selenide was explored using x-ray photoelectron spectroscopy (XPS) revealing chemical and electronic changes at the interface. Depositing Mn metal on Bi$_2$Se$_3$ without an external source of Se shows unexpected bonding within the Mn layer due to Mn-Se bonding as Se diffuses out of the Bi$_2$Se$_3$ layer…
We implement the molecular beam epitaxy method to embed the black-phosphorus-like bismuth nanosheets into the bulk ferromagnet Cr$_2$Te$_3$. As a typical surfactant, bismuth lowers the surface tensions and mediates the layer-by-layer growth of Cr$_2$Te$_3$. Meanwhile, the bismuth atoms precipitate into black-phosphorus-like nanosheets with the lateral size of several tens of nanometers. In Cr$_2$Te$_3$ embedded with Bi-nanosheets, we observe simultaneously a large topological Hall effect together with the magnetic susceptibility plateau and magnetoresistivity anomaly. As a control experiment, …
The Fermi surface of elemental bismuth consists of three small rotationally equivalent electron pockets, offering a valley degree of freedom to charge carriers. A relatively small magnetic field can confine electrons to their lowest Landau level. This is the quantum limit attained in other dilute metals upon application of sufficiently strong magnetic field. Here, we report on the observation of another threshold magnetic field never encountered before in any other solid. Above this field, $B_{\rm{empty}}$, one or two valleys become totally empty. Drying up a Fermi sea by magnetic field in the…
Topological insulators are immensely investigated for their surface states related properties as these materials can be used for various spintronics, quantum computing, and optoelectronics applications. In this perspective, different thicknesses of bismuth selenide thin films are deposited on the 250 nm SiO2 substrate with the help of thermal deposition. The motive of this study is to investigate the surface and bulk-related behaviour with different thicknesses. The deposited films are characterized through GI-XRD (grazing incidence X-ray diffractometer) and Raman spectroscopy, which ensure th…
Bismuth selenide is both a thermoelectric material and topological insulator. Defects and dopants create conduction in thermoelectric applications. However, such defects may degrade the performance as a topological insulator (TI). Magnetic impurities such as iron open a band gap at the Dirac point on the surface. Since magnetically-doped TIs are important in technological applications, a good understanding of their properties is needed. In this article, 77Se nuclear magnetic resonance (NMR) spectroscopy has been used to investigate Fe-doped Bi2Se3. Spin-lattice relaxation measurements indicate…
Monolayer van der Waals (vdW) magnets provide an exciting opportunity for exploring two-dimensional (2D) magnetism for scientific and technological advances, but the intrinsic ferromagnetism has only been observed at low temperatures. Here, we report the observation of room temperature ferromagnetism in manganese selenide (MnSe$_x$) films grown by molecular beam epitaxy (MBE). Magnetic and structural characterization provides strong evidence that in the monolayer limit, the ferromagnetism originates from a vdW manganese diselenide (MnSe$_2$) monolayer, while for thicker films it could originat…
Three-dimensional (3D) Dirac semimetals are new quantum materials and can be viewed as 3D analogues of graphene. Many fascinating electronic properties have been proposed and realized in 3D Dirac semimetals, which demonstrates their potential applications in next generation quantum devices. Bismuth-antimony Bi1-xSbx can be tuned from a topological insulator to a band insulator through a quantum critical point at x ~ 4%, where 3D Dirac fermions appear. Here, we report on a magnetotransport study of Bi1-xSbx at such a quantum critical point. An unusual magnetic-field induced semimetal-semiconduc…
Here, we report the catalytic degradation of organic compounds by exploiting the magnetoelectric (ME) nature of cobalt ferrite-bismuth ferrite (CFO-BFO) core-shell nanoparticles. The combination of magnetostrictive CFO with the multiferroic BFO gives rise to a magnetoelectric engine that purifies water under wireless magnetic fields via advanced oxidation processes, without involvement of any sacrificial molecules or co-catalysts. Magnetostrictive CoFe2O4 nanoparticles are fabricated using hydrothermal synthesis, followed by sol-gel synthesis to create the multiferroic BiFeO3 shell. We perform…
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…
We consider the effect of electron-phonon coupling in semimetals in high magnetic fields, with regard to elastic modes that can lead to a redistribution of carriers between pockets. We show that in a clean three dimensional system, at each Landau level crossing, this leads to a discontinuity in the magnetostriction, and a divergent contribution to the elastic modulus. We estimate the magnitude of this effect in the group V semimetal Bismuth.
Magnetic phase transitions in multiferroic bismuth ferrite (BiFeO3) induced by magnetic field, epitaxial strain, and composition modification are considered. These transitions from a spatially modulated spin spiral state to a homogenous antiferromagnetic one are accompanied by the release of latent magnetization and a linear magnetoelectric effect that makes BiFeO3-based materials efficient room-temperature single phase multiferroics.
A mechanism is proposed based on the Kubo formula to generate a spin-polarized magneto-optical current of Dirac electrons in solids which have strong spin-orbit interactions such as bismuth. The ac current response functions are calculated in the isotropic Wolff model under an external magnetic field, and the selection rules for Dirac electrons are obtained. By using the circularly polarized light and tuning its frequency, one can excite electrons concentrated in the spin-polarized lowest Landau level when the chemical potential locates in the band gap, so that spin-polarization in the magneto…
We report on the low-frequency current fluctuations and electronic noise in thin-films made of bismuth selenide topological insulators. The films were prepared via the graphene-like mechanical exfoliation and used as the current conducting channels in the four- and two-contact devices. Analysis of the resistance dependence on the film thickness indicates that the surface contribution to conductance is dominant in our samples. It was established that the current fluctuations have the noise spectrum close to the pure 1/f in the frequency range from 1 to 10 kHz (f is the frequency). The relative …
