Search

The authors have requested that this preprint be removed from Research Square.

We successfully identified native point defects that occur in Bi2Te3 crystals by combining high-resolution bias-dependent scanning tunneling microscopy and density functional theory based calculations. As-grown Bi2Te3 crystals contain vacancies, antisites, and interstitial defects that may result in bulk conductivity and therefore may change the insulating bulk character. Here, we demonstrate the interplay between the growth conditions and the density of different types of native near-surface defects. In particular, scanning tunneling spectroscopy reveals the dependence on not only the local atomic environment but also on the growth kinetics and the resulting sample doping from n-type toward intrinsic crystals with the Fermi level positioned inside the energy gap. Our results establish a bias-dependent STM signature of the Bi2Te3 native defects and shed light on the link between the native defects and the electronic properties of Bi2Te3, which is relevant for the synthesis of topological insulator materials and the related functional properties.

Description, Kagome ferromagnet Fe3Sn exhibits large magnetic thermoelectric effect due to Berry curvature enhanced by a nodal plane., Anomalous Nernst effect (ANE), converting a heat flow to transverse electric voltage, originates from the Berry phase of electronic wave function near the Fermi energy EF. Thus, the ANE provides a sensitive probe to detect a topological state that produces large Berry curvature. In addition, a magnet that exhibits a large ANE using low-cost and safe elements will be useful to develop a novel energy harvesting technology. Here, we report our observation of a high ANE exceeding 3 microvolts per kelvin above room temperature in the kagome ferromagnet Fe3Sn with the Curie temperature of 760 kelvin. Our theoretical analysis clarifies that a “nodal plane” produces a flat hexagonal frame with strongly enhanced Berry curvature, resulting in the large ANE. Our discovery of the large ANE in Fe3Sn opens the path for the previously unexplored functionality of flat degenerate electronic states and for developing flexible film thermopile and heat current sensors.

The off-diagonal (electric, thermal, and thermoelectric) transport coefficients of a solid can acquire an anomalous component due to the nontrivial topology of the Bloch waves. We present a study of the anomalous Hall effect (AHE), anomalous Nernst effect (ANE), and thermal Hall effect in the Heusler-Weyl ferromagnet ${\mathrm{Co}}_{2}\mathrm{MnGa}$. The anomalous Wiedemann-Franz law, linking electric and thermal responses, was found to be valid over the whole temperature window. This indicates that the AHE has an intrinsic origin and the Berry spectrum is smooth in the immediate vicinity of the Fermi level. We extract ${\ensuremath{\alpha}}_{ij}^{A}$ from our ANE data and find that the ${\ensuremath{\alpha}}_{ij}^{A}/{\ensuremath{\sigma}}_{ij}^{A}$ ratio approaches ${k}_{B}/e$ at room temperature. Scrutinizing all topological magnets previously explored, we observe that this ratio is a sizable fraction of ${k}_{B}/e$ at room temperature. We provide a rough explanation for this feature by arguing that the two anomalous transverse coefficients depend on universal constants, the Berry curvature averaged over a window set by either the Fermi wavelength (for Hall) or the de Broglie thermal length (for Nernst). The universal scaling indicates that the widths of the two windows approaches each other at room temperature.

Quantum materials with strong transport responses to disparate physical quantities are of great fundamental significance and may hold technological potentials. The interplay between interactions and topology drive such responses through the effects of spontaneous symmetry breaking and the associated domain configurations on quantum transport. Here we provide a comprehensive description of the magnetism of Mn3Ge, an antiferromagnetic kagomebased semimetal with room temperature transport anomalies associated with topologically protected Weyl nodes. Using polarized neutron diffraction, we show the all-important magnetic structure is anti-chiral and coplanar carrying the symmetry of a ferromagnet without appreciable magnetization. We probe and classify the long wavelength excitations that determine its macroscopic responses including a set of collective magneto-elastic modes. We develop a phenomenological spin Hamiltonian with exchange, Dzyaloshinskii-Moriya, and crystal field interactions to describe its collective magnetism. The itinerant character of the magnetism that drives quantum transport is apparent in spin wave damping and extended magnetic interactions. Our work provides the scientific basis for manipulation of the chiral antiferromagnetic texture of Mn3Ge to control its topological quantum transport., Comment: Main text has 40 pages, 6 figures. Supplemental Information has 14 pages, 2 figures

Thermoelectric generation using the anomalous Nernst effect (ANE) has great potential for application in energy harvesting technology because the transverse geometry of the Nernst effect should enable efficient, large-area and flexible coverage of a heat source. For such applications to be viable, substantial improvements will be necessary not only for their performance but also for the associated material costs, safety and stability. In terms of the electronic structure, the anomalous Nernst effect (ANE) originates from the Berry curvature of the conduction electrons near the Fermi energy1,2. To design a large Berry curvature, several approaches have been considered using nodal points and lines in momentum space3–10. Here we perform a high-throughput computational search and find that 25 percent doping of aluminium and gallium in alpha iron, a naturally abundant and low-cost element, dramatically enhances the ANE by a factor of more than ten, reaching about 4 and 6 microvolts per kelvin at room temperature, respectively, close to the highest value reported so far. The comparison between experiment and theory indicates that the Fermi energy tuning to the nodal web—a flat band structure made of interconnected nodal lines—is the key for the strong enhancement in the transverse thermoelectric coefficient, reaching a value of about 5 amperes per kelvin per metre with a logarithmic temperature dependence. We have also succeeded in fabricating thin films that exhibit a large ANE at zero field, which could be suitable for designing low-cost, flexible microelectronic thermoelectric generators11–13. Aluminium- and gallium-doped iron compounds show a large anomalous Nernst effect owing to a topological electronic structure, and their films are potentially suitable for designing low-cost, flexible microelectronic thermoelectric generators.

In this work, we have studied the oxidation process of the bismuth doped graphene in the ambient air. Complete oxidation of the bismuth clusters and that of the graphene are firmly confirmed. The influence of oxygen on the graphene is characterized by means of Hall measurement and SdH oscillation. All transport measurements demonstrate a hole-type doping behavior. Our work also demonstrates that the short-range scattering mechanism is enhanced in doped graphene due to accumulated O-species adsorbates after being exposed in the atmosphere for 40 days and is suppressed after annealing. This investigation may open a new perspective for fabricating the graphene metal oxide devices.

Non-collinear antiferromagnet Mn3Sn is a functional material that exhibits the magneto-optical Kerr effect (MOKE) as well as the anomalous Hall effect, arising from the nonvanishing Berry curvature in the broken time-reversal symmetry lattice system likewise the ferromagnets. Mn3Ge, isostructural to Mn3Sn, is also expected to exhibit a similar MOKE but has not been demonstrated yet. In this study, we performed the MOKE measurement in a Mn3Ge single crystal and obtained a large polar MOKE signal (∼8.2 mdeg) and a longitudinal MOKE signal (∼5.6 mdeg). Furthermore, by applying hyperfine polishing and annealing to the surface, we rebuilt a homogenous surface and largely improved the reproducibility of the MOKE signal in Mn3Ge.

High-mobility (Smx Bi1-x )2 Se3 topological insulators (with x = 0.05) show a Curie temperature of about 52 K, and the carrier concentration and Fermi wave vector can be manipulated by intentional Te introduction with no significant influence on the Curie temperature. The origin of the ferromagnetism is attributed to the trivalent Sm dopant, as confirmed by X-ray magnetic circular dichroism and first-principles calculations. The carrier concentration is on the order of 10(19) cm(-3) and the mobility can reach about 7200 cm(2) V(-1) s(-1) with pronounced Shubnikov-de Haas oscillations.

We observe quantized Hall plateaus and Shubnikov de Haas oscillations in 10 at% Fe-doped Bi2Se3 flakes. All the features of the quantum transport coincide while normalizing the field-angle variable magnetoresistance to the perpendicular direction. The Hall step gives a specific contribution of ~1 e2/h per quintuple layer. This reveals a two-dimensional (2D) transport of the bulk electrons in the topological insulators. The crystal is demonstrated with an obvious ferromagnetism. Further evidences including a Berry phase of zero, a weak localization and a large effective mass rule out the contribution of the topological surface states (SS), suggesting that a great care should be taken to pindown the transport of the topological SS in topological insulators.

We investigated the topological insulator (TI) Bi

Topological insulators (TIs) are renowned for their exotic topological surface states (TSSs) that reside in the top atomic layers, and hence, detailed knowledge of the surface top atomic layers is of utmost importance. Here we present the remarkable morphology changes of Bi2Te3 surfaces, which have been freshly cleaved in air, upon subsequent systematic annealing in ultrahigh vacuum and the resulting effects on the local and area-averaging electronic properties of the surface states, which are investigated by combining scanning tunneling microscopy (STM), scanning tunneling spectroscopy (STS), and Auger electron spectroscopy (AES) experiments with density functional theory (DFT) calculations. Our findings demonstrate that the annealing induces the formation of a Bi bilayer atop the Bi2Te3 surface. The adlayer results in n-type doping, and the atomic defects act as scattering centers of the TSS electrons. We also investigated the annealing-induced Bi bilayer surface on Bi2Te3 via voltage-dependent quasi-particle-interference (QPI) mapping of the surface local density of states and via comparison with the calculated constant-energy contours and QPI patterns. We observed closed hexagonal patterns in the Fourier transform of real-space QPI maps with secondary outer spikes. DFT calculations attribute these complex QPI patterns to the appearance of a second cone due to the surface charge transfer between the Bi bilayer and the Bi2Te3. Annealing in ultrahigh vacuum offers a facile route for tuning of the topological properties and may yield similar results for other topological materials.

Employing the graphene sheets (GSs), the electron scattering constants are measured in the high-angle annular dark-field (HAADF) imaging by the scanning transmission electron microscopy. Single scattering is found to be dominant until the layer number of 200, complying with a simple relation of I = Io(1 - e(-tau/lambda)). The discrete layer counting of the GSs enables precise determination of incident depths. This work results values of lambda = 48.2, 61.4, 97.9 and 115.6 nm for 80, 120, 160 and 200 keV electrons, respectively. The uncertainties with the mean free paths and the cross sections are confined to 10 percent. The dependences on the electron beam energy and the collection angle are discussed based on a multislice simulation.

We report on the temperature-induced quantum decoupling between the surface states, demonstrated by weak antilocalization measurements, in the topological insulator Bi2−0.15(TeSe)3+0.15 nanoplates. The samples are prepared by a catalyst-free vapor–solid process with the dimension of 10 μm and the thickness of 20 nm. The channel indicator is extracted from the weak antilocalization, which presents a transition from 0.5 to 1 with the increasing temperature. This reveals the coherent decoupling between the two surface states, during which the dephasing length reaches the plate thickness. A bulk-mediated intersurface coupling model interprets the transition.

We report on the observation of complex superlattices at the surface of the topological insulator Bi2Te3. Scanning tunneling microscopy reveals the existence of two different periodic structures in addition to the Bi2Te3 atomic lattice, which is found to strongly affect the local electronic structure. These three different periodicities are interpreted to result from a single small in-plane rotation of the topmost quintuple layer only. Density functional theory calculations support the observed increase in the DOS near the Fermi level, and exclude the possibility that strain is at the origin of the observed Moire pattern. Exploration of Moire superlattices formed by the quintuple layers of topological insulators holds great potential for further tuning of the properties of topological insulators. Research Foundation - Flanders (FWO, Belgium); Flemish Concerted Research Action program (BOF KU Leuven) [GOA/14/007]; China Scholarship Council [2011624021]; FWO; U.S. National Science Foundation [DMR-1206354]; San Diego Supercomputer Center (SDSC) Trestles [DMR060009N]; National Key Projects for Basic Research of China [2013CB922103]; National Natural Science Foundation of China [91421109, 11522432]; PAPD project; Natural Science Foundation of Jiangsu Province [BK20130054] The research in Leuven and Antwerp has been supported by the Research Foundation - Flanders (FWO, Belgium). The research in Leuven received additional support from the Flemish Concerted Research Action program (BOF KU Leuven, Project No. GOA/14/007). Z.L. thanks the China Scholarship Council for financial support (No. 2011624021). K.S. acknowledges support from the FWO. K.P. was supported by U.S. National Science Foundation DMR-1206354 and San Diego Supercomputer Center (SDSC) Trestles under DMR060009N. T.C. and F.S. acknowledge the financial support of the National Key Projects for Basic Research of China (Grant Nos: 2013CB922103), the National Natural Science Foundation of China (Grant Nos: 91421109, 11522432), the PAPD project, and the Natural Science Foundation of Jiangsu Province (Grant BK20130054).

Thin Bi2Te3 flakes, with as few as 3 quintuple layers, are optically visualized on the SiO2-capped Si substrates. Their optical contrasts vary with the illumination wavelength, flake thickness and capping layers. The maximum contrast appears at the optimized light with the 570 nm wavelength. The contrast turns reversed when the flake is reduced to less than 20 quintuple layers. A calculation based on the Fresnel law describes the above observation with the constructions of the layer number-wave length-contrast three-dimensional (3D) diagram and the cap thickness-wavelength-contrast 3D diagram, applicative in the current studies of topological insulating flakes.

Few-layer graphene sheets were prepared by splitting expanded graphite using high-power sonication. Atomic-level calibrated scanning transmission electron microscopy was used to obtain efficient layer statistics, enabling optimization of the experimental conditions. This resulted in a two-step splitting mechanism in which the mean number of layers was first reduced to less than 20 by heating to 1100 °C and then to a few-layer region by a 5-min 104 W L−1 – power-density sonication. Raman spectroscopic analysis confirms the above mechanism and demonstrates that the sheets are largely free of defects and functional groups.

We present evidence for the existence and control of bulk-surface coupling in ${\mathrm{Bi}}_{2}{\mathrm{Te}}_{2}\mathrm{Se}$ nanoribbons. Our magnetoresistance measurements reveal that the number of coherent channels contributing to quantum interference in the nanoribbons changes abruptly when the film thickness exceeds the bulk phase relaxation length. We interpret this observation as an evidence for bulk-mediated coupling between metallic states located on opposite surfaces. This hypothesis is supported by additional magnetoresistance measurements conducted under a set of gate voltages and in a parallel magnetic field, the latter of which alters the intersurface coupling in a controllable way.

Enhancing the transport contribution of surface states in topological insulators is vital if they are to be incorporated into practical devices. Such efforts have been limited by the defect behaviour of Bi2Te3 (Se3) topological materials, where the subtle bulk carrier from intrinsic defects is dominant over the surface electrons. Compensating such defect carriers is unexpectedly achieved in (Cu0.1Bi0.9)2Te3.06 crystals. Here we report the suppression of the bulk conductance of the material by four orders of magnitude by intense ageing. The weak antilocalization analysis, Shubnikov–de Haas oscillations and scanning tunnelling spectroscopy corroborate the transport of the topological surface states. Scanning tunnelling microscopy reveals that Cu atoms are initially inside the quintuple layers and migrate to the layer gaps to form Cu clusters during the ageing. In combination with first-principles calculations, an atomic tunnelling–clustering picture across a diffusion barrier of 0.57 eV is proposed., Enhancing the transport properties of surface states in topological insulators is vital if they are to be incorporated into practical devices. Towards this end, Chen et al. study the transport in aged (Cu0.1Bi0.9)2Te3.06, where the ageing process suppresses bulk conductance by up to four orders of magnitude.

We investigated the topological insulator (TI) Bi2Te3 in four different environments (ambient, ultra-high vacuum (UHV), nitrogen gas and organic solvent environment) using scanning probe microscopy (SPM) techniques. Upon prolonged exposure to ambient conditions and organic solvent environments the cleaved surface of the pristine Bi2Te3 is observed to be strongly modified during SPM measurements, while imaging of freshly cleaved Bi2Te3 in UHV and nitrogen gas shows considerably less changes of the Bi2Te3 surface. We conclude that the reduced surface stability upon exposure to ambient conditions is triggered by adsorption of molecular species from ambient, including H2O, CO2, etc which is verified by Auger electron spectroscopy. Our findings of the drastic impact of exposure to ambient on the Bi2Te3 surface are crucial for further in-depth studies of the intrinsic properties of the TI Bi2Te3 and for potential applications that include room temperature TI based devices operated under ambient conditions.

Metallic Bi2Te3 crystalline sheets with the room-temperature resistivity of above 10 m{\Omega} 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 metallic topological insulator., Comment: accepted by EPJD, 2013

The universal conductance fluctuations (UCFs), one of the most important manifestations of mesoscopic electronic interference, have not yet been demonstrated for the two-dimensional surface state of topological insulators (TIs). Even if one delicately suppresses the bulk conductance by improving the quality of TI crystals, the fluctuation of the bulk conductance still keeps competitive and difficult to be separated from the desired UCFs of surface carriers. Here we report on the experimental evidence of the UCFs of the two-dimensional surface state in the bulk insulating Bi2Te2Se nanoribbons. The solely-B\perp-dependent UCF is achieved and its temperature dependence is investigated. The surface transport is further revealed by weak antilocalizations. Such survived UCFs of the topological surface states result from the limited dephasing length of the bulk carriers in ternary crystals. The electron-phonon interaction is addressed as a secondary source of the surface state dephasing based on the temperature-dependent scaling behavior.

Here we synthesized the antimony doped [Formula: see text] nanoplates by the solvothermal method. The angle-dependent magnetoconductance study was carried out and all the [Formula: see text] were found to be normalized to the perpendicular field, indicating a clear 2D electronic state. The features of weak antilocalization and universal conductance fluctuations were clearly identified in the magnetoresistance transport of the 4-probe nanodevices. The dephasing lengths are extracted respectively according to the Hikami-Larkin-Nagaoka theory. It is attributed to the involvement of the dynamic spin centers. The dephasing lengths are found to increase with the decreasing temperature following a [Formula: see text] law with [Formula: see text]. This reveals the additional dephasing source of electron-phonon interaction, which is often absent for pure 2D electronic systems.

A Zn-based in situ cleavage method is applied to fabricate few-layer graphene devices. This approach avoids unintentional electron-beam irradiation damage, in addition to creating a series of clean graphene devices with well controlled layer numbers. As prepared bilayer graphene surprisingly achieves a magnetoresistance ratio as high as 350% at 1.9 K and 100% at room temperature. For this reason, in situ cleavage method/electron-beam lithographic could provide a more effective way to fabricate modern day carbon electronic components.

Thin Bi2Te3 flakes, with as few as 3 quintuple layers, are optically visualized on the SiO2-capped Si substrates. Their optical contrasts vary with the illumination wavelength, flake thickness and capping layers. The maximum contrast appears at the optimized light with the 570 nm wavelength. The contrast turns reversed when the flake is reduced to less than 20 quintuple layers. A calculation based on the Fresnel law describes the above observation with the constructions of the layer number-wave length-contrast three-dimensional (3D) diagram and the cap thickness-wavelength-contrast 3D diagram, applicative in the current studies of topological insulating flakes.

Free-standing graphene sheets (GS) with several to over a hundred layers are prepared by splitting the expandable graphite. The raw material is firstly transferred to a heating chamber for the thermal flashing at 1500 οC in a hydrogen chamber. The expanded powder (1 mg) is then dispersed in 10 ml of the PmPV/DCE suspension for high-power sonication and further centrifugation. After drop-cast onto a holey Formvar film, the GSs are suspended on the grid. The electron scattering is carried out in a Tecnai F20 TEM/STEM with a field emission gun. A high-angle annular dark field (HAADF) detector is fitted to collect the scattered electrons with a tunable collecting angle. The quantitative STEM image simulation is carried out using amultislice algorithm [4].

Universal conductance fluctuations (UCFs) are extracted in the magnetoresistance responses in bulk-insulating Bi2Te2Se microflakes. Their two-dimensional character is demonstrated by field-tilting magnetoresistance measurements. Their origin from the surface electrons is determined by the fact that the UCF amplitudes remain unchanged while applying an in-plane field to suppress the coherence of bulk electrons. After considering the ensemble average in a batch of micrometer-sized samples, the intrinsic UCF magnitude of over 0.37 e2/h is obtained. This agrees with the theoretical prediction on topological surface states. All the lines of evidence point to the successful observation of the UCF of topological surface states.