Chemically induced ferromagnetism near room temperature in single crystal (Zn1-x Cr x )Te half-metal.

Magnetic semiconductors are at the core of recent spintronics research endeavors. Chemically doped II-VI diluted magnetic semiconductors, such as (Zn1-x Cr x )Te, provide a promising platform in this quest. However, a detailed knowledge of the microscopic nature of magnetic ground state is necessary for any practical application. Here, we report on the synergistic study of (Zn1-x Cr x )Te single crystals using elastic neutron scattering measurements and density functional calculations. For the first time, our research unveils the intrinsic properties of ferromagnetic state in a macroscopic specimen of (Zn0.8Cr0.2)Te. The ferromagnetism is onset at T C ∼ 290 K and remains somewhat independent to modest change in the substitution coefficient x. We show that magnetic moments on Zn/Cr sites develop ferromagnetic correlation in the a-c plane with a large ordered moment of µ = 3.08 µ B. Magnetic moment across the lattice is induced via the mediation of Te sites, uncoupled to the number of dopant carriers as inferred from the density functional calculation. Additionally, the ab initio calculations also reveal half-metallicity in x = 0.2 composition. These properties are highly desirable for future spintronic applications.

Local orbital degeneracy lifting as a precursor to an orbital-selective Peierls transition.

Fundamental electronic principles underlying all transition metal compounds are the symmetry and filling of the d-electron orbitals and the influence of this filling on structural configurations and responses. Here we use a sensitive local structural technique, x-ray atomic pair distribution function analysis, to reveal the presence of fluctuating local-structural distortions at high temperature in one such compound, CuIr2S4. We show that this hitherto overlooked fluctuating symmetry-lowering is electronic in origin and will modify the energy-level spectrum and electronic and magnetic properties. The explanation is a local, fluctuating, orbital-degeneracy-lifted state. The natural extension of our result would be that this phenomenon is likely to be widespread amongst diverse classes of partially filled nominally degenerate d-electron systems, with potentially broad implications for our understanding of their properties.

Conductance Spectroscopy of Exfoliated Thin Flakes of Nb xBi2Se3.

We study unconventional superconductivity in exfoliated single crystals of a promising three-dimensional (3D) topological superconductor candidate, Nb-doped Bi2Se3 through differential conductance spectroscopy and magneto-transport. The strong anisotropy of the critical field along the out-of-plane direction suggests that the thin exfoliated flakes are in the quasi-2D limit. Normal metal-superconductor (NS) contacts with either high or low transparencies made by depositing gold leads onto Nb-doped Bi2Se3 flakes both show significant enhancement in zero bias conductance and coherence dips at the superconducting energy gap. Such behavior is inconsistent with conventional Blonder-Tinkham-Klapwijk theory. Instead, we discuss how our results are consistent with p-wave pairing symmetry, supporting the possibility of topological superconductivity in Nb-doped Bi2Se3. Finally, we observe signatures of multiple superconducting energy gaps, which could originate from multiple Fermi surfaces reported earlier in bulk crystals.

Determination of the energy band gap of Bi2Se3.

Despite intensive investigations of Bi2Se3 in past few years, the size and nature of the bulk energy band gap of this well-known 3D topological insulator still remain unclear. Here we report on a combined magneto-transport, photoluminescence and infrared transmission study of Bi2Se3, which unambiguously shows that the energy band gap of this material is direct and reaches E g = (220 ± 5) meV at low temperatures.

Evidence for an anomalous current-phase relation in topological insulator Josephson junctions.

Josephson junctions with topological insulator weak links can host low-energy Andreev-bound states giving rise to a current-phase relation that deviates from sinusoidal behaviour. Of particular interest are zero-energy Majorana-bound states that form at a phase difference of π. Here we report on interferometry studies of Josephson junctions and superconducting quantum interference devices (SQUIDs) incorporating topological insulator weak links. We find that the nodes in single-junction diffraction patterns and SQUID oscillations are lifted and independent of chemical potential. At high temperatures, the SQUID oscillations revert to conventional behaviour, ruling out asymmetry. The node-lifting of the SQUID oscillations is consistent with low-energy Andreev-bound states exhibiting a nonsinusoidal current-phase relation, co-existing with states possessing a conventional sinusoidal current-phase relation. However, the finite nodal currents in the single-junction diffraction pattern suggest an anomalous contribution to the supercurrent possibly carried by Majorana-bound states, although we also consider the possibility of inhomogeneity.

Cu(Ir1 - xCrx)2S4: a model system for studying nanoscale phase coexistence at the metal-insulator transition.

Increasingly, nanoscale phase coexistence and hidden broken symmetry states are being found in the vicinity of metal-insulator transitions (MIT), for example, in high temperature superconductors, heavy fermion and colossal magnetoresistive materials, but their importance and possible role in the MIT and related emergent behaviors is not understood. Despite their ubiquity, they are hard to study because they produce weak diffuse signals in most measurements. Here we propose Cu(Ir1 - xCrx)2S4 as a model system, where robust local structural signals lead to key new insights. We demonstrate a hitherto unobserved coexistence of an Ir(4+) charge-localized dimer phase and Cr-ferromagnetism. The resulting phase diagram that takes into account the short range dimer order is highly reminiscent of a generic MIT phase diagram similar to the cuprates. We suggest that the presence of quenched strain from dopant ions acts as an arbiter deciding between the competing ground states.

Quantum oscillations in the topological superconductor candidate Cu(0.25)Bi2Se3.

Quantum oscillations are generally studied to resolve the electronic structure of topological insulators. In Cu(0.25)Bi(2)Se(3), the prime candidate of topological superconductors, quantum oscillations are still not observed in magnetotransport measurement. However, using torque magnetometry, quantum oscillations (the de Haas-van Alphen effect) were observed in Cu(0.25)Bi(2)Se(3). The doping of Cu in Bi(2)Se(3) increases the carrier density and the effective mass without increasing the scattering rate or decreasing the mean free path. In addition, the Fermi velocity remains the same in Cu(0.25)Bi(2)Se(3) as that in Bi(2)Se(3). Our results imply that the insertion of Cu does not change the band structure and that conduction electrons in Cu doped Bi(2)Se(3) sit in the linear Dirac-like band.

Quantum oscillations in magnetothermopower measurements of the topological insulator Bi2Te3.

We report the magnetothermopower measurements of the nonmetallic topological insulator Bi(2)Te(3) in magnetic fields up to 35 T. Quantum oscillations arising from surface states are observed in both thermoelectric and conductivity tensors. The inferred surface thermopower has a peak magnitude ~1 mV/K possibly as a result of surface electron and bulk phonon interaction. At the n = 1 Landau level, we resolve additional quantum oscillations signaling Landau sublevels.

Bulk band gap and surface state conduction observed in voltage-tuned crystals of the topological insulator Bi2Se3.

We report a transport study of exfoliated few monolayer crystals of topological insulator Bi2Se3 in an electric field effect geometry. By doping the bulk crystals with Ca, we are able to fabricate devices with sufficiently low bulk carrier density to change the sign of the Hall density with the gate voltage V(g). We find that the temperature T and magnetic field dependent transport properties in the vicinity of this V(g) can be explained by a bulk channel with activation gap of approximately 50 meV and a relatively high-mobility metallic channel that dominates at low T. The conductance (approximately 2×7e2/h), weak antilocalization, and metallic resistance-temperature profile of the latter lead us to identify it with the protected surface state. The relative smallness of the observed gap implies limitations for electric field effect topological insulator devices at room temperature.

Detailed mapping of the local Ir4+ dimers through the metal-insulator transitions of CuIr2S4 thiospinel by X-ray atomic pair distribution function measurements.

The evolution of the short-range structural signature of the Ir4+ dimer state in CuIr2S4 thiospinel has been studied across the metal-insulator phase transitions as the metallic state is induced by temperature, Cr doping, and x-ray fluence. An atomic pair distribution function (PDF) approach reveals that there are no local dimers that survive into the metallic phase when this is invoked by temperature and doping. The PDF shows Ir4+ dimers when they exist, regardless of whether or not they are long-range ordered. At 100 K, exposure to a 98 keV x-ray beam melts the long-range dimer order within a few seconds, though the local dimers remain intact. This shows that the metallic state accessed on warming and doping is qualitatively different from the state obtained under x-ray irradiation.

Quantum oscillations and hall anomaly of surface states in the topological insulator Bi2Te3.

Topological insulators are insulating materials that display massless, Dirac-like surface states in which the electrons have only one spin degree of freedom on each surface. These states have been imaged by photoemission, but little information on their transport parameters, for example, mobility, is available. We report the observation of Shubnikov-de Haas oscillations arising from the surface states in nonmetallic crystals of Bi(2)Te(3). In addition, we uncovered a Hall anomaly in weak fields, which enables the surface current to be seen directly. Both experiments yield a surface mobility (9000 to 10,000 centimeter(2) per volt-second) that is substantially higher than in the bulk. The Fermi velocity of 4 x 10(5) meters per second obtained from these transport experiments agrees with angle-resolved photoemission experiments.

Transmission of topological surface states through surface barriers.

Topological surface states are a class of novel electronic states that are of potential interest in quantum computing or spintronic applications. Unlike conventional two-dimensional electron states, these surface states are expected to be immune to localization and to overcome barriers caused by material imperfection. Previous experiments have demonstrated that topological surface states do not backscatter between equal and opposite momentum states, owing to their chiral spin texture. However, so far there is no evidence that these states in fact transmit through naturally occurring surface defects. Here we use a scanning tunnelling microscope to measure the transmission and reflection probabilities of topological surface states of antimony through naturally occurring crystalline steps separating atomic terraces. In contrast to non-topological surface states of common metals (copper, silver and gold), which are either reflected or absorbed by atomic steps, we show that topological surface states of antimony penetrate such barriers with high probability. This demonstration of the extended nature of antimony's topological surface states suggests that such states may be useful for high current transmission even in the presence of atomic-scale irregularities-an electronic feature sought to efficiently interconnect nanoscale devices.

Superconductivity in CuxBi2Se3 and its implications for pairing in the undoped topological insulator.

Bi2Se3 is one of a handful of known topological insulators. Here we show that copper intercalation in the van der Waals gaps between the Bi2Se3 layers, yielding an electron concentration of approximately 2x10{20} cm{-3}, results in superconductivity at 3.8 K in CuxBi2Se3 for 0.12

Low temperature magnetothermoelectric effect and magnetoresistance in Te vapor annealed Bi2Te3.

The electrical properties of single crystals of p-type Bi(2)Te(3) are shown to be tuned by annealing as-grown crystals in elemental Te vapor at temperatures in the range of 400-420 °C. While as-grown nominally stoichiometric Bi(2)Te(3) has p-type conductivity below room temperature, Te vapor annealed Bi(2)Te(3) shows a cross over from p- to n-type behavior. The temperature dependent resistivity of the Te annealed crystals shows a characteristic broad peak near 100 K. Applied magnetic fields give rise to a large low temperature magnetothermoelectric effect in the Te annealed samples and enhance the low temperature peak in the resistivity. Further, Te annealed Bi(2)Te(3) shows a large positive magnetoresistance, ∼ 200% at 2 K, and ∼ 15% at room temperature. The annealing procedure described can be employed to optimize the properties of Bi(2)Te(3) for study as a topological insulator.

Observation of time-reversal-protected single-dirac-cone topological-insulator states in Bi2Te3 and Sb2Te3.

We show that the strongly spin-orbit coupled materials Bi2Te3 and Sb2Te3 and their derivatives belong to the Z2 topological-insulator class. Using a combination of first-principles theoretical calculations and photoemission spectroscopy, we directly show that Bi2Te3 is a large spin-orbit-induced indirect bulk band gap (delta approximately 150 meV) semiconductor whose surface is characterized by a single topological spin-Dirac cone. The electronic structure of self-doped Sb2Te3 exhibits similar Z2 topological properties. We demonstrate that the dynamics of spin-Dirac fermions can be controlled through systematic Mn doping, making these materials classes potentially suitable for topological device applications.

Topological surface states protected from backscattering by chiral spin texture.

Topological insulators are a new class of insulators in which a bulk gap for electronic excitations is generated because of the strong spin-orbit coupling inherent to these systems. These materials are distinguished from ordinary insulators by the presence of gapless metallic surface states, resembling chiral edge modes in quantum Hall systems, but with unconventional spin textures. A key predicted feature of such spin-textured boundary states is their insensitivity to spin-independent scattering, which is thought to protect them from backscattering and localization. Recently, experimental and theoretical efforts have provided strong evidence for the existence of both two- and three-dimensional classes of such topological insulator materials in semiconductor quantum well structures and several bismuth-based compounds, but so far experiments have not probed the sensitivity of these chiral states to scattering. Here we use scanning tunnelling spectroscopy and angle-resolved photoemission spectroscopy to visualize the gapless surface states in the three-dimensional topological insulator Bi(1-x)Sb(x), and examine in detail the influence of scattering from disorder caused by random alloying in this compound. We show that, despite strong atomic scale disorder, backscattering between states of opposite momentum and opposite spin is absent. Our observations demonstrate that the chiral nature of these states protects the spin of the carriers. These chiral states are therefore potentially useful for spin-based electronics, in which long spin coherence is critical, and also for quantum computing applications, where topological protection can enable fault-tolerant information processing.

A tunable topological insulator in the spin helical Dirac transport regime.

Helical Dirac fermions-charge carriers that behave as massless relativistic particles with an intrinsic angular momentum (spin) locked to its translational momentum-are proposed to be the key to realizing fundamentally new phenomena in condensed matter physics. Prominent examples include the anomalous quantization of magneto-electric coupling, half-fermion states that are their own antiparticle, and charge fractionalization in a Bose-Einstein condensate, all of which are not possible with conventional Dirac fermions of the graphene variety. Helical Dirac fermions have so far remained elusive owing to the lack of necessary spin-sensitive measurements and because such fermions are forbidden to exist in conventional materials harbouring relativistic electrons, such as graphene or bismuth. It has recently been proposed that helical Dirac fermions may exist at the edges of certain types of topologically ordered insulators-materials with a bulk insulating gap of spin-orbit origin and surface states protected against scattering by time-reversal symmetry-and that their peculiar properties may be accessed provided the insulator is tuned into the so-called topological transport regime. However, helical Dirac fermions have not been observed in existing topological insulators. Here we report the realization and characterization of a tunable topological insulator in a bismuth-based class of material by combining spin-imaging and momentum-resolved spectroscopies, bulk charge compensation, Hall transport measurements and surface quantum control. Our results reveal a spin-momentum locked Dirac cone carrying a non-trivial Berry's phase that is nearly 100 per cent spin-polarized, which exhibits a tunable topological fermion density in the vicinity of the Kramers point and can be driven to the long-sought topological spin transport regime. The observed topological nodal state is shown to be protected even up to 300 K. Our demonstration of room-temperature topological order and non-trivial spin-texture in stoichiometric Bi(2)Se(3).M(x) (M(x) indicates surface doping or gating control) paves the way for future graphene-like studies of topological insulators, and applications of the observed spin-polarized edge channels in spintronic and computing technologies possibly at room temperature.

Observation of unconventional quantum spin textures in topological insulators.

A topologically ordered material is characterized by a rare quantum organization of electrons that evades the conventional spontaneously broken symmetry-based classification of condensed matter. Exotic spin-transport phenomena, such as the dissipationless quantum spin Hall effect, have been speculated to originate from a topological order whose identification requires a spin-sensitive measurement, which does not exist to this date in any system. Using Mott polarimetry, we probed the spin degrees of freedom and demonstrated that topological quantum numbers are completely determined from spin texture-imaging measurements. Applying this method to Sb and Bi(1-x)Sb(x), we identified the origin of its topological order and unusual chiral properties. These results taken together constitute the first observation of surface electrons collectively carrying a topological quantum Berry's phase and definite spin chirality, which are the key electronic properties component for realizing topological quantum computing bits with intrinsic spin Hall-like topological phenomena.

Quantum interference in macroscopic crystals of nonmetallic Bi2Se3.

Photoemission experiments have shown that Bi2Se3 is a topological insulator. By controlled doping, we have obtained crystals of Bi2Se3 with nonmetallic conduction. At low temperatures, we uncover a novel type of magnetofingerprint signal which involves the spin degrees of freedom. Given the mm-sized crystals, the observed amplitude is 200-500x larger than expected from universal conductance fluctuations. The results point to very long phase-breaking lengths in an unusual conductance channel in these nonmetallic samples. We discuss the nature of the in-gap conducting states and their relation to the topological surface states.

Phase transitions of Dirac electrons in bismuth.

The Dirac Hamiltonian, which successfully describes relativistic fermions, applies equally well to electrons in solids with linear energy dispersion, for example, in bismuth and graphene. A characteristic of these materials is that a magnetic field less than 10 tesla suffices to force the Dirac electrons into the lowest Landau level, with resultant strong enhancement of the Coulomb interaction energy. Moreover, the Dirac electrons usually come with multiple flavors or valley degeneracy. These ingredients favor transitions to a collective state with novel quantum properties in large field. By using torque magnetometry, we have investigated the magnetization of bismuth to fields of 31 tesla. We report the observation of sharp field-induced phase transitions into a state with striking magnetic anisotropy, consistent with the breaking of the threefold valley degeneracy.