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Magnetic semiconductors are at the core of recent spintronics research endeavors. Chemically doped II-VI diluted magnetic semiconductors, such as (Zn$_{1-x}$Cr$_{x}$)Te, provide 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 (Zn$_{1-x}$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 macroscopic specimen of (Zn$_{0.8}$Cr$_{0.2}$)Te. The ferromagnetism is onset at $T_c \sim$ 290 K and remains somewhat independent to modest change in the substitution coefficient x. We show that magnetic moments on Zn/Cr site develop ferromagnetic correlation in a-c plane with large ordered moment of $\mu$ = 3.08 $\mu_B$. Magnetic moment across the lattice is induced via the mediation of Te site, 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.

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 of one such compound, \cis . We show that this hitherto overlooked fluctuating symmetry lowering is electronic in origin and will significantly 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., Comment: 10 pages 3 figures

We report an unexpected positive hydrostatic pressure derivative of the superconducting transition temperature in the doped topological insulator \NBS via $dc$ SQUID magnetometry in pressures up to 0.6 GPa. This result is contrary to reports on the homologues \CBS and \SBS where smooth suppression of $T_c$ is observed. Our results are consistent with recent Ginzburg-Landau theory predictions of a pressure-induced enhancement of $T_c$ in the nematic multicomponent $E_u$ state proposed to explain observations of rotational symmetry breaking in doped Bi$_2$Se$_3$ superconductors., Comment: 5 pages, 5 figures

We present resistivity and magnetization measurements on proton-irradiated crystals demonstrating that the superconducting state in the doped topological superconductor Nb$_x$Bi$_2$Se$_3$ (x = 0.25) is surprisingly robust against disorder-induced electron scattering. The superconducting transition temperature $T_c$ decreases without indication of saturation with increasing defect concentration, and the corresponding scattering rates far surpass expectations based on conventional theory. The low-temperature variation of the London penetration depth $\Delta\lambda(T)$ follows a power law ($\Delta\lambda(T)\sim T^2$) indicating the presence of symmetry-protected point nodes. Our results are consistent with the proposed robust nematic $E_u$ pairing state in this material., Comment: 6 pages, 5 figures

The low-temperature variation of the London penetration depth $\lambda (T)$ in the candidate topological superconductor Nb$_x$Bi$_2$Se$_3$ (x = 0.25) is reported for several crystals. The measurements were carried out by means of a tunnel-diode oscillator (TDO) technique in both field orientations ($H_{rf} \parallel$ $c$ and $H_{rf} \parallel$ $ab$ planes). All samples exhibited power law behavior at low temperatures ($\Delta\lambda\sim T^2$) clearly indicating the presence of point nodes in the superconducting order parameter. The results presented here are consistent with a nematic odd-parity spin-triplet $E_u$ pairing state in Nb$_x$Bi$_2$Se$_3$., Comment: 6 pages, 5 figures

The magnetic and electronic properties of the magnetically doped topological insulator Bi$_{\rm 2-x}$Mn$_{\rm x}$Te$_3$ were studied using electron spin resonance (ESR) and measurements of static magnetization and electrical transport. The investigated high quality single crystals of Bi$_{\rm 2-x}$Mn$_{\rm x}$Te$_3$ show a ferromagnetic phase transition for $x\geq 0.04$ at $T_{C}\approx 12$ K. The Hall measurements reveal a p-type finite charge-carrier density. Measurements of the temperature dependence of the ESR signal of Mn dopants for different orientations of the external magnetic field give evidence that the localized Mn moments interact with the mobile charge carriers leading to a Ruderman-Kittel-Kasuya-Yosida-type ferromagnetic coupling between the Mn spins of order 2-3 meV. Furthermore, ESR reveals a low-dimensional character of magnetic correlations that persist far above the ferromagnetic ordering temperature.

The search for unconventional superconductivity has been focused on materials with strong spin-orbit coupling and unique crystal lattices. Doped bismuth selenide (Bi$_2$Se$_3$) is a strong candidate given the topological insulator nature of the parent compound and its triangular lattice. The coupling between the physical properties in the superconducting state and its underlying crystal symmetry is a crucial test for unconventional superconductivity. In this paper, we report direct evidence that the superconducting magnetic response couples strongly to the underlying 3-fold crystal symmetry in the recently discovered superconductor with trigonal crystal structure, niobium (Nb)-doped bismuth selenide (Bi$_2$Se$_3$). More importantly, we observed that the magnetic response is greatly enhanced along one preferred direction spontaneously breaking the rotational symmetry. Instead of a simple 3-fold crystalline symmetry, the superconducting hysteresis loop shows dominating 2-fold and 4-fold symmetry. This observation confirms the breaking of the rotational symmetry and indicates the presence of nematic order in the superconducting ground state of Nb-doped Bi$_2$Se$_3$. Further, heat capacity measurements display an exponential decay in superconducting state and suggest that there is no line node in the superconducting gap. These observations provide strong evidence of odd-parity topological superconductivity., Comment: 10 pages, 9 figures

Transport and torque magnetometry measurements are performed at high magnetic fields and low temperatures in a series of p-type (Ca-doped) Bi$_{2}$Se$_{3}$ crystals. The angular dependence of the Shubnikov-de Haas and de Haas-van Alphen quantum oscillations enables us to determine the Fermi surface of the bulk valence band states as a function of the carrier density. At low density, the angular dependence exhibits a downturn in the oscillations frequency between $0^\circ$ and $90^\circ$, reflecting a bag-shaped hole Fermi surface. The detection of a single frequency for all tilt angles rules out the existence of a Fermi surface with different extremal cross-sections down to $24$~meV. There is therefore no signature of a camel-back in the valence band of our bulk samples, in accordance with the direct band gap predicted by $GW$ calculations., Comment: A supplemental material file giving a more detailed description of our work is available upon request

We study Fabry-Perot interference in hybrid devices, each consisting of a mesoscopic superconducting disk deposited on the surface of a three-dimensional topological insulator. Such structures are hypothesized to contain protected zero modes known as Majorana fermions bound to vortices. The interference manifests as periodic conductance oscillations of magnitude $\sim 0.1$ $e^2/h$. These oscillations show no strong dependence on bulk carrier density or sample thickness, suggesting that they result from phase coherent transport in surface states. However, the Fabry-Perot interference can be tuned by both top and back gates, implying strong electrostatic coupling between the top and bottom surfaces of topological insulator., Comment: 5 pages, 3 figures. Accepted by Appl. Phys. Lett

Cu$_x$Bi$_2$Se$_3$ has drawn much attention as the leading candidate to be the first topological superconductor and the realization of coveted Majorana particles in a condensed matter system. However, there has been increasing controversy about the nature of its superconducting phase. This study sheds light on present ambiguity in the normal state electronic state, by providing a complete look at the quantum oscillations in magnetization in Cu$_x$Bi$_2$Se$_3$ at intense high fields up to 31T. Our study focuses on the angular dependence of the quantum oscillation pattern in a low carrier concentration. As magnetic field tilts from along the crystalline c-axis to ab-plane, the change of the oscillation period follows the prediction of the ellipsoidal Fermi surface. As the doping level changes, the 3D Fermi surface is found to transform into quasi-cylindrical at high carrier density. Such a transition is potentially a Lifshitz transition of the electronic state in Cu$_x$Bi$_2$Se$_3$., Comment: 6 pages, 6 figures, submitted to Phys. Rev. B

Topological insulators (TIs) have attracted immense interest because they host helical surface states. Protected by time-reversal symmetry, they are robust to non-magnetic disorder. When superconductivity is induced in these helical states, they are predicted to emulate p-wave pairing symmetry, with Majorana states bound to vortices. Majorana bound states possess non-Abelian exchange statistics which can be probed through interferometry. Here, we take a significant step towards Majorana interferometry by observing pronounced Fabry-Perot oscillations in a TI sandwiched between a superconducting and normal lead. For energies below the superconducting gap, we observe a doubling in the frequency of the oscillations, arising from the additional phase accumulated from Andreev reflection. When a magnetic field is applied perpendicular to the TI surface, a number of very sharp and gate-tunable conductance peaks appear at or near zero energy, which has consequences for interpreting spectroscopic probes of Majorana fermions. Our results demonstrate that TIs are a promising platform for exploring phase-coherent transport in a solid-state system., Comment: 9 pages, 7 figures

Josephson junctions made of closely-spaced conventional superconductors on the surface of 3D topological insulators have been proposed to host Andreev bound states (ABSs) which can include Majorana fermions. Here, we present an extensive study of the supercurrent carried by low energy ABSs in Nb/Bi$_2$Se$_3$/Nb Josephson junctions in various SQUIDs as we modulate the carrier density in the Bi$_2$Se$_3$ barriers through electrostatic top gates. As previously reported, we find a precipitous drop in the Josephson current at a critical value of the voltage applied to the top gate. This drop has been attributed to a transition where the topologically trivial 2DEG at the surface is nearly depleted, causing a shift in the spatial location and change in nature of the helical surface states. We present measurements that support this picture by revealing qualitative changes in the temperature and magnetic field dependence of the critical current across this transition. In particular, we observe pronounced fluctuations in the critical current near total depletion of the 2DEG that demonstrate the dynamical nature of the supercurrent transport through topological low energy ABSs., Comment: 6 pages, 6 figures

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(Ir$_{1-x}$Cr$_x$)$_2$S$_4$ as a model system, where robust local structural signals lead to key new insights. We demonstrate a hitherto unobserved coexistence of a 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.

Angle resolved photoemission spectroscopy is used to observe changes in the electronic structure of bulk-doped topological insulator Cu$_x$Bi$_2$Se$_3$ as additional copper atoms are deposited onto the cleaved crystal surface. Carrier density and surface-normal electrical field strength near the crystal surface are estimated to consider the effect of chemical surface gating on atypical superconducting properties associated with topological insulator order, such as the dynamics of theoretically predicted Majorana Fermion vortices.

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 $\pi$. 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, coexisting 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., Comment: 6 pages, 4 figures

Topological surface states, a new kind of electronic state of matter, have recently been observed on the cleaved surfaces of crystals of a handful of small band gap semiconductors. The underlying chemical factors that enable these states are crystal symmetry, the presence of strong spin orbit coupling, and an inversion of the energies of the bulk electronic states that normally contribute to the valence and conduction bands. The goals of this review are to briefly introduce the physics of topological insulators to a chemical audience and to describe the chemistry, defect chemistry, and crystal structures of the compounds in this emergent field., Comment: Submitted to Journal of Materials Chemistry, 47 double spaced pages, 9 figures

We perform a point-contact Andreev reflection spectroscopic study of the topological superconducting material, Cu0.25Bi2Se3, in the ballistic regime using a normal-metal gold tip. We observe distinct point-contact spectra on the superconducting and non-superconducting regions of the crystal surface: the former shows a marked zero-bias conductance peak, indicative of unconventional superconductivity, while the latter exhibits a pseudogap-like feature. In both cases the measured differential conductance spectra exhibit a large linear background, preventing direct quantitative comparison with theory. We attribute this background to inelastic scattering at the tip-sample interface, and compare the background-subtracted spectra with a single-band p-wave model., Comment: 10 pages, 3 figures

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 Hass - 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 of Bi$_2$Se$_3$., Comment: 5 pages, 4 figures

Topological insulators (TIs) are novel materials that manifest spin-polarized Dirac states on their surfaces or at interfaces made with conventional matter. We have measured the electron kinetics of bulk doped TI Bi$_2$Se$_3$ with angle resolved photoemission spectroscopy while depositing cathodic and anodic adatoms on the TI surfaces to add charge carriers of the opposite sign from bulk dopants. These P-N overlayer interfaces create Dirac point transport regimes and larger interface potentials than previous N-N type surface deposition studies, revealing unconventional Rashba-like and surface-bulk electron interactions, and an unusual characteristic distribution of spectral weight near the Dirac point in TI Dirac point interfaces. The electronic structures of P-N doped topological interfaces observed in these experiments are an important step towards the understanding of solid interfaces with topological materials., Comment: Submitted to Phys. Rev. B. 12 pages, including supplemental material. This is a substantially revised version of arXiv:1105.4794

Using angle-resolved photoemission spectroscopy, we report electronic structure for representative members of ternary topological insulators. We show that several members of this family, such as Bi2Se2Te, Bi2Te2Se, and GeBi2Te4, exhibit a singly degenerate Dirac-like surface state, while Bi2Se2S is a fully gapped insulator with no measurable surface state. One of these compounds, Bi2Se2Te, shows tunable surface state dispersion upon its electronic alloying with Sb (SbxBi2-xSe2Te series). Other members of the ternary family such as GeBi2Te4 and BiTe1.5S1.5 show an in-gap surface Dirac point, the former of which has been predicted to show nonzero weak topological invariants such as (1;111); thus belonging to a different topological class than BiTe1.5S1.5. The measured band structure presented here will be a valuable guide for interpreting transport, thermoelectric, and thermopower measurements on these compounds. The unique surface band topology observed in these compounds contributes towards identifying designer materials with desired flexibility needed for thermoelectric and spintronic device fabrication., Comment: 9 pages, 6 figures; Related results at http://online.kitp.ucsb.edu/online/topomat11/hasan/

The optical conductivity and the spectral weight of four topological insulators with increasing chemical compensation (Bi2Se3, Bi2-xCaxSe3, Bi2Se2Te, Bi2Te2Se) have been measured from 5 to 300 K and from sub-THz to visible frequencies. The effect of compensation is clearly observed in the infrared spectra, through the suppression of an extrinsic Drude term and the appearance of strong absorption peaks, that we assign to electronic transitions among localized states. From the far-infrared spectral weight of the most compensated sample (Bi2Te2Se) one can estimate a density of charge-carriers in the order of 10^17/cm^3 in good agreement with transport data. Those results demonstrate that the low-energy electrodynamics in single crystals of topological insulators, even at the highest degree of compensation presently achieved, is still affected by extrinsic charge excitations., Comment: 5 pages, 4 figures

The fractional quantum Hall (FQH) state is a topological state of matter resulting from the many-body effect of interacting electrons and is of vast interest in fundamental physics. The experimental observation of topological surface states (SSs) in three-dimensional bulk solids has allowed the study of a correlated chiral Dirac fermion system, which can host a single Dirac valley without spin degeneracy. Recent theoretical studies suggest that the fractional quantum Hall effect (FQHE) might be observable in topological insulators. However, due to the dominant bulk conduction it is difficult to probe the strong correlation effect in topological insulators from resistivity measurements. Here we report the discovery of FQH states in Bi2Te3 from thermopower measurements. The surface thermopower is ten times greater than that of bulk, which makes possible the observation of fractional-filled Landau levels in SSs. Thermopower hence provides a powerful tool to investigate correlated Dirac fermions in topological insulators. Our observations demonstrate that Dirac topological SSs exhibit strongly correlated phases in a high magnetic field, and would enable studies of a variety of exotic fractional quantum Hall physics and other correlated phenomena in this newly discovered chiral Dirac system.

We report high-resolution spin-resolved photoemission spectroscopy (Spin-ARPES) measurements on the parent compound Sb of the first discovered 3D topological insulator Bi{1-x}Sb{x} [D. Hsieh et al., Nature 452, 970 (2008) Submitted 2007]. By modulating the incident photon energy, we are able to map both the bulk and (111) surface band structure, from which we directly demonstrate that the surface bands are spin polarized by the spin-orbit interaction and connect the bulk valence and conduction bands in a topologically non-trivial way. A unique asymmetric Dirac surface state gives rise to a $k$-splitting of its spin polarized electronic channels. These results complement our previously published works on this materials class and re-confirm our discovery of first bulk (3D) topological insulator - topological order in bulk solids. [Invited article for NJP-IOP Focus issue on "Topological Insulators"], Comment: Invited article for NJP-IOP Focus issue on "Topological Insulators", Experimental discovery of 3D topological insulators (topological order in bulk solids) reported at KITP (2007) Conference Proceeding at http://online.itp.ucsb.edu/online/motterials07/hasan/ (2007)

The development of spin-based applications of topological insulators requires the knowledge and understanding of spin texture configuration maps as they change via gating in the vicinity of an isolated Dirac node. An isolated (graphene-like) Dirac node, however, does not exist in Bi2Te3. While the isolation of surface states via transport channels has been promisingly achieved in Bi2Te3, it is not known how spin textures modulate while gating the surface. Another drawback of Bi2Te3 is that it features multiple band crossings while chemical potential is placed near the Dirac node (at least 3 not one as in Bi2Se3 and many other topological insulators) and its buried Dirac point is not experimentally accessible for the next generation of experiments which require tuning the chemical potential near an isolated (graphene-like) Dirac node. Here, we image the spin texture of Bi2Te3 and suggest a simple modification to realize a much sought out isolated Dirac node regime critical for almost all potential applications (of topological nature) of Bi2Te3. Finally, we demonstrate carrier control in magnetically and nonmagnetically doped Bi2Te3 essential for realizing giant magneto-optical effects and dissipationless spin current devices involving a Bi2Te3-based platform., Comment: 5 pages, 4 Figures

Topological insulators embody a newly discovered state of matter characterized by conducting spin-momentum locked surface states that span the bulk band gap. So far, most of the study on topological insulator surfaces has been limited to understanding their properties without strong Coulomb perturbation or breaking of time reversal symmetry. We have used deposited iron, with a large positive ionization state and significant magnetic moment as a strong probe to modify the surface electronic structure of the Bi2Se3 surface at the gap energy scale. We observe that such perturbation leads to the creation of multiple Dirac fermions consistent with Z2 or Mod(2) symmetry. Taken collectively, these results are a helpful guide in manipulating topological surfaces for probing fundamental physics or developing device applications., Comment: 4 Figures, 15 pages, For an expanded version of this paper see arXiv:1103.3411

Three dimensional (3D) topological insulators are novel states of quantum matter that feature spin-momentum locked helical Dirac fermions on their surfaces and hold promise to open new vistas in spintronics, quantum computing and fundamental physics. Experimental realization of many of the predicted topological phenomena requires finding multi-variant topological band insulators which can be multiply connected to magnetic semiconductors and superconductors. Here we present our theoretical prediction and experimental discovery of several new topological insulator classes in AB2X4(124), A2B2X5(225), MN4X7(147), A2X2X'(221) [A,B=Pb,Ge,Sb,Bi and M,N=Pb,Bi and X,X'=Chalcogen family]. We observe that these materials feature gaps up to about 0.35eV. Multi-variant nature allows for diverse surface dispersion tunability, Fermi surface spin-vortex or textured configurations and spin-dependent electronic interference signaling novel quantum transport processes on the surfaces of these materials. Our discovery also provides several new platforms to search for topological-superconductivity (arXiv:0912.3341v1 (2009)) in these exotic materials., Comment: 11 pages, 4 Figures

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 nontopological 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.

The structural misfit compound (PbSe)1.16(TiSe2)2 is reported. It is a superconductor with a Tc of 2.3 K. (PbSe)1.16(TiSe2)2 derives from a parent compound, TiSe2, which shows a charge density wave transition and no superconductivity. The crystal structure, characterized by high resolution electron microscopy and powder x-ray diffraction, consists of two layers of 1T-TiSe2 alternating with a double layer of (100) PbSe. Transport measurements suggest that the superconductivity is induced by charge transfer from the PbSe layers to the TiSe2 layers., Comment: 17 pages, 4 figures. To be published in Physical Review B

We show that by Ca-doping the Bi2Se3 topological insulator, the Fermi level can be fine tuned to fall inside the band gap and therefore suppress the bulk conductivity. Non-metallic Bi2Se3 crystals are obtained. On the other hand, the Bi2Se3 topological insulator can also be induced to become a bulk superconductor, with Tc ~ 3.8 K, by copper intercalation in the van der Waals gaps between the Bi2Se3 layers. Likewise, an as-grown crystal of metallic Bi2Te3 can be turned into a non-metallic crystal by slight variation of the Te content. The Bi2Te3 topological insulator shows small amounts of superconductivity with Tc ~ 5.5 K when reacted with Pd to form materials of the type PdxBi2Te3.

We report a transport study of exfoliated few monolayer crystals of topological insulator Bi$_2$Se$_3$ in an electric field effect (EFE) 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 $\times$ 7$e^2/h$), weak anti-localization, 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 EFE topological insulator devices at room temperature., Comment: 4 pages, 4 figures. In new version, panels have been removed from Figures 1, 2, and 4 to improve clarity. Additional data included in Figure 4. Introduction and discussion revised and expanded

The development of ferromagnetism in Mn-doped Bi2Te3 is characterized through measurements on a series of single crystals with different Mn content. Scanning tunneling microscopy analysis shows that the Mn substitutes on the Bi sites, forming compounds of the type Bi2-xMnxTe3, and that the Mn substitutions are randomly distributed, not clustered. Mn doping first gives rise to local magnetic moments with Curie-like behavior, but by the compositions Bi1.96Mn0.04Te3 and Bi1.91Mn0.09Te3 a second order ferromagnetic transition is observed, with Tc ~ 9-12 K. The easy axis of magnetization in the ferromagnetic phase is perpendicular to the Bi2Te3 basal plane. Thermoelectric power and Hall effect measurements show that the Mn-doped Bi2Te3 crystals are p-type. Angle resolved photoemission spectroscopy measurements show that the topological surface states that are present in pristine Bi2Te3 are also present in ferromagnetic Mn-doped Bi2-xMnxTe3, and that the dispersion relations of the surface states are changed in a subtle fashion.

Both the theoretical and experimental discovery of single-Dirac-cone topological-insulator-class was reported at arXiv:0812.2078 (2008) [Y. Xia et.al., Nature Physics 5, 398-402 (2009) http://www.nature.com/nphys/journal/v5/n6/full/nphys1294.html]. Here we report the first observation of Spin-Momentum Helical Locking and Spin-Vortex structures in Bi2Se3 and Bi2Te3, demonstrate the existence of Topological-Order at 300K and report a material realization of topological-transport-regime for helical Dirac fermions. Our results reveal a one-to-one spin-momentum locked Dirac structure in Bi2Se3 and Bi2Te3 that is nearly 100% 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-transport-regime. The observed topological nodal Dirac ground state is found to be protected even up to room temperature (300 K). Our results pave the way for future transport based studies of topological insulators, and possible room temperature applications of protected spin-polarized edge channels we observe with spin-ARPES in spintronic technology. All of these new results are made possible due to the Spin-resolved-ARPES (Mott polarimetric) technique [http://www.nature.com/nature/journal/v460/n7259/full/nature08234.html ] ., Comment: 17 pages, 4 Figures, Published nature-Online in July-2009, Submitted to NATURE in April-2009

We report high-resolution spin-resolved photoemission spectroscopy (Spin-ARPES) measurements on the parent compound Sb of the recently discovered 3D topological insulator Bi1-xSbx [D. Hsieh et al., Nature 452, 970 (2008)]. By modulating the incident photon energy, we are able to map both the bulk and (111) surface band structure, from which we directly demonstrate that the surface bands are spin polarized by the spin-orbit interaction and connect the bulk valence and conduction bands in a topologically non-trivial way. A unique asymmetric Dirac surface state gives rise to a k-splitting of its spin polarized electronic channels. These results complement our previously published works on this materials class and re-confirm our discovery of topological insulator states in the Bi-Sb series., Comment: 5 pages, 5 figures

When electrons are subject to a large external magnetic field, the conventional charge quantum Hall effect \cite{Klitzing,Tsui} dictates that an electronic excitation gap is generated in the sample bulk, but metallic conduction is permitted at the boundary. Recent theoretical models suggest that certain bulk insulators with large spin-orbit interactions may also naturally support conducting topological boundary states in the extreme quantum limit, which opens up the possibility for studying unusual quantum Hall-like phenomena in zero external magnetic fields. Bulk Bi{1-x}Sbx single crystals are predicted to be prime candidates for one such unusual Hall phase of matter known as the topological insulator. The hallmark of a topological insulator is the existence of metallic spin-textured surface states that are higher dimensional analogues of the edge states that characterize a quantum spin Hall insulator. Here, using incident-photon-energy-modulated angle-resolved photoemission spectroscopy, we report the direct observation of massive Dirac particles in the bulk of Bi0.9Sb0.1, locate the Kramers' points at the sample's boundary and provide a comprehensive mapping of the topological Dirac insulator's gapless surface modes. These findings taken together suggest that the observed surface state on the boundary of the bulk insulator is a realization of the much sought exotic "topological metal". They also suggest that this material has potential application in developing next-generation quantum computing devices that may incorporate "light-like" bulk carriers and topologically protected spin-textured edge-surface currents. This work is a detailed version of [Hsieh et.al., NATURE 452, 970 (2008), {Submitted in November 2007}]., Comment: 12 pages, 7 figures, This is a detailed version of the work presented at NATURE 452, 970 (2008), {Submitted in November 2007}

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 novel topological order whose identification requires a spin sensitive measurement. Using Spin-resolved-ARPES, we probe the spin degrees of freedom and demonstrate that topological quantum numbers are uniquely determined from spin-texture Berry Phase imaging measurements. Applying this method to pure antimony (Sb) and Bi-Sb, we identify the origin of its novel Topological Order and the negative value of the mirror Chern number. These results taken together constitute the first observation of surface electrons collectively carrying a topological Berry's phase and definite mirror Chern chirality in pure Antimony (Sb) which are the key electronic properties for realizing topological quantum computing via the interface Majorana fermion framework. This paper contains the details of the above mentioned previously reported (Science \textbf{323}, 919 (2009)) results., Comment: 6 Figures, 10 Pages, RevTex Format, Detailed version of Hsieh et.al., SCIENCE 323, 919 (2009)

We show that the strongly spin-orbit coupled materials Bi2Te3 and Sb2Te3 (first non-Bi topological insulator) and their derivatives belong to the Z2 (Time-Reversal-Protected, elastic backscattering suppressed) 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 (about 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 surface spin-only Dirac fermions can be controlled through systematic Mn doping, making these materials classes potentially suitable for exploring novel topological physics. We emphasize (theoretically and experimentally) that the Dirac node is well within the bulk-gap and not degenerate with the bulk valence band., Comment: 5 Pages, 4 Figures, Accepted for publication in Physical Review Letters (submitted, June 2009)

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 ~ 2 x 10^20cm-3, results in superconductivity at 3.8 K in CuxBi2Se3 for x between 0.12 and 0.15. This demonstrates that Cooper pairing is possible in Bi2Se3 at accessible temperatures, with implications for study of the physics of topological insulators and potential devices., Comment: 6 pages, 4 figures

Photoemission experiments have shown that Bi$_2$Se$_3$ is a topological insulator. By controlled doping, we have obtained crystals of Bi$_2$Se$_3$ with non-metallic 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 200-500$\times$ larger than expected from universal conductance fluctuations. The results point to very long phase breaking lengths in an unusual conductance channel in these non-metallic samples. We discuss the nature of the in-gap conducting states and their relation to the topological surface states., Comment: 4 pages, 4 figures, changes in text in final paragraph

Recent theories and experiments have suggested that strong spin-orbit coupling effects in certain band insulators can give rise to a new phase of quantum matter, the so-called topological insulator, which can show macroscopic entanglement effects. Such systems feature two-dimensional surface states whose electrodynamic properties are described not by the conventional Maxwell equations but rather by an attached axion field, originally proposed to describe strongly interacting particles. It has been proposed that a topological insulator with a single spin-textured Dirac cone interfaced with a superconductor can form the most elementary unit for performing fault-tolerant quantum computation. Here we present an angle-resolved photoemission spectroscopy study and first-principle theoretical calculation-predictions that reveal the first observation of such a topological state of matter featuring a single-surface-Dirac-cone realized in the naturally occurring Bi$_2$Se$_3$ class of materials. Our results, supported by our theoretical predictions and calculations, demonstrate that undoped compound of this class of materials can serve as the parent matrix compound for the long-sought topological device where in-plane surface carrier transport would have a purely quantum topological origin. Our study further suggests that the undoped compound reached via n-to-p doping should show topological transport phenomena even at room temperature., Comment: 3 Figures, 18 pages, Submitted to NATURE PHYSICS in December 2008

Topological insulators are a new class of insulators in which a bulk gap for electronic excitations is generated by strong spin orbit coupling. These novel materials are distinguished from ordinary insulators by the presence of gapless metallic boundary states, akin to the chiral edge modes in quantum Hall systems, but with unconventional spin textures. Recently, experiments and theoretical efforts have provided strong evidence for both two- and three-dimensional topological insulators and their novel edge and surface states in semiconductor quantum well structures and several Bi-based compounds. A key characteristic of these spin-textured boundary states is their insensitivity to spin-independent scattering, which protects them from backscattering and localization. These chiral states are 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. Here we use a scanning tunneling microscope (STM) to visualize the gapless surface states of the three-dimensional topological insulator BiSb and to examine their scattering behavior from disorder caused by random alloying in this compound. Combining STM and angle-resolved photoemission spectroscopy, we show that despite strong atomic scale disorder, backscattering between states of opposite momentum and opposite spin is absent. Our observation of spin-selective scattering demonstrates that the chiral nature of these states protects the spin of the carriers; they therefore have the potential to be used for coherent spin transport in spintronic devices., Comment: to be appear in Nature on August 9, 2009

Three dimensional (3D) topological insulators are quantum materials with a spin-orbit induced bulk insulating gap that exhibit quantum-Hall-like phenomena in the absence of applied magnetic fields. The proposed applications of topological insulators in device geometries rely on the ability to tune the chemical potential on their surfaces in the vicinity of the Dirac node. Here, we demonstrate a suite of surface control methods based on a combination of photo-doping and molecular-doping to systematically tune the Dirac fermion density on the topological (111) surface of Bi2Te3. Their efficacy is demonstrated via direct electronic structure topology measurements using high resolution angle-resolved photoemission spectroscopy (ARPES). These results open up new opportunities for probing topological behavior of Dirac electrons on the Bi2Te3 surface. At least one of the methods demonstrated here can be successfully applied to other topological insulators such as the Bi{1-x}Sb{x}, Sb2Te3 and Bi2Se3 which will be shown elsewhere. More importantly, our methods of topological surface state manipulation demonstrated here are highly suitable for future spectroscopic studies of topological phenomena which will complement the transport results gained from the traditional electrical gating techniques., Comment: 4 Figures, 12 pages

Electron systems that possess light-like dispersion relations or the conical Dirac spectrum, such as graphene and bismuth, have recently been shown to harbor unusual collective states in high magnetic fields. Such states are possible because their light-like electrons come in spin pairs that are chiral,which means that their direction of propagation is tied to a quantity called pseudospin that describes their location in the crystal lattice. An emerging direction in quantum materials research is the manipulation of atomic spin-orbit coupling to simulate the effect of a spin dependent magnetic field,in attempt to realize novel spin phases of matter. This effect has been proposed to realize systems consisting of unpaired Dirac cones that are helical, meaning their direction of propagation is tied to the electron spin itself, which are forbidden to exist in graphene or bismuth. The experimental existence of topological order can not be determined without spin-resolved measurements. Here we report a spin-and angle-resolved photoemission study of the hexagonal surface of the Bi2Te3 and Bi{2-x}MnxTe3 series, which is found to exhibit a single helical Dirac cone that is fully spin-polarized. Our observations of a gap in the bulk spin-degenerate band and a spin-resolved surface Dirac node close to the chemical potential show that the low energy dynamics of Bi2Te3 is dominated by the unpaired spin-helical Dirac modes. Our spin-texture measurements prove the existence of a rare topological phase in this materials class for the first time, and suggest its suitability for novel 2D Dirac spin device applications beyond the chiral variety or traditional graphene., Comment: 13 pages, 4 figures

The growth and elementary properties of p-type Bi2Se3 single crystals are reported. Based on a hypothesis about the defect chemistry of Bi2Se3, the p-type behavior has been induced through low level substitutions (1 percent or less) of Ca for Bi. Scanning tunneling microscopy is employed to image the defects and establish their charge. Tunneling and angle resolved photoemission spectra show that the Fermi level has been lowered into the valence band by about 400 meV in Bi1.98Ca0.02Se3 relative to the n-type material. p-type single crystals with ab plane Seebeck coefficients of +180 microVK-1 at room temperature are reported. These crystals show a giant anomalous peak in the Seebeck coefficient at low temperatures, reaching +120 microVK-1 at 7 K, giving them a high thermoelectric power factor at low temperatures. In addition to its interesting thermoelectric properties, p-type Bi2Se3 is of substantial interest for studies of technologies and phenomena proposed for topological insulators., Comment: v2: STM characterization of n and p type Bi2Se3 is added

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 novel topological order whose identification requires a spin sensitive measurement, which does not exist to this date in any system (neither in Hg(Cd)Te quantum wells nor in the topological insulator BiSb). Using Mott polarimetry, we probe the spin degrees of freedom of these quantum spin Hall states and demonstrate that topological quantum numbers are uniquely determined from spin texture imaging measurements. Applying this method to the Bi{1-x}Sb{x} series, we identify the origin of its novel order and unusual chiral properties. These results taken together constitute the first observation of surface electrons collectively carrying a geometrical quantum (Berry's) phase and definite chirality (mirror Chern number, n_M =-1), which are the key electronic properties for realizing topological computing bits with intrinsic spin Hall-like topological phenomena. Our spin-resolved results not only provides the first clear proof of a topological insulating state in nature but also demonstrate the utility of spin-resolved ARPES technique in measuring the quantum spin Hall phases of matter., Comment: 15 pages, 3 figures, first Submitted to SCIENCE on July-22, 2008

When electrons are subject to a large external magnetic field, the conventional charge quantum Hall effect \cite{Klitzing,Tsui} dictates that an electronic excitation gap is generated in the sample bulk, but metallic conduction is permitted at the boundary. Recent theoretical models suggest that certain bulk insulators with large spin-orbit interactions may also naturally support conducting topological boundary states in the extreme quantum limit, which opens up the possibility for studying unusual quantum Hall-like phenomena in zero external magnetic field. Bulk Bi$_{1-x}$Sb$_x$ single crystals are expected to be prime candidates for one such unusual Hall phase of matter known as the topological insulator. The hallmark of a topological insulator is the existence of metallic surface states that are higher dimensional analogues of the edge states that characterize a spin Hall insulator. In addition to its interesting boundary states, the bulk of Bi$_{1-x}$Sb$_x$ is predicted to exhibit three-dimensional Dirac particles, another topic of heightened current interest. Here, using incident-photon-energy-modulated (IPEM-ARPES), we report the first direct observation of massive Dirac particles in the bulk of Bi$_{0.9}$Sb$_{0.1}$, locate the Kramers' points at the sample's boundary and provide a comprehensive mapping of the topological Dirac insulator's gapless surface modes. These findings taken together suggest that the observed surface state on the boundary of the bulk insulator is a realization of the much sought exotic "topological metal". They also suggest that this material has potential application in developing next-generation quantum computing devices., Comment: 16 pages, 3 Figures. Submitted to NATURE on 25th November(2007)

The interface between a superconductor and a topological insulator has been proposed to harbor novel quasiparticles that realize physical schemes for fault-tolerant quantum computation. Here, we present high resolution angle-resolved photoemission experimental results, which along with first principles calculations, suggest that the surface-edge states of Bi2Se3 form a topological 2D metal. When magnetic atoms are deposited, the surface tends to lose Kramers' degeneracy and a k-space connection thread between the bulk valence and conduction bands is lost. Our observed states carry a \pi Berry's phase suggesting that although the real materials are often electron doped fully undoped Bi2Se3 would be a Z2 topological insulator at room temperature., Comment: 11 pages and 5 figures

The recently discovered iron arsenide superconductors, which display superconducting transition temperatures as high as 55 K, appear to share a number of general features with high-Tc cuprates, including proximity to a magnetically ordered state and robustness of the superconductivity in the presence of disorder. Here we show that superconductivity in Fe1+dSe, the parent compound of the superconducting arsenide family, is destroyed by very small changes in stoichiometry. Further, we show that non-superconducting Fe1+dSe is not magnetically ordered down to low temperatures. These results suggest that robust superconductivity and immediate instability against an ordered magnetic state should not be considered as intrinsic characteristics of iron-based superconducting systems, and that Fe1+dSe may present a unique opportunity for determining which materials characteristics are critical to the existence of superconductivity in high Tc iron arsenide superconductors and which are not., Comment: Updated to reflect final version and include journal reference

We report the characterization of layered, 2H-type CuxTaS2, for x between 0 and 0.12. The charge density wave (CDW), at 70 K for TaS2, is destabilized with Cu doping. The sub-1K superconducting transition in undoped 2H-TaS2 jumps quickly to 2.5 K at low x, increases to 4.5 K at the optimal composition Cu0.04TaS2, and then decreases at higher x. The electronic contribution to the specific heat, first increasing and then decreasing as a function of Cu content, is 12 mJ mol-1 K-2 at Cu0.04TaS2. Electron diffraction studies show that the CDW remains present at the optimal superconducting composition, but with both a changed q vector and decreased coherence length. We present an electronic phase diagram for the system., Comment: 7 pages, 9 figures. To be published in Physical Review B

DC and ac magnetization, resistivity, specific heat, and neutron diffraction data reveal that stoichiometric LaOFeP is metallic and non-superconducting above T = 0.35 K, with gamma = 12.5 mJ/mol*K. Neutron diffraction data at room temperature and T = 10 K are well described by the stoichiometric, tetragonal ZrCuSiAs structure and show no signs of structural distortions or long range magnetic ordering, to an estimated detectability limit of 0.07 uB/Fe. We propose a model, based on the shape of the iron-pnictide tetrahedron, that explains the differences between LaOFeP and LaOFeAs, the parent compound of the recently discovered high-Tc oxyarsenides, which, in contrast, shows both structural and spin density wave (SDW) transitions., Comment: Submitted to PRB Rapid Comm

The low-temperature magnetic structure of \HG has been studied by high-resolution powder neutron diffraction. Long-range incommensurate magnetic order sets in at T$_N\sim$22K with propagation vector \textbf{k}=(0,0,$\sim$0.18). On cooling below T$_N$, the propagation vector increases and saturates at the commensurate value \textbf{k}=(0,0,0.25). The magnetic structure below T$_N$ consists of ferromagnetic layers in the \textit{ab}-plane stacked in a spiral arrangement along the \textit{c}-axis. Symmetry analysis using corepresentations theory reveals a point group symmetry in the ordered magnetic phase of 422 (D$_4$), which is incompatible with macroscopic ferroelectricity. This finding indicates that the spontaneous electric polarization observed experimentally cannot be coupled to the magnetic order parameter.