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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.

The magnetic structure of multiferroic Ni$_3$V$_2$O$_8$ has been investigated using non-resonant X-ray magnetic scattering. Incident circularly polarized X-rays combined with full polarization analysis of the scattered beam is shown to yield high sensitivity to the components of the cycloidal magnetic order, including their relative phases. New information on the magnetic structure in the ferroelectric phase is obtained, where it is found that the magnetic moments on the "cross-tie" sites are quenched relative to those on the "spine" sites. This implies that the onset of ferroelectricity is associated mainly with spine site magnetic order. We also demonstrate that our technique enables the imaging of multiferroic domains through polarization enhanced topography. This approach is used to image the domains as the sample is cycled by an electric field through its hysteresis loop, revealing the gradual switching of domains without nucleation., Comment: 9 pages, 6 figures

The temperature and pressure dependence of the partial density of phonon states of iron atoms in superconducting Fe1.01Se was studied by 57Fe nuclear inelastic scattering (NIS). The high energy resolution allows for a detailed observation of spectral properties. A sharpening of the optical phonon modes and shift of all spectral features towards higher energies by ~4% with decreasing temperature from 296 K to 10 K was found. However, no detectable change at the tetragonal - orthorhombic phase transition around 100 K was observed. Application of a pressure of 6.7 GPa, connected with an increase of the superconducting temperature from 8 K to 34 K, results in an increase of the optical phonon mode energies at 296 K by ~12%, and an even more pronounced increase for the lowest-lying transversal acoustic mode. Despite these strong pressure-induced modifications of the phonon-DOS we conclude that the pronounced increase of Tc in Fe1.01Se with pressure cannot be described in the framework of classical electron-phonon coupling. This result suggests the importance of spin fluctuations to the observed superconductivity.

The gallium substituted and calcium deficient variants of geometrically frustrated b-CaCr2O4, b-CaCr2-2xGa2xO4 (0.02<= x<= 0.25) and b-Ca1-yCr2O4 (0.075<= y<= 0.15), have been investigated by x-ray powder diffraction, magnetization and specific heat measurements. This allows for a direct comparison of the effects, in a geometrically frustrated magnet, of the static disorder that arises from non-magnetic substitution and the dynamic disorder that arises from hole doping. In both cases, disturbing the Cr3+ lattice results in a reduction in the degree of magnetic frustration. On substitution of Ga, which introduces disorder without creating holes, a gradual release of spins from ordered antiferromagnetic states is observed. In contrast, in the calcium deficient compounds the introduction of holes induces static ferrimagnetic ordering and much stronger perturbations of the b-CaCr2O4 host., Comment: 23 pages, 10 figures

We have extended our new materials class search for the experimental realization of Z2 topological insulators from binary [Bi2Se3-class, Xia et.al., Nature Phys. 5, 398 (2009)] and the ternary [Half-Heusler class, Lin et.al., arXiv:1003.0155v1 (2010); arXiv:1003.2615v1 (2010)] series to non-Heusler Li-based ternary intermetallic series Li2M'X ($M'$=Cu, Ag, and Au, $X$=Sb and Bi) with CuHg2Ti-type structure. We discovered that the distorted-Li2AgSb is a lightweight compound harboring a 3D topological insulator state with Z2=-1 although the groundstate lies near a critical point, whereas the related Li2CuSb-type compounds are topologically trivial. Non-Heusler ternary Li2M'X series (with a number of variant compounds) we identified here is a new platform for deriving novel stoichiometric compounds, artificial quantum-well/heterostructures, nano-wires, nano-ribbons and nanocrystals. We have grown some of these bulk materials (experimental results will be reported separately)., Comment: 3 figures, 4+ pages

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

Topological insulators (TI) realize a novel state of quantum matter that are distinguished by topological invariants of bulk band structure rather than spontaneously broken symmetries. A number of exotic quantum phenomena have been predicted to exist in multiply-connected geometries which require an enormous amount of materials flexibility. We have extended our previous search for TI materials from binary (Bi2X3 series) to the thermoelectric ternary compounds. We discover that the distorted LuPtSb is the first ternary compound harboring a 3D topological insulator state. We also show that the half-Heusler LuPtSb-type series is a natural platform that hosts a range of candidate compounds, alloys and artificial heterostructures (quantum-wells). We also discovered several different paradigms of trivial and non-trivial topological ordering in this class, including a metallic nontrivial topological state in YAuPb. Some of these materials are grown (results will be reported separately)., Comment: 6 Pages, 3 Figures

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.

We have searched for time-reversal symmetry breaking fields in the non-centrosymmetric superconductor Mg$_{10}$Ir$_{19}$B$_{16}$ via muon spin relaxation in zero applied field, and we measured the temperature dependence of the superfluid density by muon spin rotation in transverse field to investigate the superconducting pairing symmetry in two polycrystalline samples of signficantly different purities. In the high purity sample, we detected no time-reversal symmetry breaking fields greater than 0.05 G. The superfluid density was also found to be exponentially-flat as T$\to $0, and so can be fit to a single-gap BCS model. In contrast, the lower purity sample showed an increase in the zero-field $\mu$SR relaxation rate below T$_c$ corresponding to a characteristic field strength of 0.6 G. While the temperature-dependence of the superfluid density was also found to be consistent with a single-gap BCS model, the magnitude as T$\to $0 was found to be much lower for a given applied field than in the case of the high purity sample. These findings suggest that the dominant pairing symmetry in high quality Mg$_{10}$Ir$_{19}$B$_{16}$ samples corresponds to the spin-singlet channel, while sample quality drastically affects the superconducting properties of this system., Comment: 6 pages, 5 figures, revised version resubmitted to PRB

Neutron scattering and magnetization measurements have been performed on the stuffed pyrochlore system Tb2+xTi2-2xNbxO7. We find that despite the introduction of chemical disorder and increasingly antiferromagnetic interactions, a spin glass transition does not occur for T >= 1.5 K and cooperative paramagnetic behavior exists for all x. For x = 1, Tb3NbO7, an antiferromagnetically ordered state coexisting with cooperative paramagnetic behavior is seen without applying any external fields or pressure, a situation advantageous for studying this cooperative behavior.

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

The Cu-doped topological insulator Bi$_2$Se$_3$ has recently been found to undergo a superconducting transition upon cooling, raising the possibilities that it is the first known "topological superconductor" or realizes a novel non-Abelian superconducting state. Its true nature depends critically on the bulk and surface state band topology. We present the first photoemission spectroscopy results where by examining the band topology at many different copper doping values we discover that the topologically protected spin-helical surface states remain well protected and separate from bulk Dirac bands at the Fermi level where Copper pairing occurs in the optimally doped topological insulator. The addition of copper is found to result in nonlinear electron doping and strong renormalization of the topological surface states. These highly unusual observations strongly suggest that superconductivity on the topological surface of Cu$_x$Bi$_2$Se$_3$ cannot be of any conventional type in account of the general topological theory. Characteristics of the three dimensional bulk Dirac band structure are reported for the first time with respect to the superconducting doping state and topological invariant properties which should help formulate a specific theory for this novel superconductor., Comment: 4 Figures, 5 pages, Submitted December 2009

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)

The magnetic susceptibilities and specific heats of the crystalline garnet and glass forms of Mn3Al2Si3O12 are reported. This allows a direct comparison of the degree of magnetic frustration of the triangle-based garnet lattice and the structurally disordered solid at the same composition for isotropic spin 5/2 Mn^2+ (3d^5). The results show that the glass phase shows more pronounced signs of magnetic frustration than the crystalline phase. Through comparison of the specific heats of Ca3Al2Si3O12 (grossular) and Mn3Al2Si3O12 (spessartine) garnets, information is provided concerning the anomalous extra specific heat in the latter material.

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

We report that the 122 type Sr$_{1-x}$Ca$_x$Co$_2$P$_2$ solid solution undergoes an anomalous structural transition from the uncollapsed to the collapsed ThCr$_2$Si$_2$ structure at a distinct onset composition near $x=0.5$. Correlated with the structural changes, the electronic system evolves from a nearly ferromagnetic Fermi liquid to an antiferromagnetic metal, through a complex crossover regime. The structural collapse, driven by P-P bonding across the (Sr,Ca) layers, is much more pronounced in this system than it is in the analogous Fe-based system, indicating a strong sensitivity of structure to total electron count in the transition metal pnictide 122 family., Comment: 5 pages, 7 figures, accepted by PRB

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

Ni2SiO4, Liebenbergite, is an example of a quasi-one-dimensional magnet made up of frustrated corner sharing triangles of Ni2+ (S = 1) ions that propagate parallel to the b axis. Ni2SiO4 is isostructural with olivine, a common mineral of varying composition Fe2-xMgxSiO4, and is described in the orthorhombic space group Pnma. A synthetic polycrystalline sample of Ni2SiO4 was studied using constant wavelength powder neutron diffraction. Diffraction spectra were collected above and below the antiferromagnetic ordering transition (TN ~ 34 K) and were used to refine the atomic and magnetic structures of Ni2SiO4. Corepresentational theory was used to determine the symmetry-allowed magnetic structures after the Neel transition and the refned magnetic structure evidences both ferromagnetic and antiferromagnetic inter-chain interactions, and ferromagnetic intra-chain coupling. The competition between the magnetic interactions can be seen in the canting of the moments away from a collinear arrangement., Comment: 4 pages, 2 figures, 1 table, conference proceeding

Tetragonal iron selenide, FeSe, the layered parent compound of the recently discovered superconducting arsenide family, has previously been shown to be non magnetic and superconducting with a critical temperature near 8 K. There has, however, been a lack of consensus as to whether selenium vacancies present due to large deviations from ideal stoichiometry are required to give rise to the superconductivity. Here we describe the results of experiments that demonstrate simply that superconducting iron selenide can only be synthesized as a pure material when near stoichiometric (i.e. FeSe). Significant selenium deficiency or excess gives rise to secondary magnetic phases, and a suppression of the superconductivity.

Single crystals of Fe$_{1/4}$TaS$_{2}$ have been studied by using magneto-optical (MO) imaging and radio-frequency (rf) magnetic susceptibility, $\chi$. Real time MO images reveal unusual, slow dynamics of dendritic domain formation, the details of which are strongly dependent upon magnetic and thermal history. Measurements of $\chi(T)$ show well-defined, local moment ferromagnetic transition at $T\approx 155$ K as well as thermal hysteresis for 50 K$

Iron Selenide, Fe1.01Se, the layered parent compound of the recently discovered superconducting arsenide family, has previously been shown to be non magnetic and superconducting with a critical temperature of 8 K. Here we show that copper can be substituted at the iron site in Fe1.01Se up to a solubility limit of 20-30 %, after which a first order transition to the three-dimensional CuFeSe2 structure type is observed. As little as 1.5 % percent copper is sufficient to suppress the superconductivity, and 4 % drives the system through a metal-insulator transition. A local magnetic moment is introduced, which maximizes near 12% doping, where a spin-glass transition near 15 K is observed.

In this letter we show that superconducting Fe1.01Se undergoes a structural transition at 90 K from a tetragonal to an orthorhombic phase but that non-superconducting Fe1.03Se does not. Further, high resolution electron microscopy study at low temperatures reveals an unexpected additional modulation of the crystal structure of the superconducting phase involving displacements of the Fe atoms, and that the non-superconducting material shows a distinct, complex nanometer-scale structural modulation. Finally, we show that magnetism is not the driving force for the phase transition in the superconducting phase., Comment: 5 pages, 5 figures

Superconductivity in LaNiPO is disrupted by small (~5%) amounts of non-stoichiometry on the lanthanum site, even though the electronic contribution to the heat capacity increases with increasing non-stoichiometry. All samples also exhibit specific heat anomalies consistent with the presence of ferromagnetic spin fluctuations (Tsf ~ 14 K). Comparison of layered nickel phosphide and nickel borocarbide superconductors reveals different structure-property correlations in the two families., Comment: Submitted to Phys. Rev. B

Electric control of multiferroic domains is demonstrated through polarized magnetic neutron diffraction. Cooling to the cycloidal multiferroic phase of Ni3V2O8 in an electric field (E) causes the incommensurate Bragg reflections to become neutron spin polarizing, the sense of neutron polarization reversing with E. Quantitative analysis indicates the E-treated sample has handedness that can be reversed by E. We further show close association between cycloidal and ferroelectric domains through E-driven spin and electric polarization hysteresis. We suggest that definite cycloidal handedness is achieved through magneto-elastically induced Dzyaloshinskii-Moriya interactions., Comment: 4 pages, 5 figures. Updated affiliations and references. Minor changes to text and figures

The coupling between localized spins and phonons can lead to shifts in the dielectric constant of insulating materials at magnetic ordering transitions. Studies on isostructural SeCuO3 (ferromagnetic) and TeCuO3 (antiferromagnetic) illustrate how the q-dependent spin-spin correlation function couples to phonon frequencies leading to a shift in the dielectric constant. A model is discussed for this spin-phonon coupling. The magnetodielectric coupling in multiferroic materials can be very large at a ferroelectric transition temperature. This coupling is investigated in the recently identified multiferroic Ni3V2O8., Comment: 4 pages, 3 figures. Originally appeared in: The Twelfth US-Japan Seminar on Dielectric and Piezoelectric Ceramics, p. 215 (2005) (unpublished conference proceedings). The manuscript has not been modified or updated in any way from this version

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

In this letter, we report that the superconductivity transition temperature in beta-Fe1.01Se increases from 8.5 to 36.7 K under applied pressure of 8.9 GPa. It then decreases at higher pressure. A dramatic change in volume is observed at the same time Tc rises, due to a collapse of the separation between the Fe2Se2 layers. A clear transition to a linear resistivity normal state is seen on cooling at all pressures. No static magnetic ordering is observed for the whole p-T phase diagram. We also report that at higher pressure (starting around 7 GPa and completed at 38 GPa), Fe1.01Se transforms to a hexagonal NiAs-type structure and displays non-magnetic, insulating behavior. The inclusion of electron correlation in band structure caculations is necessary to describe this behavior, signifying that such correlations are important in this chemical system. Our results strongly support unconventional superconductivity in beta-Fe1.01Se., Comment: 17 pages, 4 figures

Unlike the parent phases of the iron-arsenide high Tc superconductors, undoped FeSe is not magnetically ordered and exhibits superconductivity with Tc~9K. Equally surprising is the fact that applied pressure dramatically enhances the modest Tc to ~37K. We investigate the electronic properties of FeSe using 77Se NMR to search for the key to the superconducting mechanism. We demonstrate that the electronic properties of FeSe are very similar to those of electron-doped FeAs superconductors, and that antiferromagnetic spin fluctuations are strongly enhanced near Tc. Furthermore, applied pressure enhances spin fluctuations. Our findings suggest a link between spin fluctuations and the superconducting mechanism in FeSe., Comment: Accepted for publication in Phys. Rev. Lett. after minor revision

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 systematic low temperature measurements of the DC magnetization, AC susceptibility, and heat capacity of dysprosium pyrogermanate (Dy2Ge2O7) single crystal and powder samples. Our results confirm that Dy2Ge2O7 is an anisotropic antiferromagnet. The isothermal field dependent magnetization and the integrated magnetic entropy both indicate that the Dy3+ ions behave as Ising-like spins, analogous to those in the pyrochlore spin ice materials. Both single-spin and collective spin relaxation phenomena appear to lead to spin freezing in this material, again in analogy to observations in the spin ice materials, suggesting that such phenomena may be generic to a broader class of magnetic materials., Comment: Phys. Rev. B, in press (2008)

This work reports on the novel Heusler superconductor ZrNi2Ga. Compared to other nickel-based superconductors with Heusler structure, ZrNi2Ga exhibits a relatively high superconducting transition temperature of Tc=2.9 K and an upper critical field of 1.5 T. Electronic structure calculations show that this relatively high transition temperature is caused by a van Hove singularity, which leads to an enhanced density of states at the Fermi energy. The van Hove singularity originates from a higher order valence instability at the L-point in the electronic structure. The enhanced density of states at the Fermi level was confirmed by specific heat and susceptibility measurements. Although many Heusler compounds are ferromagnetic, our measurements of ZrNi2Ga indicate a paramagnetic state above Tc and could not reveal any traces of magnetic order down to temperatures of at least 0.35 K. We investigated in detail the superconducting state with specific heat, magnetization, and resistivity measurements. The resulting data show the typical behavior of a conventional, weakly coupled BCS (s-wave) superconductor., Comment: 27 pages in preprint style, 11 Figures

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

We report the observation of superconductivity in La3Ni4P4O2 at 2.2 K. The layer stacking in this compound results in an asymmetric distribution of charge reservoir layers around the Ni2P2 planes. The estimated Wilson ratio, Rw ~ 5, indicates the presence of a strongly enhanced normal state susceptibility, but many of the basic superconducting characteristics are conventional. The estimated electronic contribution to the specific heat, gamma ~ 6.2 mJ mol-Ni^-1K^-2, is about 2/3 of that found in layered nickel borocarbide superconductors., Comment: Updated to reflect final version. Added journal reference

Neutron diffraction and magnetization measurements of the magneto refrigerant Mn1+yFe1-yP1-xGex reveal that the ferromagnetic and paramagnetic phases correspond to two very distinct crystal structures, with the magnetic entropy change as a function of magnetic field or temperature being directly controlled by the phase fraction of this first-order transition. By tuning the physical properties of this system we have achieved a maximum magnetic entropy change exceeding 74 J/Kg K for both increasing and decreasing field, more than twice the value of the previous record., Comment: 6 Figures. One table

The crystal structures of the triangular lattice, layered anhydrous alums KCr(SO4)2, RbCr(SO4)2 and KAl(SO4)2 are characterized by X-ray and neutron powder diffraction at temperatures between 1.4 and 773 K. The compounds all crystallize in the space group P-3, with octahedral coordination of the trivalent cations. In all cases, small amounts of disorder in the stacking of the triangular layers of corner sharing MO6 octahedra and SO4 tetrahedra is seen, with the MO6-SO4 network rotated in opposite directions between layers. The electron diffraction study of KCr(SO4)2 supports this model, which on average can be taken to imply trigonal prismatic coordination for the M3+ ions; as was previously reported for the prototype anhydrous alum KAl(SO4)2. The temperature dependent magnetic susceptibilities for ACr(SO4)2 (A = K,Rb,Cs) indicate the presence of predominantly ferromagnetic interactions. Low temperature powder neutron diffraction reveals that the magnetic ordering is ferromagnetic in-plane, with antiferromagnetic ordering between planes below 3 K., Comment: Accepted to the Journal of Solid State Chemistry

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 crystal structures of the A2B2O7-x Niobium-based pyrochlores Y2(Nb0.86Y0.14)2O6.91, CaYNb2O7, and Y2NbTiO7 are reported, determined by powder neutron diffraction. These compounds represent the first observation of B-site displacements in the pyrochlore structure: the B-site ions are found to be displaced from the ideal pyrochlore positions, creating electric dipoles. The orientations of these dipoles are fully analogous to orientations of the magnetic moments in Ising spin based magnetically frustrated pyrochlores. Diffuse scattering in electron diffraction patterns shows that the displacements are only short range ordered, indicative of geometric frustration of the collective dielectric state of the materials. Comparison to the crystal structure of the Nb5+ (d0) pyrochlore La2ScNbO7 supports the prediction that charge singlets, driven by the tendency of Nb to form metal-metal bonds, are present in these pyrochlores. The observed lack of long-range order to these singlets suggests that Nb4+-based pyrochlores represent the dielectric analogy to the geometric frustration of magnetic moments observed in rare earth pyrochlores., Comment: Accepted to Journal of Physics: Condensed Matter

We report the properties of two new isostructural compounds, U3Bi4Ni3 and U3Bi4Rh3. The first of these compounds is non-metallic, and the second is a nearly ferromagnetic metal, both as anticipated from their electron count relative to other U-based members of the larger 3-4-3 family. For U3Bi4Rh3, a logarithmic increase of C/T below 3 K, a resistivity proportional to T^4/3, and the recovery of Fermi-liquid behavior in both properties with applied fields greater than 3T, suggest that U3Bi4Rh3 may be a new example of a material displaying ferromagnetic quantum criticality., Comment: 24 pages, 7 figures, submitted to Physical Review B

The synthesis and characterization of the pyrochlore solid solutions, Y2Ti2-xNbxO7-y, Lu2Ti2-xNbxO7-y, Y2Ti2-xTaxO7-y and Lu2TiTaO7-y (-0.4