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A series of garnets of formula Er3+xGa5-xO12 is described, for which we report the crystal structures for both polycrystalline and single-crystal samples. The x limit in the garnet phase is between 0.5 and 0.6 under our conditions, with the Er fully occupying the normal garnet site plus half-occupying the octahedral site at x = 0.5 in place of the Ga normally present. Long-range antiferromagnetic order with spin ice-like frustration is suggested by the transition temperature (TN=0.8K) being much lower than the Curie-Weiss theta. The magnetic ordering temperature does not depend on the Er excess, but there is increasing residual entropy as the Er excess is increased, highlighting the potential for unusual magnetic behavior in this system., 13 pages, 4 figures

A previously unreported layered spin 1/2 triangular lattice polymorph of TiI3 is described, synthesized under 6 GPa of applied pressure at 900 C, but stable at atmospheric pressure. This air-sensitive material has a CdI2-type layered structure (P-3m1 (#164), a = 4.012 A and c = 6.641 A at 120 K, Z = 1 of Ti0.667I2) with an in-plane triangular lattice, related to that of TiI4 (Ti0.5I2). Although the TiI3 formula is consistent with expectations for a layered honeycomb lattice of spin 1/2 Ti(III), there appears to be disorder in the crystal structure. Magnetic susceptibility and heat capacity measurements suggest that the material undergoes several low temperature phase transitions.

Quantum spin liquids (QSLs) are topologically ordered exotic states of matter that host fractionalized excitations. Kitaev proposed a particular route towards a QSL via strongly bond-dependent interactions on the hexagonal lattice. A number of candidate Kitaev QSL materials have been pursued, but all have appreciable non-Kitaev interactions, which put these systems far from the QSL regime. Using time-domain terahertz spectroscopy (TDTS) we observed a broad magnetic continuum over a wide range of temperature and field in the honeycomb cobalt-based magnet, BaCo$_2$(AsO$_4$)$_2$, which has been proposed to be more ideal versions of a Kitaev QSL. Applying a small in-plane magnetic field of $\sim$ 0.5 T suppresses the magnetic order and at at even higher fields gives rise to a spin-polarized state. With 4T magnetic field oriented principally out-of-plane, a broad magnetic continuum was observed that could be consistent with a field induced QSL. Our results indicate BaCo$_2$(AsO$_4$)$_2$ to be a promising QSL candidate.

The Kitaev model predicts that quantum spin liquids (QSLs) will form at low temperatures under certain special conditions, and materials hosting the QSL state are frequently sought. The layered honeycomb lattice material ��-RuCl3 has emerged as a prime candidate for displaying the Kitaev QSL state. Here we describe a new polymorph of RuI3 with a layered honeycomb lattice structure, synthesized at moderately high pressures and stable under ambient conditions. Preliminary characterization reveals metallic, paramagnetic behavior, the absence of long-range magnetic order down to 0.35 K and an unusually large T-linear contribution to the heat capacity at low temperatures. We propose that this RuI3 phase, with a layered honeycomb lattice and strong spin-orbit coupling, provides a new route for the characterization of quantum materials.

In the present work, we investigate the electronic structure of the two-dimensional (2D) ferromagnet Cr2Ge2Te6 by photoemission spectroscopy and ab initio calculations. Our results demonstrate the presence of multiple hole-type bands in the vicinity of the Fermi level indicating that the material can support high electrical conductivity by manipulating the chemical potential. Also, our photon energy dependent angle resolved photoemission experiment revealed that several of the hole bands exhibit weak dispersion with varied incident photon energy providing experimental signature for its two dimensionality. These findings can pave the way for further studies towards the application of Cr2Ge2Te6 in electronic devices., 8 pages, 3 figures

Cobalt pyrochlore fluoride NaCaCo$_2$F$_7$ is a disordered frustrated magnet composed of Co$^{2+}$ ions with an effective spin-$\frac{1}{2}$ magnetic moment and exhibits spin freezing below $T_f \sim$2.4 K. We perform ultrasound velocity measurements on a single crystal of the cubic NaCaCo$_2$F$_7$. The temperature dependence of the bulk modulus (the breathing elastic mode) exhibits Curie-type softening upon cooling below $\sim$20 K down to $T_f$, which is suppressed by the magnetic field. This Curie-type softening should be a precursor to the enhancement of the strength of exchange disorder via the spin-lattice coupling, which causes the spin freezing. In contrast to the magnetic-field-suppressed Curie-type softening in the bulk modulus, the trigonal shear modulus exhibits softening with a characteristic minimum upon cooling, which is enhanced by the magnetic field at temperatures below $\sim$20 K. This magnetic-field-enhanced elastic anomaly in the trigonal shear modulus suggests a coupling of the lattice to the dynamical spin-cluster state. For NaCaCo$_2$F$_7$, the observed elastic anomalies reveal an occurrence of magnetic-field-induced crossover from an isostructural lattice instability toward the spin freezing to a trigonal lattice instability arising from the emergent dynamical spin-cluster state., 8 pages, 5 figures

The crystal structures of the Sr1-xCaxRuO3 perovskites are investigated using both long range and local structural probes. High resolution synchrotron powder X-ray diffraction characterization at ambient temperature shows that the materials are orthorhombic to high precision, and we support previous work showing that Ca2+ substitution for Sr2+ primarily changes the tilting of rigid corner-sharing RuO6 octahedra at their shared oxygen vertices. X-ray pair distribution function analysis for SrRuO3, CaRuO3 and one intermediate composition show them to be locally monoclinic, and no long range or local phase transitions are observed between 80 and 300 K for materials with intermediate compositions. High-resolution transmission electron microscopy shows that the Sr/Ca distribution is random at the nanoscale. We plot magnetic characteristics such as the ferromagnetic Tc, Curie-Weiss theta, effective moment, and ambient temperature susceptibility vs. the octahedral tilt and unit cell volume., Comment: 20 Figures

Currently, there is a flurry of research interest on materials with an unconventional electronic structure, and we have already seen significant progress in their understanding and engineering towards real-life applications. The interest erupted with the discovery of graphene and topological insulators in the previous decade. The electrons in graphene simulate massless Dirac Fermions with a linearly dispersing Dirac cone in their band structure, while in topological insulators, the electronic bands wind non-trivially in momentum space giving rise to gapless surface states and bulk bandgap. Weyl semimetals in condensed matter systems are the latest addition to this growing family of topological materials. Weyl Fermions are known in the context of high energy physics since almost the beginning of quantum mechanics. They apparently violate charge conservation rules, displaying the "chiral anomaly", with such remarkable properties recently theoretically predicted and experimentally verified to exist as low energy quasiparticle states in certain condensed matter systems. Not only are these new materials extremely important for our fundamental understanding of quantum phenomena, but also they exhibit completely different transport phenomena. For example, massless Fermions are susceptible to scattering from non-magnetic impurities. Dirac semimetals exhibit non-saturating extremely large magnetoresistance as a consequence of their robust electronic bands being protected by time reversal symmetry. These open up whole new possibilities for materials engineering and applications including quantum computing. In this review, we recapitulate some of the outstanding properties of WTe$_2$, namely, its non-saturating titanic magnetoresistance due to perfect electron and hole carrier balance up to a very high magnetic field observed for the very first time. (Continued. Please see the main article)., 33 pages, 7 figures

The success of black phosphorus in fast electronic and photonic devices is hindered by its rapid degradation in presence of oxygen. Orthorhombic tin selenide is a representative of group IV-VI binary compounds that are robust, isoelectronic, and share the same structure with black phosphorus. We measured the band structure of SnSe and found highly anisotropic valence bands that form several valleys having fast dispersion within the layers and negligible dispersion across. This is exactly the band structure desired for efficient thermoelectric generation where SnSe has shown a great promise.

It has been long hoped that the realization of long-range ferromagnetic order in two-dimensional (2D) van der Waals (vdW) crystals, combined with their rich electronic and optical properties, would open up new possibilities for magnetic, magnetoelectric and magneto-optic applications. However, in 2D systems, the long-range magnetic order is strongly hampered by thermal fluctuations which may be counteracted by magnetic anisotropy, according to the Mermin-Wagner theorem. Prior efforts via defect and composition engineering, and proximity effect only locally or extrinsically introduce magnetic responses. Here we report the first experimental discovery of intrinsic long-range ferromagnetic order in pristine Cr2Ge2Te6 atomic layers by scanning magneto-optic Kerr microscopy. In such a 2D vdW soft ferromagnet, for the first time, an unprecedented control of transition temperature of ~ 35% - 57% enhancement is realized via surprisingly small fields (, to appear in Nature

MoTe_2, with the orthorhombic T_d phase, is a new type (type-II) of Weyl semimetal, where the Weyl Fermions emerge at the boundary between electron and hole pockets. Non-saturating magnetoresistance (MR), and superconductivity were also observed in T_d-MoTe_2. Understanding the superconductivity in T_d-MoTe_2, which was proposed to be topologically non-trivial, is of eminent interest. Here, we report high-pressure (p_max = 1.3 GPa) muon spin rotation experiments on the temperature-dependent magnetic penetration depth in T_d-MoTe_2. A substantial increase of the superfluid density n_s/m^* and a linear scaling with T_c is observed under pressure. Moreover, the superconducting order parameter in T_d-MoTe_2 is determined to be two gap (s+s)-wave symmetric. We also excluded time reversal symmetry breaking in the SC state with sensitive zero-field ${\mu}$SR experiments. Considering the previous report \cite{Balicas1} on the strong suppression of T_c in T_d-MoTe_2 by disorder, we suggest that s^{+-} (topological order parameter) state is more likely to be realized in MoTe_2 than the s^{++} (trivial) state. Should s^{+-} be the SC gap symmetry, the T_d-MoTe_2 is, to our knowledge, the first known example of a time reversal invariant topological (Weyl) superconductor., Comment: 15 pages and 9 figures

We report the detailed optical properties of Cd$_3$As$_2$ crystals in a wide parameter space: temperature, magnetic field, carrier concentration and crystal orientation. We investigate high-quality crystals synthesized by three different techniques. In all the studied samples, independently of how they were prepared and how they were treated before the optical experiments, our data indicate conspicuous fluctuations in the carrier density (up to 30%). These charge puddles have a characteristic scale of 100 $\mu$m, they become more pronounced at low temperatures, and possibly, they become enhanced by the presence of crystal twinning. The Drude response is characterized by very small scattering rates ($\sim 1$ meV) for as-grown samples. Mechanical treatment, such as cutting or polishing, influences the optical properties of single crystals, by increasing the Drude scattering rate and also modifying the high frequency optical response. Magneto-reflectivity and Kerr rotation are consistent with electron-like charge carriers and a spatially non-uniform carrier density., Comment: Accepted in Physical Review B

By combining bulk sensitive soft-X-ray angular-resolved photoemission spectroscopy and accurate first-principles calculations we explored the bulk electronic properties of WTe$_2$, a candidate type-II Weyl semimetal featuring a large non-saturating magnetoresistance. Despite the layered geometry suggesting a two-dimensional electronic structure, we find a three-dimensional electronic dispersion. We report an evident band dispersion in the reciprocal direction perpendicular to the layers, implying that electrons can also travel coherently when crossing from one layer to the other. The measured Fermi surface is characterized by two well-separated electron and hole pockets at either side of the $\Gamma$ point, differently from previous more surface sensitive ARPES experiments that additionally found a significant quasiparticle weight at the zone center. Moreover, we observe a significant sensitivity of the bulk electronic structure of WTe$_2$ around the Fermi level to electronic correlations and renormalizations due to self-energy effects, previously neglected in first-principles descriptions.

We report measurements on MgB2 up to ~40GPa. Increasing pressure yields a monotonous decrease of the lattice parameters and of the c/a ratio, but no structural transition down to parameters smaller than those of AlB2. The transition superconducting temperature also decreases with temperature in a sample dependent way. The results are explained by an increase of the filling of the 2D pxy bands with pressure, the Mg stoichiometry determining the starting position of the Fermi level. Our measurements indicate that these hole bands are the relevant ones for superconductivity., submitted March 9th 2001, PRB accepted

We present a model of the lattice dynamics of the rare earth titanate pyrochlores R2Ti2O7 (R=Tb, Dy, Ho), which are important materials in the study of frustrated magnetism. The phonon modes are obtained by density functional calculations, and these predictions are verified by comparison with scattering experiments. Single crystal inelastic neutron scattering is used to measure acoustic phonons along high symmetry directions for R=Tb, Ho; single crystal inelastic x-ray scattering is used to measure numerous optical modes throughout the Brillouin zone for R=Ho; and powder inelastic neutron scattering is used to estimate the phonon density of states for R=Tb, Dy, Ho. Good agreement between the calculations and all measurements is obtained, allowing confident assignment of the energies and symmetries of the phonons in these materials under ambient conditions. The knowledge of the phonon spectrum is important for understanding spin-lattice interactions, and can be expected to be transferred readily to other members of the series to guide the search for unconventional magnetic excitations., Comment: 15 pages, 11 figures

The recent discovery of extreme magnetoresistance in LaSb introduced lanthanum monopnictides as a new platform to study topological semimetals (TSMs). In this work we report the discovery of extreme magnetoresistance in LaBi, confirming lanthanum monopnictides as a promising family of TSMs. These binary compounds with the simple rock-salt structure are ideal model systems to search for the origin of extreme magnetoresistance. Through a comparative study of magnetotransport effects in LaBi and LaSb, we construct a triangular temperature-field phase diagram that illustrates how a magnetic field tunes the electronic behavior in these materials. We show that the triangular phase diagram can be generalized to other topological semimetals with different crystal structures and different chemical compositions. By comparing our experimental results to band structure calculations, we suggest that extreme magnetoresistance in LaBi and LaSb originates from a particular orbital texture on their qasi-2D Fermi surfaces. The orbital texture, driven by spin-orbit coupling, is likely to be a generic feature of various topological semimetals., Comment: 9 pages, 11 figures

Time reversal symmetry (TRS) protects the metallic surface modes of topological insulators (TIs). The transport signature of robust metallic surface modes of TIs is a plateau that arrests the exponential divergence of the insulating bulk with decreasing temperature. This universal behavior is observed in all TI candidates ranging from Bi2Te2Se to SmB6. Recently, several topological semimetals (TSMs) have been found that exhibit extreme magnetoresistance (XMR) and TI universal resistivity behavior revealed only when breaking TRS, a regime where TIs theoretically cease to exist. Among these new materials, TaAs and NbP are nominated for Weyl semimetal due to their lack of inversion symmetry, Cd3As2 is nominated for Dirac semimetal due to its linear band crossing at the Fermi level, and WTe2 is nominated for resonant compensated semimetal due to its perfect electron-hole symmetry. Here we introduce LaSb, a simple rock-salt structure material without broken inversion symmetry, without perfect linear band crossing, and without perfect electron-hole symmetry. Yet LaSb portrays all the exotic field induced behaviors of the aforementioned semimetals in an archetypal fashion. It shows (a) the universal TI resistivity with a plateau at 15 K, revealed by a magnetic field, (b) ultrahigh mobility of carriers in the plateau region, (c) quantum oscillations with a non-trivial Berry phase, and (d) XMR of about one million percent at 9 tesla rivaled only by WTe2 and NbP. Due to its dramatic simplicity, LaSb is the ideal model system to formulate a theoretical understanding of the exotic consequences of breaking TRS in TSMs., 4 figures, 25 pages including supplementary information

A long-standing issue in topological insulator research has been to find a material that provides an ideal platform for characterizing topological surface states without interference from bulk electronic states and can reliably be fabricated as bulk crystals. This material would be a bulk insulator, have a surface state Dirac point energy well isolated from the bulk valence and conduction bands, have high surface state electronic mobility, and be growable as large, high quality bulk single crystals. Here we show that this major materials obstacle in the field is overcome by crystals of lightly Sn-doped Bi1.1Sb0.9Te2S (Sn-BSTS) grown by the Vertical Bridgeman method, which we characterize here via angle-resolved photoemission spectroscopy, scanning tunneling microscopy, transport studies of the bulk and surface states, and X-ray diffraction and Raman scattering. We present this new material as a bulk topological insulator that can be reliably grown and studied in many laboratories around the world., 21 pages, 5 figures

Elucidating the nature of the large, non-saturating magnetoresistance in WTe2 is a significant step in functionalizing this phenomenon for applications. Here, Mo, Re, and Ta doped WTe2 are compared to determine whether isovalent and aliovalent substitutions have different effects on the large magnetoresistance. By 1% substitution, isoelectronic doping reduces the magnetoresistance by a factor of 1.2 with an apparent linear trend, whereas aliovalent doping reduces the effect by over an order of magnitude while following a higher-order decay. The apparent increased sensitivity of the magnetoresistive effect to aliovalent doping over simple isoelectronic disorder supports the conclusion that the large magnetoresistance in WTe2 arises from interactions between balanced hole and electron populations., Submitted to Materials Research Bulletin on May 31, 2015

High quality single crystals of WTe$_2$ were grown using a Te flux followed by a cleaning step involving self-vapor transport. The method is reproducible and yields consistently higher quality single crystals than are typically obtained via halide assisted vapor transport methods. Magnetoresistance (MR)values at 9 Tesla and 2 Kelvin as high as 1.75 million \%, nearly an order of magnitude higher than previously reported for this material, were obtained on crystals with residual resistivity ratio (RRR) of approximately 1250. The MR follows a near B$^2$ law (B = 1.95(1)) and, assuming a semiclassical model, the average carrier mobility for the highest quality crystal was found to be ~167,000 cm$^2$/Vs at 2 K. A correlation of RRR, MR ratio and average carrier mobility ($\mu_{avg}$) is found with the cooling rate during the flux growth., Comment: 7 pages, 3 figures, 1 table

NaCaNi$_2$F$_7$ is an insulating, frustrated A$_2$B$_2$F$_7$ pyrochlore with magnetic S = 1 Ni$^{2+}$ on the pyrochlore B site. Non-magnetic Na and Ca are disordered on the A-site. Magnetic susceptibility measurements made on an oriented single crystal, grown in a floating zone furnace, show isotropic behavior at temperatures between 5 and 300 K, with an effective moment of 3.7 $\mu_B$/Ni. Despite displaying a large Curie-Weiss theta (-129 K), spin-ordering-related features are not seen in the susceptibility or specific heat until a spin glass transition at 3.6 K. This yields an empirical frustration index of f = -${\theta}_{CW}$/T$_f$ $\approx$ 36. The spin glass behavior is substantiated by a shift of the freezing temperature with frequency in the AC susceptibility, bifurcation in the DC susceptibility, and by a broad maximum in the magnetic specific heat. The observations as made on large single crystals suggest that NaCaNi$_2$F$_7$ is likely a realization of a frustrated spin 1 pyrochlore antiferromagnet with weak bond disorder., Comment: 15 Pages, 5 Figures, 2 Tables

The Ho2Ti2O7, Er2Ti2O7 and Yb2Ti2O7 pyrochlores were studied by synchrotron X-ray diffraction to determine whether the (002) peak, forbidden in the pyrochlore space group Fd-3m but observed in single crystal neutron scattering measurements, is present due to a deviation of their pyrochlore structure from Fd-3m symmetry. Synchrotron diffraction measurements on precisely synthesized stoichiometric and non-stoichiometric powders and a crushed floating zone crystal of Ho2Ti2O7 revealed that the (002) reflection is absent in all cases to a sensitivity of approximately one part in 30,000 of the strongest X-ray diffraction peak. This indicates to high sensitivity that the structural space group of these rare earth titanate pyrochlores is Fd-3m, and that thus the (002) peak observed in the neutron scattering experiments has a non-structural origin. The cell parameters and internal strain for lightly stuffed Ho2+xTi2-xO7 are also presented., 23 pages, 8 figures

We report the crystal growth, crystal structure and basic magnetic properties of a new cobalt-based pyrochlore, NaSrCo$_2$F$_7$. Na and Sr are completely disordered on the non-magnetic large atom A sites, while magnetic S=3/2 Co$^{2+}$ fully occupies the pyrochlore lattice B sites. This system exhibits an isotropic magnetic susceptibility with strong antiferromagnetic interactions (${\theta}_{CW}$ = -127(1)), a large effective moment (${\rho_{eff}}$ = 5.9(1) ${\mu_B}$/Co) and no spin freezing until 3 K. Thus NaSrCo$_2$F$_7$ is a geometrically frustrated antiferromagnet with a frustration index f = -${\theta_{CW}}$/T$_f$ = 42. AC susceptibility, DC susceptibility, and heat capacity are utilized to characterize the spin freezing at low temperatures. We propose that NaSrCo$_2$F$_7$, compared here to the related material NaCaCo$_2$F$_7$, may be the realization of a frustrated pyrochlore antiferromagnet with weak bond disorder. The strong magnetic frustration at an easily accessible temperature and the availability of large single crystals make this one of the potentially interesting alternatives to the more commonly studied rare earth oxide pyrochlores., Comment: 14 pages, 5 figures, 2 tables

Recent experimental results have emphasized two aspects of Tb2Ti2O7 which have not been taken into account in previous attempts to construct theories of Tb2Ti2O7: the role of small levels of structural disorder, which appears to control the formation of a long-range ordered state of as yet unknown nature; and the importance of strong coupling between spin and lattice degrees of freedom, which results in the hybridization of crystal field excitons and transverse acoustic phonons. In this work we examine the juncture of these two phenomena and show that samples with strongly contrasting behavior vis-a-vis the structural disorder (i.e. with and without the transition to the ordered state), develop identical magnetoelastic coupling. We also show that the comparison between single crystal and powder samples is more complicated than previously thought - the correlation between lattice parameter (as a measure of superstoichiometric Tb$^{3+}$) and the existence of a specific heat peak, as observed in powder samples, does not hold for single crystals., Comment: 8 pages, 4 figures; resubmitted version

We report a reinvestigation of superconducting Sn$_{1-x}$In$_{x}$Te at both low and high In doping levels. Analysis of the superconductivity reveals a fundamental change as a function of \textit{x}: the system evolves from a weakly coupled to a strongly coupled superconductor with increasing indium content. Hall Effect measurements further show that the carrier density does not vary linearly with Indium content; indeed at high Indium content, the samples are overall \textit{n}-type, which is contrary to expectations of the standard picture of In$^{1+}$ replacing Sn$^{2+}$ in this material. Density functional theory calculations probing the electronic state of In in SnTe show that it does not act as a trivial hole dopant, but instead forms a distinct, partly filled In 5\textit{s} - Te 5\textit{p} hybridized state centered around E$_F$, very different from what is seen for other nominal hole dopants such as Na, Ag, and vacant Sn sites. We conclude that superconducting In-doped SnTe therefore cannot be considered as a simple hole doped semiconductor., Comment: 12 pages and 7 figures

We employ the chemical fragment formalism to perform a targeted superconductor search in the Nb-Ru-B system, yielding the orthorhombic metal-rich boride NbRuB, which displays BCS-like superconductivity with a Tc = 3.1 K. NbRuB is derived from the chemical fragments Nb3B2 + Ru3B, in which the Nb3B2 fragment contains B-B dimers and the Ru3B fragment contains isolated B atoms. A charge transfer occurs between the fragments. The results indicate that the fragment formalism is a useful chemical tool for the design of new intermetallic superconductors much the same way as the charge reservoir concept has been a useful chemical tool for the design of new copper oxide superconductors.

Electrons incident from a normal metal onto a superconductor are reflected back as holes - a process called Andreev reflection. In a normal metal where the Fermi energy is much larger than a typical superconducting gap, the reflected hole retraces the path taken by the incident electron. In graphene with ultra low disorder, however, the Fermi energy can be tuned to be smaller than the superconducting gap. In this unusual limit, the holes are expected to be reflected specularly at the superconductor-graphene interface due to the onset of interband Andreev processes, where the effective mass of the reflected holes change sign. Here we present measurements of gate modulated Andreev reflections across the low disorder van der Waals interface formed between graphene and the superconducting NbSe2. We find that the conductance across the graphene-superconductor interface exhibits a characteristic suppression when the Fermi energy is tuned to values smaller than the superconducting gap, a hallmark for the transition between intraband retro- and interband specular- Andreev reflections.

Magnetoresistance is the change of a material's electrical resistance in response to an applied magnetic field. In addition to its intrinsic scientific interest, it is a technologically important property, placing it in "Pasteur's quadrant" of research value: materials with large magnetorsistance have found use as magnetic sensors 1, in magnetic memory 2, hard drives 3, transistors 4, and are the subject of frequent study in the field of spintronics 5, 6. Here we report the observation of an extremely large one-dimensional positive magnetoresistance (XMR) in the layered transition metal dichalcogenide (TMD) WTe2; 452,700 percent at 4.5 Kelvin in a magnetic field of 14.7 Tesla, and 2.5 million percent at 0.4 Kelvin in 45 Tesla, with no saturation. The XMR is highly anisotropic, maximized in the crystallographic direction where small pockets of holes and electrons are found in the electronic structure. The determination of the origin of this effect and the fabrication of nanostructures and devices based on the XMR of WTe2 will represent a significant new direction in the study and uses of magnetoresistivity. *The published version of the paper includes co-authors Tian Liang and Max Hirschberger. **This paper has been published with new MR data to 60T where the MR of WTe2 reaches 13 million percent (at 0.5K) and still shows no signs of saturation. We also have new electron diffraction patterns to lower temperature (10K). We discuss the possible origin of the MR as coming from an electron-hole 'resonance' condition established by a perfect n/p ratio of 1 (more details in a new "extended data" section). This makes WTe2, possibly, the first realization of a perfectly balanced semimetal. ***The paper is published as "Large non-saturating magnetoresistance in WTe2" in Nature (2014), DOI:10.1038/nature13763, Nature, 2014

We report the magnetic characterization of the frustrated transition metal pyrochlore NaCaCo$_2$F$_7$. This material has high spin Co$^{2+}$ in CoF$_6$ octahedra in a pyrochlore lattice, and disordered non-magnetic Na and Ca on the large-atom sites in the structure. Large crystals grown by the floating zone method were studied. The magnetic susceptibility is isotropic, the Co moment is larger than the spin-only value, and in spite of the large Curie Weiss theta (-140 K), freezing of the spin system, as characterized by peaks in the ac and dc susceptibility and specific heat, does not occur until around 2.4 K. This yields a frustration index of f = $-\theta_{CW}$/$T_f$ $\approx$ 56, an indication that the system is highly frustrated. The observed entropy loss at the freezing transition is low, indicating that magnetic entropy remains present in the system at 0.6 K. The compound may be the realization of a frustrated pyrochlore antiferromagnet with weak bond disorder. The high magnetic interaction strength, strong frustration, and the availability of large single crystals makes NaCaCo$_2$F$_7$ an interesting alternative to rare earth oxide pyrochlores for the study of geometric magnetic frustration in pyrochlore lattices., Comment: Submitted to PRL; 14 pages, 4 figures, 2 tables

The electronic structure basis of the extremely large magnetoresistance in layered non-magnetic tungsten ditelluride has been investigated by angle-resolved photoelectron spectroscopy. Hole and electron pockets of approximately the same size were found at the Fermi level, suggesting that carrier compensation should be considered the primary source of the effect. The material exhibits a highly anisotropic, quasi one-dimensional Fermi surface from which the pronounced anisotropy of the magnetoresistance follows. A change in the Fermi surface with temperature was found and a high-density-of-states band that may take over conduction at higher temperatures and cause the observed turn-on behavior of the magnetoresistance in WTe$_2$ was identified.

Ca10(Pt3As8)(Fe2As2)5 is the parent compound for a class of Fe-based high-temperature superconductors where superconductivity with transition temperatures up to 30 K can be introduced by partial element substitution. We present a combined high-resolution high-energy x-ray diffraction and elastic neutron scattering study on a Ca10(Pt3As8)(Fe2As2)5 single crystal. This study reveals the microscopic nature of two distinct and continuous phase transitions to be very similar to other Fe-based high-temperature superconductors: an orthorhombic distortion of the high-temperature tetragonal Fe-As lattice below T_S = 110(2) K followed by stripe-like antiferromagnetic ordering of the Fe moments below T_N = 96(2) K. These findings demonstrate that major features of the Fe-based high-temperature superconductors are very robust against variations in chemical constitution as well as structural imperfection of the layers separating the Fe-As layers from each other and confirms that the Fe-As layers primarily determine the physics in this class of material., Comment: 5 pages, 2 figures

In this letter, we report on an analytical technique for optical investigations of semitransparent samples. By Fourier transforming optical spectra with Fabry-Perot resonances we extract information about sample thickness and its discrete variations. Moreover, this information is used to recover optical spectra devoid of Fabry-Perot fringes, which simplifies optical modelling, and can reveal previously concealed spectral features. To illustrate its use, we apply our technique to a Si wafer as well as six different cleavable layered materials, including topological insulators, thermoelectrics, and magnetic insulators. In the layered materials, we find strong evidence of large step edges and thickness inhomogeneity, and cannot conclusively exclude the presence of voids in the bulk of cleaved samples. This could strongly affect the interpretation of transport and optical data of crystals with topologically protected surfaces states., Comment: 6 pages, 3 figures

Pb$_{0.77}$Sn$_{0.23}$Se is a novel alloy of two promising thermoelectric materials PbSe and SnSe that exhibits a temperature dependent band inversion below 300 K. Recent work has shown that this band inversion also coincides with a trivial to nontrivial topological phase transition. To understand how the properties critical to thermoelectric efficiency are affected by the band inversion, we measured the broadband optical response of Pb$_{0.77}$Sn$_{0.23}$Se as a function of temperature. We find clear optical evidence of the band inversion at $160\pm15$ K, and use the extended Drude model to accurately determine a $T^{3/2}$ dependence of the bulk carrier lifetime, associated with electron-acoustic phonon scattering. Due to the high bulk carrier doping level, no discriminating signatures of the topological surface states are found, although their presence cannot be excluded from our data., Comment: 11 pages, 6 figures

We report that Sb2Te, a natural superlattice phase consisting of two elemental Sb2 layers interleaved with single Sb2Te3 layers, becomes ferromagnetic at low temperatures on doping with small percentages of Mn. Ferromagnetism appears for Mn concentrations as low as Sb1.98Mn0.02Te, where a ferromagnetic Tc of ~ 8.6 K is observed. Tc decreases with increasing Mn content in the stoichiometric materials but increases with increasing Te excess in materials of the type Sb1.93-yMn0.07Te1+y, starting at ~ 3 K at y = 0 and reaching a Tc of ~ 8.9 K at y = 0.06.

Using circular dichroism-angle resolved photoemission spectroscopy (CD-ARPES), we report a study of the effect of angular momentum transfer between polarized photons and topological surface states on the surface of highly bulk insulating topological insulator Bi2Te2Se. The photoelectron dichroism is found to be strongly modulated by the frequency of the helical photons including a dramatic sign-flip. Our results suggest that the observed dichroism and its sign-flip are consequences of strong coupling between the photon field and the spin-orbit nature of the Dirac modes on the surface. Our studies reveal the intrinsic dichroic behavior of topological surface states and point toward the potential utility of bulk insulating topological insulators in device applications., 5 pages, 4 figures

We describe the topological surface states of Bi$_4$Se$_3$, a compound in the infinitely adaptive Bi$_2$-Bi$_2$Se$_3$ natural superlattice phase series, determined by a combination of experimental and theoretical methods. Two observable cleavage surfaces, terminating at Bi or Se, are characterized by angle resolved photoelectron spectroscopy and scanning tunneling microscopy, and modeled by ab-initio density functional theory calculations. Topological surface states are observed on both surfaces, but with markedly different dispersions and Kramers point energies. Bi$_4$Se$_3$ therefore represents the only known compound with different topological states on differently terminated surfaces., 5 figures references added Published in PRB: http://link.aps.org/doi/10.1103/PhysRevB.88.081108

The synthesis, structure, and elementary magnetic and electronic properties are reported for layered compounds of the type Na3-xMIr2O6 and Na3-xM2IrO6, where M is a transition metal from the 3d series (M=Zn, Cu, Ni, Co, Fe and Mn). The rhombohedral structures, in space group R-3m, were determined by refinement of neutron and synchrotron powder diffraction data. No clear evidence for long range 2:1 or 1:2 honeycomb-like M/Ir ordering was found in the neutron powder diffraction patterns except in the case of M = Zn, thus in general the compounds are best designated as sodium deficient ��-NaFeO2-type phases with formulas Na1-xM1/3Ir2/3O2 or Na1-xM2/3Ir1/3O2. Synchrotron powder diffraction patterns indicate that several of the compounds likely have honeycomb in-plane metal-iridium ordering with disordered stacking of the layers. All the compounds are sodium deficient under our synthetic conditions and are black and insulating. Weiss constants derived from magnetic susceptibility measurements indicate that Na0.62Mn0.61Ir0.39O2, Na0.80Fe2/3Ir1/3O2, Na0.92Ni1/3Ir2/3O2, Na0.86Cu1/3Ir2/3O2, and Na0.89Zn1/3Ir2/3O2 display dominant antiferromagnetic interactions. For Na0.90Co1/3Ir2/3O2 the dominant magnetic interactions at low temperature are ferromagnetic while at high temperatures they are antiferromagnetic; there is also a change in the effective moment. Low temperature specific heat measurements (to 2 K) on Na0.92Ni1/3Ir2/3O2 indicate the presence of a broad magnetic ordering transition. X-ray absorption spectroscopy shows that iridium is at or close to the 4+ oxidation state in all compounds. 23Na nuclear magnetic resonance measurements comparing Na2IrO3 to Na0.92Ni1/3Ir2/3O2 and Na0.89Zn1/3Ir2/3O2 provide strong indications that the electron spins are short-range ordered in the latter two materials. All of the compounds are spin glasses., Journal of Solid State Chemistry to be published, 43 pages, 16 figures

This is a revised version of a manuscript that was originally posted here in February of 2014. It has been accepted at the journal Inorganic Chemistry after reviews that included those of two crystallographers who made sure all the t's were crossed and the i's were dotted. The old work (from 1968) that said that Cd3As2 was noncentrosymmetric was mistaken, with the authors of that study making a type of error that in the 1980s became infamous in crystallography. As a result of the increased scrutiny of the issue of centrosymmetricity of the 1980's, there are now much better analysis tools to resolve the issue fully, and its important to understand that not just our crystals are centrosymmetric, even the old guy's crystals were centrosymmetric (and by implication everyone's are). There is no shame in having made that error back in the day and those authors would not find the current centrosymmetric result controversial; their paper is excellent in all other aspects. This manuscript describes how the structure is determined, explains the structure schematically, calculates the electronic structure based on the correct centrosymmetric crystal structure, and gives the structural details that should be used for future analysis and modeling., Accepted by ACS Inorganic Chemistry

We have probed the low temperature magnetic behavior of the ordered spin ice material Tb2Sn2O7 through ac magnetic susceptibility measurements of both the pure material and samples with small percentages of Ti substituted on the Sn sublattice. We observe a clear signature for the previously reported ordering transition at TC = 850 mK, as well as evidence for dynamic freezing at temperatures well below TC, confirming the persistence of significant magnetic fluctuations deep in the spin-ordered regime. The long range ordering transition was completely suppressed with as little as 5% Ti for Sn substitution, and 10% Ti substitution resulted in a spin-glass-like spin freezing transition near 250 mK. The results demonstrate that the long range magnetic ordering is surprisingly fragile in this system.

We perform systematic angle-resolved photoemission spectroscopic measurements on the lead tin telluride Pb1-xSnxTe pseudobinary alloy system. We show that the (001) crystalline surface, which is a crystalline surface symmetric about the (110) mirror planes of the Pb1-xSnxTe crystal, pos- sesses four metallic surface states within its surface Brillouin zone. Our systematic Fermi surface and band topology measurements show that the observed Dirac-like surface states lie on the symmetric momentum-space cuts. We further show that upon going to higher electron binding energies, the surface states' isoenergetic countours in close vicinity of each X point are observed to hybridize with each other, leading to a Fermi surface fractionalization and the Lifshitz transition. In addition, systematic incident photon energy dependent measurements are performed, which enable us to un- ambiguously identify the surface states from the bulk bands. These systematic measurements of the surface and bulk electronic structure on Pb1-xSnxTe, supported by our first principles calculation results, for the first time, show that the Pb1-xSnxTe system belongs to the topological crystalline insulator phase due to the four band inversions at the L points in its Brillouin zone, which has been recently theoretically predicted., 4 pages, 4 Figures, Submitted May '12

It is predicted that electrons on the surface of a topological insulator can acquire a mass (massive Dirac fermion) by opening up a gap at the Dirac point when time-reversal symmetry is broken via the out-of-plane magnetization. We report photoemission studies on a series of topological insulator materials focusing on the spectral behavior in the vicinity of the Dirac node. Our results show that the spectral intensity is suppressed resulting in a "gap"-like feature in materials with or without any magnetic impurity or doping. The Zeeman gap in magnetically doped samples, expected to be rather small, is likely masked by the non-magnetic strong spectral weight suppression involving a large energy scale we report. The photoemission spectral weight suppression observed around the Dirac node thus cannot be taken as the sole evidence for a time-reversal symmetry breaking magnetic gap. We discuss a few possible extrinsic and kinematic origins of the Dirac point spectral weight suppression ("gap") observed in many commonly studied topological materials., 10 pages, 3 Figures

We describe the crystal growth, crystal structure, and basic electrical properties of Bi2Te1.6S1.4, which incorporates both S and Te in its Tetradymite quintuple layers in the motif -[Te0.8S0.2]-Bi-S-Bi-[Te0.8S0.2]-. This material differs from other Tetradymites studied as topological insulators due to the increased ionic character that arises from its significant S content. Bi2Te1.6S1.4 forms high quality crystals from the melt and is the S-rich limit of the ternary Bi-Te-S {\gamma}-Tetradymite phase at the melting point. The native material is n-type with a low resistivity; Sb substitution, with adjustment of the Te to S ratio, results in a crossover to p-type and resistive behavior at low temperatures. Angle resolved photoemission study shows that topological surface states are present, with the Dirac point more exposed than it is in Bi2Te3 and similar to that seen in Bi2Te2Se. Single crystal structure determination indicates that the S in the outer chalcogen layers is closer to the Bi than the Te, and therefore that the layers supporting the surface states are corrugated on the atomic scale., Comment: To be published in Physical Review B Rapid Communications 16 douuble spaced pages. 4 figures 1 table

We report spin- and angle-resolved photoemission studies of a topological insulator from the infinitely adaptive series between elemental Bi and Bi$_2$Se$_3$. The compound, based on Bi$_4$Se$_3$, is a 1:1 natural superlattice of alternating Bi$_2$ layers and Bi$_2$Se$_3$ layers; the inclusion of S allows the growth of large crystals, with the formula Bi$_4$Se$_{2.6}$S$_{0.4}$. The crystals cleave along the interfaces between the Bi$_2$ and Bi$_2$Se$_3$ layers, with the surfaces obtained having alternating Bi or Se termination. The resulting terraces, observed by photoemission electron microscopy, create avenues suitable for the study of one-dimensional topological physics. The electronic structure, determined by spin- and angle- resolved photoemission spectroscopy, shows the existence of a surface state that forms a large, hexagonally shaped Fermi surface around the $\Gamma$ point of the surface Brillouin zone, with the spin structure indicating that this material is a topological insulator., Comment: published version, 5 pages, 4 figures

We report extensive measurements on a new compound (Yb0.24Sn0.76)Ru that crystallizes in the cubic CsCl structure. Valence band photoemission and L3 x-ray absorption show no divalent component in the 4f configuration of Yb. Inelastic neutron scattering (INS) indicates that the eight-fold degenerate J-multiplet of Yb3+ is split by the crystalline electric field (CEF) into a {\Gamma}7 doublet ground state and a {\Gamma}8 quartet at an excitation energy 20 meV. The magnetic susceptibility can be fit very well by this CEF scheme under the assumption that a {\Gamma}6 excited state resides at 32 meV; however, the {\Gamma}8/{\Gamma}6 transition expected at 12 meV was not observed in the INS. The resistivity follows a Bloch- Gr\"uneisen law shunted by a parallel resistor, as is typical of systems subject to phonon scattering with no apparent magnetic scattering. All of these properties can be understood as representing simple local moment behavior of the trivalent Yb ion. At 1 K, there is a peak in specific heat that is too broad to represent a magnetic phase transition, consistent with absence of magnetic reflections in neutron diffraction. On the other hand, this peak also is too narrow to represent the Kondo effect in the {\Gamma}7 ground state doublet. On the basis of the field-dependence of the specific heat, we argue that antiferromagnetic shortrange order (possibly co-existing with Kondo physics) occurs at low temperatures. The long-range magnetic order is suppressed because the Yb site occupancy is below the percolation threshold for this disordered compound.

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

We report that small amounts of metal atom non-stoichiometry are possible in the ZnCr2O4 and MgCr2O4 spinels. The non-stoichiometry, though less than 2%, significantly impacts TN and the nature of the magnetic correlations above TN. The Zn1+xCr2-xO4 spinel is particularly sensitive. While stoichiometric ZnCr2O4 displays antiferromagnetic short range correlations in the susceptibility above TN, ferromagnetic correlations are observed in non-stoichiometric, hole doped Zn1+xCr2-xO4. The Mg1+xCr2-xO4 spinels are less profoundly affected by non-stoichiometry, though significant changes are also observed. We contrast the magnetic properties of Zn1+xCr2-xO4 and Mg1+xCr2-xO4 (x=0, 0.02, 0.04) with those of materials with the equivalent amounts of isovalent non-magnetic Ga3+ substituted on the Cr3+ site to separate the effects of static site disorder and hole doping., Comment: 21 pages, 7 figures, To be published in Physical Review B

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.

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., 3 Figures, 18 pages, Submitted to NATURE PHYSICS in December 2008

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., 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

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., v2: STM characterization of n and p type Bi2Se3 is added