arXiv subjects

Robert J. Cava

Publications and source records attributed to Robert J. Cava.

At least 145 records · Page 8Linked to original sources

arXiv2015

Zr$_5$Sb$_3$$_-$$_x$Ru$_x$, a new superconductor in the W$_5$Si$_3$ structure type

We report that at low Ru contents, up to x = 0.2, the Zr$_5$Sb$_3$$_-$$_x$Ru$_x$ solid solution forms in the hexagonal Mn$_5$Si$_3$ structure type of the host (x = 0), but that at higher Ru contents (x = 0.4 - 0.6) the solid solution transforms into the tetragonal W$_5$Si$_3$ structure type. We find that tetragonal Zr$_5$Sb$_2$$_.$$_4$Ru$_0$$_.$$_6$ is superconducting at 5 K, significantly higher than the transition temperature of hexagonal Zr$_5$Sb$_3$ (x = 0), which has a T$_c$ of 2.3 K. In support of a hypothesis that certain structure types are favorable for superconductivity, we describe how the W$_5$Si$_3$ and Tl$_5$Te$_3$ structure types, both of which support superconductivity, are derived from the parent Al$_2$Cu type structure, in which superconductors are also found. Electronic structure calculations show that in Zr$_1$$_0$Sb$_5$Ru, a model for the new superconducting compound, the Fermi level is located on a peak in the electronic density of states.

cond-mat.supr-con↗

arXiv2015

Breakdown of Three-dimensional Dirac Semimetal State in pressurized Cd3As2

We report the first observation of a pressure-induced breakdown of the 3D-DSM state in Cd3As2, evidenced by a series of in-situ high-pressure synchrotron X-ray diffraction (XRD) and single crystal transport measurements. We find that Cd3As2 undergoes a structural phase transition from a metallic tetragonal (T) phase in space group I41/acd to a semiconducting monoclinic (M) phase in space group P21/c at critical pressure 2.57 GPa, above this pressure, an activation energy gap appears, accompanied by distinct switches in Hall resistivity slope and electron mobility. These changes of crystal symmetry and corresponding transport properties manifest the breakdown of the 3D-DSM state in pressurized Cd3As2.

cond-mat.supr-con↗

arXiv2015

Potential ring of Dirac nodes in a new polymorph of Ca$_3$P$_2$

We report the crystal structure of a new polymorph of Ca$_3$P$_2$, and an analysis of its electronic structure. The crystal structure was determined through Rietveld refinements of powder synchrotron x-ray diffraction data. Ca$_3$P$_2$ is found to be a variant of the Mn$_5$Si$_3$ structure type, with a Ca ion deficiency compared to the ideal 5:3 stoichiometry to yield a charge-balanced compound. We also report the observation of a secondary phase, Ca$_5$P$_3$H, in which the Ca and P sites are fully occupied and the presence of interstitial hydride ions creates a closed-shell electron-precise compound. We show via electronic structure calculations of Ca$_3$P$_2$ that the compound is stabilized by a gap in the density of states compared to the hypothetical compound Ca$_5$P$_3$. Moreover, the calculated band structure of Ca$_3$P$_2$ indicates that it should be a three-dimensional Dirac semimetal with a highly unusual ring of Dirac nodes at the Fermi level. The Dirac states are protected against gap opening by a mirror plane in a manner analogous to graphene. The results suggest that further study of the electronic properties of Ca$_3$P$_2$ will be of interest.

cond-mat.mtrl-sci↗

arXiv2015

Unconventional transformation of spin Dirac phase across a topological quantum phase transition

The topology of a topological material can be encoded in its surface states. These surface states can only be removed by a bulk topological quantum phase transition into a trivial phase. Here we use photoemission spectroscopy to image the formation of protected surface states in a topological insulator as we chemically tune the system through a topological transition. Surprisingly, we discover an exotic spin-momentum locked, gapped surface state in the trivial phase that shares many important properties with the actual topological surface state in anticipation of the change of topology. Using a spin-resolved measurement, we show that apart from a surface band-gap these states develop spin textures similar to the topological surface states well-before the transition. Our results offer a general paradigm for understanding how surface states in topological phases arise and are suggestive for future realizing Weyl arcs, condensed matter supersymmetry and other fascinating phenomena in the vicinity of topological quantum criticality.

cond-mat.mes-hall↗

arXiv2015

Gold-Gold Bonding: The Key to Stabilizing the 19-Electron Ternary Phases LnAuSb (Ln = La-Nd and Sm) as New Dirac Semimetals

We report a new family of ternary 111 hexagonal LnAuSb (Ln = La-Nd, Sm) compounds that, with a 19 valence electron count, has one extra electron compared to all other known LnAuZ compound. The "19th" electron is accommodated by Au-Au bonding between the layers; this Au-Au interaction drives the phases to crystallize in the YPtAs-type structure rather than the more common LiGaGe-type. This is critical, as the YPtAs structure type has the symmetry-allowed band crossing necessary for the formation of Dirac semimetals. Band structure, density of stats, and crystal orbital calculations confirm this picture, which results in a nearly complete band gap between full and empty electronic states and stable compounds; we can thus present a structural stability phase diagram for the LnAuZ (Ln = Ge, As, Sn, Sb, Pb, Bi) family of phases. Those calculations also show that LaAuSb has a bulk Dirac cone below the Fermi level. The YPtAs-type LnAuSb family reported here is an example of the uniqueness of gold chemistry applied to a rigidly closed shell system in an unconventional way.

cond-mat.str-el↗

arXiv2015

Observation of Fermi Arc Surface States in a Topological Metal: A New Type of 2D Electron Gas beyond Z2 Topological Insulators

In a topological insulator, it is the electrons on the surface or edge that carry the signature of topology. Recently, a novel topological state has been proposed in metals or semimetals (gapless) whose band-structure is similar to that of a three-dimensional analog of graphene. However, to this date the signature of its topology remains an open question. We report the experimental discovery of a pair of polarized Fermi arc surface state modes in the form of a new type of two-dimensional polarized electron gas on the surfaces of Dirac semimetals. These Fermi arc surface states (FASS) are observed to connect across an even number of bulk band gapless nodes and found to have their spin uniquely locked to their momentum. We show that these states are distinctly different from the topological surface states (TSS) seen in all known topological insulators. Our observed exotic two-dimensional states not only uncover the novel topology of gapless Dirac metals (such as sodium tribismuth Na$_3$Bi) but also opens new research frontiers for the utilization of topological Fermi arc electron gases for a wide range of fundamental physics and spintronic studies.

cond-mat.mes-hall↗

arXiv2015

A large new family of filled skutterudites stabilized by electron count

Based on the interplay of theory and experiment, a large new family of filled group 9 (Co, Rh and Ir) skutterudites is designed and synthesized. The new materials fill the empty cages in the structures of the known binary CoSb3, RhSb3 and IrSb3 skutterudites with alkaline, alkaline earth, and rare earth atoms to create compounds of the type AyB4X12; A atoms fill the cages to a fraction y, B are the group 9 transition metals, and X is a mixture of electronegative main group elements chosen to achieve chemical stability by adjusting the electron counts to electron-precise values. Forty-three new compounds are reported, antimony-tin and phosphorous-silicon based, with 63 compositional variations presented. The new family of compounds is large and general. The results described here can be extended to the synthesis of hundreds of new group 9 filled skutterudites.

cond-mat.mtrl-sci↗

arXiv2015

Raman study of magnetic excitations and magneto-elastic coupling in alpha-SrCr2O4

Using Raman spectroscopy, we investigate the lattice phonons, magnetic excitations, and magneto-elastic coupling in the distorted triangular-lattice Heisenberg antiferromagnet alpha-SrCr2O4, which develops helical magnetic order below 43 K. Temperature dependent phonon spectra are compared to predictions from density functional theory calculations which allows us to assign the observed modes and identify weak effects arising from coupled lattice and magnetic degrees of freedom. Raman scattering associated with two-magnon excitations is observed at 20 meV and 40 meV. These energies are in general agreement with our ab-initio calculations of exchange interactions and earlier theoretical predictions of the two-magnon Raman response of triangular-lattice antiferromagnets. The temperature dependence of the two-magnon excitations indicates that spin correlations persist well above the Néel temperature.

cond-mat.str-el↗

arXiv2014

Evidence for a New Excitation at the Interface Between a High-Tc Superconductor and a Topological Insulator

High-temperature superconductors exhibit a wide variety of novel excitations. If contacted with a topological insulator, the lifting of spin rotation symmetry in the surface states can lead to the emergence of unconventional superconductivity and novel particles. In pursuit of this possibility, we fabricated high critical-temperature (Tc ~ 85 K) superconductor/topological insulator (Bi2Sr2CaCu2O8+delta/Bi2Te2Se) junctions. Below 75 K, a zero-bias conductance peak (ZBCP) emerges in the differential conductance spectra of this junction. The magnitude of the ZBCP is suppressed at the same rate for magnetic fields applied parallel or perpendicular to the junction. Furthermore, it can still be observed and does not split up to at least 8.5 T. The temperature and magnetic field dependence of the excitation we observe appears to fall outside the known paradigms for a ZBCP.

cond-mat.supr-con↗

arXiv2014

Intrinsic disorder in graphene on transition metal dichalcogenide heterostructures

The electronic properties of two-dimensional materials such as graphene are extremely sensitive to their environment, especially the underlying substrate. Planar van der Waals bonded substrates such as hexagonal boron nitride (hBN) have been shown to greatly improve the electrical performance of graphene devices by reducing topographic variations and charge fluctuations compared to amorphous insulating substrates}. Semiconducting transition metal dichalchogenides (TMDs) are another family of van der Waals bonded materials that have recently received interest as alternative substrates to hBN for graphene as well as for components in novel graphene-based device heterostructures. Additionally, their semiconducting nature permits dynamic gate voltage control over the interaction strength with graphene. Through local scanning probe measurements we find that crystalline defects intrinsic to TMDs induce scattering in graphene which results in significant degradation of the heterostructure quality, particularly compared to similar graphene on hBN devices.

cond-mat.mtrl-sci↗

arXiv2014

3D Dirac semimetals: current materials, design principles and predictions of new materials

Design principles and novel predictions of new 3D Dirac semimetals are presented, along with the context of currently known materials. Current materials include those based on a topological to trivial phase transition, such as in TlBiSe$_{2-x}$S$_x$ and Hg$_{1-x}$Cd$_x$Te, Bi$_{1-x}$Sb$_x$, Bi$_{2-x}$In$_x$Se$_3$, and Pb$_{1-x}$Sn$_x$Se. Some more recently revealed materials, Na$_3$Bi and Cd$_3$As$_2$, are 3D Dirac semimetals in their native composition. The different design principles presented each yield novel predictions for new candidates. For Case I, 3D Dirac semimetals based on charge balanced compounds, BaAgBi, SrAgBi, YbAuSb, PtBi$_2$ and SrSn$_2$As$_2$ are identified as candidates. For Case II, 3D Dirac semi-metals in analogy to graphene, BaGa$_2$ is identified as a candidate, and BaPt and Li$_2$Pt are discussed. For Case III, 3D Dirac semi-metals based on glide planes and screw axes, TlMo$_3$Te$_3$ and the AMo$_3$X$_3$ family in general (A=K, Na, In, Tl, X=Se,Te) as well as the Group IVb trihalides such as HfI$_3$ are identified as candidates. Finally we discuss conventional intermetallic compounds with Dirac cones, and identify Cr$_2$B as a potentially interesting material.

cond-mat.mtrl-sci↗

arXiv2014

Observation of Distinct Bulk and Surface Chemical Environments in a Topological Insulator under Magnetic doping

The influence of magnetic dopants on the electronic and chemical environments in topological insulators (TIs) is a key factor when considering possible spintronic applications based on topological surface state properties. Here we provide spectroscopic evidence for the presence of distinct chemical and electronic behavior for surface and bulk magnetic doping of Bi2Te3. The inclusion of Mn in the bulk of Bi2Te3 induces a genuine dilute ferromagnetic state, with reduction of the bulk band gap as the Mn content is increased. Deposition of Fe on the Bi2Te3 surface, on the other hand, favors the formation of iron telluride already at coverages as low as 0.07 monolayer, as a consequence of the reactivity of the Te-rich surface. Our results identify the factors that need to be controlled in the realization of magnetic nanosystems and interfaces based on TIs.

cond-mat.mtrl-sci↗

arXiv2014

Landau Quantization and Quasiparticle Interference in the Three-Dimensional Dirac Semimetal Cd3As2

Condensed matter systems provide a rich setting to realize Dirac and Majorana fermionic excitations and the possibility to manipulate them in materials for potential applications. Recently, it has been proposed that Weyl fermions, which are chiral, massless particles, can emerge in certain bulk materials or in topological insulator multilayers and can produce unusual transport properties, such as charge pumping driven by a chiral anomaly. A pair of Weyl fermions protected by crystalline symmetry, effectively forming a massless Dirac fermion, has been predicted to appear as low energy excitations in a number of candidate materials termed three-dimensional (3D) Dirac semimetals. Here we report scanning tunneling microscopy (STM) measurements at sub-Kelvin temperatures and high magnetic fields on one promising host material, the II-V semiconductor Cd3As2. Our study provides the first atomic scale probe of Cd3As2, showing that defects mostly influence the valence band, consistent with the observation of ultra-high mobility carriers in the conduction band. By combining Landau level spectroscopy and quasiparticle interference (QPI), we distinguish a large spin-splitting of the conduction band in a magnetic field and its extended Dirac-like dispersion above the expected regime. A model band structure consistent with our experimental findings suggests that for a specific orientation of the applied magnetic field, Weyl fermions are the low-energy excitations in Cd3As2.

cond-mat.mes-hall↗

arXiv2013

The Chemical Instability of Na2IrO3 in Air

We report that Na2IrO3, which has a layered honeycomb iridium oxide sublattice interleaved by Na planes, decomposes in laboratory air while maintaining the same basic crystal structure. The decomposition reaction was monitored by time-dependent powder x-ray diffraction under different ambient atmospheres, through which it was determined that it occurs only in the simultaneous presence of both CO2 and H2O. A hydrated sodium carbonate is the primary decomposition product along with altered Na2IrO3. The diffraction signature of the altered Na2IrO3 is quite similar to that of the pristine material, which makes the detection of decomposition difficult in a sample handled under ordinary laboratory conditions. The decomposed samples show a significantly decreased magnetic susceptibility and the disappearance of the low temperature antiferromagnetic transition considered to be characteristic of the phase. Samples that have never been exposed to air after synthesis display a previously unreported magnetic transition at 5K.

cond-mat.mtrl-sci↗

arXiv2013

Separating the bulk and surface n- to p-type transition in the topological insulator GeBi(4-x)SbxTe7

We identify the multi-layered compound GeBi4Te7 to be a topological insulator with a freestanding Dirac point, slightly above the valence band maximum, using angle-resolved photoemission spectroscopy (ARPES) measurements. The spin polarization satisffies the time reversal symmetry of the surface states, visible in spin-resolved ARPES. For increasing Sb content in GeBi(4-x)SbxTe7 we observe a transition from n- to p-type in bulk sensitive Seebeck coefficient measurements at a doping of x = 0.6. In surface sensitive ARPES measurements a rigid band shift is observed with Sb doping, accompanied by a movement of the Dirac point towards the Fermi level. Between x = 0.8 and x = 1 the Fermi level crosses the band gap, changing the surface transport regime. This difference of the n- to p-type transition between the surface region and the bulk is caused by band bending effects which are also responsible for a non-coexistence of insulating phases in the bulk and in the near surface region.

cond-mat.mtrl-sci↗

arXiv2013

Experimental Realization of a Three-Dimensional Dirac Semimetal

The three dimensional (3D) Dirac semimetal, which has been predicted theoretically, is a new electronic state of matter. It can be viewed as 3D generalization of graphene, with a unique electronic structure in which conduction and valence band energies touch each other only at isolated points in momentum space (i.e. the 3D Dirac points), and thus it cannot be classified either as a metal or a semiconductor. In contrast to graphene, the Dirac points of such a semimetal are not gapped by the spin-orbit interaction and the crossing of the linear dispersions is protected by crystal symmetry. In combination with broken time-reversal or inversion symmetries, 3D Dirac points may result in a variety of topologically non-trivial phases with unique physical properties. They have, however, escaped detection in real solids so far. Here we report the direct observation of such an exotic electronic structure in cadmium arsenide (Cd3As2) by means of angle-resolved photoemission spectroscopy (ARPES). We identify two momentum regions where electronic states that strongly disperse in all directions form narrow cone-like structures, and thus prove the existence of the long sought 3D Dirac points. This electronic structure naturally explains why Cd3As2 has one of the highest known bulk electron mobilities. This realization of a 3D Dirac semimetal in Cd3As2 not only opens a direct path to a wide spectrum of applications, but also offers a robust platform for engineering topologically-nontrivial phases including Weyl semimetals and Quantum Spin Hall systems.

cond-mat.mes-hall↗

arXiv2013

Single-Crystal Growth and Thermoelectric Properties of Ge(Bi,Sb)4Te7

The thermoelectric properties between 10 and 300 K and the growth of single crystals of n-type and p-type GeBi4Te7, GeSb4Te7, and the Ge(Bi1-xSbx)4Te7 solid solution are reported. Single crystals were grown by the modified Bridgman method, and p-type behavior was achieved by the substitution of Bi by Sb in GeBi4Te7. The thermopower in the Ge(Bi1-xSbx)4Te7 solid solution ranges from -117 muVK^-1 to +160 muVK^-1. The crossover from n-type to p-type is continuous with increasing Sb content and is observed at x = 0.15. The highest thermoelectric efficiencies among the tested n-type and p-type samples are ZnT = 0.11 and ZpT = 0.20, respectively. For an optimal n-p couple in this alloy system the composite figure of merit is ZnpT = 0.17 at room temperature.

cond-mat.mtrl-sci↗

arXiv2012

Proximity-induced high-temperature superconductivity in topological insulators Bi2Se3 and Bi2Te3

Interest in the superconducting proximity effect has been reinvigorated recently by novel optoelectronic applications as well as by the possible emergence of the elusive Majorana fermion at the interface between topological insulators and superconductors. Here we produce high-temperature superconductivity in Bi2Se3 and Bi2Te3 via proximity to Bi2Sr2CaCu2O8+δ, in order to access increasing temperature and energy scales for this phenomenon. This was achieved by a new mechanical bonding technique we developed, enabling the fabrication of high-quality junctions between materials, unobtainable by conventional approaches. We observe proximity-induced superconductivity in Bi2Se3 and Bi2Te3 persisting up to at least 80K, a temperature an order of magnitude higher than any previous observations. Moreover, the induced superconducting gap in our devices reaches values of 10mV, significantly enhancing the relevant energy scales. Our results open new directions for fundamental studies in condensed matter physics and enable a wide range of applications in spintronics and quantum computing.

cond-mat.supr-con↗