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The discovery of nickelate superconductivity provided the first example of a non-copper-based material with superconductivity strongly analogous to the cuprates, but recent findings raise questions and inconsistencies around the electron counts and doping phase diagrams. We show using superconducting La$_4$Ni$_3$O$_{10}$ that there are unconventional interlayer and interorbital intrinsic doping effects that render the $d_{x^2-y^2}$ orbital occupation similar to the cuprates. The results enable a consistent framework for nickelate superconductivity, while maintaining the connection between cuprate and nickelate superconductors.

High-quality single crystals of KCo$_2$As$_2$ with the body-centered tetragonal ThCr$_2$Si$_2$ structure were grown using KAs self flux. Structural, magnetic, thermal, and electrical transport were investigated. No clear evidence for any phase transitions was found in the temperature range 2 to 300 K. The in-plane electrical resistivity $\rho$ versus temperature $T$ is highly unusual, showing a $T^4$ behavior below 30 K and an anomalous positive curvature up to 300 K which is different from the linear behavior expected from the Bloch-Gr\"uneisen theory for electron scattering by acoustic phonons. This positive curvature has been previously observed in the in-plane resistivity of high-conductivity layered delafossites such as PdCoO$_2$ and PtCoO$_2$. The in-plane $\rho(T\to0) = 0.36~\mu\Omega$ cm of KCo$_2$As$_2$ is exceptionally small for this class of compounds. The material also exhibits a nearly linear magnetoresistance at low $T$ which attains a value of about 40% at $T=2$K and magnetic field $H= 80$ kOe. The magnetic susceptibility $\chi$ of KCo$_2$As$_2$ is isotropic and about an order of magnitude smaller than the values for the related compounds SrCo$_2$As$_2$ and BaCo$_2$As$_2$. The $\chi$ increases above 100 K which is found from our first-principles calculations to arise from a sharp peak in the electronic density of states just above the Fermi energy $E_{\rm F}$. Heat capacity $C_{\rm p}(T)$ data at low $T$ yield an electronic density of states $N(E_{\rm F})$ that is about 36% larger than predicted by the first-principles theory. The $C_{\rm p}(T)$ data near room temperature suggest the presence of excited optic vibration modes which may also be the source of the positive curvature in $\rho(T)$. Our results show that KCo$_2$As$_2$ provides a new avenue for investigating the physics of high-purity metals., Comment: 13 pages, 14 figures

We investigated Sr$_3$Ru$_2$O$_7$, a quantum critical metal that shows a metamagnetic quantum phase transition and electronic nematicity, through density functional calculations. These predict a ferromagnetic ground state in contrast to the experimentally observed paramagnetism, raising the question of competing magnetic states and associated fluctuations that may suppress magnetic order. We did a search to identify such low energy antiferromagnetically ordered metastable states. We find that the lowest energy antiferromagnetic state has a striped order. This corresponds to the E-type order that has been shown to be induced by Mn alloying. We also note significant transport anisotropy in this E-type ordered state. These results are discussed in relation to experimental observations.

We report tests of various density functionals for ferromagnetic, Fe, Co and Ni with a focus on characterizing the behavior of the so-called strongly constrained and appropriately normed (SCAN) functional. It is found that SCAN is closer in behavior to functionals that yield localized behavior, such as hybrid functionals, than other semilocal functionals that are tested. The results are understood in terms of a tendency to differentiate orbitals, favoring integer occupation, which is necessary for a correct description of atomic systems, but inappropriate for the open shell metallic ferromagnetic metals studied here.

The quantum spin continuum and classical spin freezing, associated with a glassy state, represent two opposite extremes of a correlated electronic material. Here, we report the coexistence of a quantum spin continuum with a weak spin glass order in Co-doped CaRuO$_{3}$ perovskite near the chemical doping dependent metal-insulator transition boundary. Inelastic neutron measurements on Ca(Co$_{0.15}$Ru$_{0.85}$)O$_{3}$ at low temperature, $T$ = 1.5 K, reveal a continuum spectrum in the $Q-E$ space due to uncorrelated spin fluctuations. This persists across the glass transition at $T_G \simeq$23 K. Furthermore, scaling of the dynamic susceptibility yields a very small scaling coefficient $\alpha$ $\simeq$ 0.1, suggesting extreme locality of the dynamic properties. The experimental results indicate the realization of a narrow regime where the distinction between continuum dynamic behavior and glass-like regimes is reduced., Comment: 6 pages, 4 figures

We report properties of the reported transparent conductor CuI, including the effect of heavy $p$-type doping. The results, based on first principles calculations, include analysis of the electronic structure and calculations of optical and dielectric properties. We find that the origin of the favorable transparent conducting behavior lies in the absence in the visible of strong interband transitions between deeper valence bands and states at the valence band maximum that become empty with $p$-type doping. Instead, strong interband transitions to the valence band maximum are concentrated in the infrared with energies below 1.3 eV. This is contrast to the valence bands of many wide band gap materials. Turning to the mobility we find that the states at the valence band maximum are relatively dispersive. This originates from their antibonding Cu $d$ - I $p$ character. We find a modest enhancement of the Born effective charges relative to nominal values, leading to a dielectric constant $\varepsilon(0)$=6.3. This is sufficiently large to reduce ionized impurity scattering, leading to the expectation that the properties of CuI can be still can be significantly improved through sample quality.

Transition metal sulfide perovskites offer lower band gaps and greater tunability than oxides, along with other desirable properties for applications. Here we explore dimensional reduction as a tuning strategy using the Ruddlesden-Popper phases in the Ba-Zr-S system as a model. The three dimensional perovskite BaZrS$_3$ is a direct band semiconductor, with a band gap of 1.5 eV suitable for solar photovoltaic application. However, the three known members of the Ruddlesden-Popper series, are all indirect gap materials, and additionally have lower fundamental band gaps. This is accompanied in the case of by a band structure that is more favorable for carrier transport for oriented samples. The layered Ruddlesden-Popper compounds, show significantly anisotropic optical properties, as may be expected. The optical spectra show tails at low energy, which may complicate experimental characterization of these materials.

Sr$_2$RuO$_4$, an unconventional superconductor, is known to possess an incommensurate spin density wave instability driven by Fermi surface nesting. Here we report a static spin density wave ordering with a commensurate propagation vector $q_c$ = (0.25 0.25 0) in Fe-doped Sr$_2$RuO$_4$, despite the magnetic fluctuations persisting at the incommensurate wave vectors $q_{ic}$ = (0.3 0.3 L) as in the parent compound. The latter feature is corroborated by the first principles calculations, which show that Fe substitution barely changes the nesting vector of the Fermi surface. These results suggest that in addition to the known incommensurate magnetic instability, Sr$_2$RuO$_4$ is also in proximity to a commensurate magnetic tendency that can be stabilized via Fe doping., Comment: 20 pages, 4 figures, 47 references

The electronic ground state of Ca3LiOsO6 was recently considered within an intermediate coupling regime that revealed J=3/2 spin-orbit entangled magnetic moments. Through inelastic neutron scattering and density functional theory we investigate the magnetic interactions and probe how the magnetism is influenced by the change in hierarchy of interactions as we move from Ca3LiOsO6 (5d3) to Ca3LiRuO6 (4d3). An alteration of the spin-gap and ordered local moment is observed, however the magnetic structure, Neel temperature and exchange interactions are unaltered. To explain this behavior it is necessary to include both spin-orbit coupling and hybridization, indicating the importance of an intermediate coupling approach when describing 5$d$ oxides.

The pressure-induced reemergence of the second high-Tc superconducting phase (SC-II) in the alkali-metal intercalated AxFe2-ySe2 (A = K, Rb, Cs, Tl) remains an enigma and proper characterizations on the superconducting- and normal-state properties of the SC-II phase were hampered by the intrinsic inhomogeneity and phase separation. To elucidate this intriguing problem, we performed a detailed high-pressure magnetotransport study on the recently discovered (Li1-xFex)OHFe1-ySe single crystals, which have high Tc~40 K and share similar Fermi surface topology as AxFe2-ySe2, but are free from the sample complications. We found that the ambient-pressure Tc~41 K is suppressed gradually to below 2 K upon increasing pressure to Pc ~5 GPa, above which a SC-II phase with higher Tc emerges and the Tc increases progressively to above 50 K up to 12.5 GPa. Interestingly, our high-precision resistivity data enable us to uncover the sharp transition of the normal state from a Fermi liquid for SC-I phase (0 < P < 5 GPa) to a non-Fermi-liquid for SC-II phase (P > 5GPa). In addition, the reemergence of high-Tc SC-II phase is found to accompany with a concurrent enhancement of electron carrier density. Since high-pressure structural study based on the synchrotron X-ray diffraction rules out the structural transition below 10 GPa, the observed SC-II phase with enhanced carrier density should be ascribed to an electronic origin associated with a pressure-induced Fermi surface reconstruction., Comment: 14 pages, 4 figures

NaSbS2 is a semiconductor that was recently shown to have remarkable efficacy as a solar absorber indicating efficient charge collection even in defected material. We report first principles calculations of properties that show (1) an indirect gap only slightly smaller than the direct gap, which may impede recombination of photoexcited carriers, (2) highly anisotropic electronic and optical properties reflecting a layered crystal structure, (3) a pushed up valence band maximum due to repulsion from the Sb 5s states and (4) cross-gap hybridization between the S p derived valence bands and the Sb 5p states. This latter feature leads to enhanced Born effective charges that can provide local screening and therefore defect tolerance. These features are discussed in relation to the performance of the compound as a semiconductor with efficient charge collection.

The importance of electron-hole interband interactions is widely acknowledged for iron-pnictide superconductors with high transition temperatures (Tc). However, high-Tc superconductivity without hole carriers has been suggested in FeSe single-layer films and intercalated iron-selenides, raising a fundamental question whether iron pnictides and chalcogenides have different pairing mechanisms. Here, we study the properties of electronic structure in the high-Tc phase induced by pressure in bulk FeSe from magneto-transport measurements and first-principles calculations. With increasing pressure, the low-Tc superconducting phase transforms into high-Tc phase, where we find the normal-state Hall resistivity changes sign from negative to positive, demonstrating dominant hole carriers in striking contrast to other FeSe-derived high-Tc systems. Moreover, the Hall coefficient is remarkably enlarged and the magnetoresistance exhibits anomalous scaling behaviors, evidencing strongly enhanced interband spin fluctuations in the high-Tc phase. These results in FeSe highlight similarities with high-Tc phases of iron pnictides, constituting a step toward a unified understanding of iron-based superconductivity.

The pentatellurides, ZrTe5 and HfTe5 are layered compounds with one dimensional transition-metal chains that show a never understood temperature dependent transition in transport properties as well as recently discovered properties suggesting topological semimetallic behavior. Here we show that these materials are semiconductors and that the electronic transition is due to a combination of bipolar effects and different anisotropies for electrons and holes. We report magneto-transport properties for two kinds of ZrTe5 single crystals grown with the chemical vapor transport (S1) and the flux method (S2), respectively. These have distinct transport properties at zero field: the S1 displays a metallic behavior with a pronounced resistance peak and a sudden sign reversal in thermopower at approximately 130 K, consistent with previous observations of the electronic transition; in strikingly contrast, the S2 exhibits a semiconducting-like behavior at low temperatures and a positive thermopower over the whole temperature range. Refinements on the single-crystal X-ray diffraction and the energy dispersive spectroscopy analysis revealed the presence of noticeable Te-vacancies in the sample S1, confirming that the widely observed anomalous transport behaviors in pentatellurides actually take place in the Te-deficient samples. Electronic structure calculations show narrow gap semiconducting behavior, with different transport anisotropies for holes and electrons. For the degenerately doped n-type samples, our transport calculations can result in a resistivity peak and crossover in thermopower from negative to positive at temperatures close to that observed experimentally. Our present work resolves the longstanding puzzle regarding the anomalous transport behaviors of pentatellurides, and also resolves the electronic structure in favor of a semiconducting state.

The structural properties of LaCu$_{6-x}$Au$_x$ have been studied using neutron diffraction, x-ray diffraction, and heat capacity measurements. The continuous orthorhombic-monoclinic structural phase transition in LaCu$_{6}$ is suppressed linearly with Au substitution until a complete suppression of the structural phase transition occurs at the critical composition, $x_{c}$ = 0.3. Heat capacity measurements at low temperatures indicate residual structural instability at $x_c$ that extends well into the orthorhombic phase. The instability is ferroelastic in nature, with density functional theory (DFT) calculations showing negligible coupling to electronic states near the Fermi level. The data and calculations presented here are consistent with the zero temperature termination of a continuous structural phase transition suggesting that the LaCu$_{6-x}$Au$_x$ series hosts an elastic quantum critical point., Comment: 9 pages, 11 figures

The influence of spin-orbit coupling (SOC) on the physical properties of the 5d2 system Sr2MgOsO6 is probed via a combination of magnetometry, specific heat measurements, elastic and inelastic neutron scattering, and density functional theory calculations. Although a significant degree of frustration is expected, we find that Sr2MgOsO6 orders in a type I antiferromagnetic structure at the remarkably high temperature of 108 K. The measurements presented allow for the first accurate quantification of the size of the magnetic moment in a 5d2 system of 0.60(2) muB - a significantly reduced moment from the expected value for such a system. Furthermore, significant anisotropy is identified via a spin excitation gap, and we confirm by first principles calculations that SOC not only provides the magnetocrystalline anisotropy, but also plays a crucial role in determining both the ground state magnetic order and the size of the local moment in this compound. Through comparison to Sr2ScOsO6, it is demonstrated that SOC-induced anisotropy has the ability to relieve frustration in 5d2 systems relative to their 5d3 counterparts, providing an explanation of the high TN found in Sr2MgOsO6., Comment: Submitted to Scientific Reports

Calculations of the electronic and magnetic properties of the non-magnetic metallic compound YFe$_2$Si$_2$ are reported. These show that at the density functional level a magnetic state involving ordering along the $c$-axis. The electronic structure is three dimensional, and is similar to that of the unconventional superconductor YFe$_2$Ge$_2$ and as well as that of the high pressure collapsed tetragonal phase of KFe$_2$As$_2$, which is also a superconductor. Based on the results in relation to experiment, we infer that properties of YFe$_2$Si$_2$ are strongly influenced by a nearby antiferromagnetic quantum critical point.

The electronic structure, magnetic and structural properties of the superconductor ThFeAsN are discussed in relation to the Fe-pnictide and Fe-chalcogenide superconductors based on results of first principles calculations. The electronic structure is that of a high density of states semimetal. It shows approximately nested hole and electron Fermi surfaces of Fe $d$ character involving the $xz,yz$ and $xy$ orbitals. There is a strong tendency towards magnetism at the GGA level, and this magnetism is important for describing the Fe-As bonding, but greatly overestimates the magnetic ordering. The lowest energy magnetic state at the GGA level is the stripe order, and this particular order couples strongly to electrons near $E_F$. ThFeAsN is therefore strongly similar to the Fe-pnictide family of superconductors, although it is a particularly anisotropic member.

We report a density functional study of the electronic structure and magnetism of Y2Ni7. The results show itinerant magnetism very similar to that in the weak itinerant ferromagnet Ni3Al. The electropositive Y atoms in Y2Ni7 serves to donate charge to the Ni host mostly in the form of $s$ electrons. The non-spin-polarized state shows a high density of states at the Fermi level, N(EF) due to flat bands. This leads to the ferromagnetic instability. However, there are also several much more dispersive bands crossing E(F), which should promote the conductivity. Spin fluctuation effects appear to be comparable to or weaker than Ni3Al, based on comparison with experimental data. Y2Ni7 provides a uniaxial analogue to cubic Ni3Al for studying weak itinerant ferromagnetism, suggesting detailed measurements of its low temperature physical properties and spin fluctuations, as well experiments under pressure.

In a pressure-temperature (P-T) diagram for synthesizing IrTe2 compounds, the well-studied trigonal (H) phase with the CdI2-type structure is stable at low pressures. The superconducting cubic (C) phase can be synthesized under higher temperatures and pressures. A rhombohedral phase with the crystal structure similar to the C phase can be made at ambient pressure; but the phase contains a high concentration of Ir deficiency. In this paper, we report that a rarely studied monoclinic (M) phase can be stabilized in narrow ranges of pressure and temperature in this P-T diagram. The peculiar crystal structure of the M-IrTe2 eliminates the tendency to form Ir-Ir dimers found in the H phase. The M phase has been fully characterized by structural determination and measurements of electrical resistivity, thermoelectric power, DC magnetization, and specific heat. These physical properties have been compared with those in the H and C phases of Ir1-xTe2. Moreover, magnetic and transport properties and specific heat of the M-IrTe2 can be fully justified by calculations with the density-functional theory presented in this paper., Comment: 23 pages, 9 figures, 3 tables, 29 references

The magnetic susceptibility, crystal and magnetic structures, and electronic structure of double perovskite Sr2ScOsO6 are reported. Using both neutron and x-ray powder diffraction we find that the crystal structure is monoclinic P21/n from 3.5 to 300 K. Magnetization measurements indicate an antiferromagnetic transition at TN=92K, one of the highest transition temperatures of any double perovskite hosting only one magnetic ion. Type I antiferromagnetic order is determined by neutron powder diffraction, with an Os moment of only 1.6(1) muB, close to half the spin-only value for a crystal field split 5d electron state with t2g^3 ground state. Density functional calculations show that this reduction is largely the result of strong Os-O hybridization, with spin-orbit coupling responsible for only a ~0.1 muB reduction in the moment., Comment: 5 pages, 4 figures

We report x-ray absorption and photoemission spectroscopy of the electronic structure in the normal state of metallic YFe2Ge2. The data reveal evidence for large fluctuating spin moments on the Fe sites, as indicated by exchange multiplets appearing in the Fe 3s core level photoemission spectra, even though the compound does not show magnetic order. The magnitude of the multiplet splitting is comparable to that observed in the normal state of the Fe-pnictide superconductors. This shows a connection between YFe2Ge2 and the Fe-based superconductors even though it contains neither pnictogens nor chalcogens. The implication is that the chemical range of compounds showing at least one of the characteristic magnetic signatures of the Fe-based superconductors is broader than previously thought., Comment: To appear

Ta$_4$Pd$_3$Te$_{16}$ is a recently discovered superconductor that has been suggested to be an unconventional superconductor near magnetism. We report electronic structure calculations showing that in spite of the layered crystal structure the material is an anisotropic three dimensional metal. The Fermi surface contains prominent one and two dimensional features, including nested 1D sheets, a 2D cylindrical section and a 3D sheet. The electronic states that make up the Fermi surface are mostly derived from Te $p$ states, with small Ta $d$ and Pd $d$ contributions. This places the compound far from magnetic instabilities. The results are discussed in terms of multiband superconductivity.

Single crystal x-ray diffraction, magnetic susceptibility, heat capacity, and electrical resistivity measurements are reported for the new tetragonal compound Ce$_{2}$PdGe$_{3}$, which forms in the space group $P4_{2}/mmc$ (\#131) $-$ a relative of the $\alpha$-ThSi$_2$-type structure. Measurements reveal a two-part antiferromagnetic phase transition at $T_{\rm{N,1}}$ $=$ 10.7 K and $T_{\rm{N,2}}$ $=$ 9.6 K and subsequent ferromagnetic ordering near $T_{\rm{C}}$ $\approx$ 2.25 K. The ordered ground state emerges from a lattice of Ce ions that are hybridized with the conduction electrons, as revealed by the enhanced electronic coefficient of the specific heat $\gamma$ $\approx$ 50 mJ/mol-Ce-K$^2$ (extrapolated to $T$ $=$ 0 for $T$ $<$ $T_{\rm{C}}$). Electronic structure calculations suggest that there is significant f-electron weight in the density of states near the Fermi energy and that the Fermi surface includes sheets with distinct nesting vectors. Chemical/structural disorder also plays an important role, as evidenced by results from single crystal x-ray diffraction, the width of the peaks in the heat capacity at $T_{\rm{N}}$ and $T_{\rm{C}}$, and the small residual resistivity ratio RRR $=$ $\rho_{\rm{300K}}$/$\rho_{\rm{0}}$ $=$ 1.8., Comment: 8 pages, 8 figures

The anharmonic lattice dynamics of rock-salt thermoelectric compounds SnTe and PbTe are investigated with inelastic neutron scattering (INS) and first-principles calculations. The experiments show that, surprisingly, although SnTe is closer to the ferroelectric instability, phonon spectra in PbTe exhibit a more anharmonic character. This behavior is reproduced in first-principles calculations of the temperature-dependent phonon self-energy. Our simulations reveal how the nesting of phonon dispersions induces prominent features in the self-energy, which account for the measured INS spectra and their temperature dependence. We establish that the phase-space for three-phonon scattering processes, rather than just the proximity to the lattice instability, is the mechanism determining the complex spectrum of the transverse-optical ferroelectric mode.

We report density functional studies of electron rich interfaces between KTaO3 or KNbO3 and CaSnO3 or ZnSnO3 and in particular the nature of the interfacial electron gasses that can be formed. We find that depending on the details these may occur on either the transition metal or stannate sides of the interface and in the later case can be shifted away from the interface by ferroelectricity. We also present calculations for bulk KNbO3, KTaO3, CaSnO3, BaSnO3 and ZnSnO3, showing the different transport and optical properties that may be expected on the two sides of such interfaces. The results suggest that these interfaces may display a wide range of behaviors depending on conditions, and in particular the interplay with ferroelectricity suggests that electrical control of these properties may be possible., Comment: published version

We report electronic structure calculations for BaTi$_2$Sb$_2$O and discuss the results in relation to the observed superconductivity of this material when hole doped with Na. The Fermi surface shows several sheets. These include a nested nearly 2D cylinder. There are also two sheets, which are three dimensional, in spite of the layered crystal structure. A magnetic instability associated with Fermi surface nesting is found. A sign-changing s-wave state, different from the one in the Fe-based superconductors, is predicted within a scenario of spin-fluctuation mediated superconductivity., Comment: Typos corrected. References updated

We use core-valence-valence (CVV) Auger spectra to probe the Coulomb repulsion between holes in the valence band of Fe pnictide superconductors. By comparing the two-hole final state spectra to density functional theory calculations of the single particle density of states, we extract a measure of the electron correlations that exist in these systems. Our results show that the Coulomb repulsion is highly screened and can definitively be considered as weak. We also find that there are differences between the 1111 and 122 families and even a small variation as a function of the doping, x, in Ba(Fe1 xCox)2As2. We discuss how the values of the hole-hole Coulomb repulsion obtained from our study relate to the onsite Coulomb parameter "U" used in model and first principles calculations based on dynamical mean field theory, and establish an upper bound for its effective value. Our results impose stringent constraints on model based phase diagrams, Comment: 16 pages, 4 figures

We respond to the comment of Bramwell et al (arXiv:1111.4168v1) to our original publication (S. R. Dunsiger et al, Phys. Rev. Lett. 107, 207207 (2011)), detailing muon spin rotation measurements of the Spin Ice compound Dy2Ti2O7., Comment: 2 pages; 1 figure; response to arXiv:1111.4168v1

The thermoelectric transport properties of CaMg2Bi2, EuMg2Bi2, and YbMg2Bi2 were characterized between 2 and 650K. As synthesized, the polycrystalline samples are found to have lower p-type carrier concentrations than single-crystalline samples of the same empirical formula. These low carrier concentration samples possess the highest mobilities yet reported for materials with the CaAl2Si2 structure type, with a mobility of ~740cm$^2$/V/s observed in EuMg2Bi2 at 50K. Despite decreases in the Seebeck coefficient (\alpha) and electrical resistivity (\rho) with increasing temperature, the power factor (\alpha^2/\rho) increases for all temperatures examined. This behavior suggests a strong asymmetry in the conduction of electrons and holes. The highest figure of merit (zT) is observed in YbMg2Bi2, with zT approaching 0.4 at 600K for two samples with carrier densities of approximately 2x10^{18}cm^{-3} and 8x10^{18}cm^{-3} at room temperature. Refinements of neutron powder diffraction data yield similar behavior for the structures of CaMg2Bi2 and YbMg2Bi2, with smooth lattice expansion and relative expansion in $c$ being ~35% larger than relative expansion in $a$ at 973K. First principles calculations reveal an increasing band gap as Bi is replaced by Sb then As, and subsequent Boltzmann transport calculations predict an increase in \alpha for a given $n$ associated with an increased effective mass as the gap opens. The magnitude and temperature dependence of \alpha suggests higher zT is likely to be achieved at larger carrier concentrations, roughly an order of magnitude higher than those in the current polycrystalline samples, which is also expected from the detailed calculations.

In a recent Letter Scanlon and Watson reported their first principles results on hydrogen in Cu2O. Their main conclusions are: (1) an interstitial H in Cu2O prefers to occupy the tetrahedral site, which is coordinated with four Cu cations, in all three charge states (+1, neutral, and -1); (2) H will bind with a Cu vacancy and form an electrically active H-VCu defect complex, which is amphoteric with (+/0) and (0/-)transition levels at Ev + 0.1 and Ev + 1.1 eV, respectively. However, these two conclusions contradict two generally observed behaviors of H in oxides: (i) cationic H usually binds with an O atom, forming a single O-H bond, while the anionic H usually binds with cations with multi-coordination; (ii) H usually passivates cation vacancies in oxides. In this Comment, we explicitly show that with charge state +1, H prefers to bind with a single O anion rather than with four Cu cations and that H-VCu does not induce any defect levels inside the band gap., Comment: 2 pages and 1 figure

We present inelastic neutron scattering measurements and first principles calculations examining the intermetallic marcasite CrSb2. The observed spin wave dispersion implies that the magnetic interactions are strongly one-dimensional with antiferromagnetic chains parallel to the crystalline c-axis. Such low-dimensional excitations are unexpected in a semiconducting intermetallic system. Moreover this material may be further interesting in that the magnetic anisotropy may enhance thermoelectric properties along particular crystallographic directions., Comment: 5 pages, 4 figures, Submitted to an APS journal

We report density functional calculations addressing the electronic structure and magnetic properties of delafossite PdCrO2. We find substantial magnetic interactions in the c-axis direction as well as beyond first nearest neighbors in-plane, so that PdCrO2 is a 3D frustrated antiferromagnet. We also find substantial coupling between the Cr moments and the Pd derived conduction electrons.

Theory predicts the low-temperature magnetic excitations in spin ices consist of deconfined magnetic charges, or monopoles. A recent transverse-field (TF) muon spin rotation (muSR) experiment [S T Bramwell et al, Nature 461, 956 (2009)] reports results claiming to be consistent with the temperature and magnetic field dependence anticipated for monopole nucleation - the so-called second Wien effect. We demonstrate via a new series of muSR experiments in Dy_2Ti_2O_7 that such an effect is not observable in a TF muSR experiment. Rather, as found in many highly frustrated magnetic materials, we observe spin fluctuations which become temperature independent at low temperatures, behavior which dominates over any possible signature of thermally nucleated monopole excitations., Comment: 6 pages; 4 figures; published in Phys Rev. Lett. 107, 207207 (2011); Supplementary material and body of paper combined together in 1 file

Understanding the microscopic processes affecting the bulk thermal conductivity is crucial to develop more efficient thermoelectric materials. PbTe is currently one of the leading thermoelectric materials, largely thanks to its low thermal conductivity. However, the origin of this low thermal conductivity in a simple rocksalt structure has so far been elusive. Using a combination of inelastic neutron scattering measurements and first-principles computations of the phonons, we identify a strong anharmonic coupling between the ferroelectric transverse optic (TO) mode and the longitudinal acoustic (LA) modes in PbTe. This interaction extends over a large portion of reciprocal space, and directly affects the heat-carrying LA phonons. The LA-TO anharmonic coupling is likely to play a central role in explaining the low thermal conductivity of PbTe. The present results provide a microscopic picture of why many good thermoelectric materials are found near a lattice instability of the ferroelectric type.

We have performed low-temperature specific heat $C$ and thermal conductivity $\kappa$ measurements on the Ni-pnictide superconductors BaNi$_2$As$_2$ ($T_\mathrm{c}$=0.7 K and SrNi$_2$P$_2$ ($T_\mathrm{c}$=1.4 K). The temperature dependences $C(T)$ and $\kappa(T)$ of the two compounds are similar to the results of a number of s-wave superconductors. Furthermore, the concave field responses of the residual $\kappa$ for BaNi$_2$As$_2$ rules out the presence of nodes on the Fermi surfaces. We postulate that fully gapped superconductivity could be universal for Ni-pnictide superconductors. Specific heat data on Ba$_{0.6}$La$_{0.4}$Ni$_2$As$_2$ shows a mild suppression of $T_\mathrm{c}$ and $H_\mathrm{c2}$ relative to BaNi$_2$As$_2$., Comment: 5 pages, 3 figures, to be published in J. Phys.: Conf. Ser

We present neutron diffraction measurements on single crystal samples of non-superconducting Ba(Fe1-xCrx)2As2 as a function of Cr-doping for 0<=x<=0.47. The average SDW moment is independent of concentration for x<=0.2 and decreases rapidly for x>=0.3. For concentrations in excess of 30% chromium, we find a new G-type antiferromagnetic phase which rapidly becomes the dominant magnetic ground state. Strong magnetism is observed for all concentrations measured and competition between these ordered states and superconductivity naturally explains the absence of superconductivity in the Cr-doped materials., Comment: 4 pages, 3 figures

Here, we present a de Haas-van Alphen (dHvA) effect1 study on the newly discovered LaFeAsO1-xFx compounds2,3 in order to unveil the topography of the Fermi surface associated with their antiferromagnetic and superconducting phases, which is essential for understanding their magnetism, pairing symmetry and superconducting mechanism. Calculations 4 and surface-sensitive measurements 5,6,7 provided early guidance, but lead to contradictory results, generating a need for a direct experimental probe of their bulk Fermi surface. In antiferromagnetic LaFeAsO1-xFx 8,9 we observe a complex pattern in the Fourier spectrum of the oscillatory component superimposed onto the magnetic torque signal revealing a reconstructed Fermi surface, whose geometry is not fully described by band structure calculations. Surprisingly, several of the same frequencies, or Fermi surface cross-sectional areas, are also observed in superconducting LaFeAsO1-xFx (with a superconducting transition temperature Tc ~ 15 K). Although one could attribute this to inhomogeneous F doping, the corresponding effective masses are largely enhanced with respect to those of the antiferromagnetic compound. Instead, this implies the microscopic coexistence of superconductivity and antiferromagnetism on the same Fermi surface in the underdoped region of the phase diagram of the LaFeAsO1-xFx series. Thus, the dHvA-effect reveals a more complex Fermi surface topography than that predicted by band structure calculations4 upon which the currently proposed superconducting pairing scenarios10,11,12,13 are based, which could be at the origin of their higher Tcs when compared to their phosphide analogs., Comment: 22 pages, supplementary information inclosed

We investigate the effect of $A$-site size differences in the double perovskites BiScO$_3$-$M$NbO$_3$ ($M$$=$Na, K and Rb) using first-principles calculations. We find that the polarization of these materials is 70$\sim$90 $\mu$C/cm$^2$ along the rhombohedral direction. The main contribution to the high polarization comes from large off-centerings of Bi ions, which are strongly enhanced by the suppression of octahedral tilts as the $M$ ion size increases. A high Born effective charge of Nb also contributes to the polarization and this contribution is also enhanced by increasing the $M$ ion size.

We report an extensive study on the intrinsic bulk electronic structure of the high-temperature superconductor CeFeAsO0.89F0.11 and its parent compound CeFeAsO by soft and hard x-ray photoemission, x-ray absorption and soft-x-ray emission spectroscopies. The complementary surface/bulk probing depth, and the elemental and chemical sensitivity of these techniques allows resolving the intrinsic electronic structure of each element and correlating it with the local structure, which has been probed by extended-x-ray absorption fine structure spectroscopy. The measurements indicate a predominant 4f1 (i.e. Ce3+) initial state configuration for Cerium and an effective valence-band-to-4f charge-transfer screening of the core hole. The spectra also reveal the presence of a small Ce f0 initial state configuration, which we assign to the occurrence of an intermediate valence state. The data reveal a reasonably good agreement with the partial density of states as obtained in standard density functional calculations over a large energy range. Implications for the electronic structure of these materials are discussed., Comment: Accepted for publication in Phys. Rev. B

Experiments that have been interpreted as providing evidence that the pseudogap phase in cuprates is an electronic nematic are discussed from the point of view of lattice structure. We conclude that existing experiments are not sufficient to prove a nematic origin of the pseudogap in underdoped cuprates., Comment: No changes. Fig. 2 is replaced because the previous version did not render correctly on all software

Hanaguri et al (Science, 8th of January 2010, p. 181) have reported STM measurements on an Fe-based superconductor Fe(Se,Te). After Fourier-transforming their data they found three sets of sharp peaks in the reciprocal space. They interpreted one as a Bragg peak (an umklapp scattering) and two as resulting from quasiparticle interference (QPI) We point out that at least one of these two peaks is also a Bragg peak, corresponding to another reciprocal lattice vector, and therefore is not a QPI peak, and the third peak has similar structure, too sharp for a QPI peak in a nodeless superconductor with an isotropic gap, proposed by Hanaguri et al. We argue that this peak must also be a Bragg peak related to a surface reconstruction doubling the unit cell. We also calculate the QPI pattern, assuming an isotropic gap, and find that indeed it is quite different from the experiment. Finally, we speculate about possible origin of the magnetic field dependence of the Bragg peaks in this compound., Comment: An improved, more informative abstract created

The doping and temperature dependent thermopower of SnTe is calculated from the first principles band structure using Boltzmann transport theory. We find that the $p$-type thermopower is inferior to PbTe consistent with experimental observations, but that the $n$-type thermopower is substantially more favorable.

The orbital symmetries of electron doped iron-arsenide superconductors Ba(Fe1-xCox)2As2 have been measured with x-ray absorption spectroscopy. The data reveal signatures of Fe d electron itinerancy, weak electronic correlations, and a high degree of Fe-As hybridization related to the bonding topology of the Fe dxz+yz states, which are found to contribute substantially at the Fermi level. The energies and detailed orbital character of Fe and As derived unoccupied s and d states are found to be in remarkably good agreement with the predictions of standard density functional theory., Comment: Accepted for publication in Phys. Rev. B, 3 figures. Minor corrections added

Electronic structure and lattice dynamics calculations on thallium halides show that the Born effective charges in these compounds are more than twice larger than the nominal ionic charges. This is a result of cross-band-gap hybridization between Tl-p and halogen-p states. The large Born charges cause giant splitting between longitudinal and transverse optic phonon modes, bringing the lattice close to ferroelectric instability. Our calculations indeed show spontaneous lattice polarization upon lattice expansion starting at 2%. It is remarkable that the apparently ionic thallium halides with a simple cubic CsCl structure and large differences in electronegativity between cations and anions can be very close to ferroelectricity. This can lead to effective screening of defects and impurities that would otherwise be strong carrier traps and may therefore contribute to the relatively good carrier transport properties in TlBr radiation detectors., Comment: PDF only

The polar behavior of double perovskite (Bi,Pb)ZnNbO$_6$ and (Bi,Sr)ZnNbO$_6$ was investigated using first principles density functional calculations within the local density approximation. These materials have both $A$-site size disorder and ions with sterochemical activity. We found a strong ferroelectric distortion in both materials. The polarization of the Pb material is $>$80 $\mu$C/cm$^2$ along the rhombohedral direction and the Sr based material is only slightly inferior. The high polarization results mainly from a large off-centering of Bi and the large Born effective charge of Nb, which yields a large contribution polarization although the Nb off-centers by a smaller amount. Neither of these materials favors a tetragonal state, and therefore solid solutions with PbTiO$_3$ may show morphotoropic phase boundaries.

We discuss the discrepancy between the measured optical Drude weight and band structure calculations in LaFePO and other iron-based superconductors. This discrepancy is mostly due to mass renormalization arising from electronic correlation effects., Comment: 3 pages

The {57}Fe-specific phonon density of states of Ba(Fe(1-x)Co(x))2As2 single crystals (x=0.0, 0.08) was measured at cryogenic temperatures and at high pressures with nuclear-resonant inelastic x-ray scattering. Measurements were conducted for two different orientations of the single crystals, yielding the orientation-projected {57}Fe-phonon density of states (DOS) for phonon polarizations in-plane and out-of-plane with respect to the basal plane of the crystal structure. In the tetragonal phase at 300 K, a clear stiffening was observed upon doping with Co. Increasing pressure to 4 GPa caused a marked increase of phonon frequencies, with the doped material still stiffer than the parent compound. Upon cooling, both the doped and undoped samples showed a stiffening, and the parent compound exhibited a discontinuity across the magnetic and structural phase transition. These findings are generally compatible with the changes in volume of the system upon doping, increasing pressure, or increasing temperature, but an extra softening of high-energy modes occurs with increasing temperature. First-principles computations of the phonon DOS were performed and showed an overall agreement with the experimental results, but underestimate the Grueneisen parameter. This discrepancy is explained in terms of a magnetic Grueneisen parameter, causing an extra phonon stiffening as magnetism is suppressed under pressure.

We report density functional studies of the Fe$_{1-x}$Cu$_x$Se alloy done using supercell and coherent potential approximation methods. Magnetic behavior was investigated using the disordered local moment approach. We find that Cu occurs in a nominal $d^{10}$ configuration and is highly disruptive to the electronic structure of the Fe sheets. This would be consistent with a metal insulator transition due to Anderson localization. We further find a strong cross over from a weak moment itinerant system to a local moment magnet at $x \approx 0.12$. We associate this with the experimentally observed jump near this concentration. Our results are consistent with the characterization of this concentration dependent jump as a transition to a spin-glass.

Through a systematic high resolution angle-resolved photoemission study of the iron pnictide compounds (Ba,Sr)Fe$_2$As$_2$, we show that the electronic structures of these compounds are significantly reconstructed across the spin density wave ordering, which cannot be described by a simple folding scenario of conventional density wave ordering. Moreover, we find that LDA calculations with an incorporated suppressed magnetic moment of 0.5$\mu_{\tiny{\textrm{B}}}$ can match well the details in the reconstructed electronic structure, suggesting that the nature of magnetism in the pnictides is more itinerant than local, while the origin of suppressed magnetic moment remains an important issue for future investigations.