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High-resolution angle- and spin-resolved photoemission spectroscopy reveals new features of the electronic structure of the ferromagnetic triple-layered ruthenate Sr$_4$Ru$_3$O$_{10}$. There are narrow spectral peaks $\sim$30 meV below the Fermi-level in two regions of the Brillouin zone: a hole-like band at the zone-center and a saddle-point van Hove singularity at the zone edge. Below T$_c$ each feature is almost completely spin-polarized, with opposite sign polarization and with strong Kondo-coherence-like temperature-dependent spectral weight variation suggestive of strong Hund's metal correlations. In addition, there are distinct Fermi surfaces for wide electron-like minority spin bands around the zone center and narrow hole-like majority spin Fermi surface contours around the zone corners. The origin of these features is in general agreement with density functional calculations, if they are shifted to reduce the exchange splitting, and scaled to take into account effects of correlation. Furthermore, the deduced narrow band origins from the tri-layer splitting of $d_{xz/yz}$ orbitals implies a layer-specific spin-polarization contribution from the narrow bands. Over a larger energy range, net spin-majority polarization of incoherent Ru $d$-bands is observed to extend down to the top of the oxygen bands, where additional narrow oxygen bands contribute to the magnetism with spin-minority polarization., Comment: 11 pages, 5 figures plus supplement 8 pages, 4 figures

Previous high-resolution angle-resolved photoemission (ARPES) studies of URu$_2$Si$_2$ have characterized the temperature-dependent behavior of narrow-band states close to the Fermi level ($E_\mathrm{F}$) at low photon energies near the zone center, with an emphasis on electronic reconstruction due to Brillouin zone folding. A substantial challenge to a proper description is that these states interact with other hole-band states that are generally absent from bulk-sensitive soft x-ray ARPES measurements. Here we provide a more global $k$-space context for the presence of such states and their relation to the bulk Fermi surface topology using synchrotron-based wide-angle and photon energy-dependent ARPES mapping of the electronic structure using photon energies intermediate between the low-energy regime and the high-energy soft x-ray regime. Small-spot spatial dependence, $f$-resonant photoemission, Si 2$p$ core-levels, x-ray polarization, surface-dosing modification, and theoretical surface slab calculations are employed to assist identification of bulk versus surface state character of the $E_\mathrm{F}$-crossing bands and their relation to specific U- or Si-terminations of the cleaved surface. The bulk Fermi surface topology is critically compared to density functional theory and to dynamical mean field theory calculations. In addition to clarifying some aspects of the previously measured high symmetry $\Gamma$, Z and X points, incommensurate 0.6a* nested Fermi-edge states located along Z-N-Z are found to be distinctly different from the density functional theory Fermi surface prediction. The temperature evolution of these states above $T_{HO}$, combined with a more detailed theoretical investigation of this region, suggests a key role of the N-point in the hidden order transition., Comment: topical review 47 pages, 12 figures, proof edits, hyperlinked TOC

At ambient pressure, lithium molybdenum purple bronze (Li0.9Mo6O17) is a quasi-one dimensional solid in which the anisotropic crystal structure and the linear dispersion of the underlying bands produced by electronic correlations possibly bring about a rare experimental realization of Tomomaga-Luttinger liquid physics. It is also the sole member of the broader purple molybdenum bronzes family where a Peierls instability has not been identified at low temperatures. The present study reports a pressure-induced series of phase transitions between 0 and 12 GPa. These transitions are strongly reflected in infrared spectroscopy, Raman spectroscopy, and x-ray diffraction. The most dramatic effect seen in optical conductivity is the metallization of the c-axis, concomitant to the decrease of conductivity along the b-axis. This indicates that high pressure drives the material away from its quasi-one dimensional behavior at ambient pressure. While the first pressure-induced structure of the series is resolved, the identification of the underlying mechanisms driving the dimensional change in the physics remains a challenge., Comment: 10 pages, 12 figures

In this set of three papers, we present the results of a combined study by density-functional (LDA) band theory (NMTO) and angle-resolved photoemission spectroscopy (ARPES) of lithium purple bronze, 2(Li$_{1x}$Mo$_{6}$O$_{17}$). This material is particularly notable for its unusually robust quasi-one-dimensional (quasi-1D) behavior. The band structure, in a large energy window around the Fermi energy, is basically 2D and formed by three Mo $t_{2g}$-like extended Wannier orbitals (WOs) per cell, each one giving rise to a 1D band running at a 120$^{\circ }$ angle to the two others. A structural "dimerization" from $\mathbf{c}/2$ to $\mathbf{c}$ gaps the $xz$ and $yz$ bands while leaving the $xy$ bands metallic in the gap but resonantly coupled to the gap edges and, hence, to the two other directions. The resulting complex shape of the quasi-1D Fermi surface (FS), verified by our ARPES, thus depends strongly on the Fermi energy position in the gap, implying a great sensitivity to Li stoichiometry of properties dependent on the FS, such as FS nesting or superconductivity. The band structure, expressed as a six-band, analytical tight-binding (TB) Hamiltonian, is verified in detail by the recognition and application of an ARPES selection rule that enables, for the first time, the separation in ARPES spectra of the two barely split $xy$ bands and the observation of their complex split FS. The strong resonances prevent either a two-band TB model or a related real-space ladder picture from giving a valid description of the low-energy electronic structure. Down to a temperature of 6$\,$K we find no evidence for a theoretically expected downward renormalization of perpendicular single particle hopping due to LL fluctuations in the quasi-1D chains.

Analyzing temperature dependent photoemission (PE) data of the ferromagnetic Kondo-lattice (KL) system YbNiSn in the light of the Periodic Anderson model (PAM) we show that the KL behavior is not limited to temperatures below a temperature T_K, defined empirically from resistivity and specificic heat measurements. As characteristic for weakly hybridized Ce and Yb systems, the PE spectra reveal a 4f-derived Fermi level peak, which reflects contributions from the Kondo resonance and its crystal electric field (CEF) satellites. In YbNiSn this peak has an unusual temperature dependence: With decreasing temperature a steady linear increase of intensity is observed which extends over a large interval ranging from 100 K down to 1 K without showing any peculiarities in the region of T_K ~ TC= 5.6 K. In the light of the single-impurity Anderson model (SIAM) this intensity variation reflects a linear increase of 4f occupancy with decreasing temperature, indicating an onset of Kondo screening at temperatures above 100 K. Within the PAM this phenomenon could be described by a non-Fermi liquid like T- linear damping of the self-energy which accounts phenomenologically for the feedback from the closely spaced CEF-states., Comment: Accepted to Phys. Rev. B

The temperature-dependent evolution of the Kondo lattice is a long-standing topic of theoretical and experimental investigation and yet it lacks a truly microscopic description of the relation of the basic $f$-$d$ hybridization processes to the fundamental temperature scales of Kondo screening and Fermi-liquid lattice coherence. Here, the temperature-dependence of $f$-$d$ hybridized band dispersions and Fermi-energy $f$ spectral weight in the Kondo lattice system CeCoIn$_5$ is investigated using $f$-resonant angle-resolved photoemission (ARPES) with sufficient detail to allow direct comparison to first principles dynamical mean field theory (DMFT) calculations containing full realism of crystalline electric field states. The ARPES results, for two orthogonal (001) and (100) cleaved surfaces and three different $f$-$d$ hybridization scenarios, with additional microscopic insight provided by DMFT, reveal $f$ participation in the Fermi surface at temperatures much higher than the lattice coherence temperature, $T^*\approx$ 45 K, commonly believed to be the onset for such behavior. The identification of a $T$-dependent crystalline electric field degeneracy crossover in the DMFT theory $below$ $T^*$ is specifically highlighted., Comment: 10 pages, 5 figures plus supplement 11 pages, 10 figures

Using angle resolved photoemission spectroscopy (ARPES) we report the first band dispersions and distinct features of the bulk Fermi surface (FS) in the paramagnetic metallic phase of the prototypical metal-insulator transition material V$_2$O$_3$. Along the $c$-axis we observe both an electron pocket and a triangular hole-like FS topology, showing that both V 3$d$ $a_{1g}$ and $e_g^{\pi}$ states contribute to the FS. These results challenge the existing correlation-enhanced crystal field splitting theoretical explanation for the transition mechanism and pave the way for the solution of this mystery., Comment: 5 pages, 4 figures plus supplement 12 pages, 3 figures, 1 table

The angle resolved photoemission spectroscopy lineshapes of quasi one-dimensional (1d) Li0.9Mo6O17 display both agreement with and departures from the one-band Tomonaga-Luttinger model. We show that the departures can be understood by explicitly accounting for the four modes arising from the two quasi-1d bands known to cross the Fermi energy. The key assumption is that the antisymmetric charge mode is gapped with a magnitude near the temperature (T) of a mysterious 25K powerlaw resistivity upturn. The gap is consistent with the lack of a charge or spin density wave accompanying the upturn, is able to control the upturn T, and prevents crossover to a Fermi liquid (FL) down to the superconducting transition at 1.9K., Comment: 5 pages 4 figures

The mixed valent compound SmB6 is of high current interest as the first candidate example of topologically protected surface states in a strongly correlated insulator and also as a possible host for an exotic bulk many-body state that would manifest properties of both an insulator and a metal. Two different de Haas van Alphen (dHvA) experiments have each supported one of these possibilities, while angle resolved photoemission spectroscopy (ARPES) for the (001) surface has supported the first, but without quantitative agreement to the dHvA results. We present new ARPES data for the (110) surface and a new analysis of all published dHvA data and thereby bring ARPES and dHvA into substantial consistency around the basic narrative of two dimensional surface states., Comment: 5 pages, 4 figures + supplement (12 pages, 6 figures)

To resolve the controversial issue of the topological nature of the electronic structure of YbB$_{6}$, we have made a combined study using density functional theory (DFT) and angle resolved photoemission spectroscopy (ARPES). Accurate determination of the low energy band topology in DFT requires the use of modified Becke-Johnson exchange potential incorporating the spin-orbit coupling and the on-site Coulomb interaction $U$ of Yb $4f$ electrons as large as 7 eV. We have double-checked the DFT result with the more precise GW band calculation. ARPES is done with the non-polar (110) surface termination to avoid band bending and quantum well confinement that have confused ARPES spectra taken on the polar (001) surface termination. Thereby we show definitively that YbB$_{6}$ has a topologically trivial B 2$p$-Yb 5$d$ semiconductor band gap, and hence is a non-Kondo non-topological insulator (TI). In agreement with theory, ARPES shows pure divalency for Yb and a $p$-$d$ band gap of 0.3 eV, which clearly rules out both of the previous scenarios of $f$-$d$ band inversion Kondo TI and $p$-$d$ band inversion non-Kondo TI. We have also examined the pressure-dependent electronic structure of YbB$_{6}$, and found that the high pressure phase is not a Kondo TI but a \emph{p}-\emph{d} overlap semimetal., Comment: The main text is 6 pages with 4 figures, and the supplementary information contains 6 figures. 11 pages, 10 figures in total To be appeared in Phys. Rev. Lett. (Online publication is around March 16 if no delays.)

We have performed soft-X-ray angle resolved photoemission for metallic V$_2$O$_3$. Combining a micro focus beam (40 x 65 ${\mu}$m$^2$) and micro positioning techniques with a long working distance microscope, we have succeeded in observing band dispersions from tiny cleavage surfaces with typical size of the several tens of ${\mu}$m. The photoemission spectra show a clear position dependence reflecting the morphology of the cleaved sample surface. By selecting high quality flat regions on the sample surface, we have succeeded in band mapping using both photon-energy and polar-angle dependences, opening the door to three-dimensional ARPES for typical three dimensional correlated materials where large cleavage planes are rarely obtained., Comment: 5 pages, 4 figures, to be published in Journal of Synchrotron Radiation

The recent conjecture of a topologically-protected surface state in SmB$_6$ and the verification of robust surface conduction below 4 K have prompted a large effort to understand the surface states. Conventional Hall transport measurements allow current to flow on all surfaces of a topological insulator, so such measurements are influenced by contributions from multiple surfaces of varying transport character. Instead, we study magnetotransport of SmB$_6$ using a Corbino geometry, which can directly measure the conductivity of a single, independent surface. Both (011) and (001) crystal surfaces show a strong negative magnetoresistance at all magnetic field angles measured. The (011) surface has a carrier mobility of $122\text{ cm}^2/\text{V}\cdot\text{sec}$ with a carrier density of $2.5\times10^{13} \text{ cm}^{-2}$, which are significantly smaller than indicated by Hall transport studies. This mobility value can explain a failure so far to observe Shubnikov-de Haas oscillations. Analysis of the angle-dependence of conductivity on the (011) surface suggests a combination of a field-dependent enhancement of the carrier density and a suppression of Kondo scattering from native oxide layer magnetic moments as the likely origin of the negative magnetoresistance. Our results also reveal a hysteretic behavior whose magnitude depends on the magnetic field sweep rate and temperature. Although this feature becomes smaller when the field sweep is slower, does not disappear or saturate during our slowest sweep-rate measurements, which is much slower than a typical magnetotransport trace. These observations cannot be explained by quantum interference corrections such as weak anti-localization, but are more likely due to an extrinsic magnetic effect such as the magnetocaloric effect or glassy ordering., Comment: 29 pages, 12 figures, PDFLaTeX. This new version is a combination of the prior version and arXiv:1410.7430

High temperature superconductivity in cuprates arises from an electronic state that remains poorly understood. We report the observation of a related electronic state in a non-cuprate material Sr2IrO4 in which the unique cuprate Fermiology is largely reproduced. Upon surface electron doping through in situ deposition of alkali-metal atoms, angle-resolved photoemission spectra of Sr2IrO4 display disconnected segments of zero-energy states, known as Fermi arcs, and a gap as large as 80 meV. Its evolution toward a normal metal phase with a closed Fermi surface as a function of doping and temperature parallels that in the cuprates. Our result suggests that Sr2IrO4 is a useful model system for comparison to the cuprates., Comment: Science, 12 June 2014

Taken together and viewed holistically, recent theory, low temperature (T) transport, photoelectron spectroscopy and quantum oscillation experiments have built a very strong case that the paradigmatic mixed valence insulator SmB6 is currently unique as a three-dimensional strongly correlated topological insulator (TI). As such, its many-body T-dependent bulk gap brings an extra richness to the physics beyond that of the weakly correlated TI materials. How will the robust, symmetry-protected TI surface states evolve as the gap closes with increasing T? For SmB6 exploiting this opportunity first requires resolution of other important gap-related issues, its origin, its magnitude, its T-dependence and its role in bulk transport. In this paper we report detailed T-dependent angle resolved photoemission spectroscopy (ARPES) measurements that answer all these questions in a unified way., Comment: 30 pages 10 figures; updated references, a few revised discussions

We prove theoretically that certain strongly correlated Kondo insulators are topological crystalline insulators with nontrivial topology protected by crystal symmetries. In particular, we find that SmB$_6$ is such a material. In addition to a nontrivial Z$_2$ topological index protected by time reversal symmetry, SmB$_6$ also has nontrival mirror Chern numbers protected by mirror symmetries. On the $(100)$ surface of SmB$_6$, the nontrivial mirror Chern numbers do not generate additional surface states beyond those predicted by the Z$_2$ topological index. However, on the $(110)$ surface, two more surface Dirac points are predicted. Remarkably, we find that for SmB$_6$ both the Z$_2$ topological index and the mirror Chern numbers are independent of microscopic details, which enables us to obtain surface state properties that are universal., Comment: 4 pages + 3 pages Supplementary Information, 3 figures

In Kondo insulator samarium hexaboride SmB$_6$, strong correlation and band hybridization lead to an insulating gap and a diverging resistance at low temperature. The resistance divergence ends at about 5 Kelvin, a behavior recently demonstrated to arise from the surface conductance. However, questions remain whether and where a topological surface state exists. Quantum oscillations have not been observed to map the Fermi surface. We solve the problem by resolving the Landau Level quantization and Fermi surface topology using torque magnetometry. The observed Fermi surface suggests a two dimensional surface state on the (101) plane. Furthermore, the tracking of the Landau Levels in the infinite magnetic field limit points to -1/2, which indicates a 2D Dirac electronic state.

Iridium-based 5d transition-metal oxides are attractive candidates for the study of correlated electronic states due to the interplay of enhanced crystal-field, Coulomb and spin-orbit interaction energies. At ambient pressure, these conditions promote a novel Jeff = 1/2 Mott insulating state, characterized by a gap of the order of ~0.1 eV. We present high-pressure electrical resistivity measurements of single crystals of Sr2IrO4 and Sr3Ir2O7. While no indications of a pressure-induced metallic state up to 55 GPa were found in Sr2IrO4, a strong decrease of the gap energy and of the resistance of Sr3Ir2O7 between ambient pressure and 104 GPa confirm that this compound is in the proximity of a metal-insulator transition., Comment: 5 pages, 4 figures

The electronic structure of (Ce,Yb)CoIn5 has been studied by a combination of photoemission, x-ray absorption and bulk property measurements. Previous findings of a Ce valence near 3+ for all x and of an Yb valence near 2.3+ for x>0.3 were confirmed. One new result of this study is that the Yb valence for x<0.2 increases rapidly with decreasing x from 2.3+ toward 3+, which correlates well with de Haas van Alphen results showing a change of Fermi surface around x=0.2. Another new result is the direct observation by angle resolved photoemission Fermi surface maps of about 50% cross sectional area reductions of the \alpha- and \beta-sheets for x=1 compared to x=0, and a smaller, essentially proportionate, size change of the \alpha-sheet for x=0.2. These changes are found to be in good general agreement with expectations from simple electron counting. The implications of these results for the unusual robustness of superconductivity and Kondo coherence with increasing x in this alloy system are discussed.

We study the transport properties of the Kondo insulator SmB$_6$ with a specialized configuration designed to distinguish bulk-dominated conduction from surface-dominated conduction. We find that as the material is cooled below 4 K, it exhibits a crossover from bulk to surface conduction with a fully insulating bulk. We take the robustness and magnitude of the surface conductivity, as is manifest in the literature of SmB$_6$, to be strong evidence for the topological insulator metallic surface states recently predicted for this material., Comment: 23 pages, 8 figures. We updated minor editorial changes and references to match the published version

Temperature dependent photoemission spectroscopy in Li0.9Mo6O17 contributes to evidence for one dimensional physics that is unusually robust. Three generic characteristics of the Luttinger liquid are observed, power law behavior of the k-integrated spectral function down to temperatures just above the superconducting transition, k-resolved lineshapes that show holon and spinon features, and quantum critical (QC) scaling in the lineshapes. Departures of the lineshapes and the scaling from expectations in the Tomonaga Luttinger model can be partially described by a phenomenological momentum broadening that is presented and discussed. The possibility that some form of 1d physics obtains even down to the superconducting transition temperature is assessed., Comment: submitted to JPCM, Special issue article "Physics in one dimension"

We have performed high-resolution hard X-ray photoemission spectroscopy for the metal-insulator transition (MIT) system (V(1-x)Cr(x))2O3 in the paramagnetic metal, paramagnetic insulator and antiferromagentic insulator phases. The quality of the spectra enables us to conclude that the on-site Coulomb energy U does not change through the MIT, which eliminate all but one theoretical MIT scenario in this paradigm material., Comment: 4 pages, 3 figures

Angle resolved photoemission spectroscopy (ARPES) has been performed on quasi-one dimensional Li0.9Mo6O17 using photon energy 500 eV. Measured band dispersions are in agreement with those from both low photon energy measurements and band structure calculations. The momentum integrated ARPES spectrum is well fit by the finite temperature Luttinger liquid (LL)spectral function, with an anomalous exponent 0.6 that is the same within experimental uncertainty as the value found with photon energy 30 eV. These identical findings at both low and high photon energies are entirely consistent with reasoning based on the crystal structure, that the quasi-one dimensional chains lie two layers below the cleavage plane so that the observed spectroscopic LL behavior of Li0.9Mo6O17 is a bulk property., Comment: Accepted for publication in Physical Review B

We present high-resolution bulk-sensitive photoemission spectra of (V$_{1-x}$M$_x$)$_2$O$_3$ (M=Cr, Ti). The measurements were made for the paramagnetic metal (PM), paramagnetic insulator (PI), and antiferromagnetic insulator (AFI) phases of (V$_{1-x}$M$_x$)$_2$O$_3$ with the samples of $x$ = 0, 0.012, and 0.028 for Cr-doping and $x$ = 0.01 for Ti-doping. In the PM phase, we observe a prominent quasiparticle peak in general agreement with theory, which combines dynamical mean-field theory with the local density approximation (LDA+DMFT). The quasiparticle peak shows a significantly larger peak width and weight than in the theory. For both the PI and AFI phases, the vanadium 3d parts of the valence spectra are not simple one peak structures. For the PI phase, there is not yet a good theoretical understanding of these structures. The size of the electron removal gap increases, and spectral weight accumulates in the energy range closer to the chemical potential, when the PI to AFI transition occurs. Spectra taken in the same phases with different compositions show interesting monotonic changes as the dopant concentration increases, regardless of the dopant species. With increased Cr-doping, the AFI phase gap decreases and the PI phase gap increases., Comment: 13 pages, 16 figures. accepted for publication in Physical Review B

Using x-ray absorption spectroscopy at the Ru-$L_{2,3}$ edge we reveal that the Ru$^{4+}$ ions remain in the $S$=1 spin state across the rare 4d-orbital ordering transition and spin-gap formation. We find using local spin density approximation + Hubbard U (LSDA+U) band structure calculations that the crystal fields in the low temperature phase are not strong enough to stabilize the $S$=0 state. Instead, we identify a distinct orbital ordering with a significant anisotropy of the antiferromagnetic exchange couplings. We conclude that La$_{4}$Ru$_{2}$O$_{10}$ appears to be a novel material in which the orbital physics drives the formation of spin-singlet dimers in a quasi 2-dimensional $S$=1 system., Comment: 5 pages, 4 figures, and 1 table

Temperature dependent high resolution photoemission spectra of quasi-1 dimensional Li$_{0.9}$Mo$_6$O$_{17}$ evince a strong renormalization of its Luttinger liquid density-of-states anomalous exponent. We trace this new effect to interacting charge neutral critical modes that emerge naturally from the two-band nature of the material. Li$_{0.9}$Mo$_6$O$_{17}$ is shown thereby to be a paradigm material that is capable of revealing new Luttinger physics., Comment: 4 pages, 3 figures. Accepted for publication by Phys. Rev. Lett

Studying the antiferromagnetic phase of the Hubbard model by dynamical mean field theory, we observe striking differences with static (Hartree-Fock) mean field: The Slater band is strongly renormalized and spectral weight is transferred to spin-polaron side bands. Already for intermediate values of the interaction $U$ the overall bandwidth is larger than in Hartree-Fock, and the gap is considerably smaller. Such differences survive any renormalization of $U$. Our photoemission experiments for Cr-doped V$_2$O$_3$ show spectra qualitatively well described by dynamical mean field theory., Comment: 6 pages, 5 figures - one figure added and further details about quasiparticle dispersion

We report angle resolved photoemission (ARPES) spectra of $\eta$-Mo$_4$O$_{11}$, a layered metal that undergoes two charge density wave (CDW) transitions at 109 K and 30 K. We have directly observed the ``hidden one-dimensional (hidden-1d)'' Fermi surface and an anisotropic gap opening associated with the 109 K transition, in agreement with the band theoretical description of the CDW transition. In addition, as in other hidden-1d materials such as NaMo$_6$O$_{17}$, the ARPES line shapes show certain anomalies, which we discuss in terms of non-Fermi liquid physics and possible roles of disorder., Comment: 3 figures; Erratum added to include missed references

The Kondo resonance is the spectral manifestation of the Kondo properties of the impurity Anderson model, and also plays a central role in the dynamical mean-field theory (DMFT) for correlated electron lattice systems. This article presents an overview of electron spectroscopy studies of the resonance for the 4f electrons of cerium compounds, and for the 3d electrons of V_2O_3, including beginning efforts at using angle resolved photoemission to determine the k-dependence of the resonance. The overview includes the comparison and analysis of spectroscopy data with theoretical spectra as calculated for the impurity model and as obtained by DMFT, and the Kondo volume collapse calculation of the cerium alpha-gamma phase transition boundary, with its spectroscopic underpinnings., Comment: 32 pages, 11 figures, 151 references; paper for special issue of J. Phys. Soc. Jpn. on "Kondo Effect--40 Years after the Discovery"

The combination of bandstructure theory in the local density approximation with dynamical mean field theory was recently successfully applied to V$_2$O$_3$ -- a material which undergoes the f amous Mott-Hubbard metal-insulator transition upon Cr doping. The aim of this sh ort paper is to emphasize two aspects of our recent results: (i) the filling of the Mott-Hubbard gap with increasing temperature, and (ii) the peculiarities of the Mott-Hubbard transition in this system which is not characterized by a diver gence of the effective mass for the $a_{1g}$-orbital., Comment: 2 pages, 3 figures, SCES'04 conference proceedings

We propose a computational scheme for the ab initio calculation of Wannier functions (WFs) for correlated electronic materials. The full-orbital Hamiltonian H is projected into the WF subspace defined by the physically most relevant partially filled bands. The Hamiltonian H^{WF} obtained in this way, with interaction parameters calculated by constrained LDA for the Wannier orbitals, is used as an ab initio setup of the correlation problem, which can then be solved by many-body techniques, e.g., dynamical mean-field theory (DMFT). In such calculations the self-energy operator \Sigma(e) is defined in WF basis which then can be converted back into the full-orbital Hilbert space to compute the full-orbital interacting Green function G(r,r',e). Using G(r,r',e) one can evaluate the charge density, modified by correlations, together with a new set of WFs, thus defining a fully self-consistent scheme. The Green function can also be used for the calculation of spectral, magnetic and electronic properties of the system. Here we report the results obtained with this method for SrVO3 and V2O3. Comparisons are made with previous results obtained by the LDA+DMFT approach where the LDA DOS was used as input, and with new bulk-sensitive experimental spectra., Comment: 36 pages, 14 figures

Photoemission spectra of the paramagnetic insulating (PI) phase of (V_0.972Cr_0.028)_2O_3, taken in ultra high vacuum up to the unusually high temperature (T) of 800 K, reveal a property unique to the Mott-Hubbard (MH) insulator and not observed previously. With increasing T the MH gap is filled by spectral weight transfer, in qualitative agreement with high-T theoretical calculations combining dynamical mean field theory and band theory in the local density approximation., Comment: 4 pages, 4 figures

Angle resolved photoemission spectroscopy line shapes measured for quasi-one-dimensional Li$_{0.9}$Mo$_6$O$_{17}$ samples grown by a temperature gradient flux technique are found to show Luttinger liquid behavior, consistent with all previous data by us and other workers obtained from samples grown by the electrolyte reduction technique. This result eliminates the sample growth method as a possible origin of considerable differences in photoemission data reported in previous studies of Li$_{0.9}$Mo$_6$O$_{17}$., Comment: Some text added

We establish the quasi-one-dimensional Li purple bronze as a photoemission paradigm of Luttinger liquid behavior. We also show that generalized signatures of electron fractionalization are present in the angle resolved photoemission spectra for quasi-two-dimensional purple bronzes and certain cuprates. An important component of our analysis for the quasi-two-dimensional systems is the proposal of a ``melted holon'' scenario for the k-independent background that accompanies but does not interact with the peaks that disperse to define the Fermi surface., Comment: 7 pages, 8 figures

We present the first observation of a prominent quasi-particle peak in the photoemission spectrum of the metallic phase of V_2O_3 and report new spectral calculations that combine the local density approximation with the dynamical mean-field theory (using quantum Monte Carlo simulations) to show the development of such a distinct peak with decreasing temperature. The experimental peak width and weight are significantly larger than in the theory., Comment: 4 pages, 3 figures, supercedes cond-mat/0108044

The elucidation of Landau Fermi liquid quasi-particles and their absence in strongly correlated electron systems lies at the heart of modern research on the quantum mechanics of electrons in condensed matter. Photoemission spectroscopy of the single particle spectral function is a central experimental tool for such studies. A general paradigm of quasi-particle formation is the Fermi level resonance associated with the Kondo physics of the Anderson impurity model, an effective self consisent version of which is utilized in dynamic mean field theories of general lattice systems which may or may not literally display Kondo physics. A general paradigm of quasi-particle absence is the Luttinger liquid physics of the Tomonaga-Luttinger model. This paper presents an overview of the theoretical ideas and shows examples in photoemission spectra, taken from the work of the author and his collaborators, of quasi-particle formation in impurity and lattice Kondo and non-Kondo correlated electron systems, contrasted with quasi-particle absence in a quasi-one-dimensional system., Comment: 28 pages, 9 figures, APS Frank Isakson Prize paper

auto-ignore This paper has been withdrawn by the authors because its results have been superceded by new experimental data and new theory presented in S.-K. Mo et al., cond-mat/0212110., Comment: Superceded by cond-mat/0212110

Complementary angle-resolved photoemission and bulk-sensitive k-resolved resonant inelastic x-ray scattering of divalent hexaborides reveal a >1 eV X-point gap between the valence and conduction bands, in contradiction to the band overlap assumed in several models of their novel ferromagnetism. This semiconducting gap implies that carriers detected in transport measurements arise from defects, and the measured location of the bulk Fermi level at the bottom of the conduction band implicates boron vacancies as the origin of the excess electrons. The measured band structure and X-point gap in CaB_6 additionally provide a stringent test case for proper inclusion of many-body effects in quasi-particle band calculations., Comment: 4 pages, 3 figures; new RIXS analysis; accepted for publication in PRL

Boron K-edge soft x-ray emission and absorption are used to address the fundamental question of whether divalent hexaborides are intrinsic semimetals or defect-doped bandgap insulators. These bulk sensitive measurements, complementary and consistent with surface-sensitive angle-resolved photoemission experiments, confirm the existence of a bulk band gap and the location of the chemical potential at the bottom of the conduction band., Comment: 5 pages, 2 figures, submitted to VUV-13

A dramatic temperature dependent enhancement of U 5f spectral weight at $E_F$ is observed in angle-resolved photoemission measurements of $URu_2Si_2$ at the center of an X-point hole-pocket. Comparison of this temperature dependent behavior for excitation both at and below the U $5d \to 5f$ resonant threshold is presented., Comment: 4 pages, 1 figure, submitted to SCES'01, figure font corrected

Bulk-sensitive high-resolution Ce 4f spectra have been obtained from 3d $\to$ 4f resonance photoemission measurements on La$_{1-x}$Ce$_x$Al$_2$ and La$_{1-x}$Ce$_x$Ru$_2$ for $x = 0.0, 0.04, 1.0$. The 4f spectra of low-Kondo-temperature ($T_{K}$) (La,Ce)Al$_2$ are essentially identical except for a slight increase of the Kondo peak with $x$, which is consistent with a known increase of $T_{K}$ with $x$. In contrast, the 4f spectra of high-$T_{K}$ (La,Ce)Ru$_2$ show a Kondo-like peak and also a 0.5 eV structure which increases strongly with $x$. The resonance photon-energy dependences of the two contributions are different and the origin of the 0.5 eV structure is still uncertain., Comment: submitted to SCES 2001, two-columnn format, modified text

In contrast to our recent finding of an X-point band gap in divalent hexaborides, we report here that angle resolved photoemission spectroscopy (ARPES) data shows that the gap is absent for trivalent LaB$_6$ and is absent or nearly so for mixed valent SmB$_6$. This finding demonstrates a nontrivial evolution of the band structure from divalent to trivalent hexaborides., Comment: submitted to SCES '01

Quasi-low-dimensional (quasi-low-D) inorganic materials are not only ideally suited for angle resolved photoemission spectroscopy (ARPES) but also they offer a rich ground for studying key concepts for the emerging paradigm of non-Fermi liquid (non-FL) physics. In this article, we discuss the ARPES technique applied to three quasi-low-D inorganic metals: a paradigm Fermi liquid (FL) material TiTe$_{2}$, a well-known quasi-1D charge density wave (CDW) material K$_{0.3}$MoO$_{3}$ and a quasi-1D non-CDW material Li$_{0.9}$Mo$_{6}$O$_{17}$. With TiTe$_2$, we establish that a many body theoretical interpretation of the ARPES line shape is possible. We also address the fundamental question of how to accurately determine the {\bf k}$_F$ value from ARPES. Both K$_{0.3}$MoO$_{3}$ and Li$_{0.9}$Mo$_{6}$O$_{17}$ show quasi-1D electronic structures with non-FL line shapes. A CDW gap opening is observed for K$_{0.3}$MoO$_{3}$, whereas no gap is observed for Li$_{0.9}$Mo$_{6}$O$_{17}$. We show, however, that the standard CDW theory, even with strong fluctuations, is not sufficient to describe the non-FL line shapes of K$_{0.3}$MoO$_{3}$. We argue that a Luttinger liquid (LL) model is relevant for both bronzes, but also point out difficulties encountered in comparing data with theory. We interpret this situation to mean that a more complete and realistic theory is necessary to understand these data., Comment: 23 pages, including 21 figures; to appear in a special issue of J. Elec. Spectr. Rel. Phenom

This paper has been withdrawn by the authors due to new theoretical evidence and experimental proof that the semiconducting bandgap reported in this paper and ascribed to a surface region is in fact a bulk property of divalent hexaborides. As reported in J. D. Denlinger et al., cond-mat/0107429, which supercedes this paper, bulk-sensitive boron K-edge soft x-ray emission provides a complementary confirmation of the X-point band gap identified by angle-resolved photoemission., Comment: This paper is withdrawn and has been superceded by cond-mat/0107429, showing the band gap to be a bulk property

A recent letter by Xue et al. (PRL v.83, 1235 ('99)) reports a Fermi-Liquid (FL) angle resolved photoemission (ARPES) lineshape for quasi one-dimensional Li0.9Mo6O17, contradicting our report (PRL v.82, 2540 ('99)) of a non-FL lineshape in this material. Xue et al. attributed the difference to the improved angle resolution. In this comment, we point out that this reasoning is flawed. Rather, we find that their data have fundamental differences from other ARPES results and also band theory., Comment: To be published as a PRL Comment

We report the detailed non-Fermi liquid (NFL) lineshape of the dispersing excitation which defines the Fermi surface (FS) for quasi-one-dimensional Li_{0.9}Mo_{6}O_{17}. The properties of Li_{0.9}Mo_{6}O_{17} strongly suggest that the NFL behavior has a purely electronic origin. Relative to the theoretical Luttinger liquid lineshape, we identify significant similarities, but also important differences., Comment: 5 pages, 3 eps figures