arXiv subjects

G. A. Sawatzky

Publications and source records attributed to G. A. Sawatzky.

At least 73 records · Page 4Linked to original sources

arXiv2007

High multipole transitions in NIXS: valence and hybridization in 4f systems

Momentum-transfer (q) dependent non-resonant inelastic x-ray scattering measurements were made at the N4,5 edges for several rare earth compounds. With increasing q, giant dipole resonances diminish, to be replaced by strong multiplet lines at lower energy transfer. These multiplets result from two different orders of multipole scattering and are distinct for systems with simple 4f^0 and 4f^1 initial states. A many-body theoretical treatment of the multiplets agrees well with the experimental data on ionic La and Ce phosphate reference compounds. Comparing measurements on CeO2 and CeRh3 to the theory and the phosphates indicates sensitivity to hybridization as observed by a broadening of 4f^0-related multiplet features. We expect such strong, nondipole features to be generic for NIXS from f-electron systems.

cond-mat.str-el↗

arXiv2007

Anisotropies in insulating La$_{2-x}$Sr$_x$CuO$_4$: angular resolved photoemission and optical absorption

Due to the orthorhombic distortion of the lattice, the electronic hopping integrals along the $a$ and $b$ diagonals, the orthorhombic directions, are slightly different. We calculate their difference in the LDA and find $t_{a}^{\prime}-t_{b}^{\prime}\approx 8 $meV. We argue that electron correlations in the insulating phase of La$_{2-x}$Sr$_{x}$CuO$_{4}$, i. e. at doping $x\leq 0.055,$ dramatically enhance the $(t_{a}^{\prime}-t_{b}^{\prime}) $-splitting between the $a$- and $b$-hole valleys. In particular, we predict that the intensity of both angle-resolved photoemission and of optical absorption is very different for the $a$ and $b$ nodal points.

cond-mat.str-el↗

arXiv2007

Cu $K$-edge Resonant Inelastic X-Ray Scattering in Edge-Sharing Cuprates

We present calculations for resonant inelastic x-ray scattering (RIXS) in edge-shared copper oxide systems, such as CuGeO$_{3}$ and Li$_{2}$CuO$_{2}$, appropriate for hard x-ray scattering where the photoexcited electron lies above oxygen 2p and copper 3d orbital energies. We perform exact diagonalizations of the multi-band Hubbard and determine the energies, orbital character and resonance profiles of excitations which can be probed via RIXS. We find excellent agreement with recent results on Li$_{2}$CuO$_{2}$ and CuGeO$_{3}$ in the 2-7 eV photon energy loss range.

cond-mat.str-el↗

arXiv2007

Non-resonant inelastic x-ray scattering involving excitonic excitations

In a recent publication Larson \textit{et al.} reported remarkably clear $d$-$d$ excitations for NiO and CoO measured with x-ray energies well below the transition metal $K$ edge. In this letter we demonstrate that we can obtain an accurate quantitative description based on a local many body approach. We find that the magnitude of $\vec{q}$ can be tuned for maximum sensitivity for dipole, quadrupole, etc. excitations. We also find that the direction of $\vec{q}$ with respect to the crystal axes can be used as an equivalent to polarization similar to electron energy loss spectroscopy, allowing for a determination of the local symmetry of the initial and final state based on selection rules. This method is more generally applicable and combined with the high resolution available, could be a powerful tool for the study of local distortions and symmetries in transition metal compounds including also buried interfaces.

cond-mat.str-el↗

arXiv2007

Metal to insulator transition in manganites - optical conductivity changes up to 24 eV

The electronic response of doped manganites at the transition from the paramagnetic insulating to the ferromagnetic metallic state in $\rm La_{1-x}Ca_{x}MnO_3$ for $\rm (x=0.3,0.2)$ was investigated by dc conductivity, ellipsometry, and VUV reflectance for energies between 0 and 24 eV. A stablized Kramers-Kronig transformation yields the optical conductivity and reveals changes in the optical spectral weight up to 24 eV at the metal to insulator transition. In the observed energy range, the spectral weight is conserved within $\rm 0.3 %$. The redistribution of spectral weight between low and high energies has important ramifications for the down-folding of low-energy Hamiltonians. We discuss the importance of the charge-transfer, Coulomb onsite, Jahn-Teller, and screening effects to the electronic structure.

cond-mat.str-el↗

arXiv2006

Interface hole-doping in cuprate-titanate superlattices

The electronic structure of interfaces between YBa$_2$Cu$_3$O$_6$ and SrTiO$_3$ is studied using local spin density approximation (LSDA) with intra-atomic Coulomb repulsion (LSDA+U). We find a metallic state in cuprate/titanate heterostructures with the hole carriers concentrated substantially in the CuO$_2$-layers and in the first interface TiO$_2$ and SrO planes. This effective interface doping appears due to the polarity of interfaces, caused by the first incomplete copper oxide unit cell. Interface-induced high pre-doping of CuO$_2$-layers is a key mechanism controlling the superconducting properties in engineered field-effect devices realized on the basis of cuprate/titanate superlattices.

cond-mat.str-el↗

arXiv2006

Strain amplification of the 4k$_F$ chain charge instability in Sr$_{14}$Cu$_{24}$O$_{41}$

We have used resonant soft x-ray scattering (RSXS) to study the misfit strain in Sr$_{14}$Cu$_{24}$O$_{41}$ (SCO), a cuprate that contains both doped spin ladders and spin chains, as well as a "control" sample without holes, La$_{6}$Ca$_{8}$Cu$_{24}$O$_{41}$ (LCCO). The misfit strain wave in SCO is strongly temperature (T)-dependent and is accompanied by a substantial hole modulation. In LCCO the strain wave is weaker, shows no hole modulation, and is T-independent. The observed strain wave vector, $L_c=0.318$, is close to the 4k$_F$ instability of the chain. Our results indicate that the chain charge order observed in SCO by several groups is a 4k$_F$ charge density wave (CDW) amplified by the misfit strain in this material. This demonstrates a new mechanism for CDW formation in condensed matter and resolves several contraversies over the transport properties of SCO.

cond-mat.str-el↗

arXiv2006

Comment on " Low-Lying Quasiparticle States and Hidden Collective Charge Instabilities in Parent Cobaltate Superconductors"

Qian et al [1] recently reported angular-resolved photoemission spectroscopy (ARPES) measurements for Na0.8CoO2 that show two concentric Fermi surfaces (FS) split by a delta k_F that varies by a factor of three around the Brillouin zone (BZ). The surfaces occupy 70+/-5% of the full 2D BZ and were interpreted as the bonding and antibonding splitting (BAS) of the a1g bands, with an unspecified effect of magnetic ordering. Below we show that this interpretation is not possible, and, in fact, no valid intepretation of the observed spectra in terms of the bulk electronic structure of Na0.8CoO2 can be found.

cond-mat.mtrl-sci↗

arXiv2006

Nitrogen based magnetic semiconductors

We describe a possible pathway to new magnetic materials with no conventional magnetic elements present. The substitution of Nitrogen for Oxygen in simple non magnetic oxides leads to holes in N 2$p$ states which form local magnetic moments. Because of the very large Hund's rule coupling of Nitrogen and O 2$p$ electrons and the rather extended spatial extend of the wave functions these materials are predicted to be ferromagnetic metals or small band gap insulators. Experimental studies support the theoretical calculations with regard to the basic electronic structure and the formation of local magnetic moments. It remains to be seen if these materials are magnetically ordered and if so below what temperature.

cond-mat.str-el↗

arXiv2006

Polarization dependence of x-ray absorption spectra in Na_xCoO_2

In order to shed light on the electronic structure of Na_xCoO_2, and motivated by recent Co L-edge X-ray absorption spectra (XAS) experiments with polarized light, we calculate the electronic spectrum of a CoO_6 cluster including all interactions between 3d orbitals. We obtain the ground state for two electronic occupations in the cluster that correspond nominally to all O in the O^{-2} oxidation state, and Co^{+3} or Co^{+4}. Then, all excited states obtained by promotion of a Co 2p electron to a 3d electron, and the corresponding matrix elements are calculated. A fit of the observed experimental spectra is good and points out a large Co-O covalency and cubic crystal field effects, that result in low spin Co 3d configurations. Our results indicate that the effective hopping between different Co atoms plays a major role in determining the symmetry of the ground state in the lattice. Remaining quantitative discrepancies with the XAS experiments are expected to come from composition effects of itineracy in the ground and excited states.

cond-mat.str-el↗

arXiv2006

Experimental evidence of paired hole states in model high-$T_c$ compounds

The distribution of holes in Sr$_{14-x}$Ca$_x$Cu$_{24}$O$_{41}$ (SCCO) is revisited with semi-emperical reanalysis of the x-ray absorption (XAS) data and exact-diagonalized cluster calculations. A new interpretation of the XAS data leads to much larger ladder hole densities than previously suggested. These new hole densities lead to a simple interpretation of the hole crystal (HC) recently reported with 1/3 and 1/5 wave vectors along the ladder. Our interpretation is consistent with paired holes in the rung of the ladders. Exact diagonalization results for a minimal model of the doped ladders suggest that the stabilization of spin structures consisting of 4 spins in a square plaquette as a result of resonance valence bond (RVB) physics suppresses the hole crystal with a 1/4 wave vector.

cond-mat.str-el↗

arXiv2006

Spectral Properties of Holstein and Breathing Polarons

We calculate the spectral properties of the one-dimensional Holstein and breathing polarons using the self-consistent Born approximation. The Holstein model electron-phonon coupling is momentum independent while the breathing coupling increases monotonically with the phonon momentum. We find that for a linear or tight binding electron dispersion: i) for the same value of the dimensionless coupling the quasiparticle renormalization at small momentum in the breathing polaron is much smaller, ii) the quasiparticle renormalization at small momentum in the breathing polaron increases with phonon frequency unlike in the Holstein model where it decreases, iii) in the Holstein model the quasiparticle dispersion displays a kink and a small gap at an excitation energy equal to the phonon frequency w0 while in the breathing model it displays two gaps, one at excitation energy w0 and another one at 2w0. These differences have two reasons: first, the momentum of the relevant scattered phonons increases with increasing polaron momentum and second, the breathing bare coupling is an increasing function of the phonon momentum. These result in an effective electron-phonon coupling for the breathing model which is an increasing function of the total polaron momentum, such that the small momentum polaron is in the weak coupling regime while the large momentum one is in the strong coupling regime. However the first reason does not hold if the free electron dispersion has low energy states separated by large momentum, as in a higher dimensional system for example, in which situation the difference between the two models becomes less significant.

cond-mat.str-el↗

arXiv2005

Quantum melting of the hole crystal in the spin ladder of Sr14-xCaxCu24O41

The "spin ladder" is a reduced-dimensional analogue of the high temperature superconductors that was predicted to exhibit both superconductivity and an electronic charge density wave or "hole crystal" (HC). Both phenomena have been observed in the doped spin ladder system Sr14-xCaxCu24O41 (SCCO), which at x=0 exhibits a HC which is commensurate at all temperatures. To investigate the effects of discommensuration we used resonant soft x-ray scattering (RSXS) to study SCCO as a function of doped hole density, d. The HC forms only with the commensurate wave vectors L_L = 1/5 and L_L = 1/3 and exhibits a simple temperature scaling T_(1/3) / T_(1/5) = 5/3. For irrational wave vectors the HC "melts", perhaps through the motion of topological defects carrying fractional charge.

cond-mat.str-el↗

arXiv2005

Spatially modulated "Mottness" in La2-xBaxCuO4

Stripe phases were predicted to arise in doped antiferromagnets through competition between magnetism and the kinetic energy of mobile carriers (typically holes). In copper-oxides the main experimental evidence for stripes is neutron scattering from La1.48Nd0.4Sr0.12CuO4 (LNSCO) and La1.875Ba0.125CuO4 (LBCO) which reveals coexisting static spin and charge order whose wavelengths differ by a factor of two, reminiscent of charged rivers separating regions of oppositely-phased antiferromagnetism. A neutron is an electrically neutral object, however, so does not detect charge but rather its associated lattice distortion ; it is not known if the "stripe" phase in LNSCO and LBCO actually involves ordering of the doped holes. Here we present a study of the charge order in LBCO with resonant soft x-ray scattering (RSXS). We observe giant resonances at both the mobile carrier and upper-Hubbard band features in the OK edge. These demonstrate a substantial modulation in the doped hole density as well as the amount of spectral weight near the correlated gap, i.e. the degree of "Mottness". The peak-to-trough amplitude of the valence modulation is estimated to be 0.063 holes, which if interpreted with a model of the stripe form factor suggests an integrated area of 0.59 holes under a single stripe. While only an estimate, this number agrees with what is expected for half-filled stripes.

cond-mat.str-el↗

arXiv2005

Spectroscopy of stripe order in La1.8Sr0.2NiO4 using resonant soft x-ray diffraction

Strong resonant enhancements of the charge-order and spin-order superstructure-diffraction intensities in La1.8Sr0.2NiO4 are observed when x-ray energies in the vicinity of the Ni L2,3 absorption edges are used. The pronounced photon-energy and polarization dependences of these diffraction intensities allow for a critical determination of the local symmetry of the ordered spin and charge carriers. We found that not only the antiferromagnetic order but also the charge-order superstructure resides within the NiO2 layers; the holes are mainly located on in-plane oxygens surrounding a Ni2+ site with the spins coupled antiparallel in close analogy to Zhang-Rice singlets in the cuprates.

cond-mat.str-el↗

arXiv2005

Hole crystallization in the spin ladder of Sr14Cu24O41

One of the deepest questions in condensed matter physics concerns what other phases compete with superconductivity in high-transition-temperature (high-Tc) superconductors. One candidate is the "stripe" phase, in which the carriers (holes) condense into rivers of charge separating regions of antiferromagnetism. A related but lesser known system is the "spin ladder", which consists of two coupled chains of magnetic ions forming an array of rungs. A doped ladder can be thought of as a high-Tc material with lower dimensionality, and has been predicted to exhibit both superconductivity and an insulating "hole crystal" phase in which the carriers are localised through many-body interactions. The competition between the two resembles that between static stripes and superconductivity in high-Tc materials. Here we report evidence, from resonant x-ray scattering, for the existence of a hole crystal in the doped spin ladder of Sr14Cu24O41. This phase exists without a detectable distortion in the structural lattice, indicating it arises from many-body effects. Our measurements confirm theoretical predictions and support the picture that proximity to charge ordered states is a general property of superconductivity in copper-oxides.

cond-mat.str-el↗

arXiv2004

Physics of cuprates with the two-band Hubbard model - The validity of the one-band Hubbard model

We calculate the properties of the two-band Hubbard model using the Dynamical Cluster Approximation. The phase diagram resembles the generic phase diagram of the cuprates, showing a strong asymmetry with respect to electron and hole doped regimes, in agreement with experiment. Asymmetric features are also seen in one-particle spectral functions and in the charge, spin and d-wave pairing susceptibility functions. We address the possible reduction of the two-band model to a low-energy single-band one, as it was suggested by Zhang and Rice. Comparing the two-band Hubbard model properties with the single-band Hubbard model ones, we have found similar low-energy physics provided that the next-nearest-neighbor hopping term t' has a significant value ($t'/t \approx 0.3$). The parameter t' is the main culprit for the electron-hole asymmetry. However, a significant value of t' cannot be provided in a strict Zhang and Rice picture where the extra holes added into the system bind to the existing Cu holes forming local singlets. We notice that by considering approximate singlet states, such as plaquette ones, reasonable values of t', which capture qualitatively the physics of the two-band model can be obtained. We conclude that a single-band t-t'-U Hubbard model captures the basic physics of the cuprates concerning superconductivity, antiferromagnetism, pseudogap and electron-hole asymmetry, but is not suitable for a quantitative analysis or to describe physical properties involving energy scales larger than about 0.5 eV.

cond-mat.str-el↗

arXiv2004

Zooming-in on the charge ordering in YBa2Cu3O6.5

We report direct evidence of charge/orbital ordering of low energy electronic states of $Cu$ in YBa$_2$Cu$_3$O$_{6+x}$ ortho-II phase in both the $CuO_3$ chain and the CuO$_2$ plane. Huge enhancement of the $({1/2},0,0)$ superstructure Bragg peak is observed when photon energy is tuned to the $Cu L_{2,3}$ absorption edge with large polarization dependence. The ordering in the $CuO_2$ plane discovered here sheds new light on how the one dimensional $Cu-O$ chains affect the $CuO_2$ plane, and why many normal and superconducting state properties of this system exhibit strong anisotropy.

cond-mat.supr-con↗