arXiv subjects

G. A. Sawatzky

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

At least 37 records · Page 2Linked to original sources

arXiv2013

Electronic superlattice revealed by resonant scattering from random impurities in Sr3Ru2O7

Resonant elastic x-ray scattering (REXS) is an exquisite element-sensitive tool for the study of subtle charge, orbital, and spin superlattice orders driven by the valence electrons, which therefore escape detection in conventional x-ray diffraction (XRD). Although the power of REXS has been demonstrated by numerous studies of complex oxides performed in the soft x-ray regime, the cross section and photon wavelength of the material-specific elemental absorption edges ultimately set the limit to the smallest superlattice amplitude and periodicity one can probe. Here we show -- with simulations and REXS on Mn-substituted Sr$_3$Ru$_2$O$_7$ -- that these limitations can be overcome by performing resonant scattering experiments at the absorption edge of a suitably-chosen, dilute impurity. This establishes that -- in analogy with impurity-based methods used in electron-spin-resonance, nuclear-magnetic resonance, and Mössbauer spectroscopy -- randomly distributed impurities can serve as a non-invasive, but now momentum-dependent probe, greatly extending the applicability of resonant x-ray scattering techniques.

cond-mat.str-el↗

arXiv2013

Surface-enhanced charge-density-wave instability in underdoped Bi2201

Neutron and x-ray scattering experiments have provided mounting evidence for spin and charge ordering phenomena in underdoped cuprates. These range from early work on stripe correlations in Nd-LSCO to the latest discovery of charge-density-waves in YBCO. Both phenomena are characterized by a pronounced dependence on doping, temperature, and an externally applied magnetic field. Here we show that these electron-lattice instabilities exhibit also a previously unrecognized bulk-surface dichotomy. Surface-sensitive electronic and structural probes uncover a temperature-dependent evolution of the CuO2 plane band dispersion and apparent Fermi pockets in underdoped Bi2201, which is directly associated with an hitherto-undetected strong temperature dependence of the incommensurate superstructure periodicity below 130K. In stark contrast, the structural modulation revealed by bulk-sensitive probes is temperature independent. These findings point to a surface-enhanced incipient charge-density-wave instability, driven by Fermi surface nesting. This discovery is of critical importance in the interpretation of single-particle spectroscopy data and establishes the surface of cuprates and other complex oxides as a rich playground for the study of electronically soft phases.

cond-mat.supr-con↗

arXiv2012

Distinct Charge Orders in the Planes and Chains of Ortho-III-Ordered YBa$_2$Cu$_3$O$_{6+δ}$ Superconductors Identified by Resonant Elastic X-ray Scattering

Recently, charge density wave (CDW) order in the CuO$_2$ planes of underdoped YBa$_2$Cu$_3$O$_{6+δ}$ was detected using resonant soft x-ray scattering. An important question remains: is the chain layer responsible for this charge ordering? Here, we explore the energy and polarization dependence of the resonant scattering intensity in a detwinned sample of YBa$_2$Cu$_3$O$_{6.75}$ with ortho-III oxygen ordering in the chain layer. We show that the ortho-III CDW order in the chains is distinct from the CDW order in the planes. The ortho-III structure gives rise to a commensurate superlattice reflection at $Q$=[0.33 0 $L$] whose energy and polarization dependence agrees with expectations for oxygen ordering and a spatial modulation of the Cu valence in the chains. Incommensurate peaks at [0.30 0 $L$] and [0 0.30 $L$] from the CDW order in the planes are shown to be distinct in $Q$ as well as their temperature, energy, and polarization dependence, and are thus unrelated to the structure of the chain layer. Moreover, the energy dependence of the CDW order in the planes is shown to result from a spatial modulation of energies of the Cu 2$p$ to 3$d_{x^2-y^2}$ transition, similar to stripe-ordered 214 cuprates.

cond-mat.supr-con↗

arXiv2012

Observation of charge accumulation and onsite Coulomb repulsion at transition metal impurities in the iron pnictides

We report a combined valence band photoemission and Auger spectroscopy study of single crystalline Ca(Fe,Co)2As2 and Ba(Fe,TM)2As2 with TM=Ni or Cu. The valence band photoemission data show directly that the TM-states move to higher binding energies with increasing atomic number, contributing less and less to the states close to the Fermi level. Furthermore, the 3d8 final state of the LVV Auger decay, which is observed for Ni and Cu, unambiguously reveals the accumulation of charge at these impurities. We also show that the onsite Coulomb interaction on the impurity strongly increases when moving from Co over Ni to Cu. Our results quantify the impurity potentials and imply that the superconducting state is robust against impurity scattering.

cond-mat.supr-con↗

arXiv2012

Oxygen vacancies at titanate interfaces: two-dimensional magnetism and orbital reconstruction

We show that oxygen vacancies at titanate interfaces induce a complex multiorbital reconstruction which involves a lowering of the local symmetry and an inversion of t2g and eg orbitals resulting in the occupation of the eg orbitals of Ti atoms neighboring the O vacancy. The orbital reconstruction depends strongly on the clustering of O vacancies and can be accompanied by a magnetic splitting between the local eg orbitals with lobes directed towards the vacancy and interface dxy orbitals. The reconstruction generates a two-dimensional interface magnetic state not observed in bulk SrTiO3. Using generalized gradient approximation (LSDA) with intra-atomic Coulomb repulsion (GGA+U), we find that this magnetic state is common for titanate surfaces and interfaces.

cond-mat.str-el↗

arXiv2012

Long-range incommensurate charge fluctuations in (Y,Nd)Ba2Cu3O(6+x)

There are increasing indications that superconductivity competes with other orders in cuprate superconductors, but obtaining direct evidence with bulk-sensitive probes is challenging. We have used resonant soft x-ray scattering to identify two-dimensional charge fluctuations with an incommensurate periodicity of $\bf \sim 3.2$ lattice units in the copper-oxide planes of the superconductors (Y,Nd)Ba$_2$Cu$_3$O$_{6+x}$ with hole concentrations $0.09 \leq p \leq 0.13$ per planar Cu ion. The intensity and correlation length of the fluctuation signal increase strongly upon cooling down to the superconducting transition temperature, $T_c$; further cooling below $T_c$ abruptly reverses the divergence of the charge correlations. In combination with prior observations of a large gap in the spin excitation spectrum, these data indicate an incipient charge-density-wave instability that competes with superconductivity.

cond-mat.str-el↗

arXiv2012

Mott versus Slater-type metal-insulator transition in Mn-substituted Sr3Ru2O7

We present a temperature-dependent x-ray absorption (XAS) and resonant elastic x-ray scattering (REXS) study of the metal-insulator transition (MIT) in Sr3(Ru1-xMnx)2O7. The XAS results reveal that the MIT drives the onset of local antiferromagnetic correlations around the Mn impurities, a precursor of the long-range antiferromagnetism detected by REXS at T_order<T_MIT. This establishes that the MIT is of the Mott-type (electronic correlations) as opposed to Slater-type (magnetic order). While this behavior is induced by Mn impurities, the (1/4,1/4,0) order exists for a wide range of Mn concentrations, and points to an inherent instability of the parent compound.

cond-mat.str-el↗

arXiv2012

Probing the role of Co substitution in the electronic structure of iron-pnictides

The role of Co substitution in the low-energy electronic structure of Ca(Fe$_{0.944}$Co$_{0.056}$)$_2$As$_2$ is investigated by resonant photoemission spectroscopy and density functional theory. The Co 3d-state center-of-mass is observed at 250 meV higher binding energy than Fe's, indicating that Co posses one extra valence electron, and that Fe and Co are in the same 2+ oxidation state. Yet, significant Co character is detected for the Bloch wavefunctions at the chemical potential, revealing that the Co 3d electrons are part of the Fermi sea determining the Fermi surface. This establishes the complex role of Co substitution in CaFe2As2, and the inadequacy of a rigid-band shift description.

cond-mat.supr-con↗

arXiv2012

Magnetism and superconductivity at LAO/STO-interfaces: the role of Ti 3d interface electrons

Ferromagnetism and superconductivity are in most cases adverse. However, recent experiments reveal that they coexist at interfaces of LaAlO3 and SrTiO3. We analyze the magnetic state within density functional theory and provide evidence that magnetism is not an intrinsic property of the two-dimensional electron liquid at the interface. We demonstrate that the robust ferromagnetic state is induced by the oxygen vacancies in SrTiO3- or in the LaAlO3-layer. This allows for the notion that areas with increased density of oxygen vacancies produce ferromagnetic puddles and account for the previous observation of a superparamagnetic behavior in the superconducting state.

cond-mat.str-el↗

arXiv2012

Utility of the inverse partial fluorescence for electronic structure studies of battery materials

X-ray absorption spectroscopy (XAS) is one of the most widely used experimental techniques to study the electronic and spatial structure of materials. Fluorescence yield mode is bulk-sensitive, but has several serious problems coming from saturation effects. In this study, we show the usefulness of partial fluorescence yields in addressing these problems. We discuss the different behaviors of La2NiMnO6 and LiMnO2 at the Mn 2p absorption edges. The total fluorescence yield produces misleading spectra for LiMnO2 due to the absence of high-Z (Z: atomic number) elements. We conclude that the measurement of the inverse partial fluorescence yield is essential in studies of LiMnO2, which is a hotly debated Li-ion battery material.

cond-mat.mtrl-sci↗

arXiv2011

Electronic phase transitions in Pr$_{0.5}$Ca$_{0.5}$MnO$_3$ epitaxial thin films revealed by resonant soft x-ray scattering

We report the study of magnetic and orbital order in Pr$_{0.5}$Ca$_{0.5}$MnO$_3$ epitaxial thin films grown on (LaAlO$_3$)$_{0.3}$-(SrAl$_{0.5}$Ta$_{0.5}$O$_3$)$_{0.7}$ (LSAT) (011)$_c$. In a new experimental approach, the polarization and energy dependence of resonant soft x-ray scattering are used to reveal significant modifications of the magnetic order in the film as compared to the bulk, namely (i) a different magnetic ordering wave vector, (ii) a different magnetic easy axis and (iii) an additional magnetic reordering transition at low temperatures. These observations indicate a strong impact of the epitaxial strain on the spin order, which is mediated by the orbital degrees of freedom and which provides a promising route to tune the magnetic properties of manganite films. Our results further demonstrate that resonant soft x-ray scattering is a very suitable technique to study the magnetism in thin films, to which neutron scattering cannot easily be applied due to the small sample volume.

cond-mat.str-el↗

arXiv2011

Electronic structure and self energies of randomly substituted solids using density functional theory and model calculations

We describe procedures to obtain the electronic structure of disordered systems using either tight binding like models or quite directly from ab inito density functional band structure calculations. The band structure is calculated using super cells much larger than those containing a single minority component atom. We average over a large number of different super cell calculations containing different randomly positioned minority component atoms in the super cell as well as a varying total number of minority component atoms, weighted by the statistical probability. We develop an efficient and simple algorithm for unfolding of these bands, based on Bloch's theorem. The unfolded band-structure obtained in this way exhibits momentum and energy broadened structures replacing the gaps observed in often used single super cell calculations. Using the super cell averaged band-structure one can introduce a self-energy, resulting from the scattering of randomly positioned alloy components. The self-energy is causal, and shows strong energy and some momentum dependence. The self-energy shows rather non-trivial behavior and is in general non-zero at the Fermi-energy, resulting in an ill or undefined Fermi surface. The real-part of the self-energy at the Fermi-energy relates to an apparent violation of Luttinger's theorem. There is no simple relation between the apparent Fermi-surface volume and the electron count. Examples introducing these effects both for model and real binary alloy systems are presented.

cond-mat.mtrl-sci↗

arXiv2011

Resonant elastic soft x-ray scattering in oxygen-ordered YBa_2Cu_3O_{6+delta}

Static charge-density wave (CDW) and spin-density wave (SDW) order has been convincingly observed in La-based cuprates for some time. However, more recently it has been suggested by quantum oscillation, transport and thermodynamic measurements that density wave order is generic to underdoped cuprates and plays a significant role in YBa_2Cu_3O_{6+delta} (YBCO). We use resonant soft x-ray scattering at the Cu L and O K edges to search for evidence of density wave order in Ortho-II and Ortho-VIII oxygen-ordered YBCO. We report a null result -- no evidence for static CDW order -- in both Ortho-II and Ortho-VIII ordered YBCO. While this does not rule out static CDW order in the CuO_2 planes of YBCO, these measurements place limits on the parameter space (temperature, magnetic field, scattering vector) in which static CDW order may exist. In addition, we present a detailed analysis of the energy and polarization dependence of the Ortho-II superstructure Bragg reflection [0.5 0 0] at the Cu L edge. The intensity of this peak, which is due to the valence modulations of Cu in the chain layer, is compared with calculations using atomic scattering form factors deduced from x-ray absorption measurements. The calculated energy and polarization dependence of the scattering intensity is shown to agree very well with the measurement, validating the approach and providing a framework for analyzing future resonant soft x-ray scattering measurements.

cond-mat.supr-con↗

arXiv2011

An in-vacuum diffractometer for resonant elastic soft x-ray scattering

We describe the design, construction and performance of a 4-circle in-vacuum diffractometer for resonant elastic soft x-ray scattering and reflectivity. The diffractometer, installed on the REIXS beamline at the Canadian Light Source, includes 9 in-vacuum motions driven by in-vacuum stepper motors and operates in ultra-high vacuum at base pressure of 2 x10^-10 Torr. Cooling to a base temperature of 18 K is provided with a closed-cycle cryostat. The diffractometer includes a choice of 3 photon detectors: a photodiode, a channeltron and a 2D sensitive channelplate detector. Along with variable slit and filter options, these detectors are suitable for studying a wide range of phenomena having both weak and strong diffraction signals. Example measurements of diffraction and reflectivity in Nd-doped (La,Sr)_2CuO_4 and thin film (Ga,Mn)As are shown.

cond-mat.str-el↗

arXiv2011

Magnetic Frustration in a Mn Honeycomb Lattice Induced by Mn-O-O-Mn Pathways

We investigated the electronic structure of layered Mn oxide Bi3Mn4O12(NO3) with a Mn honeycomb lattice by x-ray absorption spectroscopy. The valence of Mn was determined to be 4+ with a small charge-transfer energy. We estimated the values of superexchange interactions up to the fourth nearest neighbors (J1, J2, J3, and J4) by unrestricted Hartree-Fock calculations and a perturbation method. We found that the absolute values of J1 through J4 are similar with positive (antiferromagnetic) J1 and J4, and negative (ferromagnetic) J2 and J3, due to Mn-O-O-Mn pathways activated by the smallness of charge-transfer energy. The negative J3 provides magnetic frustration in the honeycomb lattice to prevent long-range ordering.

cond-mat.str-el↗

arXiv2010

The importance of inter-site coherences in the x-ray absorption spectra of mixed-valent systems

We study the importance of inter-site coherences and quantum interference effects in the x-ray absorption spectroscopy (XAS) of mixed-valent systems. We demonstrate its importance, first for a simple diatomic mixed-valent molecule to elucidate the physics involved, and finally for mixed-valent Ti oxides, using a model calculation including full spin and orbital multiplicities. Our calculations demonstrate the inefficacy of conventional approaches of describing the XAS from mixed-valent systems as incoherent combinations of XAS from the pure-valent end members, and that multiplets forbidden in the single-site approximation can be reached within a multi-site description. These conclusions play an important role in the interpretation of XAS and resonant x-ray scattering (RXS) in terms of the electronic structure of strongly correlated systems.

cond-mat.str-el↗

arXiv2010

Unraveling the Nature of Charge Excitations in La$_2$CuO$_4$ with Momentum-Resolved Cu $K$-edge Resonant Inelastic X-ray Scattering

Results of model calculations using exact diagonalization reveal the orbital character of states associated with different Raman loss peaks in Cu $K$-edge resonant inelastic X-ray scattering (RIXS) from La$_{2}$CuO$_{4}$. The model includes electronic orbitals necessary to highlight non-local Zhang-Rice singlet, charge transfer and $d$-$d$ excitations, as well as states with apical oxygen 2$p_z$ character. The dispersion of these excitations is discussed with prospects for resonant final state wave-function mapping. A good agreement with experiments emphasizes the substantial multi-orbital character of RIXS profiles in the energy transfer range 1-6 eV.

cond-mat.str-el↗

arXiv2010

Where Are the Extra d Electrons in Transition-Metal Substituted Fe Pnictides?

Transition-metal substitution in Fe pnictides leading to superconductivity is usually interpreted in terms of carrier doping to the system. We report on a density functional calculation of the local substitute electron density and demonstrate that substitutions like Co and Ni for Fe do not carrier dope but rather are isovalent to Fe. We find that the extra d electrons for Co and Ni are almost totally located within the muffin-tin sphere of the substituted site. We suggest that Co and Ni act more like random scatterers scrambling momentum space and washing out parts of the Fermi surface.

cond-mat.supr-con↗