arXiv subjects

H. Wadati

Publications and source records attributed to H. Wadati.

At least 37 records · Page 2Linked to original sources

arXiv2014

Electronic correlations and Hund's coupling effects in SrMoO$_3$ revealed by photoemission spectroscopy

We investigate the electronic structure of a perovskite-type Pauli paramagnet SrMoO3 (t2g2) thin film using hard x-ray photoemission spectroscopy and compare the results to the realistic calculations that combine the density functional theory within the local-density approximation (LDA) with the dynamical-mean field theory (DMFT). Despite the clear signature of electron correlations in the electronic specific heat, the narrowing of the quasiparticle bands is not observed in the photoemission spectrum. This is explained in terms of the characteristic effect of Hund's rule coupling for partially-filled t2g bands, which induces strong quasiparticle renormalization already for values of Hubbard interaction which are smaller than the bandwidth. The interpretation is supported by additional model DMFT calculations including Hund's rule coupling, that show renormalization of low-energy quasiparticles without affecting the overall bandwidth. The photoemission spectra show additional spectral weight around -2 eV that is not present in the LDA+DMFT. We interpret this weight as a plasmon satellite, which is supported by measured Mo, Sr and Oxygen core-hole spectra that all show satellites at this energy.

cond-mat.str-el↗

arXiv2013

Insulator-to-Superconductor Transition upon Electron Doping in a BiS$_{2}$-Based Superconductor Sr$_{1-x}$La$_{x}$FBiS$_{2}$

Effects of electron doping on the BiS$_2$-based superconductors Sr$_{1-x}$La$_x$FBiS$_2$ ($0\le x\le 0.6$) have been investigated using the systematically synthesized polycrystals. The pristine compound is a band insulator with the BiS$_2$ layer, which accommodates electron carriers through the La substitution for Sr, as evidenced by the change in x-ray absorption spectra reflecting the occupancy of Bi 6$p$ orbitals. With increasing the carrier density, the resistivity progressively decreases and a bad metallic state appears for $x\ge0.45$, where bulk superconductivity manifests itself below approximately 3 K. The value of $T_{\rm c}$ gradually increases with decreasing $x$ from 0.6 to 0.45 and immediately decreases down to zero at the critical concentration of $x\sim 0.4$, resulting in an insulator-superconductor transition highly sensitive to the carrier density. Thermodynamic measurements furthermore have revealed the possible enhancement of the superconducting coupling strength as the insulating phase is approached. The obtained superconducting phase diagram is markedly different from the broad dome-shaped superconducting phase previously reported for $R$O$_{1-x}$F$_x$BiS$_2$ ($R$: rare-earth ion), suggesting a strong influence of the blocking layer on the superconductivity. Instead all these features are similar to those observed in Li-intercalated ZrNCl superconductor, except for the critical electron concentration of as low as 6% in the latter compound. For the present superconductor, notably, the existence of hole-type carriers has been indicated in the normal state from the Hall effect measurements. The Sr$_{1-x}$La$_x$FBiS$_2$ system providing the phase diagram for the rigid-band doping in the BiS$_2$ layer would be another prototypical example of superconductivity derived from a doped layered band insulator, hosting both hole-like and electron-like Fermi surfaces.

cond-mat.supr-con↗

arXiv2013

Spectroscopic studies on the electronic and magnetic states of Co-doped perovskite manganite Pr0.8Ca0.2Mn1-yCoyO3 thin films

We have investigated the electronic and magnetic properties of Co-doped Pr0.8Ca0.2MnO3 thin films using various spectroscopic techniques. X-ray absorption and hard x-ray photoemission spectroscopy revealed that the substituted Co ions are in the divalent state, resulting in hole doping on the Mn atoms. Studies of element-selective magnetic properties by x-ray magnetic circular dichroism found a large orbital magnetic moment for the Co ions. These spectroscopic studies reveal that the substituted Co ions play several roles of hole doping for Mn, ferromagnetic superexchange coupling between the Co2+ and Mn4+ ions, and orbital magnetism of the Co2+ ions. Competition among these complex interactions produces the unique electronic and magnetic behaviors including enhanced coercivity of the Co-doped Pr0.8Ca0.2MnO3.

cond-mat.str-el↗

arXiv2013

Electronic structure of hole-doped delafossite oxides CuCr_{1-x}Mg_{x}O_{2}

We report the detailed electronic structure of a hole-doped delafossite oxide CuCr_{1-x}Mg_{x}O_{2} (0 <= x <= 0.03) studied by photoemission spectroscopy (PES), soft x-ray absorption spectroscopy (XAS), and band-structure calculations within the local-density approximation +U (LDA+U) scheme. Cr/Cu 3p-3d resonant PES reveals that the near-Fermi-level leading structure has primarily the Cr 3d character with a minor contribution from the Cu 3d through Cu 3d-O 2p-Cr 3d hybridization, having good agreement with the band-structure calculations. This indicates that a doped hole will have primarily the Cr 3d character. Cr 2p PES and L-edge XAS spectra exhibit typical Cr^{3+} features for all x, while the Cu L-edge XAS spectra exhibited a systematic change with x. This indicates now that the Cu valence is monovalent at x=0 and the doped hole should have Cu 3d character. Nevertheless, we surprisingly observed two types of charge-transfer satellites that should be attributed to Cu^{+} (3d^{10}) and Cu^{2+} (3d^{9}) like initial states in Cu 2p-3d resonant PES spectrum for at x=0, while Cu 2p PES spectra with no doubt shows the Cu^{+} character even for the lightly doped samples. We propose that these contradictory results can be understood by introducing no only the Cu 4s state, but also finite Cu 3d,4s-Cr 3d charge transfer via O 2p states in the ground-state electronic configuration.

cond-mat.str-el↗

arXiv2013

Phase competitions in epitaxial Pr$_{0.5}$Ca$_{0.5}$MnO$_3$/La$_{0.5}$Sr$_{0.5}$MnO$_3$ superlattices

We studied the charge-orbital ordering in the superlattice of charge-ordered insulating Pr$_{0.5}$Ca$_{0.5}$MnO$_3$ and ferromagnetic metallic La$_{0.5}$Sr$_{0.5}$MnO$_3$ by resonant soft x-ray diffraction. A temperature-dependent incommensurability is found in the orbital order. In addition, a large hysteresis is observed that is caused by phase competition between insulating charge ordered and metallic ferromagnetic states. No magnetic phase transitions are observed in contrast to bulk, confirming the unique character of the superlattice. The deviation from the commensurate orbital order can be directly related to the decrease of ordered-layer thickness that leads to a decoupling of the orbital-ordered planes along the c axis.

cond-mat.str-el↗

arXiv2012

Large spin-orbit splitting and weakly-anisotropic superconductivity revealed with single-crystalline noncentrosymmetric CaIrSi3

We report normal and superconducting properties of the Rashba-type noncentrosymmetric com- pound CaIrSi3, using single crystalline samples with nearly 100% superconducting volume fraction. The electronic density of states revealed by the hard x-ray photoemission spectroscopy can be well explained by the relativistic first-principle band calculation. This indicates that strong spin-orbit interaction indeed affects the electronic states of this compound. The obtained H - T phase diagram exhibits only approximately 10% anisotropy, indicating that the superconducting properties are almost three dimensional. Nevertheless, strongly anisotropic vortex pinning is observed.

cond-mat.supr-con↗

arXiv2012

Imprinting magnetic information in manganites with X-rays

The effect of x-rays on an orbital and charge ordered epitaxial film of a Pr$_{0.5}$Ca$_{0.5}$MnO$_{3}$ is presented. As the film is exposed to x-rays, the antiferromagnetic response increases and concomitantly the conductivity of the film improve. These results are discussed in terms of a persistent x-ray induced doping, leading to a modification of the magnetic structure. This effect allows writing electronic and magnetic domains in the film and represents a novel way of manipulating magnetism.

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

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

Origin of the large polarization in multiferroic YMnO$_3$ thin films revealed by soft and hard x-ray diffraction

We investigated the magnetic structure of an orthorhombic YMnO3 thin film by resonant soft x-ray and hard x-ray diffraction. We observed a temperature-dependent incommensurate magnetic reflection below 45 K and a commensurate lattice-distortion reflection below 35 K. These results demonstrate that the ground state is composed of coexisting E-type and cycloidal states. Their different ordering temperatures clarify the origin of the large polarization to be caused by the E-type antiferromagnetic states in the orthorhombic YMnO3 thin film.

cond-mat.str-el↗

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

Bulk sensitive x-ray absorption spectroscopy free of self-absorption effects

We demonstrate a new method of x-ray absorption spectroscopy (XAS) that is bulk sensitive, like traditional fluorescence yield measurements, but is not affected by self-absorption or saturation effects. This measure of XAS is achieved by scanning the incident photon energy through an absorption edge and using an energy sensitive photon detector to measure the partial fluorescence yield (PFY). The x-ray emission from any element or core-hole excitation that is not resonant with the absorption edge under investigation is selected from the PFY. It is found that the inverse of this PFY spectrum, which we term inverse partial fluorescence yield (IPFY), is linearly proportional to the x-ray absorption cross-section without any corrections due to saturation or self-absorption effects. We demonstrate this technique on the Cu L and Nd M absorption edges of the high-Tc cuprate LNSCO by measuring the O K PFY and comparing the total electron yield, total fluorescence yield and IPFY spectra.

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

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↗

arXiv2010

Valence evaluation of LiMnO2 and related battery materials by x-ray absorption spectroscopy

We present an x-ray absorption study of the oxidation states of transition-metal-ions of LiMnO2 and its related materials, widely used as cathodes in Li-ion batteries. The comparison between the obtained spectrum and the configuration-interaction cluster-model calculations showed that the Mn3+ in LiMnO2 is a mixture of the high-spin and low-spin states. We found that Li deficiencies occur in the case of Cr substitution, whereas there are no Li deficiencies in the case of Ni substitution. We conclude that the substitution of charge-transfer-type Ni or Cu is effective for LiMnO2 battery materials.

cond-mat.mtrl-sci↗

arXiv2009

Interface reconstruction in V-oxide heterostructures determined by x-ray absorption spectroscopy

We present an x-ray absorption study of the dependence of the V oxidation state on the thickness of LaVO$_3$ (LVO) and capping LaAlO$_3$ (LAO) layers in the multilayer structure of LVO sandwiched between LAO. We found that the change of the valence of V as a function of LAO layer thickness can be qualitatively explained by a transition between electronically reconstructed interfaces and a chemical reconstruction. The change as a function of LVO layer thickness is complicated by the presence of a considerable amount of V$^{4+}$ in the bulk of the thicker LVO layers.

cond-mat.str-el↗