arXiv subjects
Publications and source records attributed to G. A. Sawatzky.
A recent article suggested that the saturation of low energy spectral weight observed by X-ray absorption spectroscopy in the cuprates at high hole doping could be explained within the single-band Hubbard model. We show that this result is an artifact of inappropriate integration limits.
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.
We report nonresonant inelastic x-ray scattering from the semi-core 5d levels of several actinide compounds. Dipole-forbidden, high-multipole features form a rich bound-state spectrum dependent on valence electron configuration and spin-orbit and Coulomb interactions. Cross-material comparisons, together with the anomalously high Coulomb screening required for agreement between atomic multiplet theory and experiment, demonstrate sensitivity to the neighboring electronic environment, such as is needed to address long-standing questions of electronic localization and bonding in 5f compounds.
We develop the theory for shallow-core to valence excitations when the multiplet spread is larger than the core-hole attraction, e.g., if the core and valence orbitals have the same principal quantum number. This results in a cross-over from bound to virtual-bound excited states with increasing energy and in large differences between dipole and high-order multipole transitions, as observed in inelastic x-ray scattering. The theory is important to obtain ground state information from x-ray spectroscopies of strongly correlated transition metal, rare-earth and actinide systems.
Density functional theory applied to a simple ionic material, MgO, is used as a model system to clarify several aspects of electronic driven mechanism to compensate for the diverging electrostatic potential in the polar structures. We demonstrate that in the stoichiometric free standing films, the electronic reconstruction is limited by the band gap. This produces a residual electric field in the bulk of the sample which is extremely sensitive to tiny deviations in electron transfer between two surfaces of the slab. In heterostructures, the band gap is replaced by a new effective energy scale set by the band alignment of its component. This changes the reconstruction pathways so that the electronic mechanism can benefit from the smallest energy scale possible.
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.
We present a temperature-dependent resonant elastic soft x-ray scattering (REXS) study of the metal-insulator transition in Sr3(Ru1-xMnx)2O7, performed at both Ru and Mn L-edges. Resonant magnetic superstructure reflections, which indicate an incipient instability of the parent compound, are detected below the transition. Based on modelling of the REXS intensity from randomly distributed Mn impurities, we establish the inhomogeneous nature of the metal-insulator transition, with an effective percolation threshold corresponding to an anomalously low x<0.05 Mn substitution.
We have investigated the shifts of the core-level photoemission spectra of La$_{0.6}$Sr$_{0.4}$MnO$_3$ thin films grown on three kinds of substrates, SrTiO$_3$, (LaAlO$_3$)$_{0.3}$-(SrAl$_{0.5}$Ta$_{0.5}$O$_3$)$_{0.7}$, and LaAlO$_3$. The experimental shifts of the La 4d and Sr 3d core levels are almost the same as the calculation, which we attribute to the absence of covalency effects on the Madelung potentials at these atomic sites due to the nearly ionic character of these atoms. On the other hand, the experimental shifts of the O $1s$ and Mn $2p$ core levels are negligibly small, in disagreement with the calculation. We consider that this is due to the strong covalent character of the Mn-O bonds.
X-ray absorption spectra on the overdoped high-temperature superconductors Tl_2Ba_2CuO_{6+delta} (Tl-2201) and La_{2-x}Sr_xCuO_{4+delta} (LSCO) reveal a striking departure in the electronic structure from that of the underdoped regime. The upper Hubbard band, identified with strong correlation effects, is not observed on the oxygen K edge, while the lowest-energy prepeak gains less intensity than expected above p ~ 0.21. This suggests a breakdown of the Zhang-Rice singlet approximation and a loss of correlation effects or a significant shift in the most fundamental parameters of the system, rendering single-band Hubbard models inapplicable. Such fundamental changes suggest that the overdoped regime may offer a distinct route to understanding in the cuprates.
We investigated the electronic structure of the SrTiO$_3$/LaAlO$_3$ superlattice (SL) by resonant soft x-ray scattering. The (003) peak, which is forbidden for our "ideal" SL structure, was observed at all photon energies, indicating reconstruction at the interface. From the peak position analyses taking into account the effects of refraction, we obtained evidence for electronic reconstruction of Ti 3d and O $2p$ states at the interface. From reflectivity analyses, we concluded that the AlO$_2$/LaO/TiO$_2$/SrO and the TiO$_2$/SrO/AlO$_2$/LaO interfaces are quite different, leading to highly asymmetric properties.
Once again the condensed matter world has been surprised by the discovery of yet another class of high temperature superconductors. The discovery of iron-pnictide (FeAs) and chalcogenide (FeSe) based superconductors with a $T_c$ of up to 55 K is again evidence of how complex the many body problem really is, or in another view how resourceful nature is. The first reactions would of course be that these new materials must in some way be related to the copper-oxide based superconductors for which a large number of theories exist although a general consensus regarding the correct theory has not yet been reached. Here we point out that the basic physical paradigm of the new iron based superconductors is entirely different from the cuprates. Their fundamental properties, structural and electronic, are dominated by the exceptionally large pnictide polarizabilities.
Multiferroicity in LiCu2O2 single crystals is studied using resonant soft x-ray magnetic scattering, hard x-ray diffraction, heat capacity, magnetic susceptibility, and electrical polarization. Two magnetic transitions are found at 24.6 K (T1) and 23.2 K (T2). Our data are consistent with a sinusoidal spin structure at T2<T<T1 and with a helicoidal spin structure at T<T2 giving rise to ferroelectricity. Surprisingly, above T2 the correlation lengths of the spin structures increase as the temperature increases with dramatic changes of ~42% along the c-axis. Our results demonstrate the interplay of the geometrical frustration and the electronic and magnetic polarizations.
Sr3(Ru1-xMnx)2O7, in which 4d-Ru is substituted by the more localized 3d-Mn, is studied by x-ray dichroism and spin-resolved density functional theory. We find that Mn impurities do not exhibit the same 4+ valence of Ru, but act as 3+ acceptors; the extra eg electron occupies the in-plane 3dx2-y2 orbital instead of the expected out-of-plane 3d3z2-r2. We propose that the 3d-4d interplay, via the ligand oxygen orbitals, is responsible for this crystal-field level inversion and the material's transition to an antiferromagnetic, possibly orbitally-ordered, low-temperature state.
Resonant soft X-ray scattering with photon energies near the O K and the Cu L3 edges was used to study charge ordering in the system La_{1.8-x}Eu_{0.2}Sr_xCuO_4 as a function of temperature for x = 0.125 and 0.15. From the superstructure diffraction intensities a charge ordering with a doping dependent wave vector is derived which is in this system well below the transition temperature of the low-temperature tetragonal phase but well above the onset of spin ordering. This indicates that charge ordering is the primary driving force for the formation of stripe-like phases in two-dimensional doped cuprates. Analysis of the lineshape of the scattered intensity as a function of photon energy yields evidence for a high hole concentration in the stripes.
We present a first-principle study of spin-orbit coupling effects on the Fermi surface of Sr2RuO4 and Sr2RhO4. For nearly degenerate bands, spin-orbit coupling leads to a dramatic change of the Fermi surface with respect to non-relativistic calculations; as evidenced by the comparison with experiments on Sr2RhO4, it cannot be disregarded. For Sr2RuO4, the Fermi surface modifications are more subtle but equally dramatic in the detail: spin-orbit coupling induces a strong momentum dependence, normal to the RuO2 planes, for both orbital and spin character of the low-energy electronic states. These findings have profound implications for the understanding of unconventional superconductivity in Sr2RuO4.
One of the keys to the high-temperature superconductivity puzzle is the identification of the energy scales associated with the emergence of a coherent condensate of superconducting electron pairs. These might provide a measure of the pairing strength and of the coherence of the superfluid, and ultimately reveal the nature of the elusive pairing mechanism in the superconducting cuprates. To this end, a great deal of effort has been devoted to investigating the connection between the superconducting transition temperature Tc and the normal-state pseudogap crossover temperature T*. Here we present a review of a large body of experimental data that suggests a coexisting two-gap scenario, i.e. superconducting gap and pseudogap, over the whole superconducting dome.
The discovery of quantum oscillations in the normal-state electrical resistivity of YBa2Cu3O6.5 provides the first evidence for the existence of Fermi surface (FS) pockets in an underdoped cuprate. However, the pockets' electron vs. hole character, and the very interpretation in terms of closed FS contours, are the subject of considerable debate. Angle-resolved photoemission spectroscopy (ARPES), with its ability to probe electronic dispersion as well as the FS, is ideally suited to address this issue. Unfortunately, the ARPES study of YBa2C3O7-d (YBCO) has been hampered by the technique's surface sensitivity. Here we show that this stems from the polarity and corresponding self-doping of the YBCO surface. By in-situ deposition of potassium atoms on the cleaved surface, we are able to continuously tune the doping of a single sample from the heavily overdoped to the underdoped regime. This reveals the progressive collapse of the normal-metal-like FS into four disconnected nodal FS arcs, or perhaps into hole but not electron pockets, in underdoped YBCO6.5.
The detection of quantum oscillations in the electrical resistivity of YBa2Cu3O6.5 provides direct evidence for the existence of Fermi surface pockets in an underdoped cuprate. We present a theoretical study of the electronic structure of YBa2Cu3O7-d (YBCO) aiming at establishing the nature of these Fermi pockets, i.e. CuO2 plane versus CuO chain or BaO. We argue that electron correlation effects, such as orbital-dependent band distortions and highly anisotropic self-energy corrections, must be taken into account in order to properly interpret the quantum oscillation experiments.