Nominal doping and partition of doped holes between planar and apical orbitals in La2-xSrxCuO4

By considering both the average structural parameters obtained from Rietveld refinement of neutron powder diffraction data, and the local structural parameters obtained from the atomic pair distribution function, we have tested the recent hypothesis of Perry et al [Perry et al., Phys. Rev. B v.65, 144501 (2002)] that doping in La2-xSrxCuO4 system occurs as localized defects of predominantly Cud3z^2-r^2--Opz character associated with the Sr dopants accompanied by a local destruction of the Jahn-Teller distortion. While the structural parameters behave qualitatively according to the prediction of this model, a quantitative analysis indicates that doped holes predominantly appear in the planar Cudx^2-y^2--Opx,y band as is normally assumed. However, a small amount of the doped charge does enter the Cud3z^2-r^2--Opz orbitals and this should be taken into account when theoretical phase diagrams are compared to experiment. We present a calibration curve, p = x (1.00(1) - 0.45(7) x), for the planarcharge doping, p, vs strontium content, x, for the La2-xSrxCuO4 system.Comment: 6 pages, 4 figures, submitted to Phys. Rev.

Structural response to local charge order in underdoped but superconducting La2-x(Sr,Ba)xCuO4

We report an anomalous local structural response in the CuO2 planes associated with the appearance of charge inhomogeneities at low temperature in underdoped but superconducting La2-x(Sr,Ba)xCuO4. We used pair distribution function analysis of neutron powder diffraction data. The increase in the Cu-O bond length distribution at low temperature has an onset temperature which correlates with observations of charge and spin freezing seen by other probes.Comment: 4 pages, 3 figure

Microscopic Charge Inhomogeneities in Underdoped La_2-xSr_xCuO_4: Local Structural Evidence

We present local structural evidence for the existence of charge inhomogeneities at low temperature in underdoped and optimally doped La_2-xSr_xCuO_4. The inhomogeneities disappear for x > 0.2. The evidence for the charge inhomogeneities comes from an anomalous increase in the in-plane Cu-O bond length distribution in the underdoped samples as well as evidence for CuO_6 octahedral tilt inhomogeneities in the intermediate range structure. Preliminary analysis of the temperature dependence of this phenomenon indicates that the inhomogeneities set in at temperatures in the range 60 K < Tco < 130 K which depends on doping.Comment: 8 pages, 7 figures, to appear in J. Supercond., proceedings of the conference "Major Trends in Superconductivity in the New Millenium, Klosters, Switzerland, April 1st-6th 2000

Cu(Ir1−x_{1-x}Crx_x)2_2S4_4: a model system for studying nanoscale phase coexistence at the metal-insulator transition

Increasingly, nanoscale phase coexistence and hidden broken symmetry states are being found in the vicinity of metal-insulator transitions (MIT), for example, in high temperature superconductors, heavy fermion and colossal magnetoresistive materials, but their importance and possible role in the MIT and related emergent behaviors is not understood. Despite their ubiquity, they are hard to study because they produce weak diffuse signals in most measurements. Here we propose Cu(Ir$_{1-x}$Cr$_x$)$_2$S$_4$ as a model system, where robust local structural signals lead to key new insights. We demonstrate a hitherto unobserved coexistence of a Ir$^{4+}$ charge-localized dimer phase and Cr-ferromagnetism. The resulting phase diagram that takes into account the short range dimer order, is highly reminiscent of a generic MIT phase diagram similar to the cuprates. We suggest that the presence of quenched strain from dopant ions acts as an arbiter deciding between the competing ground states

Phase separation and nanostructuring in the thermoelectric material PbTe1-xSx

The average and local structures of the (PbTe)1-x(PbS)x system of thermoelectric materials has been studied using the Rietveld and atomic pair distribution function (PDF) methods. Samples with 0:25 < x are macroscopically phase separated. Phase separation was suppressed in a quenched x = 0:5 sample which, nonetheless, exhibited a partial spinodal decomposition. The promising thermoelectric material with x = 0:16 showed intermediate behavior. Combining TEM and bulk scattering data suggests that the sample is a mixture of PbTe rich material and a partially spinodally decomposed phase similar to the quenched 50% sample. This results in a nano-meter scale inhomogeneous material that accounts for its very low thermal conductivity.Comment: 9 pages, 9 figures, 4 tables, submitted to PR

Charge-screening role of cc-axis atomic displacements in YBa2_2Cu3_3O6+x_{6+x} and related superconductors

The importance of charge reservoir layers for supplying holes to the CuO$_2$ planes of cuprate superconductors has long been recognized. Less attention has been paid to the screening of the charge transfer by the intervening ionic layers. We address this issue in the case of YBa$_2$Cu$_3$O$_{6+x}$, where CuO chains supply the holes for the planes. We present a simple dielectric-screening model that gives a linear correlation between the relative displacements of ions along the $c$ axis, determined by neutron powder diffraction, and the hole density of the planes. Applying this model to the temperature dependent shifts of ions along the $c$ axis, we infer a charge transfer of 5-10% of the hole density from the planes to the chains on warming from the superconducting transition to room temperature. Given the significant coupling of $c$-axis displacements to the average charge density, we point out the relevance of local displacements for screening charge modulations and note recent evidence for dynamic screening of in-plane quasiparticles. This line of argument leads us to a simple model for atomic displacements and charge modulation that is consistent with images from scanning-tunneling microscopy for underdoped Bi$_2$Sr$_2$CaCu$_2$O$_{8+\delta}$.Comment: 12 pages, 10 figures; final version, accepted for publication in Phys. Rev.

Neutron powder diffraction atomic pair distribution function analysis using the ARCS chopper spectrometer at the Spallation Neutron Source

The frst neutron powder diffraction based atomic pair distribution functions (PDFs) are reported from the new wide angular-range chopper spectrometer ARCS at the Spallation Neutron Source at Oak Ridge National Laboratory. The spectrometer was run in white-beam mode, with no Fermi chopper. The PDF patterns of Si, Ni, and Al2O3 were refined using the PDFfit method and the results compared to data collected at the NPDF diffractometer at Los Alamos National Laboratory. The resulting fits are of high quality demonstrating that quantitatively reliable powder diffraction data can be obtained from ARCS when operated in this configuration.Comment: 4 pages, 5 figures, submitted to Journal of Applied Crystallograph

Room temperature local nematicity in FeSe superconductor

We report pair distribution function measurements of the iron-based superconductor FeSe above and below the structural transition temperature. Structural analysis reveals a local orthorhombic distortion with a correlation length of about 4 nm at temperatures where an average tetragonal symmetry is observed. The analysis further demonstrates that the local distortion is larger than the distortion at temperatures where the average observed symmetry is orthorhombic. Our results suggest that the low-temperature macroscopic nematic state in FeSe forms from an imperfect ordering of orbital-degeneracy-lifted nematic fluctuations which persist up to at least 300 K.Comment: 6 pages, 4 figure

Quantum liquid with strong orbital fluctuations: the case of a pyroxene family

We discuss quasi one-dimensional magnetic Mott insulators of the pyroxene family where spin and orbital degrees of freedom remain tightly bound. We analyze their excitation spectrum and outline the conditions under which the orbital degrees of freedom become liberated so that the excitations become dispersive and the spectral weight shifts to energies much smaller than the exchange integral.Comment: 5 pages, 5 figures, Supplemental Material, revised versio

Insulating and metallic spin glass in Kx_{x}Fe2−δ−y_{2-\delta-y}Niy_{y}Se2_{2} (0.06 ≤\leq yy ≤\leq 1.44) single crystals

We report electron doping effects by Ni in K$_{x}$Fe$_{2-\delta-y}$Ni$_{y}$Se$_{2}$ (0.06 $\leq$ $y$ $\leq$ 1.44) single crystal alloys. A rich ground state phase diagram is observed. Small amount of Ni ($\sim$ 4\%) suppressed superconductivity below 1.8 K, inducing insulating spin glass magnetic ground state for higher Ni content. With further Ni substitution, metallic resistivity is restored. For high Ni concentration in the lattice the unit cell symmetry is high symmetry $I4/mmm$ with no phase separation whereas both $I4/m + I4/mmm$ space groups were detected in the phase separated crystals when concentration of Ni $<$ Fe. The absence of superconductivity coincides with the absence of crystalline Fe vacancy order.Comment: 6 pages, 4 figure