Tuning the 4f-state occupancy of cerium in highly correlated CeSi/ Fe multilayers: a study by x-ray absorption spectroscopy

Spectra of x-ray absorption and magnetic circular dichroism were measured at M4,5(3d) and L2,3(2p) edges of Ce in multilayers [Ce(1-x)Six/Fe]xn, with x between 0.1 and 0.65. The study uncovers the highly correlated nature of this layered system. An alpha-phase like electronic configuration of Ce is observed, with ordered magnetic moments on the 4f and 5d electrons induced by the interaction with Fe. Increasing the Si content reduces the strength of the hy-bridization between the 4f and conduction-band states which is reflected in a growing occupation and magnetic polarization of the 4f states. Variations of the shape and intensity of the L2,3-edge dichroism spectra, discussed in a simple phenomenological model, show the importance of the exchange interaction between the Ce-4f and 5d electrons, spin polarized by the interaction with Fe at the interfaces, for the electronic structure of Ce at high Si concentration and low temperature. A model of the band structure of rare-earth transition-metal compounds permits to argue that magnetic order on the Ce 4f electrons in the multilayers is due to different mechanisms: to hybridization of the Ce-4f with the Fe-3d states at low Si concentration and to intra-atomic 4f-5d exchange at high Si concentration. This is at variance with magnetic order in the intermetallics CeSi2-delta and CeSi which results from interaction between the localized 4f magnetic moments mediated by the Si-derived (s,p) conduction electrons, in competition with the Kondo effect.Comment: 31 pages, 9 figures, submitted to Phys. Rev.

Interrelation between the pseudogap and the incoherent quasi-particle features of high-Tc superconductors

Using a scenario of a hybridized mixture of localized bipolarons and conduction electrons, we demonstrate for the latter the simultaneous appearance of a pseudogap and of strong incoherent contributions to their quasi-particle spectrum which arise from phonon shake-off effects. This can be traced back to temporarily fluctuating local lattice deformations, giving rise to a double-peak structure in the pair distribution function, which should be a key feature in testing the origin of these incoherent contributions, recently seen in angle-resolved photoemission spectroscopy (ARPES).Comment: 4 pages, 3 figures, to be published in Phys. Rev. Let

From ferromagnetism to spin-density wave: Magnetism in the two channel periodic Anderson model

The magnetic properties of the two-channel periodic Anderson model for uranium ions, comprised of a quadrupolar and a magnetic doublet are investigated through the crossover from the mixed-valent to the stable moment regime using dynamical mean field theory. In the mixed-valent regime ferromagnetism is found for low carrier concentration on a hyper-cubic lattice. The Kondo regime is governed by band magnetism with small effective moments and an ordering vector \q close to the perfect nesting vector. In the stable moment regime nearest neighbour anti-ferromagnetism dominates for less than half band filling and a spin density wave transition for larger than half filling. $T_m$ is governed by the renormalized RKKY energy scale \mu_{eff}^2 ^2 J^2\rho_0(\mu).Comment: 4 pages, RevTeX, 3 eps figure

Inelastic X-ray Scattering by Electronic Excitations in Solids at High Pressure

Investigating electronic structure and excitations under extreme conditions gives access to a rich variety of phenomena. High pressure typically induces behavior such as magnetic collapse and the insulator-metal transition in 3d transition metals compounds, valence fluctuations or Kondo-like characteristics in $f$-electron systems, and coordination and bonding changes in molecular solids and glasses. This article reviews research concerning electronic excitations in materials under extreme conditions using inelastic x-ray scattering (IXS). IXS is a spectroscopic probe of choice for this study because of its chemical and orbital selectivity and the richness of information it provides. Being an all-photon technique, IXS has a penetration depth compatible with high pressure requirements. Electronic transitions under pressure in 3d transition metals compounds and $f$-electron systems, most of them strongly correlated, are reviewed. Implications for geophysics are mentioned. Since the incident X-ray energy can easily be tuned to absorption edges, resonant IXS, often employed, is discussed at length. Finally studies involving local structure changes and electronic transitions under pressure in materials containing light elements are briefly reviewed.Comment: submitted to Rev. Mod. Phy

Combined local-density and dynamical mean field theory calculations for the compressed lanthanides Ce, Pr, and Nd

This paper reports calculations for compressed Ce (4f^1), Pr (4f^2), and Nd (4f^3) using a combination of the local-density approximation (LDA) and dynamical mean field theory (DMFT), or LDA+DMFT. The 4f moment, spectra, and the total energy among other properties are examined as functions of volume and atomic number for an assumed face-centered cubic (fcc) structure.Comment: 15 pages, 9 figure

Pressure induced high-spin to low-spin transition in FeS evidenced by x-ray emission spectroscopy

We report the observation of the pressure-induced high-spin to low-spin transition in FeS using new high-pressure synchrotron x-ray emission spectroscopy techniques. The transition is evidenced by the disappearance of the low-energy satellite in the Fe K$\beta$ emission spectrum of FeS. Moreover, the phase transition is reversible and closely related to the structural phase transition from a manganese phosphide-like phase to a monoclinic phase. The study opens new opportunities for investigating the electronic properties of materials under pressure.Comment: ReVTeX, 4 pages, 3 figures inserted with epsfig. minor modifications before submission to PR

Possible charge inhomogeneities in the CuO2 planes of YBa2Cu3O6+x (x=0.25, 0.45, 0.65, 0.94) from pulsed neutron diffraction

The atomic pair distribution functions (PDF) of four powder samples of YBa2Cu3O6+x (x=0.25, 0.45, 0.65, 0.94) at 15 K have been measured by means of pulsed neutron diffraction. The PDF is modelled using a full-profile fitting approach to yield structural parameters. In contrast to earlier XAFS work we find no evidence of a split apical oxygen site. However, a slightly improved fit over the average crystallographic model results when the planar Cu(2) site is split along the z-direction. This is interpreted in terms of charge inhomogeneities in the CuO2 planes.Comment: 8 pages, 3 figure

Slow crossover in YbXCu4 intermediate valence compounds

We compare the results of measurements of the magnetic susceptibility Chi(T), the linear coefficient of specific heat Gamma(T)=C(T)/T and 4f occupation number nf(T) for the intermediate valence compounds YbXCu4 (X = Ag, Cd, In, Mg, Tl, Zn) to the predictions of the Anderson impurity model, calculated in the non-crossing approximation (NCA). The crossover from the low temperature Fermi liquid state to the high temperature local moment state is substantially slower in the compounds than predicted by the NCA; this corresponds to the ''protracted screening'' recently predicted for the Anderson Lattice. We present results for the dynamic susceptibility, measured through neutron scattering experiments, to show that the deviations between theory and experiment are not due to crystal field effects, and we present x-ray-absorption fine-structure (XAFS) results that show the local crystal structure around the X atoms is well ordered, so that the deviations probably do not arise from Kondo Disorder. The deviations may correlate with the background conduction electron density, as predicted for protracted screening.Comment: Submitted to Physical Review B on June 7, 2000, accepted for publication November 2, 2000. Changes to the original manuscript include: 1) a discussion of the relation of the slow crossover to the conduction electron density; 2) a discussion of the relation of the reported results to earlier photoemission results; and, 3) minor editorial change

Reduction of the Yb valence in YbAl3 nanoparticles

Measurements of specific heat, dc magnetic susceptibility, and Yb LII and LIII x-ray absorption near-edge structure XANES and extended x-ray absorption fine structure EXAFS on YbAl3 milled alloys are reported. X-ray diffraction patterns are consistent with a reduction in particle size down to 10 nm and an increase in the lattice strain up to 0.4% for 120 h of milling time. A decrease in the mean valence from 2.86 for the unmilled alloy to 2.70 for 120 h milled YbAl3 is obtained from the analysis of XANES spectra. From the analysis of spectra in the EXAFS region, an increase in the mean-square disorder of neighbor distance with milling time is detected in good agreement with the results of x-ray diffraction. Size effects strongly influence the magnetic and thermal properties. The value for the maximum of the magnetic susceptibility decreases around 30% for 120 h milled alloy and an excess specific heat, with a peak around 40 K in the milled samples, is derived. These changes in the physical properties along the milled YbAl3 alloys are associated with the reduction in particle size. Such a reduction leads to the existence of a large number of Yb2+ atoms at the surface with respect to the bulk affecting the overall electronic state

Ongoing Laboratory Performance Study on Chemical Analysis of Hydrophobic and Hydrophilic Compounds in Three Aquatic Passive Samplers

The quality of chemical analysis is an important aspect of passive sampling-based environmental assessments. The present study reports on a proficiency testing program for the chemical analysis of hydrophobic organic compounds in silicone and low-density polyethylene (LDPE) passive samplers and hydrophilic compounds in polar organic chemical integrative samplers. The median between-laboratory coefficients of variation (CVs) of hydrophobic compound concentrations in the polymer phase were 33% (silicone) and 38% (LDPE), similar to the CVs obtained in four earlier rounds of this program. The median CV over all rounds was 32%. Much higher variabilities were observed for hydrophilic compound concentrations in the sorbent: 50% for the untransformed data and a factor of 1.6 after log transformation. Limiting the data to the best performing laboratories did not result in less variability. Data quality for hydrophilic compounds was only weakly related to the use of structurally identical internal standards and was unrelated to the choice of extraction solvent and extraction time. Standard deviations of the aqueous concentration estimates for hydrophobic compound sampling by the best performing laboratories were 0.21 log units for silicone and 0.27 log units for LDPE (factors of 1.6 to 1.9). The implications are that proficiency testing programs may give more realistic estimates of uncertainties in chemical analysis than within-laboratory quality control programs and that these high uncertainties should be taken into account in environmental assessments