X-ray photoemission study of NiS_{2-x}Se_x (x = 0.0 - 1.2)

Electronic structure of NiS_{2-x}Se_x system has been investigated for various compositions (x) using x-ray photoemission spectroscopy. An analysis of the core level as well as the valence band spectra of NiS_2 in conjunction with many-body cluster calculations provides a quantitative description of the electronic structure of this compound. With increasing Se content, the on-site Coulomb correlation strength (U) does not change, while the band width W of the system increases, driving the system from a covalent insulating state to a pd-metallic state.Comment: 19 pages, 6 figures, To appear in Phys. Rev. B, 200

One particle spectral weight of the three dimensional single band Hubbard model

Dynamic properties of the three-dimensional single-band Hubbard model are studied using Quantum Monte Carlo combined with the maximum entropy technique. At half-filling, there is a clear gap in the density of states and well-defined quasiparticle peaks at the top (bottom) of the lower (upper) Hubbard band. We find an antiferromagnetically induced weight above the naive Fermi momentum. Upon hole doping, the chemical potential moves to the top of the lower band where a robust peak is observed. Results are compared with spin-density-wave (SDW) mean-field and self consistent Born approximation results, and also with the infinite dimensional Hubbard model, and experimental photoemission (PES) for three dimensional transition-metal oxides.Comment: 11 pages, REVTeX, 16 figures included using psfig.sty. Ref.30 correcte

Soft X-ray spectroscopic study of dense strontium-doped lanthanum manganite cathodes for solid oxide fuel cell applications

The evolution of the Mn charge state, chemical composition, and electronic structure of La0.8 Sr0.2 Mn O3 (LSMO) cathodes during the catalytic activation of solid oxide fuel cell (SOFC) has been studies using X-ray spectroscopy of as-processed, exposed, and activated dense thin LSMO films. Comparison of O K-edge and Mn L3,2-edge X-ray absorption spectra from the different stages of LSMO cathodes revealed that the largest change after the activation occurred in the Mn charge state with little change in the oxygen environment. Core-level X-ray photoemission spectroscopy and Mn L 3 resonant photoemission spectroscopy studies of exposed and as-processed LSMO determined that the SOFC environment (800°C ambient pressure of O2) alone results in La deficiency (severest near the surface with Sr doping >0.55) and a stronger Mn4+ contribution, leading to the increased insulating character of the cathode prior to activation. Meanwhile, O K-edge X-ray absorption measurements support Sr/La enrichment nearer the surface, along with the formation of mixed Srx Mny Oz and/or passive Mn Ox and SrO species. © 2010 The Electrochemical Society