Systematic Study on Fluorine-doping Dependence of Superconducting and Normal State Properties in LaFePO1-xFx

We have investigated the fluorine-doping dependence of lattice constants, transports and specific heat for polycrystalline LaFePO1-xFx. F doping slightly and monotonically decreases the in-plane lattice parameter. In the normal state, electrical resistivity at low temperature is proportional to the square of temperature and the electronic specific heat coefficient has large value, indicating the existence of moderate electron-electron correlation in this system. Hall coefficient has large magnitude, and shows large temperature dependence, indicating the low carrier density and multiple carriers in this system. Temperature dependence of the upper critical field suggests that the system is a two gap superconductor. The F-doping dependence of these properties in this system are very weak, while in the FeAs system (LaFeAsO), the F doping induces the large changes in electronic properties. This difference is probably due to the different F-doping dependence of the lattice in these two systems. It has been revealed that a pure effect of electron doping on electronic properties is very weak in this Fe pnictide compound.Comment: 8 pages, 5 figures, accepted for publication in J. Phys. Soc. Jp

Normal State Spin Dynamics of Five-band Model for Iron-pnictides

Normal state spin dynamics of the recently discovered iron-pnictide superconductors is discussed by calculating spin structure factor S(q, omega) in an itinerant five-band model within RPA approximation. Due to the characteristic Fermi surface structure of iron-pnictide, column like response is found at (pi, 0) in extended Brillouin zone in the undoped case, which is consistent with the recent neutron scattering experiment. This indicates that the localized spin model is not necessary to explain the spin dynamics of this system. Furthermore, we show that the temperature dependence of inelastic neutron scattering intensity can be well reproduced in the itinerant model. We also study NMR 1/T_1T in the same footing calculation and show that the itinerant model can capture the magnetic property of iron-pnictide superconductors.Comment: 4 page

Paramagnetic Phase of a Heavy-Fermion Compound, CeFePO, Probed by 57Fe M\"{o}ssbauer Spectroscopy

57Fe M\"{o}ssbauer spectroscopy was applied to an iron-based layered compound CeFePO. At temperatures from 9.4 to 293 K, no magnetic splitting was observed in the M\"ossbauer spectra of CeFePO indicating a paramagnetic phase of the Fe magnetic sublattice. All the spectra were fitted with a small quadrupole splitting, and the Debye temperature of CeFePO was found to be \sim448 K. The isomer shift at room temperature, 0.32 mm/s, was almost equal to those of LnFeAsO (Ln = La, Ce, Sm). Comparing s-electron density using the isomer shifts and unit cell volumes, it was found that the Fe of CeFePO has a similar valence state to other layered iron-based quaternary oxypnictides except LaFePO

Structural and superconducting properties in LaFeAs1-xSbxO1-yFy

We report the antimony (Sb) doping effect in a prototype system of iron-based supercon-ductors LaFeAsO1-yFy (y=0, 0.1, 0.15). X-ray powder diffraction indicates that the lattice pa-rameters increase with Sb content within the doping limit. Rietveld structural refinements show that, with the partial substitution of Sb for As, while the thickness of the Fe2As2 layers increases significantly, that of the La2O2 layers shrinks simultaneously. So a negative chemical pressure is indeed "applied" to the superconducting-active Fe2As2 layers, in con-trast to the effect of positive chemical pressure by the phosphorus doping. Electrical resis-tance and magnetic susceptibility measurements indicate that, while the Sb doping hardly influences the SDW anomaly in LaFeAsO, it recovers SDW order for the optimally-doped sample of y=0.1. In the meantime, the superconducting transition temperature can be raised up to 30 K in LaFeAs1-xSbxO1-yFy with x=0.1 and y=0.15. The Sb doping effects are discussed in term of both J1-J2 model and Fermi Surface (FS) nesting scenario.Comment: 7 pages, 4 figures, 1 table. to be published in Science in China Series

Superconductivity above 50K in LnFeAsO1-y (Ln= Nd, Sm, Gd, Tb and Dy) Synthesized by High-pressure Technique

We have succeeded in synthesizing single-phase polycrystalline samples of oxygen-deficient oxypnictide superconductors, LnFeAsO1-y (Ln: lanthanide elements) with Ln=La, Ce, Pr, Nd, Sm, Gd, Tb and Dy using high-pressure synthesis technique. It is found out that the synthesis pressure is the most important parameter for synthesizing single-phase samples, in particular for the heavier Ln?s, such as Tb and Dy. The lattice parameters systematically decrease with the atomic number of Ln, reflecting the shrinkage of Ln ionic radius. For the lighter Ln?s (La, Ce, Pr, Nd), Tc increases monotonously with decreasing the lattice parameters from 26K for Ln=La to 54K for Ln=Nd, then stays at the constant value around 53K for the heavier counterpart (Nd, Sm, Gd, Tb and Dy). The results suggest the intimate relationship between the crystal structural parameters and the superconductivity on the one hand, as well as the possible existence of the inherent maximum Tc on the other, which is located around 50 K in the LnFeAsO based materials.Comment: 14 pages, 10 figures,Accepted for publication in Journal of the Physical Society of Japan Vol.78No.

Heavily electron-doped electronic structure and isotropic superconducting gap in AxFe2Se2 (A=K,Cs)

The low energy band structure and Fermi surface of the newly discovered superconductor, AxFe2Se2 (A=K,Cs), have been studied by angle-resolved photoemission spectroscopy. Compared with iron pnictide superconductors, AxFe2Se2 (A=K,Cs) is the most heavily electron-doped with Tc~30 K. Only electron pockets are observed with an almost isotropic superconducting gap of ~10.3 meV, while there is no hole Fermi surface near the zone center, which indicates the inter-pocket hopping or Fermi surface nesting is not a necessary ingredient for the unconventional superconductivity in iron-based superconductors. Thus, the sign changed s$_\pm$ pairing symmetry, a leading candidate proposed for iron-based superconductors, becomes conceptually irrelevant in describing the superconducting state here. A more conventional s-wave pairing is a better description.Comment: 4 pages, 4 figures, published online in Nature Materials 201

First-principles Electronic Structure of Superconductor Ca4_4Al2_2O6_6Fe2_2P2_2: Comparison with LaFePO and Ca4_4Al2_2O6_6Fe2_2As2_2

We investigate the electronic structures of iron-based superconductors having perovskite-like blocking layers, %Ca$_4$Al$_2$O$_6$Fe$_2$(As$_{1-x}$P$_x$)$_2$ from first principles. Ca$_4$Al$_2$O$_6$Fe$_2$P$_2$ and Ca$_4$Al$_2$O$_6$Fe$_2$As$_2$ from first principles. Ca$_4$Al$_2$O$_6$Fe$_2$P$_2$ is found to have two hole-like Fermi surfaces around $\Gamma$, and one hole-like Fermi surface around M in the unfolded Brillouin zone. This is in contrast with LaFePO, where no Fermi surface is found around M. The relationship of their band structures and measured transition temperatures of superconductivity is discussed. The number of Fermi surfaces in Ca$_4$Al$_2$O$_6$Fe$_2$P$_2$ is also different from that of Ca$_4$Al$_2$O$_6$Fe$_2$As$_2$, in which only one Fermi surface is formed around $\Gamma$. Analysis using maximally localized Wannier functions clarifies that the differences between their band structures originate mainly from the pnictogen height. We then analyze the alloying effect on the electronic structure of Ca$_4$Al$_2$O$_6$Fe$_2$AsP. It is found that its electronic structure is similar to that of Ca$_4$Al$_2$O$_6$Fe$_2$P$_2$ and Ca$_4$Al$_2$O$_6$Fe$_2$As$_2$ with the average crystal structure, though Ca$_4$Al$_2$O$_6$Fe$_2$AsP contains the pnictogen height disorder. We calculate the generalized susceptibility for Ca$_4$Al$_2$O$_6$Fe$_2$(As$_{1-x}$P$_x$)$_2$ and clarify the factors determining its tendency.Comment: 5 figures, to be published in J. Phys. Soc. Jp

d- and f-orbital correlations in the REFeAsO compounds

We estimate theoretically the strength of the local Coulomb interaction for the Fe 3d and Ce 4f shells in the REFeAsO compunds. In LaFeAsO and CeFeAsO we obtain values of the local Coulomb interaction parameter U for both Fe and Ce which are larger than those of elemental Fe and Ce metals. The Fe 3d bandwidth of REFeAsO is found to increase slightly as one moves along the RE-series. Using a combined local density approximation and dynamical mean-field theory (LDA+DMFT) approach, we study the behaviour of the localized 4f states along the rare-earth oxyarsenides REFeAsO series (RE=Ce,Pr,Nd). In CeFeAsO the occupied Ce 4f band is located just below the Fe 3d band leading possibly to a Kondo screening of the 4f local moment under applied pressure, while the unscreened local moment behaviour is expected for the Pr and Nd compounds.Comment: 7 pages, 2 figures, 1 tabl

Local moment versus Kondo behavior of the 4f-electrons in rare-earth iron oxypnictides

We consider the role played by the 4f states in the rare-earth oxyarsenides REOFeAs (RE=Ce,Pr,Nd) and the oxyphosphate CeOFeP, using a first-principles technique that combines the local density approximation and dynamical mean-field theory (LDA+DMFT). In the Pr and Nd compounds, the 4f states are located well below and above the Fermi level E_F, and essentially do not interact with the iron 3d bands located near E_F, resulting in local moment behavior. In the Ce compounds, our results reveal a qualitatively different picture, with the 3d-4f hybridization being sufficiently strong to give rise to an observable Kondo screening of the local 4f moment. Our LDA+DMFT electronic structure calculations allow us to estimate the Kondo temperature T_K for both CeOFeP and CeOFeAs. For the phosphate, the order of magnitude of our estimate is consistent with the experimental observation of T_K around 10 K. At ambient pressure, T_K is found to be negligibly small for CeOFeAs. Under applied hydrostatic pressure, we predict an exponential increase of T_K which reaches values comparable to the superconducting T_c around 40 K at pressures above 10 GPa. We conjecture that the competition between the Kondo effect and superconductivity may be at the origin of the monotonous decrease of T_c observed in CeOFeAs under pressure. We argue that the quantitative aspects of this competition are inconsistent with a weak-coupling BCS description of the superconductivity in the oxyarsenides.Comment: 6 pages, 3 figure

Electronic Structure Calculation by First Principles for Strongly Correlated Electron Systems

Recent trends of ab initio studies and progress in methodologies for electronic structure calculations of strongly correlated electron systems are discussed. The interest for developing efficient methods is motivated by recent discoveries and characterizations of strongly correlated electron materials and by requirements for understanding mechanisms of intriguing phenomena beyond a single-particle picture. A three-stage scheme is developed as renormalized multi-scale solvers (RMS) utilizing the hierarchical electronic structure in the energy space. It provides us with an ab initio downfolding of the global band structure into low-energy effective models followed by low-energy solvers for the models. The RMS method is illustrated with examples of several materials. In particular, we overview cases such as dynamics of semiconductors, transition metals and its compounds including iron-based superconductors and perovskite oxides, as well as organic conductors of kappa-ET type.Comment: 44 pages including 38 figures, to appear in J. Phys. Soc. Jpn. as an invited review pape