Some important aspects of the electronic structure of the iron oxypnictides depend very sensitively on small changes in interatomic distances and bond angles within the iron-pnictogen subunit. Using first-principles full-potential electronic structure calculations, we investigate this sensitive dependence, contrasting in particular LaOFeAs and LaOFeP. The width of the Fe-bands is significantly larger for LaOFeP, indicating a better metal and weaker electronic correlations. When calculated at their experimental crystal structure these two materials have significantly different low-energy band structure. The topology of the Fermi surface changes when going from LaOFeP to LaOFeAs, with a three-dimensional hole pocket present in the former case transforming into a tube with two-dimensional dispersion. We show that the low-energy band structure of LaOFeAs evolves towards that of LaOFeP as the As atom is lowered closer to the Fe plane with respect to its experimental position. The physical origin of this sensitivity to the iron-pnictogen distance is the covalency of the iron-pnictogen bond, leading to strong hybridization effects. To illustrate this, we construct Wannier functions, which are found to have a large spatial extension when the energy window is restricted to the bands with dominant iron character. Finally, we show that the Fe bandwidth slightly increases as one moves along the rare-earth series in ReOFeAs and discuss the physical origin of this effect.
We study the magnetic excitations of undoped iron oxypnictides using a three-dimensional Heisenberg model with single-ion anisotropy. Analytic forms of the spin wave dispersion, velocities, and structure factor are given. Aside from quantitative comparisons which can be made to inelastic neutron scattering experiments, we also give qualitative criteria which can distinguish various regimes of coupling strength. The magnetization reduction due to quantum zero point fluctuations shows clear dependence on the c-axis coupling.
The iron-oxypnictide compounds, recently reported as a new class of superconductors when appropriately doped, exhibit large Seebeck coefficients, of the order of -100 microV/K, while keeping good electrical conductivity. Their power factor shows a peak at low temperatures, suggesting possible applications of these materials in thermoelectric cooling modules in the liquid nitrogen temperature range.
We present the first infrared and optical study in the normal state of ab-plane oriented single crystals of the iron-oxypnictide superconductor LaFePO. We find that this material is a low carrier density metal with a moderate level of correlations and exhibits signatures of electron-boson coupling. The data is consistent with the presence of coherent quasiparticles in LaFePO.
Pairing symmetry in oxypnictides, a new family of multiband high-Tc superconductors, is partially imposed by the positions of multiple Fermi pockets, which itself can give rise to new order parameters, such as s+,- states or the state of dx^2-y^2 symmetry. Other pairing states may appear on small pockets for long range interactions, but they are expected to be sensitive to defects. We identify the competing antiferromagnetic order with the triplet exciton transition in the semi- metallic background and discuss whether its coexistence with superconductivity explains the doping dependence of Tc.
We have performed a temperature-dependent angle-integrated laser photoemission study of iron oxypnictide superconductors LaFeAsO:F and LaFePO:F exhibiting critical transition temperatures (Tc's) of 26 K and 5 K, respectively. We find that high-Tc LaFeAsO:F exhibits a temperature-dependent pseudogap-like feature extending over ~0.1 eV about the Fermi level at 250 K, whereas such a feature is absent in low-Tc LaFePO:F. We also find ~20-meV pseudogap-like features and signatures of superconducting gaps both in LaFeAsO:F and LaFePO:F. We discuss the possible origins of the unusual pseudogap-like f…
We study a four-band model for the iron oxypnictides, in which the superconducting properties are assumed to be determined by the interband coupling between hole-like and electron-like Fermi sheets. We show that reasonable parameters can account for the angle-resolved photoemission spectra showing multiple gaps in Ba$_{1-x}$K$_x$Fe$_2$As$_2$, and for the temperature dependence of the superfluid density. At the same time, the zero-temperature value of the superfluid density shows a conventional scaling with the number of carriers.
Photoemission spectroscopy with low-energy tunable photons on oxygen-deficient iron-based oxypnictide superconductors NdFeAsO0.85 (Tc=52K) reveals a distinct photon-energy dependence of the electronic structure near the Fermi level (EF). A clear shift of the leading-edge can be observed in the superconducting states with 9.5 eV photons, while a clear Fermi cutoff with little leading-edge shift can be observed with 6.0 eV photons. The results are indicative of the superconducting gap opening not on the hole-like ones around Gamma (0,0) point but on the electron-like sheets around M(pi,pi) point…
Early studies have found quasi-reversible magnetization curves in polycrystalline bulk rare-earth iron oxypnictides that suggest either wide-spread obstacles to intergranular current or very weak vortex pinning. In the present study of polycrystalline samarium and neodymium rare-earth iron oxypnictide samples made by high pressure synthesis, the hysteretic magnetization is significantly enhanced. Magneto optical imaging and study of the field dependence of the remanent magnetization as a function of particle size both show that global currents over the whole sample do exist but that the interg…
The electronic structure in the normal state of CeFeAsO0.89F0.11 oxypnictide superconductors has been investigated with x-ray absorption and photoemission spectroscopy. All the data exhibit signatures of Fe d-electron itinerancy. Exchange multiplets appearing in the Fe 3s core level indicate the presence of itinerant spin fluctuations. These findings suggest that the underlying physics and the origin of superconductivity in these materials are likely to be quite different from those of the cuprate high-temperature superconductors. These materials provide opportunities for elucidating the role …
A new class of high temperature superconductors based on iron and arsenic was recently discovered, with superconducting transition temperature as high as 55 K. Here we show, using microscopic theory, that the normal state of the iron pnictides at high temperatures is highly anomalous, displaying a Curie Weiss susceptibility and a linear temperature dependence of the resistivity. Below a coherence scale T*, the resistivity sharply drops and susceptibility crosses over to Pauli-like temperature dependence. Remarkably, the coherence-incoherence crossover temperature is a very strong function of t…
We report on the synthesis and structural/ microstructural studies of iron based fluorine doped LaOFeAs superconductors. We have successfully synthesized fluorine doped superconducting LaO1-xFxFeAs materials by choosing lower temperature (1150^0C) and longer synthesis duration (60 hours) as compared to the standard values of these employed in the pioneering first contribution [Kamihara et al 2008 J Am Chem Soc 130 3296]. Decrease of lattice parameters as determined by x-ray diffraction confirm the substitution of fluorine. The superconducting transition temperature is 27.5 K which is observed …
The sign-reversing fully gapped superconducting state, which is expected to be realized in oxypnictide superconductors, can be prominently affected by nonmagnetic impurities due to the interband scattering of Cooper pairs. We study this problem based on the isotropic two-band BCS model: In oxypnictide superconductors, the interband impurity scattering $I'$ is not equal to the intraband one $I$. In the Born scattering regime, the reduction in Tc is sizable and the impurity-induced density of states (DOS) is prominent if $I\sim I'$, due to the interband scattering. Although impurity-induced DOS …
Zero field and longitudinal field muon spin relaxation measurements have been performed in optimally doped and overdoped superconductors LaFeAsO$_{1-x}$F$_x$ in order to investigate the magnetic fluctuation over a wide range of temperature and longitudinal field. We have observed no sign of magnetic fluctuation against temperature in the muons' time window (10$^{-5}\sim$ 10$^{-9}$s). Considering the current results and other results, i.e., spin fluctuation observed by neutron scattering, pseudogap-like behaviors by NMR and photoemission spectroscopy, it is suggested that not only the spin fluc…
We have performed ^{31}P-NMR measurements on Ce(Ru_{1-x}Fe_{x})PO in order to investigate ferromagnetic (FM) quantum criticality, since heavy-fermion (HF) ferromagnet CeRuPO with a two-dimensional structure turns to a HF paramagnet by an isovalent Fe-substitution for Ru. We found that Ce(Ru_{0.15}Fe_{0.85})PO shows critical fluctuations down to \sim 0.3 K, as well as the continuous suppression of Curie temperature and the ordered moments by the Fe-substitution. These experimental results suggest the presence of a FM quantum critical point (QCP) at x \sim 0.86, which is a rare example among iti…
We present the first comprehensive derivation of the intrinsic electronic phase diagram of the iron-oxypnictide superconductors in the normal state based on the analysis of the electrical resistivity $ρ$ of both LaFeAsO$_{1-x}$F$_x$ and SmFeAsO$_{1-x}$F$_x$ for a wide range of doping. Our data give clear-cut evidence for unusual normal state properties in these new materials. In particular, the emergence of superconductivity at low doping levels is accompanied by distinct anomalous transport behavior in $ρ$ of the normal state which is reminiscent of the spin density wave (SDW) signature in th…
We report 75As-NQR/NMR studies on the oxygen-deficient iron(Fe)-based oxypnictide superconductors LaFeAsO_{0.6} (T_c=28 K) along with the results on LaFeAsO, LaFeAsO_{0.75}(T_c=20 K) and NdFeAsO_{0.6}(T_c=53 K). Nuclear spin-lattice relaxation rate 1/T_1 of 75As NQR at zero field on LaFeAsO_{0.6} has revealed a T^3 dependence below T_c upon cooling without the coherence peak just below T_c, evidencing the unconventional superconducting state with the line-node gap. We have found an intimate relationship between the nuclear quadrupole frequencyof 75As and T_c for four samples used in this study…
We investigate the electronic states of a one-dimensional two-orbital Hubbard model with band splitting by the exact diagonalization method. The Luttinger liquid parameter $K_ρ$ is calculated to obtain superconducting (SC) phase diagram as a function of on-site interactions: the intra- and inter-orbital Coulomb $U$ and $U'$, the Hund coupling $J$, and the pair transfer $J'$. In this model, electron and hole Fermi pockets are produced when the Fermi level crosses both the upper and lower orbital bands. We find that the system shows two types of SC phases, the SC \Roman{u'-large} for $U>U'$ and …
We report systematic $^{75}$As NMR studies on LaFeAs(O$_{1-x}$F$_{x}$) ($0\le x\le0.14$). At $x=0.04$ near the phase boundary, from resistivity, spin-lattice relaxation rate $1/T_1$, and NMR spectrum measurements, we found weak magnetic order at $T_N\simeq 30$ K. Antiferromagnetic (AFM) fluctuations proved through $1/T_1$ are suppressed significantly with F-doping, and pseudogap behavior without pronounced AFM fluctuations is observed at $x=0.11$ where $T_c$ is maximum. This significant suppression of $1/T_1T$ upon F-doping while $T_c$ remains nearly unchanged suggests that low-energy AFM fluc…
We reexamine the novel phase diagrams of antiferromagnetism (AFM) and high-Tc$ superconductivity (HTSC) for a disorder-free CuO$_2$ plane based on an evaluation of local hole density ($p$) by site-selective Cu-NMR studies on multilayered copper oxides. Multilayered systems provide us with the opportunity to research the characteristics of the disorder-free CuO$_2$ plane. The site-selective NMR is the best and the only tool used to extract layer-dependent characteristics. Consequently, we have concluded that the uniform mixing of AFM and SC is a general property inherent to a single CuO$_2$ pla…
High-temperature (high-$T_{\rm c}$) superconductivity appears as a consequence of the carrier-doping of an undoped parent compound exhibiting antiferromagnetic order; thereby, ground-state properties of the parent compound are closely relevant to the superconducting state. On the basis of the concept, a spin-fluctuation has been addressed as an origin of pairing of the superconducting electrons in cuprates. Whereas, there is growing interest in the pairing mechanism such as an unconventional spin-fluctuation or an advanced orbital-fluctuation due to the characteristic multi-orbital system in i…
We report systematic 57Fe-NMR and 75As-NMR/NQR studies on an underdoped sample (T_c=20 K), an optimally doped sample (T_c=28 K), and an overdoped sample (T_c=22 K) of oxygen-deficient iron (Fe)-based oxypnictide superconductor LaFeAsO_{1-y}$. A microscopic phase separation between superconducting domains and magnetic domains is shown to take place in the underdoped sample, indicating a local inhomogeneity in association with the density distribution of oxygen deficiencies. As a result, 1/T_1T in the normal state of the superconducting domain decreases significantly upon cooling at both the Fe …
We perform transport measurements and band structure calculations of electron-doped LaFeAsO1-xHx over a wide range of x from 0.01 to 0.66. The T^2 and sqrt(T) dependency of the resistivity are observed at x ~ 0.17 and 0.41, respectively. The sign change of RH without opening of the spin-density-wave gap for 0.45 < x < 0.58 and T < TN as well as the calculated non-nested Fermi surface at x = 0.5 indicate the more localized nature of the AF2 as compared to spin density wave phase at non-doped sample. Considering the results from band calculations and the finite size of Hund' s rule coupling, the…
We have successfully prepared the new layered oxypnictides $Sr_4Sc_2O_6M_2As_2$ (M=Fe and Co). They adopt the tetragonal structure, being the same as that of $Sr_4Sc_2O_6Fe_2P_2$. The lattice constants are a=0.4045 nm and c= 0.5802 nm for M=Fe, and a=0.4045 nm and c=1.5695 nm for M=Co, respectively. Their transport and magnetic properties have been systematically studied. The temperature dependence of Hall coefficient and thermoelectric powder for $Sr_4Sc_2O_6Fe_2As_2$ compound show complicated behavior, similar to that of iron-based parent compounds LnOFeAs and $BaFe_2As_2$. It suggests that …
A new layered oxypnictide (Fe2P2)(Sr4Sc2O6) have been synthesized by solid-state reaction. This material has an alternating layer stacking structure of anti-fluorite Fe2P2 and perovskite-based Sr4Sc2O6 oxide layers. Space group of the material is P4/nmm and lattice constants a and c are 4.016 A and 15.543 A, respectively. The interlayer Fe-Fe distance corresponding to the c-axis length is the longest ever reported in the iron-based oxypnictide systems. In both magnetization and resistivity measurements, the present compound exhibited superconductivity below 17 K, which is much higher than that…
Iron-based oxypnictides substituted with yttrium have been prepared via a conventional solid state reaction. The product after first 50 hours of reaction showed diamagnetic-like transition at around 10 K but was not superconducting, while additional 72 hours of high temperature heat treatment was required to yield superconducting sample which was doped with fluoride. Temperature dependence of the susceptibility shows both screening and Meissner effect at around 10 K, while resistance as a function of temperature displayed a drop at around the same temperature.
The synthesis, structural and physical properties of iron lanthanide oxypnictide superconductors, L4Fe2As2Te1-xO4 (L = Pr, Sm, Gd), with transition temperature at ~ 25 K are reported. Single crystals have been grown at high pressure using cubic anvil technique. The crystal structure consists of layers of L2O2 tetrahedra separated by alternating layers of chains of Te and of Fe2As2 tetrahedra: -L2O2-Te-L2O2-Fe2As2-L2O2-Te-L2O2- (space group: I4/mmm, a ~ 4.0, c ~ 29.6 Å). Substitution of oxygen by fluorine increases the critical temperature, e.g. in Gd4Fe2As2Te1-xOyF4-y up to 45 K. Magnetic torq…
In the family of the iron-based superconductors, the $RE$FeAsO-type compounds (with $RE$ being a rare-earth metal) exhibit the highest bulk superconducting transition temperatures ($T_{\mathrm{c}}$) up to $55\ \textrm{K}$ and thus hold the key to the elusive pairing mechanism. Recently, it has been demonstrated that the intrinsic electronic structure of SmFe$_{0.92}$Co$_{0.08}$AsO ($T_{\mathrm{c}}=18\ \textrm{K}$) is highly nontrivial and consists of multiple band-edge singularities in close proximity to the Fermi level. However, it remains unclear whether these singularities are generic to th…
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 …
Effective low-energy Hamiltonians for several different families of iron-based superconductors are compared after deriving them from the downfolding scheme based on first-principles calculations. Systematic dependences of the derived model parameters on the families are elucidated, many of which are understood from the systematic variation of the covalency between Fe-3d and pnictogen-/chalcogen-p orbitals.
In the family of iron-based superconductors, LaFeAsO-type materials possess the simplest electronic structure due to their pronounced two-dimensionality. And yet they host superconductivity with the highest transition temperature Tc=55K. Early theoretical predictions of their electronic structure revealed multiple large circular portions of the Fermi surface with a very good geometrical overlap (nesting), believed to enhance the pairing interaction and thus superconductivity. The prevalence of such large circular features in the Fermi surface has since been associated with many other iron-base…
We discuss the role of striction in the intertwined magnetic and structural phase transitions in the underdoped iron-pnictides. The magneto-elastic coupling to acoustic modes is then derived and estimated in framework of the multiband spectrum for itinerant electrons with nesting features. We argue that the 1-st order character of the magneto-elastic phase transition originates from the lattice instabilities near the onset of spin-density wave order introducing, thus, a shear acoustic mode as a new order parameter. Taking non-harmonic termis in the lattice energy into account may explain the s…
We investigate the magnetic phase diagram of the newly discovered iron-based high temperature oxypnictide superconductors of the type RO$_{1-x}$F$_x $FeAs, with rare earths R=La, Sm, Nd, Pr and Ce by means of {\it ab initio} SGGA and SGGA+U density functional computations. We find undoped LaOFeAs to be a Mott insulator when incorporating electronic correlations via SGGA+U for any physically relevant value of $U$. The doped compounds are according to SGGA conductors with a transition from an antiferromagnetic to a non-magnetic state at a hole doping of concentration $x_c$=0.075 for R=Nd, Pr and…
We report plane-polarized Raman scattering spectra of iron oxypnictide superconductor NdFeAsO$_{1-x}$F$_x$ single crystals with varying fluorine $x$ content. The spectra exhibit sharp and symmetrical phonon lines with a weak dependence on fluorine doping $x$. The temperature dependence does not show any phonon anomaly at the superconducting transition. The Fe related phonon intensity shows a strong resonant enhancement below 2 eV. We associate the resonant enhancement to the presence of an interband transition around 2 eV observed in optical conductivity. Our results point to a rather weak cou…
Fluoride-doped iron-based oxypnictides containing rare-earth gadolinium (GdFeAsO0.8F0.2) and co-doping with yttrium (Gd0.8Y0.2FeAsO0.8F0.2) have been prepared via conventional solid state reaction at ambient pressure. The non-yttrium substituted oxypnictide show superconducting transition as high as 43.9 K from temperature dependent resistance measurements with the Meissner effect observed at a lower temperature of 40.8 K from temperature dependent magnetization measurements. By replacing a small amount of gadolinium with yttrium Tc was observed to be lowered by 10 K which might be caused by a…
Iron-based superconductors have grown to be a new continent of high Tc superconductors comparable to cuprates. The optimal critical temperature (Tc) of 56 K in electron-doped 1111-type iron oxypnictides attracts considerable attention of physicists and chemists. Carrier doping is not only essential to induce superconductivity but also is a critical parameter that governs the electronic, magnetic, and crystallographic properties of ground states in high-Tc superconductors. Hydride ion (H-) which is an anionic state of hydrogen acts as an efficient electron donor in the 1111-type, leading to sev…
The 1111-type iron arsenide hydride CaFe1-xCoxAsH was synthesized by high-pressure solid-state reaction, and its electronic structure and superconducting properties were investigated. Bulk superconductivity was observed at x = 0.07-0.26. A maximum superconducting critical temperature Tcmax of 23 K was observed at x = 0.07. These values are in agreement with those of CaFe1-xCoxAsF. The calculated Fermi surface of CaFeAsH has a small three-dimensional 3D hole pocket around the Gamma point. This is a result of weak covalent bonding between the As 4p and H 1s orbitals. No such covalency exists in …
We investigate interplay between magnetic fluctuations and superconductivity in the effective five-band Hubbard model for iron-oxypnictide superconductors on the basis of the fluctuation-exchange approximation. As for the normal-state properties, we find the pseudogap behavior in the NMR relaxation rate and the spectral weight in the electron-doped region, while we cannot find such behavior in the hole-doped region. The pseudogap behavior originates from the band structure effect, that is, existence of high density of states just below the Fermi level. Solving the superconducting Eliashberg eq…
We investigated the effects of phosphorus substitution on the shape of the Tc(x) dome in 1111-type SmFeAs1-yPyO1-xHx (0 < x < 0.5). Hydride ion substitution of oxide sites (O2- -> H-) exerts a chemical pressure effect, i.e., a structural reduction of the Pn-Fe-Pn angle α (Pn = P, As) and also dopes electrons into the FePn layer to induce superconductivity. Isovalent phosphorus substitution (P3- -> As3-) can induce only a chemical pressure effect, i.e., an increase of α for La-substitution of Sm-sites. As y increases from 0.0 to 0.5, the single Tc dome gradually splits into two domes, similar t…
We present results of ab-initio calculations of the electronic band structure, lattice dynamical properties, and elastic constants of LaOFeAs, the parent compound of the recently discovered superconducting iron-oxypnictide (LaO1-xFxFeAs). The total and partial electronic density of states (EDOS) of the undoped LaOFeAs (in the insulating or metallic state) are extracted from the electronic band structure. The phonon dispersion and the phonon density of states (PDOS) are also studied. Possible implications of the band structure, EDOS, and PDOS of LaOFeAs on the eventual appearance of high-Tc sup…
The iron-based oxypnictide superconductor SmFeAsO0.8F0.2 was synthesized under high-pressure and investigated by measuring dc magnetic susceptibility. The zero-field cooled (ZFC) magnetic susceptibility confirmed the bulk superconductivity of the sample with a critical temperature of Tc = 50 K and a significant jump in the magnetization at 4.3 K, usually attributed to the antiferromagnetic ordering of Sm3+ ions in this system. Since the occurrence of the jump depends on the cooling history, our data strongly suggest a spin-glass-like behaviour.
The recent discovery of superconductivity in the so-called iron-oxypnictide family of compounds has generated intense interest. The layered crystal structure with transition metal ions in planar square lattice form and the discovery of spin-density-wave order near 130 K seem to hint at a strong similarity with the copper oxide superconductors. A burning current issue is the nature of the ground state of the parent compounds. Two distinct classes of theories have been put forward depending on the underlying band structures: local moment antiferromagnetic ground state for strong coupling approac…
The occurrence of high temperature superconductivity, and the competition with magnetism, in stoichiometric and doped LaOFeAs and isostructural iron-oxypnictides is raising many fundamental questions about the electronic structure and magnetic interactions in this class of materials. There are now sufficient experimental data that it may be possible to identify the important issues whose resolution will lead to the understanding of this system. In this paper we address a number of the important issues. One important characteristic is the Fe-As distance (or more abstractly the pnictogen (Pn) he…
