Elastic neutron scattering studies of an optimized LaFeAsO single crystal reveal that upon cooling, an onset of the tetragonal (T)-to-orthorhombic (O) structural transition occurs at $T_\texttt{S} \approx 156$ K, and it exhibits a sharp transition at $T_\texttt{P} \approx 148$ K. We argue that in the temperature range $T_\texttt{S}$ to $T_\texttt{P}$, T and O structures may dynamically coexist possibly due to nematic spin correlations recently proposed for the iron pnictides, and we attribute $T_\texttt{P}$ to the formation of long-range O domains from the finite local precursors. The antiferromagnetic structure emerges at $T_\texttt{N} \approx 140$ K, with the iron moment direction along the O \emph{a} axis. We extract the iron magnetic form factor and use the tabulated $\langle j_0\rangle$ of Fe, Fe$^{2+}$ and Fe$^{3+}$ to obtain a magnetic moment size of $\sim$0.8 $μ_\texttt{B}$ at 9.5 K.
By using variational Monte Carlo method, we examine an effective low-energy model for LaFeAsO derived from an ab initio downfolding scheme. We show that quantum and many-body fluctuations near a quantum critical point largely reduce the antiferromagnetic (AF) ordered moment and the model not only quantitatively reproduces the small ordered moment in LaFeAsO, but also explains the diverse dependence on LaFePO, BaFe2As2 and FeTe. We also find that LaFeAsO is under large orbital fluctuations, sandwiched by the AF Mott insulator and weakly correlated metals. The orbital fluctuations and Dirac-cone…
We report 19-F NMR investigation of the new high temperature superconductor LaFeAsO(0.89)F(0.11) (Tc ~ 28K). We demonstrate that low frequency spin fluctuations exhibit pseudo gap behavior above Tc. We also deduce the London penetration depth lambda from NMR line broadening below Tc.
We present calculations of structural and magnetic properties of the iron-pnictide superconductor LaFeAsO including electron-electron correlations. For this purpose we apply a fully charge self-consistent combination of Density-Functional Theory with the Dynamical Mean-Field theory, allowing for the calculation of total energies. We find that the inclusion of correlation effects gives a good agreement of the Arsenic z position with experimental data even in the paramagnetic (high-temperature) phase. Going to low temperatures, we study the formation of the ordered moment in the striped spin-den…
Hydrogen (H)-doped LaFeAsO is a prototypical iron-based superconductor. However, its phase diagram extends beyond the standard framework, where a superconducting (SC) phase follows an antiferromagnetic (AF) phase upon carrier doping; instead, the SC phase is sandwiched between two AF phases appearing in lightly and heavily H-doped regimes. We performed nuclear magnetic resonance (NMR) measurements under pressure, focusing on the second AF phase in the heavily H-doped regime. The second AF phase is strongly suppressed when a pressure of 3.0 GPa is applied, and apparently shifts to a highly H-do…
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…
Two families of high temperature superconductors whose critical temperatures are higher than 50K are known. One is the copper oxides and the other is the iron-based superconductors. Comparisons of mechanisms between these two in terms of common ground as well as distinctions will greatly help in searching for higher Tc superconductors. However, studies on mechanisms for the iron family based on first principles calculations are few. Here we first show that the superconductivity emerges in the state-of-the-art numerical calculations for an ab initio multi-orbital model of an electron-doped iron…
The nature and value of the order parameters (OPs) in the superconducting Fe-based oxypnictides REFeAsO_(1-x)F_x (RE = rare earth) are a matter of intense debate, also connected to the pairing mechanism which is probably unconventional. Point-contact Andreev-reflection experiments on LaFeAsO_(1-x)F_x gave us direct evidence of three energy scales in the superconducting state: a nodeless superconducting OP, Delta1 = 2.8-4.6 meV, which scales with the local Tc of the contact; a larger unconventional OP that gives conductance peaks at 9.8-12 meV, apparently closes below Tc and decreases on increa…
Epitaxial thin films of LaFeAsO were fabricated on MgO (001) and mixed-perovskite (La, Sr)(Al, Ta)O3 (001) single-crystal substrates by pulsed laser deposition using a Nd:YAG second harmonic source and a 10 at.% F-doped LaFeAsO disk target. Temperature dependences of the electrical resistivities showed no superconducting transition in the temperature range of 2-300 K, and were similar to those of undoped polycrystalline bulk samples. The transmittance spectrum exhibited a clear peak at ~0.2 eV, which is explained by ab-initio calculations.
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}$. A microscopic phase separation between superconducting domains and magnetic domains is shown to take place in the underdoped sample, indicating a local inhomogeneity in association with the density distribution of oxygen deficiencies. As a result, 1/T_1T in the normal state of the superconducting domain decreases significantly upon cooling at both the Fe …
Effective Hamiltonians for LaFeAsO and LaFePO are derived from the downfolding scheme based on first-principles calculations and provide insights for newly discovered superconductivity in the family of LnFeAsO$_{1-x}$F$_x$, Ln = La, Ce, Pr, Nd, Sm, and Gd. Extended Hubbard Hamiltonians for five maximally localized Wannier orbitals per Fe are constructed dominantly from five-fold degenerate iron-3$d$ bands. They contain parameters for effective Coulomb and exchange interactions screened by the polarization of other electrons away from the Fermi level. The onsite Coulomb interaction estimated as…
We have studied the interplay of magnetism and superconductivity in LaFeAsO$_{1-x}$F$_x$ and Ca(Fe$_{1-x}$Co$_x$)$_2$As$_2$. While antiferromagnetic spin density wave formation is suppressed and superconductivity evolves, all samples show a doping independent strong increase of the normal state susceptibility upon heating which appears a general feature of iron pnictides. The data provide evidence for robust local antiferromagnetic correlations persisting even in the superconducting regime of the phase diagram.
An iron-based superconductor LaFeAsO$_{1-x}$H$_x$ (0 $\leq x \leq$ 0.6) undergoes two antiferromagnetic (AF) phases upon H doping. We investigated the second AF phase ($x$=0.6) using NMR techniques under pressure. At pressures up to 2 GPa, the ground state is a spin-density-wave state with a large gap; however, the gap closes at 4.0 GPa, suggesting a pressure-induced quantum critical point. Interestingly, the gapped excitation coexists with gapless magnetic fluctuations at pressures between 2 and 4 GPa. This coexistence is attributable to the lift up of the $d_{xy}$ orbital to the Fermi level,…
We study how Co- and Ni-substitution affect the electronic structure of the iron-based superconductor, LaFeAsO. We perform {\it ab initio} supercell calculations and unfold the first Brillouin zone (BZ) to calculate the spectral function in the BZ for the normal cell. The charge density distribution in real space shows that doped extra electrons are trapped around Co (Ni) atom. This seems to mean that Co(Ni)-substitution does not work as carrier doping. However, the present momentum-space analysis indicates that the Fermi-surface volume indeed expands by substitutions, which can be well descri…
We have measured element-specific Fe-phonon densities of states (Fe-PDOS) of LaFeAsO_{1-x}F_{x} (x = 0, 0.11) and La_{1-x}Ca_{x}FePO (x = 0.13) by using nuclear resonant inelastic scattering of synchrotron radiation. The Fe-PDOS of superconductor LaFeAsO_{0.89}F_{0.11} (Tc = 26 K) and that of non-superconductor LaFeAsO have similar structures to both below Tc (15 K) and above Tc (298 K) and, therefore, fluorine doping does not have notable effect on the Fe-PDOS. As for the superconductor La_{0.87}Ca_{0.13}FePO (Tc = 5.4K), the entire structure of Fe-PDOS resembles with that of LaFeAsO_{1-x}F_{…
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…
A puzzle in the iron-based superconductor LaFeAsO_{1-x}F_x is that the magnetic moment obtained by first-principle electronic structure calculations is unexpectedly much larger than the experimentally observed one. For example, the calculated value is ~ 2.0 μ_B in the mother compound, while it is ~ 0.3 μ_B in experiments. We find that the puzzle is solved within the framework LDA + U by expanding the U value into a slightly negative range. We show U dependence of the obtained magnetic moment in both the undoped x=0.0 and doped x = 0.125. These results reveal that the magnetic moment is drastic…
By using a two-step method, we successfully synthesized the iron based new superconductor LaFeAsO_{0.9}F_{0.1-δ}$. The resistive transition curves under different magnetic fields were measured, leading to the determination of the upper critical field Hc2(T) of this new superconductor. The value of Hc2 at zero temperature is estimated to be about 50 Tesla roughly. In addition, the Hall effect and magnetoresistance were measured in wide temperature region. A negative Hall coefficient R_H has been found, implying a dominant conduction mainly by electron-like charge carriers in this material. The …
We present an approach that combines the local density approximation (LDA) and the dynamical mean-field theory (DMFT) in the framework of the full-potential linear augmented plane waves (FLAPW) method. Wannier-like functions for the correlated shell are constructed by projecting local orbitals onto a set of Bloch eigenstates located within a certain energy window. The screened Coulomb interaction and Hund's coupling are calculated from a first-principle constrained RPA scheme. We apply this LDA+DMFT implementation, in conjunction with continuous-time quantum Monte-Carlo, to study the electroni…
For a newly discovered iron-based high $T_c$ superconductor LaFeAsO$_{1-x}$F$_x$, we have constructed a minimal model, where inclusion of all the five Fe $d$ bands is found to be necessary. Random-phase approximation is applied to the model to investigate the origin of superconductivity. We conclude that the multiple spin fluctuation modes arising from the nesting across the disconnected Fermi surfaces realize an extended s-wave pairing, while d-wave pairing can also be another candidate.
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…
Nuclear magnetic resonance (NMR) measurements of an iron (Fe)-based superconductor LaFeAsO_{1-x}F_x (x = 0.08 and 0.14) were performed at ambient pressure and under pressure. The relaxation rate 1/T_1 for the overdoped samples (x = 0.14) shows T-linear behavior just above T_c, and pressure application enhances 1/T_1T similar to the behavior of T_c. This implies that 1/T_1T = constant originates from the Korringa relation, and an increase in the density of states at the Fermi energy D(E_F) leads to the enhancement of T_c. In the underdoped samples (x = 0.08), 1/T_1T measured at ambient pressure…
LDA+DMFT (Local Density Approximation combined with Dynamical Mean-Field Theory) computation scheme has been used to calculate spectral properties of LaFeAsO -- the parent compound for new high-T$_c$ iron oxypnictides. Coulomb repulsion $U$ and Hund's exchange $J$ parameters for iron 3d electrons were calculated using \textit {first principles} constrained density functional theory scheme in Wannier functions formalism. Resulting values strongly depend on the number of states taken into account in calculations: when full set of O-$2p$, As-$4p$, and Fe-3d orbitals with corresponding bands are i…
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…
Millimeter-sized single crystals of LaFeAsO, LaFeAsO1-xFx, and LaFe1-xCoxAsO were grown in NaAs flux at ambient pressure. The detailed growth procedure and crystal characterizations are reported. The as-grown crystals have typical dimensions of 3 * 4 * 0.05-0.3 mm3 with the crystallographic c-axis perpendicular to the plane of the plate-like single crystals. Some crystals manifest linear dimensions as large as 4-5 mm. X-ray and neutron single crystal scattering confirmed that LaFeAsO crystals exhibit a structural phase transition at Ts ~ 154 K and a magnetic phase transition at TSDW ~ 140 K. T…
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.
We report the results of $^{77}$Se--nuclear magnetic resonance (NMR) in $α$-FeSe, which exhibits a similar crystal structure to the LaFeAsO$_{1-x}$F$_x$ superconductor and shows superconductivity at 8 K. The nuclear-spin lattice relaxation rate $1/T_1$ shows $T^3$ behavior below the superconducting transition temperature $T_c$ without a coherence peak. The $T_1T=$ const. behavior, indicative of the Fermi liquid state, can be seen in a wide temperature range above $T_c$. The superconductivity in $α$-FeSe is also an unconventional one as well as LaFeAsO$_{1-x}$F$_x$ and related materials. The Fe…
Iron arsenide superconductors based on the material LaFeAsO1-xFx are characterized by a two-dimensional Fermi surface (FS) consisting of hole and electron pockets yielding structural and antiferromagnetic transitions at x = 0. Electron doping by substituting O2- with F- suppresses these transitions and gives rise to superconductivity with a maximum Tc = 26 K at x = 0.1. However, the over-doped region cannot be accessed due to the poor solubility of F- above x = 0.2. Here we overcome this problem by doping LaFeAsO with hydrogen. We report the phase diagram of LaFeAsO1-xHx (x < 0.53) and, in add…
Photoemission spectroscopy is used to investigate the electronic structure of the newly discovered iron-based superconductors LaFeAsO_{1-x}F_x and LaFePO_{1-x}F_x. Line shapes of the Fe 2p core-level spectra suggest an itinerant character of Fe 3d electrons. The valence-band spectra are generally consistent with band-structure calculations except for the shifts of Fe 3d-derived peaks toward the Fermi level. From spectra taken in the Fe 3p -> 3d core-absorption region, we have obtained the experimental Fe 3d partial density of states, and explained it in terms of a band-structure calculation wi…
The electronic structures of the iron-based superconductors have been intensively studied by using angleresolved photoemission spectroscopy (ARPES). A considerable amount of research has been focused on the LaFeAsO family, showing the highest transition temperatures, where previous ARPES studies have found much larger Fermi surfaces than bulk theoretical calculations would predict. The discrepancy has been attributed to the presence of termination-dependent surface states. Here, using photoemission spectroscopy with a sub-micron focused beam spot (nano-ARPES) we have successfully measured the …
An optimally doped iron-based superconductor LaFeAsO$_{0.92}$F$_{0.08}$ with $T_c = 29$ K has been studied by inelastic powder neutron scattering. The magnetic excitation at $Q=1.15$ Å$^{-1}$ is enhanced below $T_c$, leading to a peak at $E_{res}\sim13$ meV as the resonance mode, in addition to the formation of a gap at low energy below the crossover energy $Δ_{c}\sim10 meV$. The peak energy at $Q=1.15$ Å$^{-1}$ corresponds to $5.2 k_B T_c$ in good agreement with the other values of resonance mode observed in the various iron-based superconductors, even in the high-$T_c$ cuprates. Although the…
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 measured the electronic structure of an iron arsenic parent compound LaFeAsO using angle resolved photoemission spectroscopy (ARPES). By comparing with a full-potential Linear Augmented PlaneWave calculation we show that the extra large Gamma hole pocket measured via ARPES comes from electronic structure at the sample surface. Based on this we discuss the strong polarization dependence of the band structure and a temperature-dependent hole-like band around the M point. The two phenomena give additional evidences for the existence of the surface-driven electronic structure.
We discuss the novel superconducting characteristics and unusual normal-state properties of iron (Fe)-based pnictide superconductors REFeAsO$_{1-y}$ (RE=La,Pr,Nd) and Ba$_{0.6}$K$_{0.4}$Fe$_2$As$_2$($T_{c}=$ 38 K) by means of $^{57}$Fe-NMR and $^{75}$As-NQR/NMR. In the superconducting state of LaFeAsO$_{0.7}$ ($T_{c}=$ 28 K), the spin component of the $^{57}$Fe-Knight shift decreases to almost zero at low temperatures, which provide firm evidence of the superconducting state formed by spin-singlet Cooper pairing. The nuclear spin-lattice relaxation rates $(1/T_{1})$ in LaFeAsO$_{0.7}$ and Ba$_…
The wave-vector (q) and doping dependences of the magnetic energy, iron moment, and effective exchange interactions in LaFeAsO, BaFe2As2, and SrFe2As2\ are studied by self-consistent LSDA calculations for co-planar spin spirals. For the undoped compounds, the calculated total energy, E(q), reaches its minimum at q corresponding to stripe anti-ferromagnetic order. In LaFeAsO, this minimum becomes flat already at low levels of electron-doping and shifts to an incommensurate q at delta=0.2, where delta is the number of additional electrons (delta>0) or holes (delta<0) per Fe. In BaFe2As2 and SrFe…
We determine the nature of the magnetic quantum critical point in the doped LaFeAsO using a set of constrained density functional calculations that provide ab initio coefficients for a Landau order parameter analysis. The system turns out to be remarkably close to a quantum tricritical point, where the nature of the phase transition changes from first to second order. We compare with the effective field theory and discuss the experimental consequences.
We have investigated the electronic structure of LaFeAsO$_{1-x}$F$_{x}$ (x = 0; 0.1; 0.2) by angle-integrated photoemission spectroscopy and local density approximation (LDA) based band structure calculations. The valence band consists of a low energy peak at E = -0.25 eV and a broad structure around E = -5 eV in qualitative agreement with LDA. From the photon energy dependence of these peaks we conclude that the former derives almost exclusively from Fe 3d states. This constitutes experimental evidence for the strong iron character of the relevant states in a broad window around EF and confir…
The newly discovered iron-based superconductors have triggered renewed enormous research interest in the condensed matter physics community. Nuclear magnetic resonance (NMR) is a low-energy local probe for studying strongly correlated electrons, and particularly important for high-$T_{\rm C}$ superconductors. In this paper, we review NMR studies on the structural transition, antiferromagnetic order, spin fluctuations, and superconducting properties of several iron-based high-$T_{\rm C}$ superconductors, including LaFeAsO$_{1-x}$F$_x$, LaFeAsO$_{1-x}$, BaFe$_2$As$_2$, Ba$_{1-x}$K$_x$Fe$_2$As$_2…
Inelastic neutron scattering measurements demonstrate that the magnetic interactions in antiferromagnetic LaFeAsO are two-dimensional. Spin wave velocities within the Fe layer and the magnitude of the spin gap are similar to the \textit{A}Fe$_2$As$_2$ based materials. However, the ratio of interlayer and intralayer exchange is found to be less than $\sim 10^{-4}$ in LaFeAsO, very similar to the cuprates, and $\sim$ 100 times smaller than that found in \textit{A}Fe$_2$As$_2$ compounds. The results suggest that the effective dimensionality of the magnetic system is highly variable in the parent …
Orbital polarization and electronic correlation are two essential aspects in understanding the normal state and superconducting properties of multiorbital FeAs-based superconductors. In this Letter, we present a systematical study on the orbital polarization of iron pnictides from weak to strong Coulomb correlations within the KRSB approach. The magnetic phase diagram of the two-orbital model for LaFeAsO clearly shows that the striped antiferromagnetic metallic phase with considerable orbital polarization exists over a wide doping range. The reversal of the orbital polarization occurs in the i…
High temperature superconductivity is often found in the vicinity of antiferromagnetism. This is also true in LaFeAsO$_{1-x}$F$_{x}$ ($x \leq$ 0.2) and many other iron-based superconductors, which leads to proposals that superconductivity is mediated by fluctuations associated with the nearby magnetism. Here we report the discovery of a new superconductivity dome without low-energy magnetic fluctuations in LaFeAsO$_{1-x}$F$_{x}$ with 0.25$\leq x \leq$0.75, where the maximal critical temperature $T_c$ at $x_{opt}$ = 0.5$\sim$0.55 is even higher than that at $x \leq$ 0.2. By nuclear magnetic res…
To examine the role of magnetism in superconductivity of iron-based superconductors, we first present first-principles optical calculations on three representative parent compounds: LaFeAsO, BaFe2As2 and LiFeAs. Both nonmagnetic (NM) and spin-density wave (SDW) with striped antiferromagnetic order are considered. Due to their layer structure, these compounds in NM states show anomalously large optical anisotropy with a conductivity ratio $σ_{zz}/σ{xx}$ as large as 313% in LaFeAsO and 530% in LiFeAs. Interestingly the giant optical anisotropy is significantly suppressed by SDW. On the other han…
We present results from a detailed experimental investigation of LaFeAsO, the parent material in the series of "FeAs" based oxypnictide superconductors. Upon cooling this material undergoes a tetragonal-orthorhombic crystallographic phase transition at ~160 K followed closely by an antiferromagnetic ordering near 145 K. Analysis of these phase transitions using temperature dependent powder X-ray and neutron diffraction measurements is presented. A magnetic moment of ~0.35 Bohr magnetons per iron is derived from Mossbauer spectra in the low temperature phase. Evidence of the structural transiti…
Electronic and magnetic properties of the heavily H-doped LaFeAsO$_{1-x}$H$_x$ $(x\sim0.5 )$ were studied in the framework of the density functional theory combined with the dynamical mean field theory (DFT+DMFT). We found a stripe-like-ordered structure of hydrogen and oxygen atoms, as a ground state, with the same configuration as the antiferromagnetic (AF) order. The new configuration could explain the existing experimental results related to the heavily H-doped LaFeAsO$_{1-x}$H$_x$, such as an in-plane electronic anisotropy and a non-uniform magnetic behavior. A significant anisotropy was …
Recent several experiments revealed that novel bipartite magnetic/superconducting phases widely exist in iron pnictides and chalcogenides. Nevertheless, the origin of the two-dome superconducting phases in iron-based compounds still remains unclear. Here we theoretically investigated the electronic structures, magnetic and superconducting properties of three representative iron-based systems, i.e. LaFeAsO1-xHx, LaFeAs1-xPxO and KFe2As2. We found that in addition to the degenerate in-plane anisotropic xz/yz orbitals, the quasi-degenerate in-plane isotropic orbitals drive these systems entering …
The ternary iron arsenide BaFe2As2 with the tetragonal ThCr2Si2-type structure exhibits a spin density wave (SDW) anomaly at 140 K, very similar to LaFeAsO, the parent compound of the iron arsenide superconductors. BaFe2As2 is a poor Pauli-paramagnetic metal and undergoes a structural and magnetic phase transition at 140 K, accompanied by strong anomalies in the specific heat, electrical resistance and magnetic susceptibility. In the course of this transition, the space group symmetry changes from tetragonal (I4/mmm) to orthorhombic (Fmmm). 57Fe Moessbauer spectroscopy experiments show a singl…
The wave-vector q and doping (x,y) dependences of the magnetic energy, iron moment, and effective exchange interactions in LaFeAsO{1-x}F{x} and Ba{1-2y}K{2y}Fe2As2 are studied by self-consistent LSDA calculations for co-planar spin spirals. For the undoped compounds (x=0, y=0), the minimum of the calculated total energy, E(q), is for q corresponding to stripe antiferromagnetic order. Already at low levels of electron doping (x), this minimum becomes flat in LaFeAsO{1-x}F{x} and for x>=5, it shifts to an incommensurate q. In Ba{1-2y}K{2y}Fe2As2, stripe order remains stable for hole doping up to…
While for a long time iron based superconductors have been investigated looking at the average crystalline structure there is now growing interest on the divergence of local from the average structure. Here we use advanced data analysis of EXAFS, a fast and local probe, which has key advantages compared to crystallographic measurements, in unveiling the dynamics of the local structure. The results show that the Fe-As pair oscillates in the double-well potential both in undoped and in cobalt doped LaFeAsO crystals. The parameters and the characteristics of the double-well potential are determin…
Orbital ordering has recently emerged as another important state in iron based superconductors, and its role for superconductivity as well as its connection to magnetic order and orthorhombic lattice distortion are heavily debated. In order to search for signatures of this so-called nematic phase in oxypnictides, we revisit the normal state properties of the pnictide superconductor LaFeAsO$_{1-x}$F$_x$ with a focus on resistivity, Nernst effect, thermal expansion, and $^{75}$As NMR data. The transport properties at the underdoped level $x=0.05$ exhibit pronounced anomalies at about the same te…
The electron-doped high-transition-temperature (T_c) iron-based pnictide superconductor LaFeAsO_{1-x}H_x has a unique phase diagram: superconducting (SC) double domes are sandwiched by antiferromagnetic phases at ambient pressure and they turn to a single dome with a maximum T_c that exceeds 45K at a pressure of 3.0 GPa. We studied whether spin fluctuations are involved in increasing T_c under a pressure of 3.0 GPa by using ^{75}As nuclear magnetic resonance (NMR) technique. The ^{75}As-NMR results for the powder samples show that T_c increases up to 48 K without the influence of spin fluctuat…
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…
The evolution of low-energy spin dynamics in the iron-based superconductor LaFeAsO$_{1-x}$F$_x$ was studied over a broad doping, temperature, and magnetic field range (x = 0 - 0.15, T up to 480K, H up to 30T) by means of As nuclear magnetic resonance (NMR). An enhanced spin-lattice relaxation rate divided by temperature, 1/T1T, in underdoped superconducting samples (x = 0.045, 0.05 and 0.075) suggests the presence of antiferromagnetic spin fluctuations, which are strongly reduced in optimally-doped (x = 0.10) and completely absent in overdoped (x = 0.15) samples. In contrast to previous analys…
We study superconductivity in the two-dimensional 16-band d-p model extracted from a tight-binding fit to the band structure of LaFeAsO, using the random phase approximation. When the intraorbital repulsion U is larger than the interorbital one U', an extended s-wave (s+--wave) pairing with sign reversal of order parameter is mediated by antiferromagnetic spin fluctuations, while when U<U' another kind of s-wave (s++-wave) pairing without sign reversal is mediated by ferro-orbital fluctuations. The s++-wave pairing is enhanced due to the electron-phonon coupling and then can be expanded over t…
The new quaternary iron arsenide-fluoride SrFeAsF with the tetragonal ZrCuSiAs-type structure was synthesized and the crystal structure was determined by X-ray powder diffraction (P4/nmm, a = 399.30(1), c = 895.46(1) pm). SrFeAsF undergoes a structural and magnetic phase transition at 175 K, accompanied by strong anomalies in the specific heat, electrical resistance and magnetic susceptibility. In the course of this transition, the space group symmetry changes from tetragonal (P4/nmm) to orthorhombic (Cmme). 57Fe Moessbauer spectroscopy experiments show a single signal at room temperature at a…
We study the condition for optimizing superconductivity in the iron pnictides from the lattice structure point of view. Studying the band structure of the hypothetical lattice structure of LaFeAsO, the hole Fermi surface multiplicity is found to be maximized around the Fe-As-Fe bond angle regime where the arsenic atoms form a regular tetrahedron. Superconductivity is optimized within this three hole Fermi surface regime, while the stoner factor of the antiferromagnetism has an overall tendency of increasing upon decreasing the bond angle. Combining also the effect of the varying the Fe-As bond…
For the iron-based high $T_c$ superconductor LaFeAsO$_{1-x}$F$_x$, we construct a minimal model, where all of the five Fe $d$ bands turn out to be involved. We then investigate the origin of superconductivity with a five-band random-phase approximation by solving the Eliashberg equation. We conclude that the spin fluctuation modes arising from the nesting between the disconnected Fermi pockets realise, basically, an extended s-wave pairing, where the gap changes sign across the nesting vector.
The role of nematic fluctuations for unconventional superconductivity has been subject of intense discussions for many years. In iron-based superconductors, the most established probe for electronic-nematic fluctuations, i.e. the elastoresistivity seems to imply that superconductivity is reinforced by electronic-nematic fluctuations, since the elastoresistivity amplitude peaks at or close to optimal $T_C$. However, on the over-doped side of the superconducting dome, the diminishing elastoresistivity suggests a negligible importance in the mechanism of superconductivity. Here we introduce the N…
We present a systematic ab initio study based on density-functional calculations to understand impurity effects in iron-based superconductors. Effective tight-binding Hamiltonians for the d-bands of LaFeAsO with various transition-metal impurities such as Mn, Co, Ni, Zn, and Ru are constructed using maximally-localized Wannier orbitals. Local electronic structures around the impurity are quantitatively characterized by their onsite potential and transfer hoppings to neighboring sites. We found that the impurities are classified into three groups according to the derived parameters: For Mn, Co,…
We study hydrogen doping effects in an iron-based superconductor LaFeAsO_(1-y) by using the first-principles calculation and explore the reason why the superconducting transition temperature is remarkably enhanced by the hydrogen doping. The present calculations reveal that a hydrogen cation stably locating close to an iron atom attracts a negatively-charged FeAs layer and results in structural distortion favorable for further high temperature transition. In fact, the lattice constant a averaged over the employed supercell shrinks and then the averaged As-Fe-As angle approaches 109.74 degrees …
