The ongoing search for new superconductors has recently yielded a new family of oxypnictides composed of alternating La_2O_{2-x}F_x and Fe_2As_2 layers [1-4] with transition temperatures T_c of 25-28 K, which can be raised to 40-43 K by replacing La with Ce [5] or Sm [6] or to 52 K by replacing La with Nd and Pr [7, 8]. Recent experiments and band structure calculations have suggested an unconventional multiband superconductivity in the layers of paramagnetic Fe ions, which would normally destroy superconductivity in the traditional mechanism of the s-wave Cooper pairing. Here we report very high-field resistance measurements up to 45T, which show a remarkable enhancement of the upper critical fields B_c2 at low temperatures, as compared to those expected from the already high slopes of dB_c2/dT ~ 2T/K near T_c . The deduced B_c2(0) ~ 63-65 T exceeds the paramagnetic limit, consistent with strong coupling and important two-band effects in LaFeAsO_0.89F_0.11. We argue that oxypnictides are emerging as a new class of high-field superconductors surpassing the B_c2 of Nb_3Sn, MgB_2, and the Chevrel phases and perhaps approaching the 100T field benchmark of the high-T_c cuprates.
Electrical resistivity measurements under high pressures up to 29 GPa were performed for oxypnictide compound LaFeAsO. We found a pressure-induced superconductivity in LaFeAsO. The maximum value of Tc is 21 K at ~12 GPa. The pressure dependence of the Tc is similar to those of LaFeAsO1-xFx series reported previously.
Here we report the superconductivity in the LaFeAsO1-xFx system prepared by high pressure synthesis. The highest onset superconducting transition temperature (Tc) in this La-based system is 41.0 K with the nominal composition of LaFeAsO1-xFx (x = 0.6), which is higher than that reported previously by ambient pressure synthesis. The increase of Tc can be attributed to the further shrinkage of crystal lattice that causes the stronger chemical pressure on the Fe-As plane, which is induced by the increased F-doping level under high pressure synthesis.
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…
Low energy spin fluctuations are studied for the electron-doped Fe-based superconductor LaFeAsO(1-x)F(x) by inelastic neutron scattering up to the energy transfer of w = 15 meV using polycrystalline samples. Superconducting samples (x=0.057, Tc=25 K and x=0.082, Tc=29 K) show dynamical spin susceptibility chi"(w) almost comparable with the parent sample's. However chi"(w) is almost vanished in the x=0.158 sample where the superconductivity is highly suppressed. These results are compatible with the theoretical suggestions that the spin fluctuation plays an important role for the superconductiv…
Undoped LaFeAsO, parent compound of the newly found high-Tc superconductor, exhibits a sharp decrease in the temperature-dependent resistivity at ~160 K. The anomaly can be suppressed by F doping and the superconductivity appears correspondingly, suggesting a close associate of the anomaly with the superconductivity. We examined the crystal structures, magnetic properties and superconductivity of undoped (normal conductor) and 14 at.% F-doped LaFeAsO (Tc = 20 K) by synchrotron X-ray diffraction, DC magnetic measurements, and ab initio calculations to demonstrate that the anomaly is associated …
By a systematic study of the hydrogen-doped LaFeAsO system by means of dc resistivity, dc magnetometry, and muon-spin spectroscopy we addressed the question of universality of the phase diagram of rare-earth-1111 pnictides. In many respects, the behaviour of LaFeAsO_(1-x)H_(x) resembles that of its widely studied F-doped counterpart, with H^- realizing a similar (or better) electron-doping in the LaO planes. In a x = 0.01 sample we found a long-range SDW order with T_n = 119 K, while at x = 0.05 the SDW establishes only at 38 K and, below T_c = 10 K, it coexists at a nanoscopic scale with bulk…
The experimental observation of superconductivity in LaFeAsO appearing on doping is analyzed with the group-theoretical approach that evidently led in a foregoing paper (J. Supercond 24:2103, 2011) to an understanding of the cause of both the antiferromagnetic state and the accompanying structural distortion in this material. Doping, like the structural distortions, means also a reduction of the symmetry of the pure perfect crystal. In the present paper we show that this reduction modifies the correlated motion of the electrons in a special narrow half-filled band of LaFeAsO in such a way that…
We studied the electric and magnetic behavior near the phase boundary between antiferromagnetic (AF) and superconducting (SC) phases for a prototype of high-T_c pnictides LaFeAsO_{1-x}F_{x} by using nuclear magnetic resonance, and found that paramagnetic-metal (PM) domains segregate from AF domains. PM domains grow in size with increasing electron doping level and are accompanied by the onset of superconductivity, and thus application of pressure or increasing the doping level causes superconductivity. The existence of PM domains cannot be explained by the existing paradigm that focuses only o…
The 1111-type iron-based superconductor LnFeAsO1-xFx (Ln stands for lanthanide) is the first material with a Tc above 50 K, other than cuprate superconductors. Electron doping into LaFeAsO by H, rather than F, revealed a double-dome-shaped Tc-x diagram, with a first dome (SC1, 0.05<x<0.20) and a second dome (SC2, 0.2<x<0.5). Here, we report the Tc for the whole hydrogen-doping range in LaFeAsO1-xHx under pressures of up to 19 GPa. Tc rises to 52 K at 6 GPa for the Tc-valley composition between the two Tc domes. This is the first instance of the Tc exceeding 50 K in La-1111-type iron-based supe…
As-vacancies (V_As) in La-1111-systems, which are nominally non-magnetic defects, are shown to create in their vicinity by symmetry ferromagnetically oriented local magnetic moments due to the strong, covalent bonds with neighboring Fe atoms that they break. From microscopic theory in terms of an appropriately modified Anderson-Wolff model, we find that the moment formation results in a substantially enhanced paramagnetic susceptibility in both the normal and superconducting (SC) state. Despite the V_As act as magnetic scatterers, they do not deteriorate SC properties which can even be improve…
We observed a drastic Tc suppression caused by no more than 3 at.% of Zn doped to the optimized superconductor LaFeAsO0.85 (Tc = 26 K). The electrical resistivity and magnetic susceptibility measurements suggested that it is likely due to impurity scatterings rather than losing the metallic nature, seeming to support the s+/- pairing model proposed for the Fe pnictide superconductor.
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.
Here we report the synthesis and basic characterization of LaFe1-xCoxAsO for several values of x. The parent phase LaFeAsO orders antiferromagnetically (TN ~ 145 K). Replacing Fe with Co is expected to both electron dope the system and introduce disorder in the FeAs layer. For x = 0.05 antiferromagnetic order is destroyed and superconductivity is observed at Tconset = 11.2 K. For x = 0.11 superconductivity is observed at Tc(onset) = 14.3 K, and for x = 0.15 Tc = 6.0 K. Superconductivity is not observed for x = 0.2 and 0.5, but for x = 1, the material appears to be ferromagnetic (Tc ~ 56 K) as …
We argue that the newly discovered superconductivity in a nearly magnetic, Fe-based layered compound is unconventional and mediated by antiferromagnetic spin fluctuations, though different from the usual superexchange and specific to this compound. This resulting state is an example of extended s-wave pairing with a sign reversal of the order parameter between different Fermi surface sheets. The main role of doping in this scenario is to lower the density of states and suppress the pair-breaking ferromagnetic fluctuations.
The isostructural transition in the tetragonal phase, with sizable change in the anion-height, is realized in heavily H-doped LaFeAsO and (La,P) co-doped CaFe$_2$As$_2$. In these compounds, the superconductivity with higher-Tc (40~50 K) is realized near the isostructural transition. To reveal the origin of the anion-height instability and its important role in realizing the higher-Tc state, we develop the orbital-spin fluctuation theory by including the vertex correction. It is found that the non-nematic orbital fluctuations, which induce the anion-height instability, can develop near the magn…
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_{…
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…
We use neutron scattering to study the structural distortion and antiferromagnetic (AFM) order in LaFeAsO$_{1-x}$F$_{x}$ as the system is doped with fluorine (F) to induce superconductivity. In the undoped state, LaFeAsO exhibits a structural distortion, changing the symmetry from tetragonal (space group $P4/nmm$) to orthorhombic (space group $Cmma$) at 155 K, and then followed by an AFM order at 137 K. Doping the system with F gradually decreases the structural distortion temperature, but suppresses the long range AFM order before the emergence of superconductivity. Therefore, while supercond…
The Fe-based Oxypnicide superconductors have generated a huge amount of interest; they are a high temperature superconductor, with a Tc of 55K, but do not have the two dimensional copper oxygen layer that was thought essential for superconductivity at these high temperatures. Initial studies have hinted towards the possibility of a spin density wave (SDW) in these compounds and how they could play an important role in the superconductivity. SDW's occur at low temperatures in low-dimensional materials with strong electron correlations or in metals with a high density of states at the Fermi surf…
The electrical resistivity and Hall coefficient of LaFeAsO0.95F0.05 polycrystalline samples were measured in pulsed magnetic fields up to m0H = 60 T from room temperature to 1.5 K. The resistance of the normal state shows a negative temperature coefficient (dr/dT < 0) below 70 K for this composition, indicating insulating ground state in underdoped LaFeAsO system in contrast to heavily doped compound. The charge carrier density obtained from Hall effect can be described as constant plus a thermally activated term with an energy gap DE = 630 K. Upper critical field, Hc2, estimated from resistiv…
We report Zn-doping effect in the parent and F-doped LaFeAsO oxy-arsenides. Slight Zn doping in LaFe$_{1-x}$Zn$_{x}$AsO drastically suppresses the resistivity anomaly around 150 K associated with the antiferromagnetic (AFM) spin density wave (SDW) in the parent compound. The measurements of magnetic susceptibility and thermopower confirm further the effect of Zn doping on AFM order. Meanwhile Zn doping does not affect or even enhances the $T_c$ of LaFe$_{1-x}$Zn$_{x}$AsO$_{0.9}$F$_{0.1}$, in contrast to the effect of Zn doping in high-$T_c$ cuprates. We found that the solubility of Zn content …
To probe manifestations of multiband superconductivity in oxypnictides, we measured the angular dependence of the magnetic torque $τ(θ)$ in the mixed state of LaO$_{0.9}$F$_{0.1}$FeAs single crystals as a function of temperature $T$ and magnetic fields $H$ up to 18 T. The paramagnetic contribution of the Fe ions is properly treated in order to extract the effective mass anisotropy parameter $γ=(m_c/m_{ab})^{1/2}$ from $τ(θ)$. We show that $γ$ depends strongly on both $T$ and $H$, reaching a maximum value of $\sim$ 10 followed by a decrease towards values close to 1 as $T$ is lowered. The obser…
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…
We present measurements of the thermal expansion coefficient alpha of polycrystalline LaFeAsO1-xFx (x <= 0.1). The magnetic and structural transitions of the samples with x <= 0.04 give rise to large anomalies in alpha(T), while the onset of superconductivity in the crystals with x >= 0.05 is not resolved. Above the structural transition, the thermal expansion coefficient of LaFeAsO is significantly enhanced. This is attributed to fluctuations, which also affect the electrical transport properties of the compound. The complete absence of these fluctuations in the superconducting samples even f…
We have synthesized a quaternary fluoroarsenide SrFeAsF with the ZrCuSiAs-type structure (P4/nmm, a = 0.3999 and c = 0.8973 nm), which is composed of an alternately stacked (FeAs)- and (SrF)+ layers, analogous to the FeAs-based superconductor LaFeAsO. SrFeAsF shows metallic type conduction with the anomaly at ~180 K. The partial replacement of the Fe with Co suppresses the anomaly and induces the superconductivity, while the maximal Tc (4 K for SrFe0.875Co0.125AsF) is much lower than that of the Co-substituted LaFeAsO. Replacement of (LaO)+ layers with (SrF)+ layers results in a enlargement of…
We performed angle-resolved photoemission spectroscopy (ARPES) studies of the electronic structure of the nematic phase in LaFeAsO. Degeneracy breaking between the dxz and dyz hole bands near the Γ and M point is observed in the nematic phase. Different temperature dependent band splitting behaviors are observed at the Γ and M points. The energy of the band splitting near the M point decreases as the temperature decreases while it has little temperature dependence near the Γ point. The nematic nature of the band shift near the M point is confirmed through a detwin experiment using a piezo devi…
The interplay between magnetism and superconductivity in LaFeAsO_0.945F_0.055 was studied as a function of hydrostatic pressure up to p~2.4GPa by means of muon-spin rotation (\muSR) and magnetization measurements. The application of pressure leads to a substantial decrease of the magnetic ordering temperature T_N and a reduction of the magnetic phase volume and, at the same time, to a strong increase of the superconducting transition temperature T_c and the diamagnetic susceptibility. From the volume sensitive \muSR measurements it can be concluded that the superconducting and the magnetic are…
We present $^{75}$As Nuclear Magnetic and Quadrupole Resonance results (NMR, NQR) on a new set of LaFeAsO$_{1-x}$F$_x$ polycrystalline samples. Improved synthesis conditions led to more homogenized samples with better control of the fluorine content. The structural$\equiv$nematic, magnetic, and superconducting transition temperatures have been determined by NMR spin-lattice relaxation rate and AC susceptibility measurements. The so-determined phase diagram deviates from the published one especially for low F-doping concentrations. However, if the doping level is determined from the NQR spectra…
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 report $^{57}$Fe-NMR studies on the oxygen-deficient iron (Fe)-based oxypnictide superconductor LaFeAsO$_{0.7}$ ($T_{c}=$ 28 K) enriched by $^{57}$Fe isotope. In the superconducting state, the spin component of $^{57}$Fe-Knight shift $^{57}K$ decreases almost to zero at low temperatures and the nuclear spin-lattice relaxation rate $^{57}(1/T_{1})$ exhibits a $T^{3}$-like dependence without the coherence peak just below $T_{c}$, which give firm evidence of the unconventional superconducting state formed by spin-singlet Cooper pairing. All these events below $T_c$ are consistently argued in t…
We report $^{75}$As nuclear magnetic resonance (NMR) / nuclear quadrupole resonance (NQR) and transmission electron microscopy (TEM) studies on LaFeAsO$_{1-x}$F$_{x}$. There are two superconducting domes in this material. The first one appears at 0.03 $\leq$ $x$ $\leq$ 0.2 with $T_{\rm c}$$^{max}$ = 27 K, and the second one at 0.25 $\leq$ $x$ $\leq$ 0.75 with $T_{\rm c}$$^{max}$ = 30 K. By NMR and TEM, we demonstrate that a $C4$-to-$C2$ structural phase transition (SPT) takes place above both domes, with the transition temperature $T_{\rm s}$ varying strongly with $x$. In the first dome, the S…
Here, we investigated the interrelationship between pressure and correlation in the LaFeAsO compound by the density functional theory method combined with the dynamical mean field theory (DFT+DMFT) method. The spectral function and the occupation number (ON) of Fe-3d orbitals at different pressures were extracted from the calculations, and the importance of the role of correlation in superconductivity in iron-based compounds was indicated. The measured ON of Fe-3d orbitals demonstrated charge transfer between them and also the crucial role of the Fe-3dxy (xy) orbital in superconductivity in th…
We report on an experimental study of the effect of Mn impurities in the optimally doped LaFeAsO$_{0.89}$F$_{0.11}$ compound. The results show that a very tiny amount of Mn, of the order of 0.1\%, is enough to destroy superconductivity and to recover at low temperatures both the magnetic ground state and the orthorhombic structure of the pristine LaFeAsO parent compound. The results are discussed within a model where electron correlations enhance the Ruderman-Kittel-Kasuya-Yosida interaction among impurities.
We studied the quantum critical behavior of the second antiferromagnetic (AF) phase in the heavily electron-doped high-$T_c$ pnictide, LaFeAsO$_{1-x}$H$_x$ by using $^{75}$As and $^{1}$H nuclear-magnetic-resonance (NMR) technique. In the second AF phase, we observed a spatially modulated spin-density-wave-like state up to $x$=0.6 from the NMR spectral lineshape and detected a low-energy excitation gap from the nuclear relaxation time $T_1$ of $^{75}$As. The excitation gap closes at the AF quantum critical point (QCP) at $x \approx 0.49$. The superconducting (SC) phase in a lower-doping regime …
The effect of atomic disorder induced by neutron irradiation on the crystal structure and electronic states near $E_F$ of the lightly overdoped LaFeAsO$_{0.85}$F$_{0.15}$ ($T_c=21K$) was studied by X-ray diffraction and $^{75}$As NMR. The irradiation of the polycrystalline sample by "moderate" neutron fluence of $Φ=(0;0.5;1.6)\cdot10^{19}cm^{-2}$ at $T=50^{\circ}C$ leads to the suppression of superconductivity. It is shown that neutron irradiation produces an anisotropic expansion of the tetragonal lattice almost due to an increase of the Fe-As distance. A partial loss of the 2D character of t…
The Nernst effect has recently proven as a sensitive probe for detecting unusual normal state properties of unconventional superconductors. Here we present a systematic study of the Nernst effect of the iron pnictide superconductor \laf with a particular focus on its evolution upon doping. For the parent compound we observe a huge negative Nernst coefficient accompanied with a severe violation of the Sondheimer cancellation in the spin density wave (SDW) ordered state. Surprisingly, an unusual and enhanced Nernst signal is also found at underdoping ($x=0.05$) despite the presence of bulk super…
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…
In layered single band systems, the interlayer conductivity depends on the orientation of the in-plane magnetic field and takes maximum values when the magnetic field is perpendicular to flat regions of the Fermi surface. Extending this known results to multi-band systems, we propose an experiment to extract information about their Fermi surface topology. We discuss application of the formula to a FeAs-based superconductor, LaFeAsO$_{1-x}$F$_x$. We show that the magnetically ordered state in the parent compound is clearly distinguished from the paramagnetic state by the oscillation period in t…
The superconducting properties of LaFeAsO$_{1-x}$F$_{x}$ in conditions of optimal electron-doping are investigated upon the application of external pressure up to $\sim 23$ kbar. Measurements of muon-spin spectroscopy and dc magnetometry evidence a clear mutual independence between the critical temperature $T_{c}$ and the low-temperature saturation value for the ratio $n_{s}/m^{*}$ (superfluid density over effective band mass of Cooper pairs). Remarkably, a dramatic increase of $\sim 30$ % is reported for $n_{s}/m^{*}$ at the maximum pressure value while $T_{c}$ is substantially unaffected in …
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…
We present a study concerning the partial substitution of yttrium at the lanthanum site of the undoped LaFeAsO and superconducting LaFeAsO0.85F0.15 compounds. We prepared samples with a nominal yttrium content up to 70% producing simultaneous shrinkage of both the a- and c-lattice parameters by 1.8% and 1.7%, respectively. The chemical pressure provided by the partial substitution with this smaller ion size causes a lowering of the spin density wave temperature in the undoped compounds, as well as an increase of the superconducting transition temperatures in the doped ones. The 15% fluorine-do…
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…
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…
The crystal structure and numerous normal and superconducting state properties of layered tetragonal (P4/nmm) LaFeAsO, with F-doping of 11 %, are reported. Resistivity measurements give an onset transition temperature Tc = 28.2 K, and low field magnetic susceptibility data indicate bulk superconductivity. In applied magnetic field, analysis of the resistive transition results in a critical field Hc2 = 30 T and a coherence length 35 A. An upper limit for the electron carrier concentration of 1 x 10^21 cm-3 is inferred from Hall data just above Tc. Strong electron-electron correlations are sugge…
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…
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…
The local structure of the parent and doped LaFeAsO1-xFx (pnictide) compounds were studied by x-ray absorption spectroscopy. In the doped system, the Fe-As and Fe-Fe correlations are well modeled by an Einstein model with no low temperature anomalies. For the Fe-As bonds, the Einstein temperatures are identical for the doped (11%) and undoped samples, but the doped sample is found to have a lower level of static disorder. For the Fe-Fe correlation, doping enhances the effective Einstein temperature of Fe-Fe atom correlation. The results suggest that the onset of superconductivity in the F dope…
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,…
The ionization energy theory is used to calculate the evolution of the resistivity and specific heat curves with respect to different doping elements in the recently discovered superconducting Pnictide materials. Subsequently, the electron-conduction mechanism in the Pnictides above the structural transition temperature is explained unambiguously, which is also consistent with other strongly correlated matter, such as cuprates, manganites, titanates and magnetic semiconductors. Therefore, the superconductivity is not uniquely corresponds to the electronic properties above the structural transi…
The thermopower and Nernst effect were investigated for undoped parent compounds LaFeAsO and LaNiAsO. Both thermopower and Nernst signal in iron-based LaFeAsO are significantly larger than those in nickel-based LaNiAsO. Furthermore, abrupt changes in both thermopower and Nernst effect are observed below the structural phase transition temperature and spin-density wave (SDW) type antiferromagnetic (AFM) order temperature in Fe-based LaFeAsO. On the other hand, Nernst effect is very small in the Ni-based LaNiAsO and it is weakly temperature-dependent, reminiscent of the case in normal metals. We…
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…
We report the synthesis and characterization of the novel silicide LaFeSiH displaying superconductivity with onset at 11 K. We find that this pnictogen-free compound is isostructural to LaFeAsO, with a similar low-temperature tetragonal to orthorhombic distortion. Using density functional theory we show that this system is also a multiband metal in which the orthorhombic distortion is likely related to single-stripe antiferromagnetic order. Electrical resistivity and magnetic susceptibility measurements reveal that these features occur side-by-side with superconductivity, which is suppressed b…
We report the realization of superconductivity by an isovalent doping with phosphorus in LaFeAsO. X-ray diffraction shows that, with the partial substitution of P for As, the Fe$_2$As$_2$ layers are squeezed while the La$_2$O$_2$ layers are stretched along the c-axis. Electrical resistance and magnetization measurements show emergence of bulk superconductivity at $\sim$10 K for the optimally-doped LaFeAs$_{1-x}$P$_{x}$O ($x=0.25\sim0.3$). The upper critical fields at zero temperature is estimated to be 27 T, much higher than that of the LaFePO superconductor. The occurrence of superconductivit…
We report on the magnetic behavior of oxygen deficient LaFeAsO1-x (x-0.10) compound, prepared by one-step synthesis, which crystallizes in the tetragonal (S.G. P4/nmm) structure at room temperature. Resistivity measurements show a strong anomaly near 150 K, which is ascribed to the spin density wave (SDW) instability. On the other hand, dc magnetization data shows paramagnetic-like features down to 5 K, with an effective moment of 0.83 mB/Fe. 57Fe Mossbauer studies (MS) have been performed at 95 and 200 K. The spectra at both temperatures are composed of two sub-spectra. At 200 K the major one…
We report a systematic study by 75As nuclear-quadrupole resonance in LaFeAsO1-xFx. The antiferromagnetic spin fluctuation (AFSF) found above the magnetic ordering temperature TN = 58 K for x = 0.03 persists in the regime 0.04 < x < 0.08 where superconductivity sets in. A dome-shaped x-dependence of the superconducting transition temperature Tc is found, with the highest Tc = 27 K at x = 0.06 which is realized under significant AFSF. With increasing x further, the AFSF decreases, and so does Tc. These features resemble closely the cuprates La2-xSrxCuO4. In x = 0.06, the spin-lattice relaxation …
$^{75}$As and $^{139}$La NMR and nuclear quadrupole resonance (NQR) studies on Zn-substituted LaFeAsO$_{0.85}$ have been performed to investigate the Zn-impurity effects microscopically. Although superconductivity in LaFeAsO$_{0.85}$ disappears by 3% Zn substitution, we found that NMR/NQR spectra and NMR physical quantities in the normal state are hardly changed, indicating that the crystal structure and electronic states are not modified by Zn substitution. Our results suggest that the suppression of superconductivity by Zn substitution is not due to the change of the normal-state properties,…
$^{75}$As Nuclear Magnetic (NMR) and Quadrupolar (NQR) Resonance were used, together with Mössbauer spectroscopy, to investigate the magnetic state induced by Mn for Fe substitutions in F-doped LaFe$_{1-x}$Mn$_{x}$AsO superconductors. The results show that $0.5$% of Mn doping is enough to suppress the superconducting transition temperature $T_c$ from 27 K to zero and to recover the magnetic structure observed in the parent undoped LaFeAsO. Also the tetragonal to orthorhombic transition of the parent compound is recovered by introducing Mn, as evidenced by a sharp drop of the NQR frequency. The…
