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 terms of the extended s$_{\pm}$-wave pairing with a sign reversal of the order parameter among Fermi surfaces. In the normal state, we found the remarkable decrease of $1/T_1T$ upon cooling for both the Fe and As sites, which originates from the decrease of low-energy spectral weight of spin fluctuations over whole ${\bm q}$ space upon cooling below room temperature. Such behavior has never been observed for other strongly correlated superconductors where an antiferromagnetic interaction plays a vital role in mediating the Cooper pairing.
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 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}$. A microscopic phase separation between superconducting domains and magnetic domains is shown to take place in the underdoped sample, indicating a local inhomogeneity in association with the density distribution of oxygen deficiencies. As a result, 1/T_1T in the normal state of the superconducting domain decreases significantly upon cooling at both the Fe …
Zero field and longitudinal field muon spin relaxation measurements have been performed in optimally doped and overdoped superconductors LaFeAsO$_{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 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 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.
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…
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 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 report $^{75}$As nuclear quadrupole resonance (NQR) studies on superconducting oxypnictide LaFeAsO$_{0.92}$F$_{0.08}$ ($T_{\rm c}$ = 23 K). The temperature dependence of the spin lattice relaxation rate (1/$T_1$) decreases below $T_{\rm c}$ without a coherence (Hebel-Slichter) peak and shows a temperature dependence that is not simple power-law nor exponential. We show that the result can be understood in terms of two superconducting gaps of either $d$- or ${\pm}s$-wave symmetry, with the larger gap $Δ_1\sim 4 k_{\rm B}T_{\rm c}$ and the smaller one $Δ_2 \sim 1.5 k_{\rm B}T_{\rm c}$. Our re…
We report a 75-As single crystal NMR investigation of LaFeAsO, the parent phase of a pnictide high Tc superconductor. We demonstrate that spin dynamics develop a strong two-fold anisotropy within each orthorhombic domain below the tetragonal-orthorhombic structural phase transition at T[TO]~156 K. This intermediate state with a dynamical breaking of the rotational symmetry freezes progressively into a spin density wave (SDW) below T[SDW]~142 K. Our findings are consistent with the presence of a spin nematic state below T[TO] with an incipient magnetic order.
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…
Electrical resistivity and magnetic susceptibility measurements under high pressure were performed on an iron-based superconductor LaFePO. A steep increase in superconducting transition temperature (Tc) of LaFePO with dTc/dP > 4 K/GPa to a maximum of 8.8 K for P = 0.8 GPa was observed. These results are similar to isocrystalline LaFeAsO1-xFx system reported previously. X-ray diffraction measurements were also performed under high pressure up to 10 GPa, where linear compressibility ka and kc are presented.
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…
We will probe the intrinsic behavior of spin susceptibility chi_(spin) in the LaFeAsO(1-x)F(x) superconductor (x ~ 0.1, Tc ~ 27K) using 19-F and 75-As NMR techniques. Our new results firmly establish the pseudo-gap behavior with Delta_(PG)/kB ~ 140K. The estimated magnitude of chi_(spin) at 290K, ~1.8x10^(-4) [emu/mol-Fe], is approximately twice larger than that in high Tc cuprates. We also show that chi_(spin) levels off below ~50K down to Tc.
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.
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 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 anisotropy of the nuclear spin-lattice relaxation rate $1/T_{1}$ of $^{75}$As was investigated in the iron-based superconductor LaFeAs(O$_{1-x}$F$_{x}$) ($x = 0.07, 0.11$ and 0.14) as well as LaFeAsO. While the temperature dependence of the normal-state $1/T_1T$ in the superconducting (SC) $x = 0.07$ is different from that in the SC $x = 0.11$, their anisotropy of $1/T_1$, $R \equiv (1/T_{1})_{H \parallel ab}/(1/T_{1})_{H \parallel c}$ in the normal state is almost the same ($\simeq$ 1.5). The observed anisotropy is ascribable to the presence of the local stripe correlations with $Q = (π, …
Results of 75As NMR and NQR measurements are reported for superconducting samples of LaFeAsO1-xFx with various x values. The x dependent widths of the superconducting transition and those of the NQR spectra indicate that the optimally doped LaFeAsO1-xFx sample with the superconducting transition temperature Tc ~28 K has the smallest width or smallest inhomogeneity of the superconducting order parameter Δ. In the analyses of the temperature (T) dependence of the NMR longitudinal relaxation rate 1/T1, we have tried to use a simple relation 1/T1 ~ T^n to see how fast 1/T1 decreases when the super…
LaFe1-yCoyAsO1-xFx (x=0.11) with various y values were prepared and their electrical resistivities, superconducting diamagnetisms and Hall coefficients have been measured. 75As- and 135La-NMR studies have also been carried out In spite of the successful Co-doping, we have not found any meaningful correlation of Tc with y, which indicates that the Tc-suppression by Co-doping is considered not to be so significant as expected for superconductors with nodes. Even for superconductors without nodes, it may not be easy to expect this small effect on Tc, if there are two different (disconnected) Ferm…
The electron-doped high-transition-temperature (T_c) iron-based pnictide superconductor LaFeAsO_{1-x}H_x has a unique phase diagram: superconducting (SC) double domes are sandwiched by antiferromagnetic phases at ambient pressure and they turn to a single dome with a maximum T_c that exceeds 45K at a pressure of 3.0 GPa. We studied whether spin fluctuations are involved in increasing T_c under a pressure of 3.0 GPa by using ^{75}As nuclear magnetic resonance (NMR) technique. The ^{75}As-NMR results for the powder samples show that T_c increases up to 48 K without the influence of spin fluctuat…
The temperature dependence of electron spin resonance (ESR) was studied in the oxypnictide superconductors LaFeAsO$_{1-x}$F$_x$ (x = 0.0 and 0.13). In the samples, the ESR signal indicates that the g factor and peak-to-peak linewidth strongly depend on temperature, especially at low temperatures. It indicates a strong coupling picture with existence of local moment. The dependence mentioned above gradually attenuates, and tends to saturation around room-temperature. This behavior could be ascribed to "bottleneck" effect due to coupling of local moment and itinerant electron. In addition, a Cur…
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 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…
$^{75}$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,…
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…
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…
We determine the phase diagram of LaFe$_{1-x}$Co$_x$AsO single crystals by using nuclear magnetic resonance (NMR). Up to a nominal doping of $x=0.03$, it follows the phase diagram for F-doped polycrystals. Above $x=0.03$, the F-doped samples become superconducting, whereas for Co-doping the structural and magnetic transitions can be observed up to $x=0.042$, and superconductivity occurs only for higher doping levels and with reduced transition temperatures. For dopings up to $x=0.056$, we find evidence for short-range magnetic order. By means of relaxation-rate measurements, we map out the mag…
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…
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 h…
We report our extensive 57Fe-, 75As-, 139La-, and 1H-NMR studies of La_{0.8}Y_{0.2}FeAsO_{1-y} (La_{0.8}Y_{0.2}1111) and LaFeAsO_{1-y}H_{x}(La1111H), where doping yttrium (Y) and hydrogen (H) into optimally doped LaFeAsO_{1-y} (La1111(OPT)) increases T_c=28 K to 34 and 32 K, respectively. In the superconducting (SC) state, the measurements of nuclear-spin lattice-relaxation rate 1/T_1 have revealed in terms of a multiple fully gapped s_\pm-wave model that the SC gap and T_c in La_{0.8}Y_{0.2}1111 become larger than those in La1111(OPT) without any change in doping level. In La1111H, the SC gap…
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$_…
Nuclear magnetic resonance (NMR) measurements of an iron (Fe)-based superconductor LaFeAsO_{1-x}F_x (x = 0.08 and 0.14) were performed at ambient pressure and under pressure. The relaxation rate 1/T_1 for the overdoped samples (x = 0.14) shows T-linear behavior just above T_c, and pressure application enhances 1/T_1T similar to the behavior of T_c. This implies that 1/T_1T = constant originates from the Korringa relation, and an increase in the density of states at the Fermi energy D(E_F) leads to the enhancement of T_c. In the underdoped samples (x = 0.08), 1/T_1T measured at ambient pressure…
We report an 75As-NMR study on iron (Fe)-based superconductors with thick perovskitetype blocking layers Sr4(Mg0.5-xTi0.5+x)2O6Fe2As2 with x=0 and 0.2. We have found that antiferromagnetic (AFM) order takes place when x=0, and superconductivity (SC) emerges below Tc=36 K when x=0.2. These results reveal that the Fe-pnictides with thick perovskitetype blocks also undergo an evolution from the AFM order to the SC by doping electron carriers into FeAs planes through the chemical substitution of Ti+4 ions for Mg+2 ions, analogous to the F-substitution in LaFeAsO compound. The reason why the Tc=36 …
We present results from a detailed experimental investigation of LaFeAsO, the parent material in the series of "FeAs" based oxypnictide superconductors. Upon cooling this material undergoes a tetragonal-orthorhombic crystallographic phase transition at ~160 K followed closely by an antiferromagnetic ordering near 145 K. Analysis of these phase transitions using temperature dependent powder X-ray and neutron diffraction measurements is presented. A magnetic moment of ~0.35 Bohr magnetons per iron is derived from Mossbauer spectra in the low temperature phase. Evidence of the structural transiti…
The structural, electronic, and magnetic properties of the superconducting NdFeAsO$_{1-x}$F$_{x}$ phases ($T_C=43 {\rm K}$ for $x=0.15$) have been investigated experimentally by high-resolution synchrotron x-ray powder diffraction, magnetization and $^{75}$As NMR measurements. Density-functional calculations were performed to calculate and analyze the electric field gradient and the density of states. Compared to LaFeAsO family, the NdFeAsO family shows a contraction of the lattice parameters with shorter rare-earth (RE)-As bond distances, an increased thickness of the As-Fe$_2$-As layer, and …
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…
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…
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…
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 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 …
We report 75As NMR measurements of the spin-lattice relaxation in the superconducting state of LaFeAsO_(0.9)F_(0.1) and As-deficient LaFeAs_(1-d)O_0.9F_0.1. The temperature behavior of 1/T_1 below T_c changes drastically from a T^3-dependence for LaFeAsO_(0.9)F_(0.1) to a T^5-dependence for the As-deficient sample. These results, together with the previously reported unexpected increase of T_c and the slope of the upper critical field near T_c for the As-deficient sample, are discussed in terms of non-universal SC gaps in Fe-pnictides and the effect of As deficiency as an exotic case where non…
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,…
75As-nuclear magnetic resonance (NMR) on an iron-based superconductor LaFeAsO1-xFx (x=0.14) was performed under a pressure of 3GPa. Enhancement of superconducting transition temperature Tc was confirmed from the relaxation rate 1/T1; Tc goes up to 40K by applying pressure up to 3GPa. 1/T1T, which is temperature independent just above Tc and gives a measure of the density of states (DOS) at the Fermi energy, enhances by applying pressure. These facts suggest that the increase of the DOS leads to the enhancement of Tc. On the other hand, anomalous behavior of 1/T1T observed at high temperatures …
We report muon-spin relaxation measurements on SrFeAsF, which is the parent compound of a newly discovered iron-arsenic-fluoride based series of superconducting materials. We find that this material has very similar magnetic properties to LaFeAsO, such as separated magnetic and structural transitions (TN = 120 K, Ts = 175 K), contrasting with SrFe2As2 where they are coincident. The muon oscillation frequencies fall away very sharply at TN, which suggests that the magnetic exchange between the layers is weaker than in comparable oxypnictide compounds. This is consistent with our specific heat m…
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…
We report that the incorporation of hydroxide ions (OH)- significantly enhances the superconducting transition temperature (Tc) in the LnFeAsO-based superconductors (Ln1111: Ln = La, Ce and Pr). For La1111, Tc of the (OH)- incorporated sample synthesized using high-pressure technique becomes 35 K, which is higher by 7 K than the typical optimally-doped La1111 superconductors. Similar enhancement in Tc is also observed for Ce1111 and Pr1111. 1H-NMR measurement have confirmed the existence of hydrogen atoms in the samples. Accompanying the (OH)- incorporation, the lattice parameters are largely …
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 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…
$^{75}$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…
A neptunium analogue of the LaFeAsO tetragonal layered compound has been synthesized and characterized by a variety of experimental techniques. The occurrence of long-range magnetic order below a critical temperature T_N = 57 K is suggested by anomalies in the temperature-dependent magnetic susceptibility, electrical resistivity, Hall coefficient, and specific heat curves. Below T_N, powder neutron diffraction measurements reveal an antiferromagnetic structure of the Np sublattice, with an ordered magnetic moment of 1.70(0.07) μ_B aligned along the crystallographic c-axis. No magnetic order ha…
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$_2…
The transition temperature Tc~26 K of the recently discovered superconductor LaFeAs(O,F) has been demonstrated to be extremely sensitive to the lanthanide ion, reaching 55 K for the Sm containing oxypnictides. Therefore, it is important to determine how the moment on the lanthanide affects the overall magnetism in these systems. Here we report a neutron diffraction study of the Nd oxypnictides. Long ranged antiferromagnetic order is apparent in NdFeAsO below 1.96 K. Rietveld refinement shows that both Fe and Nd magnetic ordering are required to describe the observed data with the staggered mom…
We investigated the homogeneous coexistence of spin-density-wave (SDW) and superconducting (SC) states via 75As-nuclear magnetic resonance (NMR) in CaFe(1-x)Co(x)AsF and found that the electronic and magnetic properties of this compound are intermediate between those of LaFeAsO(1-x)F(x) and Ba(Fe(1-x)Co(x))2As2. For 6% Co-doped samples, the paramagnetic spectral weight completely disappears in the crossover regime between the SDW and SC phases followed by the anomalous behavior of relaxation rate (1/T1), implying that the two phases are not segregated. The 59Co-NMR spectra show that spin momen…
We investigate interplay between magnetic fluctuations and superconductivity in the effective five-band Hubbard model for iron-oxypnictide superconductors on the basis of the fluctuation-exchange approximation. As for the normal-state properties, we find the pseudogap behavior in the NMR relaxation rate and the spectral weight in the electron-doped region, while we cannot find such behavior in the hole-doped region. The pseudogap behavior originates from the band structure effect, that is, existence of high density of states just below the Fermi level. Solving the superconducting Eliashberg eq…
Muon Spin Rotation ($μ$SR) and $^{19}$F Nuclear Magnetic Resonance (NMR) measurements were performed to investigate the effect of Mn for Fe substitutions in La$_{1-y}$Y$_{y}$Fe$_{1-x}$Mn$_x$AsO$_{0.89}$F$_{0.11}$ superconductors. While for $y = 0$ a very low critical concentration of Mn ($x = 0.2$%) is needed to quench superconductivity, as $y$ increases the negative chemical pressure introduced by Y for La substitution stabilizes superconductivity and for $y= 20$% it is suppressed at Mn contents an order of magnitude larger. A magnetic phase arises once superconductivity is suppressed both fo…
We performed nuclear magnetic resonance (NMR) measurements to investigate the evolution of spin-density-wave (SDW) and superconducting (SC) states upon electron doping in CaFe_{1-x}Co_{x}AsF, which exhibits an intermediate phase diagram between those of LaFeAsO_{1-x}F_x and Ba(Fe_{1-x}Co_x)_2As_2. We found that homogeneous coexistence of the incommensurate SDW and SC states occurs only in a narrow doping region around the crossover regime, which supports S_{+-}-wave symmetry. However, only the structural phase transition survives upon further doping, which agrees with predictions from orbital …
Measurements of the electrical resistivities, Hall coefficients, thermoelectric powers, electronic specific heat coefficients have been carried out for samples of LnFe1-yMyAsO1-xFx (Ln=La, Nd; M=Co, Mn; x=0.11) obtained by M atom dopings to the superconducting LnFeAsO1-xFx (Ln1111) system. The NMR longitudinal relaxation rates 1/T1 have also been measured for samples of LaFe1-yCoyAsO1-xFx with various x values. Co atoms doped to the superconducting LnFeAsO1-xFx are nonmagnetic, and the Tc-suppression by the Co atoms has been found to be too weak to understand by the pair breaking effect expect…
Since the discovery of high transition-temperature (Tc) superconductivity in copper oxides two decades ago, continuous efforts have been devoted to searching for similar phenomenon in other compounds. With the exception of MgB2 (Tc =39 K), however, Tc is generally far lower than desired. Recently, breakthrough has been made in a new class of oxypnictide compounds. Following the initial discovery of superconductivity in LaO1-x FxFeAs (Tc =26 K), Tc onset has been raised to 55 K in ReO1-xFxFeAs (Re: Ce, Pr, Nd, Sm). Meanwhile, unravelling the nature of the energy associated with the formation of…
Since the discovery of superconductivity in the cuprates two decades ago, it has been firmly established that the CuO_2 plane is consequential for high T_C superconductivity and a host of other very unusual properties. A new family of superconductors with the general composition of LaFeAsO_(1-x)F_x has recently been discovered but with the conspicuous lacking of the CuO_2 planes, thus raising the tantalizing questions of the different pairing mechanisms in these oxypnictide superconductors. Intimately related to pairing in a superconductor are the superconducting gap, its value, structure, and…
