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 and T_c also increase slightly even though a decrease in carrier density and some disorders are significantly introduced. As a consequence, we suggest that the optimization of both the structural parameters and the carrier doping level to fill up the bands is crucial for increasing T_c among these La1111-based compounds through the optimization of the Fermi surface topology.
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 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…
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 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…
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 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 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.
We report systematic 57Fe-NMR and 75As-NMR/NQR studies on an underdoped sample (T_c=20 K), an optimally doped sample (T_c=28 K), and an overdoped sample (T_c=22 K) of oxygen-deficient iron (Fe)-based oxypnictide superconductor LaFeAsO_{1-y}$. A microscopic phase separation between superconducting domains and magnetic domains is shown to take place in the underdoped sample, indicating a local inhomogeneity in association with the density distribution of oxygen deficiencies. As a result, 1/T_1T in the normal state of the superconducting domain decreases significantly upon cooling at both the Fe …
We 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 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 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 $^{57}$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 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,…
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…
$^{75}$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,…
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 …
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 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…
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$_…
$^{75}$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…
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 …
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$_2…
Hydrogen (H)-doped LaFeAsO is a prototypical iron-based superconductor. However, its phase diagram extends beyond the standard framework, where a superconducting (SC) phase follows an antiferromagnetic (AF) phase upon carrier doping; instead, the SC phase is sandwiched between two AF phases appearing in lightly and heavily H-doped regimes. We performed nuclear magnetic resonance (NMR) measurements under pressure, focusing on the second AF phase in the heavily H-doped regime. The second AF phase is strongly suppressed when a pressure of 3.0 GPa is applied, and apparently shifts to a highly H-do…
75As-nuclear magnetic resonance (NMR) on an iron-based superconductor LaFeAsO1-xFx (x=0.14) was performed under a pressure of 3GPa. Enhancement of superconducting transition temperature Tc was confirmed from the relaxation rate 1/T1; Tc goes up to 40K by applying pressure up to 3GPa. 1/T1T, which is temperature independent just above Tc and gives a measure of the density of states (DOS) at the Fermi energy, enhances by applying pressure. These facts suggest that the increase of the DOS leads to the enhancement of Tc. On the other hand, anomalous behavior of 1/T1T observed at high temperatures …
Muon Spin Rotation ($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…
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…
