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 on the relationship between superconductivity and antiferromagnetism. Based on orbital fluctuation theory, the existence of PM domains is evidence of the ferroquadrupole state.
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…
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 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…
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…
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…
High-quality superconducting LaFeAsO$_{1-x}$F$_{x}$ thin films were grown on single crystalline LaAlO$_{3}$ substrates with critical temperatures (onset) up to 28 K. Resistive measurements in high magnetic fields up to 40 T reveal a paramagnetically limited upper critical field, $μ_{0}H_{c2}$(0) around 77 T and a remarkable steep slope of -7.5 T/K near $T_{c}$. From transport measurements we observed a weak link behavior in low magnetic fields and the evidence for a broad reversible regime.
$^{75}$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 $^{75}$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 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 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 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 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…
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 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$_2…
We present calculations of structural and magnetic properties of the iron-pnictide superconductor LaFeAsO including electron-electron correlations. For this purpose we apply a fully charge self-consistent combination of Density-Functional Theory with the Dynamical Mean-Field theory, allowing for the calculation of total energies. We find that the inclusion of correlation effects gives a good agreement of the Arsenic z position with experimental data even in the paramagnetic (high-temperature) phase. Going to low temperatures, we study the formation of the ordered moment in the striped spin-den…
In this Letter we report the LDA+DMFT (method combining Local Density Approximation with Dynamical Mean-Field Theory) results for magnetic properties of parent superconductor LaFeAsO in paramagnetic phase. Calculated uniform magnetic susceptibility shows linear dependence at intermediate temperatures in agreement with experimental data. For high temperatures ($>$1000 K) calculations show saturation and then susceptibility decreases with temperature. Contributions to temperature dependence of the uniform susceptibility are strongly orbitally dependent. It is related to the form of the orbitally…
Hydrogen (H)-doped LaFeAsO is a prototypical iron-based superconductor. However, its phase diagram extends beyond the standard framework, where a superconducting (SC) phase follows an antiferromagnetic (AF) phase upon carrier doping; instead, the SC phase is sandwiched between two AF phases appearing in lightly and heavily H-doped regimes. We performed nuclear magnetic resonance (NMR) measurements under pressure, focusing on the second AF phase in the heavily H-doped regime. The second AF phase is strongly suppressed when a pressure of 3.0 GPa is applied, and apparently shifts to a highly H-do…
We have studied Ni-substitution effect in LaFe$_{1-x}$Ni$_{x}$AsO ($0\leq x \leq0.1$) by the measurements of x-ray diffraction, electrical resistivity, magnetic susceptibility, and heat capacity. The nickel doping drastically suppresses the resistivity anomaly associated with spin-density-wave ordering in the parent compound. Superconductivity emerges in a narrow region of $0.03\leq x \leq0.06$ with the maximum $T_c$ of 6.5 K at $x$=0.04, where enhanced magnetic susceptibility shows up. The upper critical field at zero temperature is estimated to exceed the Pauli paramagnetic limit. The much l…
A $^{59}$Co nuclear magnetic resonance (NMR) measurement was performed on the single-crystalline ferromagnetic (FM) superconductor UCoGe under a pressure of 1.09 GPa, where the FM state is suppressed and superconductivity occurs in the paramagnetic (PM) state, to study the superconducting (SC) state in the PMstate. $^{59}$Co-NMR spectra became broader but hardly shifted across the SC transition temperature. The Knight-shift change determined from fitting the spectral peak with a Gaussian was much smaller than the spin part of the Knight shift; this is in good agreement with the spin-triplet pa…
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…
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 present In NMR measurements in a novel thermodynamic phase of CeCoIn5 in high magnetic field, where exotic superconductivity coexists with the incommensurate spin-density wave order. We show that the NMR spectra in this phase provide direct evidence for the emergence of the spatially distributed normal quasiparticle regions. The quantitative analysis for the field evolution of the paramagnetic magnetization and newly-emerged low-energy quasiparticle density of states is consistent with the nodal plane formation, which is characterized by an order parameter in the Fulde-Ferrell-Larkin-Ovchin…
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 report $^{75}$As NMR measurements in CaFe$_2$As$_2$, made under applied pressures up to 0.83 GPa produced by a standard clamp pressure cell. Our data reveal phase segregation of paramagnetic (PM) and antiferromagnetic (AFM) phases over a range of pressures, with the AFM phase more than 90 % dominant at low temperatures. In situ RF susceptibility measurements indicate the presence of superconductivity. $^{75}$As spin-lattice relaxation experiments indicate that the $^{75}$As nuclei sample the superconductivity while in the magnetically-ordered environment.
Anomalous field evolution of the mixed-state linewidth in the second superconducting dome of LaFeAsO$_{1-x}M_x$ ($M={\rm F,H}$)
PSI Center for Neutron and Muon Sciences CNM（瑞士保罗谢尔研究所中子与μ子科学中心）；Université Grenoble Alpes, CEA, Grenoble INP, IRIG-PHELIQS（格勒诺布尔阿尔卑斯大学）；Dipartimento di Fisica e Astronomia “Augusto Righi”, Università di Bologna（博洛尼大学物理与天文学系）；CNR-SPIN（意大利国家研究委员会自旋物理研究所）；Dipartimento di Fisica, Università degli Studi di Pavia（帕维亚大学物理系）；Leibniz-Institute for Solid State and Materials Research, IFW-Dresden（德累斯顿莱布尼茨固体与材料研究所）；CrystMat Company（CrystMat公司）
We give a quantitative analysis of the published results of nuclear magnetic resonance (NMR) experiments for k-(ET)2X family of organic charge transfer salts by using the phenomenological spin fluctuation model of Moriya, and Millis, Monien and Pines (M-MMP). For temperatures above T_NMR ~ 50 K, the model gives a good quantitative description of the data for the paramagnetic metallic phase of several k-(ET)2X materials, with an antiferromagnetic correlation length which increases with decreasing temperature; growing to several lattice constants by T_NMR. It is shown that the fact that the dime…
We performed $^{59}$Co nuclear magnetic resonance (NMR) measurements of single-crystalline U$_6$Co. There is a small decrease in the Knight shift in the superconducting (SC) state, but this change mainly arises from the SC diamagnetic effect. The negligible change of the spin part of the Knight shift, together with the absence of the Pauli-paramagnetic effect in the SC U$_6$Co, is understood as a consequence of the small spin susceptibility. The nuclear spin-lattice relaxation rate $1/T_1$ is also measured in the SC state under the magnetic field, and exhibits a tiny Hebel-Slichter peak just b…
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…
139La NMR study was performed in grain aligned (c|| H0) sample of LaCoPO and polycrystalline LaFePO. Knight shift is isotropic and temperature independent in LaFePO. It is strongly temperature dependent and anisotropic in LaCoPO. The spin-lattice relaxation rate in LaCoPO clearly reveals the existence of 3D spin fluctuations both in the paramagnetic and ferromagnetic state over and above the dominant 2D spin fluctuations in the paramagnetic state, observed earlier from 31P NMR measurements in the same oriented sample. The spin fluctuation parameters in LaCoPO determined from 139La NMR relaxati…
The putative spin-triplet superconductor UTe2 has an Ising-like magnetic anisotropy, indicating the Cooper pair spins parallel to the easy-axis. However, the upper critical field for the hard-axis direction is much larger than that for the easy-axis, implying the strong suppression of the Pauli depairing effect even for the hard-axis direction. This observation is consistent with the recent NMR measurements which show the tiny decrease of the Knight shift below the transition temperature Tc for hard-axis magnetic fields. We clarify that these behaviors are naturally understood as a result of m…
Bulk single crystals of manganese phosphide (MnP) were grown from melt at 1 GPa and 1200 C by using a cubic-anvil, high-pressure, and high-temperature technique. The obtained black colored crystals exhibit a plate-like morphology, with flat surfaces and maximum dimensions up to 4 x 2 x 0.5 mm3. The orthorhombic crystal structure was confirmed by X-ray diffraction [Pnma, 62, Z = 4, a = 5.2510(4) Å, b = 3.1670(3) Å, c = 5.90098 (4) Å and V = 98.279(14) Å3]. Temperature-dependent magnetization measurements reveal the occurrence of two successive transitions: a paramagnetic to ferromagnetic transi…
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 …
We demonstrate that the anisotropy R of the paramagnetic spin fluctuations grows toward Tc at 75As sites in the optimally electron-doped superconductor Ba[(Fe0.92Co0.08)2]2As2, with stronger spin fluctuations along the c-axis. Our finding is in remarkable contrast with the case of high T$_c$ cuprates, where R is independent of temperature above Tc.
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…
We report results of 75As nuclear magnetic resonance (NMR) experiments on a self-flux grown single crystal of BaFe2As2. A first-order antiferromagnetic (AF) transition near 135 K was detected by the splitting of NMR lines, which is accompanied by simultaneous structural transition as evidenced by a sudden large change of the electric field gradient tensor at the As site. The NMR results lead almost uniquely to the stripe spin structure in the AF phase. The data of spin-lattice relaxation rate indicate development of anisotropic spin fluctuations of the stripe-type with decreasing temperature i…
We report the first magneto-caloric and calorimetric observations of a magnetic-field-induced phase transition within a superconducting state to the long-sought exotic "FFLO" superconducting state first predicted over 50 years ago. Through the combination of bulk thermodynamic calorimetric and magnetocaloric measurements in the organic superconductor $κ$ - (BEDT-TTF)$_2$Cu(NCS)$_2$, as a function of temperature, magnetic field strength, and magnetic field orientation, we establish for the first time that this field-induced first-order phase transition at the paramagnetic limit $H_p$ for tradit…
We report an NMR and magnetometry study on the expanded intercalated fulleride Cs_3C_60 in both its A15 and face centered cubic structures. NMR allowed us to evidence that both exhibit a first-order Mott transition to a superconducting (SC) state, occuring at distinct critical pressures p_c and temperatures T_c. Though the ground state magnetism of the Mott phases differs, their high $T$ paramagnetic and SC properties are found similar, and the phase diagrams versus unit volume per C_60 are superimposed. Thus, as expected for a strongly correlated system, the inter-ball distance is the relveva…
Observation of an anomalous temperature dependence of the spin susceptibility, along with a spin gap in NMR, in the quantum paramagnetic normal state of Iron Pnictides is a signature of an unusual metallic state. We argue that both these anomalous features are associated with a wide fluctuational regime dominated by dynamical, short-ranged and frustrated spin correlations in a strongly correlated metal. Using LDA+DMFT, we show that both these features can be quantitatively undertstood in the doped Fe-pnictides. We argue that such spin correlations naturally arise in a Mottness scenario, where …
We investigate the vortex state with Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) modulations suggested for a high field phase of CeCoIn_5. On the basis of the quasiclassical Eilenberger theory, we calculate the three dimensional structure of pair potentials, internal magnetic fields, paramagnetic moments, and electronic states, for the s-wave and the d-wave pairings comparatively. The π-phase shift of the pair potential at the FFLO nodal plane or at the vortex core induces sharp peak states in the local density of states, and enhances the local paramagnetic moment. We also discuss the NMR spectrum…
In Ba(Fe0.95Co0.05)2As2 all of the 75As NMR intensity at the paramagnetic resonance position vanishes abruptly below Tonset(SDW)=56 K, indicating that magnetic (spin density wave) order is present in all of the sample volume, despite bulk superconductivity below Tc=15 K. The two phases thus coexist homogeneously at the microscopic scale. In Ba0.6K0.4Fe2As2, on the other hand, the signal loss below Tonset(SDW)~75 K is not complete, revealing that magnetic order is bound to finite-size areas of the sample, while the remaining NMR signal shows a clear superconducting response below Tc=37 K. Thus,…
We theoretically investigate the Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) state by using the microscopic quasi-classical Eilenberger equation. The Pauli paramagnetic effects and the orbital depairing effects due to vortices are treated in an equal footing for three dimensional spherical Fermi surface model and $s$-wave pairing. The field evolution of the LO state is studied in detail, such as the $H$-$T$ phase diagram, spatial structures of the order parameter, the paramagnetic moment, and the internal filed. Field-dependences of various thermodynamic quantities: the paramagnetic moment, entrop…
The iron pnictide and chalcogenide compounds are a subject of intensive investigations due to their high temperature superconductivity.\cite{a-LaFeAsO} They all share the same structure, but there is significant variation in their physical properties, such as magnetic ordered moments, effective masses, superconducting gaps and T$_c$. Many theoretical techniques have been applied to individual compounds but no consistent description of the trends is available \cite{np-review}. We carry out a comparative theoretical study of a large number of iron-based compounds in both their magnetic and param…
We study a model of a d-wave superconductor with strong potential scatterers in the presence of antiferromagnetic correlations and apply it to experimental nuclear magnetic resonance (NMR) results on Zn impurities in the superconducting state of YBCO. We then focus on the contribution of impurity-induced paramagnetic moments, with Hubbard correlations in the host system accounted for in Hartree approximation. We show that local magnetism around individual impurities broadens the line, but quasiparticle interference between impurity states plays an important role in smearing out impurity satell…
We report $^{75}$As nuclear magnetic resonance (NMR) measurements of single-crystalline Ca(Fe$_{1-x}$Co$_x$)$_2$As$_2$ ($x$ = 0.023, 0.028, 0.033, and 0.059) annealed at 350~$^{\circ}$C for 7 days. From the observation of a characteristic shape of $^{75}$As NMR spectra in the stripe-type antiferromagnetic (AFM) state, as in the case of $x$ = 0 ($T_{\rm N}$ = 170 K), clear evidence for the commensurate AFM phase transition with the concomitant structural phase transition is observed in $x$ = 0.023 ($T_{\rm N}$ = 106 K) and $x$ = 0.028 ($T_{\rm N}$ = 53 K). Through the temperature dependence of …
We report nuclear magnetic resonance (NMR) studies of the intercalated iron selenide superconductor (Tl, Rb)$_{y}$Fe$_{2-x}$Se$_2$ ($T_c = 32$ K). Single-crystal measurements up to 480 K on both $^{77}$Se and $^{87}$Rb nuclei show a superconducting phase with no magnetic order. The Knight shifts $K$ and relaxation rates $1/T_1T$ increase very strongly with temperature above $T_c$, before flattening at 400 K. The quadratic $T$-dependence and perfect proportionality of both $K$ and $1/T_1T$ data demonstrate their origin in paramagnetic moments. A minimal model for this pseudogap-like response is…
$^{73}$Ge and $^{59}$Co nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) measurements have been performed on a $^{73}$Ge-enriched single-crystalline sample of the ferromagnetic superconductor UCoGe in the paramagnetic state. The $^{73}$Ge NQR parameters deduced from NQR and NMR are close to those of another isostructural ferromagnetic superconductor URhGe. The Knight shifts of the Ge and Co sites are well scaled to each other when the magnetic field is parallel to the $b$ or $c$ axis. The hyperfine coupling constants of Ge are estimated to be close to those of Co. The la…
