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, both phase diagrams can be reconciled. The absence of bulk coexistence of magnetism and superconductivity and a nanoscale separation into low-doping-like and high-doping-like regions have been confirmed. Additional frequency dependent intensity, spin-spin, and spin-lattice relaxation rate measurements on underdoped samples at the boundary of magnetism and superconductivity indicate that orthorhombicity and magnetism originate from the low-doping-like regions, and superconductivity develops at first in the high-doping-like regions.
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 …
$^{75}$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,…
Some of recent advances in the NMR and NQR studies of high-Tc superconductors YBa2Cu3O7-d and YBa2Cu4O8 are presented. The topics concerned are the understanding of magnetic phase diagram, impurity substitution effects and vortex core states in the mixed states.
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 report on Cu nuclear quadrupole resonance (NQR) and NMR studies of an optimally hole-doped superconductor Ca2-xNaxCuO2Cl2 (Tc ~ 28 K for x ~ 0.2). In spite of robust oxygen composition, we observed a multiple broad NQR frequency spectrum and nonexponential Cu nuclear spin-lattice relaxation, being similar to those of La2-xSrxCuO4-d.
We report Cd NMR and Re NQR studies on Cd2Re2O7, the first superconductor among pyrochlore oxides Tc=1 K. Re NQR spectrum at zero magnetic field below 100 K rules out any magnetic or charge order. The spin-lattice relaxation rate below Tc exhibits a pronounced coherence peak and behaves within the weak-coupling BCS theory with nearly isotropic energy gap. Cd NMR results point to moderate ferromagnetic enhancement at high temperatures followed by rapid decrease of the density of states below the structural transition temperature of 200 K.
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.
In order to investigate the relationship between superconductivity and magnetism in bilayer-hydrate cobaltate Na_x(H_3O)_zCoO_2 \cdot yH_2O, Co nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) measurements were performed on three different samples, which demonstrate various ground states at low temperatures. The appearance of small internal fields is observed in the NQR spectra below approximately 6 K on one of the samples that possesses the largest c-axis length and the highest NQR frequency. The other two samples exhibit superconducting transition in zero magnetic fiel…
We report $^{121/123}$Sb nuclear quadrupole resonance (NQR) and $^{51}$V nuclear magnetic resonance (NMR) measurements on kagome metal CsV$_3$Sb$_5$ with $T_{\rm c}=2.5$ K. Both $^{51}$V NMR spectra and $^{121/123}$Sb NQR spectra split after a charge density wave (CDW) transition, which demonstrates a commensurate CDW state. The coexistence of the high temperature phase and the CDW phase between $91$ K and $94$ K manifests that it is a first order phase transition. At low temperature, electric-field-gradient fluctuations diminish and magnetic fluctuations become dominant. Superconductivity eme…
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.
$^{75}$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 139La, 57Fe and 75As nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) measurements on powders of the new LaO1-xFxFeAs superconductor for x = 0 and x = 0.1 at temperatures up to 480 K, and compare our measured NQR spectra with local density approximation (LDA) calculations. For all three nuclei in the x = 0.1 material, it is found that the local Knight shift increases monotonically with an increase in temperature, and scales with the macroscopic susceptibility, suggesting a single magnetic degree of freedom. Surprisingly, the spin lattice relaxation rates for al…
Magnetization and 63Cu NMR-NQR relaxation measurements are used to study the superconducting fluctuations in YBa2Cu3O6+x (YBCO) oriented powders. In optimally doped YBCO the fluctuating negative magnetization M_{fl}(H,T) is rather well described by an anisotropic Ginzburg-Landau (GL) functional and the curves M_{fl}/sqrt{H} cross at Tc. In underdoped YBCO, instead, over a wide temperature range an anomalous diamagnetism is observed, stronger than in the optimally doped compound by about an order of magnitude. The field and temperature dependences of M_{fl} cannot be described either by an anis…
We report 73Ge-NMR and NQR results for ferromagnetic (FM) superconductor URhGe. The magnitude and direction of the internal field, H_int, and parameters of the electric field gradient at the Ge site were determined experimentally. Using powdered polycrystalline samples oriented by different methods, the field dependences of NMR shift and nuclear spin relaxation rates for H_0 // c (easy axis) and H_0 // b were obtained. From the NMR shifts for H_0 // b, we confirmed a gradual suppression of the Curie temperature and observed a phase separation near the spin reorientation. The observation of the…
We discuss the novel superconducting characteristics and unusual normal-state properties of iron (Fe)-based pnictide superconductors REFeAsO$_{1-y}$ (RE=La,Pr,Nd) and Ba$_{0.6}$K$_{0.4}$Fe$_2$As$_2$($T_{c}=$ 38 K) by means of $^{57}$Fe-NMR and $^{75}$As-NQR/NMR. In the superconducting state of LaFeAsO$_{0.7}$ ($T_{c}=$ 28 K), the spin component of the $^{57}$Fe-Knight shift decreases to almost zero at low temperatures, which provide firm evidence of the superconducting state formed by spin-singlet Cooper pairing. The nuclear spin-lattice relaxation rates $(1/T_{1})$ in LaFeAsO$_{0.7}$ and Ba$_…
The dependence of the Maki-Thompson (MT) and of the density of states depletion (DOS) contributions from superconducting fluctuations (SF) to NMR-NQR relaxation is derived in the framework of the diagrammatic theory, applied to layered three dimensional (3D) high T_c superconductors. The regularization procedure devised for the conductivity (Buzdin and Varlamov, Phys. Rev. B, 58, 14195 (1998)) is used in order to avoid the divergence of the DOS term. The theoretical results are discussed in the light of NMR-NQR measurements in YBCO and compared with the recent theory (Eschrig et al., Phys. Rev…
Motivated by the recent observation of ferromagnetic spin correlations in the filled skutterudite SrFe$_4$As$_{12}$ [Ding et al., Phys. Rev. B 98, 155149 (2018)], we have carried out $^{75}$As nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) measurements to investigate the role of magnetic fluctuations in a newly discovered isostructural superconductor SrOs$_4$As$_{12}$ with a superconducting transition temperature of $T_{\rm c}$ $\sim$ 4.8 K. Knight shift $K$ determined by the NQR spectrum under a small magnetic field ($\le$ 0.5 T) is nearly independent of temperature, …
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…
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…
The relationship between charge density wave (CDW) orders and superconductivity in arsenide superconductor SrPt$_2$As$_2$ with $T_c$ = 5.2 K which crystallizes in the CaBe$_2$Ge$_2$-type structure was studied by $^{75}$As nuclear magnetic resonance (NMR) measurements up to 520 K, and $^{75}$As nuclear quadrupole resonance (NQR) and $^{195}$Pt-NMR measurements down to 1.5 K. At high temperature, $^{75}$As-NMR spectrum and nuclear spin relaxation rate ($1/T_1$) have revealed two distinct CDW orders, one realized in the As-Pt-As layer below $T_{\rm CDW}^{\rm As(1)}$ $=$ 410 K and the other in the…
We present the results of $^{75}$As nuclear magnetic resonance (NMR), nuclear quadrupole resonance (NQR), and resistivity measurements in KFe$_2$As$_2$ under pressure ($p$). The temperature dependence of the NMR shift, nuclear spin-lattice relaxation time ($T_1$) and resistivity show a crossover between a high-temperature incoherent, local-moment behavior and a low-temperature coherent behavior at a crossover temperature ($T^*$). $T^*$ is found to increase monotonically with pressure, consistent with increasing hybridization between localized $3d$ orbital-derived bands with the itinerant elect…
Co nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) studies were performed in the recently discovered UCoGe, in which the ferromagnetic and superconducting (SC) transitions were reported to occur at $T_{\rm Curie} \sim 3$ K and $T_S \sim 0.8$ K (N. T. Huy {\it et al.}, Phys. Rev. Lett. {\bf 99} (2007) 067006), in order to investigate the coexistence of ferromagnetism and superconductivity as well as the normal-state and SC properties from a microscopic point of view. From the nuclear spin-lattice relaxation rate $1/T_1$ and Knight-shift measurements, we confirmed that fe…
We report results of 75As nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) experiments as well as 7Li NMR on different samples of self flux grown LiFeAs and 5 % Co doped LiFeAs single crystals, and a polycrystalline LiFeAs sample. We were able to distinguish the samples by their slightly different quadrupole frequencies, $ν_Q$, which is a direct measure of the electric field gradient (EFG) at the As site. Interestingly, samples with a large quadrupole frequency appear to show a different Knight shift and spin lattice relaxation in the superconducting state from those wit…
We report 75As-nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) measurements on transition-metal arsenides LaRu2As2, KCa2Fe4As4F2, and A2Cr3As3. In the superconducting state of LaRu2As2, a Hebel- Slichter coherence peak is found in the temperature dependence of the spin-lattice relaxation rate-1/T1 just below Tc, which indicates that LaRu2As2 is a full-gap superperconducor. For KCa2Fe4As4F2, antiferromagnetic spin fluctuations are observed in the normal state. We further find that the anisotropy rate RAF = Tc1/Tab1 is small and temperature independent, implying that the …
The electronic and magnetic properties of the collapsed-tetragonal CaPd$_2$As$_2$ superconductor (SC) with a transition temperature of 1.27 K have been investigated by $^{75}$As nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) measurements. The temperature ($T$) dependence of the nuclear spin lattice relaxation rates (1/$T_1$) and the Knight shifts indicate the absence of magnetic correlations in the normal state. In the SC state, 1/$T_1$ measured by $^{75}$As NQR shows a clear Hebel-Slichter (HS) peak just below $T_{\rm c}$ and decreases exponentially at lower $T$, conf…
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 present our NMR studies of double-layer hydrated cobalt oxides NaxCoO2-yH2O (x ~ 0.35, y ~ 1.3) with various Tc = 0 - 4.8 K and magnetic transition temperatures. High-resolution $^{1}$H NMR spectrum served as an evidence for the existence of H$_{3}$O$^{+}$ oxonium ions. $^{23}$Na nuclear spin-lattice relaxation rates served to detect local field fluctuations sensitive to Tc. $^{59}$Co nuclear quadrupole resonance (NQR) spectra served to classify the various Tc samples. From the classification by $^{59}$Co NQR frequency, the double-layer hydrated compounds were found to have two superconduct…
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 the nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) measurements for non-centrosymmetric superconductors Re7B3, LaBiPt, and BiPd containing heavy elements. For all three compounds, the spin-lattice relaxation rate 1/T1 shows a coherence peak just below Tc and decreases exponentially at low temperatures, which indicates that an isotropic superconducting gap is dominant in these compounds. In BiPd, the height of the coherence peak just below Tc is much suppressed, which suggests that there exists a substantial component of gap with nodes in this compound. Our re…
We report $^{75}$As nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) studies on the superconductor Rb$_{2}$Cr$_{3}$As$_{3}$ with a quasi one-dimensional crystal structure. Below $T\sim$ 100 K, the spin-lattice relaxation rate (1/$T_{1}$) divided by temperature, 1/$T_{1}T$, increases upon cooling down to $T_{\rm c}$ = 4.8 K, showing a Curie-Weiss-like temperature dependence. The Knight shift also increases with decreasing temperature. These results suggest ferromagnetic spin fluctuation. In the superconducting state, 1/$T_{1}$ decreases rapidly below $T_{\text{c}}$ withou…
The static and the dynamic spin correlations in the low temperature collapsed tetragonal and the high temperature tetragonal phase in CaFe2As2 have been investigated by 75As nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) measurements. Through the temperature (T) dependence of the nuclear spin lattice relaxation rates (1/T1) and the Knight shifts, although stripe-type antiferromagnetic (AFM) spin correlations are realized in the high temperature tetragonal phase, no trace of the AFM spin correlations can be found in the non-superconducting, low temperature, collapsed te…
We report the $^{75}$As-NQR and NMR studies on the iron arsenide superconductor Li$_{x}$FeAs with $T_{\rm c} \sim 17$ K. The spin lattice relaxation rate, $1/T_{1}$, decreases below $T_{\rm c}$ without a coherence peak, and can be fitted by gaps with s$^{\pm}$-wave symmetry in the presence of impurity scattering. In the normal state, both $1/T_{1}T$ and the Knight shift decrease with decreasing temperature but become constant below $T \leq 50 K$. Estimate of the Korringa ratio shows that the spin correlations are weaker than that in other families of iron arsenides, which may account for the l…
$^{73}$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…
We report In-NQR and Co-NMR experiments of CeCoIn$_5$ that undergoes a superconducting transition with a record high $T_{\rm c}$ = 2.3 K to date among heavy-fermion superconductors. At zero magnetic field, an anomalous temperature ($T$) dependence of nuclear spin-lattice relaxation rate $1/T_1$ of $^{115}$In is explained by the relation $1/T_1\propto T\cdotχ_Q(T)^{3/4}$ based on the anisotropic spin-fluctuations model in case of the proximity to an antiferromagnetic (AFM) quantum critical point (QCP). The novel behavior of $1/T_1\sim T^{1/4}$ over a wide $T$ range of $T_{\rm c} < T < 40$ K ari…
We report $^{125}$Te nuclear magnetic resonance and $^{181}$Ta nuclear quadrupole resonance studies on single-crystal Ta$_{4}$Pd$_{3}$Te$_{16}$, which has a quasi-one-dimensional structure and superconducts below $T_{\rm c}=4.3$ K. $^{181}$Ta with spin $I=7/2$ is sensitive to quadrupole interactions, while $^{125}$Te with spin $I=1/2$ can only relax by magnetic interactions. By comparing the spin-lattice relaxation rate ( $1/T_{1}$) of $^{181}$Ta and $^{125}$Te, we found that electric-field-gradient (EFG) fluctuations develop below $80$ K. The EFG fluctuations are enhanced with decreasing temp…
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 demonstrate that the spin dynamics in underdoped Y(1-z)Ca(z)Ba(2)Cu(3)O(y) for y=~6.0 exhibit qualitatively the same behavior to underdoped La(2-x)Sr(x)CuO(4) for an equal amount of hole concentration p=z/2=x<0.11. However,a spin-gap appears as more holes are doped into the CuO(2) plane by increasing the oxygen concentration to y=~6.5 for a fixed value of Ca concentration z. Our results also suggest that Ca doping causes disorder effects that enhance the low frequency spin fluctuations.
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…
Pressure-induced superconductivity was studied for a spin-ladder cuprate Sr$_2$Ca$_{12}$Cu$_{24}$O$_{41}$ using nuclear magnetic resonance (NMR) under pressures up to the optimal pressure 3.8 GPa. Pressure application leads to a transitional change from a spin-gapped state to a Fermi-liquid state at temperatures higher than $T_c$. The relaxation rate $1/T_1$ shows activated-type behavior at an onset pressure, whereas Korringa-like behavior becomes predominant at the optimal pressure, suggesting that an increase in the density of states (DOS) at the Fermi energy leads to enhancement of $T_c$. N…
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 the $^{121/123}$Sb-NMR/nuclear quadrupole resonance (NQR) measurements on the newly-discovered superconductor BaTi$_2$Sb$_2$O with a two-dimensional Ti$_2$O square-net layer formed with Ti$^{3+}$ (3$d^1$). NQR measurements revealed that the in-plane four-fold symmetry is broken at the Sb site below $T_{\rm A} \sim$ 40 K, without an internal field appearing at the Sb site. These exclude a spin-density wave (SDW)/ charge density wave (CDW) ordering with incommensurate correlations, but can be understood with the commensurate CDW ordering at $T_{\rm A}$. The spin-lattice relaxation rate…
We report Cu-NMR/NQR and F-NMR studies on the multilayered high-T_c copper oxides Ba_2Ca_{n-1}Cu_nO_{2n}F_2 with n=2,3,4, where n is the number of CuO_2 planes. It is revealed that bi-layered Ba_2CaCu_2O_4F_2 is an underdoped superconductor with hole carriers, which are introduced into CuO_2 planes by an unexpected deviation from the nominal content of apical fluorines. In a previous paper, we proposed a self-doping mechanism as the origin of carrier doping in n=3 and n=4; in the mechanism, electrons are transferred from the inner CuO_2 plane (IP) to the outer one (OP). However, since it has b…
^{69,71}Ga NMR/NQR studies have been performed on a single crystal of the transuranium superconductor PuRhGa_{5} with Tc ~ 9 K. We have observed a ^{69}Ga NQR line at ~29.15 MHz, and assigned it to the $4i$ Ga site using the NMR results. The ^{69}Ga NQR spin-lattice relaxation rate 1/T_{1} shows no coherence peak just below Tc, but obeys a T^{3} behavior below Tc. This result strongly suggests that PuRhGa_{5} is an unconventional superconductor having an anisotropic superconducting gap.
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 …
In order to investigate the coexistence of magnetism and superconductivity on a microscopic scale, local studies using zero-field spin-echo ^{99,101}Ru NMR and ^{63,65}Cu NQR have been carried out on both superconducting and non-superconducting samples of magnetically ordered RuSr_{2}EuCu_{2}O_{8} and RuSr_{2}GdCu_{2}O_{8}. ^{99,101}Ru NMR signals were observed at 1.3 K over two distinct frequency ranges. The high frequency spectra (110 to 150 MHz), which are essentially the same for all samples, are characterized by five sharp peaks for each isotope corresponding to a hyperfine field of appro…
We present a detailed NQR, NMR and $μ$SR study of a magnetic phase obtained during a topotactic chemical reaction of YBa$_{2}$Cu$_{3}$O$_{6.5}$ high- temperature superconductor with low-pressure water vapor. Our studies give straightforward evidence that the ''empty'' Cu(1) chains play the role of an easy water insertion channel. It is shown that the NQR spectrum of the starting material transforms progressively under insertion of water, and completely disappears when one H$_{2}$O molecule is inserted per unit cell. Similarly, a Cu ZFNMR signal characteristic of this water inserted material ap…
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 …
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…
We report an 75As-nuclear quadrupole resonance (NQR) study on heavily electron-doped LaFeAsO_1-xF_x(La1111) with Tc=5 K. Nuclear spin relaxation rate (1/T1) measurement has revealed that a Hebel-Slichter (HS) peak partially recovers in heavily electron-overdoped regimes where the nesting condition of hole and electron Fermi surfaces(FSs) becomes significantly worse. This is in contrast to previous results reported in optimally doped La1111 with Tc=28 K where a lack of the HS peak was reported. It indicates that the interband scattering between the hole and electron FSs is strongly suppressed b…
We have synthesized various samples of the $x=2/3$ phase of sodium cobaltate Na$_{x}$CoO$_{2}$ and performed X-ray powder diffractions spectra to compare the diffraction with the structure proposed previously from NMR/NQR experiments [H. Alloul \emph{et al.}, EPL \textbf{85}, 47006 (2009)]. Rietveld analysis of the data are found in perfect agreement with those, and confirm the concentration x=2/3 obtained in the synthesis procedure. They even give indications on the atomic displacements of Na inside the unit cell. The detailed NQR data allow us to identify the NQR transitions and electric fie…
We report on 139La and 63Ccu NMR/NQR measurements in the high-Tc superconductor La1.90Sr0.10CuO4 with Tc=26.5 K. Spin fluctuations probed by 139La spin-lattice relaxation (T1), continuously slow down on cooling through Tc. We argue that spin-freezing and superconductivity are bulk effects in this sample. Thus, both phenomena have to coexist microscopically. The distribution of 139La T1 values at low temperature reveals a wide spread of spin fluctuation frequencies in CuO2 planes. A simple estimate shows that Cu nuclei at sites where electronic fluctuations are the slowest are not observable be…
We study the effect of thermal fluctuations of the s-wave order parameter of a quasi two dimensional superconductor on the nuclear spin relaxation rate near the transition temperature Tc. We consider both the effects of the amplitude fluctuations and the Berezinskii-Kosterlitz-Thouless (BKT) phase fluctuations in weakly coupled layered superconductors. In the treatment of the amplitude fluctuations we employ the Gaussian approximation and evaluate the longitudinal relaxation rate 1/T1 for a clean s-wave superconductor, with and without pair breaking effects, using the static pair fluctuation p…
We report 75As-nuclear quadrupole resonance (NQR) studies on (Ca_4Al_2O_{6-y})(Fe_2As_2) with Tc=27K, which unravel unique normal-state properties and point to unconventional nodeless superconductivity (SC). Measurement of nuclear-spin-relaxation rate 1/T_1 has revealed a significant development of two dimensional (2D) antiferromagnetic (AFM) spin fluctuations down to Tc, in association with the fact that FeAs layers with the smallest As-Fe-As bond angle are well separated by thick perovskite-type blocking layer. Below Tc, the temperature dependence of 1/T_1 without any trace of the coherence …
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,…
A 63Cu and 139La NMR/NQR study of superconducting (Tc=7 K) La1.94Sr0.06CuO4 single crystal is reported. Coexistence of spin-glass and superconducting phases is found below ~5 K from 139La NMR relaxation. 63Cu and 139La NMR spectra show that, upon cooling, CuO2 planes progressively separate into two magnetic phases, one of them having enhanced antiferromagnetic correlations. These results establish the AF-cluster nature of the spin-glass. We discuss how this phase can be related to the microsegregation of mobile holes and to the possible pinning of charge-stripes.
