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^{75}As and ^{139}La NMR and nuclear quadrupole resonance (NQR) studies on Zn-substituted LaFeAsO_{0.85} have been performed to microscopically investigate the Zn-impurity effects. 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, but due to strong nonmagnetic pair-breaking effect to superconductivity.

Nonmagnetic impurity effect was studied on the n-type Fe-based superconductor BaFe1.87Co0.13As2 (Tc = 25 K) by a successful Zn substitution for Fe up to 7 at.%. Magnetic susceptibility, electrical resistivity, specific heat, and Hall coefficient measurements indicated that Tc linearly decreases with the Zn concentration and disappears at 7 at.%. The result is quantitatively comparable with what was observed for YBCO, while it disagrees with a recent report for the p-type Ba0.5K0.5Fe2As2. Fragile SC against a nonmagnetic impurity was first confirmed for the n-type 122 Fe-based superconductor., 14 pages, 5 figures

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 field, while these two samples show different ground states in the magnetic fields greater than 5 T. The comparison of the NMR spectra of these two samples obtained in high magnetic fields reveals the appearance of static internal magnetic fields at the Co site below 4 K in the sample that possesses the intermediate c-axis length and the NQR frequency., 11 pages, 10 figures, accepted for publication in Phys. Rev. B

The M-1222 compounds are synthesized in near single phase form. These compounds crystallise in I4/mmm Tetragonal structure. None of the studied compound is superconducting but they asre weakly magnetic. This is first report on synthesis of Cr and Mn -1222 compounds. These compounds are synthesized at ultra conditions of HPHT that is the 6 Gpa and 1400 C., 14 Pages: text + figs. accepted: materials leters (2006)

Various samples of sodium cobalt oxyhydrate with relatively large amounts of Na$^{+}$ ions were synthesized by a modified soft-chemical process in which a NaOH aqueous solution was added in the final step of the procedure. From these samples, a superconducting phase diagram was determined for a section of a cobalt valence of $\sim$+3.48, which was compared with a previously obtained one of $\sim$+3.40. The superconductivity was significantly affected by the isovalent exchanger of Na$^{+}$ and H$_{3}$O$^{+}$, rather than by variation of Co valence, suggesting the presence of multiple kinds of Fermi surface. Furthermore, the high-field magnetic susceptibility measurements for one sample up to 30 T indicated an upper critical field much higher than the Pauli limit supporting the validity of the spin-triplet pairing mechanism., 4 figures and 1 table

We measured $^{23}$Na-NMR spectra and nuclear spin-lattice relaxation rates $^{23}(1/T_1)$ of superconducting and non-superconducting bilayer hydrate $Na_xCoO_2-yH_2O$ (x ~ 0.3, y ~ 1.3). The central resonance frequency shows a small but various shift due to the difference in the shielding effect by intercalated $H_2O$ molecules. The different shielding effect also gives a large difference in the magnitude of $^{23}(1/T_1)$., 2 pages with 2 figures, submitted to Physica B (SCES '05)

The sodium rhodate NaRh2O4 was synthesized for the first time and characterized by neutron and x-ray diffraction studies, measurements of magnetic susceptibility, specific heat, electrical resistivity, and the Seebeck coefficient. NaRh2O4 crystallizes in the CaFe2O4-type structure, which is comprised of a characteristic RhO6 octahedra network. The compound is metallic in nature, probably reflecting the 1 to 1 mixed valence character of Rh(III) and Rh(IV) in the network. For further studies of the compound, the Rh valence was varied significantly by means of an aliovalent substitution: the full range solid solution between NaRh2O4 and CaRh2O4 was achieved and characterized as well. The metallic state was dramatically altered, and a peculiar magnetism developed in the low Na concentration range., Accepted for publication in Chem. Mater

A weak magnetic order was found in a non-superconducting bilayered-hydrate Na$_{x}$CoO$_{2}\cdot y$H$_{2}$O sample by a Co Nuclear Quadrupole Resonance (NQR) measurement. The nuclear spin-lattice relaxation rate divided by temperature $1/T_1T$ shows a prominent peak at 5.5 K, below which a Co-NQR peak splits due to an internal field at the Co site. From analyses of the Co NQR spectrum at 1.5 K, the internal field is evaluated to be $\sim$ 300 Oe and is in the $ab$-plane. The magnitude of the internal field suggests that the ordered moment is as small as $\sim 0.015$ $\mu_B$ using the hyperfine coupling constant reported previously. It is shown that the NQR frequency $\nu_Q$ correlates with magnetic fluctuations from measurements of NQR spectra and $1/T_1T$ in various samples. The higher-$\nu_Q$ sample has the stronger magnetic fluctuations. A possible phase diagram in Na$_{x}$CoO$_{2}\cdot y$H$_{2}$O is depicted using $T_c$ and $\nu_Q$, in which the crystal distortion along the c-axis of the tilted CoO$_2$ octahedron is considered to be a physical parameter. Superconductivity with the highest $T_c$ is seemingly observed in the vicinity of the magnetic phase, suggesting strongly that the magnetic fluctuations play an important role for the occurrence of the superconductivity., Comment: 5 pages, 6 figures, submitted to J. Phys. Soc. Jpn

We synthesized powder samples of Na$_{x}$CoO$_{2}\cdot y$H$_{2}$O changing the volume of the water in the hydration process, then investigated their superconducting properties,. It was proved that the volume of water is one of key parameters to obtain a single phase of Na$_{x}$CoO$_{2}\cdot y$H$_{2}$O with good superconducting properties. The transition temperature, $T_{c}$, of the sample changed gradually while it was stored in the atmosphere of 70% humidity. Superconducting behavior under high magnetic field was very sensitive to $T_{c}$. $H_{c2}$ of a high quality sample with high $T_{c}$ seemed very high., 7 pages (3 figures included) and two extra figures (gif), proceedings of TICS'04 & WLTP7

We synthesized the five batches of the samples of the novel P3 type superconductor, Na$_{x}$(H$_{3}$O)$_{y'}$CoO$_{2}\cdot y''$H$_{2}$O, by the soft chemical process starting from $\alpha$-NaCoO$_{2}$. The chemical and structural properties varied rather widely from batch to batch, with a result that $T_{c}$ varied from 4.6 K to 3.2 K. The magnetic susceptibility above $T_{c}$ shows upturn at low temperature as in the case of the P2 phase. The $T_{c}$ seems to be well correlated to the lattice parameters., Comment: 2 pages, 2 figures, and 1 table, to be published in J. Phys. Soc. Jpn. 73 (9) with possible minor revisions

Comprehensive low-temperature specific heat data C(T,H) of Na_0.35CoO2-1.3H_2O with temperature T down to 0.6 K and the magnetic field H up to 8 T are presented. For the normal state, the values of gamma_n=13.94 mJ/mol K2, and Debye temperature 362 K are reported. At zero field, a very sharp superconducting anomaly was observed at Tc=4.5 K with DeltaC/gamma_nTc=1.45. The superconducting volume fraction is estimated to be 47.4 % based on the consideration of entropy balance at Tc for the second-order superconducting phase transition. In the superconducting state, the electronic contribution C_es at H=0 can be well described by the model of the line nodal order parameter. In low H, gamma(H) H^1/2 which is also a manifestation of the line nodes. The behaviors of both Tc(H) and gamma(H) suggest the anisotropy of Hc2 or possible crossovers or transitions occurring in the mixed state., Published as a Rapid Communication in Phys. Rev. B. New measurements on the new Na_0.35CoO2-1.3H_2O sample. The results in the mixed state are emphasized. Related to cond-mat/0308031. Another paper cond-mat/0409760 from Berkeley group also discusses similar issues

The solid solution between the ferromagnetic metal SrRuO$_3$ and the enhanced paramagnetic metal SrRhO$_3$ was recently reported [K. Yamaura et al., Phys. Rev. B 69 (2004) 024410], and an unexpected feature was found in the specific heat data at $x$=0.9 of SrRu$_{1-x}$Rh$_x$O$_3$. The feature was reinvestigated further by characterizing additional samples with various Ru concentrations in the vicinity of $x$=0.9. Specific heat and magnetic susceptibility data indicate that the feature reflects a peculiar magnetism of the doped perovskite, which appears only in the very narrow composition range 0.85$, Comment: Accepted for publication in a special issue of Physica B (the proceedings of SCES04)

Nuclear-magnetic-resonance (NMR) studies were performed in Na$_{0.7}$CoO$_2$ to investigate its magnetic properties from the microscopic point of view. Na$_{0.7}$CoO$_2$ is a starting compound of the recently discovered superconductor Na$_{0.35}$CoO$_2$$\cdot 1.3$H$_2$O, in which Co atoms form a triangular structure. Although $^{23}$Na-NMR results show no magnetic anomaly down to 1.5 K, Knight shift ($^{23}K$) and $^{23}(1/T_1T)$ of $^{23}$Na continue to increase, suggestive of the vicinity of the magnetic phase. From the relation between $^{23}K$ and $^{23}(1/T_1T)$, it is shown that ferromagnetic fluctuations are dominant below 100 K. In addition to the ferromagnetic correlations, antiferromagnetic fluctuations are also developed in a low temperature region below 4 K. Magnetic fluctuations suggested by our experiment are discussed., 5 pages, 6 figures, submitted to J. Phys. Soc. Jpn

We have performed Co-nuclear quadrupole resonance (NQR) studies on Na$_{x}$CoO$_{2}\cdot y$H$_{2}$O compounds with different Na ($x$) and hydrate ($y$) contents. Two samples with different Na contents but nearly the same $T_c$ values ($x$ = 0.348, $T_c$ = 4.7 K ; $x$ = 0.339, $T_c$ = 4.6 K) were investigated. The spin-lattice relaxation rate $1/T_1$ in the superconducting (SC) and normal states is almost the same for the two samples except just above $T_c$. NQR measurements were also performed on different-hydrate-content samples with different $T_c$ values, which were prepared from the same Na-content ($x$ = 0.348) sample. From measurements of $1/T_1$ using the different-hydrate-content samples, it was found that a low-$T_c$ sample with $T_c = 3.9$ K has a larger residual density of states (DOS) in the SC state and a smaller increase of $1/T_1T$ just above $T_c$ than a high-$T_c$ sample with $T_c$ = 4.7 K. The former behavior is consistent with that observed in unconventional superconductors, and the latter suggests the relationship between $T_c$ and the increase in DOS just above $T_c$. This increase, which is seemingly associated with the two-dimensionality of the CoO$_2$ plane, is considered to be one of the most important factors for the occurrence of superconductivity., 5 pages, 5 figures, To be published in J. Phys. Soc. Jpn

The tri-layered perovskite Sr4Rh3O10 is reported for the first time. High-pressure and high-temperature heating (6 GPa and 1500 C) brought about successful preparation of a polycrystalline sample of the expected member at n=3 of Srn+1RhnO3n+1. Neutron-diffraction studies revealed the orthorhombic crystal structure (Pbam) at room temperature and 3.4 K. Local structure distortions rotationally tilt the RhO6 octahedra ~12 degrees in the perovskite-based blocks along the c-axis, and approximately a 20 % disorder was found in sequence of the alternating rotational tilt. The sample was also investigated by measurements of specific heat, thermopower, magnetic susceptibility, and electrical resistivity. The data clearly revealed enhanced paramagnetism and electrically conducting character, which reflected nature of the correlated 4d5-electrons of Rh4+. However, no clear signs of magnetic and electrical transitions were observed above 2 K and below 70 kOe, providing a remarkable contrast to the rich electronic phenomena for the significantly relevant ruthenate, Sr4Ru3O10., Accepted for publication in Chem. Mater

High-energy (h$\nu$ = 5.95 keV) synchrotron Photoemission spectroscopy (PES) is used to study bulk electronic structure of Na$_{0.35}$CoO$_{2}$.1.3H$_{2}$O, the layered superconductor. In contrast to 3-dimensional doped Co oxides, Co $\it{2p}$ core level spectra show well-separated Co$^{3+}$ and Co$^{4+}$ ions. Cluster calculations suggest low spin Co$^{3+}$ and Co$^{4+}$ character, and a moderate on-site Coulomb correlation energy U$_{dd}\sim$3-5.5 eV. Photon dependent valence band PES identifies Co $\it{3d}$ and O $\it{2p}$ derived states, in near agreement with band structure calculations., Comment: 4 pages 4 figures Revised text added reference

The solid-solution SrRu$_{1-x}$Rh$_x$O$_3$ ($0\le x \le1$) is a variable-electron-configuration system forming in the nearly-cubic-perovskite basis, ranging from the ferromagnetic 4$d^4$ to the enhanced paramagnetic 4$d^5$. Polycrystalline single-phase samples were obtained over the whole composition range by a high-pressure-heating technique, followed by measurements of magnetic susceptibility, magnetization, specific heat, thermopower, and electrical resistivity. The ferromagnetic order in long range is gradually suppressed by the Rh substitution and vanishes at $x \sim 0.6$. The electronic term of specific-heat shows unusual behavior near the critical Rh concentration; the feature does not match even qualitatively with what was reported for the related perovskites (Sr,Ca)RuO$_3$. Furthermore, another anomaly in the specific heat was observed at $x \sim 0.9$., Accepted for publication in PRB

Comprehensive studies of the low-temperature specific heat C(T,H) in NaxCoO2-yH2O are presented. At H=0, a very sharp anomaly was observed at T=4.7 K indicating the existence of bulk superconductivity. There exists the T^2 term in C(T,H=0) in the superconducting state manifesting the line nodal superconducting order parameter. The superconducting volume fraction is estimated to be 26.6 % based on the consideration of entropy conservation at Tc for the second-order superconducting phase transition. An abrupt change of the slope in Tc(H) was observed. Possible scenarios such as the multiple phase transitions in the mixed state are discussed., 10 pages, 4 figures; the statement of entropy imbalance in the previous version was withdrawn

We have studied the magnetic properties of the non-superconducting RuSr2Ln1.5Ce0.5Cu2O10 (Ln=Y, Dy and Ho, Ru-1222) compounds synthesized under high pressure (6 Gpa) at elevated temperature. The materials become magnetically ordered at TM =152(2) K regardless of Ln. The wide ferromagnetic-like hysteresis loops which open at 5 K, close themselves around Tirr= 90-100 K and the remanent magnetizations (Mrem) and the coercive fields (HC) become zero. Surprisingly, at Tirr, Comment: 15 pages of text with figure. Submitted to Phys. Rev. B

The title quasi-1D copper oxides (0=< x =, To be published in PRB

科研費報告書収録論文(課題番号:16310081/研究代表者:白井正文/ナノ磁性材料におけるスピン構造とそのダイナミクスに関する理論研究)