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Register a new userOrbital Properties of Sr3Ru2O7 and Related Ruthenates Probed by 17O-NMR
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We report a site-separated $^{17}$O-NMR study of the layered perovskite ruthenate Sr$_3$Ru$_2$O$_7$, which exhibits nearly two-dimensional transport properties and itinerant metamagnetism at low temperatures. The local hole occupancies and the spin densities in the oxygen $2p$ orbitals are obtained by means of tight-binding analyses of electric field gradients and anisotropic Knight shifts. These quantities are compared with two other layered perovskite ruthenates: the two-dimensional paramagnet Sr$_2$RuO$_4$ and the three-dimensional ferromagnet SrRuO$_3$. The hole occupancies at the oxygen sites are very large, about one hole per ruthenium atom. This is due to the strong covalent character of the Ru-O bonding in this compound. The magnitude of the hole occupancy might be related to the rotation or tilt of the RuO$_6$ octahedra. The spin densities at the oxygen sites are also large, 20-40% of the bulk susceptibilities, but in contrast to the hole occupancies, the spin densities strongly depend on the dimensionality. This result suggests that the density-of-states at the oxygen sites plays an essential role for the understanding of the complex magnetism found in the layered perovskite ruthenates.
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We have investigated the spin dynamics in the bilayered perovskite Sr3Ru2O7 as a function of magnetic field and temperature using 17O-NMR. This system sits close to a metamagnetic quantum critical point (MMQCP) for the field perpendicular to the ruthenium oxide planes. We confirm Fermi-liquid behavior at low temperatures except for a narrow field region close to the MMQCP. The nuclear spin-lattice relaxation rate divided by temperature 1/T1T is enhanced on approaching the metamagnetic critical field of 7.9 T and at the critical field 1/T1T continues to increase and does not show Fermi- liquid behavior down to 0.3 K. The temperature dependence of T1T in this region suggests the critical temperature Theta to be 0 K, which is a strong evidence that the spin dynamics possesses a quantum critical character. Comparison between uniform susceptibility and 1/T1T reveals that antiferromagnetic fluctuations instead of two-dimensional ferromagnetic fluctuations dominate the spin fluctuation spectrum at the critical field, which is unexpected for itinerant metamagnetism.
We report temperature and thermal-cycling dependence of surface and bulk structures of double-layered perovskite Sr3Ru2O7 single crystals. The surface and bulk structures were investigated using low-energy electron diffraction (LEED) and single-crystal X-ray diffraction (XRD) techniques, respectively. Single-crystal XRD data is in good agreement with previous reports for the bulk structure with RuO6 octahedral rotation, which increases with decreasing temperature (~ 6.7(6)degrees at 300 K and ~ 8.1(2) degrees at 90 K). LEED results reveal that the octahedra at the surface are much more distorted with a higher rotation angle (~ 12 degrees between 300 and 80 K) and a slight tilt ((4.5pm2.5) degrees at 300 K and (2.5pm1.7) degrees at 80 K). While XRD data confirms temperature dependence of the unit cell height/width ratio (i.e. lattice parameter c divided by the average of parameters a and b) found in a prior neutron powder diffraction investigation, both bulk and surface structures display little change with thermal cycles between 300 and 80 K.
The S=1/2 Heisenberg spin chain compound SrCuO2 doped with different amounts of nickel (Ni), palladium (Pd), zinc (Zn) and cobalt (Co) has been studied by means of Cu nuclear magnetic resonance (NMR). Replacing only a few of the S=1/2 Cu ions with Ni, Pd, Zn or Co has a major impact on the magnetic properties of the spin chain system. In the case of Ni, Pd and Zn an unusual line broadening in the low temperature NMR spectra reveals the existence of an impurity-induced local alternating magnetization (LAM), while exponentially decaying spin-lattice relaxation rates $T_1^{-1}$ towards low temperatures indicate the opening of spin gaps. A distribution of gap magnitudes is proven by a stretched spin-lattice relaxation and a variation of $T_1^{-1}$ within the broad resonance lines. These observations depend strongly on the impurity concentration and therefore can be understood using the model of finite segments of the spin 1/2 antiferromagnetic Heisenberg chain, i.e. pure chain segmentation due to S = 0 impurities. This is surprising for Ni as it was previously assumed to be a magnetic impurity with S = 1 which is screened by the neighboring copper spins. In order to confirm the S = 0 state of the Ni, we performed x-ray absorption spectroscopy (XAS) and compared the measurements to simulated XAS spectra based on multiplet ligand-field theory. Furthermore, Zn doping leads to much smaller effects on both the NMR spectra and the spin-lattice relaxation rates, indicating that Zn avoids occupying Cu sites. For magnetic Co impurities, $T_1^{-1}$ does not obey the gap like decrease, and the low-temperature spectra get very broad. This could be related to the increase of the Neel temperature which was observed by recent muSR and susceptibility measurements, and is most likely an effect of the impurity spin $S eq0$.
Sb-NMR/NQR study has revealed a formation of a pseudogap at the Fermi level in the density of states in a valence fluctuating compound CeIrSb. The nuclear spin-lattice relaxation rate divided by temperature, 1/T_1T has a maximum around 300 K and decreases significantly as 1/T_1T ~ T^2, followed by a 1/T_1T = const. relation at low temperature. This temperature dependence of 1/T_1T is well reproduced by assuming a V-shaped energy gap with a residual density of states at the Fermi level. The size of energy gap for CeIrSb is estimated to be about 350 K, which is by one order of magnitude larger than those for the isostructural Kondo semiconductors CeRhSb and CeNiSn. Despite the large difference in the size of energy gap, CeIrSb, CeRhSb and CeNiSn are indicated to be classified into the same group revealing a V-shaped gap due to c-f hybridization. The temperature dependence of the Knight shift measured in a high magnetic field agrees with the formation of this pseudogap.
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 all nuclei also scale with one another, despite the fact that the form factors for each site sample different regions of q-space. This result suggests a lack of any q-space structure in the dynamical spin susceptibility that might be expected in the presence of antiferromagnetic correlations. Rather, our results are more compatible with simple quasi-particle scattering. Furthermore, we find that the increase in the electric field gradient at the As cannot be accounted for by LDA calculations, suggesting that structural changes, in particular the position of the As in the unit cell, dominate the NQR response.
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