Magnetic ground state of pyrochlore oxides close to metal-insulator boundary probed by muon spin rotation

Magnetism of ruthernium pyrochlore oxides A2Ru2O7 (A = Hg, Cd, Ca), whose electronic properties within a localized ion picture are characterized by non-degenerate t2g orbitals (Ru5+, 4d3) and thereby subject to geometrical frustration, has been investigated by muon spin rotation/relaxation (muSR) technique. The A cation (mostly divalent) was varied to examine the effect of covalency (Hg > Cd > Ca) on their electronic property. In a sample with A = Hg that exhibits a clear metal-insulator (MI) transition below >> 100 K (which is associated with a weak structural transition), a nearly commensurate magnetic order is observed to develop in accordance with the MI transition. Meanwhile, in the case of A = Cd where the MI transition is suppressed to the level of small anomaly in the resistivity, the local field distribution probed by muon indicates emergence of a certain magnetic inhomogeneity below {\guillemotright} 30 K. Moreover, in Ca2Ru2O7 that remains metallic, we find a highly inhomogeneous local magnetism below >>25 K that comes from randomly oriented Ru moments and thus described as a "frozen spin liquid" state. The systematic trend of increasing randomness and itinerant character with decreasing covalency suggests close relationship between these two characters. As a reference for the effect of orbital degeneracy and associated Jahn-Teller instability, we examine a tetravalent ruthernium pyrochlore, Tl2Ru2O7 (Ru4+, 4d4), where the result of muSR indicates a non-magnetic ground state that is consistent with the formation of the Haldane chains suggested by neutron diffraction experiment.Comment: 12 pages, 13 figure

Incommensurate spin correlations induced by magnetic Fe ions substituted into overdoped Bi1.75Pb0.35Sr1.90CuO6+z

Spin correlations in the overdoped region of Bi1.75Pb0.35Sr1.90CuO6+z have been explored with Fe-doped single crystals characterized by neutron scattering, muon-spin-rotation (muSR) spectroscopy, and magnetic susceptibility measurements. Static incommensurate spin correlations induced by the Fe spins are revealed by elastic neutron scattering. The resultant incommensurability delta is unexpectedly large (~0.2 r.l.u.), as compared with delta ~ 1/8 in overdoped superconductor La2-xSrxCuO4. Intriguingly, the large delta in this overdoped region is close to the hole concentration p. This result is reminiscent of the delta ~ p trend observed in underdoped La2-xSrxCuO4; however, it is inconsistent with the saturation of delta in the latter compound in the overdoped regime. While our findings in Fe-doped Bi1.75Pb0.35Sr1.90CuO6+z support the commonality of incommensurate spin correlations in high-Tc cuprate superconductors, they also suggest that the magnetic response might be dominated by a distinct mechanism in the overdoped region.Comment: 4 pages, 5 figures. Revision in introduction, discussion, and conclusion

Local electronic structure of interstitial hydrogen in MgH2_2 inferred from muon study

Magnesium hydride has great potential as a solid hydrogen (H) storage material because of its high H storage capacity of 7.6 wt%. However, its slow hydrogenation and dehydrogenation kinetics and the high temperature of 300 $^\circ$C required for decomposition are major obstacles to small-scale applications such as automobiles. The local electronic structure of interstitial H in MgH$_2$ is an important fundamental knowledge in solving this problem, which has been studied mainly based on density functional theory (DFT). However, few experimental studies have been performed to assess the results of DFT calculations. We have therefore introduced muon (Mu) as pseudo-H into MgH$_2$ and investigated the corresponding interstitial H states by analyzing their electronic and dynamical properties in detail. As a result, we observed multiple Mu states similar to those observed in wide-gap oxides, and found that their electronic states can be attributed to relaxed-excited states associated with donor/acceptor levels predicted by the recently proposed "ambipolarity model". This provides an indirect support for the DFT calculations on which the model is based via the donor/acceptor levels. An important implication of the muon results for improved hydrogen kinetics is that dehydrogenation, serving as a $reduction$ for hydrides, stabilizes the interstitial H$^-$ state.Comment: 14 pages, 9 figure

Direct observation of oxygen polarization in Sr2_2IrO4_4 by O KK-edge x-ray magnetic circular dichroism

X-ray absorption spectroscopy (XAS) and magnetic circular dichroism (XMCD) measurements at the oxygen (O) $K$-edge were performed to investigate the magnetic polarization of ligand O atoms in the weak ferromagnetic (WFM) phase of the Ir perovskite compound Sr$_2$IrO$_4$. With the onset of the WFM phase below $T_{\rm N}\simeq240$ K, XMCD signals corresponding to XAS peaks respectively identified as originating from the magnetic moments of apical and planar oxygen (O$_{\rm A}$ and O$_{\rm P}$) in the IrO$_6$ octahedra were observed. The observation of magnetic moments at O$_{\rm A}$ sites is consistent (except for the relative orientation) with that suggested by prior muon spin rotation ($\mu$SR) experiment in the non-collinear antiferromagnetic (NC-AFM) phase below $T_{\rm M}\approx100$ K. Assuming that the O$_{\rm A}$ magnetic moment observed by $\mu$SR is also responsible for the corresponding XMCD signal, the magnetic moment of O$_{\rm P}$ is estimated to be consistent with the previous $\mu$SR result. Since the O$_{\rm A}$ XMCD signal is mainly contributed by Ir 5$d$ $zx$ and $yz$ orbitals which also hybridize with O$_{\rm P}$, it is inferred that the relatively large O$_{\rm P}$ magnetic moment is induced by Ir 5$d$ $xy$ orbitals. Moreover, the inversion of O$_{\rm A}$ moments relative to Ir moments between the two magnetic phases revealed by XMCD suggests the presence of competing magnetic interactions for O$_{\rm A}$, with which the ordering of O$_{\rm A}$ moments in the NC-AFM phase may be suppressed to $T_{\rm M}$.Comment: 6 pages, 6 figure