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