A novel route to phase formation of cobalt oxyhydrates using KMnO4 as an oxidizing agent

We have first succeefully synthesized the sodium cobalt oxyhydrate superconductors using KMnO4 as a de-intercalating and oxidizing agent. It is a novel route to form the superconductive phase of NaxCoO2.yH2O without resorting to the commonly used Br2/CH3CN solution. The role of the KMnO4 is to de-intercalate the Na+ from the parent compound Na0.7CoO2 and oxidize the Co ion as a result. The higher molar ratio of KMnO4 relative to the sodium content tends to remove more Na+ from the parent compound and results in a slight expansion of the c-axis in the unit cell. The superconducting transition temperature is 4.6-3.8 K for samples treated by the aqueous KMnO4 solution with the molar ratio of KMnO4 relative to the sodium content in the range of 0.3 and 2.29.Comment: 10 pages, 3 figure

Slow spin relaxation in a highly polarized cooperative paramagnet

We report measurements of the ac susceptibility of the cooperative paramagnet Tb2Ti2O7 in a strong magnetic field. Our data show the expected saturation maximum in chi(T) and also an unexpected low frequency dependence (< 1 Hz) of this peak, suggesting very slow spin relaxations are occurring. Measurements on samples diluted with nonmagnetic Y3+ or Lu3+ and complementary measurements on pure and diluted Dy2Ti2O7 strongly suggest that the relaxation is associated with dipolar spin correlations, representing unusual cooperative behavior in a paramagnetic system.Comment: Accepted for publication in Physical Review Letter

Quantum and thermal spin relaxation in diluted spin ice: Dy(2-x)MxTi2O7 (M = Lu, Y)

We have studied the low temperature a.c. magnetic susceptibility of the diluted spin ice compound Dy(2-x)MxTi2O7, where the magnetic Dy ions on the frustrated pyrochlore lattice have been replaced with non-magnetic ions, M = Y or Lu. We examine a broad range of dilutions, 0 <= x <= 1.98, and we find that the T ~ 16 K freezing is suppressed for low levels of dilution but re-emerges for x > 0.4 and persists to x = 1.98. This behavior can be understood as a non-monotonic dependence of the quantum spin relaxation time with dilution. The results suggest that the observed spin freezing is fundamentally a single spin process which is affected by the local environment, rather than the development of spin-spin correlations as earlier data suggested.Comment: 26 pages, 9 figure

Geometrical Magnetic Frustration in Rare Earth Chalcogenide Spinels

We have characterized the magnetic and structural properties of the CdLn2Se4 (Ln = Dy, Ho), and CdLn2S4 (Ln = Ho, Er, Tm, Yb) spinels. We observe all compounds to be normal spinels, possessing a geometrically frustrated sublattice of lanthanide atoms with no observable structural disorder. Fits to the high temperature magnetic susceptibilities indicate these materials to have effective antiferromagnetic interactions, with Curie-Weiss temperatures theta ~ -10 K, except CdYb2S4 for which theta ~ -40 K. The absence of magnetic long range order or glassiness above T = 1.8 K strongly suggests that these materials are a new venue in which to study the effects of strong geometrical frustration, potentially as rich in new physical phenomena as that of the pyrochlore oxides.Comment: 17 pages, 5 figures, submitted to Phys Rev B; added acknowledgement