Structural characterization, magnetic behavior and high-resolution EELS study of new perovskites Sr2Ru2−xCoxO6−δ (0.5?x?1.5) |
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Authors: | AD Lozano-Gorrín JE Greedan P Núñez GA Botton |
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Institution: | a Brockhouse Institute for Materials Research, McMaster University, Hamilton, Ont., Canada L8S 4M1 b Department of Chemistry, McMaster University, 1280 Main Street W., Hamilton, Ont., Canada L8S 4M1 c Departamento de Química Inorgánica, Universidad de La Laguna, 38206-La Laguna, Tenerife, Spain d Departamento de Física Fundamental II, Universidad de La Laguna, 38200-La Laguna, Tenerife, Spain |
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Abstract: | New oxides of general formula Sr2Ru2−xCoxO6−δ (0.5?x?1.5) have been synthesized as polycrystalline materials and characterized structurally by X-ray diffraction. For 0.5?x<0.67 the orthorhombic, Pnma, perovskite structure of the end member, SrRuO3, is found. At x=0.67 a phase separation into an Ru-rich Pnma phase and a Co-rich I2/c phase occurs. The I2/c form is also found for x=1.0 but another orthorhombic phase, Imma, obtains for x=1.33 and 1.5. Reductive weight losses indicate negligible oxygen non-stoichiometry, i.e., δ∼0, for all compositions even those rich in Co. High-resolution electron energy loss spectroscopy (EELS) indicates that cobalt is high-spin Co3+ or high-spin Co4+ for all x. Appropriate combinations of Ru4+, Ru5+, HS Co3+ and HS Co4+ are proposed for each x which are consistent with the observed Ru(Co)-O distances. Significant amounts of Co4+ must be present for large x values to explain the short observed distances. Broad maxima in the d.c. susceptibilities are found between 78 and 97 K with increasing x, along with zero-field-cooled (ZFC) and field-cooled (FC) divergences suggesting glassy magnetic freezing. A feature near 155 K for all samples indicates a residual amount of ferromagnetic SrRuO3 not detected by X-ray diffraction. |
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Keywords: | Ru-Co perovskites Solid solution Miscibility gap X-ray powder diffraction Glassy magnetism Cobalt L-edge Electron energy loss spectroscopy |
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