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Li5OsO6 and Li5ReO6 polycrystalline samples were synthesized by conventionalsolid state methods. Employing powder neutron diffraction data, the crystalstructure of Li5OsO6 was re-investigated. Li5OsO6 crystallizes in C2/m spacegroup in an ordered NaCl structure type where a = 5.0472(1) A, b = 8.7827(2) A,c = 5.0079(1) A, Beta = 109.777(2) degree and V = 208.90(1).A^3 Magneticsusceptibility and heat capacity data indicate an AFM long range order below40K although there is evidence for low dimensional short range order above 80K.As well, the frustration index, f = |theta|/TN ~1, in contrast to theisostructural and isoelectronic compound, Li4MgReO6, which is a spin glassbelow 12K and has f ~ 14. An attempt was made to rationalize these differencesusing spin dimer analysis. The key results are that the spin exchangeinteractions in the Re-based compound are stronger and are consistent with afrustrated triangular lattice model while a low dimensional short range ordermodel is better for Li5OsO6. The main reason for this is a strong Jahn-Tellerdistortion in the OsO6 octahedron material which constrains the unpairedelectron to occupy the dxy orbital.

Long Range Antiferromagnetic Ordering in the S = 1/2 Ordered Rock Salt  Oxide, Li5OsO6: Comparison with the Isoelectronicand Isostructural Spin  Glass, Li4MgReO6