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On the high magnetic-ordering temperature of the 5d magnetic oxide Ca3LiOsO6 crystallizing in a trigonal crystal structure: density functional analysis.

The 5d magnetic oxide Ca(3)LiOsO(6) has a trigonal arrangement of its LiOsO(6) chains parallel to the c-direction and hence has triangular arrangements of high-spin Os(5+) (d(3)) ions but exhibits no spin frustration and undergoes a long-range antiferromagnetic ordering at a high temperature. The origin of this apparently puzzling observation was examined by evaluating the nearest-neighbor Os-O···O-Os spin exchange interactions of Ca(3)LiOsO(6) on the basis of density functional calculations. Our study shows that, of the two nearest-neighbor interchain spin exchanges, one dominates over the other and that the intrachain spin exchange and the dominating interchain spin exchange are strong and form a three-dimensional antiferromagnetic spin lattice with no spin frustration, which is responsible for the long-range antiferromagnetic ordering of Ca(3)LiOsO(6) at high temperature. In determining the strengths of the Os-O···O-Os exchange interactions of Ca(3)LiOsO(6), the Li(+) and Ca(2+) ions of the O···Li(+)···O and O···Ca(2+)···O linkages are found to play only a minor role.