OsSe2 is Pyrite structured and crystallizes in the cubic Pa-3 space group. The structure is three-dimensional. Os4+ is bonded to six equivalent Se2- atoms to form corner-sharing OsSe6 octahedra. The corner-sharing octahedral tilt angles are 63°. All Os–Se bond lengths are 2.50 Å. Se2- is bonded in a 4-coordinate geometry to three equivalent Os4+ and one Se2- atom. The Se–Se bond length is 2.55 Å.
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