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CaGa2 crystallizes in the hexagonal P6_3/mmc space group. The structure is three-dimensional. Ca is bonded in a 12-coordinate geometry to twelve equivalent Ga atoms. There are six shorter (3.02 Å) and six longer (3.38 Å) Ca–Ga bond lengths. Ga is bonded in a 10-coordinate geometry to six equivalent Ca and four equivalent Ga atoms. There are three shorter (2.68 Å) and one longer (3.07 Å) Ga–Ga bond lengths.
CaGa2 is hexagonal omega structure structured and crystallizes in the hexagonal P6/mmm space group. The structure is three-dimensional. Ca is bonded to twelve equivalent Ga atoms to form a mixture of face and edge-sharing CaGa12 cuboctahedra. All Ca–Ga bond lengths are 3.31 Å. Ga is bonded in a 9-coordinate geometry to six equivalent Ca and three equivalent Ga atoms. All Ga–Ga bond lengths are 2.48 Å.