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CaC4 is Silicon tetrafluoride-like structured and crystallizes in the cubic Pn-3m space group. The structure is zero-dimensional and consists of two CaC4 clusters. Ca2+ is bonded in a tetrahedral geometry to four equivalent C+0.50- atoms. All Ca–C bond lengths are 2.47 Å. C+0.50- is bonded in a single-bond geometry to one Ca2+ atom.
CaC4 crystallizes in the tetragonal P4/mmm space group. The structure is three-dimensional. Ca2+ is bonded in a 1-coordinate geometry to sixteen equivalent C+0.50- atoms. All Ca–C bond lengths are 2.75 Å. C+0.50- is bonded in a 7-coordinate geometry to four equivalent Ca2+ and three equivalent C+0.50- atoms. There is one shorter (1.44 Å) and two longer (1.49 Å) C–C bond length.