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Ca2TlSn crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two Ca2TlSn ribbons oriented in the (1, 0, 0) direction. Ca is bonded in a linear geometry to one Tl and one Sn atom. The Ca–Tl bond length is 3.18 Å. The Ca–Sn bond length is 3.02 Å. Tl is bonded in a linear geometry to two equivalent Ca atoms. Sn is bonded in a linear geometry to two equivalent Ca atoms.
Ca2TlSn is Heusler structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Ca is bonded in a body-centered cubic geometry to four equivalent Tl and four equivalent Sn atoms. All Ca–Tl bond lengths are 3.36 Å. All Ca–Sn bond lengths are 3.36 Å. Tl is bonded in a body-centered cubic geometry to eight equivalent Ca atoms. Sn is bonded in a body-centered cubic geometry to eight equivalent Ca atoms.