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Hf2TcNi crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two Hf2TcNi ribbons oriented in the (1, 0, 0) direction. Hf is bonded in a linear geometry to one Tc and one Ni atom. The Hf–Tc bond length is 2.26 Å. The Hf–Ni bond length is 2.41 Å. Tc is bonded in a linear geometry to two equivalent Hf atoms. Ni is bonded in a linear geometry to two equivalent Hf atoms.
Hf2TcNi is Heusler structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Hf is bonded in a body-centered cubic geometry to four equivalent Tc and four equivalent Ni atoms. All Hf–Tc bond lengths are 2.80 Å. All Hf–Ni bond lengths are 2.80 Å. Tc is bonded in a body-centered cubic geometry to eight equivalent Hf atoms. Ni is bonded in a body-centered cubic geometry to eight equivalent Hf atoms.