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TbSi2 is hexagonal omega structure structured and crystallizes in the hexagonal P6/mmm space group. The structure is three-dimensional. Tb is bonded to twelve equivalent Si atoms to form a mixture of edge and face-sharing TbSi12 cuboctahedra. All Tb–Si bond lengths are 3.09 Å. Si is bonded in a 9-coordinate geometry to six equivalent Tb and three equivalent Si atoms. All Si–Si bond lengths are 2.37 Å.
TbSi crystallizes in the orthorhombic Pnma space group. The structure is three-dimensional. Tb4+ is bonded in a 7-coordinate geometry to seven equivalent Si4- atoms. There are a spread of Tb–Si bond distances ranging from 2.96–3.17 Å. Si4- is bonded in a 9-coordinate geometry to seven equivalent Tb4+ and two equivalent Si4- atoms. Both Si–Si bond lengths are 2.50 Å.
Tb2Si3 crystallizes in the orthorhombic Cmcm space group. The structure is three-dimensional. there are two inequivalent Tb sites. In the first Tb site, Tb is bonded in a 4-coordinate geometry to four equivalent Si atoms. There are two shorter (2.88 Å) and two longer (3.04 Å) Tb–Si bond lengths. In the second Tb site, Tb is bonded in a 11-coordinate geometry to eleven Si atoms. There are a spread of Tb–Si bond distances ranging from 3.17–3.26 Å. There are three inequivalent Si sites. In the first Si site, Si is bonded in a 7-coordinate geometry to three equivalent Tb and four Si atoms. There are two shorter (2.37 Å) and two longer (2.40 Å) Si–Si bond lengths. In the second Si site, Si is bonded in a 9-coordinate geometry to eight Tb and one Si atom. The Si–Si bond length is 2.30 Å. In the third Si site, Si is bonded in a 7-coordinate geometry to four equivalent Tb and three Si atoms.
Tb3Si crystallizes in the hexagonal P6_3/mmc space group. The structure is three-dimensional. Tb is bonded in a 4-coordinate geometry to four equivalent Si atoms. There are two shorter (3.15 Å) and two longer (3.36 Å) Tb–Si bond lengths. Si is bonded to twelve equivalent Tb atoms to form a mixture of face and corner-sharing SiTb12 cuboctahedra.