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TbBr crystallizes in the trigonal R-3m space group. The structure is two-dimensional and consists of six TbBr sheets oriented in the (0, 0, 1) direction. Tb is bonded in a 3-coordinate geometry to three equivalent Br atoms. All Tb–Br bond lengths are 2.93 Å. Br is bonded in a 3-coordinate geometry to three equivalent Tb atoms.
Tb6Br7 crystallizes in the monoclinic C2/m space group. The structure is three-dimensional. there are three inequivalent Tb sites. In the first Tb site, Tb is bonded in a distorted rectangular see-saw-like geometry to four Br atoms. There are a spread of Tb–Br bond distances ranging from 2.82–3.08 Å. In the second Tb site, Tb is bonded in a 3-coordinate geometry to three Br atoms. There are one shorter (3.00 Å) and two longer (3.02 Å) Tb–Br bond lengths. In the third Tb site, Tb is bonded to five Br atoms to form distorted edge-sharing TbBr5 square pyramids. There are a spread of Tb–Br bond distances ranging from 2.88–3.17 Å. There are four inequivalent Br sites. In the first Br site, Br is bonded in a square co-planar geometry to four equivalent Tb atoms. In the second Br site, Br is bonded in a 3-coordinate geometry to three Tb atoms. In the third Br site, Br is bonded in a distorted see-saw-like geometry to four Tb atoms. In the fourth Br site, Br is bonded in a 3-coordinate geometry to three Tb atoms.
Tb5Br8 crystallizes in the monoclinic C2/m space group. The structure is three-dimensional. there are three inequivalent Tb sites. In the first Tb site, Tb is bonded in a 5-coordinate geometry to five Br atoms. There are four shorter (2.92 Å) and one longer (3.46 Å) Tb–Br bond lengths. In the second Tb site, Tb is bonded in a rectangular see-saw-like geometry to four Br atoms. There are two shorter (2.88 Å) and two longer (3.05 Å) Tb–Br bond lengths. In the third Tb site, Tb is bonded to six Br atoms to form edge-sharing TbBr6 octahedra. There are four shorter (2.85 Å) and two longer (2.86 Å) Tb–Br bond lengths. There are four inequivalent Br sites. In the first Br site, Br is bonded in a 3-coordinate geometry to three Tb atoms. In the second Br site, Br is bonded in a distorted T-shaped geometry to three Tb atoms. In the third Br site, Br is bonded in a 2-coordinate geometry to three Tb atoms. In the fourth Br site, Br is bonded in a distorted T-shaped geometry to three Tb atoms.