CsHoSiS4 crystallizes in the orthorhombic P2_12_12_1 space group. Cs(1) is bonded in a 8-coordinate geometry to one S(2), two equivalent S(3), two equivalent S(4), and three equivalent S(1) atoms. Ho(1) is bonded in a 7-coordinate geometry to one S(1), two equivalent S(2), two equivalent S(3), and two equivalent S(4) atoms. Si(1) is bonded in a tetrahedral geometry to one S(1), one S(2), one S(3), and one S(4) atom. There are four inequivalent S sites. In the first S site, S(1) is bonded in a 5-coordinate geometry to three equivalent Cs(1), one Ho(1), and one Si(1) atom. In the second S site, S(2) is bonded in a distorted see-saw-like geometry to one Cs(1), two equivalent Ho(1), and one Si(1) atom. In the third S site, S(3) is bonded in a 5-coordinate geometry to two equivalent Cs(1), two equivalent Ho(1), and one Si(1) atom. In the fourth S site, S(4) is bonded in a 3-coordinate geometry to two equivalent Cs(1), two equivalent Ho(1), and one Si(1) atom.
CsHoSiS4 crystallizes in the orthorhombic P2_12_12_1 space group. Cs(1) is bonded in a 8-coordinate geometry to one S(2), two equivalent S(3), two equivalent S(4), and three equivalent S(1) atoms. The Cs(1)-S(2) bond length is 3.45 Å. There is one shorter (3.65 Å) and one longer (3.87 Å) Cs(1)-S(3) bond length. Both Cs(1)-S(4) bond lengths are 3.76 Å. There are a spread of Cs(1)-S(1) bond distances ranging from 3.54-3.65 Å. Ho(1) is bonded in a 7-coordinate geometry to one S(1), two equivalent S(2), two equivalent S(3), and two equivalent S(4) atoms. The Ho(1)-S(1) bond length is 2.80 Å. There is one shorter (2.78 Å) and one longer (2.98 Å) Ho(1)-S(2) bond length. There is one shorter (2.85 Å) and one longer (2.91 Å) Ho(1)-S(3) bond length. There is one shorter (2.81 Å) and one longer (2.84 Å) Ho(1)-S(4) bond length. Si(1) is bonded in a tetrahedral geometry to one S(1), one S(2), one S(3), and one S(4) atom. The Si(1)-S(1) bond length is 2.12 Å. The Si(1)-S(2) bond length is 2.13 Å. The Si(1)-S(3) bond length is 2.14 Å. The Si(1)-S(4) bond length is 2.15 Å. There are four inequivalent S sites. In the first S site, S(1) is bonded in a 5-coordinate geometry to three equivalent Cs(1), one Ho(1), and one Si(1) atom. In the second S site, S(2) is bonded in a distorted see-saw-like geometry to one Cs(1), two equivalent Ho(1), and one Si(1) atom. In the third S site, S(3) is bonded in a 5-coordinate geometry to two equivalent Cs(1), two equivalent Ho(1), and one Si(1) atom. In the fourth S site, S(4) is bonded in a 3-coordinate geometry to two equivalent Cs(1), two equivalent Ho(1), and one Si(1) atom.