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SCs is alpha boron-derived structured and crystallizes in the orthorhombic Immm space group. The structure is three-dimensional. Cs1+ is bonded in a 6-coordinate geometry to six equivalent S1- atoms. There are four shorter (3.52 Å) and two longer (3.61 Å) Cs–S bond lengths. S1- is bonded in a 7-coordinate geometry to six equivalent Cs1+ and one S1- atom. The S–S bond length is 2.12 Å.
Cs2S is Cotunnite structured and crystallizes in the orthorhombic Pnma space group. The structure is three-dimensional. there are two inequivalent Cs1+ sites. In the first Cs1+ site, Cs1+ is bonded in a 3-coordinate geometry to three equivalent S2- atoms. There are one shorter (3.51 Å) and two longer (3.68 Å) Cs–S bond lengths. In the second Cs1+ site, Cs1+ is bonded to four equivalent S2- atoms to form a mixture of edge and corner-sharing CsS4 tetrahedra. There are a spread of Cs–S bond distances ranging from 3.47–3.56 Å. S2- is bonded in a 9-coordinate geometry to seven Cs1+ atoms.
SSSCs crystallizes in the triclinic P-1 space group. The structure is three-dimensional. there are two inequivalent Cs1+ sites. In the first Cs1+ site, Cs1+ is bonded in a 10-coordinate geometry to ten S+0.33- atoms. There are a spread of Cs–S bond distances ranging from 3.57–4.12 Å. In the second Cs1+ site, Cs1+ is bonded in a 11-coordinate geometry to eleven S+0.33- atoms. There are a spread of Cs–S bond distances ranging from 3.60–4.25 Å. There are six inequivalent S+0.33- sites. In the first S+0.33- site, S+0.33- is bonded in a 8-coordinate geometry to six Cs1+ and two S+0.33- atoms. There are one shorter (2.06 Å) and one longer (3.47 Å) S–S bond lengths. In the second S+0.33- site, S+0.33- is bonded in a 6-coordinate geometry to five Cs1+ and two S+0.33- atoms. The S–S bond length is 2.04 Å. In the third S+0.33- site, S+0.33- is bonded in a 4-coordinate geometry to two equivalent Cs1+ and two S+0.33- atoms. The S–S bond length is 2.06 Å. In the fourth S+0.33- site, S+0.33- is bonded in a 4-coordinate geometry to two Cs1+ and two S+0.33- atoms. The S–S bond length is 2.11 Å. In the fifth S+0.33- site, S+0.33- is bonded in a 2-coordinate geometry to three equivalent Cs1+ and two S+0.33- atoms. The S–S bond length is 2.09 Å. In the sixth S+0.33- site, S+0.33- is bonded in a 5-coordinate geometry to three Cs1+ and two S+0.33- atoms.
Cs2S3 crystallizes in the orthorhombic Cmc2_1 space group. The structure is three-dimensional. there are two inequivalent Cs1+ sites. In the first Cs1+ site, Cs1+ is bonded in a 7-coordinate geometry to seven S+0.67- atoms. There are a spread of Cs–S bond distances ranging from 3.44–3.74 Å. In the second Cs1+ site, Cs1+ is bonded in a 7-coordinate geometry to seven S+0.67- atoms. There are a spread of Cs–S bond distances ranging from 3.53–3.75 Å. There are two inequivalent S+0.67- sites. In the first S+0.67- site, S+0.67- is bonded in a 7-coordinate geometry to six Cs1+ and one S+0.67- atom. The S–S bond length is 2.09 Å. In the second S+0.67- site, S+0.67- is bonded in a 4-coordinate geometry to two Cs1+ and two equivalent S+0.67- atoms.