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Tl3VS4 crystallizes in the cubic I-43m space group. The structure is three-dimensional and consists of two Tl3VS4 frameworks. V5+ is bonded in a tetrahedral geometry to four equivalent S2- atoms. All V–S bond lengths are 2.17 Å. Tl1+ is bonded in a 12-coordinate geometry to four equivalent S2- atoms. All Tl–S bond lengths are 3.13 Å. S2- is bonded in a distorted single-bond geometry to one V5+ and three equivalent Tl1+ atoms.
Tl3TaS4Tl3VS4 crystallizes in the cubic P-43m space group. The structure is three-dimensional and consists of one Tl3TaS4 framework and one Tl3VS4 framework. In the Tl3TaS4 framework, Ta5+ is bonded in a tetrahedral geometry to four equivalent S2- atoms. All Ta–S bond lengths are 2.29 Å. Tl1+ is bonded in a 12-coordinate geometry to four equivalent S2- atoms. All Tl–S bond lengths are 3.17 Å. S2- is bonded in a distorted single-bond geometry to one Ta5+ and three equivalent Tl1+ atoms. In the Tl3VS4 framework, V5+ is bonded in a tetrahedral geometry to four equivalent S2- atoms. All V–S bond lengths are 2.17 Å. Tl1+ is bonded in a 12-coordinate geometry to four equivalent S2- atoms. All Tl–S bond lengths are 3.17 Å. S2- is bonded in a distorted single-bond geometry to one V5+ and three equivalent Tl1+ atoms.