TlCr3S5 crystallizes in the monoclinic space group C2/m with the lattice parameters a = 19.293(4), b = 3.4653(9), c = 11.962(2) Å, β = 122.18(3)°, V = 676.8(3) Å3, Z = 4. The structure was refined to R = 0.067 and Rw = 0.048. CrS6 octahedra are joined by common edges and faces leading to a three dimensional network with channels parallel to the crystallographic b-axis. The Tl atoms are confined within these channels.
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