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TlAs is Zincblende, Sphalerite structured and crystallizes in the cubic F-43m space group. The structure is three-dimensional. Tl1+ is bonded to four equivalent As1- atoms to form corner-sharing TlAs4 tetrahedra. All Tl–As bond lengths are 2.75 Å. As1- is bonded to four equivalent Tl1+ atoms to form corner-sharing AsTl4 tetrahedra.
Tl3As crystallizes in the hexagonal P6_3/mmc space group. The structure is one-dimensional and consists of two Tl3As ribbons oriented in the (0, 0, 1) direction. Tl1+ is bonded in a 12-coordinate geometry to two equivalent As3- atoms. Both Tl–As bond lengths are 3.37 Å. As3- is bonded in a 12-coordinate geometry to six equivalent Tl1+ atoms.