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X-ray single crystal diffraction studies on the Gd 5 Si 4x Sn x  series with 0 ≤  x  ≤ 3 revealed an increase in the interslab  T — T  ( T  = Si, Sn) dimer distances and transition from Gd 5 Si 4 -type structures for 0 ≤  x  ≤ 1.5 ( d  T—T  = 2.49–2.71 Å) to the Pu 5 Rh 4 -type structure for  x  = 2 ( d  T—T  = 3.04 Å). The Ti 5 Ga 4 -type structure, which is a stuffed version of the hexagonal Mn 5 Si 3  structure, was observed for the Gd 5 SiSn 3  sample ( x  = 3). Tight-binding linear-muffin-tin-orbital (TB-LMTO) calculations on Gd 5 Si 2 Sn 2  show that the interslab ( T 1— T 1) dimer stretching and the structural transition from the Gd 5 Si 4 -type to the Pu 5 Rh 4 -type results from the influence of the 5 p  atomic orbital energy and the larger size of the Sn atoms on the electronic structure, as compared to the Si and Ge atoms in Gd 5 Si 4  and Gd 5 Si 2 Ge 2 .

Structural variations in Gd 5 Si 4-x Sn x : size vs. electronic effects