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The title compounds were synthesized from RE, REI 3  (RE = Ce, Gd, Y) and Al or Ga under an Ar atmosphere at 930 - 950 °C. The non-stoichiometric Ce 2+x I 2 Al 2+y  and Ce 2 + x I 2 Ga 2+y  compounds crystallize in the space group R3̄m (No. 166) with lattice constants a = 4.3645(3), c = 35.914(2) Å for the Al and a = 4.3009(2), c = 35.680(4) Å for the Ga compound. Excess electron density found in the Wyckoff position 3a could be due to a fractional occupation by Ce or M (x = 0.06, y = 0 or x = 0, y = 0.11 in the case of the Ga compound). The stoichiometric Gd 2 I 2 Ga 2  and Y 2 I 2 Ga 2  compounds crystallize in the space group P3̄m1 (No. 164) with lattice constants a = 4.1964(1) and 4.1786(7) Å , c = 11.4753(4) and 11.434(2) Å , respectively. Their structures feature M-centered (M = Al, Ga) RE trigonal prisms condensed via common rectangular faces. The electronic origin of the surplus of metal atoms in the octahedral voids between the I-layers of the Ce compounds was explored via extended Hückel-type calculations. Magnetic susceptibility, electrical resistivity and heat capacity measurements have also been carried out. These reveal a metal-insulator transition of Gd 2 I 2 Ga 2  at 40 K.

RE 2+x I 2 M 2+y (RE = Ce,Gd, Y; M = Al, Ga): Reduced Rare Earth Halides with a Hexagonal Metal Atom Network