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PmCl2 is zeta iron carbide structured and crystallizes in the tetragonal P4_2/mnm space group. The structure is three-dimensional. Pm is bonded to six equivalent Cl atoms to form a mixture of edge and corner-sharing PmCl6 octahedra. The corner-sharing octahedral tilt angles are 39°. There are two shorter (2.82 Å) and four longer (2.84 Å) Pm–Cl bond lengths. Cl is bonded in a 3-coordinate geometry to three equivalent Pm atoms.
PmCl3 crystallizes in the hexagonal P6_3/mmc space group. The structure is one-dimensional and consists of two PmCl3 ribbons oriented in the (0, 0, 1) direction. Pm3+ is bonded to six equivalent Cl1- atoms to form distorted face-sharing PmCl6 pentagonal pyramids. All Pm–Cl bond lengths are 2.75 Å. Cl1- is bonded in an L-shaped geometry to two equivalent Pm3+ atoms.