Nd2H5 crystallizes in the tetragonal I4_1md space group. There are two inequivalent Nd sites. In the first Nd site, Nd(1) is bonded in a distorted body-centered cubic geometry to three equivalent H(2) and eight equivalent H(1) atoms. In the second Nd site, Nd(2) is bonded in a distorted body-centered cubic geometry to three equivalent H(2) and eight equivalent H(1) atoms. There are two inequivalent H sites. In the first H site, H(1) is bonded to two equivalent Nd(1) and two equivalent Nd(2) atoms to form HNd4 tetrahedra that share corners with six equivalent H(2)Nd6 octahedra, corners with sixteen equivalent H(1)Nd4 tetrahedra, edges with six equivalent H(1)Nd4 tetrahedra, and faces with two equivalent H(2)Nd6 octahedra. The corner-sharing octahedral tilt angles range from 53-58°. In the second H site, H(2) is bonded to three equivalent Nd(1) and three equivalent Nd(2) atoms to form HNd6 octahedra that share corners with four equivalent H(2)Nd6 octahedra, corners with twenty-four equivalent H(1)Nd4 tetrahedra, edges with four equivalent H(2)Nd6 octahedra, and faces with eight equivalent H(1)Nd4 tetrahedra. The corner-sharing octahedral tilt angles range from 1-2°.
Nd2H5 crystallizes in the tetragonal I4_1md space group. There are two inequivalent Nd sites. In the first Nd site, Nd(1) is bonded in a distorted body-centered cubic geometry to three equivalent H(2) and eight equivalent H(1) atoms. All Nd(1)-H(2) bond lengths are 2.71 Å. There are four shorter (2.32 Å) and four longer (2.40 Å) Nd(1)-H(1) bond lengths. In the second Nd site, Nd(2) is bonded in a distorted body-centered cubic geometry to three equivalent H(2) and eight equivalent H(1) atoms. There is one shorter (2.70 Å) and two longer (2.72 Å) Nd(2)-H(2) bond lengths. There are four shorter (2.33 Å) and four longer (2.40 Å) Nd(2)-H(1) bond lengths. There are two inequivalent H sites. In the first H site, H(1) is bonded to two equivalent Nd(1) and two equivalent Nd(2) atoms to form HNd4 tetrahedra that share corners with six equivalent H(2)Nd6 octahedra, corners with sixteen equivalent H(1)Nd4 tetrahedra, edges with six equivalent H(1)Nd4 tetrahedra, and faces with two equivalent H(2)Nd6 octahedra. The corner-sharing octahedral tilt angles range from 53-58°. In the second H site, H(2) is bonded to three equivalent Nd(1) and three equivalent Nd(2) atoms to form HNd6 octahedra that share corners with four equivalent H(2)Nd6 octahedra, corners with twenty-four equivalent H(1)Nd4 tetrahedra, edges with four equivalent H(2)Nd6 octahedra, and faces with eight equivalent H(1)Nd4 tetrahedra. The corner-sharing octahedral tilt angles range from 1-2°.