LiHo2Ta2O8 crystallizes in the monoclinic C2 space group. Li(1) is bonded in a 4-coordinate geometry to two equivalent O(1), two equivalent O(3), and two equivalent O(4) atoms. There are two inequivalent Ho sites. In the first Ho site, Ho(1) is bonded in a 8-coordinate geometry to two equivalent O(1), two equivalent O(2), two equivalent O(3), and two equivalent O(4) atoms. In the second Ho site, Ho(2) is bonded in a 8-coordinate geometry to two equivalent O(1), two equivalent O(2), two equivalent O(3), and two equivalent O(4) atoms. There are two inequivalent Ta sites. In the first Ta site, Ta(1) is bonded in a 6-coordinate geometry to two equivalent O(1), two equivalent O(2), and two equivalent O(3) atoms. In the second Ta site, Ta(2) is bonded in a distorted octahedral geometry to two equivalent O(1), two equivalent O(2), and two equivalent O(4) atoms. There are four inequivalent O sites. In the first O site, O(1) is bonded to one Li(1), one Ho(1), one Ho(2), one Ta(1), and one Ta(2) atom to form distorted OLiHo2Ta2 trigonal bipyramids that share corners with three equivalent O(1)LiHo2Ta2 trigonal bipyramids, edges with four equivalent O(2)Ho2Ta2 tetrahedra, and  an edgeedge with one O(1)LiHo2Ta2 trigonal bipyramid. In the second O site, O(2) is bonded to one Ho(1), one Ho(2), one Ta(1), and one Ta(2) atom to form distorted OHo2Ta2 tetrahedra that share corners with four equivalent O(2)Ho2Ta2 tetrahedra and edges with four equivalent O(1)LiHo2Ta2 trigonal bipyramids. In the third O site, O(3) is bonded in a 4-coordinate geometry to one Li(1), one Ho(1), one Ho(2), and one Ta(1) atom. In the fourth O site, O(4) is bonded in a 4-coordinate geometry to one Li(1), one Ho(1), one Ho(2), and one Ta(2) atom.
LiHo2Ta2O8 crystallizes in the monoclinic C2 space group. Li(1) is bonded in a 4-coordinate geometry to two equivalent O(1), two equivalent O(3), and two equivalent O(4) atoms. Both Li(1)-O(1) bond lengths are 2.18 Å. Both Li(1)-O(3) bond lengths are 2.57 Å. Both Li(1)-O(4) bond lengths are 1.91 Å. There are two inequivalent Ho sites. In the first Ho site, Ho(1) is bonded in a 8-coordinate geometry to two equivalent O(1), two equivalent O(2), two equivalent O(3), and two equivalent O(4) atoms. Both Ho(1)-O(1) bond lengths are 2.37 Å. Both Ho(1)-O(2) bond lengths are 2.42 Å. Both Ho(1)-O(3) bond lengths are 2.29 Å. Both Ho(1)-O(4) bond lengths are 2.41 Å. In the second Ho site, Ho(2) is bonded in a 8-coordinate geometry to two equivalent O(1), two equivalent O(2), two equivalent O(3), and two equivalent O(4) atoms. Both Ho(2)-O(1) bond lengths are 2.47 Å. Both Ho(2)-O(2) bond lengths are 2.47 Å. Both Ho(2)-O(3) bond lengths are 2.31 Å. Both Ho(2)-O(4) bond lengths are 2.31 Å. There are two inequivalent Ta sites. In the first Ta site, Ta(1) is bonded in a 6-coordinate geometry to two equivalent O(1), two equivalent O(2), and two equivalent O(3) atoms. Both Ta(1)-O(1) bond lengths are 2.07 Å. Both Ta(1)-O(2) bond lengths are 2.20 Å. Both Ta(1)-O(3) bond lengths are 1.93 Å. In the second Ta site, Ta(2) is bonded in a distorted octahedral geometry to two equivalent O(1), two equivalent O(2), and two equivalent O(4) atoms. Both Ta(2)-O(1) bond lengths are 2.23 Å. Both Ta(2)-O(2) bond lengths are 2.01 Å. Both Ta(2)-O(4) bond lengths are 1.94 Å. There are four inequivalent O sites. In the first O site, O(1) is bonded to one Li(1), one Ho(1), one Ho(2), one Ta(1), and one Ta(2) atom to form distorted OLiHo2Ta2 trigonal bipyramids that share corners with three equivalent O(1)LiHo2Ta2 trigonal bipyramids, edges with four equivalent O(2)Ho2Ta2 tetrahedra, and  an edgeedge with one O(1)LiHo2Ta2 trigonal bipyramid. In the second O site, O(2) is bonded to one Ho(1), one Ho(2), one Ta(1), and one Ta(2) atom to form distorted OHo2Ta2 tetrahedra that share corners with four equivalent O(2)Ho2Ta2 tetrahedra and edges with four equivalent O(1)LiHo2Ta2 trigonal bipyramids. In the third O site, O(3) is bonded in a 4-coordinate geometry to one Li(1), one Ho(1), one Ho(2), and one Ta(1) atom. In the fourth O site, O(4) is bonded in a 4-coordinate geometry to one Li(1), one Ho(1), one Ho(2), and one Ta(2) atom.