For all 10 EMs, the CSP set of crystal structures generated with the PBE0/aug-cc-pVTZ multipole model was further optimized using plane-wave-based periodic DFT as implemented in the VASP package. For each EM, all structures on the respective CSP landscape within 10 kJ mol -1 of the global energy minimum were re-optimized. For ATZ, the energy window was increased to within 12 kJ mol -1 of the global energy minimum due to finding the experimental match just below 12 kJ mol -1 . This re-optimization was performed in a three-step procedure that has been found to improve the convergence rate of periodic DFT optimizations for crystal structures. The first step involves optimizing only the atomic positions with the unit cell fixed, the second step optimizes both atomic positions and unit-cell parameters, and the third step is a final single-point calculation which updates the plane wave basis set to the newly relaxed lattice parameters to provide an accurate final energy.