For each molecule, we began by extracting its in-crystal conformation from the corresponding CSD entry (where there is more than one entry, we select only the first listed in the database). This molecular conformation was optimised in DFT (as implemented in Gaussian(47)), using the PBE0 exchange-correlation functional, a Pople-type 6-311G** basis , and Grimme's D3 dispersion correction with Becke-Johnson damping . Distributed multipole analysis (DMA, using the GDMA package) was performed on the resulting molecular conformers' charge densities to obtain atom-centred multipoles, as part of the model potential applied during lattice energy minimisation of trial crystal structures; multipoles up to hexadecapole were calculated for all atoms. The MUL-FIT software was used to fit atomic point charges for each molecule to best describe the molecular electrostatic potential. The resulting molecular conformers and their sets of multipoles are then used as the inputs to CSP, with each unique molecule represented by a single conformer and corresponding set of atomic multipoles and charges.