We wanted to identify new {Dy(Cp R )2} + synthetic targets with small substituents, in order to allow close approach of the Cp R ligands to increase the axial crystal field and improve SMM performance. The workflow was as follows: (1) {Dy(Cp R )2} + fragments were built from a standardized {Dy(C5)2} + framework (Table ); (2) diverse conformational isomers of {Dy(Cp R )2} + were generated with a genetic algorithm in OpenBabel; and, (3) the size of the largest cluster for each conformer was determined with AtomAccess (see ESI for further details). The method was benchmarked with common {Dy(Cp R )2} + fragments A-C (Figure ) that consistently exhibit equatorial interactions, and known isolated dysprosocenium cations (E, F). Using AtomAccess we see that fragments A-C reasonably reproduce the largest cluster distributions from XRD (Table ) and correctly predict two or more equatorial interactions (largest clusters ≥24.1% SA). The distributions from E and F confirm that a single equatorial coordination site can be accommodated (i.e. conformations exist with > 14.5% SA), but also that E and F can rearrange to shield the Dy(III) ion from equatorial coordination (i.e.