As a further test, the entire workflow was applied to the pyrene dimer, to test whether it could quickly and accurately reduce a large field of potential conformers to a small, accurately ordered list of optimized structures. Optimization using loose thresholds (ORCA keyword LooseOPT ) produced an ensemble containing several of the previously published structures, but also many spurious minima. At this point, any duplicate structures were removed, and further optimization was done using B97-3c in conjuction with very tight thresholds (the VeryTightOPT, VeryTightSCF, and DefGrid3 ORCA keywords). Again, duplicates were removed, and final optimization was performed using ωB97X-D4/def2-SVP. Final single points were computed using ωB97X-V/def2-TZVP. While we use ωB97X-V/def2-QZVPP for final single points in the rest of this work, def2-TZVP was used here to allow for comparison with the previously published results. The results are shown in Section 3.2.