With the 3c method of choice determined, we next revisited the refinement of the CRESTgenerated ensemble. All 73 members of the conformational ensemble generated by CREST from the previous paper were reoptimized using B97-3c. In doing so, we were able to reduce the 73 conformer pyrene homodimer CREST ensemble down to 10 unique structures, with the rest discarded either as duplicates, or for having too high an energy (>12 kJ/mol). The geometries of the remaining structures were optimized using ωB97X-D4/def2-SVP, after which an additional two structures became duplicates. The final eight conformers included the six solution-phase dimers identified in our previous paper, or close approximations thereto, namely the 0SP-L, 0G , 60G1, 60G2, 67qG, and 90X conformers. For some conformers, the long axes were misaligned by as much as 12 • , relative to the previously published conformers, but the conformers were still recognizable. It is likely that at least part of the small difference in geometries is due to the smaller basis set used during optimization.