Nevertheless, simple fits to Gaussian peaks perform noticeably better, with most fits yielding r 2 above 0.9. In part, this method enables better fits of subpopulations as discussed above. Further refinement of torsion patterns may resolve such subpopulations, improving the accuracy of ETKDG-style fits. For sampling torsion angles from the Gaussian fits, we have generated the cumulative sum across all angles 0-360 Comparing individual torsion preferences between the experimental COD geometries and the lowest-energy CREST/GFN2 conformers indicated good correlation (i.e., median r 2 above 0.6 for acyclic torsions and above 0.8 for ring torsions), with most cases of poor correlation deriving from few examples in the COD set.