To determine the degree of correlation between the COD experimental torsion preferences and the computed gas-phase preferences, the r 2 of the kernel density estimation (KDE) for both acyclic and ring torsion patterns was compiled in Figure . The KDE is used to smooth the histogram (i.e., representing uncertainty in the individual torsions) and to avoid issues when correlating areas with few or no torsions in the COD with the regions where some torsions were present in the combined set. The r 2 then correlates the KDE of the experimental COD torsion preferences and the KDE of the computed CREST/GFN2 gasphase preferences for each torsion pattern. A total of 127 patterns yield r 2 > 0.8, and the median acyclic r 2 is 0.61, indicating that while there are some differences, the torsional preferences yield reasonable correlation.