The RMSD for H-NMR predictions are smaller with B3LYP/cc-pVTZ, indicating better alignment with experimental data. This improvement is particularly notable for hydrogens attached to carbons engaged in complex bonding environments. For example, hydrogens on the junction carbons (C1-C4), where the multiple C-C bonds create unique electronic environments, are better predicted by B3LYP. Similarly, the hydrogens on the flag carbon, C5 and boat tip carbon C10, which exhibit different interactions in the chair and boat isomers, are more accurately modelled by B3LYP, as indicated by the dashed line boxes in Figure (b). Hydrogens on C5 and C10 play an important role in differentiating the chair and the boat isomers due to their distinct spatial arrangements in the chair and boat conformations. The slightly better performance of B3LYP in predicting these ¹H-NMR shifts reinforces its utility for studying the hydrogen environments in complex isomers like exo-TCD.