Besides the modB3LYP (aHF = 0.10) functional identified in Sec. 3. and). Nevertheless, uncertainties due to the lack of explicit treatment of solvent or crystal environments motivate our broader definition. Using the more stringent requirement to predict canonical SCO behavior, we observe that M06-L (i.e., 78 out of 95 SCOs) performs the best in comparison to TPSSh or modB3LYP (aHF = 0.10) because most of the complexes are predicted to be LS at 0 K with an HS state that is stabilized at room temperature (Figure and Supporting Information Table and Figure ).