Beyond qualitative identification of SCO complexes using an energy cutoff, we quantify SCO behavior with T1/2 values predicted by the 23 DFAs and modB3LYP functionals in comparison to experimentally reported T1/2 values. The T1/2 values corresponding to single-step SCO behavior are reported only for 76 of the complexes in SCO-95, while the remaining systems either exhibit two-step SCO behavior or a single-step SCO event without a reported T1/2 in the manuscript (Figure and Supporting Information Figure and Table ). In order to make a comparison between computationally predicted T1/2 values and experimentally reported T1/2 values for more systems, we also attempted to estimate experimental T1/2 as the average of low-T and high-T of crystallization, but the presence of outliers motivates our focus on only the 76 complexes for which T1/2 is directly reported (Figure and Supporting Information Tables Next, we compare T1/2 values predicted from the 23 DFAs and modB3LYP functionals with varying aHF against those reported experimentally. As could be expected, despite experimentally observed SCO behavior, if DGH-L is not predicted to be within 5 kcal/mol, then T1/2 values will not be reasonable. Thus, only modB3LYP (aHF = 0.10), M06-L, and TPSSh predict reasonable T1/2 values (i.e., between 0 and 1000 K, Figure and Supporting Information Table ). Nevertheless, the T1/2 values predicted by modB3LYP (aHF = 0.10), TPSSh, and M06-L also show limited correlation with experimentally reported values, with Pearson's r of ca. 0.36 for all three functionals (Figure and Supporting Information Figures ). While all three functionals show similar degree of correlation to experimentally reported values, closer examination reveals that the complexes for which DFA and experimental predictions are consistent (i.e., within < 10 K) vary between the functionals (Figure and Supporting Information Figures S32-S34 and Table ). The T1/2 values predicted by M06-L are comparable to experimental values for three complexes (refcodes: BAXJUI 185 , OJIPIH 186 , PEJQIF 187 ), while sets of two entirely different complexes are predicted consistently for TPSS (refcodes: IMAHIO 188 and OTUJUJ 189 ) and modB3LYP (aHF = 0.10, refcodes: JOMNIK 190 and VESMOX 191 , Figure and Supporting Information Figures S32-S34 and Table ). Of these complexes, only BAXJUI 185 that was well-predicted by M06-L also has a T1/2 value around an often-targeted room temperature (294 K) value. If we widen our target for consistency to 40 K, we find only a single complex (refcode: VIFNAC 151 ) for which all three functionals predict T1/2 values that are consistent with experiments (Figure and Supporting Information Figures S32-S34 and Table ). Thus, while broadly predicting SCO behavior within energetic bounds is readily achieved, T1/2 represents an expectedly more challenging target and one that should be judged across a large set of complexes, rather than the few cases for which one functional may serendipitously perform well. We next aimed to identify if the errors in DFA prediction of T1/2 could be attributed to any specific ligand chemistry or SCO behavior. We find that there are complexes for which DFApredicted T1/2 values are considerably larger than their specific experimentally reported values (by 100 K or more) but within the range of overall experimentally reported T1/2 values, i.e., 100 K < T1/2 < 450 K (Supporting Information Table ). For example, there are three hexakis monodentate complexes (refcodes: GOGSAZ 192 , NIGXUY 150 , and YAGYIP 157 ) for which DFApredicted T1/2 values of all three functionals are larger than experimentally reported values, but examination of the manuscripts for these complexes indicates they all exhibit gradual, single-step SCO behavior (Supporting Information Table and Figure ).