The "triazine propeller" depicted in Fig. has been con- Charge-separation metrics for S 1 through S 10 are provided in Table and additional metrics can be found in meaning d e-h , although reasonable correlation is also observed using CMOs. Given what we now understand from the analysis presented herein, we can state that because long-range CT transitions are dominated by a single NTO pair, we expect excellent correspondence between (∆r) NTO and d e-h . As a first example, we consider low-lying singlet excitations in a set of 29 intermolecular CT dimers assembled from common small-molecule electron donors (acenes, stilbenes, thiophenes, etc.) and acceptors (tetracyanoquinone and its fluorinated analogues). In calculations at the TD-B3LYP/6-31+G* level, we find that the S 0 → S 1 and S 0 → S 2 transitions are dominated by a single NTO pair in every single case, with λ 2 1 (S 1 ) ≥ 0.99 and λ 2 1 (S 2 ) ≥ 0.94. For S 0 → S 3 , λ 2 1 ≥ 0.90 except for a few cases involving complexes of meso-diphenyl tetrathia [22]annulene[2,1,2,1] (DPTTA) with fluorinated tetracyanoquinone, for which λ 2 1 = 0.83. As a result, we expect that (∆r) NTO should correlate reasonably well with d e-h for the S 1 , S 2 , and S 3 states of these dimers.