In the present section, we examine the representationdependence of both Λ and Γ in the context of their use as CT diagnostics. We use the data set assembled by Tozer and co-workers for testing Λ; the same data set has also been used to evaluate the diagnostic properties of Γ. (Geometries are provided in the Supporting Information; see Tables and for the excitation energies.) This data set consists of numerous 59 singlet excited states including numerous 1 nπ * and 1 ππ * transitions of two dipeptides and a tripeptide, the 1 B 2u and 1 B 3u states of acenes up to hexacene, the 1 B u state of polyacetylenes H(C 2 H 2 ) n H up to n = 5, several excited states of N -phenylpyrrole and 4-(N,N -dimethylamino)benzonitrile (DMABN), and finally a variety of singlet excited states of N 2 , CO, H 2 CO, and HCl. Benchmark excitation energies are taken from Ref. 9 and used to determine errors that are plotted below as functions of Λ or Γ. Following Ref. 9, we use the cc-pVTZ basis set for all calculations in this section, except for the molecules N 2 , CO, and H 2 CO that are responsible for all of the Rydberg transitions in the data set. For these molecules, we use the doubly-augmented d-aug-cc-pVTZ basis set instead. For brevity, we refer to these calculations as "TD-DFT/triple-ζ". We focus on the hybrid functionals B3LYP and PBE0 since errors are much larger for semilocal functionals. (See Fig. smaller. The DMABN molecule is a special case that is often classified as a CT state, but whose excitation is relatively accurate even for a global hybrid functional such as B3LYP. The explanation is that the nominal CT state has a rather large value of Λ CMO , due to the molecule's compact size, indicating that electron and hole are not well separated. Because Λ is not invariant to unitary transformations, its numerical value may change dramatically upon rotating the orbitals. A vivid demonstration comes from using Boys-localized orbitals; see Fig. . Nearly all transitions, including localized valence excitations, exhibit rather small values of Λ Boys , such that the overall scale is quite compressed even while the theoretical limits (0 ≤ Λ Boys ≤ 1) remain the same. In the Boys MO representation, Λ provides no diagnostic ability whatsoever, as the Rydberg and CT states have similar values of Λ Boys as compared to localized excitations.