The aug-cc-pVTZ+5s5p5d5f basis set was used for most ab initio calculations, unless indicated otherwise. The basis set was constructed by supplementing the standard aug-cc-pVTZ basis with five s, five p, five d, and five f additional diffuse functions with exponents decreasing progressively by a factor of 2. All electronic structure calculations were carried out using Q-Chem. The Dyson orbitals obtained using the above EOM-EA/SF and EOM-IP approaches are shown in Fig. 2.426 Å 2 , while those for b 1 Σ  are 2.049 vs. 2.257 Å 2 . The 〈𝑅 〉 differences are largely due to the long-range tails of the wave functions, rather than their short-range amplitudes, which is why they are not observable in Fig. . To illustrate this point, Fig. shows one-dimensional plots of the 𝑦 dipole operator (𝑦 ) multiplied by the EOM-EA/SF and EOM-IP Dyson orbitals for the X 3 Σ  transition. The graph reveals a more diffuse tail of the orbital computed using EOM-IP.