where in this case LS and HS for the entire node indicate respectively S = 1 2 and S = 9 2 . At the CASCI level, using the high-spin optimized LASSCF orbitals, J = -3.81 cm -1 for the (11,10) 3d active space, and J = -6.25 cm -1 for the (11,20) 3d+3d ′ active space. The optimized active orbitals for the (11,20) case and their occupancies are depicted and labeled in Fig. of the SI. The optimized orbitals in the (11,10) case appear similar to the 3d orbitals in SI Fig. when visualized, although see below.