These energies correspond to diagonal elements of the model space LASSI Hamiltonian matrix, and in general, one expects that statelets with a higher energy would contribute less to the final wave functions than states with lower energy. However, excluding the nonphysical core-ionization statelet in the (11,10) results, the fragment statelets in the (11,10) active space have both higher weights and higher energy gaps compared to the LASSCF reference state than those in the larger (11,20) active space. This implies that the Hamiltonian couplings, that is, the off-diagonal Hamiltonian matrix elements between the charge-transfer model states and other model states, are likely larger for the (11,10) statelets than for the (11,20) statelets. This implies that ϵ n is larger, but so is, i.e.,