was performed to save disk space and reduce computational demand. The molecular orbitals (MOs) were optimized in state-averaged CASSCF calculations in the RASSCF module, where the active space was defined by the nine 4f electrons in the seven 4f orbitals of Dy(III). Three such calculations were performed independently for each possible spin state, where 21 roots were included for S = 5/2, 224 roots were included for S = 3/2, and 490 roots were included for S = 1/2. The wavefunctions obtained from these CASSCF calculations were then mixed by spin orbit coupling in the RASSI module, where all 21 S = 5/2 states, 128 of the S = 3/2 states, and 130 of the S = 1/2 states were included. SINGLE_ANISO was used to decompose the resulting spin-orbit wave functions into the CF Hamiltonian formalism. Diamond was employed for molecular graphics. DFT geometry optimizations and vibrational analyses were performed on the cation of 1-Y, 2-Y, the monomer of 3-Y, and 4-Y, for the purposes of assigning experimental IR spectra (Figures ).