OpenMolcas 60 (version v19.11-d14be45) was used to perform CASSCF-SO calculations on 1-Sm and 1-Eu to determine the electronic structure. The molecular geometry from a single crystal XRD structure was used with no optimization, selecting a single molecule from the asymmetric unit and taking the largest disorder component only. Electron integrals were calculated in the SEWARD module using basis sets from the ANO-RCC library with VTZP quality on the metal atom, VDZP quality on the P and O atoms and VDZ quality on all other atoms, employing the second-order DKH Hamiltonian to account for scalar relativistic effects. Resolution of identity Cholesky decomposition of the two-electron integrals with on-the-fly auxiliary atomic compact Cholesky decomposition (acCD) basis sets was used to save disk space and to reduce computational demand. The molecular orbitals (MOs) were optimized using state-averaged CASSCF (SA-CASSCF) calculations in the RASSCF module, with a CAS(n,7) calculation where the active space included the valence 4f electrons (n) and the seven 4f orbitals. For 1-Sm, SA-CASSCF calculations were performed for all possible spins and configuration state functions: 7 heptets. For 1-Eu, SA-CASSCF calculations were performed for all possible spins and the following number of roots: 1 octet, 48 sextets, 392 quartets, and 560 doublets. A subset of these roots was then mixed by spin orbit coupling in the RASSI module, where 1 octet, 48 sextets, 119 quartets and 113 doublets 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. Density functional theory was used to optimize the hydrogen positions of 1-Yb, while all other atoms were kept frozen at the crystal structure positions; this was done using the PBE density functional with the Stuttgart RSC 1997 ECP for Yb and cc-pDVZ basis set for the ligand atoms, and dispersion interactions were included with the D3 dispersion correction. All DFT calculations were performed with Gaussian 16 Rev C.01. 76 Multiwfn 3.8 was used to perform analysis of the total electron density.