OpenMolcas was used to perform CASSCF-SO calculations on 1-Dy to determine its electronic structure (Figures S99 and S100 and Table ). The molecular geometry from the single crystal XRD structure was used with no optimization, taking the largest disorder component only. Integrals were performed in the SEWAD module using basis sets from ANO-RCC library with VTZP quality for Dy atoms, VDZP quality for the N atoms, and VDZ quality for all remaining atoms, employing the secondorder DKH Cholesky decomposition of the two-electron integrals with a threshold of 10 -8