Tailoring single-ion magnet properties of coordination polymer CHDyNO (Dy-CP) using the radial effective charge model (RECM) and superposition model (SPM).

We investigate Dy-based coordination polymer CHDyNO (Dy-CP) exhibiting single-ion magnet (SIM) properties, , quantum tunnelling of magnetization (QTM), magnetic anisotropy, magnetic relaxation, and effective energy barrier (). To elucidate the underlying mechanisms, crystal field parameters (CFPs) for Dy ions were modelled using the radial effective charge model (RECM) and superposition model (SPM), and the computational packages SIMPRE and SPECTRE. The modelled CFPs enable the prediction of the energy levels and associated wave functions, which successfully explain the field-induced Dy-CP SIM properties. The so-calculated magnetic susceptibility and isothermal magnetization match the experimental data reasonably well. The smaller energy separations of the first ( ∼ 31 cm) and the second ( = 74 cm) excited Kramers doublets suggest small = 65 cm for Dy-CP. The magnetic moments of Dy ions exhibit an easy-axis type magnetic anisotropy in the ground state, but change orientation in the excited states due to mixing of states from different Kramers doublets. Low-symmetry CF components play a crucial role in connecting different |±M〉 states within the ground multiplet, resulting in QTM and magnetic relaxation to the ground state occurring the excited states. The RECM and SPM calculated CFP sets are standardized employing the 3DD package to enable meaningful comparison and assessing their mutual equivalence. The results demonstrate the correlation between structural and electronic features of the molecule and site symmetry and distortion of the local coordination polyhedra with SIM properties, offering insights for rational design of new SIMs. The importance of considering low-symmetry aspects in CFP modelling for accurate predictions of magnetic properties is highlighted. This study provides deeper understanding of field-induced behaviour in rare-earth-based SIMs and approaches for rationalization of experimentally measured SIMs' properties.