Crystal-Packing-Dependent Magnetic Relaxation in Octahedral Co(II) Single-Molecule Magnets

Abstract In this study, the influence of crystal packing on magnetic relaxation in Co(II)-based single-molecule magnets (SMMs) incorporating bzimpy and its carboxylated analogue is investigated. Although both complexes share similar coordination environments, their packing structures differ markedly, leading to distinct relaxation pathways. Specifically, the unsubstituted complex shows dominant Raman relaxation, whereas the substituted analogue exhibits additional Direct process contributions. These results demonstrate that subtle crystal lattice effects significantly modulate the magnetic relaxation behavior of Co(II) SMMs.