Influence of the supramolecular architecture on the magnetic properties of a DyIIIsingle-molecule magnet: an ab initio investigation
Résumé
Single-crystal angular-resolved magnetometry and wavefunction-based calculations have been used to reconsider the magneticproperties of a recently reported DyIII-based single-molecule magnet, namely [Dy(hfac)3(L1)] with hfac− = 1,1,1,5,5,5-hexafluoroacetylacetonateand L1 = 2-(4,5-bis(propylthio)-1,3-dithiol-2-ylidene)-6-(pyridin-2-yl)-5H-[1,3]dithiolo[4',5':4,5]benzo[1,2-d]imidazole. The magnetic susceptibility and magnetization at low temperature are found to be strongly influenced by supramolecularinteractions. Moreover, taking into account the hydrogen-bond networks in the calculations allows to explain the orientationof the magnetic axes. This strongly suggests that hydrogen bonds play an important role in the modulation of the electrostaticenvironment around the DyIII center that governs the nature of its magnetic ground-state and the orientation of its anisotropy axes.We thus show here that SMM properties that rely on supramolecular organization may not be transferable into single-moleculedevices.