The two mononuclear complexes of the formula [Dy(tta)₃(L)] (1) and [Dy(hfac)₃(L)] (2) (where tta^- = 2-thenoytrifluoroacetylacetonate and hfac^- = 1,1,1,5,5,5-hexafluoroacetylacetonate) were obtained from the coordination reaction of the Dy(tta)₃·2H₂O or Dy(hfac)₃·2H₂O units with the 1,10-phenantroline-5,6-dione ligand (L). Their structures have been determined by X-ray diffraction studies on single crystals, and they revealed a supramolecular assembly of tetramers through σ-π interactions. Both complexes displayed a Single-Molecule Magnet (SMM) behavior without an external applied magnetic field. Magnetic relaxation happened through Orbach, Raman and Quantum Tunneling of the Magnetization (QTM). Wavefunction theory calculations were realized to rationalize the magnetic properties.

The mononuclear single-molecule magnet (SMM) [Dy(tta)₃(L)]⋅C₆H₁₄ (1) (where tta⁻ = 2-thenoyltrifluoroacetonate and L = 4,5-bis(propylthio)-tetrathiafulvalene-2-(2-pyridyl)benzimidazole-methyl-2-pyridine) was studied by spectro-electrochemistry. The resulting electronic spectra of the three oxidation states 1, 1⁺∙, and 1²⁺ were rationalized by time-dependent density functional theory (TD-DFT) calculations starting from the DFT optimized structures. The modulation of the magnetic anisotropy of the Dy^III center upon oxidation was also inspected at the Complete Active Space Self-Consistent Field (CASSCF) level of calculation.

The complexes [Dy₂(tta)₆(H2SQ)] (Dy-H₂SQ) and [Dy₂(tta)₆(Q)]·2CH₂Cl₂ (Dy-Q) (tta⁻ = 2-thenoyltrifluoroacetonate) were obtained from the coordination reaction of the Dy(tta)₃·2H₂O units with the 2,2′-benzene-1,4-diylbis(6-hydroxy-4,7-di-tert-butyl-1,3-benzodithiol-2-ylium-5-olate ligand (H₂SQ) and its oxidized form 2,2′-cyclohexa-2,5-diene-1,4-diylidenebis(4,7-di-tert-butyl-1,3-benzodithiole-5,6-dione (Q). The chemical oxidation of H₂SQ in Q induced an increase in the coordination number from 7 to 8 around the Dy^III ions and by consequence a modulation of the field-induced Single-Molecule Magnet behavior. Computational results rationalized the magnetic properties of each of the dinuclear complexes.