Synthesis, Structures, and Single‐Molecule Magnet Behaviour of High‐Nuclearity Nickel(II) Dicubane‐Type Complexes with Pyridyl–Alcohol Ligands

The condensation reaction between two chemically different tetranuclear cubane-like clusters [Ni((3)-Cl)(Cl)(HL)](4) (1; HL=2-methyl-1-(pyridin-2-yl)propan-2-ol) and [Ni((3)-OH)(Cl)(HL)](4) (2) provides new access to higher nuclearity complexes, as shown with the synthesis of the octanuclear complex [Ni-8((3)-Cl)(3)((3)-OH)(5)(-Cl)(2)Cl-6(HL)(7)] (3). In one instance, we also isolated the heptanuclear complex [Ni-7((3)-Cl)(2)((3)-OH)(6)Cl-4(H2O)(2)(HL)(6)]Cl-2 (4). Magnetic properties measured by superconducting quantum interference device (SQUID) susceptometry evidenced S=8 and S=5 ground states for complexes3 and 4, respectively. In particular, alternating current (ac) susceptometry evidenced slow relaxation of the magnetisation for complex3, and suggests a similar behaviour at sub-kelvin temperatures for complex4.