Spin Ice‐like Magnetic Relaxation of a Two‐dimensional Network based on Manganese(III) Salen‐type Single‐Molecule Magnets

Spin ice is an exotic type of magnetism displayed by bulk rare‐earth pyrochlore oxides. We discovered a spin ice‐like magnetic relaxation of [{Mn(saltmen)}4{Mn(CN)6}](ClO4)⋅13 H2O (saltmen2−=N,N′‐(1,1,2,2‐tetramethylethylene)bis(salicylideneiminate)). This magnetic system can be considered as a two‐dimensional network of MnIII salen‐type single‐molecule magnets (SMMs) in which each SMM unit (ST=4) has two orthogonally oriented axial anisotropies and is connected ferromagnetically through the [Mn(CN)6]3− unit (S=1). This work illustrates that a two‐dimensional SMM network with competition between the ferromagnetic interaction and local noncollinear magnetic anisotropies on SMMs is a new type of magnetic system exhibiting slow relaxation of magnetization with a Davidson‐Cole‐type broad distribution of the relaxation time. Spin ice‐like magnetic relaxation was found in a two‐dimensional network of MnIII salen‐type single‐molecule magnets with ST=4. The spin ice‐like behavior was a consequence of the competition between the ferromagnetic interaction and local noncollinear magnetic anisotropies on the single‐molecule magnets.