Magnetic Archimedean Tessellations in Metal-Organic Frameworks

The self-assembly of trivalent lanthanide ions with ditopic organic spacers results in the formation of complex tiling patterns that mimic the structural motifs of quasi-periodic 2D materials. The assembly of trans-{LnI₂}⁺ nodes (Ln = Gd, Dy) with both closed-shell and anion radicals of 4,4'-bipyridine affords rare examples of Archimedean tessellations in a metal-organic framework. We furthermore demonstrate occurrence of sizable magnetic exchange interactions and slow relaxation of magnetization behaviour in a complex tessellation pattern. The implementation of Archimedean tessellations in lanthanide(III) coordination solids couriers a strategy to design elusive quasi-periodic metal-organic frameworks with inimitable magnetic properties