 The researchers have discovered two-dimensional, 2D, porphyrin frameworks with giant magnetic and isotropy energies, MAEs, which could be used as promising candidates for future spintronic applications. They replaced the hydrogen atoms on the edges of the re-based 2D porphyrin framework with hydroxyl and amino radicals, resulting in an increase of MAE from 24 MeV to 60 MeV. This was due to the charge redistributions and energy shifts of the Re5D orbitals caused by the functional radicals. These results suggest that the incorporation of functional radicals into 2D porphyrins may provide a viable route towards the development of magnetic organic materials with tunable MAE for use in spintronic applications. This article was authored by Peng Wang, Xue Jiang, Jun Hu, and others.