Hierarchical Self‐Assembly of Supramolecular Spintronic Modules into 1D‐ and 2D‐Architectures with Emergence of Magnetic Properties

Hierarchical self‐assembly of complex supramolecular architectures allows for the emergence of novel properties at each level of complexity. The reaction of the ligand components A and B with Fe^II cations generates the [2×2] grid‐type functional building modules 1 and 2 , presenting spin‐transition properties and preorganizing an array of coordination sites that sets the stage for a second assembly step. Indeed, binding of La^III ions to 1 and of Ag^I ions to 2 leads to a 1D columnar superstructure 3 and to a wall‐like 2D layer 4 , respectively, with concomitant modulation of the magnetic properties of 1 and 2 . Thus, to each of the two levels of structural complexity generated by the two sequential self‐assembly steps corresponds the emergence of novel functional features.