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Cooperative Self-Assembly Enables Two-Dimensional H-type Aggregation of a Sterically Crowded Perylene-Bisimide Dimer

Identifying the role of multiple cooperative supramolecular interactions and the working mechanism underlying the formation of sophisticated, well-defined self-assembled architectures is definitely a challenging and formidable task in understanding the complexity in chemical systems and engineering the properties of advanced materials. The topological design of multifunctional tectons, capable of self-organizing into patterned supramolecular assemblies comprising stacked aromatic molecules, is of particular importance because it can lead to the predictable emergence of controlled functions with tailored electronic properties. Herein, we provide spectroscopic, structural, and mechanistic insights on metal-ion-mediated self-assembly of a charged, amphiphilic perylene-bisimide (PBI) dimer S into two-dimensional (2D) arrays consisting of parallel columnar PBI stacks with a precise spatial arrangement and pattern behavior, using a readily accessible design strategy. The building block (S), a centrosymmetric PB...