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AbstractThe amine groups from the periphery of poly(propylenimine) dendrimers [DAB‐(NH2)n] (n = 4 and 8) were reacted with the carboxylic groups of five different first and second generation self‐assembling dendrons. The amidation was mediated by the peptide bond forming reagent 2‐chloro‐4,6‐dimethoxy‐1,3,5‐triazine (CDMT)/N‐methylmorpholine (NMM). All the resulting dendronized dendrimers self‐assemble into helical pyramidal columns that self‐organize into columnar hexagonal and columnar rectangular 2D lattices and in supramolecular spheres that self‐organize into 3D Pm3n and P42/mnm tetragonal lattices. The structural and retrostructural analysis of the supramolecular dendrimers by X‐ray diffraction experiments demonstrated that supramolecular dendritic spheres are assembled from various spherical fragments, including conical and half‐sphere in which the DAB dendrimer is confined to their apex. Dendritic‐crown is the most frequently encountered conformation of the dendronized dendrimers that is responsible for the assembly of helical pyramidal columns.
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