Two series of self-complementary daisy chain monomers, in which a secondary ammonium ion-containing arm is grafted onto a macrocycle with either a [24]-or [25] crown-8 constitution, have been synthesized. In the solid-and'gas'-phases, the parent [24] crown-8- based monomer forms dimeric superstructures, as revealed by X-ray crystallography and mass spectrometry, respectively. Elucidation of the complicated solution-phase behavior ...