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The mechanism and thermodynamic functions of the self-assembly of a family of covalently linked oligomeric naphthalenediimides (NDIs) were investigated through variable-temperature NMR and CD studies. The NDIs were shown to self-assemble into helical supramolecular nanotubes via an isodesmic polymerisation mechanism, and regardless of the oligomer length a surprising entropy–enthalpy compensation was observed.

Graphical abstract: The thermodynamics of the self-assembly of covalently linked oligomeric naphthalenediimides into helical organic nanotubes

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