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Viologen-based ditopic bis-pyridinyl-triazole bidentate ligands self-assemblein the presence of palladium ions into supramolecular polymers whose structureis imposed by the directed formation of coordination bonds. Light-irradiationof these electron-responsive supramolecular materials triggers a photo-inducedelectron transfer yielding isolated {\pi}-radicals and dimers of radicals. Thephotoreduction events and the associated dimerization steps trigger alarge-scale reorganization occurring within the supramolecular network yieldingaggregates or gels depending on the irradiation conditions (power, duration).Detailed electrochemical, spectro-electrochemical and photochemical analyseswere conducted to understand the mechanisms at stakes in these light-inducedaggregation and gelation.

Photoredox Processes in the Aggregation and Gelation of Electron-responsive Supramolecular Polymers Based on Viologens