In the early studies, on Oxygenic Photosynthesis, the “quantasome hypothesis” led to seminal discoveries correlating the structure of natural photosystems with their complementary photo-redox functions. Indeed, and despite the vast bio-diversity footprint, just one protein complex is used by Nature as the H2O-photolyzer: photosystem II (PSII). Man-made systems are still far from replicating the complexity of PSII, showing the ideal co-localization of Light Harvesting antennas with the functional Reaction Center (LH-RC). Here we report the design of multi-perylenebisimide (PBI) networks shaped to function by interaction with a polyoxometalate water oxidation catalyst (Ru4POM).Our results point to overcome the classical “photo-dyad” model, based on a donor-acceptor binary combination, with integrated artificial “quantasomes” formed both in solution and on photoelectrodes, showing a: (i) red-shifted, light harvesting efficiency (LHE>40%), (ii) favorable exciton accumulation and negligible excimeric loss; (iii) a robust amphiphilic structure; (iv) dynamic aggregation into large 2D-paracrystalline domains.[5] Photoexcitation of the PBI-quantasome triggers one of the highest driving force for photo-induced electron transfer applied so far.

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