Artificial light-harvesting dendritic system with sequential energy transfer and ultrahigh antenna effect for efficient photocatalysis in aqueous solution.

An efficient two-step sequential supramolecular artificial light-harvesting system has been successfully constructed using self-assembled nanoparticles of cyanostilbene-cored dendrimers (CS-1 and CS-2) as donors, along with the fluorescent dye Nile red (NiR) and near-infrared (NIR) emitter MTSIC as acceptors in aqueous media. Through supramolecular interactions, the dendritic assemblies efficiently transfer energy in a sequential manner, first to NiR and then to MTSIC, resulting in an exceptionally high antenna effect (up to 97.7) and near-quantitative energy transfer efficiencies (reaching 99.2 %). These performance metrics closely mimic those observed in natural light-harvesting systems. Remarkably, by precisely modulating the donor-acceptor ratio, the CS-2-NiR system exhibits bright white-light emission with CIE coordinates of (0.32, 0.32), aligning almost perfectly with ideal white-light standards. Furthermore, the harvested energy was successfully harnessed to drive an aerobic cross-dehydrogenative coupling (CDC) reaction, yielding an excellent isolated yield (up to 91 %). This study introduces a novel biomimetic approach for solar-to-chemical energy conversion in aqueous environments, effectively emulating critical features of natural photosynthesis while demonstrating potential applications in artificial light-harvesting and photocatalytic synthesis.