Photophysics of plasmonically enhanced self-assembled artificial light-harvesting nanoantennas.

The design of efficient artificial light-harvesting antennas is essential for enabling the widespread use of solar energy. Natural photosynthetic systems offer valuable inspiration, but many rely on complex pigment-protein interactions and have limited spectral coverage, which pose challenges for rational design. Chlorosome mimics, which are self-assembling pigment aggregates inspired by green photosynthetic bacteria, offer structural simplicity, flexible tunability, and strong excitonic coupling through pigment-pigment interactions. However, these pigment aggregates suffer from limited absorption in the green and near-infrared regions and, similarly to other light-harvesting systems, reduced energy transfer efficiency at high donor concentrations. One promising strategy to overcome these limitations is the integration of plasmonic nanoparticles, which enhance local electromagnetic fields, increase spectral coverage, and make new energetic pathways accessible. Although plasmonic enhancement has been widely studied in pigment-protein complexes like Photosystem I and light-harvesting complexes (LHCs), its application to pigment-pigment self-assembled systems remains largely unexplored. This perspective presents recent advances in biomimetic light-harvesting design with chlorosome mimics and explores the potential for plasmonic enhancement of photophysics in these systems. We examine the structure of chlorosomes and their artificial mimics to understand the role of pigment-pigment interactions in facilitating highly efficient energy transfer.