Minding the Gap between Plant and Bacterial Photosynthesis within a Self-Assembling Biohybrid Photosystem

Many strategies for meeting mankind's future energy demands through the exploitation of plentiful solar energy have been influenced by the efficient and sustainable processes of natural photosynthesis. A limitation affecting solar energy conversion based on photosynthetic proteins is the selective spectral coverage that is the consequence of their particular natural pigmentation. Here we demonstrate the bottom-up formation of semisynthetic, polychromatic photosystems in mixtures of the chlorophyll-based LHCII major light harvesting complex from the oxygenic green plant Arabidopsis thaliana, the bacteriochlorophyll-based photochemical reaction center (RC) from the anoxygenic purple bacterium Rhodobacter sphaeroides and synthetic quantum dots (QDs). Polyhistidine tag adaptation of LHCII and the RC enabled predictable self-assembly of LHCII/RC/QD nanoconjugates, the thermodynamics of which could be accurately modeled and parametrized. The tricomponent biohybrid photosystems displayed enhanced solar energy conversion via either direct chlorophyll-to-bacteriochlorophyll energy transfer or an indirect pathway enabled by the QD, with an overall energy transfer efficiency comparable to that seen in natural photosystems.