Publication date: 8th October 2020
Bio-hybrid nanomaterials have great potential for combining the most desirable aspects of biomolecules with the conceptual aspects of nanotechnology, both to potentially develop new solar energy harvesting technology and also to understand fundamental properties of natural systems. The plant antenna protein Light-Harvesting Complex II (LHCII) is extremely efficient at solar energy absorption and subsequent energy transfer in nature and has been demonstrated to perform effectively when incorporated into artificial nanoscale assemblies. The combination of chlorophyll and carotenoid pigments within LHCII provide relatively good absorption coverage across the visible spectrum, except for a ‘green gap’ of minimal absorption between 520-620nm. Here, we demonstrate that this spectral gap can be efficiently filled in a membrane-based assembly of LHCII together with non-covalently incorporated synthetic chromophores. Texas Red, an organic chromophore, was selected as the energy donor as it can be crosslinked onto the headgroup of a lipid, stabilising it within a model lipid membrane system. These “proteoliposomes” (protein-lipid vesicles) act as energy-transferring nanomaterials which offer the modularity to assemble a range of concentrations of the LHCII proteins and the complementary chromophores. A comprehensive analysis of the system on both the ensemble-level and the single-proteoliposome-level revealed highly efficient energy transfer both in solution and when deposited onto surfaces. This was achieved by utilising a combination of steady-state and time-resolved fluorescence spectroscopy alongside fluorescence lifetime imaging microscopy (FLIM). Lipid nanodiscs allow the investigation of energy transfer from lipid-tagged chromophores to membrane reconstituted LHCII, on a single protein level. Very recent ultrafast spectroscopy investigations have revealed the picosecond timescale of this energy transfer, and give insight into the nanoscale interactions between chromophore-linked lipids and light-harvesting membrane proteins. This system provides a platform for controllable distance-dependant energy transfer from synthetic chromophores to light-harvesting proteins, and demonstrates the potential of self-assembly driven bio-hybrid enhancement of natural systems.
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