National Institutes of Health/National Institute of Environmental Health Sciences (NIH/NIEHS)
P30-ES002109
United States
National Science Foundation (NSF, United States)
CMMI-2240309
United States
Office of Naval Research (ONR)
N00014-19-1-2344
United States
National Science Foundation (NSF, United States)
NSF CCF-1956054
United States
Citation
Journal: Chem / Year: 2024 Title: Sculpting photoproducts with DNA origami. Authors: Jeffrey Gorman / Stephanie M Hart / Torsten John / Maria A Castellanos / Dvir Harris / Molly F Parsons / James L Banal / Adam P Willard / Gabriela S Schlau-Cohen / Mark Bathe / Abstract: Natural light-harvesting systems spatially organize densely packed dyes in different configurations to either transport excitons or convert them into charge photoproducts, with high efficiency. In ...Natural light-harvesting systems spatially organize densely packed dyes in different configurations to either transport excitons or convert them into charge photoproducts, with high efficiency. In contrast, artificial photosystems like organic solar cells and light-emitting diodes lack this fine structural control, limiting their efficiency. Thus, biomimetic multi-dye systems are needed to organize dyes with the sub-nanometer spatial control required to sculpt resulting photoproducts. Here, we synthesize 11 distinct perylene diimide (PDI) dimers integrated into DNA origami nanostructures and identify dimer architectures that offer discrete control over exciton transport versus charge separation. The large structural-space and site-tunability of origami uniquely provides controlled PDI dimer packing to form distinct excimer photoproducts, which are sensitive to interdye configurations. In the future, this platform enables large-scale programmed assembly of dyes mimicking natural systems to sculpt distinct photophysical products needed for a broad range of optoelectronic devices, including solar energy converters and quantum information processors.
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