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Title | Sculpting photoproducts with DNA origami. |
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Journal, issue, pages | Chem, Vol. 10, Issue 5, Page 1553-1575, Year 2024 |
Publish date | May 9, 2024 |
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 / |
PubMed 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. |
External links | Chem / PubMed:38827435 / PubMed Central |
Methods | EM (single particle) |
Resolution | 13.8 Å |
Structure data | EMDB-43592: PDI-containing spoke of a hexagonal wireframe DNA origami |
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