title: Regeneration of Light-Harvesting Complexes via Dynamic Replacement of Photodegraded Chromophores.
abstract: All-synthetic molecular donor-acceptor complexes are designed, which are capable of counteracting the effect of photoinduced degradation of donor chromophores. Anionic gallium protoporphyrin IX (GaPP) and semiconducting carbon nanotube (CNT) are used as a model donor-acceptor complex, which is assembled using DNA oligonucleotides. The GaPP-DNA-CNT complex produces an anodic photocurrent in a photoelectrochemical cell, which steadily decays due to photo-oxidation. By modulating the chemical environment, we showed that the photodegraded chromophores may be dissociated from the complex, whereas the DNA-coated carbon nanotube acceptors are kept intact. Reassociation with fresh porphyrins leads to the full recovery of GaPP absorption and photocurrents. This strategy could form a basis for improving the light-harvesting performance of molecular donor-acceptor complexes and extending their operation lifetime.
authors.affiliation: †School of Mechanical Engineering and ‡Department of Chemistry, Purdue University, West Lafayette, Indiana 47907, United States.
authors.forename: Hanyu
authors.initials: H
authors.lastname: Zhang
authors.affiliation: †School of Mechanical Engineering and ‡Department of Chemistry, Purdue University, West Lafayette, Indiana 47907, United States.
authors.forename: Jing
authors.initials: J
authors.lastname: Pan
authors.affiliation: †School of Mechanical Engineering and ‡Department of Chemistry, Purdue University, West Lafayette, Indiana 47907, United States.
authors.forename: Srijana
authors.initials: S
authors.lastname: Ghimire
authors.affiliation: †School of Mechanical Engineering and ‡Department of Chemistry, Purdue University, West Lafayette, Indiana 47907, United States.
authors.forename: Matthew A
authors.initials: MA
authors.lastname: Bork
authors.affiliation: †School of Mechanical Engineering and ‡Department of Chemistry, Purdue University, West Lafayette, Indiana 47907, United States.
authors.forename: Molly M
authors.initials: MM
authors.lastname: Riccitelli
authors.affiliation: †School of Mechanical Engineering and ‡Department of Chemistry, Purdue University, West Lafayette, Indiana 47907, United States.
authors.forename: David R
authors.initials: DR
authors.lastname: McMillin
authors.affiliation: †School of Mechanical Engineering and ‡Department of Chemistry, Purdue University, West Lafayette, Indiana 47907, United States.
authors.forename: Jong Hyun
authors.initials: JH
authors.lastname: Choi
mesh_terms: D004396:Coloring Agents / Q000737:chemistry* / Q000528:radiation effects; D004247:DNA / Q000737:chemistry* / Q000528:radiation effects; D004553:Electric Conductivity; D004579:Electron Transport; D005708:Gallium / Q000737:chemistry*; D008027:Light; D045342:Light-Harvesting Protein Complexes / Q000737:chemistry* / Q000528:radiation effects; D008422:Materials Testing; D037742:Nanotubes, Carbon / Q000737:chemistry* / Q000528:radiation effects; D011524:Protoporphyrins / Q000737:chemistry* / Q000528:radiation effects; D059027:Recycling / Q000379:methods; D012666:Semiconductors
chemical_list: D004396:Coloring Agents; D045342:Light-Harvesting Protein Complexes; D037742:Nanotubes, Carbon; D011524:Protoporphyrins; D004247:DNA; C028025:protoporphyrin IX; D005708:Gallium
keywords: carbon nanotubes; donor−acceptor complex; photocurrent; photoelectrochemistry; porphyrin