title: Primary charge-recombination in an artificial photosynthetic reaction center.
abstract: Photoinduced primary charge-separation and charge-recombination are characterized by a combination of time-resolved optical and EPR measurements of a fullerene-porphyrin-linked triad that undergoes fast, stepwise charge-separation processes. The electronic coupling for the energy-wasting charge recombination is evaluated from the singlet-triplet electronic energy gap in the short-lived, primary charge-separated state. The electronic coupling is found to be smaller by approximately 40% than that for the primary charge-separation. This inhibition of the electronic interaction for the charge-recombination to excited triplet state largely results from a symmetry-broken electronic structure modulated by configuration interaction between 3(b1u,b3g) and 3(au, b3g) electronic states of the free-base porphyrin.
authors: Department of Chemistry, University of Chicago, Chicago, IL 60637, USA.
authors: Yasuhiro
authors: Y
authors: Kobori
authors: Seigo
authors: S
authors: Yamauchi
authors: Kimio
authors: K
authors: Akiyama
authors: Shozo
authors: S
authors: Tero-Kubota
authors: Hiroshi
authors: H
authors: Imahori
authors: Shunichi
authors: S
authors: Fukuzumi
authors: James R
authors: JR
authors: Norris
mesh_terms: D004583:Electrons; D037741:Fullerenes / Q000737:chemistry*; D008956:Models, Chemical; D036103:Nanotechnology; D010777:Photochemistry / Q000379:methods*; D045322:Photosynthetic Reaction Center Complex Proteins; D011166:Porphyrins / Q000737:chemistry*; D013050:Spectrometry, Fluorescence
chemical_list: D037741:Fullerenes; D045322:Photosynthetic Reaction Center Complex Proteins; D011166:Porphyrins