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CHEMISTRY
Primary charge-recombination in an artificial photosynthetic reaction center

Yasuhiro Kobori , Seigo Yamauchi , Kimio Akiyama , Shozo Tero-Kubota , Hiroshi Imahori , Shunichi Fukuzumi ^¶, and James R. Norris, Jr. ^, ||, 

Department of Chemistry and ^||Institute for Biophysical Dynamics, University of Chicago, Chicago, IL 60637; Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Sendai 980-8577, Japan; Department of Molecular Engineering, Graduate School of Engineering, Kyoto University, Katsura, Nishikyo-ku, Kyoto 615-8510, Japan; and ^¶Department of Material and Life Science, Graduate School of Engineering, Solution Oriented Research for Science and Technology, Japan Science and Technology Agency, Osaka University, Suita, Osaka 565-0871, Japan

Communicated by Donald H. Levy, University of Chicago, Chicago, IL, June 2, 2005 (received for review February 17, 2005)

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 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(b_1u,b_3g) and ³(a_u, b_3g) electronic states of the free-base porphyrin.

electronic coupling | long-range electron transfer | molecular orbital symmetry

To whom correspondence should be addressed at: Department of Chemistry, University of Chicago, 5735 South Ellis Avenue, Chicago, IL 60637. E-mail: jrnorris{at}uchicago.edu.

© 2005 by The National Academy of Sciences of the USA

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