Efficient Multistep Photoinitiated Electron Transfer in a Molecular Pentad

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Science  13 Apr 1990:
Vol. 248, Issue 4952, pp. 199-201
DOI: 10.1126/science.248.4952.199


A synthetic five-part molecular device has been prepared that uses a multistep electron transfer strategy similar to that of photosynthetic organisms to capture light energy and convert it to chemical potential in the form of long-lived charge separation. It consists of two covalently linked porphyrin moieties, one containing a zinc ion (PZn) and the other present as the free base (P). The metailated porphyrin bears a carotenoid polyene (C) and the other a diquinone species (QA-QB). Excitation of the free-base porphyrin in a chloroform solution of the pentad yields an initial charge-separated state, C-PZn-P.+.-QA--QB, with a quantum yield of 0.85. Subsequent electron transfer steps lead to a final charge-separated state, C.+-PZn-P-QA-QB.-, which is formed with an overall quantum yield of 0.83 and has a lifetime of 55 microseconds. Irradiation of the free-base form of the pentad, C-P-P-QA-QB, gives a similar charge-separated state with a lower quantum yield (0.15 in dichloromethane), although the lifetime is increased to ∼340 microseconds. The artificial photosynthetic system preserves a significant fraction (∼1.0 electron volt) of the initial excitation energy (1.9 electron volts) in the long-lived, charge-separated state.

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