Crossref journal-article
American Association for the Advancement of Science (AAAS)
Science (221)
Abstract

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 (P Zn ) and the other present as the free base (P). The metallated porphyrin bears a carotenoid polyene (C) and the other a diquinone species (Q A -Q B ). Excitation of the free-base porphyrin in a chloroform solution of the pentad yields an initial charge-separated state, C-P Zn -P ⋅+ -Q A ⋅- -Q B , with a quantum yield of 0.85. Subsequent electron transfer steps lead to a final charge-separated state, C ⋅+ -P Zn -P-Q A -Q B ⋅- , 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-Q A -Q B , 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.

Bibliography

Gust, D., Moore, T. A., Moore, A. L., Lee, S.-J., Bittersmann, E., Luttrull, D. K., Rehms, A. A., DeGraziano, J. M., Ma, X. C., Gao, F., Belford, R. E., & Trier, T. T. (1990). Efficient Multistep Photoinitiated Electron Transfer in a Molecular Pentad. Science, 248(4952), 199–201.

Authors 12
  1. Devens Gust (first)
  2. Thomas A. Moore (additional)
  3. Ana L. Moore (additional)
  4. Seung-Joo Lee (additional)
  5. Edith Bittersmann (additional)
  6. David K. Luttrull (additional)
  7. Aden A. Rehms (additional)
  8. Janice M. DeGraziano (additional)
  9. Xiaochun C. Ma (additional)
  10. Feng Gao (additional)
  11. Robert E. Belford (additional)
  12. Todd T. Trier (additional)
References 13 Referenced 216
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Dates
Type When
Created 18 years, 10 months ago (Oct. 5, 2006, 6:10 p.m.)
Deposited 1 year, 7 months ago (Jan. 12, 2024, 10:36 a.m.)
Indexed 4 months, 4 weeks ago (April 4, 2025, 1:25 a.m.)
Issued 35 years, 4 months ago (April 13, 1990)
Published 35 years, 4 months ago (April 13, 1990)
Published Print 35 years, 4 months ago (April 13, 1990)
Funders 0

None

@article{Gust_1990, title={Efficient Multistep Photoinitiated Electron Transfer in a Molecular Pentad}, volume={248}, ISSN={1095-9203}, url={http://dx.doi.org/10.1126/science.248.4952.199}, DOI={10.1126/science.248.4952.199}, number={4952}, journal={Science}, publisher={American Association for the Advancement of Science (AAAS)}, author={Gust, Devens and Moore, Thomas A. and Moore, Ana L. and Lee, Seung-Joo and Bittersmann, Edith and Luttrull, David K. and Rehms, Aden A. and DeGraziano, Janice M. and Ma, Xiaochun C. and Gao, Feng and Belford, Robert E. and Trier, Todd T.}, year={1990}, month=apr, pages={199–201} }