Photodriven charge separation in a carotenoporphyrin-quinone triad

Thomas A Moore, John Devens Gust, Paul Mathis, Jean Claude Mialocq, Claude Chachaty, René V. Bensasson, Edward J. Land, Denis Doizi, Paul A. Liddell, William R. Lehman, Gregory A. Nemeth, Ana L Moore

Research output: Contribution to journalArticle

258 Citations (Scopus)

Abstract

The key steps in the photosynthetic conversion of light to chemical potential energy include not only photodriven charge separation, but also prevention of the back-reaction (charge recombination). Although the first of these steps has been achieved in several biomimetic solar energy conversion systems, retarding the back-reaction has proved more difficult. This may be accomplished by rapidly moving the electron, the hole, or both away from the site of excitation to more stabilizing environments. In photosynthetic membranes, the electron is transferred sequentially over several closely coupled molecules, including tetrapyrroles and quinones1-3. In semiconductor/liquid interfacial systems both the electron and the hole migrate following excitation4,5. We now report that substantial slowing of the back-reaction has been achieved with a tripartite molecule in which a long-lived photodriven charge-separated state of relatively high potential is formed from an excited singlet state in accordance with the above principles. This molecular triad (compound I) consists of a tetraarylporphyrin covalently linked to both a carotenoid and a quinone. In solution, excitation of the porphyrin moiety by visible light results in the rapid (+.-P-Q--., with a lifetime on the μs time scale and an energy more than 1 eV above the ground state.

Original languageEnglish
Pages (from-to)630-632
Number of pages3
JournalNature
Volume307
Issue number5952
DOIs
Publication statusPublished - 1984

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Electrons
Photosynthetic membranes
Tetrapyrroles
Molecules
Chemical potential
Porphyrins
Biomimetics
Carotenoids
Potential energy
Energy conversion
Excited states
Solar energy
Ground state
Semiconductor materials
Liquids
benzoquinone

ASJC Scopus subject areas

  • General

Cite this

Photodriven charge separation in a carotenoporphyrin-quinone triad. / Moore, Thomas A; Gust, John Devens; Mathis, Paul; Mialocq, Jean Claude; Chachaty, Claude; Bensasson, René V.; Land, Edward J.; Doizi, Denis; Liddell, Paul A.; Lehman, William R.; Nemeth, Gregory A.; Moore, Ana L.

In: Nature, Vol. 307, No. 5952, 1984, p. 630-632.

Research output: Contribution to journalArticle

Moore, TA, Gust, JD, Mathis, P, Mialocq, JC, Chachaty, C, Bensasson, RV, Land, EJ, Doizi, D, Liddell, PA, Lehman, WR, Nemeth, GA & Moore, AL 1984, 'Photodriven charge separation in a carotenoporphyrin-quinone triad', Nature, vol. 307, no. 5952, pp. 630-632. https://doi.org/10.1038/307630a0
Moore TA, Gust JD, Mathis P, Mialocq JC, Chachaty C, Bensasson RV et al. Photodriven charge separation in a carotenoporphyrin-quinone triad. Nature. 1984;307(5952):630-632. https://doi.org/10.1038/307630a0
Moore, Thomas A ; Gust, John Devens ; Mathis, Paul ; Mialocq, Jean Claude ; Chachaty, Claude ; Bensasson, René V. ; Land, Edward J. ; Doizi, Denis ; Liddell, Paul A. ; Lehman, William R. ; Nemeth, Gregory A. ; Moore, Ana L. / Photodriven charge separation in a carotenoporphyrin-quinone triad. In: Nature. 1984 ; Vol. 307, No. 5952. pp. 630-632.
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