Bioinspired energy conversion

Artificial photosynthetic antenna systems have been synthesized based on carotenoid polyenes and polymer-polyenes covalently attached to tetrapyrroles. Absorption of light in the blue/green region of the spectra excites the polyenes to their S state, and ultrafast singlet energy transfer to the tetr...

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Bibliographic Details
Published in:Pure and applied chemistry 2005-06, Vol.77 (6), p.1001-1008
Main Authors: Palacios, Rodrigo E., Gould, Stephanie L., Herrero, Christian, Hambourger, Michael, Brune, Alicia, Kodis, Gerdenis, Liddell, Paul A., Kennis, John, Macpherson, Alisdair N., Gust, Devens, Moore, Thomas A., Moore, Ana L.
Format: Article
Language:English
Subjects:
antenna systems
Antennas
bioinspired
carotenoid polyenes
Carotenoids
Chemical potential
Chromophores
Conjugation
Dipole moments
Electron transfer
Electrons
Energy
Energy conversion
Energy transfer
Excitation spectra
Organic chemistry
Photosynthesis
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Description
Summary:Artificial photosynthetic antenna systems have been synthesized based on carotenoid polyenes and polymer-polyenes covalently attached to tetrapyrroles. Absorption of light in the blue/green region of the spectra excites the polyenes to their S state, and ultrafast singlet energy transfer to the tetrapyrroles occurs when the chromophores are in partial conjugation. The additional participation of other excited states of the polyene in the energy-transfer process is a requirement for perfect antenna function. Analogs of photosynthetic reaction centers consisting of tetrapyrrole chromophores covalently linked to electron acceptors and donors have been prepared. Excitation of these constructs results in a cascade of energy transfer/electron transfer which, in selected cases, forms a final charge-separated state characterized by a giant dipole moment (>150 D), a quantum yield approaching unity, a significant fraction of the photon energy stored as chemical potential, and a lifetime sufficient for reaction with secondary electron donors and acceptors. A new antenna-reaction center complex is described in which a carotenoid moiety is located in partial conjugation with the tetrapyrrole π-system allowing fast energy transfer (
ISSN:0033-4545
1365-3075
DOI:10.1351/pac200577061001