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Structure and function of photoreaction-centre chlorophyll.

J J Katz, L L Shipman, J R Norris

    Ciba Foundation Symposium
    |February 7, 1978
    PubMed
    Summary

    Electron paramagnetic resonance studies reveal that the unpaired spin in oxidized P700+ or P865+ is shared by two special chlorophyll molecules. This finding supports C2 symmetric models for reaction center chlorophyll, with implications for primary photochemistry.

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    Area of Science:

    • Photosynthesis research
    • Biophysical chemistry
    • Molecular biology

    Background:

    • The special pair of chlorophyll molecules in photosynthetic reaction centers plays a crucial role in primary charge separation.
    • Understanding the electronic structure and dynamics of this special pair is key to elucidating the mechanism of photosynthesis.
    • Existing models for the special pair include asymmetric, translationally symmetric, and C2 symmetric configurations.

    Purpose of the Study:

    • To investigate the electronic structure of the oxidized special pair in reaction centers using electron paramagnetic resonance (e.p.r.).
    • To synthesize and characterize in vitro models of special pair chlorophyll with C2 symmetry.
    • To elucidate the primary photochemistry and spin polarization mechanisms in photosynthetic reaction centers.

    Main Methods:

    • Electron paramagnetic resonance (e.p.r.) spectroscopy to study oxidized P700+ and P865+.
    • Synthesis of in vitro models with C2 symmetry using covalently linked chlorophyll macrocycles.
    • Nuclear magnetic resonance (n.m.r.) and optical spectroscopy (absorption, emission, phosphorescence) to characterize model compounds.
    • Analysis of spin polarization in the special pair triplet state.

    Main Results:

    • E.p.r. evidence suggests the unpaired spin in oxidized P700+ or P865+ is delocalized over two special chlorophyll a or bacteriochlorophyll a molecules.
    • Synthesized in vitro C2 symmetric models exhibit distinct singlet and triplet state properties.
    • Phosphorescence occurs only from the folded configuration of linked dimers, indicating an efficient non-radiative decay pathway.

    Conclusions:

    • The findings support C2 symmetric models for the special pair in photosynthetic reaction centers.
    • A radical-pair mechanism is proposed to explain the unusual spin polarization observed in the special pair triplet state.
    • The study provides insights into the fundamental processes governing primary photochemistry in photosynthesis.

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