Revealing structural involvement of chromophores in algal light harvesting complexes using symmetry-adapted perturbation theory

Toa, Zi S. Desmond; Dean, Jacob C.; Scholes, Gregory D.

doi:10.1016/j.jphotobiol.2018.11.007

Title: Revealing structural involvement of chromophores in algal light harvesting complexes using symmetry-adapted perturbation theory

Journal Article · 18 November 2018 · Journal of Photochemistry and Photobiology B: Biology

DOI: https://doi.org/10.1016/j.jphotobiol.2018.11.007 · OSTI ID:1502097

Toa, Zi S. Desmond ^[1]; Dean, Jacob C. ^[2]; Scholes, Gregory D. ^[3]

Princeton Univ., Princeton, NJ (United States); Princeton University
Southern Utah Univ., Cedar City, UT (United States)
Princeton Univ., Princeton, NJ (United States)

The attribution of quantum beats observed in the time-resolved spectroscopy of photosynthetic light-harvesting antennae to nontrivial quantum coherences has sparked a flurry of research activity beginning a decade ago. Even though investigations into the functional aspects of photosynthetic light-harvesting were supported by X-ray crystal structures, the non-covalent interactions between pigments and their local protein environment that drive such function has yet to be comprehensively explored. Using symmetry-adapted perturbation theory (SAPT), we have comprehensively determined the magnitude and compositions of these non-covalent interactions involving light-harvesting chromophores in two quintessential photosynthetic pigment-protein complexes — peridinin chlorophyll-a protein (PCP) from dinoflagellate Amphidinium carterae and phycocyanin 645 (PC645) from cryptophyte Chroomonas mesostigmatica. In PCP, the chlorophylls are dispersion-bound to the peridinins, which in turn are electrostatically anchored to the protein scaffold via their polar terminal rings. This might be an evolutionary design principle in which the relative orientation of the carotenoids towards the aqueous environment determines the arrangement of the other chromophores in carotenoid-based antennas. On the other hand, electrostatics dominate the non-covalent interactions in PC645. As a result, our ab initio simulations also suggest full protonation of the PC645 chromophores in physiological conditions, and that changes to their protonation states result in their participation as switches between folded and unfolded conformations.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Bioinspired Light-Escalated Chemistry (BioLEC); Princeton Univ., Princeton, NJ (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0019370

OSTI ID:: 1502097

Journal Information:: Journal of Photochemistry and Photobiology B: Biology, Journal Name: Journal of Photochemistry and Photobiology B: Biology Journal Issue: C Vol. 190; ISSN 1011-1344

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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