Predictive First-principles Modeling of a Photosynthetic Antenna Protein : The Fenna-Matthews-Olson Complex
Kim, Y., Morozov, D., Stadnytskyi, V., Savikhin, S., & Slipchenko, L. (2020). Predictive First-principles Modeling of a Photosynthetic Antenna Protein : The Fenna-Matthews-Olson Complex. Journal of Physical Chemistry Letters, 11(5), 1636-1643. https://doi.org/10.1021/acs.jpclett.9b03486
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Journal of Physical Chemistry LettersAuthors
Date
2020Copyright
© 2020 American Chemical Society
High efficiency of light harvesting in photosynthetic pigment-protein complexes is governed by evolutionary-perfected protein-assisted tuning of individual pigment properties and inter-pigment interactions. Due to the large number of spectrally overlapping pigments in a typical photosynthetic complex, experimental methods often fail to unambiguously identify individual chromophore properties. Here we report a first principles-based modeling protocol capable of predicting properties of pigments in protein environment to a high precision. The technique was applied to successfully uncover electronic properties of the Fenna-Matthews-Olson (FMO) pigment-protein complex. Each of the three subunits of the FMO complex contains eight strongly coupled bacteriochlorophyll a (BChl a) pigments. The excitonic structure of FMO can be described by an electronic Hamiltonian containing excitation (site) energies of BChl a pigments and electronic couplings between them. Several such Hamiltonians have been developed in the past based on the information from various spectroscopic measurements of FMO; however, fine details of the excitonic structure and energy transfer in FMO, especially assignments of short-lived high-energy sites, remain elusive. Utilizing polarizable embedding QM/MM with the effective fragment potentials (EFP) we were able to compute the electronic Hamiltonian of FMO that is in general agreement with previously reported empirical Hamiltonians and quantitatively reproduces experimental absorption and circular dichroism (CD) spectra of the FMO protein. The developed computational protocol is sufficiently simple and can be utilized for predictive modeling of other wild type and mutated photosynthetic pigment-protein complexes.
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Postdoctoral Researcher, AoFAdditional information about funding
Authors thank Prof. Gerrit Groenhof for sharing topology of BChl force fields. Y.K. and L.V.S. gratefully acknowledge support from the National Science Foundation (grant CHE1800505). S.S., V.S. and L.V.S. acknowledge support from the Department of Energy, office of Basic Energy Sciences (grant DE-SC0018239). DM acknowledges support from the Academy of Finland (grant 285481) and also thank the CSC-IT Center for Science in Espoo, Finland, for providing computational resources. This research was also supported in part through computational resources provided by Information Technology at Purdue, West Lafayette, Indiana. ...License
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