A1 Journal article (refereed)
Predictive First-principles Modeling of a Photosynthetic Antenna Protein : The Fenna-Matthews-Olson Complex (2020)
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
JYU authors or editors
Publication details
All authors or editors: Kim, Yongbin; Morozov, Dmitry; Stadnytskyi, Valentyn; Savikhin, Sergei; Slipchenko, Lyudmila
Journal or series: Journal of Physical Chemistry Letters
eISSN: 1948-7185
Publication year: 2020
Volume: 11
Issue number: 5
Pages range: 1636-1643
Publisher: American Chemical Society
Publication country: United States
Publication language: English
DOI: https://doi.org/10.1021/acs.jpclett.9b03486
Publication open access: Not open
Publication channel open access:
Publication is parallel published (JYX): https://jyx.jyu.fi/handle/123456789/67903
Abstract
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.
Keywords: proteins; pigments; modelling (representation); spectroscopy
Free keywords: pigment-protein complex; Fenna-Matthews-Olson protein; QM/MM; QM/EFP; effective fragment potential; polarizable embedding
Contributing organizations
Related projects
- Excitation energy transfer in chemical and biological systems
- Morozov, Dmitry
- Research Council of Finland
Ministry reporting: Yes
Reporting Year: 2020
JUFO rating: 3