Excited state energy fluctuations in the Fenna-Matthews-Olson complex from molecular dynamics simulations with interpolated chromophore potentials

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We analyze the environment-induced fluctuation of pigment excitation energies in the Fenna-MatthewsOlson (FMO) complex from various perspectives, by employing an interpolation-based all-atom potential energy model for describing realistic pigment vibrations. We conduct molecular dynamics simulations on a 100 ns timescale, which is an extent that can enclose the effect of static disorder, and demonstrate its timescale separation from fast dynamic disorder. We extract the spectral densities of the complex by considering both the site and the exciton bases. We show that exciton delocalization reduces the effective environmental fluctuation and rationalize this aspect based on a model of fluctuating molecular aggregates. We also obtained the spectral density of the lowest exciton state under low temperature conditions and show that it reasonably well reproduces the experimental result. Finally, by additionally performing non-equilibrium excited state trajectory simulations, we show that the system lies well within the linear response regime after photo-absorption and that the pigments do not visit anharmonic regions of the potential surface to a significant extent. This indicates that methodologies based on harmonic bath models are indeed reasonable approaches for describing the excited state dynamics of the FMO complex.
Publisher
ROYAL SOC CHEMISTRY
Issue Date
2018-02
Language
English
Article Type
Article
Keywords

LIGHT-HARVESTING COMPLEXES; AB-INITIO DESCRIPTION; SPECTRAL DENSITY; ELECTRON-PHONON; 2-DIMENSIONAL SPECTRA; FMO COMPLEX; PROTEIN; MODEL; BACTERIOCHLOROPHYLL; TRANSITIONS

Citation

PHYSICAL CHEMISTRY CHEMICAL PHYSICS, v.20, no.5, pp.3310 - 3319

ISSN
1463-9076
DOI
10.1039/c7cp06303b
URI
http://hdl.handle.net/10203/240371
Appears in Collection
CH-Journal Papers(저널논문)
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