Effect of Spectral Density Shapes on the Excitonic Structure and Dynamics of the Fenna–Matthews–Olson Trimer from Chlorobaculum tepidum

Kell, Adam; Blankenship, Robert E.; Jankowiak, Ryszard

doi:10.1021/acs.jpca.6b03107

Effect of Spectral Density Shapes on the Excitonic Structure and Dynamics of the Fenna–Matthews–Olson Trimer from Chlorobaculum tepidum

Journal Article · Wed Jul 20 00:00:00 EDT 2016 · Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory

DOI:https://doi.org/10.1021/acs.jpca.6b03107· OSTI ID:1387903

Kell, Adam ^[1]; Blankenship, Robert E. ^[2]; Jankowiak, Ryszard ^[1]

Kansas State Univ., Manhattan, KS (United States)
Washington Univ., St. Louis, MO (United States)

The Fenna–Matthews–Olson (FMO) trimer (composed of identical subunits) from the green sulfur bacterium Chlorobaculum tepidum is an important protein model system to study exciton dynamics and excitation energy transfer (EET) in photosynthetic complexes. In addition, FMO is a popular model for excitonic calculations, with many theoretical parameter sets reported describing different linear and nonlinear optical spectra. Due to fast exciton relaxation within each subunit, intermonomer EET results predominantly from the lowest energy exciton states (contributed to by BChl α 3 and 4). Using experimentally determined shapes for the spectral densities, simulated optical spectra are obtained for the entire FMO trimer. Simultaneous fits of low-temperature absorption, fluorescence, and hole-burned spectra place constraints on the determined pigment site energies, providing a new Hamiltonian that should be further tested to improve modeling of 2D electronic spectroscopy data and our understanding of coherent and dissipation effects in this important protein complex.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Photosynthetic Antenna Research Center (PARC); Kansas State Univ., Manhattan, KS (United States)

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

Grant/Contract Number:: SC0001035; SC0006678

OSTI ID:: 1387903

Journal Information:: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory, Journal Name: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory Journal Issue: 31 Vol. 120; ISSN 1089-5639

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Effect of Spectral Density Shapes on the Excitonic Structure and Dynamics of the Fenna–Matthews–Olson Trimer from Chlorobaculum tepidum

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