Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

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

Abstract

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.

Authors:
 [1];  [2];  [1]
+ Show Author Affiliations
  1. Kansas State Univ., Manhattan, KS (United States)
  2. Washington Univ., St. Louis, MO (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Photosynthetic Antenna Research Center (PARC); Kansas State Univ., Manhattan, KS (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1387903
Grant/Contract Number:  
SC0001035; SC0006678
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory
Additional Journal Information:
Journal Volume: 120; Journal Issue: 31; Related Information: PARC partners with Washington University in St. Louis (lead); University of California, Riverside; University of Glasgow, UK; Los Alamos National Laboratory; University of New Mexico; New Mexico Corsortium; North Carolina State University; Northwestern University; Oak Ridge National Laboratory; University of Pennsylvania; Sandia National Laboratories; University of Sheffield, UK; Journal ID: ISSN 1089-5639
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 59 BASIC BIOLOGICAL SCIENCES; solar (fuels); photosynthesis (natural and artificial); biofuels (including algae and biomass); bio-inspired; charge transport; membrane; synthesis (novel materials); synthesis (self-assembly)

Citation Formats

Kell, Adam, Blankenship, Robert E., and Jankowiak, Ryszard. Effect of Spectral Density Shapes on the Excitonic Structure and Dynamics of the Fenna–Matthews–Olson Trimer from Chlorobaculum tepidum. United States: N. p., 2016. Web. doi:10.1021/acs.jpca.6b03107.
Copy to clipboard
Kell, Adam, Blankenship, Robert E., & Jankowiak, Ryszard. Effect of Spectral Density Shapes on the Excitonic Structure and Dynamics of the Fenna–Matthews–Olson Trimer from Chlorobaculum tepidum. United States. https://doi.org/10.1021/acs.jpca.6b03107
Copy to clipboard
Kell, Adam, Blankenship, Robert E., and Jankowiak, Ryszard. Wed . "Effect of Spectral Density Shapes on the Excitonic Structure and Dynamics of the Fenna–Matthews–Olson Trimer from Chlorobaculum tepidum". United States. https://doi.org/10.1021/acs.jpca.6b03107. https://www.osti.gov/servlets/purl/1387903.
Copy to clipboard
@article{osti_1387903,
title = {Effect of Spectral Density Shapes on the Excitonic Structure and Dynamics of the Fenna–Matthews–Olson Trimer from Chlorobaculum tepidum},
author = {Kell, Adam and Blankenship, Robert E. and Jankowiak, Ryszard},
abstractNote = {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.},
doi = {10.1021/acs.jpca.6b03107},
journal = {Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory},
number = 31,
volume = 120,
place = {United States},
year = {Wed Jul 20 00:00:00 EDT 2016},
month = {Wed Jul 20 00:00:00 EDT 2016}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/acs.jpca.6b03107
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 25 works
Citation information provided by
Web of Science
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

The FMO Protein
journal, January 2004

Revisiting the optical properties of the FMO protein
journal, March 2010

  • Milder, Maaike T. W.; Brüggemann, Ben; van Grondelle, Rienk
  • Photosynthesis Research, Vol. 104, Issue 2-3
  • DOI: 10.1007/s11120-010-9540-1

Chlorophyll arrangement in a bacteriochlorophyll protein from Chlorobium limicola
journal, December 1975

  • Fenna, R. E.; Matthews, B. W.
  • Nature, Vol. 258, Issue 5536
  • DOI: 10.1038/258573a0

The structural basis for the difference in absorbance spectra for the FMO antenna protein from various green sulfur bacteria
journal, May 2009

The three-dimensional structure of the FMO protein from Pelodictyon phaeum and the implications for energy transfer
journal, December 2010

  • Larson, Chadwick R.; Seng, Chenda O.; Lauman, Lisa
  • Photosynthesis Research, Vol. 107, Issue 2
  • DOI: 10.1007/s11120-010-9604-2

Reinterpretation of the electron density at the site of the eighth bacteriochlorophyll in the FMO protein from Pelodictyon phaeum
journal, March 2012

Evolution of photosystem I - from symmetry through pseudosymmetry to asymmetry
journal, March 2004

Native Electrospray Mass Spectrometry Reveals the Nature and Stoichiometry of Pigments in the FMO Photosynthetic Antenna Protein
journal, May 2011

  • Wen, Jianzhong; Zhang, Hao; Gross, Michael L.
  • Biochemistry, Vol. 50, Issue 17
  • DOI: 10.1021/bi200239k

Contribution of bacteriochlorophyll conformation to the distribution of site-energies in the FMO protein
journal, April 2016

  • MacGowan, Stuart A.; Senge, Mathias O.
  • Biochimica et Biophysica Acta (BBA) - Bioenergetics, Vol. 1857, Issue 4
  • DOI: 10.1016/j.bbabio.2016.02.001

Multireference Excitation Energies for Bacteriochlorophylls A within Light Harvesting System 2
journal, February 2016

  • Anda, André; Hansen, Thorsten; De Vico, Luca
  • Journal of Chemical Theory and Computation, Vol. 12, Issue 3
  • DOI: 10.1021/acs.jctc.5b01104

Oscillating anisotropies in a bacteriochlorophyll protein: Evidence for quantum beating between exciton levels
journal, November 1997

Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems
journal, April 2007

  • Engel, Gregory S.; Calhoun, Tessa R.; Read, Elizabeth L.
  • Nature, Vol. 446, Issue 7137
  • DOI: 10.1038/nature05678

Long-lived quantum coherence in photosynthetic complexes at physiological temperature
journal, July 2010

  • Panitchayangkoon, G.; Hayes, D.; Fransted, K. A.
  • Proceedings of the National Academy of Sciences, Vol. 107, Issue 29
  • DOI: 10.1073/pnas.1005484107

Zwischenmolekulare Energiewanderung und Fluoreszenz
journal, January 1948

On the Theory of Relaxation Processes
journal, January 1957

  • Redfield, A. G.
  • IBM Journal of Research and Development, Vol. 1, Issue 1
  • DOI: 10.1147/rd.11.0019

The Theory of Relaxation Processes
book, January 1965

How Proteins Trigger Excitation Energy Transfer in the FMO Complex of Green Sulfur Bacteria
journal, October 2006

Calculation of pigment transition energies in the FMO protein: From simplicity to complexity and back
journal, October 2007

  • Adolphs, Julian; Müh, Frank; Madjet, Mohamed El-Amine
  • Photosynthesis Research, Vol. 95, Issue 2-3
  • DOI: 10.1007/s11120-007-9248-z

The Eighth Bacteriochlorophyll Completes the Excitation Energy Funnel in the FMO Protein
journal, December 2010

  • Schmidt am Busch, Marcel; Müh, Frank; El-Amine Madjet, Mohamed
  • The Journal of Physical Chemistry Letters, Vol. 2, Issue 2
  • DOI: 10.1021/jz101541b

Exciton Analysis in 2D Electronic Spectroscopy
journal, June 2005

  • Cho, Minhaeng; Vaswani, Harsha M.; Brixner, Tobias
  • The Journal of Physical Chemistry B, Vol. 109, Issue 21
  • DOI: 10.1021/jp050788d

Correlated driving and dissipation in two-dimensional spectroscopy
journal, January 2013

  • Xu, Jian; Zhang, Hou-Dao; Xu, Rui-Xue
  • The Journal of Chemical Physics, Vol. 138, Issue 2
  • DOI: 10.1063/1.4773472

An efficient method to calculate excitation energy transfer in light-harvesting systems: application to the Fenna–Matthews–Olson complex
journal, November 2011

Absence of Quantum Oscillations and Dependence on Site Energies in Electronic Excitation Transfer in the Fenna–Matthews–Olson Trimer
journal, October 2011

  • Ritschel, Gerhard; Roden, Jan; Strunz, Walter T.
  • The Journal of Physical Chemistry Letters, Vol. 2, Issue 22
  • DOI: 10.1021/jz201119j

Efficient and accurate simulations of two-dimensional electronic photon-echo signals: Illustration for a simple model of the Fenna–Matthews–Olson complex
journal, January 2010

  • Sharp, Leah Z.; Egorova, Dassia; Domcke, Wolfgang
  • The Journal of Chemical Physics, Vol. 132, Issue 1
  • DOI: 10.1063/1.3268705

Theoretical examination of quantum coherence in a photosynthetic system at physiological temperature
journal, October 2009

  • Ishizaki, A.; Fleming, G. R.
  • Proceedings of the National Academy of Sciences, Vol. 106, Issue 41
  • DOI: 10.1073/pnas.0908989106

Simulation of the two-dimensional electronic spectra of the Fenna-Matthews-Olson complex using the hierarchical equations of motion method
journal, May 2011

  • Chen, Liping; Zheng, Renhui; Jing, Yuanyuan
  • The Journal of Chemical Physics, Vol. 134, Issue 19
  • DOI: 10.1063/1.3589982

Modelling of oscillations in two-dimensional echo-spectra of the Fenna–Matthews–Olson complex
journal, February 2012

Long-Lived Electronic Coherence in Dissipative Exciton Dynamics of Light-Harvesting Complexes
journal, September 2012

  • Kreisbeck, Christoph; Kramer, Tobias
  • The Journal of Physical Chemistry Letters, Vol. 3, Issue 19
  • DOI: 10.1021/jz3012029

Exciton transfer dynamics and quantumness of energy transfer in the Fenna-Matthews-Olson complex
journal, October 2011

On the Controversial Nature of the 825 nm Exciton Band in the FMO Protein Complex
journal, March 2014

  • Kell, Adam; Acharya, Khem; Zazubovich, Valter
  • The Journal of Physical Chemistry Letters, Vol. 5, Issue 8
  • DOI: 10.1021/jz5001165

Modeling of Various Optical Spectra in the Presence of Slow Excitation Energy Transfer in Dimers and Trimers with Weak Interpigment Coupling: FMO as an Example
journal, February 2014

  • Herascu, Nicoleta; Kell, Adam; Acharya, Khem
  • The Journal of Physical Chemistry B, Vol. 118, Issue 8
  • DOI: 10.1021/jp410586f

On destabilization of the Fenna–Matthews–Olson complex of Chlorobaculum tepidum
journal, March 2014

  • Kell, Adam; Acharya, Khem; Blankenship, Robert E.
  • Photosynthesis Research, Vol. 120, Issue 3
  • DOI: 10.1007/s11120-014-9990-y

Light Harvesting in Photosystem II Core Complexes Is Limited by the Transfer to the Trap:  Can the Core Complex Turn into a Photoprotective Mode?
journal, April 2008

  • Raszewski, Grzegorz; Renger, Thomas
  • Journal of the American Chemical Society, Vol. 130, Issue 13
  • DOI: 10.1021/ja7099826

On the Shape of the Phonon Spectral Density in Photosynthetic Complexes
journal, June 2013

  • Kell, Adam; Feng, Ximao; Reppert, Mike
  • The Journal of Physical Chemistry B, Vol. 117, Issue 24
  • DOI: 10.1021/jp405094p

Spectral Hole Burning and Fluorescence Line Narrowing in Subunits of the Light-Harvesting Complex LH1 of Purple Bacteria
journal, November 1999

  • Creemers, T. M. H.; De Caro, C. A.; Visschers, R. W.
  • The Journal of Physical Chemistry B, Vol. 103, Issue 44
  • DOI: 10.1021/jp990805x

A Simplex Method for Function Minimization
journal, January 1965

Exciton Dynamics in FMO Bacteriochlorophyll Protein at Low Temperatures
journal, September 1997

  • Freiberg, Arvi; Lin, Su; Timpmann, Kõu
  • The Journal of Physical Chemistry B, Vol. 101, Issue 37
  • DOI: 10.1021/jp9633761

Toward Level-to-Level Energy Transfers in Photosynthesis:  The Fenna−Matthews−Olson Protein
journal, July 1998

  • Savikhin, Sergei; Buck, Daniel R.; Struve, Walter S.
  • The Journal of Physical Chemistry B, Vol. 102, Issue 29
  • DOI: 10.1021/jp981186f

Excited-State Structure and Dynamics in FMO Antenna Complexes from Photosynthetic Green Sulfur Bacteria
journal, December 1998

  • Vulto, Simone I. E.; Neerken, Sieglinde; Louwe, Robert J. W.
  • The Journal of Physical Chemistry B, Vol. 102, Issue 51
  • DOI: 10.1021/jp983003v

Liquid Fragility and the Glass Transition in Water and Aqueous Solutions
journal, August 2002

The ‘glass transition’ in protein dynamics: what it is, why it occurs, and how to exploit it
journal, September 2003

Exciton interaction among chlorophyll molecules in bacteriochlorophyll a proteins and bacteriochlorophyll a reaction center complexes from green bacteria
journal, June 1976

  • Olson, John M.; Ke, Bacon; Thompson, Keith H.
  • Biochimica et Biophysica Acta (BBA) - Bioenergetics, Vol. 430, Issue 3
  • DOI: 10.1016/0005-2728(76)90028-1

Exciton Simulations of Optical Spectra of the FMO Complex from the Green Sulfur Bacterium Chlorobium tepidum at 6 K
journal, November 1998

  • Vulto, Simone I. E.; de Baat, Michiel A.; Louwe, Robert J. W.
  • The Journal of Physical Chemistry B, Vol. 102, Issue 47
  • DOI: 10.1021/jp982095l

The Fate of the Triplet Excitations in the Fenna–Matthews–Olson Complex
journal, April 2015

  • Kihara, Shigeharu; Hartzler, Daniel A.; Orf, Gregory S.
  • The Journal of Physical Chemistry B, Vol. 119, Issue 18
  • DOI: 10.1021/jp512222c

Intensity Dependence of the Excited State Lifetimes and Triplet Conversion Yield in the Fenna–Matthews–Olson Antenna Protein
journal, February 2014

  • Orf, Gregory S.; Niedzwiedzki, Dariusz M.; Blankenship, Robert E.
  • The Journal of Physical Chemistry B, Vol. 118, Issue 8
  • DOI: 10.1021/jp411020a

From Atomistic Modeling to Excitation Transfer and Two-Dimensional Spectra of the FMO Light-Harvesting Complex
journal, July 2011

  • Olbrich, Carsten; Jansen, Thomas L. C.; Liebers, Jörg
  • The Journal of Physical Chemistry B, Vol. 115, Issue 26
  • DOI: 10.1021/jp202619a

Membrane orientation of the FMO antenna protein from Chlorobaculum tepidum as determined by mass spectrometry-based footprinting
journal, April 2009

  • Wen, J.; Zhang, H.; Gross, M. L.
  • Proceedings of the National Academy of Sciences, Vol. 106, Issue 15
  • DOI: 10.1073/pnas.0901691106

 -Helices direct excitation energy flow in the Fenna Matthews Olson protein
journal, October 2007

  • Muh, F.; Madjet, M. E. -A.; Adolphs, J.
  • Proceedings of the National Academy of Sciences, Vol. 104, Issue 43
  • DOI: 10.1073/pnas.0708222104

Chemical oxidation of the FMO antenna protein from Chlorobaculum tepidum
journal, July 2013

Spectral shift mechanisms of chlorophylls in liquids and proteins
journal, February 2013

  • Renge, Indrek; Mauring, Koit
  • Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, Vol. 102
  • DOI: 10.1016/j.saa.2012.10.034

Alternative Excitonic Structure in the Baseplate (BChl a –CsmA Complex) of the Chlorosome from Chlorobaculum tepidum
journal, June 2015

  • Kell, Adam; Chen, Jinhai; Jassas, Mahboobe
  • The Journal of Physical Chemistry Letters, Vol. 6, Issue 14
  • DOI: 10.1021/acs.jpclett.5b01074

Efficient Energy Transfer in Light-Harvesting Systems, III: The Influence of the Eighth Bacteriochlorophyll on the Dynamics and Efficiency in FMO
journal, November 2011

  • Moix, Jeremy; Wu, Jianlan; Huo, Pengfei
  • The Journal of Physical Chemistry Letters, Vol. 2, Issue 24
  • DOI: 10.1021/jz201259v

Atomistic Study of Energy Funneling in the Light-Harvesting Complex of Green Sulfur Bacteria
journal, January 2014

  • Huh, Joonsuk; Saikin, Semion K.; Brookes, Jennifer C.
  • Journal of the American Chemical Society, Vol. 136, Issue 5
  • DOI: 10.1021/ja412035q

Dynamics of Energy and Electron Transfer in the FMO-Reaction Center Core Complex from the Phototrophic Green Sulfur Bacterium Chlorobaculum tepidum
journal, June 2015

  • He, Guannan; Niedzwiedzki, Dariusz M.; Orf, Gregory S.
  • The Journal of Physical Chemistry B, Vol. 119, Issue 26
  • DOI: 10.1021/acs.jpcb.5b04170

Fast Energy Transfer and Exciton Dynamics in Chlorosomes of the Green Sulfur Bacterium Chlorobium tepidum
journal, June 1998

  • Pšenčík, Jakub; Polívka, Tomáš; Němec, Petr
  • The Journal of Physical Chemistry A, Vol. 102, Issue 23
  • DOI: 10.1021/jp973227y

Theory and Simulation of the Environmental Effects on FMO Electronic Transitions
journal, June 2011

  • Olbrich, Carsten; Strümpfer, Johan; Schulten, Klaus
  • The Journal of Physical Chemistry Letters, Vol. 2, Issue 14
  • DOI: 10.1021/jz2007676

Influence of Site-Dependent Pigment–Protein Interactions on Excitation Energy Transfer in Photosynthetic Light Harvesting
journal, April 2013

  • Rivera, Eva; Montemayor, Daniel; Masia, Marco
  • The Journal of Physical Chemistry B, Vol. 117, Issue 18
  • DOI: 10.1021/jp4011586

Influence of Force Fields and Quantum Chemistry Approach on Spectral Densities of BChl a in Solution and in FMO Proteins
journal, July 2015

  • Chandrasekaran, Suryanarayanan; Aghtar, Mortaza; Valleau, Stéphanie
  • The Journal of Physical Chemistry B, Vol. 119, Issue 31
  • DOI: 10.1021/acs.jpcb.5b03654
    Sort by:
    [ × clear filter / sort ]

    Works referencing / citing this record:

    On uncorrelated inter-monomer Förster energy transfer in Fenna–Matthews–Olson complexes
    journal, February 2019

    • Kell, Adam; Khmelnitskiy, Anton Yu.; Reinot, Tonu
    • Journal of The Royal Society Interface, Vol. 16, Issue 151
    • DOI: 10.1098/rsif.2018.0882

    Near shot-noise limited time-resolved circular dichroism pump-probe spectrometer
    journal, March 2018

    • Stadnytskyi, Valentyn; Orf, Gregory S.; Blankenship, Robert E.
    • Review of Scientific Instruments, Vol. 89, Issue 3
    • DOI: 10.1063/1.5009468

    Two-dimensional electronic spectra of the photosynthetic apparatus of green sulfur bacteria
    journal, March 2017

    • Kramer, Tobias; Rodriguez, Mirta
    • Scientific Reports, Vol. 7, Issue 1
    • DOI: 10.1038/srep45245
      Sort by:
      [ × clear filter / sort ]

      Similar Records in DOE PAGES and OSTI.GOV collections: