Fluorescence-excitation and Emission Spectroscopy on Single FMO Complexes

Löhner, Alexander; Ashraf , Khuram; Cogdell, Richard J.; Köhler, Jürgen

doi:10.1038/srep31875

Fluorescence-excitation and Emission Spectroscopy on Single FMO Complexes

Journal Article · Mon Aug 22 00:00:00 EDT 2016 · Scientific Reports

DOI:https://doi.org/10.1038/srep31875· OSTI ID:1388571

Löhner, Alexander ^[1]; Ashraf , Khuram ^[2]; Cogdell, Richard J. ^[2]; Köhler, Jürgen ^[1]

Univ. of Bayreuth (Germany)
Univ. of Glasgow, Scotland (United Kingdom)

In green-sulfur bacteria sunlight is absorbed by antenna structures termed chlorosomes, and transferred to the RC via the Fenna-Matthews-Olson (FMO) complex. FMO consists of three monomers arranged in C₃ symmetry where each monomer accommodates eight Bacteriochlorophyll a (BChl a) molecules. It was the first pigment-protein complex for which the structure has been determined with high resolution and since then this complex has been the subject of numerous studies both experimentally and theoretically. Here we report about fluorescence-excitation spectroscopy as well as emission spectroscopy from individual FMO complexes at low temperatures. The individual FMO complexes are subjected to very fast spectral fluctuations smearing out any possible different information from the ensemble data that were recorded under the same experimental conditions. In other words, on the time scales that are experimentally accessible by single-molecule techniques, the FMO complex exhibits ergodic behaviour.

View Accepted Manuscript (DOE)

Research Organization:: Washington Univ., St. Louis, MO (United States). Energy Frontier Research Center (EFRC) Photosynthetic Antenna Research Center (PARC)

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

Grant/Contract Number:: SC0001035

OSTI ID:: 1388571

Journal Information:: Scientific Reports, Journal Name: Scientific Reports Journal Issue: 1 Vol. 6; ISSN 2045-2322

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

References (42)

Crystal structure of the bacteriochlorophyll a protein from Chlorobium tepidum 1 1Edited by R. Huber Li, Yi-Fen; Zhou, Wenli; Blankenship, Robert E. Journal of Molecular Biology, Vol. 271, Issue 3 https://doi.org/10.1006/jmbi.1997.1189	journal	August 1997
A thermophilic green sulfur bacterium from New Zealand hot springs, Chlorobium tepidum sp. nov. Wahlund, Thomas M.; Woese, Carl R.; Castenholz, Richard W. Archives of Microbiology, Vol. 156, Issue 2 https://doi.org/10.1007/BF00290978	journal	August 1991
Sulfur oxidation in mutants of the photosynthetic green sulfur bacterium Chlorobium tepidum devoid of cytochrome c-554 and SoxB Azai, Chihiro; Tsukatani, Yusuke; Harada, Jiro Photosynthesis Research, Vol. 100, Issue 2 https://doi.org/10.1007/s11120-009-9426-2	journal	May 2009
Spectral hole burning: examples from photosynthesis Purchase, Robin; Völker, Silvia Photosynthesis Research, Vol. 101, Issue 2-3 https://doi.org/10.1007/s11120-009-9484-5	journal	August 2009
Revisiting the optical properties of the FMO protein Milder, Maaike T. W.; Brüggemann, Ben; van Grondelle, Rienk Photosynthesis Research, Vol. 104, Issue 2-3 https://doi.org/10.1007/s11120-010-9540-1	journal	March 2010
Energy transfer dynamics of the B800—B850 antenna complex of Rhodobacter sphaeroides: a hole burning study Reddy, N. R. S.; Small, G. J.; Seibert, M. Chemical Physics Letters, Vol. 181, Issue 5 https://doi.org/10.1016/0009-2614(91)90369-K	journal	July 1991
Two molecules of cytochrome c function as the electron donors to P840 in the reaction center complex isolated from a green sulfur bacterium, Chlorobium tepidum Oh-oka, Hirozo; Kamei, Shoichiro; Matsubara, Hiroshi FEBS Letters, Vol. 365, Issue 1 https://doi.org/10.1016/0014-5793(95)00433-A	journal	May 1995
Spectral hole burning in pigment-protein complexes of photosynthetic bacteria De Caro, C.; Visschers, R. W.; van Grondelle, R. Journal of Luminescence, Vol. 58, Issue 1-6 https://doi.org/10.1016/0022-2313(94)90383-2	journal	January 1994
Structure of a bacteriochlorophyll a-protein from the green photosynthetic bacterium Prosthecochloris aestuarii Matthews, B. W.; Fenna, R. E.; Bolognesi, M. C. Journal of Molecular Biology, Vol. 131, Issue 2 https://doi.org/10.1016/0022-2836(79)90076-7	journal	June 1979
Femtosecond energy transfer and spectral equilibration in bacteriochlorophyll a--protein antenna trimers from the green bacterium Chlorobium tepidum Savikhin, S.; Zhou, W.; Blankenship, R. E. Biophysical Journal, Vol. 66, Issue 1 https://doi.org/10.1016/S0006-3495(94)80769-6	journal	January 1994
Resonant emission from the B870 exciton state and electron–phonon coupling in the LH2 antenna chromoprotein Rätsep, Margus; Freiberg, Arvi Chemical Physics Letters, Vol. 377, Issue 3-4 https://doi.org/10.1016/S0009-2614(03)01193-X	journal	August 2003
Evolution of photosystem I - from symmetry through pseudosymmetry to asymmetry Ben-Shem, Adam; Frolow, Felix; Nelson, Nathan FEBS Letters, Vol. 564, Issue 3 https://doi.org/10.1016/S0014-5793(04)00360-6	journal	March 2004
The Structure and Thermal Motion of the B800–850 LH2 Complex from Rps.acidophila at 2.0Å Resolution and 100K: New Structural Features and Functionally Relevant Motions Papiz, Miroslav Z.; Prince, Steve M.; Howard, Tina Journal of Molecular Biology, Vol. 326, Issue 5 https://doi.org/10.1016/S0022-2836(03)00024-X	journal	March 2003
Structure of the photosynthetic reaction centre from Rhodobacter sphaeroides at 2.65 å resolution: cofactors and protein-cofactor interactions Ermler, Ulrich; Fritzsch, Günter; Buchanan, Susan K. Structure, Vol. 2, Issue 10 https://doi.org/10.1016/S0969-2126(94)00094-8	journal	October 1994
Red antenna states of Photosystem I trimers from Arthrospira platensis revealed by single-molecule spectroscopy Brecht, Marc; Hussels, Martin; Schlodder, Eberhard Biochimica et Biophysica Acta (BBA) - Bioenergetics, Vol. 1817, Issue 3 https://doi.org/10.1016/j.bbabio.2011.11.012	journal	March 2012
The architecture and function of the light-harvesting apparatus of purple bacteria: from single molecules to in vivo membranes Cogdell, Richard J.; Gall, Andrew; Köhler, Jürgen Quarterly Reviews of Biophysics, Vol. 39, Issue 3 https://doi.org/10.1017/S0033583506004434	journal	August 2006
Ultrafast Energy Transfer in FMO Trimers from the Green Bacterium Chlorobium tepidum Savikhin, Sergei; Struve, Walter S. Biochemistry, Vol. 33, Issue 37 https://doi.org/10.1021/bi00203a016	journal	September 1994
Singlet−Singlet Annihilation and Local Heating in FMO Complexes Gulbinas, Vidmantas; Valkunas, Leonas; Kuciauskas, Darius The Journal of Physical Chemistry, Vol. 100, Issue 45 https://doi.org/10.1021/jp961272k	journal	January 1996
Atmospheric Lifetimes and Global Warming Potentials of Hydrofluoroethers: Reactivity toward OH, UV Spectra, and IR Absorption Cross Sections Orkin, Vladimir L.; Villenave, Eric; Huie, Robert E. The Journal of Physical Chemistry A, Vol. 103, Issue 48 https://doi.org/10.1021/jp991741t	journal	December 1999
Chlorophyll arrangement in a bacteriochlorophyll protein from Chlorobium limicola Fenna, R. E.; Matthews, B. W. Nature, Vol. 258, Issue 5536 https://doi.org/10.1038/258573a0	journal	December 1975
Structure of the protein subunits in the photosynthetic reaction centre of Rhodopseudomonas viridis at 3Å resolution Deisenhofer, J.; Epp, O.; Miki, K. Nature, Vol. 318, Issue 6047 https://doi.org/10.1038/318618a0	journal	December 1985
Crystal structure of photosystem II from Synechococcus elongatus at 3.8 Å resolution Zouni, Athina; Witt, Horst-Tobias; Kern, Jan Nature, Vol. 409, Issue 6821 https://doi.org/10.1038/35055589	journal	February 2001
Three-dimensional structure of cyanobacterial photosystem I at 2.5 Å resolution Jordan, Patrick; Fromme, Petra; Witt, Horst Tobias Nature, Vol. 411, Issue 6840 https://doi.org/10.1038/35082000	journal	June 2001
Crystal structure of an integral membrane light-harvesting complex from photosynthetic bacteria McDermott, G.; Prince, S. M.; Freer, A. A. Nature, Vol. 374, Issue 6522 https://doi.org/10.1038/374517a0	journal	April 1995
Two-dimensional spectroscopy of electronic couplings in photosynthesis Brixner, Tobias; Stenger, Jens; Vaswani, Harsha M. Nature, Vol. 434, Issue 7033 https://doi.org/10.1038/nature03429	journal	March 2005
Towards complete cofactor arrangement in the 3.0 Å resolution structure of photosystem II Loll, Bernhard; Kern, Jan; Saenger, Wolfram Nature, Vol. 438, Issue 7070 https://doi.org/10.1038/nature04224	journal	December 2005
Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems Engel, Gregory S.; Calhoun, Tessa R.; Read, Elizabeth L. Nature, Vol. 446, Issue 7137 https://doi.org/10.1038/nature05678	journal	April 2007
The structure of a plant photosystem I supercomplex at 3.4 Å resolution Amunts, Alexey; Drory, Omri; Nelson, Nathan Nature, Vol. 447, Issue 7140 https://doi.org/10.1038/nature05687	journal	May 2007
Coherently wired light-harvesting in photosynthetic marine algae at ambient temperature Collini, Elisabetta; Wong, Cathy Y.; Wilk, Krystyna E. Nature, Vol. 463, Issue 7281 https://doi.org/10.1038/nature08811	journal	February 2010
Proposal for probing energy transfer pathway by single-molecule pump-dump experiment Tao, Ming-Jie; Ai, Qing; Deng, Fu-Guo Scientific Reports, Vol. 6, Issue 1 https://doi.org/10.1038/srep27535	journal	June 2016
Two-dimensional electronic spectroscopy of the B800-B820 light-harvesting complex Zigmantas, D.; Read, E. L.; Mancal, T. Proceedings of the National Academy of Sciences, Vol. 103, Issue 34 https://doi.org/10.1073/pnas.0602961103	journal	August 2006
Refinement of the x-ray structure of the RC LH1 core complex from Rhodopseudomonas palustris by single-molecule spectroscopy Richter, M. F.; Baier, J.; Southall, J. Proceedings of the National Academy of Sciences, Vol. 104, Issue 51 https://doi.org/10.1073/pnas.0704599105	journal	December 2007
Conformational switching explains the intrinsic multifunctionality of plant light-harvesting complexes Kruger, T. P. J.; Wientjes, E.; Croce, R. Proceedings of the National Academy of Sciences, Vol. 108, Issue 33 https://doi.org/10.1073/pnas.1105411108	journal	August 2011
Quantum coherence spectroscopy reveals complex dynamics in bacterial light-harvesting complex 2 (LH2) Harel, E.; Engel, G. S. Proceedings of the National Academy of Sciences, Vol. 109, Issue 3 https://doi.org/10.1073/pnas.1110312109	journal	January 2012
Spectral dynamics in the B800 band of LH2 from Rhodospirillum molischianum : a single-molecule study Hofmann, Clemens; Aartsma, Thijs J.; Michel, Hartmut New Journal of Physics, Vol. 6 https://doi.org/10.1088/1367-2630/6/1/008	journal	January 2004
Epifluorescence, confocal and total internal reflection microscopy for single-molecule experiments: a quantitative comparison Lang, E.; Baier, J.; Kohler, J. Journal of Microscopy, Vol. 222, Issue 2 https://doi.org/10.1111/j.1365-2818.2006.01579.x	journal	May 2006
Structure-Based Calculations of the Optical Spectra of the LH2 Bacteriochlorophyll-Protein Complex from Rhodopseudomonas acidophila Sauer, Kenneth; Cogdell, Richard J.; Prince, Steve M. Photochemistry and Photobiology, Vol. 64, Issue 3 https://doi.org/10.1111/j.1751-1097.1996.tb03106.x	journal	September 1996
Architecture of the Photosynthetic Oxygen-Evolving Center Ferreira, K. N. Science, Vol. 303, Issue 5665 https://doi.org/10.1126/science.1093087	journal	March 2004
Quantum Coherent Energy Transfer over Varying Pathways in Single Light-Harvesting Complexes Hildner, R.; Brinks, D.; Nieder, J. B. Science, Vol. 340, Issue 6139 https://doi.org/10.1126/science.1235820	journal	June 2013
Unraveling the Electronic Structure of Individual Photosynthetic Pigment-Protein Complexes van Oijen, A. M. Science, Vol. 285, Issue 5426 https://doi.org/10.1126/science.285.5426.400	journal	July 1999
Dynamics of Light Harvesting in Photosynthesis Cheng, Yuan-Chung; Fleming, Graham R. Annual Review of Physical Chemistry, Vol. 60, Issue 1 https://doi.org/10.1146/annurev.physchem.040808.090259	journal	May 2009
Proposal for probing energy transfer pathway by single-molecule pump-dump experiment Tao, Ming-Jie; Ai, Qing; Deng, Fu-Guo arXiv https://doi.org/10.48550/arxiv.1511.01461	text	January 2015

Cited By (5)

Light harvesting in phototrophic bacteria: structure and function Saer, Rafael G.; Blankenship, Robert E. Biochemical Journal, Vol. 474, Issue 13 https://doi.org/10.1042/bcj20160753	journal	June 2017
Single-molecule excitation–emission spectroscopy Thyrhaug, Erling; Krause, Stefan; Perri, Antonio Proceedings of the National Academy of Sciences, Vol. 116, Issue 10 https://doi.org/10.1073/pnas.1808290116	journal	February 2019
Contribution of low-temperature single-molecule techniques to structural issues of pigment–protein complexes from photosynthetic purple bacteria Löhner, Alexander; Cogdell, Richard; Köhler, Jürgen Journal of The Royal Society Interface, Vol. 15, Issue 138 https://doi.org/10.1098/rsif.2017.0680	journal	January 2018
Delocalized excitons in natural light-harvesting complexes Jang, Seogjoo J.; Mennucci, Benedetta Reviews of Modern Physics, Vol. 90, Issue 3 https://doi.org/10.1103/revmodphys.90.035003	journal	August 2018
Delocalized excitons in natural light harvesting complexes Jang, Seogjoo J.; Mennucci, Benedetta arXiv https://doi.org/10.48550/arxiv.1804.09711	text	January 2018

Similar Records

Impact of Single-Point Mutations on the Excitonic Structure and Dynamics in a Fenna–Matthews–Olson Complex

Journal Article · Sun Jun 03 20:00:00 EDT 2018 · Journal of Physical Chemistry Letters · OSTI ID:1539328

Simulated two-dimensional electronic spectroscopy of the eight-bacteriochlorophyll FMO complex

Journal Article · Sat Dec 20 23:00:00 EST 2014 · Journal of Chemical Physics · OSTI ID:22413323

Structural model and spectroscopic characteristics of the FMO antenna protein from the aerobic chlorophototroph, Candidatus Chloracidobacterium thermophilum

Journal Article · · Biochim. Biophys. Acta, Bioenerg. · OSTI ID:1065089

Related Subjects

59 BASIC BIOLOGICAL SCIENCES

Fluorescence-excitation and Emission Spectroscopy on Single FMO Complexes

Citation Formats

References (42)

Cited By (5)

Similar Records

Related Subjects