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Title: Ultrafast energy relaxation in single light-harvesting complexes

Journal Article · · Proceedings of the National Academy of Sciences of the United States of America
 [1];  [2];  [3];  [4];  [2]
  1. Department of Physics and Astronomy, Faculty of Sciences, Vrije Universiteit Amsterdam, 1081HV Amsterdam, The Netherlands,, Institute of Physics, Faculty of Mathematics and Physics, Charles University in Prague, 121 16 Prague, Czech Republic,
  2. Department of Physics and Astronomy, Faculty of Sciences, Vrije Universiteit Amsterdam, 1081HV Amsterdam, The Netherlands,
  3. Institute of Molecular, Cellular and Systems Biology, College of Medical, Veterinary and Life Sciences, University of Glasgow, Glasgow G128QQ, United Kingdom
  4. Institute of Physics, Faculty of Mathematics and Physics, Charles University in Prague, 121 16 Prague, Czech Republic,

Significance The excitation energy transfer in light-harvesting complexes is usually studied either by ultrafast bulk spectroscopy or by single-molecule spectroscopy. These methods are to a high degree complementary: Bulk spectroscopy measures ultrafast processes averaged over thousands of complexes, whereas single-molecule spectroscopy observes much slower dynamics in individual complexes. In this work, we combine these approaches using a recently developed ultrafast single-molecule spectroscopy technique. This enables us, for the first time (to our knowledge), to observe ultrafast energy relaxation with a rate around 100 fs in individual light-harvesting complexes. We determine the distribution of the relaxation times, observe changes of the relaxation time in one complex, and find how the relaxation depends on excitation wavelength.

Sponsoring Organization:
USDOE
Grant/Contract Number:
SC0001035
OSTI ID:
1238807
Journal Information:
Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 11 Vol. 113; ISSN 0027-8424
Publisher:
Proceedings of the National Academy of SciencesCopyright Statement
Country of Publication:
United States
Language:
English

References (33)

Molecular Mechanisms of Photosynthesis book December 2002
Size and structure of antenna complexes of photosynthetic bacteria as studied by singlet-singlet quenching of the bacteriochlorophyll fluorescence yield journal April 1983
Energy transfer dynamics of isolated B800–850 and B800–820 pigment-protein complexes of Rhodobacter sphaeroides and Rhodopseudomonas acidophila journal October 1988
Femtosecond energy transfer within the LH2 peripheral antenna of the photosynthetic purple bacteria Rhodobacter sphaeroides and Rhodopseudomonas palustris LL journal December 1993
Spectroscopy of Individual Light-Harvesting 2 Complexes of Rhodopseudomonas acidophila: Diagonal Disorder, Intercomplex Heterogeneity, Spectral Diffusion, and Energy Transfer in the B800 Band journal March 2000
Low-Intensity Pump-Probe Measurements on the B800 Band of Rhodospirillum molischianum journal January 2003
Fluorescence Spectral Dynamics of Single LHCII Trimers journal June 2010
Fluorescence Spectral Fluctuations of Single LH2 Complexes from Rhodopseudomonas acidophila Strain 10050 journal April 2004
Inter- and Intraband Energy Transfer in LH2-Antenna Complexes of Purple Bacteria. A Fluorescence Line-Narrowing and Hole-Burning Study journal October 1994
Intra- and Interband Transfers in the B800−B850 Antenna of Rhodospirillum m olischianum :  Redfield Theory Modeling of Polarized Pump−Probe Kinetics journal October 2003
Pathways of Energy Flow in LHCII from Two-Dimensional Electronic Spectroscopy journal November 2009
Electronic Excitation Transfer in the LH2 Complex of Rhodobacter sphaeroides journal January 1996
Energy Transfer and Exciton Annihilation in the B800−850 Antenna Complex of the Photosynthetic Purple Bacterium Rhodopseudomonas acidophila (Strain 10050). A Femtosecond Transient Absorption Study journal February 1997
Enzymatic Oxygen Scavenging for Photostability without pH Drop in Single-Molecule Experiments journal June 2012
Two-dimensional spectroscopy of electronic couplings in photosynthesis journal March 2005
Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems journal April 2007
Dynamic localization of electronic excitation in photosynthetic complexes revealed with chiral two-dimensional spectroscopy journal February 2014
Ultrafast dynamics of single molecules journal January 2014
Characterization of electronic transitions in complex molecules journal January 1950
Single-molecule pump-probe experiments reveal variations in ultrafast energy redistribution journal August 2005
Ultra-broadband 2D electronic spectroscopy of carotenoid-bacteriochlorophyll interactions in the LH1 complex of a purple bacterium journal April 2015
Two-dimensional electronic spectroscopy of the B800-B820 light-harvesting complex journal August 2006
Conformational switching explains the intrinsic multifunctionality of plant light-harvesting complexes journal August 2011
Quantum coherence spectroscopy reveals complex dynamics in bacterial light-harvesting complex 2 (LH2) journal January 2012
Single-molecule spectroscopy reveals photosynthetic LH2 complexes switch between emissive states journal June 2013
Exciton dynamics in photosynthetic complexes: excitation by coherent and incoherent light journal June 2010
Determination of the Spectral Diffusion Kernel of a Protein by Single-Molecule Spectroscopy journal January 2008
Single-Molecule Pump-Probe Detection Resolves Ultrafast Pathways in Individual and Coupled Quantum Systems journal February 2005
Effect of Disorder on Ultrafast Exciton Dynamics Probed by Single Molecule Spectroscopy journal November 2006
Quantum Coherent Energy Transfer over Varying Pathways in Single Light-Harvesting Complexes journal June 2013
Control and measurement of ultrashort pulse shapes (in amplitude and phase) with femtosecond accuracy journal January 1985
Measurement of group delay dispersion of high numerical aperture objective lenses using two-photon excited fluorescence journal January 1997
Spectral Trends in the Fluorescence of Single Bacterial Light-Harvesting Complexes: Experiments and Modified Redfield Simulations journal April 2006

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