Cited by 46Spectroscopy and Quantum Chemical StudiesPhotochemistry and Electron Transfer StudiesPhotosynthetic Processes and Mechanisms

Ultrafast energy relaxation in single light-harvesting complexes

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Malý, Pavel, Gruber, J. Michael, Cogdell, Richard J., Mančal, Tomáš, van Grondelle, Rienk·2016·Proceedings of the National Academy of Sciences

Abstract

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.

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  • Developments in experimental techniques such as ultrafast spectroscopy, single molecule spectroscopy, time-resolved microscopy and single particle imaging have enabled study of biological dynamics on increasingly small length and time scales, revealing processes necessary for living function that depend on a delicate interplay between quantum and classical physical effects.

    “Recently, developments in experimental techniques such as ultrafast spectroscopy [6], single molecule spectroscopy [7 -11], timeresolved microscopy [12 -14] and single particle imaging [15 -18] have enabled us to study biological dynamics on increasingly small length and time scales, revealing a variety of processes necessary for the function of the living system that depend on a delicate interpl”

    From The future of quantum biology (2018) · cites this paper as [11]

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  1. [33]Loudon, R. (2001) The Quantum Theory of Light . (Oxford University Press, New York), 3rd edition, pp. 68-72.

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Authors
Malý, P., Gruber, J. M., Cogdell, R. J., Mančal, T., & van Grondelle, R.
Affiliations
  • Charles University (CZ)
  • Department of Physics and Astronomy, Faculty of Sciences, Vrije Universiteit Amsterdam, 1081HV Amsterdam, The Netherlands;
Venue
Proceedings of the National Academy of Sciences
Published
2016-02-22
Volume
113
Issue
11
Pages
2934-2939
ISSN
  • 0027-8424 (ISSN-L)
  • 1091-6490
OpenAlex
W2280431368
Cited by
46
References
34
Citations by year
2026: 2 · 2025: 3 · 2024: 5 · 2023: 7 · 2022: 5 · 2021: 6 · 2020: 4 · 2019: 2 · 2018: 6 · 2017: 5 · 2016: 1
FWCI
2.21
Type
journal article
Language
en
Open access
Locations
  • Proceedings of the National Academy of Sciences (publishedVersion)
  • PubMed Central (publishedVersion)
  • PubMed (publishedVersion)
  • VU Research Portal (publishedVersion, other-oa)
  • arXiv (Cornell University) (submittedVersion)
  • OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
  • Data Archiving and Networked Services (DANS) (submittedVersion, other-oa)
  • arXiv (Cornell University)
Funders
  • EC | European Research Council (267333)
  • Nederlandse Organisatie voor Wetenschappelijk Onderzoek (700.58.305)
  • Seventh Framework Programme (GA 323901)
  • Czech Science Foundation (14-25752S)
  • U.S. Department of Energy (DE-SC0001035)
Topics
  • Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Spectroscopy and Quantum Chemical Studies
  • Physical Sciences › Chemistry › Physical and Theoretical Chemistry › Photochemistry and Electron Transfer Studies
  • Life Sciences › Biochemistry, Genetics and Molecular Biology › Molecular Biology › Photosynthetic Processes and Mechanisms
Keywords
light-harvesting complexes, LH2, purple bacteria, single-molecule fluorescence spectroscopy, pump-probe spectroscopy, distribution of relaxation times, Redfield theory, Gaussian disorder, ergodicity, excited states
MeSH terms
Bacteriochlorophylls, Energy Transfer, Lasers, Light, Rhodopseudomonas, Spectrometry, Fluorescence, Time, Normal Distribution, Microscopy, Confocal, Statistics, Nonparametric, Light-Harvesting Protein Complexes

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