Ultrafast energy relaxation in single light-harvesting complexes
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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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Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems
Engel, G. S., Calhoun, T. R., Read, E. L., Ahn, T.-K., Mančal, T., Cheng, Y.-C., Blankenship, R. E., & Fleming, G. R. (2007) · Nature · doi:10.1038/nature05678 · Cited by 3,315 · see citing works
Self-citationCharacterization of electronic transitions in complex molecules
Kasha, M. (1950) · Discussions of the Faraday Society · doi:10.1039/df9500900014 · Cited by 2,939 · see citing works
Molecular Mechanisms of Photosynthesis
Blankenship, R. E. (2002) · Wiley eBooks · doi:10.1002/9780470758472 · Cited by 2,394 · see citing works
Two-dimensional spectroscopy of electronic couplings in photosynthesis
Brixner, T., Stenger, J., Vaswani, H. M., Cho, M., Blankenship, R. E., & Fleming, G. R. (2005) · Nature · doi:10.1038/nature03429 · Cited by 1,241 · see citing works
Sundström, V., Pullerits, T., & van Grondelle, R. (1999) · The Journal of Physical Chemistry B · doi:10.1021/jp983722+ · Cited by 817 · see citing works
Diels, J.-C. M., Fontaine, J. J., McMichael, I. C., et al. (1985) · Applied Optics · doi:10.1364/ao.24.001270 · Cited by 471 · see citing works
Quantum Coherent Energy Transfer over Varying Pathways in Single Light-Harvesting Complexes
Hildner, R., Brinks, D., Nieder, J. B., Cogdell, R. J., & van Hulst, N. F. (2013) · Science · doi:10.1126/science.1235820 · Cited by 351 · see citing works
Self-citationElectronic Excitation Transfer in the LH2 Complex ofRhodobacter sphaeroides
Jimenez, R., Dikshit, S. N., Bradforth, S. E., & Fleming, G. R. (1996) · The Journal of Physical Chemistry · doi:10.1021/jp953074j · Cited by 311 · see citing works
Two-dimensional electronic spectroscopy of the B800–B820 light-harvesting complex
Zigmantas, D., Read, E. L., Mančal, T., Brixner, T., Gardiner, A. T., Cogdell, R. J., & Fleming, G. R. (2006) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.0602961103 · Cited by 216 · see citing works
Self-citationEnzymatic Oxygen Scavenging for Photostability without pH Drop in Single-Molecule Experiments
Swoboda, M., Henig, J., Cheng, H., Brugger, D., Haltrich, D., Plumeré, N., & Schlierf, M. (2012) · ACS Nano · doi:10.1021/nn301895c · Cited by 214 · see citing works
Pathways of Energy Flow in LHCII from Two-Dimensional Electronic Spectroscopy
Schlau-Cohen, G. S., Calhoun, T. R., Ginsberg, N. S., Read, E. L., Ballottari, M., Bassi, R., van Grondelle, R., & Fleming, G. R. (2009) · The Journal of Physical Chemistry B · doi:10.1021/jp9066586 · Cited by 203 · see citing works
Harel, E., & Engel, G. S. (2012) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.1110312109 · Cited by 191 · see citing works
Fluorescence Spectral Dynamics of Single LHCII Trimers
Krüger, T. P. J., Novoderezhkin, V. I., Ilioaia, C., & van Grondelle, R. (2010) · Biophysical Journal · doi:10.1016/j.bpj.2010.03.028 · Cited by 155 · see citing works
Guild, J. B., Xu, C., & Webb, W. W. (1997) · Applied Optics · doi:10.1364/ao.36.000397 · Cited by 117 · see citing works
Ma, Y., Cogdell, R. J., & Gillbro, T. (1997) · The Journal of Physical Chemistry B · doi:10.1021/jp962470e · Cited by 116 · see citing works
Self-citationHess, S., Feldchtein, F. I., Babin, A. A., et al. (1993) · Chemical Physics Letters · doi:10.1016/0009-2614(93)90090-n · Cited by 116 · see citing works
Krüger, T. P. J., Wientjes, E., Croce, R., & van Grondelle, R. (2011) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.1105411108 · Cited by 116 · see citing works
Ultrafast dynamics of single molecules
Brinks, D., Hildner, R., van Dijk, E. M. H. P., Stefani, F. D., Nieder, J. B., Hernando, J. C., & van Hulst, N. F. (2014) · Chemical Society Reviews · doi:10.1039/c3cs60269a · Cited by 109 · see citing works
van Oijen, A. M., Ketelaars, M., Köhler, J. R., Aartsma, T. J., & Schmidt, J. (2000) · Biophysical Journal · doi:10.1016/s0006-3495(00)76709-9 · Cited by 107 · see citing works
Caro, C. D., Visschers, R. W., van Grondelle, R., et al. (1994) · The Journal of Physical Chemistry · doi:10.1021/j100092a032 · Cited by 106 · see citing works
Rutkauskas, D., Novoderezkhin, V., Cogdell, R. J., & van Grondelle, R. (2004) · Biochemistry · doi:10.1021/bi0497648 · Cited by 104 · see citing works
Self-citationExciton dynamics in photosynthetic complexes: excitation by coherent and incoherent light
Mančal, T., & Valkūnas, L. (2010) · New Journal of Physics · doi:10.1088/1367-2630/12/6/065044 · Cited by 101 · see citing works
Self-citationvan Grondelle, R., Hunter, C. N., Bakker, J. G. C., et al. (1983) · Biochimica et Biophysica Acta (BBA) - Bioenergetics · doi:10.1016/0005-2728(83)90005-1 · Cited by 94 · see citing works
Novoderezhkin, V. I., Wendling, M., & van Grondelle, R. (2003) · The Journal of Physical Chemistry B · doi:10.1021/jp035432l · Cited by 90 · see citing works
Fidler, A. F., Singh, V. P., Long, P. D., Dahlberg, P. D., & Engel, G. S. (2014) · Nature Communications · doi:10.1038/ncomms4286 · Cited by 87 · see citing works
Single-molecule spectroscopy reveals photosynthetic LH2 complexes switch between emissive states
Schlau‐Cohen, G. S., Wang, Q., Southall, J., Cogdell, R. J., & Moerner, W. E. (2013) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.1310222110 · Cited by 86 · see citing works
Self-citationvan Dijk, E. M. H. P., Hernando, J. C., García-López, J. J., Crego‐Calama, M., Reinhoudt, D. N., Kuipers, L., Parajo, M. F. G., & van Hulst, N. F. (2005) · Physical Review Letters · doi:10.1103/physrevlett.94.078302 · Cited by 83 · see citing works
Bergström, H., Sundström, V., van Grondelle, R., et al. (1988) · Biochimica et Biophysica Acta (BBA) - Bioenergetics · doi:10.1016/0005-2728(88)90255-1 · Cited by 57 · see citing works
Effect of Disorder on Ultrafast Exciton Dynamics Probed by Single Molecule Spectroscopy
Hernando, J. C., van Dijk, E. M. H. P., Hoogenboom, J. P., García-López, J. J., Reinhoudt, D. N., Crego‐Calama, M., Parajo, M. F. G., & van Hulst, N. F. (2006) · Physical Review Letters · doi:10.1103/physrevlett.97.216403 · Cited by 39 · see citing works
Rutkauskas, D., Novoderezhkin, V. I., Gall, A., Olsen, J. D., Cogdell, R. J., Hunter, C. N., & van Grondelle, R. (2006) · Biophysical Journal · doi:10.1529/biophysj.105.075903 · Cited by 37 · see citing works
Self-citationDetermination of the Spectral Diffusion Kernel of a Protein by Single-Molecule Spectroscopy
Baier, J., Richter, M. F., Cogdell, R. J., Oellerich, S., & Köhler, J. R. (2008) · Physical Review Letters · doi:10.1103/physrevlett.100.018108 · Cited by 33 · see citing works
Self-citationLow-Intensity Pump-Probe Measurements on the B800 Band of Rhodospirillum molischianum
Wendling, M., van Mourik, F., van Stokkum, I. H. M., et al. (2003) · Biophysical Journal · doi:10.1016/s0006-3495(03)74864-4 · Cited by 30 · see citing works
Single-molecule pump-probe experiments reveal variations in ultrafast energy redistribution
van Dijk, E. M. H. P., Hernando, J. C., Parajo, M. F. G., & van Hulst, N. F. (2005) · The Journal of Chemical Physics · doi:10.1063/1.1940567 · Cited by 29 · see citing works
Maiuri, M., Réhault, J., Carey, A., Hacking, K., Garavelli, M., Lüer, L., Polli, D., Cogdell, R. J., & Cerullo, G. (2015) · The Journal of Chemical Physics · doi:10.1063/1.4919056 · Cited by 28 · see citing works
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Flagged first, then by citations
Research works printed but not linked: 1
- [33]Loudon, R. (2001) The Quantum Theory of Light . (Oxford University Press, New York), 3rd edition, pp. 68-72.
Cited by
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Marais, A., Adams, B., Ringsmuth, A. K., Ferretti, M., Gruber, J. M., Hendrikx, R., Schuld, M., Smith, S. L., Sinayskiy, I., Krüger, T. P. J., et al. (2018) · Journal of The Royal Society Interface · doi:10.1098/rsif.2018.0640 · Cited by 274 · see citing works
Self-citationSingle-Molecule Fluorescence Spectroscopy of Photosynthetic Systems
Kondo, T., Chen, W. J., & Schlau-Cohen, G. S. (2017) · Chemical Reviews · doi:10.1021/acs.chemrev.6b00195 · Cited by 120 · see citing works
From isolated light‐harvesting complexes to the thylakoid membrane: a single‐molecule perspective
Gruber, J. M., Malý, P., Krüger, T. P. J., & van Grondelle, R. (2018) · Nanophotonics · doi:10.1515/nanoph-2017-0014 · Cited by 14 · see citing works
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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
- Publisher
- National Academy of Sciences
- Published
- 2016-02-22
- Volume
- 113
- Issue
- 11
- Pages
- 2934-2939
- ISSN
- 0027-8424 (ISSN-L)
- 1091-6490
- PMC
- PMC4801264
- 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
- green
- www.ncbi.nlm.nih.gov
- 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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