About: Two-Dimensional Electronic Spectroscopy Reveals Ultrafast Energy Diffusion in Chlorosomes     Goto   Sponge   NotDistinct   Permalink

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  • Chlorosomes are light-harvesting antennae that enable exceptionally efficient light energy capture and excitation transfer. They are found in certain photosynthetic bacteria, some of which live in extremely low-light environments. In this work, chlorosomes from the green sulfur bacterium Chlorobaculum tepidum were studied by coherent electronic two-dimensional (2D) spectroscopy. Previously uncharacterized ultrafast energy transfer dynamics were followed, appearing as evolution of the 2D spectral line-shape during the first 200 fs after excitation. Observed initial energy flow through the chlorosome is well explained by effective exciton diffusion on a sub-100 fs time scale, which assures efficiency and robustness of the process. The ultrafast incoherent diffusion-like behavior of the excitons points to a disordered energy landscape in the chlorosome, which leads to a rapid loss of excitonic coherences between its structural subunits. This disorder prevents observation of excitonic coherences in the experimental data and implies that the chlorosome as a whole does not function as a coherent light-harvester.
  • Chlorosomes are light-harvesting antennae that enable exceptionally efficient light energy capture and excitation transfer. They are found in certain photosynthetic bacteria, some of which live in extremely low-light environments. In this work, chlorosomes from the green sulfur bacterium Chlorobaculum tepidum were studied by coherent electronic two-dimensional (2D) spectroscopy. Previously uncharacterized ultrafast energy transfer dynamics were followed, appearing as evolution of the 2D spectral line-shape during the first 200 fs after excitation. Observed initial energy flow through the chlorosome is well explained by effective exciton diffusion on a sub-100 fs time scale, which assures efficiency and robustness of the process. The ultrafast incoherent diffusion-like behavior of the excitons points to a disordered energy landscape in the chlorosome, which leads to a rapid loss of excitonic coherences between its structural subunits. This disorder prevents observation of excitonic coherences in the experimental data and implies that the chlorosome as a whole does not function as a coherent light-harvester. (en)
Title
  • Two-Dimensional Electronic Spectroscopy Reveals Ultrafast Energy Diffusion in Chlorosomes
  • Two-Dimensional Electronic Spectroscopy Reveals Ultrafast Energy Diffusion in Chlorosomes (en)
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  • Two-Dimensional Electronic Spectroscopy Reveals Ultrafast Energy Diffusion in Chlorosomes
  • Two-Dimensional Electronic Spectroscopy Reveals Ultrafast Energy Diffusion in Chlorosomes (en)
skos:notation
  • RIV/60076658:12310/12:43883532!RIV13-MSM-12310___
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  • P(GA206/09/0375), S, V, Z(MSM0021620835)
http://linked.open...iv/cisloPeriodika
  • 28
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  • 175492
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  • RIV/60076658:12310/12:43883532
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http://linked.open.../riv/klicovaSlova
  • ORGANIZATION; BCHL-C; LINEAR DICHROISM; EXCITON DYNAMICS; FEMTOSECOND SPECTROSCOPY; CHLOROFLEXUS-AURANTIACUS; BACTERIOCHLOROPHYLL-C; CHLOROBIUM-TEPIDUM; LIGHT-HARVESTING CHLOROSOMES; GREEN PHOTOSYNTHETIC BACTERIA (en)
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  • US - Spojené státy americké
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  • [651D27BB9133]
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  • JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
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  • 134
http://linked.open...iv/tvurceVysledku
  • Vácha, František
  • Augulis, Ramunas
  • Dostal, Jakub
  • Mancal, Tomas
  • Psencik, Jakub
  • Zigmantas, Donatas
http://linked.open...ain/vavai/riv/wos
  • 000306457900050
http://linked.open...n/vavai/riv/zamer
issn
  • 0002-7863
number of pages
http://bibframe.org/vocab/doi
  • 10.1021/ja3025627
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  • 12310
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