Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 134, Issue 28, Pages 11611-11617Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja3025627
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Funding
- Swedish Research Council
- Knut and Alice Wallenberg Foundation
- Wenner-Gren Foundations
- LASERLAB-EUROPE
- Grant Agency of Charles University [GAUK 129809]
- Czech Ministry of Education, Youth and Sports [MSM0021620835]
- Czech Science Foundation [206/09/0375]
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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.
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