Two-dimensional electronic spectroscopy reveals ultrafast energy diffusion in chlorosomes |
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Authors: | Dostál Jakub Man?al Tomá? Augulis Ramūnas Vácha Franti?ek P?en?ík Jakub Zigmantas Donatas |
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Institution: | Department of Chemical Physics, Lund University, Getingev?gen 60, 221 00 Lund, Sweden. |
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Abstract: | 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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