Two-Dimensional Electronic Spectroscopy Reveals Ultrafast Energy Diffusion in Chlorosomes.

Summary, in English

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.

• Author: Jakub Dostal; Tomáš Mančal; Ramunas Augulis; František Vácha; Jakub Pšenčík; Donatas Zigmantas
• Department/s: Chemical Physics; NanoLund: Centre for Nanoscience
• Publishing year: 2012
• Language: English
• Pages: 11611-11617
• Publication/Series: Journal of the American Chemical Society
• Volume: 134
• Issue: 28
• Links: http://dx.doi.org/10.1021/ja3025627
• Document type: Journal article
• Publisher: The American Chemical Society (ACS)
• Topic: Atom and Molecular Physics and Optics
• Status: Published
• ISBN/ISSN/Other: ISSN: 1520-5126