Two-dimensional electronic spectroscopy reveals ultrafast energy diffusion in chlorosomes.
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.
Department of Chemical Physics, Lund University, Getingevägen 60, 221 00 Lund, Sweden.
Jakub
J
Dostál
Tomáš
T
Mančal
Ramūnas
R
Augulis
František
F
Vácha
Jakub
J
Pšenčík
Donatas
D
Zigmantas
D002876:Chromosomes, Bacterial; D004058:Diffusion; D013057:Spectrum Analysis / Q000379:methods*