Fast Exciton Dynamics and Coherent Oscillations Revealed by Coherent 2D Spectroscopy in Chlorosomes

Mančal, Tomáš; Vacha, František; Augulis, Ramu̅nas; Pšenčı́k, Jakub; Zigmantas, Donatas

doi:10.1051/epjconf/20134108015

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2014

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“…3). Superimposed on the population dynamics oscillatory quantum coherence dynamics (identical to the observations in 27 ) are visible during the initial 1.8 ps (see Fig. S3 of the Supporting Information).…”

Section: Main Textsupporting

confidence: 56%

2D Electronic Spectroscopy Reveals Excitonic Structure in the Baseplate of a Chlorosome

Vácha

Pšenčı́k

Zigmantas

2014

J. Phys. Chem. Lett.

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In green photosynthetic bacteria, the chlorosome baseplate mediates excitation energy transfer from the interior of the light-harvesting chlorosome toward the reaction centers. However, the electronic states of the baseplate remain unexplored, hindering the mechanistic understanding of the baseplate as an excitation energy collector and mediator. Here we use two-dimensional spectroscopy to study the excited state structure and internal energy relaxation in the baseplate of green sulfur bacterium Chlorobaculum tepidum. We resolved an exciton system with four energy states, indicating that the organization of the pigments in the baseplate is more complex than was thought before and constitutes at least four bacteriochlorophyll molecules in a close contact. Based on the finding that the energy of the baseplate states is in the same range as in the adjacent Fenna-Matthews-Olson complex, we propose a "lateral" energy transfer pathway, where excitation energy can flow through the photosynthetic unit via all the states of individual complexes.

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Section: Main Textsupporting

confidence: 56%