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In situ mapping of the energy flow through the entire photosynthetic apparatus

Abstract

Absorption of sunlight is the first step in photosynthesis, which provides energy for the vast majority of organisms on Earth. The primary processes of photosynthesis have been studied extensively in isolated light-harvesting complexes and reaction centres, however, to understand fully the way in which organisms capture light it is crucial to also reveal the functional relationships between the individual complexes. Here we report the use of two-dimensional electronic spectroscopy to track directly the excitation-energy flow through the entire photosynthetic system of green sulfur bacteria. We unravel the functional organization of individual complexes in the photosynthetic unit and show that, whereas energy is transferred within subunits on a timescale of subpicoseconds to a few picoseconds, across the complexes the energy flows at a timescale of tens of picoseconds. Thus, we demonstrate that the bottleneck of energy transfer is between the constituents.

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Figure 1: The absorption spectrum of the intact C. tepidum cells (solid line) compared with the spectrum of isolated chlorosomes (dashed line) at 77 K.
Figure 2: The selected 2D spectra (absorptive part) of the intact C. tepidum cells measured between 11,900 and 13,200 cm−1 (760–840 nm) at the indicated population times at 77 K.
Figure 3: Decay-associated spectra of the FMO–RC spectral region.
Figure 4: Decay-associated spectra of the chlorosome excitation region.
Figure 5: A scheme of the excitation-energy flow through the entire photosynthetic apparatus of C. tepidum.

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Acknowledgements

We thank the group of F. Vácha for cell cultivation and for the isolation of the chlorosomes. We are grateful to D. Bína and H. Lokstein for their help with the cell viability experiments described in the Supplementary Information. The work in Lund was supported by the Swedish Research Council and the Knut and Alice Wallenberg Foundation. The work in Prague was supported by the Czech Science Foundation (project P501/12/G055).

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J.D. designed and performed the experiments, analysed the data and wrote the manuscript, J.P. designed and performed the experiments and wrote the manuscript, D.Z. conceived the idea, designed and performed the experiments and wrote the manuscript.

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Correspondence to Donatas Zigmantas.

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Dostál, J., Pšenčík, J. & Zigmantas, D. In situ mapping of the energy flow through the entire photosynthetic apparatus. Nature Chem 8, 705–710 (2016). https://doi.org/10.1038/nchem.2525

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