Journal
NATURE CHEMISTRY
Volume 4, Issue 5, Pages 389-395Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/NCHEM.1303
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Funding
- Office of Science, Office of Basic Energy Sciences, of the US Department of Energy [DE-AC02-05CH11231]
- Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences of the US Department of Energy (at LBNL and University of California, Berkeley) [DE-AC03-76SF000098]
- EU [PITN-GA-2009-238017 HARVEST, 245070 FP7-KBBE-2009-3SUNBIOPATH]
- A.A.U.W.
- LBNL
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Photosynthetic organisms harvest sunlight with near unity quantum efficiency. The complexity of the electronic structure and energy transfer pathways within networks of photosynthetic pigment-protein complexes often obscures the mechanisms behind the efficient light-absorption-to-charge conversion process. Recent experiments, particularly using two-dimensional spectroscopy, have detected long-lived quantum coherence, which theory suggests may contribute to the effectiveness of photosynthetic energy transfer. Here, we present a new, direct method to access coherence signals: a coherence-specific polarization sequence, which isolates the excitonic coherence features from the population signals that usually dominate two-dimensional spectra. With this polarization sequence, we elucidate coherent dynamics and determine the overall measurable lifetime of excitonic coherence in the major light-harvesting complex of photosystem II. Coherence decays on two distinct timescales of 47 fs and similar to 800 fs. We present theoretical calculations to show that these two timescales are from weakly and moderately strongly coupled pigments, respectively.
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