Journal
JOURNAL OF PHYSICAL CHEMISTRY B
Volume 116, Issue 25, Pages 7449-7454Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jp304649c
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Funding
- Wenner-Gren foundation
- OeAD
- Austrian Science Foundation (FWF)
- Swedish Research Council
- KAW foundation
- Swedish Energy Agency
- Czech Science Foundation [GACR 205/10/0989]
- Ministry of Education, Youth, and Sports of the Czech Republic [MEB 061107]
- Austrian Science Fund (FWF) [P 22331] Funding Source: researchfish
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A vibronic exciton model is applied to explain the long-lived oscillatory features in the two-dimensional (2D) electronic spectra of the Fenna-Matthews-Olson (FMO) complex. Using experimentally determined parameters and uncorrelated site energy fluctuations, the model predicts oscillations with dephasing times of 1.3 ps at 77 K, which is in a good agreement with the experimental results. These long-lived oscillations originate from the coherent superposition of vibronic exciton states with dominant contributions from vibrational excitations on the same pigment. The oscillations obtain a large amplitude due to excitonic intensity borrowing, which gives transitions with strong vibronic character a significant intensity despite the small Huang-Rhys factor. Purely electronic coherences are found to decay on a 200 fs time scale.
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