Journal
FARADAY DISCUSSIONS
Volume 153, Issue -, Pages 93-104Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c1fd00049g
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Funding
- Searle Foundation
- AFOSR [FA9550-09-1-0117]
- DARPA [N66001-10-1-4060]
- NSF GRF
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We present an analysis of dephasing rates for multiple zero-quantum electronic coherences in the Fenna-Matthew-Olson (FMO) pigment-protein complex using two-dimensional electronic spectroscopy. We employ the linear prediction Z-transform to determine both the frequency and decay rates of 8 individually assigned exciton-exciton coherences. Despite congestion in the spectra, we can isolate multiple crosspeaks signals and analyze their dephasing rates. A non-trivial relationship exists between the excitons and the bath determining the lifetimes of different exciton-exciton coherences. We propose that the correlations that protect long-lived electronic coherence may yield microscopic knowledge regarding the structure of the protein bath surrounding the chromophores.
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