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Volume 153, 2011
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Extracting dynamics of excitonic coherences in congested spectra of photosynthetic light harvesting antenna complexes

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Abstract

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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Publication details

The article was received on 30 Mar 2011, accepted on 27 Apr 2011 and first published on 24 May 2011


Article type: Paper
DOI: 10.1039/C1FD00049G
Citation: Faraday Discuss., 2011,153, 93-104
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    Extracting dynamics of excitonic coherences in congested spectra of photosynthetic light harvesting antenna complexes

    J. R. Caram and G. S. Engel, Faraday Discuss., 2011, 153, 93
    DOI: 10.1039/C1FD00049G

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