Nature does not rely on long-lived electronic quantum coherence for photosynthetic energy transfer
Abstract
Significance We have revisited the 2D spectroscopy of the excitation energy transfer in the Fenna–Matthews–Olson (FMO) protein. Based on 2D spectroscopic signatures, the energy transfer dynamics in the FMO protein has been argued to be supported by long-lived electronic quantum coherence on timescales up to 1.5 ps. In contrast, our analysis, based on experimental data and confirmed by theoretical calculations, shows that the electronic decoherence occurs within 60 fs, in agreement with typical dephasing times in systems under these conditions. Given the relatively well-defined structure of the FMO protein, and comparative couplings between chlorophylls to other photosynthetic systems, the observed extremely fast decoherence should be viewed as general, bringing to question any significant quantum coherent transport contributions to photosynthesis. During the first steps of photosynthesis, the energy of impinging solar photons is transformed into electronic excitation energy of the light-harvesting biomolecular complexes. The subsequent energy transfer to the reaction center is commonly rationalized in terms of excitons moving on a grid of biomolecular chromophores on typical timescales <100 fs. Today’s understanding of the energy transfer includes the fact that the excitons are delocalized over a few neighboring sites, but the role of quantum coherence is considered as irrelevant for the transfer dynamics because it typically decays within a few tens of femtoseconds. This…
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