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A remarkable amount of theoretical research has been carried out to elucidatethe physical origins of the recently observed long-lived quantum coherence inthe electronic energy transfer process in biological photosynthetic systems.Although successful in many respects, several widely used descriptions onlyinclude an effective treatment of the protein-chromophore interactions. In thiswork, by combining an all-atom molecular dynamics simulation, time-dependentdensity functional theory, and open quantum system approaches, we successfullysimulate the dynamics of the electronic energy transfer of theFenna-Matthews-Olson pigment-protein complex. The resulting characteristicbeating of populations and quantum coherences is in good agreement with theexperimental results and the hierarchy equation of motion approach. Theexperimental absorption, linear and circular dichroism spectra and dephasingrates are recovered at two different temperatures. In addition, we provide anextension of our method to include zero-point fluctuations of the vibrationalenvironment. This work thus presents one of the first steps to explain the roleof excitonic quantum coherence in photosynthetic light-harvesting complexesbased on their atomistic and molecular description.

Atomistic study of the long-lived quantum coherences in the Fenna-Matthews-Olson complex