| Summary: | We explore the feasibility of the coherent control of excitonic dynamics in light-harvesting complexes, analyzing the limits imposed by the open nature of these quantum systems. We establish feasible targets for phase and phase/amplitude control of the electronically excited state populations in the Fenna–Mathews–Olson (FMO) complex and analyze the robustness of this control with respect to orientational and energetic disorder, as well as the decoherence arising from coupling to the protein environment. We further present two possible routes to verification of the control target, with simulations for the FMO complex showing that steering of the excited state is experimentally verifiable either by extending excitonic coherence or by producing novel states in a pump–probe setup. Our results provide a first step toward coherent control of these complex biological quantum systems in an ultrafast spectroscopy setup.
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