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The influence of fast vibrations on energy transfer and conversion in naturalmolecular aggregates is an issue of central interest. This article shows theimportant role of high-energy quantized vibrations and their non-equilibriumdynamics for energy transfer in photosynthetic systems with highly localizedexcitonic states. We consider the cryptophyte antennae protein phycoerythrin545 and show that coupling to quantized vibrations which are quasi-resonantwith excitonic transitions is fundamental for biological function as itgenerates non-cascaded transport with rapid and wider spatial distribution ofexcitation energy. Our work also indicates that the non-equilibrium dynamics ofsuch vibrations can manifest itself in ultrafast beating of both excitonicpopulations and coherences at room temperature, with time scales in agreementwith those reported in experiments. Moreover, we show that mechanismssupporting coherent excitonic dynamics assist coupling to selected modes thatchannel energy to preferential sites in the complex. We therefore argue that,in the presence of strong coupling between electronic excitations and quantizedvibrations, a concrete and important advantage of quantum coherent dynamics isprecisely to tune resonances that promote fast and effective energydistribution.

The fundamental role of quantized vibrations in coherent light harvesting by cryptophyte algae