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Experimental/theoretical evidence for sustained vibration-assisted electronic(vibronic) coherence in the Photosystem II Reaction Center (PSII RC) indicatesthat photosynthetic solar-energy conversion might be optimized through theinterplay of electronic and vibrational quantum dynamics. This evidence hasbeen obtained by investigating the primary charge separation process in thePSII RC by two-dimensional electronic spectroscopy (2DES) and Redfield modelingof the experimental data. However, while conventional Fourier transformanalysis of the 2DES data allows oscillatory signatures of vibronic coherenceto be identified in the frequency domain in the form of static 2D frequencymaps, the real-time evolution of the coherences is lost. Here we apply for thefirst time wavelet analysis to the PSII RC 2DES data to obtain time-resolved 2Dfrequency maps. These maps allow us to demonstrate that i) coherence betweenthe excitons initiating the two different charge separation pathways is activefor more than 500 fs, and ii) coherence between exciton and charge-transferstates, the reactant and product of the charge separation reaction,respectively, is active for at least 1 ps. These findings imply that the PSIIRC employs coherence i) to sample competing electron transfer pathways, and ii)to perform directed, ultrafast and efficient electron transfer.

Quantum-coherent dynamics in photosynthetic charge separation revealed by wavelet analysis