To uncover the mechanism behind the high photo-electronic conversion efficiency in natural photosynthetic complexes it is essential to trace the dynamics of electronic and vibrational quantum coherences. Here we apply wavelet analysis to two-dimensional electronic spectroscopy data for three purple bacterial reaction centers with mutations that produce drastically different rates of primary charge separation. From the frequency distribution and dynamic evolution features of the quantum beating, electronic coherence with a dephasing lifetime of ~50 fs, vibronic coherence with a lifetime of ~150 fs and vibrational/vibronic coherences with a lifetime of 450 fs are distinguished. We find that they are responsible for, or couple to, different specific steps during the primary charge separation process, i.e., intradimer charge transfer inside the special bacteriochlorophyll pair followed by its relaxation and stabilization of the charge-transfer state. The results enlighten our understanding of how quantum coherences participate in, and contribute to, a biological electron transfer reaction.
Bibliographical noteFunding Information:
This work has been supported by the National Key Research and Development Program of China (No. 2019YFA0904600), the Natural Science Foundation of China (No. 21903086) to F. M., the Advanced Investigator Grant from the European Research Council (No. 267333, PHOTPROT) to R. v. G, the Biotechnology and Biological Sciences Research Council of the UK (Project BB/I022570/1) to M. R. J. and the Russian Foundation for Basic Research (No. 18-04-00105) to V. N.
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