Dynamics of diverse coherences in primary charge separation of bacterial reaction center at 77 K revealed by wavelet analysis

Fei Ma*, Elisabet Romero, Michael R. Jones, Vladimir I. Novoderezhkin, Long Jiang Yu, Rienk van Grondelle

*Corresponding author for this work

Research output: Contribution to JournalArticleAcademicpeer-review

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Abstract

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.

Original languageEnglish
Pages (from-to)225-234
Number of pages10
JournalPhotosynthesis Research
Volume151
Issue number3
Early online date28 Oct 2021
DOIs
Publication statusPublished - Mar 2022

Bibliographical note

Funding 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.

Publisher Copyright:
© 2021, The Author(s), under exclusive licence to Springer Nature B.V.

Funding

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.

FundersFunder number
PHOTPROT
Biotechnology and Biological Sciences Research CouncilBB/I022570/1
Biotechnology and Biological Sciences Research Council
European Research Council267333
European Research Council
National Natural Science Foundation of China21903086
National Natural Science Foundation of China
Russian Foundation for Basic Research18-04-00105
Russian Foundation for Basic Research
National Key Research and Development Program of China2019YFA0904600
National Key Research and Development Program of China

    Keywords

    • Bacterial reaction center
    • Primary charge separation
    • Quantum coherence
    • Wavelet analysis

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