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

作  者:Ma F*, Romero E, Jones MR, Novoderezhkin VI, Yu LJ*, van Grondelle R
影响因子:3.573
刊物名称:Photosynthesis Research
出版年份:2021
卷:  期:  页码:DOI: 10.1007/s11120-021-00881-9

论文摘要:

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.

全文链接:https://link.springer.com/article/10.1007%2Fs11120-021-00881-9