Optical Quantum Control of the Electron Transfer Reactions in Protein Flavodoxin

IF 2.8 2区 化学 Q3 CHEMISTRY, PHYSICAL The Journal of Physical Chemistry B Pub Date : 2024-11-01 DOI:10.1021/acs.jpcb.4c0425410.1021/acs.jpcb.4c04254
Na Liu, Yifei Zhang, Xi Wang, Kangwei Niu, Faming Lu*, Jie Chen* and Dongping Zhong*, 
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Abstract

The optical quantum control has been successfully applied in modulating biological processes such as energy transfer and bond isomerization. Among the reactions in realizing biological functions, the electron transfer (ET) process is fundamental; hence, the quantum control over such an ET reaction is of far-reaching significance. Here, we realized optical quantum control over ultrafast ET processes in a protein, flavodoxin, by applying various chirped excitation pulses. We observed the wavepacket dynamics within a dephasing time of less than 1 ps. Within this time window, we found that the ultrafast photoinduced ET reaction can be controlled by different chirped excitations with a rate change by a factor of about 2. Furthermore, the control effect is propagated into the subsequent ultrafast back ET reaction, showing a variation of the BET dynamics with different excitation chirps. The underlying mechanism is the initial wavepacket dynamics; the differently prepared wavepackets with chirped excitation evolve along various pathways, resulting in the changes of ET rates. The successful demonstration of optical quantum control of ultrafast biological ET is significant and opens a new avenue to explore the quantum control of real biological ET reactions.

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蛋白质黄酮苷中电子传递反应的光量子控制
光量子控制已成功应用于调节能量转移和键异构化等生物过程。在实现生物功能的反应中,电子传递(ET)过程是最基本的,因此对这种ET反应进行量子控制具有深远的意义。在这里,我们通过应用各种啁啾激发脉冲,实现了对蛋白质黄独素超快电子传递过程的光量子控制。我们观察了去相时间小于 1 ps 的波包动态。在这个时间窗口内,我们发现不同的啁啾激发可以控制超快光诱导 ET 反应,其速率变化约为 2 倍。 此外,控制效应还传播到随后的超快反向 ET 反应中,显示出不同激发啁啾的 BET 动态变化。其基本机制是初始波包动力学;不同的啁啾激发波包沿着不同的路径演化,从而导致 ET 速率的变化。光量子控制超快生物 ET 的成功演示意义重大,为探索真实生物 ET 反应的量子控制开辟了一条新途径。
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来源期刊
CiteScore
5.80
自引率
9.10%
发文量
965
审稿时长
1.6 months
期刊介绍: An essential criterion for acceptance of research articles in the journal is that they provide new physical insight. Please refer to the New Physical Insights virtual issue on what constitutes new physical insight. Manuscripts that are essentially reporting data or applications of data are, in general, not suitable for publication in JPC B.
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