Origin of long-lived quantum coherence and excitation dynamics in pigment-protein complexes.

Origin of long-lived quantum coherence and excitation dynamics in pigment-protein complexes.
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DOI:
10.1038/srep37629
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发表时间:
2016-11-23
期刊:
影响因子:
4.6
通讯作者:
Wang J
Wang J
中科院分区:
综合性期刊3区
文献类型:
--
作者:
Zhang Z;Wang J

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我们通过考虑离散声子模式来探讨长寿命量子相干的机制:这些振动模式有效地削弱了激子与环境的相互作用,这是由于激子和振动子形成了新的复合物(极化子)。这随后证明了振动相干性的作用,这极大地有助于在飞秒实验中观察到的激子相干性的长寿命特征。用解析的方法给出了振动模拉长相干时间尺度的估计。为了验证我们的理论的有效性,我们详细研究了色素蛋白质复合物,探索能量转移和相干动力学。由非相干辐射产生的基态振动相干性被证明是长期存在的,并被证明是显着的,在促进激发能量转移。这是由于详细的平衡打破,这漏斗激子的下山迁移所造成的系统的非平衡性。
We explore the mechanism for the long-lived quantum coherence by considering the discrete phonon modes: these vibrational modes effectively weaken the exciton-environment interaction, due to the new composite (polaron) formed by excitons and vibrons. This subsequently demonstrates the role of vibrational coherence which greatly contributes to long-lived feature of the excitonic coherence that has been observed in femtosecond experiments. The estimation of the timescale of coherence elongated by vibrational modes is given in an analytical manner. To test the validity of our theory, we study the pigment-protein complex in detail by exploring the energy transfer and coherence dynamics. The ground-state vibrational coherence generated by incoherent radiations is shown to be long-survived and is demonstrated to be significant in promoting the excitation energy transfer. This is attributed to the nonequilibriumness of the system caused by the detailed-balance-breaking, which funnels the downhill migration of excitons.
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