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Intramolecular vibrations enhance the quantum efficiency of excitonic energy transfer.
Photosynthesis Research ( IF 3.7 ) Pub Date : 2020-04-18 , DOI: 10.1007/s11120-020-00742-x
Hong-Guang Duan 1, 2, 3 , Peter Nalbach 4 , R J Dwayne Miller 2, 3, 5 , Michael Thorwart 1, 3
Affiliation  

We study the impact of underdamped intramolecular vibrational modes on the efficiency of the excitation energy transfer in a dimer in which each state is coupled to its own underdamped vibrational mode and, in addition, to a continuous background of environmental modes. For this, we use the numerically exact hierarchy equation of motion approach. We determine the quantum yield and the transfer time in dependence of the vibronic coupling strength, and in dependence of the damping of the incoherent background. Moreover, we tune the vibrational frequencies out of resonance with the excitonic energy gap. We show that the quantum yield is enhanced by up to 10% when the vibrational frequency of the donor is larger than at the acceptor. The vibronic energy eigenstates of the acceptor acquire then an increased density of states, which leads to a higher occupation probability of the acceptor in thermal equilibrium. We can conclude that an underdamped vibrational mode which is weakly coupled to the dimer fuels a faster transfer of excitation energy, illustrating that long-lived vibrations can, in principle, enhance energy transfer, without involving long-lived electronic coherence.

中文翻译:

分子内振动增强了激子能量转移的量子效率。

我们研究分子阻尼不足的分子内振动模式对二聚物中激发能传递效率的影响,在该二聚体中,每个状态都耦合到其自身的阻尼不足的振动模态,此外,还存在连续的环境模式背景。为此,我们使用运动方法的数字精确层次方程。我们根据振动耦合强度以及不相干背景的阻尼来确定量子产率和传输时间。此外,我们通过激子能隙来调节共振频率下的振动频率。我们表明,当施主的振动频率大于受主的振动频率时,量子产率最多可提高10%。受体的振动能本征态会增加态的密度,这导致受体在热平衡中的占据概率更高。我们可以得出结论,与二聚体弱耦合的欠阻尼振动模式可以更快地传递激发能,这说明,长寿命的振动原则上可以增强能量传递,而不会涉及长寿命的电子相干性。
更新日期:2020-04-22
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