论文标题
电子振动共振不会改变自然光收获系统中的稳态传输
Electronic-vibrational resonance does not alter steady-state transport in natural light-harvesting systems
论文作者
论文摘要
时间依赖性2D电子光谱的振荡似乎是与电子振动谐振相互作用有关的光收获系统中量子相干性的证据。但是,自然是在非平衡稳态中发生的,因此这些论点与自然过程的相关性尚不清楚。在这里,我们研究了分子内振动在光合二聚体非平衡稳态中的作用,在不相互的光激发的自然情况下。发现具有激子状态之间能量差的振动不会增加与自然非平衡稳态中的非谐振振动相比,与运输相关的位点相干性的假想部分。也就是说,振动 - 电气共振相互作用不会改变自然光线激发条件下的能量传输。
Oscillations in time-dependent 2D electronic spectra appear as evidence of quantum coherence in light-harvesting systems related to electronic-vibrational resonant interactions. Nature, however, takes place in a non-equilibrium steady-state, so the relevance of these arguments to the natural process is unclear. Here we examine the role of intramolecular vibrations in the non-equilibrium steady-state of photosynthetic dimers in the natural scenario of incoherent light excitation. It is found that vibrations resonant with the energy difference between exciton states do not increase the quantum yield nor the imaginary part of the intersite coherence that is relevant for transport compared with non-resonant vibrations in the natural non-equilibrium steady state. That is, the vibration-electronic resonance interaction does not alter energy transport under natural incoherent-light excitation conditions.