电子相干性在现实条件下是否增强了与色素相关的振动？
Does electronic coherence enhance anticorrelated pigment vibrations under realistic conditions?
摘要：
光活性分子复合物的光捕获效率在很大程度上由其电子量子态的性质决定。这些，反过来，受到分子振动状态的核自由度。在这里，我们重新审视两个最近制定的概念，分子状态之间的相干电子振动耦合将延长电子相干寿命或增强振幅的相干相关的振动模式在较长的时间。为此，我们研究了振动耦合的二聚体，并计算了直接揭示电子相干性的非线性二维（2D）电子光谱。通过测量零等待时间时二维光谱中心峰的反对角带宽，初步提取了电子相干的时间尺度。残差分析的基础上，我们确定的小振幅的长寿命振荡的交叉峰，然而，这仅仅是由于基态振动的相干性，无论有共振或非共振条件。我们的研究既没有显示出电子量子相干性的增强，也没有显示出在环境条件下的电子振动耦合的增强与电子相关的振动模式。
英文摘要：
The light-harvesting efficiency of a photoactive molecular complex is largely determined by the properties of its electronic quantum states. Those, in turn, are influenced by molecular vibrational states of the nuclear degrees of freedom. Here, we reexamine two recently formulated concepts that a coherent vibronic coupling between molecular states would either extend the electronic coherence lifetime or enhance the amplitude of the anticorrelated vibrational mode at longer times. For this, we study a vibronically coupled dimer and calculate the nonlinear two-dimensional (2D) electronic spectra which directly reveal electronic coherence. The timescale of electronic coherence is initially extracted by measuring the anti-diagonal bandwidth of the central peak in the 2D spectrum at zero waiting time. Based on the residual analysis, we identify small-amplitude long-lived oscillations in the cross-peaks, which, however, are solely due to groundstate vibrational coherence, regardless of having resonant or off-resonant conditions. Our studies neither show an enhancement of the electronic quantum coherence nor an enhancement of the anticorrelated vibrational mode by the vibronic coupling under ambient conditions.
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