在二维回波谱中解开电子和振动相干性
Disentangling electronic and vibronic coherences in two-dimensional echo spectra
摘要：
在捕光复合物的二维回波光谱中，持续时间长的振荡信号的普遍存在导致了对可能机制的研究。我们研究了振荡信号的两个原因是如何交织在一起的：（i）电子相干支持离域波状运动，以及（ii）振动谱密度中的窄带。为了解开的振动和电子的贡献，我们引入了一个时间窗口傅立叶变换的信号幅度。我们发现，2d光谱可以占主导地位的激子能量输运缺席的途径的激发。这就导致了二维谱对电子相干寿命的低估。
英文摘要：
The prevalence of long-lasting oscillatory signals in the 2d echo-spectroscopy of light-harvesting complexes has led to a search for possible mechanisms. We investigate how two causes of oscillatory signals are intertwined: (i) electronic coherences supporting delocalized wave-like motion, and (ii) narrow bands in the vibronic spectral density. To disentangle the vibronic and electronic contributions we introduce a time-windowed Fourier transform of the signal amplitude. We find that 2d spectra can be dominated by excitations of pathways which are absent in excitonic energy transport. This leads to an underestimation of the life-time of electronic coherences by 2d spectra.
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