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Raman and 2D electronic spectroscopies: A fruitful alliance for the investigation of ground and excited state vibrations in chlorophyll a
Chemical Physics ( IF 2.3 ) Pub Date : 2018-03-05 , DOI: 10.1016/j.chemphys.2018.03.003
Elena Meneghin , Danilo Pedron , Elisabetta Collini

Vibrational coherences and their time evolution are crucial for the correct description of the dynamical behavior of materials, also influencing the dynamics of electronic coherences and transport processes. For this reason, vibrational coherences are now becoming the subject of wider investigation, especially in the framework of 2D electronic spectroscopies. A correct interpretation of vibrational coherences in 2DES responses requires the comparison with Raman spectra.

Here we propose a methodology that goes beyond the typical practice of merely looking for frequencies present in both signals. In particular, we discuss suitable experimental conditions and correction procedures that allows a direct comparison of Fourier spectra obtained from the analysis of the signal beating at specific coordinates in 2D maps with resonant and non-resonant Raman spectra, to clearly identify the vibrational modes more strongly coupled with the electronic transition.

The advantages of this approach have been illustrated using Chla chromophore as a case study.



中文翻译:

拉曼光谱和二维电子光谱:研究叶绿素a的基态和激发态振动的卓有成效的联盟

振动相干及其时间演化对于正确描述材料的动力学行为至关重要,也影响电子相干和传输过程的动力学。因此,振动相干性正在成为更广泛研究的主题,尤其是在二维电子光谱学的框架中。正确解释2DES响应中的振动相干性需要与拉曼光谱进行比较。

在这里,我们提出了一种超越仅查找两个信号中存在的频率的典型实践的方法。特别是,我们讨论了合适的实验条件和校正程序,这些方法和方法可以直接比较通过分析2D映射中特定坐标处的信号跳动而获得的傅立叶光谱,并比较共振和非共振拉曼光谱,从而更清楚地识别振动模式。加上电子转换。

这种方法的优点已经使用叶绿素示出一个发色团作为个案研究。

更新日期:2018-06-03
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