We propose an X-ray Raman pump–X-ray diffraction probe scheme to follow solvation dynamics upon charge migration in a solute molecule. The X-ray Raman pump selectively prepares a valence electronic wavepacket in the solute, while the probe provides information about the entire molecular ensemble. A combination of molecular dynamics and ab initio quantum chemistry simulations is applied to a Zn–Ni porphyrin dimer in water. Using time-resolved X-ray diffraction and pair distribution functions, we extracted solvation shell dynamics.

中文翻译：

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金属卟啉二聚体超快共振激励 X 射线拉曼激发下的水溶剂重组


我们提出了一种 X 射线拉曼泵 - X 射线衍射探针方案来跟踪溶质分子中电荷迁移时的溶剂化动力学。 X 射线拉曼泵选择性地在溶质中制备价电子波包，而探针则提供有关整个分子整体的信息。将分子动力学和从头算量子化学模拟相结合应用于水中的 Zn-Ni 卟啉二聚体。利用时间分辨 X 射线衍射和对分布函数，我们提取了溶剂化壳层动力学。