Photoelectron Diffraction Imaging of a Molecular Breakup Using an X-Ray Free-Electron Laser
Photoelectron Diffraction Imaging of a Molecular Breakup Using an X-Ray Free-Electron Laser
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DOI：
10.1103/physrevx.10.021052
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发表时间：
2020-06-08
影响因子：
12.5
通讯作者：
Jahnke, Till
中科院分区：
文献类型：
--
作者：
Kastirke, Gregor;Schoeffler, Markus S.;Jahnke, Till
发展 X 射线自由电子激光器的核心动机是具有原子分辨率的时间分辨单分子成像的前景。在这里，我们展示了 X 射线光电子衍射（X 射线吸收后发射的光电子从内部照亮分子结构）可用于对 O-2 分子 X 射线诱导碎裂过程中核间距离的增加进行成像。通过测量与碎片离子一致的双光子连续 K 壳层电离的分子框架光电子发射模式，并根据测得的动能释放对数据进行排序，我们可以解决分子键伸长约 1.2 a.u 的问题。在 X 射线脉冲的持续时间内。该实验为高重复率 X 射线自由电子激光器的时间分辨泵浦探针光电子衍射成像铺平了道路。
A central motivation for the development of x-ray free-electron lasers has been the prospect of time-resolved single-molecule imaging with atomic resolution. Here, we show that x-ray photoelectron diffraction-where a photoelectron emitted after x-ray absorption illuminates the molecular structure from within-can be used to image the increase of the internuclear distance during the x-ray-induced fragmentation of an O-2 molecule. By measuring the molecular-frame photoelectron emission patterns for a two-photon sequential K-shell ionization in coincidence with the fragment ions, and by sorting the data as a function of the measured kinetic energy release, we can resolve the elongation of the molecular bond by approximately 1.2 a.u. within the duration of the x-ray pulse. The experiment paves the road toward time-resolved pump-probe photoelectron diffraction imaging at high-repetition-rate x-ray free-electron lasers.