Time-Resolved Resonant Auger Scattering Clocks Distortion of a Molecule.
Time-Resolved Resonant Auger Scattering Clocks Distortion of a Molecule.
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DOI：
10.1021/acs.jpclett.3c01347
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发表时间：
2023-06
期刊：
影响因子：
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通讯作者：
Chao Wang;Maomao Gong;Y. Cheng;V. Kimberg;Xiao-Jing Liu;O. Vendrell;K. Ueda;S. Zhang
中科院分区：
文献类型：
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作者：
Chao Wang;Maomao Gong;Y. Cheng;V. Kimberg;Xiao-Jing Liu;O. Vendrell;K. Ueda;S. Zhang
共振俄歇散射 (RAS) 提供有关核价电子跃迁的信息，并在 RAS 过程启动时留下丰富的电子结构和核构型指纹。在这里，我们建议使用飞秒 X 射线脉冲来触发扭曲分子中的 RAS，该分子是由飞秒紫外线脉冲泵浦的价激发态的核演化产生的。随着时间延迟的变化，分子变形量可以得到控制，RAS 测量可以记录它们的电子结构和变化的几何形状。这种策略在 O-H 解离价态制备的 H2O 中得到展示，其中分子和碎片线出现在 RAS 光谱中作为超快解离的特征。鉴于这种方法对多种分子的普遍性，这项工作开辟了一种新的替代泵浦探针技术，用于使用超短 X 射线探针脉冲绘制核和价态动力学。
Resonant Auger scattering (RAS) provides information on the core-valence electronic transition and impresses a rich fingerprint of the electronic structure and nuclear configuration at the time-initiating RAS process. Here, we suggest using a femtosecond X-ray pulse to trigger RAS in a distorted molecule, which is generated from the nuclear evolution on a valence excited state pumped by a femtosecond ultraviolet pulse. With the time delay varied, the amount of molecular distortion can be controlled and the RAS measurements imprint both their electronic structures and changing geometries. This strategy is showcased in H2O prepared in an O-H dissociative valence state, where molecular and fragment lines appear in RAS spectra as signatures of ultrafast dissociation. Given the generality of this approach for a broad class of molecules, this work opens a new alternative pump-probe technique for mapping the core and valence dynamics with ultrashort X-ray probe pulses.