Rebuilding the vibrational wavepacket in TRAS using attosecond X-ray pulses
Rebuilding the vibrational wavepacket in TRAS using attosecond X-ray pulses
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DOI：
10.1038/s42005-023-01507-3
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发表时间：
2024-01
影响因子：
5.5
通讯作者：
Chao Wang;Maomao Gong;Xi Zhao;Quan Wei Nan;Xin Yue Yu;Yongjun Cheng;V. Kimberg;Xiao-Jing Liu;Oriol Vendrell;K. Ueda;S. Zhang
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文献类型：
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作者：
Chao Wang;Maomao Gong;Xi Zhao;Quan Wei Nan;Xin Yue Yu;Yongjun Cheng;V. Kimberg;Xiao-Jing Liu;Oriol Vendrell;K. Ueda;S. Zhang
时间分辨X射线光电子能谱（TXPS）是一种成熟的技术，使用桌面和自由电子基超快X射线激光探测相干核波包动力学。然而，对于亚飞秒范围内的非常短的脉冲持续时间，能量分辨率变得折衷。通过将X射线脉冲共振调谐到经历俄歇衰变的核心激发态，可以减轻TXPS的这个缺点。虽然共振俄歇电子能谱（RAS）可以恢复未被宽带激发隐藏的振动结构，但波包的完全重建是一个长期的挑战。在这里，我们从理论上证明了一个核波包的完整信息，即，构成波包的振动态的布居数和相对相位可以从时间分辨RAS（TRAS）测量中检索。因此，TRAS提供了关键的见解耦合核和电子动力学在复杂系统的超短时间尺度，提供了一种替代利用飞秒和阿秒X射线探测脉冲。
Time-resolved X-ray photoelectron spectroscopy (TXPS) is a well-established technique to probe coherent nuclear wavepacket dynamics using both table-top and free-electron-based ultrafast X-ray lasers. Energy resolution, however, becomes compromised for a very short pulse duration in the sub-femtosecond range. By resonantly tuning the X-ray pulse to core-excited states undergoing Auger decay, this drawback of TXPS can be mitigated. While resonant Auger-electron spectroscopy (RAS) can recover the vibrational structures not hidden by broadband excitation, the full reconstruction of the wavepacket is a standing challenge. Here, we theoretically demonstrate how the complete information of a nuclear wavepacket, i.e., the populations and relative phases of the vibrational states constituting the wavepacket, can be retrieved from time-resolved RAS (TRAS) measurements. Thus, TRAS offers key insights into coupled nuclear and electronic dynamics in complex systems on ultrashort timescales, providing an alternative to leverage femtosecond and attosecond X-ray probe pulses.