1. Rebuilding the vibrational wavepacket in TRAS using attosecond X-ray pulses
- Author
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Wang, Chao, Gong, Maomao, Zhao, Xi, Nan, Quan Wei, Yu, Xin Yue, Cheng, Yongjun, Kimberg, Victor, Liu, Xiao Jing, Vendrell, Oriol, Ueda, Kiyoshi, Zhang, Song Bin, Wang, Chao, Gong, Maomao, Zhao, Xi, Nan, Quan Wei, Yu, Xin Yue, Cheng, Yongjun, Kimberg, Victor, Liu, Xiao Jing, Vendrell, Oriol, Ueda, Kiyoshi, and Zhang, Song Bin
- Abstract
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., QC 20240115
- Published
- 2024
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