期刊
PHYSICAL REVIEW LETTERS
卷 125, 期 7, 页码 -出版社
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevLett.125.073203
关键词
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资金
- U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (BES) [DE-AC0276SF00515]
- AMOS program in the Chemical Sciences, Geosciences, and Biosciences Division of BES at the DOE
- AMOS [DE-AC02-06CH11357, DE-SC0012376, DE-AC02-05-CH11231]
- DOE-BES Accelerator and detector research program
- MCIU/AEI/FEDER, UE [RTI2018-097355-A-I00]
- UK EPSRC [EP/R019509/1, EP/I032517/]
- [2017-T1/IND5432]
- EPSRC [EP/R019509/1, EP/I032517/1] Funding Source: UKRI
Free-electron lasers provide a source of x-ray pulses short enough and intense enough to drive nonlinearities in molecular systems. Impulsive interactions driven by these x-ray pulses provide a way to create and probe valence electron motions with high temporal and spatial resolution. Observing these electronic motions is crucial to understand the role of electronic coherence in chemical processes. A simple nonlinear technique for probing electronic motion, impulsive stimulated x-ray Raman scattering (ISXRS), involves a single impulsive interaction to produce a coherent superposition of electronic states. We demonstrate electronic population transfer via ISXRS using broad bandwidth (5.5 eV full width at half maximum) attosecond x-ray pulses produced by the Linac Coherent Light Source. The impulsive excitation is resonantly enhanced by the oxygen 1s -> 2 pi* resonance of nitric oxide (NO), and excited state neutral molecules are probed with a time-delayed UV laser pulse.
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