High Temporal and Spectral Resolution of Stimulated X-Ray Raman Signals with Stochastic Free-Electron-Laser Pulses
Abstract
The chaotic nature of x-ray free-electron-laser pulses is a major bottleneck that has limited the joint temporal and spectral resolution of spectroscopic measurements. We show how to use the stochastic x-ray field statistics to overcome this difficulty through correlation signals averaged over independent pulse realizations. No control is required over the spectral phase of the pulse, enabling immediate application of existing, noisy x-ray free-electron-laser pulses. The proposed stimulated Raman technique provides the combined broad observation bandwidth and high time-frequency resolution needed for the observation of elementary molecular events. A model is used to simulate chaotic free-electron-laser pulses and calculate their correlation properties. The resulting joint temporal and spectral resolution is exemplified for a molecular model system with time-dependent frequencies and for the RNA base uracil passing through a conical intersection. Ultrafast coherences, which constitute a direct signature of the nonadiabatic dynamics, are resolved. The detail and depth of physical information accessed by the proposed stochastic signal arevirtually identical to those obtained by phase-controlled pulses.
- Publication Date:
- Research Org.:
- Univ. of California, Irvine, CA (United States)
- Sponsoring Org.:
- USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF)
- OSTI Identifier:
- 1765435
- Alternate Identifier(s):
- OSTI ID: 1765343
- Grant/Contract Number:
- FG02-04ER15571; CHE-1953045
- Resource Type:
- Published Article
- Journal Name:
- Physical Review. X
- Additional Journal Information:
- Journal Name: Physical Review. X Journal Volume: 11 Journal Issue: 1; Journal ID: ISSN 2160-3308
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 74 ATOMIC AND MOLECULAR PHYSICS; Stochastic free-electron lasers; Optics; Atomic & molecular processes in external fields; Chemical Physics & Physical Chemistry; Laser spectroscopy; Nonlinear optics; X-ray beams & optics; Free-electron lasers
Citation Formats
Cavaletto, Stefano M., Keefer, Daniel, and Mukamel, Shaul. High Temporal and Spectral Resolution of Stimulated X-Ray Raman Signals with Stochastic Free-Electron-Laser Pulses. United States: N. p., 2021.
Web. doi:10.1103/PhysRevX.11.011029.
Cavaletto, Stefano M., Keefer, Daniel, & Mukamel, Shaul. High Temporal and Spectral Resolution of Stimulated X-Ray Raman Signals with Stochastic Free-Electron-Laser Pulses. United States. https://doi.org/10.1103/PhysRevX.11.011029
Cavaletto, Stefano M., Keefer, Daniel, and Mukamel, Shaul. Fri .
"High Temporal and Spectral Resolution of Stimulated X-Ray Raman Signals with Stochastic Free-Electron-Laser Pulses". United States. https://doi.org/10.1103/PhysRevX.11.011029.
@article{osti_1765435,
title = {High Temporal and Spectral Resolution of Stimulated X-Ray Raman Signals with Stochastic Free-Electron-Laser Pulses},
author = {Cavaletto, Stefano M. and Keefer, Daniel and Mukamel, Shaul},
abstractNote = {The chaotic nature of x-ray free-electron-laser pulses is a major bottleneck that has limited the joint temporal and spectral resolution of spectroscopic measurements. We show how to use the stochastic x-ray field statistics to overcome this difficulty through correlation signals averaged over independent pulse realizations. No control is required over the spectral phase of the pulse, enabling immediate application of existing, noisy x-ray free-electron-laser pulses. The proposed stimulated Raman technique provides the combined broad observation bandwidth and high time-frequency resolution needed for the observation of elementary molecular events. A model is used to simulate chaotic free-electron-laser pulses and calculate their correlation properties. The resulting joint temporal and spectral resolution is exemplified for a molecular model system with time-dependent frequencies and for the RNA base uracil passing through a conical intersection. Ultrafast coherences, which constitute a direct signature of the nonadiabatic dynamics, are resolved. The detail and depth of physical information accessed by the proposed stochastic signal arevirtually identical to those obtained by phase-controlled pulses.},
doi = {10.1103/PhysRevX.11.011029},
journal = {Physical Review. X},
number = 1,
volume = 11,
place = {United States},
year = {Fri Feb 12 00:00:00 EST 2021},
month = {Fri Feb 12 00:00:00 EST 2021}
}
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