Stochastic stimulated electronic x-ray Raman spectroscopy
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Resonant inelastic x-ray scattering (RIXS) is a well-established tool for studying electronic, nuclear, and collective dynamics of excited atoms, molecules, and solids. An extension of this powerful method to a time-resolved probe technique at x-ray free electron lasers (XFELs) to ultimately unravel ultrafast chemical and structural changes on a femtosecond time scale is often challenging, due to the small signal rate in conventional implementations at XFELs that rely on the usage of a monochromator setup to select a small frequency band of the broadband, spectrally incoherent XFEL radiation. Here, we suggest an alternative approach, based on stochastic spectroscopy, which uses the full bandwidth of the incoming XFEL pulses. Our proposed method is relying on stimulated resonant inelastic x-ray scattering, where in addition to a pump pulse that resonantly excites the system a probe pulse on a specific electronic inelastic transition is provided, which serves as a seed in the stimulated scattering process. The limited spectral coherence of the XFEL radiation defines the energy resolution in this process and stimulated RIXS spectra of high resolution can be obtained by covariance analysis of the transmitted spectra. We present a detailed feasibility study and predict signal strengths for realistic XFEL parameters for the CO molecule resonantly pumped at the O1s→π* transition. Our theoretical model describes the evolution of the spectral and temporal characteristics of the transmitted x-ray radiation, by solving the equation of motion for the electronic and vibrational degrees of freedom of the system self consistently with the propagation by Maxwell equations.
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Unaligned molecular targets at currently obtainable peak brilliances will give rise to soft x-ray Raman amplification of only a few per cent.
“As opposed to the studies in neon, where a Raman gain of up to eight orders of magnitude has been demonstrated [59], unaligned molecular targets at currently obtainable peak brilliances will give rise to soft x-ray Raman amplification of only a few per cent [62,63].”
From Roadmap of ultrafast x-ray atomic and molecular physics (2018) · cites this paper as [62]
In the soft x-ray range in gas-phase targets, the Raman gain could be strongly enhanced by several orders of magnitude by pre-aligning the molecular target.
“In the soft x-ray range in gas-phase targets the Raman gain could be strongly enhanced by several orders of magnitude by pre-aligning the molecular target [62].”
From Roadmap of ultrafast x-ray atomic and molecular physics (2018) · cites this paper as [62]
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Dorfman, K. E., Zhang, Y. A., & Mukamel, S. (2016) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.1610729113 · Cited by 10 · see citing works
Spectral monitoring at SwissFEL using a high-resolution on-line hard X-ray single-shot spectrometer
Dávid, C., Seniutinas, G., Makita, M., Rösner, B., Rehanek, J., Karvinen, P., Loehl, F., Abela, R., Patthey, L., & Juranić, P. (2021) · Journal of Synchrotron Radiation · doi:10.1107/s1600577521009619 · Cited by 9 · see citing works
Frequency-, Time-, and Wavevector-Resolved Ultrafast Incoherent Diffraction of Noisy X-ray Pulses
Asban, S., Cho, D., & Mukamel, S. (2019) · The Journal of Physical Chemistry Letters · doi:10.1021/acs.jpclett.9b00924 · Cited by 8 · see citing works
Fuller, F. D., Loukianov, A. D., Takanashi, T., You, D., Li, Y., Ueda, K., Fransson, T., Yabashi, M., Katayama, T., Weng, T., et al. (2021) · Communications Chemistry · doi:10.1038/s42004-021-00512-3 · Cited by 8 · see citing works
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Self-citationZhang, Y. A., Bennett, K., & Mukamel, S. (2018) · The Journal of Physical Chemistry A · doi:10.1021/acs.jpca.8b01762 · Cited by 5 · see citing works
Savchenko, V., Liu, J., Odelius, M., Ignatova, N., Gel’mukhanov, F., Polyutov, S. P., & Kimberg, V. (2021) · Physical Review A · doi:10.1103/physreva.104.032816 · Cited by 5 · see citing works
Self-citationXUV plasmonic waveguides by near-zero index heterostructures
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Seeded Multicolor FEL Pulses: Status and Future Plans
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Suresh, M. I., Russell, P. S. J., & Tani, F. (2020) · Optics Express · doi:10.1364/oe.405767 · Cited by 4 · see citing works
Resonant x-ray second-harmonic generation in atomic gases
Liu, J., Miron, C., Ågren, H., Polyutov, S. P., & Gel’mukhanov, F. (2019) · Physical Review A · doi:10.1103/physreva.100.063403 · Cited by 3 · see citing works
Probing Delocalized Current Densities in Selenophene by Resonant X-ray Sum-Frequency Generation
Cavaletto, S. M., & Mukamel, S. (2020) · Journal of Chemical Theory and Computation · doi:10.1021/acs.jctc.0c00886 · Cited by 3 · see citing works
High-resolution x-ray spectra of carbon monoxide reveal ultrafast dynamics induced by long UV pulse
Liu, J., Savchenko, V., Kimberg, V., Gel’mukhanov, F., & Odelius, M. (2021) · New Journal of Physics · doi:10.1088/1367-2630/ac0198 · Cited by 3 · see citing works
Self-citationX-ray free-electron lasers and their applications in ultrafast structural dynamics research
Liu, X., Liu, H., & Zhang, W. (2022) · Zhongguo kexue. Wulixue Lixue Tianwenxue · doi:10.1360/sspma-2022-0047 · Cited by 2 · see citing works
Noise Correlation Spectroscopy for spectroscopic measurements of low energy modes
Sparapassi, G., Tollerud, J. O., Glerean, F., & Fausti, D. (2018) · Conference on Lasers and Electro-Optics · doi:10.1364/cleo_at.2018.ath3o.7 · Cited by 1 · see citing works
Mapping molecular potentials using pump-probe spectroscopy of vibrational wave packets' revival
Blinov, S., Kimberg, V., Krasnov, P. O., Gel’mukhanov, F., & Polyutov, S. P. (2023) · Physical Review A · doi:10.1103/physreva.108.013104
Self-citation
- Authors
- Kimberg, V., & Rohringer, N.
- Affiliations
- Max Planck Institute for the Physics of Complex Systems (DE)
- Venue
- Structural Dynamics
- Publisher
- AIP Publishing
- Published
- 2016-02-09
- Volume
- 3
- Issue
- 3
- Pages
- 034101-034101
- ISSN
- 2329-7778 (ISSN-L)
- PMC
- PMC4752554
- OpenAlex
- W2244351764
- Cited by
- 36
- References
- 67
- Citations by year
- 2025: 1 · 2024: 1 · 2023: 5 · 2022: 4 · 2021: 8 · 2020: 3 · 2019: 5 · 2018: 5 · 2017: 1 · 2016: 3
- FWCI
- 5.23
- Type
- journal article
- Language
- en
- Open access
- gold
- doi.org
- Locations
- Structural Dynamics (publishedVersion, cc-by)
- Europe PMC (PubMed Central) (publishedVersion)
- PubMed Central (publishedVersion)
- PubMed (publishedVersion)
- DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
- Funders
- Knut och Alice Wallenbergs Stiftelse (KAW-2013.0020, 2013-0020)
- Max-Planck-Gesellschaft
- Vetenskapsrådet (2013.0020)
- Topics
- Physical Sciences › Physics and Astronomy › Radiation › X-ray Spectroscopy and Fluorescence Analysis
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Laser-Matter Interactions and Applications
- Physical Sciences › Physics and Astronomy › Radiation › Advanced X-ray Imaging Techniques
- Keywords
- X-ray free-electron laser, time-resolved spectroscopy, covariance analysis, spectral coherence, CO molecule, electronic transitions, femtosecond dynamics, ultrafast structural dynamics
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