Transmission spectroscopy of CF4 molecules in intense x-ray fields
(2025) In Physical Review A 111(1).- Abstract
The nonlinear interaction of x rays with matter is at the heart of understanding and controlling ultrafast molecular dynamics from an atom-specific viewpoint, providing new scientific and analytical opportunities to explore the structure and dynamics of small quantum systems. At increasingly high x-ray intensity, the sensitivity of ultrashort x-ray pulses to specific electronic states and emerging short-lived transient intermediates is of particular relevance for our understanding of fundamental multiphoton absorption processes. In this work, intense x-ray free-electron laser (XFEL) pulses at the European XFEL are combined with a gas cell and grating spectrometer for a high-intensity transmission spectroscopy study of... (More)
The nonlinear interaction of x rays with matter is at the heart of understanding and controlling ultrafast molecular dynamics from an atom-specific viewpoint, providing new scientific and analytical opportunities to explore the structure and dynamics of small quantum systems. At increasingly high x-ray intensity, the sensitivity of ultrashort x-ray pulses to specific electronic states and emerging short-lived transient intermediates is of particular relevance for our understanding of fundamental multiphoton absorption processes. In this work, intense x-ray free-electron laser (XFEL) pulses at the European XFEL are combined with a gas cell and grating spectrometer for a high-intensity transmission spectroscopy study of multiphoton-induced ultrafast molecular fragmentation dynamics in CF4. This approach unlocks the direct intrapulse observation of transient fragments, including neutral atoms, by their characteristic absorption lines in the transmitted broadband x-ray spectrum. The dynamics with and without initially producing fluorine K-shell holes are studied by tuning the central photon energy. The absorption spectra are measured at different FEL intensities to observe nonlinear effects. Transient isolated fluorine atoms and ions are spectroscopically recorded within the ultrashort pulse duration of a few tens of femtoseconds. An isosbestic point that signifies the correlated transition between intact neutral CF4 molecules and charged atomic fragments is observed near the fluorine K edge. The dissociation dynamics and the multiphoton absorption-induced dynamics encoded in the spectra are theoretically interpreted. Overall, this study demonstrates the potential of high-intensity x-ray transmission spectroscopy to study ultrafast molecular dynamics with sensitivity to specific intermediate species and their electronic structure.
(Less)
- author
- organization
- publishing date
- 2025-01
- type
- Contribution to journal
- publication status
- published
- subject
- in
- Physical Review A
- volume
- 111
- issue
- 1
- article number
- 012808
- publisher
- American Physical Society
- external identifiers
-
- scopus:85215829146
- ISSN
- 2469-9926
- DOI
- 10.1103/PhysRevA.111.012808
- language
- English
- LU publication?
- yes
- additional info
- Publisher Copyright: © 2025 authors. Published by the American Physical Society. Published by the American Physical Society under the terms of the "https://creativecommons.org/licenses/by/4.0/"Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI. Open access publication funded by Max Planck Society.
- id
- 189f8b6c-3b13-431c-97e4-886a1eac1f44
- date added to LUP
- 2025-04-22 15:07:10
- date last changed
- 2025-04-22 15:08:12
@article{189f8b6c-3b13-431c-97e4-886a1eac1f44,
abstract = {{<p>The nonlinear interaction of x rays with matter is at the heart of understanding and controlling ultrafast molecular dynamics from an atom-specific viewpoint, providing new scientific and analytical opportunities to explore the structure and dynamics of small quantum systems. At increasingly high x-ray intensity, the sensitivity of ultrashort x-ray pulses to specific electronic states and emerging short-lived transient intermediates is of particular relevance for our understanding of fundamental multiphoton absorption processes. In this work, intense x-ray free-electron laser (XFEL) pulses at the European XFEL are combined with a gas cell and grating spectrometer for a high-intensity transmission spectroscopy study of multiphoton-induced ultrafast molecular fragmentation dynamics in CF4. This approach unlocks the direct intrapulse observation of transient fragments, including neutral atoms, by their characteristic absorption lines in the transmitted broadband x-ray spectrum. The dynamics with and without initially producing fluorine K-shell holes are studied by tuning the central photon energy. The absorption spectra are measured at different FEL intensities to observe nonlinear effects. Transient isolated fluorine atoms and ions are spectroscopically recorded within the ultrashort pulse duration of a few tens of femtoseconds. An isosbestic point that signifies the correlated transition between intact neutral CF4 molecules and charged atomic fragments is observed near the fluorine K edge. The dissociation dynamics and the multiphoton absorption-induced dynamics encoded in the spectra are theoretically interpreted. Overall, this study demonstrates the potential of high-intensity x-ray transmission spectroscopy to study ultrafast molecular dynamics with sensitivity to specific intermediate species and their electronic structure.</p>}},
author = {{Jin, Rui and Fouda, Adam and Magunia, Alexander and Nam, Yeonsig and Rebholz, Marc and De Fanis, Alberto and Li, Kai and Doumy, Gilles and Baumann, Thomas M. and Straub, Michael and Usenko, Sergey and Ovcharenko, Yevheniy and Mazza, Tommaso and Montaño, Jacobo and Agåker, Marcus and Piancastelli, Maria Novella and Simon, Marc and Rubensson, Jan Erik and Meyer, Michael and Young, Linda and Ott, Christian and Pfeifer, Thomas}},
issn = {{2469-9926}},
language = {{eng}},
number = {{1}},
publisher = {{American Physical Society}},
series = {{Physical Review A}},
title = {{Transmission spectroscopy of CF4 molecules in intense x-ray fields}},
url = {{http://dx.doi.org/10.1103/PhysRevA.111.012808}},
doi = {{10.1103/PhysRevA.111.012808}},
volume = {{111}},
year = {{2025}},
}