Transmission spectroscopy of CF$_4$ molecules in intense x-ray fields

Fuente: arXiv
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Autori principali: Jin, Rui, Fouda, Adam, Magunia, Alexander, Nam, Yeonsig, Rebholz, Marc, De Fanis, Alberto, Li, Kai, Doumy, Gilles, Baumann, Thomas M., Straub, Michael, Usenko, Sergey, Ovcharenko, Yevheniy, Mazza, Tommaso, Montaño, Jacobo, Agåker, Marcus, Piancastelli, Maria Novella, Simon, Marc, Rubensson, Jan-Erik, Meyer, Michael, Young, Linda, Ott, Christian, Pfeifer, Thomas
Natura: Preprint
Pubblicazione: 2024
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author Jin, Rui
Fouda, Adam
Magunia, Alexander
Nam, Yeonsig
Rebholz, Marc
De Fanis, Alberto
Li, Kai
Doumy, Gilles
Baumann, Thomas M.
Straub, Michael
Usenko, Sergey
Ovcharenko, Yevheniy
Mazza, Tommaso
Montaño, Jacobo
Agåker, Marcus
Piancastelli, Maria Novella
Simon, Marc
Rubensson, Jan-Erik
Meyer, Michael
Young, Linda
Ott, Christian
Pfeifer, Thomas
author_facet Jin, Rui
Fouda, Adam
Magunia, Alexander
Nam, Yeonsig
Rebholz, Marc
De Fanis, Alberto
Li, Kai
Doumy, Gilles
Baumann, Thomas M.
Straub, Michael
Usenko, Sergey
Ovcharenko, Yevheniy
Mazza, Tommaso
Montaño, Jacobo
Agåker, Marcus
Piancastelli, Maria Novella
Simon, Marc
Rubensson, Jan-Erik
Meyer, Michael
Young, Linda
Ott, Christian
Pfeifer, Thomas
contents 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 multi-photon absorption processes. In this work, intense x-ray free-electron laser (XFEL) pulses at the European XFEL (EuXFEL) are combined with a gas cell and grating spectrometer for a high-intensity transmission spectroscopy study of multiphoton-induced ultrafast molecular fragmentation dynamics in CF$_4$. This approach unlocks the direct intra-pulse observation of transient fragments, including neutral atoms, by their characteristic absorption lines in the transmitted broad-band 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 few tens of femtoseconds. An isosbestic point that signifies the correlated transition between intact neutral CF$_4$ 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.
format Preprint
id arxiv_https___arxiv_org_abs_2407_04303
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Transmission spectroscopy of CF$_4$ molecules in intense x-ray fields
Jin, Rui
Fouda, Adam
Magunia, Alexander
Nam, Yeonsig
Rebholz, Marc
De Fanis, Alberto
Li, Kai
Doumy, Gilles
Baumann, Thomas M.
Straub, Michael
Usenko, Sergey
Ovcharenko, Yevheniy
Mazza, Tommaso
Montaño, Jacobo
Agåker, Marcus
Piancastelli, Maria Novella
Simon, Marc
Rubensson, Jan-Erik
Meyer, Michael
Young, Linda
Ott, Christian
Pfeifer, Thomas
Atomic Physics
Chemical Physics
Optics
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 multi-photon absorption processes. In this work, intense x-ray free-electron laser (XFEL) pulses at the European XFEL (EuXFEL) are combined with a gas cell and grating spectrometer for a high-intensity transmission spectroscopy study of multiphoton-induced ultrafast molecular fragmentation dynamics in CF$_4$. This approach unlocks the direct intra-pulse observation of transient fragments, including neutral atoms, by their characteristic absorption lines in the transmitted broad-band 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 few tens of femtoseconds. An isosbestic point that signifies the correlated transition between intact neutral CF$_4$ 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.
title Transmission spectroscopy of CF$_4$ molecules in intense x-ray fields
topic Atomic Physics
Chemical Physics
Optics
url https://arxiv.org/abs/2407.04303