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Electron population dynamics in resonant non-linear x-ray absorption in nickel at a free-electron laser

Engel, Robin Y. ; Alexander, Oliver ; Atak, Kaan ; Bovensiepen, Uwe ; Buck, Jens ; Carley, Robert ; Cascella, Michele LU orcid ; Chardonnet, Valentin ; Chiuzbaian, Gheorghe Sorin and David, Christian , et al. (2023) In Structural Dynamics 10(5).
Abstract

Free-electron lasers provide bright, ultrashort, and monochromatic x-ray pulses, enabling novel spectroscopic measurements not only with femtosecond temporal resolution: The high fluence of their x-ray pulses can also easily enter the regime of the non-linear x-ray-matter interaction. Entering this regime necessitates a rigorous analysis and reliable prediction of the relevant non-linear processes for future experiment designs. Here, we show non-linear changes in the L 3 -edge absorption of metallic nickel thin films, measured with fluences up to 60 J/cm2. We present a simple but predictive rate model that quantitatively describes spectral changes based on the evolution of electronic populations within the pulse duration.... (More)

Free-electron lasers provide bright, ultrashort, and monochromatic x-ray pulses, enabling novel spectroscopic measurements not only with femtosecond temporal resolution: The high fluence of their x-ray pulses can also easily enter the regime of the non-linear x-ray-matter interaction. Entering this regime necessitates a rigorous analysis and reliable prediction of the relevant non-linear processes for future experiment designs. Here, we show non-linear changes in the L 3 -edge absorption of metallic nickel thin films, measured with fluences up to 60 J/cm2. We present a simple but predictive rate model that quantitatively describes spectral changes based on the evolution of electronic populations within the pulse duration. Despite its simplicity, the model reaches good agreement with experimental results over more than three orders of magnitude in fluence, while providing a straightforward understanding of the interplay of physical processes driving the non-linear changes. Our findings provide important insights for the design and evaluation of future high-fluence free-electron laser experiments and contribute to the understanding of non-linear electron dynamics in x-ray absorption processes in solids at the femtosecond timescale.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Structural Dynamics
volume
10
issue
5
article number
054501
publisher
American Institute of Physics (AIP)
external identifiers
  • scopus:85174826392
  • pmid:37841290
ISSN
2329-7778
DOI
10.1063/4.0000206
language
English
LU publication?
yes
id
b9473544-4787-46cd-be3f-b9e8ac58c41b
date added to LUP
2024-01-12 08:45:13
date last changed
2024-04-27 04:11:32
@article{b9473544-4787-46cd-be3f-b9e8ac58c41b,
  abstract     = {{<p>Free-electron lasers provide bright, ultrashort, and monochromatic x-ray pulses, enabling novel spectroscopic measurements not only with femtosecond temporal resolution: The high fluence of their x-ray pulses can also easily enter the regime of the non-linear x-ray-matter interaction. Entering this regime necessitates a rigorous analysis and reliable prediction of the relevant non-linear processes for future experiment designs. Here, we show non-linear changes in the L 3 -edge absorption of metallic nickel thin films, measured with fluences up to 60 J/cm<sup>2</sup>. We present a simple but predictive rate model that quantitatively describes spectral changes based on the evolution of electronic populations within the pulse duration. Despite its simplicity, the model reaches good agreement with experimental results over more than three orders of magnitude in fluence, while providing a straightforward understanding of the interplay of physical processes driving the non-linear changes. Our findings provide important insights for the design and evaluation of future high-fluence free-electron laser experiments and contribute to the understanding of non-linear electron dynamics in x-ray absorption processes in solids at the femtosecond timescale.</p>}},
  author       = {{Engel, Robin Y. and Alexander, Oliver and Atak, Kaan and Bovensiepen, Uwe and Buck, Jens and Carley, Robert and Cascella, Michele and Chardonnet, Valentin and Chiuzbaian, Gheorghe Sorin and David, Christian and Döring, Florian and Eschenlohr, Andrea and Gerasimova, Natalia and Groot, Frank de and Guyader, Loïc Le and Humphries, Oliver S. and Izquierdo, Manuel and Jal, Emmanuelle and Kubec, Adam and Laarmann, Tim and Lambert, Charles Henri and Lüning, Jan and Marangos, Jonathan P. and Mercadier, Laurent and Mercurio, Giuseppe and Miedema, Piter S. and Ollefs, Katharina and Pfau, Bastian and Rösner, Benedikt and Rossnagel, Kai and Rothenbach, Nico and Scherz, Andreas and Schlappa, Justine and Scholz, Markus and Schunck, Jan O. and Setoodehnia, Kiana and Stamm, Christian and Techert, Simone and Vinko, Sam M. and Wende, Heiko and Yaroslavtsev, Alexander A. and Yin, Zhong and Beye, Martin}},
  issn         = {{2329-7778}},
  language     = {{eng}},
  month        = {{09}},
  number       = {{5}},
  publisher    = {{American Institute of Physics (AIP)}},
  series       = {{Structural Dynamics}},
  title        = {{Electron population dynamics in resonant non-linear x-ray absorption in nickel at a free-electron laser}},
  url          = {{http://dx.doi.org/10.1063/4.0000206}},
  doi          = {{10.1063/4.0000206}},
  volume       = {{10}},
  year         = {{2023}},
}