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

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Electron population dynamics in resonant non-linear x-ray absorption in nickel at a free-electron laser
Structural Dynamics ( IF 3.670 ) Pub Date : 2023-10-11 , DOI: 10.1063/4.0000206
Robin Y Engel , Oliver Alexander ₁ , Kaan Atak ₂ , Uwe Bovensiepen , Jens Buck , Robert Carley ₃ , Michele Cascella ₄ , Valentin Chardonnet ₅ , Gheorghe Sorin Chiuzbaian ₅ , Christian David ₆ , Florian Döring ₆ , Andrea Eschenlohr ₇ , Natalia Gerasimova ₃ , Frank de Groot ₈ , Loïc Le Guyader ₃ , Oliver S Humphries ₃ , Manuel Izquierdo ₃ , Emmanuelle Jal ₅ , Adam Kubec ₆ , Tim Laarmann , Charles-Henri Lambert ₉ , Jan Lüning ₁₀ , Jonathan P Marangos ₁ , Laurent Mercadier ₃ , Giuseppe Mercurio ₃ , Piter S Miedema ₂ , Katharina Ollefs ₇ , Bastian Pfau ₁₁ , Benedikt Rösner ₆ , Kai Rossnagel , Nico Rothenbach ₇ , Andreas Scherz ₃ , Justine Schlappa ₃ , Markus Scholz , Jan O Schunck , Kiana Setoodehnia ₃ , Christian Stamm , Simone Techert , Sam M Vinko , Heiko Wende ₇ , Alexander A Yaroslavtsev ₁₂ , Zhong Yin , Martin Beye

Affiliation

Department of Physics, Imperial College London, London, United Kingdom.
Deutsches Elektronen-Synchrotron DESY, Germany.
European XFEL, Schenefeld, Germany.
MAX IV Laboratory, Lund University, Lund, Sweden.
Sorbonne Université, CNRS, Laboratoire de Chimie Physique-Matière et Rayonnement LCPMR, Paris, France.
Paul Scherrer Institut, Villigen, Switzerland.
Faculty of Physics and Center for Nanointegration Duisburg-Essen CENIDE, University of Duisburg-Essen, Duisburg, Germany.
Debye Institute for Nanomaterials Science, Inorganic Chemistry and Catalysis, Utrecht University, Utrecht, The Netherlands.
Department of Materials, ETH Zurich, Zurich, Switzerland.
Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Berlin, Germany.
Max Born Institute for Nonlinear Optics and Short Pulse Spectroscopy, Berlin, Germany.
Department of Physics and Astronomy, Uppsala University, Uppsala, Sweden.

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 L3-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.

更新日期：2023-10-11

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