Abstract
The authors demonstrate that the paradigm of frustrated absorption in x-ray pulses generated by x-ray free-electron lasers (XFEL) can break down at extremely high intensity. The results are of relevance for the design and the interpretation of XFEL experiments, especially when terawatt-attosecond XFEL pulses are practical.
Highlights
The advent of x-ray free-electron lasers (XFELs) [1,2,3,4,5], which provide ultrafast x-ray pulses of unprecedentedly high intensity, has revolutionized various areas, covering atomic and molecular physics, solid-state physics, photochemistry, materials science, and structural biology [6,7,8,9,10]
When an atom is exposed to intense x-ray pulses generated by x-ray free-electron lasers (XFELs), it undergoes complex ionization dynamics characterized by sequential multiphoton multiple ionization
We show that the concept of frustrated absorption, which has been established as a unique feature of the XFEL interaction with light atoms, is no longer generally valid at high x-ray fluences
Summary
The advent of x-ray free-electron lasers (XFELs) [1,2,3,4,5], which provide ultrafast x-ray pulses of unprecedentedly high intensity, has revolutionized various areas, covering atomic and molecular physics, solid-state physics, photochemistry, materials science, and structural biology [6,7,8,9,10]. One of the unique features of this sequential XFEL–matter interaction is the phenomenon of frustrated absorption [16], where the degree of ionization by x rays is reduced as the pulse duration becomes close to or shorter than lifetimes of relaxation processes. This phenomenon is counterintuitive, because in this case higher intensity (shorter pulse) results in less ionization, which is the opposite of the behavior of conventional multiphoton ionization. Our finding offers critical insight regarding XFEL–matter interactions at extreme conditions of significance for future XFEL experiments
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