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Exploring the photoionization process leads to better understanding of the fundamental interactions between light and matter. Here the authors show the non-dipole contribution in the form of asymmetric photoelectron angular distribution from the ionization of argon atoms and ions.

X-ray free-electron lasers, important light sources for materials research, suffer from shot-to-shot fluctuations that necessitate complex diagnostics. Here, the authors apply machine learning to accurately predict pulse properties, using parameters that can be acquired at high-repetition rates.

Understanding the interaction of intense, femtosecond X-ray pulses with heavy atoms is crucial for gaining insights into the structure and dynamics of matter. One key aspect of nonlinear light-matter interaction was, so far, not studied systematically at free-electron lasers-its dependence on the photon energy. Here, we use resonant ion spectroscopy to map out the transient electronic structures occurring during the complex charge-up pathways of xenon. Massively hollow atoms featuring up to six simultaneous core holes determine the spectra at specific photon energies and charge states. We also illustrate how different X-ray pulse parameters, which are usually intertwined, can be partially disentangled. The extraction of resonance spectra is facilitated by the possibility of working with a constant number of photons per X-ray pulse at all photon energies and the fact that the ion yields become independent of the peak fluence beyond a saturation point. Our study lays the groundwork for spectroscopic investigations of transient atomic species in exotic, multiple-core-hole states that have not been explored previously., (© 2023. Springer Nature Limited.)

Collective behaviour is a characteristic feature in many-body systems, important for developments in fields such as magnetism, superconductivity, photonics and electronics. Recently, there has been increasing interest in the optically nonlinear response of collective excitations. Here we demonstrate how the nonlinear interaction of a many-body system with intense XUV radiation can be used as an effective probe for characterizing otherwise unresolved features of its collective response. Resonant photoionization of atomic xenon was chosen as a case study. The excellent agreement between experiment and theory strongly supports the prediction that two distinct poles underlie the giant dipole resonance. Our results pave the way towards a deeper understanding of collective behaviour in atoms, molecules and solid-state systems using nonlinear spectroscopic techniques enabled by modern short-wavelength light sources.

Many advanced applications of X-ray free-electron lasers require pulse durations and time resolutions of only a few femtoseconds. To generate these pulses and to apply them in time-resolved experiments, synchronization techniques that can simultaneously lock all independent components, including all accelerator modules and all external optical lasers, to better than the delivered free-electron laser pulse duration, are needed. Here we achieve all-optical synchronization at the soft X-ray free-electron laser FLASH and demonstrate facility-wide timing to better than 30 fs r.m.s. for 90 fs X-ray photon pulses. Crucially, our analysis indicates that the performance of this optical synchronization is limited primarily by the free-electron laser pulse duration, and should naturally scale to the sub-10 femtosecond level with shorter X-ray pulses.

Ultrafast extreme ultraviolet and X-ray free-electron lasers are set to revolutionize many domains such as bio-photonics and materials science, in a manner similar to optical lasers over the past two decades. Although their number will grow steadily over the coming decade, their complete characterization remains an elusive goal. This represents a significant barrier to their wider adoption and hence to the full realization of their potential in modern photon sciences. Although a great deal of progress has been made on temporal characterization and wavefront measurements at ultrahigh extreme ultraviolet and X-ray intensities, only few, if any progress on accurately measuring other key parameters such as the state of polarization has emerged. Here we show that by combining ultra-short extreme ultraviolet free electron laser pulses from FERMI with near-infrared laser pulses, we can accurately measure the polarization state of a free electron laser beam in an elegant, non-invasive and straightforward manner using circular dichroism.