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Extreme ultraviolet (EUV) photon beam characterization techniques, Hartmann wavefront sensing and single shot ablation imprinting, were compared along the caustic of a tightly focused free-electron laser (FEL) beam at beamline FL24 of FLASH2, the Free-electron LASer in Hamburg at DESY. The transverse coherence of the EUV FEL was determined by a Young's double pinhole experiment and used in a back-propagation algorithm which includes partial coherence to calculate the beam intensity profiles along the caustic from the wavefront measurements. A very good agreement of the profile structure and size is observed for different wavelengths between the back-propagated profiles, an indirect technique, and ablation imprints. As a result, the Hartmann wavefront sensor including its software MrBeam is a very useful, single shot pulse resolved and fast tool for non-invasive determination of focal spot size and shape and also for beam profiles along the caustic.

A change of orbital state alters the coupling between ions and their surroundings drastically. Orbital excitations are hence key to understand and control interaction of ions. Rare-earth elements with strong magneto-crystalline anisotropy (MCA) are important ingredients for magnetic devices. Thus, control of their localized 4 f magnetic moments and anisotropy is one major challenge in ultrafast spin physics. With time-resolved x-ray absorption and resonant inelastic scattering experiments, we show for Tb metal that 4 f -electronic excitations out of the ground-state multiplet occur after optical pumping. These excitations are driven by inelastic 5 d -4 f -electron scattering, altering the 4 f -orbital state and consequently the MCA with important implications for magnetization dynamics in 4 f -metals and more general for the excitation of localized electronic states in correlated materials.

Identifying the microscopic nature of non-equilibrium energy transfer mechanisms among electronic, spin, and lattice degrees of freedom is central to understanding ultrafast phenomena such as manipulating magnetism on the femtosecond timescale. Here, we use time- and angle-resolved photoemission spectroscopy to go beyond the often-used ensemble-averaged view of non-equilibrium dynamics in terms of quasiparticle temperature evolutions. We show for ferromagnetic Ni that the non-equilibrium electron and spin dynamics display pronounced variations with electron momentum, whereas the magnetic exchange interaction remains isotropic. This highlights the influence of lattice-mediated scattering processes and opens a pathway toward unraveling the still elusive microscopic mechanism of spin-lattice angular momentum transfer.

Methods of ablation imprints in solid targets are widely used to characterize focused X-ray laser beams due to a remarkable dynamic range and resolving power. A detailed description of intense beam profiles is especially important in high-energy-density physics aiming at nonlinear phenomena. Complex interaction experiments require an enormous number of imprints to be created under all desired conditions making the analysis demanding and requiring a huge amount of human work. Here, for the first time, we present ablation imprinting methods assisted by deep learning approaches. Employing a multi-layer convolutional neural network (U-Net) trained on thousands of manually annotated ablation imprints in poly(methyl methacrylate), we characterize a focused beam of beamline FL24/FLASH2 at the Free-electron laser in Hamburg. The performance of the neural network is subject to a thorough benchmark test and comparison with experienced human analysts. Methods presented in this Paper pave the way towards a virtual analyst automatically processing experimental data from start to end.

We present a femtosecond time-resolved optical pump-soft x-ray probe photoemission study in which we follow the dynamics of charge transfer at the interface of water and anatase TiO_{2}(101). By combining our observation of transient oxygen O 1s core level peak shifts at submonolayer water coverages with Ehrenfest molecular dynamics simulations we find that ultrafast interfacial hole transfer from TiO_{2} to molecularly adsorbed water is completed within the 285 fs time resolution of the experiment. This is facilitated by the formation of a new hydrogen bond between an O_{2c} site at the surface and a physisorbed water molecule. The calculations fully corroborate our experimental observations and further suggest that this process is preceded by the efficient trapping of the hole at the surface of TiO_{2} by hydroxyl species (-OH), that form following the dissociative adsorption of water. At a water coverage exceeding a monolayer, interfacial charge transfer is suppressed. Our findings are directly applicable to a wide range of photocatalytic systems in which water plays a critical role.

Wide-band-gap insulators such as NiO offer the exciting prospect of coherently manipulating electronic correlations with strong optical fields. Contrary to metals where rapid dephasing of optical excitation via electronic processes occurs, the sub-gap excitation in charge-transfer insulators has been shown to couple to low-energy bosonic excitations. However, it is currently unknown if the bosonic dressing field is composed of phonons or magnons. Here we use the prototypical charge-transfer insulator NiO to demonstrate that 1.5 eV sub-gap optical excitation leads to a renormalised NiO band-gap in combination with a significant reduction of the antiferromagnetic order. We employ element-specific X-ray reflectivity at the FLASH free-electron laser to demonstrate the reduction of the upper band-edge at the O 1s-2p core-valence resonance (K-edge) whereas the antiferromagnetic order is probed via X-ray magnetic linear dichroism (XMLD) at the Ni 2p-3d resonance (L 2 -edge). Comparing the transient XMLD spectral line shape to ground-state measurements allows us to extract a spin temperature rise of 65 ± 5 K for time delays longer than 400 fs while at earlier times a non-equilibrium spin state is formed. We identify transient mid-gap states being formed during the first 200 fs accompanied by a band-gap reduction lasting at least up to the maximum measured time delay of 2.4 ps. Electronic structure calculations indicate that magnon excitations significantly contribute to the reduction of the NiO band gap.

Extending nonlinear spectroscopic techniques into the x-ray domain promises unique insight into photoexcited charge dynamics, which are of fundamental and applied interest. We report on the observation of a third-order nonlinear process in lithium fluoride (LiF) at a free-electron laser. Exploring the yield of four-wave mixing (FWM) in resonance with transitions to strongly localized core exciton states versus delocalized Bloch states, we find resonant FWM to be a sensitive probe for the degree of charge localization: Substantial sum- and difference-frequency generation is observed exclusively when in a one- or three-photon resonance with a LiF core exciton, with a dipole forbidden transition affecting details of the nonlinear response. Our reflective geometry-based approach to detect FWM signals enables the study of a wide variety of condensed matter sample systems, provides atomic selectivity via resonant transitions, and can be easily scaled to shorter wavelengths at free-electron x-ray lasers.