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.

We introduce a wide-field magneto-optical microscope to probe magnetization dynamics with femtosecond temporal and sub-micrometer spatial resolution. We carefully calibrate the non-linear dependency between the magnetization of the sample and the detected light intensity by determining the absolute values of the magneto-optical polarization rotation. With that, an analytical transfer function is defined to directly map the recorded intensity to the corresponding magnetization, which results in significantly reduced acquisition times and relaxed computational requirements. The performance of the instrument is characterized by probing the magnetic all-optical switching dynamics of GdFe in a pump–probe experiment. The high spatial resolution of the microscope allows for accurately subdividing the laser-excited area into different fluence-regions in order to capture the strongly non-linear magnetization dynamics as a function of the optical pump intensity in a single measurement.

The advent of X-ray free-electron lasers (XFELs) has revolutionized fundamental science, from atomic to condensed matter physics, from chemistry to biology, giving researchers access to X-rays with unprecedented brightness, coherence and pulse duration. All XFEL facilities built until recently provided X-ray pulses at a relatively low repetition rate, with limited data statistics. Here, results from the first megahertz-repetition-rate X-ray scattering experiments at the Spectroscopy and Coherent Scattering (SCS) instrument of the European XFEL are presented. The experimental capabilities that the SCS instrument offers, resulting from the operation at megahertz repetition rates and the availability of the novel DSSC 2D imaging detector, are illustrated. Time-resolved magnetic X-ray scattering and holographic imaging experiments in solid state samples were chosen as representative, providing an ideal test-bed for operation at megahertz rates. Our results are relevant and applicable to any other non-destructive XFEL experiments in the soft X-ray range.

Time-resolved resonant magnetic scattering in the soft-x-ray range is a powerful tool for accessing the spatially resolved and element-specific spin dynamics in magnetic materials. So far, the application of this photon-demanding technique was limited to large-scale facilities. However, upgrades to diffraction-limited storage rings supporting only x-ray pulses beyond 100 ps, and the shift of x-ray free-electron lasers toward attosecond pulses aggravate the competition for beamtime in the picosecond time window, which is of utmost relevance for magnetism research. Here we present the development of a lab-based instrument providing sufficient photon flux up to 1.5 keV photon energy covering the soft-x-ray resonances of transition and rare-earth metal atoms. Our setup features the mandatory tunability in energy and reciprocal space in combination with sub-10 ps temporal resolution, exploiting the broadband emission of a laser-driven plasma x-ray source, which is monochromatized to about 1 eV bandwidth by a reflection zone plate. We benchmark our approach against accelerator-based soft-x-ray sources by simultaneously probing the laser-induced magnetic and structural dynamics from an antiferromagnetically coupled Fe/Cr superlattice. Our development lays the foundation for laser-driven resonant scattering experiments to study ultrafast ordering phenomena of charges, spins, and orbitals.

The vision to manipulate and control magnetism with light is driven on the one hand by fundamental questions of direct and indirect photon-spin interactions, and on the other hand by the necessity to cope with ever growing data volumes, requiring radically new approaches on how to write, read and process information. Here, we present two complementary experimental geometries to access the element-specific magnetization dynamics of complex magnetic systems via ultrafast magneto-optical spectroscopy in the extreme ultraviolet spectral range. First, we employ linearly polarized radiation of a free electron laser facility to demonstrate decoupled dynamics of the two sublattices of an FeGd alloy, a prerequisite for all-optical magnetization switching. Second, we use circularly polarized radiation generated in a laboratory-based high harmonic generation setup to show optical inter-site spin transfer in a CoPt alloy, a mechanism which only very recently has been predicted to mediate ultrafast metamagnetic phase transitions.

Time-resolved x-ray magnetic circular dichroism (XMCD) enables a unique spectroscopic view on complex spin and charge dynamics in multi-elemental magnetic materials. So far, its application in the soft-x-ray range has been limited to synchrotron-radiation sources and free-electron lasers. By combining a laser-driven plasma source with a magnetic thin-film polarizer, we generate up to 30% circular polarization in the soft-x-ray regime, enabling the first XMCD spectroscopy at the Fe L edges in a laser laboratory, to our knowledge. Our approach can be readily adapted to other transition metal L and rare earth M absorption edges, and with a temporal resolution of <10ps, a wide range of ultrafast magnetization studies can be realized.