Ultrashort optical pulses can trigger a variety of non-equilibrium processes in magnetic thin films affecting electrons and spins on femtosecond timescales. In order to probe the charge and magnetic degrees of freedom simultaneously, we developed an X-ray streaking technique that has the advantage of providing a jitter-free picture of absorption cross-section changes. In this paper, we present an experiment based on this approach, which we performed using five photon probing energies at the Ni $M_{2,3}$-edges. This allowed us to retrieve the absorption and magnetic circular dichroism time traces, yielding detailed information on transient modifications of electron and spin populations close to the Fermi level. Our findings suggest that the observed absorption and magnetic circular dichroism dynamics both depend on the extreme ultraviolet (XUV) probing wavelength, and can be described, at least qualitatively, by assuming ultrafast energy shifts of the electronic and magnetic elemental absorption resonances, as reported in recent work. However, our analysis also hints at more complex changes, highlighting the need for further experimental and theoretical studies in order to gain a thorough understanding of the interplay of electronic and spin degrees of freedom in optically excited magnetic thin films.

We use time-resolved resonant magnetic scattering experiments to investigate the laser induced demagnetization of Co/Pt multilayers with large perpendicular magnetic anisotropy. Our pump-probe approach, which relies on extreme ultraviolet pulses obtained via high-harmonic generation, allows us to monitor the temporal evolution of the system in an element-selective fashion, thus to disentangle the contributions from permanent and proximity-induced magnetic moments. By analyzing the data gathered at the Co $M_{2,3}$ and Pt O₃ edges, we are able to show that after femtosecond laser irradiation, both components display a very similar loss of magnetic order, with almost identical demagnetization amplitudes and characteristic times, but a small delay (10–20 fs) of the Pt magnetization quenching with respect to Co. Comparing our experiments with literature results, therefore, suggests that in these 3d–5d multilayers and alloys, the different constituents remain strongly coupled after optical excitation; no matter whether the thin films possess a preferred in-plane or out-of-plane easy magnetization direction.

The potential of the two-color mode implemented at the FERMI free-electron laser (FEL) source for pumping and probing selectively different atomic species has been demonstrated by time-resolved scattering experiments with permalloy (FeNi alloy) and NiFe₂O₄ samples. We monitored the ultra-fast demagnetization of Ni induced by the pump FEL pulse, by tuning the linearly-polarized FEL probe pulse to the Ni-3p resonance and measuring the scattered intensity in the transverse magneto-optical Kerr effect geometry. The measurements were performed by varying the intensity of the FEL pump pulse, tuning its wavelength to and off of the Fe-3p resonance, and by spanning the FEL probe pulse delays across the 300–900 fs range. The obtained results have evidenced that for the case of NiFe₂O₄, there is a sensible difference in the magnetic response at the Ni site when the pump pulse causes electronic excitations at the Fe site.

Instruments based on the magneto-optical Kerr effect are routinely used to probe surface magnetic properties. These tools rely on the characterization of the polarization state of reflected light from the sample to collect information on its magnetization. Here, we present a theoretical optimization of common setups based on the magneto-optical Kerr effect. A detection scheme based on a simple analyzer and photodetector and one made from a polarizing beam splitter and balanced photodetectors are considered. The effect of including a photoelastic modulator (PEM) and a lock-in amplifier to detect the signal at harmonics of the modulating frequency is studied. Jones formalism is used to derive general expressions that link the intensity of the measured signal to the magneto-optical Fresnel reflection coefficients for any orientation of the polarizing optical components. Optimal configurations are then defined as those that allow measuring the Kerr rotation and ellipticity while minimizing nonmagnetic contributions from the diagonal Fresnel coefficients in order to improve the signal-to-noise ratio (SNR). The expressions show that with the PEM, setups based on polarizing beam splitters inherently offer a twofold higher signal than commonly used analyzers, and the experimental results confirm that the SNR is improved by more than 150%. Furthermore, we find that while all proposed detection schemes measure Kerr effects, only those with polarizing beam splitters allow measuring the Kerr rotation directly when no modulator is included. This accommodates, for instance, time-resolved measurements at relatively low laser pulse repetition rates. Ultrafast demagnetization measurements are presented as an example of such applications.

It was shown recently that the Fe magnetization reversal in the Fe/MnAs/GaAs(001) epitaxial system, attained by temperature control of the regular stripe pattern of the MnAs α- and β-phases, can also be driven by an ultrashort optical laser pulse. In the present time-resolved scattering experiment, we address the dynamics of the MnAs α-β self-organized stripe pattern induced by a 100 fs optical laser pulse, using as a probe the XUV radiation from the FERMI free-electron laser. We observe a loss in the diffraction intensity from the ordered α-β stripes that occurs at two characteristic timescales in the range of ~10⁻¹² and ~10⁻¹⁰ s. We associate the first intensity drop with ultrafast electron-lattice energy exchange processes within the laser-MnAs interaction volume and the second with thermal diffusion towards the MnAs/GaAs interface. With the support of model calculations, the observed dynamics are interpreted in terms of the formation of a laterally homogeneous MnAs overlayer, the thickness of which evolves in time, correlating the MnAs microstructure dynamics with the Fe magnetization response.