In this paper, we present a spectrometer that is designed for element-specific and time-resolved transverse magneto-optic Kerr effect experiments at the high-harmonic generation pump-probe facility High Energy Laser Induced Overtone Source (HELIOS) laboratory. HELIOS delivers photons with energies between 30 eV and 72 eV with an overall time resolution of less than 40 fs. The spectrometer is based on a Rowland-circle geometry and allows for simultaneous measurements of all magnetic transition-metal elements. The setup also features easy sample transfer and alignment, and it combines high photon throughput, optimized data acquisition, and a fast switching of the magnetic field at the sample. The spectrometer performance is demonstrated by measuring the ultrafast demagnetization of permalloy. Our data are, for all practical purposes, identical to what have been reported in the earlier high-order harmonic generation work of a similar sample by Mathias et al. [Proc. Natl. Acad. Sci. U. S. A. 109, 4792-4797 (2012)], however, obtained within 15% of the acquisition time compared to their study. Furthermore, our data show a shift of the demagnetization curve of Ni relative to Fe, which has previously been interpreted as a delay of the Ni demagnetization to that of Fe [S. Mathias et al., Proc. Natl. Acad. Sci. U. S. A. 109, 4792-4797 (2012)].

The magneto-optical response of Fe and Ni during ultrafast demagnetization is studied experimentally and theoretically. We have performed pump-probe experiments in the transverse magnetooptical Kerr effect (T-MOKE) geometry using photon energies that cover the M-absorption edges of Fe and Ni between 40 to 72 eV. The asymmetry was detected by measuring the reflection of light for two different orientations of the sample magnetization. Density functional theory (DFT) was used to calculate the magneto-optical response of different magnetic configurations, representing different types of excitations: long-wavelength magnons, short wavelength magnons, and Stoner excitations. In the case of Fe, we find that the calculated asymmetry is strongly dependent on the specific type of magnetic excitation. Our modelling also reveals that during remagnetization Fe is, to a reasonable approximation, described by magnons, even though small non-linear contributions could indicate some degree of Stoner excitations as well. In contrast, we find that the calculated asymmetry in Ni is rather insensitive to the type of magnetic excitations. However, there is a weak non-linearity in the relation between asymmetry and the off-diagonal component of the dielectric tensor, which does not originate from the modifications of the electronic structure. Our experimental and theoretical results thus emphasize the need of considering a coupling between asymmetry and magnetization that may be more complex that a simple linear relationship. This insight is crucial for the microscopic interpretation of ultrafast magnetization experiments.

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Ever since its first observation, the microscopic origin of ultrafast magnetization dynamics has been actively debated. Even more questions arise when considering composite materials featuring a combination of intrinsic and proximity-induced magnetic moments. Currently, it is unknown whether the specific ultrafast dynamics of different sublattices in the popular ferromagnets consisting of 3d (Co, Fe) and 4d, 5d (Pd, Pt) transition metals are playing a crucial role in various effects, including all-optical magnetization switching. Here we investigate the element-specific dynamics of Co–Pt alloys on femtosecond and picosecond time scales using magneto-optical spectroscopy in the extended ultraviolet (EUV) region. Our results reveal that despite the proximity-induced nature of the magnetization of Pt atoms, the two sublattices in the alloy can have different responses to the optical excitation featuring distinct demagnetization rates. Additionally we show that it is important to consider the modification of magnetic anisotropy in opto-magnetic experiments as the vast majority of them are sensitive only to a single projection of the magnetic moment on the predefined axis, which may lead to experimental artifacts.

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