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Nowadays, a wealth of information on ultrafast magnetization dynamics of thin ferromagnetic films exists in the literature. Information is, however, scarce on bulk single crystals, which may be especially important for the case of multi-sublattice systems. In Heusler compounds, representing prominent examples for such multi-sublattice systems, off-stoichiometry and degree of order can significantly change the magnetic properties of thin films, while bulk single crystals may be generally produced with a much more well-defined stoichiometry and a higher degree of ordering. A careful characterization of the local structure of thin films versus bulk single crystals combined with ultrafast demagnetization studies can, thus, help to understand the impact of stoichiometry and order on ultrafast spin dynamics.Here, we present a comparative study of the structural ordering and magnetization dynamics for thin films and bulk single crystals of the family of Heusler alloys with composition Co2Fe1 − xMnxSi. The local ordering is studied by 59Co nuclear magnetic resonance (NMR) spectroscopy, while the time-resolved magneto-optical Kerr effect gives access to the ultrafast magnetization dynamics. In the NMR studies we find significant differences between bulk single crystals and thin films, both regarding local ordering and stoichiometry. The ultrafast magnetization dynamics, on the other hand, turns out to be mostly unaffected by the observed structural differences, especially on the time scale of some hundreds of femtoseconds. These results confirm hole-mediated spin-flip processes as the main mechanism for ultrafast demagnetization and the robustness of this demagnetization channel against defect states in the minority band gap as well as against the energetic position of the band gap with respect to the Fermi energy. The very small differences observed in the magnetization dynamics on the picosecond time-scale, on the other hand, can be explained by considering the differences in the electronic structure at the Fermi energy and in the heat diffusion of thin films and bulk crystals.

Co2FeSi is predicted to be a half-metallic ferromagnet with an extraordinary high magnetic moment and Curie temperature. However, a low tunnel magneto-resistance ratio, a lower spin polarization and a lower magnetic moment were experimentally observed in thin film samples. Consequently, thin Co2FeSi films of different groups were studied using spin-echo nuclear magnetic resonance (NMR). NMR probes the local hyperfine fields of the active atoms, which strongly depend on the local environment. NMR is thus able to reveal the next neighbouring shells of the Co-59 nuclei in the Co2FeSi thin films. As expected, our NMR study shows the main resonance line corresponding to Co-59 nuclei in the L2(1) environment but also additional resonance lines at the high frequency site of the main line with a spacing between adjacent resonance lines of 32 MHz. The additional resonance lines correspond to Co-59 with more Fe next neighbours than expected for the L2(1) type ordering, which is interpreted as the formation of an off-stoichiometric film yielded by sputtering from a stoichiometric target. The analysis of the NMR data and a comparison with off-stoichiometric bulk samples reveals the composition of the thin films to be about Co2Fe(Si0.92Fe0.08). This off-stoichiometry might explain the observed deviations from the expected behaviour.