Prior to the development of pulsed lasers, one assigned a single local temperature to the lattice, the electron gas, and the spins. With the availability of ultrafast laser sources, one can now drive the temperature of these reservoirs out of equilibrium. Thus, the solid shows new internal degrees of freedom characterized by individual temperatures of the electron gas T_{e}, the lattice T_{l} and the spins T_{s}. We demonstrate an analogous behavior in the spin polarization of a ferromagnet in an ultrafast demagnetization experiment: At the Fermi energy, the polarization is reduced faster than at deeper in the valence band. Therefore, on the femtosecond time scale, the magnetization as a macroscopic quantity does not provide the full picture of the spin dynamics: The spin polarization separates into different parts similar to how the single temperature paradigm changed with the development of ultrafast lasers.

Time resolved pump probe experiments with ultra short infrared pump and x-ray photoemission probe pulses require a stable magnetic reference system with reproducible magnetic properties. In search of such a system we found in iron on tungsten an ideal sample. The coercive field of this system remains constant at 12.2±1 Oe between 15 and 25 monolayers. Kerr effect measurements and scanning electron microscopy with polarization analysis images prove that the magnetization switches from single domain to single domain state. Capping with Au increases the coercive field and prevents the Fe layer from deterioration.

Surprisingly, if a ferromagnet is exposed to an ultrafast laser pulse, its apparent magnetization is reduced within less than a picosecond. Up to now, the total magnetization, i.e., the average spin polarization of the whole valence band, was not detectable on a sub-picosecond time scale. Here, we present experimental data, confirming the ultrafast reduction of the total magnetization. Soft x-ray pulses from the free electron laser in Hamburg (FLASH) extract polarized cascade photoelectrons from an iron layer excited by a femtosecond laser pulse. The spin polarization of the emitted electrons is detected by a Mott spin polarimeter.

Ultrathin Fe films on Cu(1 0 0) are self-organized into stripes of opposite perpendicular magnetization. The process of self-organization involves stripe-nucleation and stripe-creep. We present images of nucleation and creep at the micrometre scale. These observations provide evidence of both quenched and self-induced disorder in a system with competing interactions.

The laser-induced demagnetization of a ferromagnet is caused by the temperature of the electron gas as well as the lattice temperature. For long excitation pulses, the two reservoirs are in thermal equilibrium. In contrast to a picosecond laser pulse, a femtosecond pulse causes a non-equilibrium between the electron gas and the lattice. By pump pulse length dependent optical measurements, we find that the magnetodynamics in Ni caused by a picosecond laser pulse can be reconstructed from the response to a femtosecond pulse. The mechanism responsible for demagnetization on the picosecond time scale is therefore contained in the femtosecond demagnetization experiment.

The ultrafast demagnetization process allows for the generation of femtosecond spin current pulses. Here, we present a thermodynamic model of the spin current generation process, based on the chemical potential gradients as the driving force for the spin current. We demonstrate that the laser-induced spin current can be estimated by an easy to understand diffusion model.

Spin-resolved photoemission is one of the most direct ways of measuring the magnetization of a ferromagnet. If all valence band electrons contribute, the measured average spin polarization is proportional to the magnetization. This is even the case if electronic excitations are present, and thus is of particular interest for studying the response of the magnetization to a pump laser pulse. Here, we demonstrate the feasibility of ultrafast spin-resolved photoemission using free electron laser (FEL) radiation and investigate the effect of space charge on the detected spin polarization. The sample is exposed to the radiation of the FEL FLASH in Hamburg. Surprisingly, the measured spin polarization depends on the fluence of the FEL radiation: a higher FEL fluence reduces the Content from this work may be used under the terms of the Creative Commons Attribution 3.0 licence. Any further distribution of this work must maintain attribution to the author(s) and the title of the work, journal citation and DOI. measured spin polarization. Space-charge simulations can explain this effect. These findings have consequences for future spin-polarized photoemission experiments using pulsed photon sources.Keywords: spin-polarized photoemission, free electron laser radiation, space charge New J. Phys. 16 (2014) 043031 A Fognini et al New J. Phys. 16 (2014) 043031 A Fognini et al 6 New J. Phys. 16 (2014) 043031 A Fognini et al 7

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