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.
Characterization of the electronic band structure of solid state materials is routinely performed using photoemission spectroscopy. Recent advancements in short-wavelength light sources and electron detectors give rise to multidimensional photoemission spectroscopy, allowing parallel measurements of the electron spectral function simultaneously in energy, two momentum components and additional physical parameters with single-event detection capability. Efficient processing of the photoelectron event streams at a rate of up to tens of megabytes per second will enable rapid band mapping for materials characterization. We describe an open-source workflow that allows user interaction with billion-count single-electron events in photoemission band mapping experiments, compatible with beamlines at 3rd and 4rd generation light sources and table-top laser-based setups. The workflow offers an end-to-end recipe from distributed operations on single-event data to structured formats for downstream scientific tasks and storage to materials science database integration. Both the workflow and processed data can be archived for reuse, providing the infrastructure for documenting the provenance and lineage of photoemission data for future high-throughput experiments.
Ultrafast demagnetization of ferromagnetic metals can be achieved by a heat pulse propagating in the electron gas of a non-magnetic metal layer, which absorbs a pump laser pulse. Demagnetization by electronic heating is investigated on samples with different thicknesses of the absorber layer on nickel. This allows us to separate the contribution of thermalized hot electrons compared to non-thermal electrons. An analytical model describes the demagnetization amplitude as a function of the absorber thickness. The observed change of demagnetization time can be reproduced by diffusive heat transport through the absorber layer.
We show that the presence of a transiently excited hot electron gas in graphene leads to a substantial broadening of the C 1s line probed by time-resolved x-ray photoemission spectroscopy. The broadening is found to be caused by an exchange of energy and momentum between the photoemitted core electron and the hot electron gas, rather than by vibrational excitations. This interpretation is supported by a quantitative line-shape analysis that accounts for the presence of the excited electrons. Fitting the spectra to this model directly yields the electronic temperature of the system, in good agreement with electronic temperature values obtained from valence band data. Furthermore, we show how the momentum change of the outgoing core electrons leads to a detectable but very small change in the time-resolved photoelectron diffraction pattern and to a nearly complete elimination of the core level binding energy variation associated with the presence of a narrow σ band in the C 1s state.
In this paper, the design and functionalities of the high-throughput TELL sample exchange system for macromolecular crystallography is presented. TELL was developed at the Paul Scherrer Institute with a focus on speed, storage capacity and reliability to serve the three macromolecular crystallography beamlines of the Swiss Light Source, as well as the SwissMX instrument at SwissFEL.
Most experiments on ultrafast magnetodynamics have been conducted using the magneto-optical Kerr effect. Here, we compare the Kerr effect's magnetic sensitivity to the spin dynamics measured by photoemission. The magnetization dynamics on an Fe/W(110) thin film are probed by spin-resolved photoemission spectroscopy and the Kerr effect. The results reveal similarities between the spin dynamics at low binding energy and the response probed by the Kerr effect. Therefore, the Kerr effect probes states relevant for spin transport and spin flips but may not be sensitive to the entire magnetic moment in femtosecond spin dynamics experiments.
The ultrafast demagnetization effect allows for the generation of femtosecond spin current pulses, which is expected to extend the fields of spin transport and spintronics to the femtosecond time domain. thus far, directly observing the spin polarization induced by spin injection on the femtosecond time scale has not been possible. Herein, we present time-and spin-resolved photoemission results of spin injection from a laser-excited ferromagnet into a thin gold layer. The injected spin polarization is aligned along the magnetization direction of the underlying ferromagnet. Its decay time depends on the thickness of the gold layer, indicating that transport as well as storage of spins are relevant. this capacitive aspect of spin transport may limit the speed of future spintronic devices.
The laser-driven ultrafast demagnetization effect is one of the long-standing problems in solid-state physics. The time scale is given not only by the transfer of energy, but also by the transport of angular momentum away from the spin system. Through a double-pulse experiment resembling two-dimensional spectroscopy, we separate the different pathways by their nonlinear properties. We find (a) that the loss of magnetization within 400 fs is not affected by the previous excitations (linear process), and (b) we observe a picosecond demagnetization contribution that is strongly affected by the previous excitations. Our experimental approach is useful not only for studying femtosecond spin dynamics, but can also be adapted to other problems in solid-state dynamics.
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