Detection of femtosecond spin voltage pulses in a thin iron film.

We present experimental evidence of a spin voltage-a difference between the chemical potentials of the two spin directions-in a thin iron film based on spin- and time-resolved photoemission spectroscopy. This voltage is the driving force for a spin current during the ultrafast demagnetization of the sample. The observed magnitude is on the order of 50 mV, a value that is quite consistent with predictions based on particle conservation and persists for approximately 100 fs.

Detection of femtosecond spin injection into a thin gold layer by time and spin resolved photoemission.

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.

Compact setup for spin-, time-, and angle-resolved photoemission spectroscopy.

We present a compact setup for spin-, time-, and angle-resolved photoemission spectroscopy. A 10 kHz titanium sapphire laser system delivers pulses of 20 fs duration, which drive a high harmonic generation-based source for ultraviolet photons at 21 eV for photoemission. The same laser also excites the sample for pump-probe experiments. Emitted electrons pass through a hemispherical energy analyzer and a spin-filtering element. The latter is based on spin-polarized low-energy electron diffraction on an Au-passivated iridium crystal. The performance of the measurement system is discussed in terms of the resolution and efficiency of the spin filter, which are higher than those for Mott-based techniques.

Time- and momentum-resolved photoemission studies using time-of-flight momentum microscopy at a free-electron laser.

Time-resolved photoemission with ultrafast pump and probe pulses is an emerging technique with wide application potential. Real-time recording of nonequilibrium electronic processes, transient states in chemical reactions, or the interplay of electronic and structural dynamics offers fascinating opportunities for future research. Combining valence-band and core-level spectroscopy with photoelectron diffraction for electronic, chemical, and structural analyses requires few 10 fs soft X-ray pulses with some 10 meV spectral resolution, which are currently available at high repetition rate free-electron lasers. We have constructed and optimized a versatile setup commissioned at FLASH/PG2 that combines free-electron laser capabilities together with a multidimensional recording scheme for photoemission studies. We use a full-field imaging momentum microscope with time-of-flight energy recording as the detector for mapping of 3D band structures in (kx, ky, E) parameter space with unprecedented efficiency. Our instrument can image full surface Brillouin zones with up to 7 Å-1 diameter in a binding-energy range of several eV, resolving about 2.5 × 105 data voxels simultaneously. Using the ultrafast excited state dynamics in the van der Waals semiconductor WSe2 measured at photon energies of 36.5 eV and 109.5 eV, we demonstrate an experimental energy resolution of 130 meV, a momentum resolution of 0.06 Å-1, and a system response function of 150 fs.

The ultrafast Einstein-de Haas effect.

The Einstein-de Haas effect was originally observed in a landmark experiment1 demonstrating that the angular momentum associated with aligned electron spins in a ferromagnet can be converted to mechanical angular momentum by reversing the direction of magnetization using an external magnetic field. A related problem concerns the timescale of this angular momentum transfer. Experiments have established that intense photoexcitation in several metallic ferromagnets leads to a drop in magnetization on a timescale shorter than 100 femtoseconds-a phenomenon called ultrafast demagnetization2-4. Although the microscopic mechanism for this process has been hotly debated, the key question of where the angular momentum goes on these femtosecond timescales remains unanswered. Here we use femtosecond time-resolved X-ray diffraction to show that most of the angular momentum lost from the spin system upon laser-induced demagnetization of ferromagnetic iron is transferred to the lattice on sub-picosecond timescales, launching a transverse strain wave that propagates from the surface into the bulk. By fitting a simple model of the X-ray data to simulations and optical data, we estimate that the angular momentum transfer occurs on a timescale of 200 femtoseconds and corresponds to 80 per cent of the angular momentum that is lost from the spin system. Our results show that interaction with the lattice has an essential role in the process of ultrafast demagnetization in this system.

Early Stages of Ultrafast Spin Dynamics in a 3d Ferromagnet.

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.

Laser-induced ultrafast spin current pulses: a thermodynamic approach.

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.

Direct 3D mapping of the Fermi surface and Fermi velocity.

We performed a full mapping of the bulk electronic structure including the Fermi surface and Fermi-velocity distribution vF(kF) of tungsten. The 4D spectral function ρ(EB; k) in the entire bulk Brillouin zone and 6 eV binding-energy (EB) interval was acquired in ∼3 h thanks to a new multidimensional photoemission data-recording technique (combining full-field k-microscopy with time-of-flight parallel energy recording) and the high brilliance of the soft X-rays used. A direct comparison of bulk and surface spectral functions (taken at low photon energies) reveals a time-reversal-invariant surface state in a local bandgap in the (110)-projected bulk band structure. The surface state connects hole and electron pockets that would otherwise be separated by an indirect local bandgap. We confirmed its Dirac-like spin texture by spin-filtered momentum imaging. The measured 4D data array enables extraction of the 3D dispersion of all bands, all energy isosurfaces, electron velocities, hole or electron conductivity, effective mass and inner potential by simple algorithms without approximations. The high-Z bcc metals with large spin-orbit-induced bandgaps are discussed as candidates for topologically non-trivial surface states.

Erratum: "Ultrafast demagnetization by hot electrons: Diffusion or super-diffusion?" [Struct. Dyn. 3, 055101 (2016)].

[This corrects the article DOI: 10.1063/1.4964892.].

Ultrafast demagnetization by hot electrons: Diffusion or super-diffusion?

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.

X-ray Detection of Transient Magnetic Moments Induced by a Spin Current in Cu.

We have used a MHz lock-in x-ray spectromicroscopy technique to directly detect changes in magnetic moment of Cu due to spin injection from an adjacent Co layer. The elemental and chemical specificity of x rays allows us to distinguish two spin current induced effects. We detect the creation of transient magnetic moments of 3×10^{-5}µ_{B} on Cu atoms within the bulk of the 28 nm thick Cu film due to spin accumulation. The moment value is compared to predictions by Mott's two current model. We also observe that the hybridization induced existing magnetic moments at the Cu interface atoms are transiently increased by about 10% or 4×10^{-3}µ_{B} per atom. This reveals the dominance of spin-torque alignment over Joule heat induced disorder of the interfacial Cu moments during current flow.

The influence of the excitation pulse length on ultrafast magnetization dynamics in nickel.

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.

Imaging spin filter for electrons based on specular reflection from iridium (001).

As Stern-Gerlach type spin filters do not work with electrons, spin analysis of electron beams is accomplished by spin-dependent scattering processes based on spin-orbit or exchange interaction. Existing polarimeters are single-channel devices characterized by an inherently low figure of merit (FoM) of typically 10⁻4-10⁻³. This single-channel approach is not compatible with parallel imaging microscopes and also not with modern electron spectrometers that acquire a certain energy and angular interval simultaneously. We present a novel type of polarimeter that can transport a full image by making use of k-parallel conservation in low-energy electron diffraction. We studied specular reflection from Ir (001) because this spin-filter crystal provides a high analyzing power combined with a "lifetime" in UHV of a full day. One good working point is centered at 39 eV scattering energy with a broad maximum of 5 eV usable width. A second one at about 10 eV shows a narrower profile but much higher FoM. A relativistic layer-KKR SPLEED calculation shows good agreement with measurements.

Nanoscale spin reversal by non-local angular momentum transfer following ultrafast laser excitation in ferrimagnetic GdFeCo.

Ultrafast laser techniques have revealed extraordinary spin dynamics in magnetic materials that equilibrium descriptions of magnetism cannot explain. Particularly important for future applications is understanding non-equilibrium spin dynamics following laser excitation on the nanoscale, yet the limited spatial resolution of optical laser techniques has impeded such nanoscale studies. Here we present ultrafast diffraction experiments with an X-ray laser that probes the nanoscale spin dynamics following optical laser excitation in the ferrimagnetic alloy GdFeCo, which exhibits macroscopic all-optical switching. Our study reveals that GdFeCo displays nanoscale chemical and magnetic inhomogeneities that affect the spin dynamics. In particular, we observe Gd spin reversal in Gd-rich nanoregions within the first picosecond driven by the non-local transfer of angular momentum from larger adjacent Fe-rich nanoregions. These results suggest that a magnetic material's microstructure can be engineered to control transient laser-excited spins, potentially allowing faster (~ 1 ps) spin reversal than in present technologies.

Magnetic pulser and sample holder for time- and spin-resolved photoemission spectroscopy on magnetic materials.

A compact coil setup, in conjunction with a high power current pulser, is presented; developed especially for time- and spin-resolved photoemission spectroscopy measuring the sample in magnetic remanence at room temperature. A novel approach is presented where the sample is switched in the stray field of a coil pair. This enables the electrical biasing of the sample without altering the electron trajectories due to field gradients introduced by the coils. The pulser driving the coils reaches a peak power of 1 MW at 1 kA with a switching frequency up to 10 kHz suitable for experiments, for example, with state of the art repetition rates of femtosecond laser systems.

Temporal cross-correlation of x-ray free electron and optical lasers using soft x-ray pulse induced transient reflectivity.

The recent development of x-ray free electron lasers providing coherent, femtosecond-long pulses of high brilliance and variable energy opens new areas of scientific research in a variety of disciplines such as physics, chemistry, and biology. Pump-probe experimental techniques which observe the temporal evolution of systems after optical or x-ray pulse excitation are one of the main experimental schemes currently in use for ultrafast studies. The key challenge in these experiments is to reliably achieve temporal and spatial overlap of the x-ray and optical pulses. Here we present measurements of the x-ray pulse induced transient change of optical reflectivity from a variety of materials covering the soft x-ray photon energy range from 500eV to 2000eV and outline the use of this technique to establish and characterize temporal synchronization of the optical-laser and FEL x-ray pulses.

Coherence properties of individual femtosecond pulses of an x-ray free-electron laser.

Measurements of the spatial and temporal coherence of single, femtosecond x-ray pulses generated by the first hard x-ray free-electron laser, the Linac Coherent Light Source, are presented. Single-shot measurements were performed at 780 eV x-ray photon energy using apertures containing double pinholes in "diffract-and-destroy" mode. We determined a coherence length of 17 µm in the vertical direction, which is approximately the size of the focused Linac Coherent Light Source beam in the same direction. The analysis of the diffraction patterns produced by the pinholes with the largest separation yields an estimate of the temporal coherence time of 0.55 fs. We find that the total degree of transverse coherence is 56% and that the x-ray pulses are adequately described by two transverse coherent modes in each direction. This leads us to the conclusion that 78% of the total power is contained in the dominant mode.

Images of a spin-torque-driven magnetic nano-oscillator.

We present the first space- and time-resolved images of the spin-torque-induced steady-state oscillation of a magnetic vortex in a spin-valve nanostructure. We find that the vortex structure in a nanopillar is considerably more complicated than the 2D idealized structure often-assumed, which has important implications for the driving efficiency. The sense of the vortex gyration is uniquely determined by the vortex core polarity, confirming that the spin-torque acts as a source of negative damping even in such a strongly nonuniform magnetic system. The orbit radius is ∼10 nm, in agreement with micromagnetic simulations.

Direct observation of spin-torque driven magnetization reversal through nonuniform modes.

We present time-resolved x-ray images with 30 nm spatial and 70 ps temporal resolution, which reveal details of the spatially resolved magnetization evolution in nanoscale samples of various dimensions during reversible spin-torque switching processes. Our data in conjunction with micromagnetic simulations suggest a simple unified picture of magnetic switching based on the motion of a magnetic vortex. With decreasing size of the magnetic element the path of the vortex core moves from inside to outside of the nanoelement, and the switching process evolves from a curled nonuniform to an increasingly uniform mode.

Synchronized and configurable source of electrical pulses for x-ray pump-probe experiments.

A method is described for the generation of software tunable patterns of nanosecond electrical pulses. The bipolar, high repetition rate (up to 250 MHz), fast rise time (<30 ps), square pulses are suitable for applications such as the excitation sequence in dynamic pump-probe experiments. Synchronization with the time structure of a synchrotron facility is possible as well as fine control of the relative delay in steps of 10 ps. The pulse generator described here is used to excite magnetic nanostructures with current pulses. Having an excitation system which can match the high repetition rate of a synchrotron allows for utilization of the full x-ray flux and is needed in experiments which require a large photon flux. The fast rise times allow for picosecond time resolution in pump-probe experiments. All pulse pattern parameters are configurable by software.