We performed a full mapping of the bulk electronic structure including the Fermi surface and Fermi-velocity distribution v(k) of tungsten. The 4D spectral function ρ(E; k) in the entire bulk Brillouin zone and 6 eV binding-energy (E) 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.

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.

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.

Photoemission-intensity distributions I RCP/LCP (E B , k) measured for right-and left-circularly polarized soft x-rays revealed a large circular dichroism in angular distribution (CDAD) in the 4D parameter space (E B binding energy, k momentum vector). Full-field k-imaging combined with timeof-flight energy recording at a high-brilliance soft x-ray beamline allowed mapping the CDAD in the bulk Brillouin zone of tungsten and the entire d-band complex within a few hours. CDADasymmetries are very high (up to 90%), persist throughout the whole photon-energy range (300-1300 eV) and show a pronounced dependence on momentum k and binding energy E B , visualized as movies or sequences of cuts through the 4D object. One-step photoemission calculations for the same photon energies show fair agreement with the measured results. In addition to the requirement of a 'handed' experimental geometry, known from previous experiments on adsorbates and surface states, we find an anti-symmetric behavior of the CDAD with respect to two bulk mirror planes. A new symmetry condition along the perpendicular momentum k z makes CDAD a valuable tool for an unambiguous identification of high-symmetry planes in direct transitions in the periodic zone scheme. Technically, the method provides a circular polarimeter for soft, tender and hard x-rays. being sensitive to their phase-shift differences. The differential photoemission cross section is proportional to the squared total dipole matrix element that contains interference terms between different final-state partial waves. Upon reversal of the photon helicity (in case of CDAD) or switching of the electric vector between orthogonal directions (for LDAD), interference terms with odd symmetry change their signs. This is the origin of the dichroism in the photoelectron angular distribution. This phenomenon exists in the pure electric dipole approximation and thus it differs from the 'natural' CD of chiral molecules, which is described by higher-order terms in the electron-photon operator [14].In the present work we employ the technique of time-of-flight (ToF) k-microscopy for a comprehensive study of the CDAD in the soft-x-ray spectral range. This new method captures simultaneously more than one full Brillouin zone (BZ) for binding energies in a range of several eV, yielding full information from the valence bands. In the vacuum ultraviolet (VUV) range, this instrument was previously used for the study of LDAD in photoemission from Mo(110) surface states and surface resonances [15]. These states are characterized by their 2D character and their location at the surface, wherefore they fulfill the criteria discussed for adsorbate systems [13]. Earlier work on graphite [16] and Pd [17] revealed that a CDAD also exists in photoemission from crystalline samples. However, the low photon energies used essentially probe the surface character of the bands. Hence, these results cannot be considered representative for true 3D bulk states. Moreover, no information on the dependence of the CDAD on the electro...

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.

An electric current flowing in Pt, a material with strong spin-orbit coupling, leads to spins accumulating at the interfaces by virtue of the spin Hall effect and interfacial charge-spin conversion. We measure the influence of these interfacial magnetic moments onto adjacent 3d transition metal layers by x-ray absorption spectroscopy and x-ray magnetic circular dichroism in a quantitative and element-selective way, with sensitivity below 10 −5 µB per atom. In Pt(6 nm)/Co(2.5 nm), the accumulated spins cause a deviation of the Co magnetization direction, which corresponds to an effective spin-Hall angle of 0.08. The spin and orbital magnetic moments of Co are affected in equal proportion by the absorption of the spin current, showing that the transfer of orbital momentum from the recently predicted orbital Hall effect is either below our detection limit, or not directed to the 3d states of Co. For Pt/NM (NM = Ti, Cr, Cu), we find upper limits for the amount of injected spins corresponding to about 3 × 10 −6 µB per atom.

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.

We explore the ultrafast generation of spin currents in magnetic multilayer samples by applying fs laser pulses to one layer and measuring the magnetic response in the other layer by element-resolved x-ray spectroscopy. In Ni(5 nm)/Ru(2 nm)/Fe(4 nm), the Ni and Fe magnetization directions couple antiferromagnetically due to the Ruderman–Kittel–Kasuya–Yosida interaction but may be oriented parallel through an applied magnetic field. After exciting the top Ni layer with a fs laser pulse, we also find that the Fe layer underneath demagnetizes, with a 4.1±1.9% amplitude difference between parallel and antiparallel orientation of the Ni and Fe magnetizations. We attribute this difference to the influence of a spin current generated by the fs laser pulse that transfers angular momentum from the Ni into the Fe layer. Our results confirm that superdiffusive spin transport plays a role in determining the sub-ps demagnetization dynamics of synthetic antiferromagnetic layers, but also evidence large depolarization effects due to hot electron dynamics, which are independent of the relative alignment of the magnetization in Ni and Fe.