X-ray spectroscopy station for sample characterization at ELI Beamlines.

X-ray spectroscopy is a demanded tool across multiple user communities. Here we report on a new station for X-ray emission spectroscopy at the Extreme Light Infrastructure Beamlines Facility. The instrument utilizes the von Hamos geometry and works with a number of different sample types, notably including liquid systems. We demonstrate a simple and reliable method for source position control using two cameras. This approach addresses energy calibration dependence on sample position, which is a characteristic source of measurement uncertainty for wavelength dispersive spectrometers in XES arrangement. We also present a straightforward procedure for energy calibration of liquid and powder samples to a thin film reference. The developed instrumentation enabled us to perform the first experimental determination of the Kα lines of liquidized K3Fe(CN)6 as well as powdered and liquidized FeNH4(SO4)2. Finally, we report on proof-of-principle use of a colliding jet liquid sample delivery system in an XES experiment.

Time-of-flight photoelectron momentum microscopy with 80-500 MHz photon sources: electron-optical pulse picker or bandpass pre-filter.

The small time gaps of synchrotron radiation in conventional multi-bunch mode (100-500 MHz) or laser-based sources with high pulse rate (∼80 MHz) are prohibitive for time-of-flight (ToF) based photoelectron spectroscopy. Detectors with time resolution in the 100 ps range yield only 20-100 resolved time slices within the small time gap. Here we present two techniques of implementing efficient ToF recording at sources with high repetition rate. A fast electron-optical beam blanking unit with GHz bandwidth, integrated in a photoelectron momentum microscope, allows electron-optical `pulse-picking' with any desired repetition period. Aberration-free momentum distributions have been recorded at reduced pulse periods of 5 MHz (at MAX II) and 1.25 MHz (at BESSY II). The approach is compared with two alternative solutions: a bandpass pre-filter (here a hemispherical analyzer) or a parasitic four-bunch island-orbit pulse train, coexisting with the multi-bunch pattern on the main orbit. Chopping in the time domain or bandpass pre-selection in the energy domain can both enable efficient ToF spectroscopy and photoelectron momentum microscopy at 100-500 MHz synchrotrons, highly repetitive lasers or cavity-enhanced high-harmonic sources. The high photon flux of a UV-laser (80 MHz, <1 meV bandwidth) facilitates momentum microscopy with an energy resolution of 4.2 meV and an analyzed region-of-interest (ROI) down to <800 nm. In this novel approach to `sub-µm-ARPES' the ROI is defined by a small field aperture in an intermediate Gaussian image, regardless of the size of the photon spot.

Spin-filtered time-of-flight k-space microscopy of Ir - Towards the "complete" photoemission experiment.

The combination of momentum microscopy (high resolution imaging of the Fourier plane) with an imaging spin filter has recently set a benchmark in k-resolution and spin-detection efficiency. Here we show that the degree of parallelization can be further increased by time-of-flight energy recording. On the quest towards maximum information (in earlier work termed "complete" photoemission experiment) we have studied the prototypical high-Z fcc metal iridium. Large partial bandgaps and strong spin-orbit interaction lead to a sequence of spin-polarized surface resonances. Soft X-rays give access to the 4D spectral density function ρ (EB,kx,ky,kz) weighted by the photoemission cross section. The Fermi surface and all other energy isosurfaces, Fermi velocity distribution vF(kF), electron or hole conductivity, effective mass and inner potential can be obtained from the multi-dimensional array ρ by simple algorithms. Polarized light reveals the linear and circular dichroism texture in a simple manner and an imaging spin filter exposes the spin texture. One-step photoemission calculations are in fair agreement with experiment. Comparison of the Bloch spectral function with photoemission calculations uncovers that the observed high spin polarization of photoelectrons from bulk bands originates from the photoemission step and is not present in the initial state.

Hosting of surface states in spin-orbit induced projected bulk band gaps of W(1 1 0) and Ir(1 1 1).

Spin-momentum locking of surface states has attracted great interest in recent years due to envisioned technological applications in the field of spintronics. Normal metal surfaces like W(1 1 0) and Ir(1 1 1) show surface states with energy dispersions and spin-polarization textures, which are reminiscent of topologically non-trivial surface states. In order to understand this phenomenon the connection of bulk and surface states has to be explored. Using time-of-flight momentum microscopy with soft x-ray excitation, we present a comprehensive analysis of the bulk bands of W and Ir. Surface states are determined by the same method with photon excitation in the vacuum ultraviolet region. The superposition of both spectral densities reveals the hosting of surface states within the gap structure of bulk bands projected on the surface Brillouin zone. Quantitative differences in the extension of experimental and theoretical local band gaps indicate an underestimation of electron correlation effects in theory.