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.

Kink far below the Fermi level reveals new electron-magnon scattering channel in Fe.

Many properties of real materials can be modeled using ab initio methods within a single-particle picture. However, for an accurate theoretical treatment of excited states, it is necessary to describe electron-electron correlations including interactions with bosons: phonons, plasmons, or magnons. In this work, by comparing spin- and momentum-resolved photoemission spectroscopy measurements to many-body calculations carried out with a newly developed first-principles method, we show that a kink in the electronic band dispersion of a ferromagnetic material can occur at much deeper binding energies than expected (Eb = 1.5 eV). We demonstrate that the observed spectral signature reflects the formation of a many-body state that includes a photohole bound to a coherent superposition of renormalized spin-flip excitations. The existence of such a many-body state sheds new light on the physics of the electron-magnon interaction which is essential in fields such as spintronics and Fe-based superconductivity.

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.

Correlated Electron Dynamics at Surfaces Investigated via He

The neutralization of a single He^{2+} ion near a Ir surface leads to the emission of an electron pair. Via coincidence spectroscopy we give evidence that a sizable amount of these electron pairs originate from a correlated single step neutralization of the ion involving a total of four electrons from the metal. These correlated electron pairs cannot be explained in the common picture of two consecutive and independent neutralization steps. We infer a characteristic time scale for the correlated electron dynamics in the metal of 40-400 as.

Spin texture of time-reversal symmetry invariant surface states on W(110).

We find in the case of W(110) previously overlooked anomalous surface states having their spin locked at right angle to their momentum using spin-resolved momentum microscopy. In addition to the well known Dirac-like surface state with Rashba spin texture near the -point, we observe a tilted Dirac cone with circularly shaped cross section and a Dirac crossing at 0.28 × within the projected bulk band gap of tungsten. This state has eye-catching similarities to the spin-locked surface state of a topological insulator. The experiments are fortified by a one-step photoemission calculation in its density-matrix formulation.

Electron-Vibration Coupling in Molecular Materials: Assignment of Vibronic Modes from Photoelectron Momentum Mapping.

Electron-phonon coupling is one of the most fundamental effects in condensed matter physics. We here demonstrate that photoelectron momentum mapping can reveal and visualize the coupling between specific vibrational modes and electronic excitations. When imaging molecular orbitals with high energy resolution, the intensity patterns of photoelectrons of the vibronic sidebands of molecular states show characteristic changes due to the distortion of the molecular frame in the vibronically excited state. By comparison to simulations, an assignment of specific vibronic modes is possible, thus providing unique information on the coupling between electronic and vibronic excitation.

Anomalous d-like surface resonances on Mo(110) analyzed by time-of-flight momentum microscopy.

The electronic surface states on Mo(110) have been investigated using time-of-flight momentum microscopy with synchrotron radiation (hν=35 eV). This novel angle-resolved photoemission approach yields a simultaneous acquisition of the E-vs-k spectral function in the full surface Brillouin zone and several eV energy interval. (kx,ky,EB)-maps with 3.4 Å(-1) diameter reveal a rich structure of d-like surface resonances in the spin-orbit induced partial band gap. Calculations using the one-step model in its density matrix formulation predict an anomalous state with Dirac-like signature and Rashba spin texture crossing the bandgap at Γ¯ and EB=1.2 eV. The experiment shows that the linear dispersion persists away from the Γ¯-point in an extended energy- and k∥-range. Analogously to a similar state previously found on W(110) the dispersion is linear along H¯-Γ¯-H¯ and almost zero along N¯-Γ¯-N¯. The similarity is surprising since the spin-orbit interaction is 5 times smaller in Mo. A second point with unusual topology is found midway between Γ¯ and N¯. Band symmetries are probed by linear dichroism.

Spin Blocking in the Correlated Double-Electron Capture from Metal Surfaces.

The resonant capture of electrons from a metallic surface into the outer shell of a helium ion creates doubly excited states in a spin singlet (↑↓) or triplet (↑↑) configuration. Here it is shown that the capture of one or two electrons can be described in a simple quantitative model, and the capture of two electrons by He(++) proceeds in a single step. The double capture of electrons from the Fermi energy of the metal is dominated by the spin dependent electron correlation that blocks the occupation of triplet states in the ion, but creates a singlet two-hole final state at the surface, related to the concept of the exchange-correlation hole.

Correction of the deterministic part of space-charge interaction in momentum microscopy of charged particles.

Ultrahigh spectral brightness femtosecond XUV and X-ray sources like free electron lasers (FEL) and table-top high harmonics sources (HHG) offer fascinating experimental possibilities for analysis of transient states and ultrafast electron dynamics. For electron spectroscopy experiments using illumination from such sources, the ultrashort high-charge electron bunches experience strong space-charge interactions. The Coulomb interactions between emitted electrons results in large energy shifts and severe broadening of photoemission signals. We propose a method for a substantial reduction of the effect by exploiting the deterministic nature of space-charge interaction. The interaction of a given electron with the average charge density of all surrounding electrons leads to a rotation of the electron distribution in 6D phase space. Momentum microscopy gives direct access to the three momentum coordinates, opening a path for a correction of an essential part of space-charge interaction. In a first experiment with a time-of-flight momentum microscope using synchrotron radiation at BESSY, the rotation in phase space became directly visible. In a separate experiment conducted at FLASH (DESY), the energy shift and broadening of the photoemission signals were quantified. Finally, simulations of a realistic photoemission experiment including space-charge interaction reveals that a gain of an order of magnitude in resolution is possible using the correction technique presented here.

Tuning the Dirac point position in Bi(2)Se(3)(0001) via surface carbon doping.

Angular resolved photoemission spectroscopy in combination with ab initio calculations show that trace amounts of carbon doping of the Bi_{2}Se_{3} surface allows the controlled shift of the Dirac point within the bulk band gap. In contrast to expectation, no Rashba-split two-dimensional electron gas states appear. This unique electronic modification is related to surface structural modification characterized by an expansion of the top Se-Bi spacing of ≈11% as evidenced by surface x-ray diffraction. Our results provide new ways to tune the surface band structure of topological insulators.

A low energy ion source for electron capture spectroscopy.

We report on the design of an ion source for the production of single and double charged Helium ions with kinetic energies in the range from 300 eV down to 5 eV. The construction is based on a commercial sputter ion gun equipped with a Wien-filter for mass/charge separation. Retardation of the ions from the ionizer potential (2 keV) takes place completely within the lens system of the sputter gun, without modification of original parts. For 15 eV He(+) ions, the design allows for beam currents up to 30 nA, limited by the space charge repulsion in the beam. For He(2 +) operation, we obtain a beam current of 320 pA at 30 eV, and 46 pA at 5 eV beam energy, respectively. In addition, operating parameters can be optimized for a significant contribution of metastable He*(+) (2s) ions.

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.

Highly efficient multichannel spin-polarization detection.

Since the original work by Mott, the low efficiency of electron spin polarimeters, remaining orders of magnitude behind optical polarimeters, has prohibited many fundamental experiments. Here we report a solution to this problem using a novel concept of multichannel spin-polarization analysis that provides a stunning increase in efficiency by 4 orders of magnitude. This improvement was demonstrated in a setup using a hemispherical electron energy analyzer. An imaging setup proved the principal capability of resolving more than 10(5) data points in parallel.

Wurtzite-type CoO nanocrystals in ultrathin ZnCoO films.

Surface x-ray diffraction experiments reveal that, in cobalt-doped ZnO films two to five monolayers thick, Wurtzite-type CoO nanocrystals are coherently embedded within a hexagonal boron-nitride- (h-BN)-type ZnO matrix, supporting the model of a phase separation. First-principles calculations confirm that, in contrast with ZnO, the formation of h-BN-type CoO is unfavorable in the ultrathin film limit. Our results are important for understanding magnetic properties of transition metal-doped semiconductors in general.

Direct evidence for mesoscopic relaxations in cobalt nanoislands on Cu(001).

Surface x-ray diffraction in combination with scanning tunneling microscopy and molecular dynamics calculations provide first quantitative evidence for unusually large relaxations in nanometer-sized Co islands deposited on Cu(001) at 170 K. These lead to sharply reduced interatomic Co distances as low as 2.36 A as compared to bulk Co (2.51 A) involving low symmetry Co adsorption sites. Our results prove the validity of the concept of mesoscopic mismatch which governs the strain relaxation of nanosized islands in general.

Observation of depolarized ZnO(0001) monolayers: formation of unreconstructed planar sheets.

A novel nonpolar structure of 2 monolayer (ML) thick ZnO(0001) films grown on Ag(111) has been revealed, using surface x-ray diffraction and scanning tunneling microscopy. Zn and O atoms are arranged in planar sheets like in the hexagonal boron-nitride prototype structure. The observed depolarization is accompanied by a significant lateral 1.6% expansion of the lattice parameter and a 3% reduced Zn-O bond length within the sheets. The nonpolar structure stabilizes an atomically flat surface morphology unseen for ZnO surfaces thus far. The transition to the bulk wurtzite structure occurs in the 3-4 ML coverage range, connected to considerable roughening.

Oxygen-induced symmetrization and structural coherency in Fe/MgO/Fe(001) magnetic tunnel junctions.

We present x-ray diffraction experiments and multiple-scattering calculations on the structure and transport properties of a Fe/MgO/Fe(001) magnetic tunnel junction (MTJ). Coherent growth of the top Fe electrode on the MgO spacer is observed only for Fe deposition in ambient oxygen atmosphere leading to a coherent and symmetric MTJ structure characterized by FeO layers at both interfaces. This goes in parallel with calculations indicating large positive tunnel magnetoresistance (TMR) values in such symmetric junctions. The results have important implications for achieving giant TMR values.