Recovery of High-Energy Photoelectron Circular Dichroism through Fano Interference.

It is commonly accepted that the magnitude of a photoelectron circular dichroism (PECD) is governed by the ability of an outgoing photoelectron wave packet to probe the chiral asymmetry of a molecule. To be able to accumulate this characteristic asymmetry while escaping the chiral ion, photoelectrons need to have relatively small kinetic energies of up to a few tens of electron volts. Here, we demonstrate a substantial PECD for very fast photoelectrons above 500 eV kinetic energy released from methyloxirane by a participator resonant Auger decay of its lowermost O 1s excitation. This effect emerges as a result of the Fano interference between the direct and resonant photoionization pathways, notwithstanding that their individual effects are negligibly small. The resulting dichroic parameter has an anomalous dispersion: It changes its sign across the resonance, which can be considered as an analogue of the Cotton effect in the x-ray regime.

Symmetry breakdown of electron emission in extreme ultraviolet photoionization of argon.

Short wavelength free-electron lasers (FELs), providing pulses of ultrahigh photon intensity, have revolutionized spectroscopy on ionic targets. Their exceptional photon flux enables multiple photon absorptions within a single femtosecond pulse, which in turn allows for deep insights into the photoionization process itself as well as into evolving ionic states of a target. Here we employ ultraintense pulses from the FEL FERMI to spectroscopically investigate the sequential emission of electrons from gaseous, atomic argon in the neutral as well as the ionic ground state. A pronounced forward-backward symmetry breaking of the angularly resolved emission patterns with respect to the light propagation direction is experimentally observed and theoretically explained for the region of the Cooper minimum, where the asymmetry of electron emission is strongly enhanced. These findings aim to originate a better understanding of the fundamentals of photon momentum transfer in ionic matter.

Separating Dipole and Quadrupole Contributions to Single-Photon Double Ionization.

We report on a kinematically complete measurement of double ionization of helium by a single 1100 eV circularly polarized photon. By exploiting dipole selection rules in the two-electron continuum state, we observed the angular emission pattern of electrons originating from a pure quadrupole transition. Our fully differential experimental data and companion ab initio nonperturbative theory show the separation of dipole and quadrupole contributions to photo-double-ionization and provide new insight into the nature of the quasifree mechanism.

Publisher Correction: Imaging the square of the correlated two-electron wave function of a hydrogen molecule.

The original version of this Article contained an error in the fifth sentence of the first paragraph of the 'Application on H2' section of the Results, which incorrectly read 'The role of electron correlation is quite apparent in this presentation: Fig. 1a is empty for the uncorrelated Hartree-Fock wave function, since projection of the latter wave function onto the 2pσu orbital is exactly zero, while this is not the case for the fully correlated wave function (Fig. 1d); also, Fig. 1b, c for the uncorrelated description are identical, while Fig. 1e, f for the correlated case are significantly different.' The correct version replaces 'Fig. 1e, f' with 'Fig. 2e and f'.

Note: Soft X-ray transmission polarizer based on ferromagnetic thin films.

A transmission polarizer for producing elliptically polarized soft X-ray radiation from linearly polarized light is presented. The setup is intended for use at synchrotron and free-electron laser beamlines that do not directly offer circularly polarized light for, e.g., X-ray magnetic circular dichroism (XMCD) measurements or holographic imaging. Here, we investigate the degree of ellipticity upon transmission of linearly polarized radiation through a cobalt thin film. The experiment was performed at a photon energy resonant to the Co L3-edge, i.e., 778 eV, and the polarization of the transmitted radiation was determined using a polarization analyzer that measures the directional dependence of photo electrons emitted from a gas target. Elliptically polarized radiation can be created at any absorption edge showing the XMCD effect by using the respective magnetic element.

Imaging the square of the correlated two-electron wave function of a hydrogen molecule.

The toolbox for imaging molecules is well-equipped today. Some techniques visualize the geometrical structure, others the electron density or electron orbitals. Molecules are many-body systems for which the correlation between the constituents is decisive and the spatial and the momentum distribution of one electron depends on those of the other electrons and the nuclei. Such correlations have escaped direct observation by imaging techniques so far. Here, we implement an imaging scheme which visualizes correlations between electrons by coincident detection of the reaction fragments after high energy photofragmentation. With this technique, we examine the H2 two-electron wave function in which electron-electron correlation beyond the mean-field level is prominent. We visualize the dependence of the wave function on the internuclear distance. High energy photoelectrons are shown to be a powerful tool for molecular imaging. Our study paves the way for future time resolved correlation imaging at FELs and laser based X-ray sources.

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.

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.

Circular dichroism measurements at an x-ray free-electron laser with polarization control.

A non-destructive diagnostic method for the characterization of circularly polarized, ultraintense, short wavelength free-electron laser (FEL) light is presented. The recently installed Delta undulator at the LCLS (Linac Coherent Light Source) at SLAC National Accelerator Laboratory (USA) was used as showcase for this diagnostic scheme. By applying a combined two-color, multi-photon experiment with polarization control, the degree of circular polarization of the Delta undulator has been determined. Towards this goal, an oriented electronic state in the continuum was created by non-resonant ionization of the O2 1s core shell with circularly polarized FEL pulses at hν ≃ 700 eV. An also circularly polarized, highly intense UV laser pulse with hν ≃ 3.1 eV was temporally and spatially overlapped, causing the photoelectrons to redistribute into so-called sidebands that are energetically separated by the photon energy of the UV laser. By determining the circular dichroism of these redistributed electrons using angle resolving electron spectroscopy and modeling the results with the strong-field approximation, this scheme allows to unambiguously determine the absolute degree of circular polarization of any pulsed, ultraintense XUV or X-ray laser source.

Two-Particle Interference of Electron Pairs on a Molecular Level.

We investigate the photodouble ionization of H_{2} molecules with 400 eV photons. We find that the emitted electrons do not show any sign of two-center interference fringes in their angular emission distributions if considered separately. In contrast, the quasiparticle consisting of both electrons (i.e., the "dielectron") does. The work highlights the fact that nonlocal effects are embedded everywhere in nature where many-particle processes are involved.

A new compact soft x-ray spectrometer for resonant inelastic x-ray scattering studies at PETRA III.

We present a newly designed compact grating spectrometer for the energy range from 210 eV to 1250 eV, which would include the Kα(1,2) emission lines of vital elements like C, N, and O. The spectrometer is based on a grazing incidence spherical varied line spacing grating with 2400 l/mm at its center and a radius of curvature of 58 542 mm. First, results show a resolving power of around 1000 at an energy of 550 eV and a working spectrometer for high vacuum (10(-4) mbar) environment without losing photon intensity.

Single Shot Polarization Characterization of XUV FEL Pulses from Crossed Polarized Undulators.

Polarization control is a key feature of light generated by short-wavelength free-electron lasers. In this work, we report the first experimental characterization of the polarization properties of an extreme ultraviolet high gain free-electron laser operated with crossed polarized undulators. We investigate the average degree of polarization and the shot-to-shot stability and we analyze aspects such as existing possibilities for controlling and switching the polarization state of the emitted light. The results are in agreement with predictions based on Gaussian beams propagation.

Observation of a four-electron Auger process in near-K-edge photoionization of singly charged carbon ions.

Single, double, and triple ionization of C(1+) ions by single photons is investigated in the energy range of 286-326 eV, i.e., in the range from the lowest-energy K-vacancy resonances to well beyond the K-shell ionization threshold. Clear signatures of C(1+)(1s2s(2)2p(2) (2)D,(2)P) resonances are found in the triple-ionization channel. The only possible mechanism producing C(4+)(1s(2)) via these resonances is direct triple-Auger decay, i.e., a four-electron process with simultaneous emission of three electrons.

Characterization of spatial coherence of synchrotron radiation with non-redundant arrays of apertures.

A method to characterize the spatial coherence of soft X-ray radiation from a single diffraction pattern is presented. The technique is based on scattering from non-redundant arrays (NRAs) of slits and records the degree of spatial coherence at several relative separations from 1 to 15 µm, simultaneously. Using NRAs the spatial coherence of the X-ray beam at the XUV X-ray beamline P04 of the PETRA III synchrotron storage ring was measured as a function of different beam parameters. To verify the results obtained with the NRAs, additional Young's double-pinhole experiments were conducted and showed good agreement.

Angular momentum sensitive two-center interference.

In quantum mechanics the Young-type double-slit experiment can be performed with electrons either traveling through a double slit or being coherently emitted from two inversion symmetric molecular sites. In the latter one the valence photoionization cross sections of homonuclear diatomic molecules were predicted to oscillate over kinetic energy almost 50 years ago. Beyond the direct proof of the oscillatory behavior of these photoionization cross sections σ, we show that the angular distribution of the emitted electrons reveals hitherto unexplored information on the relative phase shift between the corresponding partial waves through two-center interference patterns.

Intramolecular electron scattering and electron transfer following autoionization in dissociating molecules.

Resonant Auger decay of core-excited molecules during ultrafast dissociation leads to a Doppler shift of the emitted electrons depending on the direction of the electron emission relative to the dissociation axis. We have investigated this process by angle-resolved electron-fragment ion coincidence spectroscopy. Electron energy spectra for selected emission angles for the electron relative to the molecular axis reveal the occurrence of intermolecular electron scattering and electron transfer following the primary emission. These processes amount to approximately 25% of the resonant atomic Auger intensity emitted in the studied transition.

Sudden interchannel interaction in the Tl 6p ionization above the 5d threshold

The linear magnetic dichroism in the angular distribution of Tl 5d and 6p photoelectrons and their dynamical spin polarization have been measured between hnu = 30 and 50 eV. In contrast to the Xe 5p photoionization at the 4d threshold, our results show that above the Tl 5d threshold strong interchannel coupling effects induce a sudden increase in the asymptotic phase difference of the s and d waves for the Tl 6p ionization. This shows that the valence excitation is different for resonant (Xe 4d) and nonresonant (Tl 5d) excitation from subvalence shells.