F. O. Schumann

Electron pair emission detected by time-of-flight spectrometers: Recent progress

We present results for electron coincidence spectroscopy using two time-of-flight (ToF) spectrometers. Excited by electron impact, the energy and momentum distribution of electron pairs emitted from the Cu(111) surface are resolved and a spectral feature related to the Shockley surface state is identified. By combining the two ToF spectrometers with a high-order harmonic generation light source, we demonstrate double photoemission spectroscopy in the laboratory that required synchrotron radiation in the past. Utilizing this setup, we report results for (γ,2e) on NiO(001) on Ag(001) excited with light at 30 eV photon energy.

Boosting laboratory photoelectron spectroscopy by megahertz high-order harmonics

Since the discovery of the photoelectric effect, photoelectron spectroscopy has evolved into the most powerful technique for studying the electronic structure of materials. Moreover, the recent combination of photoelectron experiments with attosecond light sources using high-order harmonic generation (HHG) allows direct observation of electron dynamics in real time. However, the efficiency of these experiments is greatly limited by space-charge effects at typically low repetition rates of photoexcitation. Here, we demonstrate HHG-based laboratory photoemission experiments at a photoelectron count rate of 1 ? 105 electrons/s and characterize the main features of the electronic band structure of Ag(001) within several seconds without significant degradation by the space-charge effects. The combination of a compact HHG light source at megahertz repetition rates with the efficient collection of photoelectrons using time-of-flight spectroscopy may allow rapid investigation of electronic bands in a flexible laboratory environment and pave the way for an efficient design of attosecond spectroscopy and microscopy.

Direct and core-resonant double photoemission from Cu(001)

We have measured the correlated electron pair emission from a Cu(001) surface by both direct and core-resonant channels upon excitation with linearly polarized photons of energy far above the 3p threshold. As expected for a single-step process mediated by electron correlation in the initial and final states, the two electrons emitted by the direct channel continuously share the sum of the energy available to them. The core-resonant channel is often considered in terms of successive and independent steps of photoexcitation and Auger decay. However, electron pairs emitted by the core-resonant channel also share their energy continuously to jointly conserve the energy of the complete process. By detecting the electron pairs in parallel over a wide range of energy, evidence of the core-resonant double photoemission proceeding by a coherent single-step process is most strikingly manifested by a continuum of correlated electron pairs with a sum energy characteristic of the process but for which the individual electrons have arbitrary energies and cannot meaningfully be distinguished as a photoelectron or Auger electron.

Phase-locked MHz pulse selector for x-ray sources

Picosecond x-ray pulses are extracted with a phase-locked x-ray pulse selector at 1.25 MHz repetition rate from the pulse trains of the accelerator-driven multiuser x-ray source BESSY II preserving the peak brilliance at high pulse purity. The system consists of a specially designed in-vacuum chopper wheel rotating with ≈1  kHz angular frequency. The wheel is driven in an ultrahigh vacuum and is levitated on magnetic bearings being capable of withstanding high centrifugal forces. Pulses are picked by 1252 high-precision slits of 70 μm width on the outer rim of the wheel corresponding to a temporal opening window of the chopper of 70 ns. We demonstrate how the electronic phase stabilization of ±2  ns together with an arrival time jitter of the individual slits of the same order of magnitude allows us to pick short single bunch x-ray pulses out of a 200 ns ion clearing gap in a multibunch pulse train as emitted from a synchrotron facility at 1.25 MHz repetition rate with a pulse purity below the shot noise detection limit. The approach is applicable to any high-repetition pulsed radiation source, in particular in the x-ray spectral range up to 10 keV. The opening window in a real x-ray beamline, its stability, as well as the limits of mechanical pulse picking techniques in the MHz range are discussed.

Correlated positron–electron emission from surfaces

We studied positron–electron pair emission from a LiF(100) surface following excitation by a positron beam with a kinetic energy of 85 eV. We show for the first time that emission of time-correlated positron–electron pairs occurs.

Mapping out electron–electron interactions in angular space

Many-body effects in solids are related to the correlation among electrons. This mutual interaction between the electrons can be probed by electron pair emission spectroscopy. We have investigated the electron pair emission from a LiF(100) surface upon excitation with low kinetic energy electrons. Our angular distributions clearly show that the emission direction of one electron is surrounded by a reduced intensity of the other electron. This depletion zone of electronic intensity is a manifestation of the exchange and correlation hole. We show that we are able to observe the full extension and shape of the depletion zone. It has an angular extension of ≈1.2 rad and is independent of the electron energy. Additionally, we discovered that the angle between the trajectories of the electrons has a profound effect on the two-dimensional energy distribution.

Correlated Electron Dynamics at Surfaces Investigated via He2+ Ion Neutralization

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.

Electron pair emission from a W(001) surface: photon versus electron excitation

The electron pair emission from a W(001) surface was studied using a coincidence time-of-flight spectrometer. The aim of this study was to compare the pair emission upon electron impact and upon photon absorption. The energy distributions are markedly different for these two experiments. From this we conclude that the photon-stimulated pair emission carries a significant contribution from a double photoemission process, while the process of first creating a photoelectron, which in a subsequent collision leads to pair emission, is of less importance.

Correlation spectroscopy of condensed matter systems

We present experimental and theoretical evidence for the potential of the two‐particle spectroscopy to explore the electron‐electron interaction in condensed matter. The experiment consists of a single electron impinging onto a clean surface. Two electrons are then emitted simultaneously and their momentum vectors are resolved. The measured energy and angular pair correlations within the pair carry direct information akin to the electron‐electron interaction in the sample. We also point out that the presence of the Fermi sea leads to a damping, and a suppression of the range of the electron‐electron interaction.

Extended energy range analysis for angle-resolved time-of-flight photoelectron spectroscopy

An approximation method for electrostatic time-of-flight (ToF) spectroscopy on photoelectrons distributed over a wide energy range is presented. This method is an extension of conventional analysis and aims at specific energy and angular regions, where distinctly different emission angles and energies are mapped to the same ToF and detector position by the spectrometer. The general formulation and the systematic errors are presented, and a practical example is demonstrated for photoelectrons from Ag(001) with kinetic energies of 0.5–25 eV.