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.

Observation and Structure Determination of an Oxide Quasicrystal Approximant.

We report on the first observation of an approximant structure to the recently discovered two-dimensional oxide quasicrystal. Using scanning tunneling microscopy, low-energy electron diffraction, and surface x-ray diffraction in combination with ab initio calculations, the atomic structure and the bonding scheme are determined. The oxide approximant follows a 3^{2}.4.3.4 Archimedean tiling. Ti atoms reside at the corners of each tiling element and are threefold coordinated to oxygen atoms. Ba atoms separate the TiO_{3} clusters, leading to a fundamental edge length of the tiling 6.7 Å.

Core-resonant double photoemission from palladium films.

We studied the core-resonant double photoemission process from palladium films with linearly polarized synchrotron radiation. We excited either the 3d or 4p core level and focused on the Auger transitions which leave two holes in the valence band. We find that the two-dimensional energy distributions are markedly different for the 3d and 4p decay. The 3d decay can be understood by a sequential emission of the two electrons while the 4p decay proceeds in a single step. Despite the large differences in the two-dimensional energy spectra we find the shape of the energy sum spectra rather similar. For the description of the 4p decay we propose a model which uses available single electron spectra, but suggest an alternative interpretation of these data. With this we are able to explain the range over which the available energy is shared. Key assumptions of the model are verified by our experiments on the 3d decay.

The LVV Auger line shape of sulfur on copper studied by Auger photoelectron coincidence spectroscopy.

We have studied the line shapes of Cu(0 0 1)-p (2 × 2)S L2VV and L3VV Auger decay by means of Auger photoelectron coincidence spectroscopy. Measuring the LVV Auger spectrum in coincidence with S 2p1/2 and 2p3/2 photoelectrons respectively, we have been able to separate the two overlapping Auger spectra and determine their intrinsic line shapes. The two Auger transitions, though shifted in energy, display an identical line shape whose main features can be qualitatively understood considering a single particle approximation but are better described within a Cini-Sawatzky (CS) approach. Comparison between the experimental and the CS calculated spectra confirms that a substantial part of the Auger lines (∼20%) can be ascribed to decay events accompanied by the excitation of one additional electron-hole pair in the valence band. For the first time, the locality of the Auger process combined with the surface sensitivity of the APECS technique and its ability to separate overlapping structures are used to study Auger transitions taking place at the the surface states of a S/noble-metal interface.

Energy relations of positron-electron pairs emitted from surfaces.

The impact of a primary positron onto a surface may lead to the emission of a correlated positron-electron pair. By means of a lab-based positron beam we studied this pair emission from various surfaces. We analyzed the energy spectra in a symmetric emission geometry. We found that the available energy is shared in an unequal manner among the partners. On average the positron carries a larger fraction of the available energy. The unequal energy sharing is a consequence of positron and electron being distinguishable particles. We provide a model which explains the experimental findings.

Dynamic screening probed by core-resonant double photoemission from surfaces.

The universal response of a sudden created core hole, predicted to occur on an attosecond (10(-18) s) time scale, lacks an experimental demonstration. With a two-dimensional coincidence spectrometer, we demonstrate an extensive energy sharing between the Ag 4p photoelectron and the N2,3VV Auger electron exceeding 10 eV. This energy width provides access to the time scale of the emission process. This is the fingerprint of the dynamic fluctuation process 4p(-1)⇌4d(-2)4f. The shakeup induced interband transitions from the Ag(100) surface are also identified by comparing the coincidence spectrum with the M4,5VV Auger transitions.

Exploring highly correlated materials via electron pair emission: the case of NiO/Ag(100).

Metal oxides like NiO are usually termed 'highly correlated', because the material properties are decisively determined by the electron-electron interaction. This makes them interesting candidates for electron pair spectroscopy which is particularly sensitive to the electron correlation. We have prepared ultrathin NiO/Ag(100) films and studied the electron pair emission upon electron impact. Compared to the metal substrate we observe an increase of the coincidence intensity by a factor of 8 for NiO. Thickness dependent measurements prove that this enhancement is an intrinsic effect rather than due to a mean free path increase of the oxide. The Néel temperature T(N) of NiO films displays a thickness dependence which allows us to tune T(N). We performed temperature dependent measurements and observed no temperature dependence of the coincidence spectra. This proves that the electron pair emission probes the local correlation rather than long range order. An enhanced coincidence intensity was also found for other oxide phases compared to their corresponding metal phases.

Spin-resolved mapping of spin contribution to exchange-correlation holes.

By means of spin-polarized electron coincidence spectroscopy we explore the fundamental issue of spin-resolved contributions to the exchange-correlation hole in many-electron systems. We present a joint experimental and theoretical study of correlated electron pair emission from a ferromagnetic Fe(001) surface induced by spin-polarized low-energy electrons. We demonstrate that the contribution to the exchange-correlation hole due to exchange is more extended than the contribution due to the screened Coulomb interaction.

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 effects in two electron photoemission.

Many-body effects in solids are ultimately related to the correlation among electrons, which can be probed by double photoelectron emission. We have investigated the electron pair emission from a Cu(111) surface upon photon absorption. We are able to observe for the first time the full extension and shape of a depletion zone around the fixed emission direction of one electron. It has an angular extension of approximately 1.2 rad, which is independent of the electron energy.

Mapping out electron-electron interactions at surfaces.

Using a high resolution coincidence technique, we measured for the first time the angular and energy correlation of an electron pair emitted from the valence band of a single crystal upon the impact of an electron with a specified momentum. We observe a hole in the measured two-particle correlation function when the two excited electrons have comparable momentum vectors, a fact traced back to exchange and repulsion among the electrons. We find the hole is not isotropic, has a finite extension, and is strongly suppressed when decoherence is operating.