Element-Selective Magnetic Imaging in Exchange-Coupled Systems by Magnetic Photoemission Microscopy

We have used a photoemission microscope to obtain element-resolved magnetic contrast in stacked magnetic thin film systems. Magnetic information is thereby provided by X-ray magnetic circular dichroism. Elemental sensitivity, which is crucial for studying magnetic coupling phenomena in systems with several different layers, is achieved by tuning the energy of the illuminating photons to atomic absorption edges. We present measurements of a Ni-coated Co micropattern on Cu(001), and a wedged Co/Cr/Fe(001) sample. In the former sample the Ni magnetization is seen to follow the magnetization of the Co pattern, thereby changing from an out-of-plane easy axis in areas without underlying Co to in…

Surface magnetism studied by photoelectron spectromicroscopy with high spatial and time resolution

Abstract Photoemission electron microscopy (PEEM) is widely used for the study of magnetic surfaces and thin films. Ferromagnetic and antiferromagnetic microstructures are investigated exploiting magnetic circular and linear dichroism in the soft X-ray range using tuneable synchrotron radiation. Local dichroism spectroscopy gives access to magnetic moments of the elements in compounds or multilayer materials. Beyond these achievements, the method bears a high future potential with respect to an increased lateral resolution via aberration correction of the electron optics and a high time resolution in the 100 ps range for the study of dynamic processes. In addition, photoelectron spin polari…

Energy- and time-resolved microscopy using PEEM: recent developments and state-of-the-art

Two novel methods of spectroscopic surface imaging are discussed, both based on photoemission electron microscopy PEEM. They are characterised by a simple electron-optical set up retaining a linear column. An imaging high-pass energy filter has been developed on the basis of lithographically-fabricated microgrids. Owing to a mesh size of only 7μm, no image distortions occur. The present energy resolution is 70 meV. The second approach employs time-of-flight energy dispersion and time-resolved detection using a Delayline Detector. In this case, the drift energy and the time resolution of the detector determine the energy resolution. The present time resolution is 180 ps, giving rise to an en…

Surface hysteresis curves of Fe(110) and Fe(100) crystals in ultrahigh vacuum — evidence of adsorbate influences

Abstract We have investigated hysteresis curves of silicon-stabilized Fe(100) and Fe(110) crystals using Polarized Secondary Electron Emission (PSEE) for surface magnetization processes and Magneto-Optical Kerr Effect (MOKE) for bulk hysteresis curves. In particular, the influence of adsorbates (oxygen and sulphur) and surface roughness on the magnetization reversal has been studied. For surface hysteresis curves we found adsorbate-induced reductions of coercive force of up to 50%; the bulk hysteresis curves showed significantly smaller deviations. Similar changes were caused by surface disorder on an atomic scale induced by ion bombardment. The results agree qualitatively with a previous e…

Strain-induced magnetic anisotropies in Co films on Mo(110)

Bulk spin polarization of magnetite from spin-resolved hard x-ray photoelectron spectroscopy

Physical review / B 104(4), 045129 (1-10) (2021). doi:10.1103/PhysRevB.104.045129

Angular-resolved electron spectroscopy from (110) surfaces of ternary Ce-based intermetallics: CePd2Si2 and CeNi2Ge2

Investigations of electronic properties were carried out for the ternary Ce-based intermetallic systems CeT2X2 (T = Ni, Pd; X = Ge, Si). To produce well-ordered and atomically clean surfaces, preparation is carried out in UHV. The polycrystalline substance was evaporated on a W(110) substrate with subsequent annealing. The single-crystalline layers obtained are characterised by MEED (thickness), AES (surface stoichiometry), LEED and SEM (surface structure). For electron-spectroscopic investigations, ARUPS (angle-resolved photoemission spectroscopy) was used. In the photoemission spectra, dispersion effects could be detected by variation of the detection angle.

A spatially resolved investigation of oxygen adsorption on polycrystalline copper and titanium by means of photoemission electron microscopy

Abstract The interaction of oxygen with polycrystalline copper and titanium surfaces was studied by means of photoemission electron microscopy. Variations in the image brightness were used to determine the work function of different Cu crystallites. The change of the work function was monitored during oxygen adsorption on both, Cu and Ti. Those changes are smooth for Cu whereas different Ti crystallites exhibit a rather complicated behavior during oxygen adsorption. The transformation of brightness versus exposure curves into work function versus coverage curves allows to determine the initial dipole moment of the adsorbed oxygen atoms. A value of about 20 mD was found for O on Cu(1 1 0). V…

Transmission of electrons through ferromagnetic material and applications to detection of electron spin polarization

The salient features of the total low energy inelastic electron scattering cross section in transition metals are described by a constant term σ 0 plus a term σ d that is proportional to the number of unoccupied d-orbitals. This simple model predicts that low energy electrons transmitted through a ferromagnetic ultrathin film acquire a transport spin polarization a(x). Using the ratio σ 0 /σ d as the only adjustable parameter, the model predicts the enhancement of the spin polarization of the low energy cascade electrons as well as a(x) in reasonable agreement with the existing observations on Fe, Co and Ni. A detector for electron spin polarization P based on the spin dependent transmissio…

New HAXPES Applications at PETRA III

The application of photoelectron spectroscopy using hard X-rays (HAXPES) is becoming increasingly popular as a powerful spectroscopic tool in materials science. The success of HAXPES lies in the fa...

Matching emission centers of electrons and photons in current-carrying silver nanoparticle films

Current flow through a nanoparticle film (two-dimensional ensemble of small tunnel-coupled metal particles on a dielectric substrate) is accompanied by electron and photon emission. It has a localized character (originates from emission centers). With an increase in applied voltage, the number of emission centers increases, and with further increase, some of them may burn out. In dark conditions, photon emission centers are visible with a bare eye. To visualize electron emission centers, emission electron microscopy is used. The conducted measurements allow comparison of the number and relative positions of electron and photon emission centers. It is shown that electrons and photons are emi…

Magnetization dynamics in polycrystalline Permalloy and epitaxial Co platelets observed by time-resolved photoemission electron microscopy

We studied the dynamic magnetization response in rectangular polycrystalline Permalloy and also epitaxial Co structures (lateral sizes comprised tens of microns at a thickness of tens of nanometers) during the action of a magnetic field pulse, using time-resolved X-ray photoemission electron microscopy with a time resolution of 10 ps. In the case of Permalloy platelets the restoring torque that is necessary for the stroboscopic image acquisition is provided by the Landau flux closure structure representing a minimum of the free energy. We investigated the dynamic response of 90° Neel domain walls. The main results are: the maximum velocity of the domain wall is 1.5 × 104 m/s, the intrinsic …

Multiphoton photoemission electron microscopy using femtosecond laser radiation

Abstract The interaction of intense, pulsed laser radiation with surfaces results in non-linear optical effects that are responsible for emission of electrons even if the photon energies are below the work function. In the present study, photoelectrons have been excited by means of femtosecond laser pulses from a frequency doubled Ti:sapphire laser with a photon energy of 3.1 eV. The spatial distribution of the photo emitted electrons was imaged using a photoemission electron microscope. All samples exhibit centres of enhanced second or higher order photoemission yield, so called ‘hot spots’. These ‘hot spots’ were preferentially excited with s-polarised light. This behaviour may be explain…

Hard x-ray photoelectron spectroscopy of buried Heusler compounds

This work reports on high energy photoelectron spectroscopy from the valence band of buried Heusler thin films (Co2MnSi and Co2FeAl0.5Si0.5) excited by photons of about 6?keV energy. The measurements were performed on thin films covered by MgO and SiOx with different thicknesses from 1 to 20?nm of the insulating layer and additional AlOx or Ru protective layers. It is shown that the insulating layer does not affect the high energy spectra of the Heusler compound close to the Fermi energy. The high resolution measurements of the valence band close to the Fermi energy indicate a very large electron mean free path of the electrons through the insulating layer. The spectra of the buried thin fi…

Soft X-ray photoelectron microscopy used for the characterization of diamond, a-C and CN , thin films

Abstract This article gives an overview about the application of X-ray photoemission electron microscopy (X-PEEM) used for the analysis of carbon thin films. We present the results of an X-ray absorption near edge structure (XANES) study of CVD diamond, a-C and CNx films on Si (100) as well as a defect analysis of a hard disc scratch test. The sp2/sp3 ratio of the carbon films was determined and mapped in the electron micrographs, which show localized defects in the surface.

Coexisting electron emission mechanisms in small metal particles observed in fs-laser excited PEEM

Abstract Silver cluster films deposited on Si(1 1 1) were investigated by spectroscopic photoelectron microscopy using fs-laser excitation tuneable between hν = 1.45–1.65 eV and 2.9–3.3 eV. With increasing coverage the films grown as stepped wedges first exhibit clusters of few nanometers diameter with narrow size distributions that later agglomerate forming larger islands up to about 100 nm diameter. The cluster films have been characterized by SEM, AFM and HR-TEM. In the 3.1 eV range the small clusters emit more effectively and the dependence of electron yield on laser power follows a quadratic power law. Microspectroscopy reveals that the Fermi level onset is sharp(

Near-Edge X-ray Absorption Fine Structure Investigation of the Quasi-One-Dimensional Organic Conductor (TMTSF)2PF6

We present high-resolution near-edge X-ray absorption fine structure (NEXAFS) measurements at the P L2/3-edges, F K-edge, C K-edge and Se M2/3-edges of the quasi-one-dimensional (1D) conductor and superconductor (TMTSF)2PF6. NEXAFS allows probing the donor and acceptor moieties separately; spectra were recorded between room temperature (RT) and 30 K at normal incidence. Spectra taken around RT were also studied as a function of the angle (θ) between the electric field of the X-ray beam and the 1D conducting direction. In contrast with a previous study of the S L2/3-edges spectra in (TMTTF)2AsF6, the Se M2/3-edges of (TMTSF)2PF6 do not exhibit a well resolved spectrum. Surprisingly, the C K-…

Magnetization dynamics in microscopic spin-valve elements: Shortcomings of the macrospin picture

We have studied ultrafast magnetodynamics in micropatterned spin-valve structures using time-resolved x-ray photoemission electron microscopy combined with x-ray magnetic circular dichroism. Exciting the system with ultrafast field pulses of $250\phantom{\rule{0.3em}{0ex}}\mathrm{ps}$ width, we find the dynamic response of the free layer to fall into two distinctly different contributions. On the one hand, it exhibits localized spin wave modes that strongly depend on the shape of the micropattern. A field pulse applied perpendicular to the exchange bias field along the diagonal of a square pattern leads to the excitation of a standing spin wave mode with two nodes along the field direction.…

Momentum Distribution of Electrons Emitted from Resonantly Excited Individual Gold Nanorods.

Electron emission by femtosecond laser pulses from individual Au nanorods is studied with a time-of-flight momentum resolving photoemission electron microscope (ToF k-PEEM). The Au nanorods adhere to a transparent indium–tin oxide substrate, allowing for illumination from the rear side at normal incidence. Localized plasmon polaritons are resonantly excited at 800 nm with 100 fs long pulses. The momentum distribution of emitted electrons reveals two distinct emission mechanisms: a coherent multiphoton photoemission process from the optically heated electron gas leads to an isotropic emission distribution. In contrast, an additional emission process resulting from the optical field enhanceme…

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

Abstract 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…

Morphological and magnetic analysis of Fe nanostructures on W(110) by using scanning tunneling microscopy and Lorentz microscopy

Abstract We investigated morphological features and magnetic properties of epitaxial Fe nanostructures (films, stripes and nanoparticles) on a W(110) surface with monoatomic steps preferentially along the direction. The nanostructures were prepared in ultra-high vacuum by using electron-beam evaporation and subsequent annealing at different temperatures. Scanning tunneling microscopy measurements in-situ revealed elongated Fe nanostructures with aspect ratios of up to . The observable shape and orientation (along or perpendicular to the monoatomic steps of the substrate) of the nanostructures depended substantially on the preparation parameters. By capping the system with 7 monolayers of Pt…

Specular reflection of spin-polarized electrons from the W(001) spin-filter crystal in a large range of scattering energies and angles

Extending previous work on the imaging spin-filter technique based on electron diffraction from W(001) in the specular (00)-LEED (low-energy electron diffraction) spot, we studied the scattering-energy and angle-of-incidence landscape of spin sensitivity $S$ and reflectivity ${I/I}_{0}$. The setup includes a spin-polarized GaAs electron source and a rotatable delay-line detector for spatially resolving detection. We measured the intensity and spin asymmetry of the specularly reflected beam for energies between 14 and 37 eV and angles of incidence between ${30}^{\ensuremath{\circ}}$ and ${60}^{\ensuremath{\circ}}$. Resulting energy-angular landscapes show rather good agreement with theory [r…

High energy, high resolution photoelectron spectroscopy of Co2Mn(1-x)Fe(x)Si

This work reports on high resolution photoelectron spectroscopy for the valence band of Co2Mn(1-x)Fe(x)Si (x=0,0.5,1) excited by photons of about 8 keV energy. The measurements show a good agreement to calculations of the electronic structure using the LDA+U scheme. It is shown that the high energy spectra reveal the bulk electronic structure better compared to low energy XPS spectra. The high resolution measurements of the valence band close to the Fermi energy indicate the existence of the gap in the minority states for all three alloys.

Circular Dichroism in Photoemission from Nonmagnetic, Low- Z Solids: A Conspicuous Effect of the Photon Spin

A new phenomenon has been observed in solid-state photoemission with circularly polarized light. Its outward appearance is similar to the circular dichroism in photoabsorption. For special observation geometries, large photoelectron intensity asymmetries arise upon reversal of the photon helicity. The effect is not based on spin-orbit interaction, as is demonstrated by the example of photoemission from graphite (Z = 6). Similar asymmetries are expected for all single-crystal solids thus opening up a new class of experiments providing new tests for photoemission theories. Detailed information on the dynamics of photoexcitation of a solid can be gained, as discussed in terms of a simple orbit…

Oxygen on Fe(110): magnetic properties of the adsorbate system

Abstract Investigations concerning the electronic and magnetic properties of oxygen adsorbed on magnetized iron films were carried out by means of angle and spin resolving photoelectron spectroscopy. Iron(1 1 0), epitaxially grown on a W(1 1 0) crystal, served as the ferromagnetic substrate. Exchange splittings of the O 2p x derived level were detected demonstrating a magnetic coupling between the chemisorbate and the iron layer. This observation indicates the presence of an induced magnetic moment within the adsorbate overlayer. Variations of the exchange splitting occurred as a function of the oxygen coverage, energy of the exciting radiation, and detection angle of the emitted photoelect…

Transmission electron microscopy investigation of oxidation of (110)NiAl single crystal with wedge-shaped profile

Abstract Low energy electron diffraction (LEED), high resolution transmission electron microscopy (HRTEM), energy-dispersive X-ray (EDX), and electron energy loss spectroscopy (EELS) investigations of oxidation processes in (110)NiAl single crystal of wedge like shape, i.e., on the sample’s areas of different thickness, were carried out. It was found that in the result of several cycles of ion etching, annealing and oxidation the upper layer of (110)NiAl is enriched with Ni. With the increase of Ni concentration from 50 to 100 at. %, the stoichiometry of the near surface area changes and the new phases of Ni3Al and Ni with Al doping are formed one after another. Up to Ni content of 75 at. %…

Photoemission from Pt(111)-(hex)-Rb and Pt(111)-(4×1)-RbO using polarised synchrotron radiation

Abstract In various experiments it has been demonstrated that the circular dichroism in the angular distribution of photoelectrons (CDAD) is not only observed from oriented initial states (aligned adsorbed molecules or magnetised samples), but also arises as a consequence of the scattering of photoelectrons from the surrounding atoms in a solid or an adsorbate. In this work we will show first measurements performed at the SGM beamline of the Brazilian Synchrotron Light Source (LNLS) on a (4×1) superstructure of 1 ML RbO adsorbed on Pt(111). Measurements from the 4s core levels of Rb adsorbed at Pt(111) were also performed at the PM-III beamline at BESSY. The measured variations of the inten…

Influence of the symmetry on the circular dichroism in angular resolved core-level photoemission

The model for angular resolved photoemission from adsorbed atoms is extended to account for the non-axial symmetry of atoms in a crystal field. In particular, circular dichroism in the angular distribution (CDAD) is theoretically investigated. A special emphasis is put on the case when incident photons are propagating along the principal axis of an atom in Cnv symmetry. The model, although mainly developed for adsorbates, may also be used as a base for emission from solid surfaces. An extension to simple bulk symmetries, like D for hexagonal or O for cubic crystals, is included. The CDAD 6 hh for normal incidence does not vanish in the extended model and reflects the symmetry of the adsorpt…

Quantitative measurements of magnetic stray field dynamics of Permalloy particles in a photoemission electron microscopy

By example of a Permalloy particle (40 × 40 μm(2) size, 30 nm thickness) we demonstrate a procedure to quantitatively investigate the dynamics of magnetic stray fields during ultrafast magnetization reversal. The measurements have been performed in a time-resolving photoemission electron microscope using the X-ray magnetic circular dichroism. In the particle under investigation, we have observed a flux-closure-dominated magnetic ground structure, minimizing the magnetic stray field outside the sample. A fast magnetic field pulse introduced changes in the micromagnetic structure accompanied with an incomplete flux closure. As a result, stray fields arise along the edges of domains, which cau…

Investigations of the corrosion protection of ultrathin a-C and a-C:N overcoats for magnetic storage devices

Abstract The thickness-dependent corrosion protection of carbon overcoats for magnetic hard disks can be analyzed by collecting X-ray absorption near edge structure (XANES) spectra at the Co L3-edge. Co is the main constituent of the protected magnetic media underneath. The spectra of the Co absorption edge display a strong peak for pure metallic, non-oxidized Co. This peak splits up into several sub-structures for oxidized Co. Therefore, XANES spectra provide a straightforward method to determine the overcoat thickness, leading to closed coverage and corrosion protection of the underlying material. A similar approach was carried out by X-ray photoelectron spectroscopy (XPS). Standard a-C:N…

Recent progress in photoemission microscopy with emphasis on chemical and magnetic sensitivity

Abstract With the improved access to synchrotron radiation sources photoemission electron microscopy is developing into a versatile analytical tool in surface and materials science. The broad spectral range and the well-defined polarization characteristics of synchrotron light permit a unique combination of topographic, chemical, and even magnetic investigations down to a mesoscopic scale. The potentiality of photoemission electron microscopy is demonstrated by several experiments on surfaces and microstructured thin film systems, which have been carried out with a newly designed instrument. We discuss its different modes of operation with respect to both microscopy and spectroscopy. A comb…

Time-of-flight photoelectron emission microscopy TOF-PEEM: first results

The time structure of the synchrotron radiation at BESSY (Berlin) is used to operate a photoemission electron microscope in a time-of-flight (TOF) mode. The electrons which are emitted from the sample surface with different energies are dispersed in a drift tube subsequent to the imaging optics. The screen of the microscope was replaced by a fast scintillator (tau = 1.4 ns) and the light is detected by an ultra fast gated intensified CCD camera (800 ps gate 1 MHz repetition rate). The resolving power in the energy domain is demonstrated and possible implications on the spatial resolution (chromatic correction) are discussed. Additionally, an improved contrast at very low emission energies i…

Spinovo rozlisena time-of-flight k-reozlisena fotoemissia Ir-- Kompletny fotoemissny experiment.

Ultramicroscopy 183, 19 - 29 (2017). doi:10.1016/j.ultramic.2017.06.025

Momentum-resolved photoelectron absorption in surface barrier scattering on Ir(111) and graphene/Ir(111)

Physical review / B 96(15), 155108 (2017). doi:10.1103/PhysRevB.96.155108

Optical magnetic circular dichroism in threshold photoemission from a magnetite thin film

Threshold photoemission excited by polarization-modulated ultraviolet femtosecond laser light is exploited for phase-sensitive detection of magnetic circular dichroism (MCD) for a magnetite thin film. Magnetite (Fe(3)O(4)) shows a magnetic circular dichroism of ∼(4.5 ± 0.3) × 10(-3) for perpendicularly incident circularly polarized light and a magnetization vector switched parallel and antiparallel to the helicity vector by an external magnetic field. The asymmetry in threshold photoemission is discussed in comparison to the magneto-optical Kerr effect. The optical MCD contrast in threshold photoemission will provide a basis for future laboratory photoemission studies on magnetic surfaces.

Suppression of the vacuum space-charge effect in fs-photoemission by a retarding electrostatic front lens

Review of scientific instruments 92(5), 053703 (2021). doi:10.1063/5.0046567

Energy- and angle-dependent threshold photoemission magnetic circular dichroism from an ultrathin Co/Pt(111) film

Threshold photoemission magnetic circular dichroism (TPMCD) in one-photon photoemission (1PPE) and two-photon photoemission (2PPE) is measured at an ultrathin Co film grown on Pt(111). Energy-dependent measurements reveal maximum asymmetries directly at the photoemission threshold (1.90% for 1PPE and 11.7% for 2PPE) which weakly decrease with increasing photon energy. The measured TPMCD asymmetries are discussed in two excitation models on the basis of spin-resolved band-structure calculations. For the model of direct band-to-band transitions in other k directions than the direction of observation (Gamma-L) ab initio calculations for 1PPE and 2PPE are performed. The theory is in reasonable …

Design for a high resolution electron energy loss microscope.

International audience; An electron optical column has been designed for High Resolution Electron Energy Loss Microscopy (HREELM). The column is composed of electron lenses and a beam separator that are placed between an electron source based on a laser excited cesium atom beam and a time-of-flight (ToF) spectrometer or a hemispherical analyzer (HSA). The instrument will be able to perform full field low energy electron imaging of surfaces with sub-micron spatial resolution and meV energy resolution necessary for the analysis of local vibrational spectra. Thus, noncontact, real space mapping of microscopic variations in vibrational levels will be made possible. A second imaging mode will al…

Spin resolved photoemission study of Co(0001) films

Abstract Thin ferromagnetic films are of great practical interest as they can exhibit a different magnetic behaviour compared to the bulk crystals due to, e.g., the surface anisotropy. The electronic and magnetic properties of thin cobalt films evaporated on W(110) have been investigated by means of angle and spin resolving photoelectron spectroscopy. The study was focused on electron spin polarization, spin resolved intensities and band structure behaviour in dependence of film thickness, excitation energy, and photoelectron detection angle. In order to interpret the experimental results, we have performed relativistic band structure calculations for the Co(0001) surface. The observed agre…

CONDENSATION OF REFRACTORY METALS IN ASYMPTOTIC GIANT BRANCH AND OTHER STELLAR ENVIRONMENTS

The condensation of material from a gas of solar composition has been extensively studied, but less so condensation in the environment of evolved stars, which has been mainly restricted to major compounds and some specific element groups such as the Rare Earth elements. Also of interest, however, are refractory metals like Mo, Ru, Os, W, Ir, and Pt, which may condense to form refractory metal nuggets (RMNs) like the ones that have been found in association with presolar graphite. We have performed calculations describing the condensation of these elements in the outflows of s-process enriched AGB stars as well as from gas enriched in r-process products. While in carbon-rich environments (C …

Direct observation of half-metallicity in the Heusler compound $Co_{2}MnSi$

Ferromagnetic thin films of Heusler compounds are highly relevant for spintronic applications owing to their predicted half-metallicity, that is, 100% spin polarization at the Fermi energy. However, experimental evidence for this property is scarce. Here we investigate epitaxial thin films of the compound Co2MnSi in situ by ultraviolet-photoemission spectroscopy, taking advantage of a novel multi-channel spin filter. By this surface sensitive method, an exceptionally large spin polarization of () % at room temperature is observed directly. As a more bulk sensitive method, additional ex situ spin-integrated high energy X-ray photoemission spectroscopy experiments are performed. All experimen…

Synthesis of refractory metal nuggets and constraints on the thermal histories of nugget-bearing Ca, Al-rich inclusions

Tiny refractory metal nuggets are mainly observed inside Ca, Al-rich inclusions (CAIs) from chondritic meteorites and are commonly assumed to be condensates from a solar composition gas. However, recent detailed studies of metal nugget compositions and their comparison with predictions from condensation show that the observed abundance patterns are extremely difficult to achieve in this way. As a test for the proposed alternative, precipitation from a silicate liquid, we conducted melting experiments, in which nine different refractory metals (nugget components) were equilibrated with each other along with a CAI-like liquid at reducing conditions. When quenched, minerals similar to those in…

Nanoelectron spectroscopy for chemical analysis: a novel energy filter for imaging x-ray photoemission spectroscopy

An ovel instrument for imaging ESCA is described. It is based on a tandem arrangement of two hemispherical energy analysers used as an imaging energy filter. The main spherical aberration (α 2 -term) of the analyser is corrected by the antisymmetry of the tandem configuration. The kinetic energy range useable for imaging extends up to 1.6 keV; this is compatible with Mg and Al Kα laboratory x-ray sources. First experiments on the chemical surface composition of a Cu0.98Bi0.02 polycrystal, a GaAs/AlGaAs heterostructure and Ag crystallites on Si(111) have been performed using synchrotron radiation. The results reveal an energy resolutio no f190 meV and a lateral resolution (edge resolution) o…

Self-Trapping of Magnetic Oscillation Modes in Landau Flux-Closure Structures

We investigated the magnetodynamics in rectangular Permalloy platelets by means of time-resolved x-ray photoemission microscopy. 10 nm thick platelets of size 16 x 32 microm were excited by an oscillatory field along the short side of the sample with a fundamental frequency of 500 MHz and considerable contributions of higher harmonics. Under the influence of the oscillatory field, the Néel wall in the initial classical Landau pattern shifts away from the center, corresponding to an induced magnetic moment perpendicular to the exciting field. This phenomenon is explained by a self-trapping effect of the dominating spin-wave mode when the system is excited just below the resonance frequency. …

Rashba splitting of the Tamm surface state on Re(0001) observed by spin-resolved photoemission and scanning tunneling spectroscopy

Physical review research 2(1), 013296 (2020). doi:10.1103/PhysRevResearch.2.013296

Chromatic and Spherical Aberration Correction Using Time-Dependent Acceleration and Lens Fields

Spatially resolved observation of dynamics in electrical and magnetic field distributions by means of a delayline detector and PEEM

Abstract Photoemission electron microscopy (PEEM) was exploited to observe the dynamics in local field distributions on microstrip-line devices with a best time resolution of 133 ps. A delayline detector system served as imaging unit capable of a time resolving data acquisition and processing. The setup can be operated at the resolution limit of the PEEM of about 20 nm while a continuously illuminating UV-lamp excites the photoelectrons in threshold photoemission. A pulsed photon source is not needed to obtain time resolved images, the time reference of the data acquisition was taken by a periodic signal (clock, here typ. 100 MHz) in phase with the pulse pattern applied to the microstrip-li…

Chalcogen adsorption and surface magnetism

Abstract Investigations concerning the electronic and magnetic properties of oxygen and sulfur adsorbed on magnetized surfaces were carried out by means of angle and spin resolving photoelectron spectroscopy. Iron(110), a polycrystalline iron alloy, and an amorphous metallic glass (Fe 79 B 16 Si 5 ) served as ferromagnetic substrates. Exchange splittings of the O 2p and S 3p derived levels could be detected, demonstrating a magnetic coupling between the chemisorbate and iron. This observation presents a prerequisite for an induced magnetic moment within the adsorbate overlayer. For sulfur an adsorbate-induced structure only in the minority spin channel near the Fermi level was observed whic…

Time-of-flight photoemission electron microscopy – a new way to chemical surface analysis

Abstract The time structure of synchrotron radiation at BESSY I (Berlin) was utilised to operate a photoemission electron microscope in the time-of-flight mode. The electrons that are emitted from the sample surface with different energies are dispersed in a drift tube subsequent to the imaging optics. Two ways of fast image detection have been explored, a fast gated intensified CCD camera (800 ps gate time) and a special counting electronics in combination with a 3D (x,y,t)-resolving delay line detector ( time resolution ps). The latter device has a lateral resolution of about 50 μm in the image plane being equivalent to 1000 pixels along the image diagonal. An energy resolution of 400 meV…

Threshold photoemission magnetic circular dichroism at the spin-reorientation transition of ultrathin epitaxial Pt/Co/Pt(111)/W(110) films

X-ray magnetic circular dichroism (MCD) is nowadays widely used for the investigation of magnetic properties of surfaces and thin films. Recently, similarly large effects have been observed for UV-VIS MCD effects both in single [1] and two-photon photoemission [2-3]. This threshold MCD effect is directly related to spin-orbit effects present at the Fermi edge. We report on the observation of threshold photoemission magnetic circular dichroism (TPMCD) in one-photon and two-photon photoemission (1PPE and 2PPE) at a Pt-capped ultrathin Co wedge grown on Pt(111)/W(110) using femtosecond laser light. TPMCD measurements result in asymmetries continuously increasing with the sample thickness. This…

Determination of surface and interface magnetic properties for the multiferroic heterostructure Co/BaTiO3using spleed and arpes

Co/BaTiO$_3$(001) is one of the most interesting multiferroic heterostructures as it combines different ferroic phases, setting this way the fundamentals for innovative technical applications. Various theoretical approaches have been applied to investigate the electronic and magnetic properties of Co/BaTiO$_3$(001). Here we determine the magnetic properties of 3 ML Co/BaTiO$_3$ by calculating spin-polarized electron diffraction as well as angle-resolved photoemission spectra, with both methods being well established as surface sensitive techniques. Furthermore, we discuss the impact of altering the BaTiO$_3$ polarization on the spectra and ascribe the observed changes to characteristic deta…

IMAGING OF DICHROISM IN PHOTOEMISSION ELECTRON MICROSCOPY AT NONMAGNETIC MATERIALS USING CIRCULARLY POLARIZED SOFT X-RAYS

A new approach for investigations of circular dichroism in the angular distribution of photoelectrons (CDAD) is presented. The image contrast using a photoemission line of a certain material is combined with imaging of the angular distribution pattern using a photoemission electron microscope (PEEM). CDAD can be used to investigate pure scattering information by means of the same instrument in microscopically selected regions on a surface. The experiment combines angle-resolved XPS imaging with the indirect mapping of the local environment of atoms by means of CDAD holography. In a conventional photoelectron diffraction or photoelectron holography experiment, it is necessary to move the sa…

Circular dichroism in x-ray photoemission from core levels of nonmagnetic species

Circular dichroism in the angular distribution of photoelectrons (CDAD) has been observed in core-level photoemission from spherically symmetric initial states of nonmagnetic species utilizing circularly polarized soft-x-ray radiation from BESSY. Up to now, CDAD was predicted and observed only for aligned initial states. The data for oriented CO molecules prove that circular x-ray dichroism in photoemission from core levels is a general phenomenon that is not restricted to ferromagnets. High asymmetries of 50% suggest future applications as an effective circular x-ray analyzer.

Valence band photoemission from thin iron films - A comparison of experimental and theoretical results

Abstract In this contribution, we report on photoemission data from thin iron films on W(110) that have been carried out by means of spin-resolved photoelectron spectroscopy as well as Magnetic Circular Dichroism in valence band photoemission at the storage ring BESSY. These techniques give complementary information on the electronic and magnetic properties, such as exchange and spin–orbit splitting. We compare our experimental data to new photoemission calculations, which have been obtained in the framework of a fully relativistic one-step theory for ferromagnetic materials.

Dopant Contrast in Semiconductors as Interpretation Challenge at Imaging by Electrons

Mechanisms responsible for the contrast between differently doped areas in semiconductors, which is observed in electron micrographs, is discussed as regards the key factors determining the sign and magnitude of the contrast. Experimental data obtained by means of the scanning electron microscope (SEM), scanning low energy electron microscope and photoelectron emission microscope are reviewed together with hints following from them for compilation of a model of the contrast mechanism.

Dichroism in angular resolved VUV-photoemission from the (0001) surfaces of thin Gd and Nd films epitaxially grown on W(110)

We present investigations of the electronic and magnetic structure of the Rare Earth valence states. In particular, we have examined ultra thin films (≤ 10 ML) of the rare earth metals gadolinium and neodymium epitaxially grown on tungsten (110). Various experiments on dichroism in angular resolved photoemission have been performed using circularly as well as linearly polarised light in the VUV-range with photon energies below 40 eV. A special emphasis was placed on the investigation of the surface state, which was observed for both Gd and Nd. A very small magnetic splitting of about 25 meV was observed for the surface state of ferromagnetic Gd. A magnetic ordering of a Nd-monolayer on a re…

Energy- and k -resolved mapping of the magnetic circular dichroism in threshold photoemission from Co films on Pt(111)

The magnetic circular dichroism in threshold photoemission (TPMCD) for perpendicularly magnetized fcc Co films on Pt(111) has been revisited. A complete mapping of the spectral function $I({E}_{B},{k}_{x},{k}_{y})$ (binding energy ${E}_{B}$, momentum parallel to surface ${k}_{x}$, ${k}_{y}$) and the corresponding TPMCD asymmetry distribution ${A}_{\mathrm{MCD}}({E}_{B},{k}_{x},{k}_{y})$ has been performed for one-photon and two-photon photoemission using time-of-flight momentum microscopy. The experimental results allow distinguishing direct from indirect transitions. The measurements reveal clear band features of direct transitions from bulk bands that show a nontrivial asymmetry pattern. …

AN EXPERIMENTAL PROOF OF THE BACK-SCATTERING MODEL FOR DICHROIC EFFECTS IN VUV PHOTOEMISSION

The energy dependence of the circular dichroism in the angular distribution of photoelectrons (CDAD) was investigated from the shallow Cs 5p core levels. Cesium was prepared in a hexagonal ordered monolayer on W(110). The results are mainly influenced by scattering of the photoelectrons within the adlayer. At low energies, the behavior observed is described by means of a model that treats only the back-scattering of photoelectrons at the potential step between the adlayer and the substrate. It leads to a simple method determining the position of the monolayer with respect to the substrate. In this approach, the back-scattering model is matched with the measured energy dependence of the CDA…

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

AbstractWe 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 "Equation missing"-point, we observe a tilted Dirac cone with circularly shaped cross section and a Dirac crossing at 0.28 × "Equation missing" "Equation missing" 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.

Soft X-ray emission spectroscopy used for the characterization of a-C and CNx thin films

Abstract We present the results of a soft X-ray emission spectroscopy study of a-C and CNx films on a Si(100) substrate. Also for the characterization of the homogeneity in depth of these films electron energy loss spectroscopy measurements with localization better than 4 nm were carried out. In case of CNx films the highest diamond-like modification occurs in the region close to the Si(100) substrate. The film density decreases with increasing distance from the substrate and becomes almost constant in range of thicknesses more than ~ 2 nm.

Electronic structure of large disc-type donors and acceptors

Searching for new pi-conjugated charge-transfer systems, the electronic structure of a new acceptor-donor pair derived from coronene (C(24)H(12)) was investigated by ultraviolet photoelectron spectroscopy (UPS). The acceptor coronene-hexaone (C(24)H(6)O(6), in the following abbreviated as COHON) and the donor hexamethoxycoronene (C(30)H(24)O(6), abbreviated as HMC) were adsorbed as pure and mixed phases on gold substrates. At low coverage, COHON adsorption leads to the appearance of a charge-transfer induced interface state 1.75 eV below the Fermi energy. At multilayer coverage the photoemission intensity of the interface state drops and the valence spectrum of neutral COHON appears. The sa…

Slater-Pauling Rule and Curie-Temperature of Co$_2$-based Heusler compounds

A concept is presented serving to guide in the search for new materials with high spin polarization. It is shown that the magnetic moment of half-metallic ferromagnets can be calculated from the generalized Slater-Pauling rule. Further, it was found empirically that the Curie temperature of Co$_2$ based Heusler compounds can be estimated from a seemingly linear dependence on the magnetic moment. As a successful application of these simple rules, it was found that Co$_2$FeSi is, actually, the half-metallic ferromagnet exhibiting the highest magnetic moment and the highest Curie temperature measured for a Heusler compound.

Element-specific magnetic moments from core-absorption magnetic circular dichroism of the doped Heusler alloyCo2Cr0.6Fe0.4Al

The magnetic circular dichroism (MCD) of core-level absorption (x-ray absorption spectroscopy, XAS) spectra in the soft x-ray region has been measured for the ferromagnetic Heusler alloy ${\mathrm{Co}}_{2}{\mathrm{Cr}}_{0.6}{\mathrm{Fe}}_{0.4}\mathrm{Al}$ at the Co, Fe, and Cr ${L}_{II,III}$ edges. The comparison of XAS spectra before and after in situ cleaning of polished surfaces revealed a pronounced selective oxidation of Cr in air. For clean surfaces we observed a MCD for all three elements with Fe showing the largest moment per atom. The MCD can be explained by the density of states of the $3d$ unoccupied states, predicted by linear muffin-tin orbital atomic sphere approximation. For …

Relation between spin–orbit induced spin polarization, Fano-effect and circular dichroism in soft x-ray photoemission

A Feynman diagram analysis of photoemission probabilities suggests a relation between two final-state spin polarization effects, the optical spin-orientation originating from the interaction with circularly polarized light ([Formula: see text], Fano effect) and the spin polarization induced by the spin-orbit scattering ([Formula: see text], Mott effect). The analysis predicts that [Formula: see text] is proportional to the product of [Formula: see text] and the circular dichroism in the angular distribution (CDAD) of photoelectrons. To confirm this prediction, the spin polarization of photoelectrons excited by soft x-ray radiation from initial spin-degenerate bulk states of tungsten using t…

Donor–anion interactions at the charge localization and charge ordering transitions of (TMTTF)2AsF6 probed by NEXAFS

High-resolution near-edge X-ray absorption fine structure (NEXAFS) measurements at the As M-edge, F K-edge and S L-edge of the Fabre salt (TMTTF)2AsF6 were performed from room temperature (RT) to 90 K, allowing to reach the charge localization regime below Tρ ≈ 230 K and to cross the charge ordering (CO) transition at TCO ≈ 102 K. The F K-edge and S L-edge spectra exhibit several transitions which have been indexed on the basis of first-principles DFT calculations. Upon cooling from RT significant energy shifts up to +0.8 eV and -0.4 eV were observed in transitions exhibited by the F 1s and S 2p spectra respectively, while the As 3p doublet does not show a significant shift. Opposite energy…

Generalization of the atomic random-phase-approximation method for diatomic molecules:N2photoionization cross-section calculations

Partial and total photoionization cross sections of ${\mathrm{N}}_{2}$ molecule are calculated using the generalization of the random-phase approximation (RPA) which earlier has been successfully applied to the description of the atomic photoionization processes. According to this method, at first the Hartree-Fock (HF) ground-state wave functions are calculated in prolate spheroidal coordinates using the fixed-nuclei approximation. With their help the zero order basis set of single particle Hartree-Fock wave functions containing both discrete excited states and continuous spectrum is calculated in the field of a frozen core of a singly charged ion. The calculations are performed for all fou…

A new approach for actinic defect inspection of EUVL multilayer mask blanks: Standing wave photoemission electron microscopy

Extreme ultraviolet lithography (EUVL) at 13.5 nm is the next generation lithography technique capable of printing sub-50 nm structures. With decreasing feature sizes to be printed, the requirements for the lithography mask also become more stringent in terms of defect sizes and densities that are still acceptable and the development of lithography optics has to go along with the development of new mask defect inspection techniques that are fast and offer high resolution (preferable in the range of the minimum feature size) at the same time. We report on the development and experimental results of a new 'at wavelength' full-field imaging technique for defect inspection of multilayer mask bl…

Magnetic circular and linear dichroism in VUV-photoemission from thin iron films on W(110)

Abstract We report on two different photoemission techniques for ferromagnetic surfaces: the phenomena of magnetic circular and linear dichroism in the angular distribution of photoelectrons MCDAD and MLDAD. MCDAD had already been studied in detail for different systems. Now we are able to compare our MCDAD results from thin iron films on W(110) to new data from magnetic linear dichroism MLDAD. Both effects (MCDAD and MLDAD) have been studied in the identical photon energy region (up to hv = 36 eV). The results will be discussed with respect to a bandstructure calculation.

Real-space observation of xenon adsorption and desorption kinetics on graphite (0001) by photoemission electron microscopy

Abstract The growth and desorption of Xe monolayers on the basal plane of graphite has been investigated by real-space imaging using photoemission electron microscopy. Adsorption kinetics was studied at different substrate temperatures (39–65 K), corresponding to different growth modes. Coexisting phases showed up as different grey values in the image. Typical domain sizes of the 2D solid phases around 60 K are of the order of one to several μm. The domains exhibit an elongated shape with their long axis oriented preferentially parallel to step edges of the substrate. With increasing coverage the brightness of the domains increases, the 2D gas-phase regions shrink and finally disappear at h…

Charge transfer in the novel donor-acceptor complexes tetra- and hexamethoxypyrene with tetracyanoquinodimethane studied by HAXPES

Abstract The effect of charge transfer (CT) in complexes of the donors tetra - and hexamethoxyprene ( TMP and HMP ) with the classical acceptor tetracyanoquinodimethane ( TCNQ ) was studied using hard X-ray photoemission (HAXPES). Microcrystals of the complex were grown via vapour diffusion from donor–acceptor mixtures. The bulk sensitivity of HAXPES at a photon energy of 6 keV completely eliminates the problem of surface contamination for such delicate organic materials grown from solution. The donor molecules were produced using a novel synthesis route functionalizing polycyclic aromatic hydrocarbons at their periphery. For comparison, spectra were also taken from thin-film samples of the…

Transient spatio-temporal domain patterns in permalloy microstructures induced by fast magnetic field pulses

The response of multidomain flux-closure structures (Landau states) in micrometer-scale magnetic thin-film elements upon fast magnetic field pulses leads to the excitation of magnetic eigenmodes and to short-lived domain patterns that do not occur in quasi-static remagnetisation. Such transient spatio-temporal patterns and particular detail features are discussed. Examples are presented for permalloy platelets of various shapes and sizes. Dynamic series of domain patterns with variable delay between field pulse and photon pulse (synchrotron radiation) have been taken using stroboscopic XMCD-PEEM. Precessional remagnetisation starts at the domain boundaries. The damped precessional motion pr…

Photoemission time-of-flight spectromicroscopy of Ag nanoparticle films on Si(111)

Abstract Time-of-flight photoemission electron microscopy was used to measure spatially resolved energy distribution curves of electrons emitted from Ag nanoparticle films with different mass thicknesses. Two-photon photoemission (2PPE) was induced by femtosecond laser pulse excitation with 3.1 eV photon energy and 200 fs pulse width. Regions of Ag nanoparticles with different average sizes and one region with a continuous 100 nm thick Ag film were deposited as a stepped wedge on a Si(1 1 1) substrate. Upon laser excitation the nanoparticle films exhibit a very high electron emission yield in the images, whereas the uncovered Si surface and the continuous Ag film are dark. The time-of-fligh…

Microscopic origin of the charge transfer in single crystals based on thiophene derivatives: A combined NEXAFS and density functional theory approach

We have investigated the charge transfer mechanism in single crystals of DTBDT-TCNQ and DTBDT-F4TCNQ (where DTBDT is dithieno[2,3-d;2',3'-d'] benzo[1,2-b;4,5-b']dithiophene) using a combination of near-edge X-ray absorption spectroscopy (NEXAFS) and density functional theory calculations (DFT) including final state effects beyond the sudden state approximation. In particular, we find that a description that considers the partial screening of the electron-hole Coulomb correlation on a static level as well as the rearrangement of electronic density shows excellent agreement with experiment and allows to uncover the details of the charge transfer mechanism in DTBDT-TCNQ and DTBDT-F4 TCNQ, as w…

Evidence of Spatially Inhomogeneous Electron Temperature in a Resonantly Excited Array of Bow-Tie Nanoantennas

We studied the excitation of large-area Au bow-tie nanoantenna arrays, which we have fabricated on indium-tin-oxide (ITO)-coated glass substrates using colloidal lithography with nanoscale polystyr...

Peculiarities of imaging one- and two-dimensional structures using an electron microscope in the mirror operation mode.

Measurements performed in an electron microscope with the mirror operation mode are most sensitive to local electric fields and geometrical roughness of any kind of the object being studied. The object with a geometrical relief is equivalent to a smooth surface with an effective distribution of microfields. Electrons forming the image interact with the local microfields for an extended time: during approach to the object, deceleration and acceleration away from the object. As a result, the electron trajectories can be strongly distorted, and the contrast changes essentially, leading to image deformation of details of the object under investigation and to lowering of the resolution. These ef…

Magnetic Circular Dichroism in Two-Photon Photoemission

We report the observation of magnetic circular dichroism (MCD) in two-photon photoemission (2PPE). The Heusler alloys Ni2MnGa and Co2FeSi were investigated by excitation with femtosecond laser light, showing MCD asymmetries of A=(3.5+/-0.5)x10;{-3} for Ni2MnGa and of A=(2.1+/-1.0)x10;{-3} for Co2FeSi, respectively. A theoretical explanation is provided based on local spin-density calculations for the magnetic dichroic response; the computed 2PPE MCD agrees well with the experiment. The observed 2PPE magnetic contrast represents an interesting alternative for future time-resolved photoemission studies on surface magnetism practicable in the laboratory.

DIRECT EVIDENCE FOR CONDENSATION IN THE EARLY SOLAR SYSTEM AND IMPLICATIONS FOR NEBULAR COOLING RATES

We have identified in an acid resistant residue of the carbonaceous chondrite Murchison a large number (458) of highly refractory metal nuggets (RMNs) that once were most likely hosted by Ca,Al-rich inclusions (CAIs). While osmium isotopic ratios of two randomly selected particles rule out a presolar origin, the bulk chemistry of 88 particles with sizes in the submicron range determined by energy dispersive X-ray (EDX) spectroscopy shows striking agreement with predictions of single-phase equilibrium condensation calculations. Both chemical composition and morphology strongly favor a condensation origin. Particularly important is the presence of structurally incompatible elements in particl…

Measurement of magnetic fields and domain structures using a photoemission electron microscope

Publisher Summary This chapter describes the theory and experiments on study of the domain structure of ferromagnets using various operation modes of a photoemission electron microscope (PEEM). The technique of PEEM allows observation of the domain boundaries on ferromagnetic surfaces arising from magnetic stray fields at definite conditions. In most cases, a very weak contrast due to the Lorentz force is formed. It can be measured by the use of digital methods of signal registration and data processing. From the form of the observed signal, conclusions about the shape of the stray field of the domain boundary can be drawn if there is additional information. The calculation of the image con…

Characterization and magnetic properties of nanoparticles based on FePt solid solution with an oxide shell

Abstract We present the results of magnetic properties investigations of ferromagnetic nanoparticles which ensembled with ferromagnetic shell. The aim of this work is to study the connection of structure–phase composition and thermal treatment with the magnetic properties, partially, with the coercive force and the exchange bias field in a two-dimension spin system of core–shell type. It is found that the exchange bias field increases with the growth of the oxide shell thickness. This is realized by annealing in a dosed oxygen flow. The decrease of the coercive force with the increase of annealing temperature is connected with the concentration effect (the concentration of ferromagnetic par…

Investigating spintronics thin film systems with synchrotron radiation

Abstract Spintronics is a research field involving a wide variety of different magnetic materials. Synchrotron radiation in the VUV and soft X-ray regime is ideally suited to investigate the relationships between magnetic properties and electronic structure of spintronics thin film stacks. Complex layered structures and nanomagnets are the main building blocks for current and future spintronics applications. In this contribution we describe the study of spintronics model systems with respect to the static and dynamic behavior with an emphasis on interfaces.

Oxygen on Fe(100) and Fe(110)

Investigations of the electronic and magnetic properties of oxygen adsorbed on magnetized iron films have been carried out by means of angle and spin resolving photoelectron spectroscopy. Iron, epitaxially grown on W(100) and W(110) crystals, served as the ferromagnetic substrate. Exchange splittings of the O 2px derived level have been detected, demonstrating a magnetic coupling between the chemisorbate and the iron layer. Variations of the exchange splitting have occurred as a function of the oxygen coverage, photon energy, and emission angle. High oxygen exposures have lead to a FeO overlayer at the surface.

Investigation of a novel material for magnetoelectronics: Co2Cr0.6Fe0.4Al

Heusler compounds are promising candidates for future spintronics device applications. The electronic and magnetic properties of Co2Cr0.6Fe0.4Al, an electron-doped derivative of Co2CrAl, are investigated using circularly polarized synchrotron radiation and photoemission electron microscopy (PEEM). Element specific imaging reveals needle shaped Cr rich phases in a homogeneous bulk of the Heusler compound. The ferromagnetic domain structure is investigated on an element-resolved basis using x-ray magnetic circular dichroism (XMCD) contrast in PEEM. The structure is characterized by micrometre-size domains with a superimposed fine ripple structure; the lateral resolution in these images is abo…

Circular dichroism in angular resolved photoemission from pure and Rb-doped C60 and C22H14 layers on platinum and tungsten

Abstract Polycrystalline C60 and Pentacene films grown on W(110) and Pt(111) have been studied in valence band photoemission using circularly polarised synchrotron radiation from BESSY with special emphasis on circular dichroism in photoemission. For thin films of C60, dichroic asymmetries of about 10% occur independent of the temperature and the substrate hinting that the rotation of the topmost layer is hindered even at room temperature. For Pentacene we found asymmetries up to 50% in the region of the σ-electrons. Moreover, we found for this molecule a dichroic asymmetry in normal emission, that is a forbidden geometry. This hints on adsorption with the molecules perpendicularly oriented…

Orbital-Resolved Partial Charge Transfer from the Methoxy Groups of Substituted Pyrenes in Complexes with Tetracyanoquinodimethane—A NEXAFS Study

It is demonstrated that the near-edge X-ray absorption fine structure (NEXAFS) provides a powerful local probe of functional groups in novel charge transfer (CT) compounds and their electronic properties. Microcrystals of tetra-/hexamethoxypyrene as donors with the strong acceptor tetracyano-p-quinodimethane (TMP/HMP-TCNQ) were grown by vapor diffusion. The oxygen and nitrogen K-edge spectra are spectroscopic fingerprints of the functional groups in the donor and acceptor moieties, respectively. The orbital selectivity of the NEXAFS pre-edge resonances allows us to precisely elucidate the participation of specific orbitals in the charge transfer process. Upon complex formation, the intensit…

Band structure tuning of Heusler compounds: Spin- and momentum-resolved electronic structure analysis of compounds with different band filling

Physical review / B 103(5), 054407 (2021). doi:10.1103/PhysRevB.103.054407

Single-Hemisphere Photoelectron Momentum Microscope With Time-of-Flight Recording

Photoelectron momentum microscopy is an emerging powerful method for angle-resolved photoelectron spectroscopy (ARPES), especially in combination with imaging spin filters. These instruments record kx-ky images, typically exceeding a full Brillouin zone. As energy filters double-hemispherical or time-of-flight (ToF) devices are in use. Here we present a new approach for momentum mapping of the full half-space, based on a single hemispherical analyzer (path radius 225 mm). Excitation by an unfocused He lamp yielded an energy resolution of 7.7 meV. The performance is demonstrated by k-imaging of quantum-well states in Au and Xe multilayers. The alpha-square-aberration term (alpha: entrance an…

Spectral Measurement of Photon Emission from Individual Gold Nanoparticles Using Scanning Tunneling Microscopy

The light emission spectra of individual Au nanoparticles induced by a scanning tunneling microscope (STM) have been investigated. Two-dimensional ensembles of tunnel-coupled Au particles were prepared by thermal evaporation onto a native oxide silicon wafer in ultrahigh vacuum (10 – 9 mbar). Our STM measurements show a single peak at photon energy 1.6 eV in the tunneling mode and two peaks at 2.2 eV (connected with the Mie plasmon) and 1.45 eV (a new peak which was not discussed in literature before) in the field emission mode.

Temperature-dependent angular resolved UV-photoemission spectroscopy from CeNi2Ge2

Abstract Pronounced temperature effects in angular resolved ultraviolet photoelectron spectroscopy from the (001) surface of the ternary heavy fermion compound CeNi 2 Ge 2 are presented. The measurements were performed on atomically clean and well-ordered thin films grown on a W(110) substrate. A strongly enhanced intensity at the Fermi edge ( ϵ F ) is observed at low-temperatures if the spectra are excited by means of HeI light ( hν =21.2 eV). In addition, the work function is dramatically increased with temperature, exhibiting an unusually high positive temperature coefficient of about 0.65 meV/K. The observed temperature dependency suggests a strong redistribution of the states near the …

Magnetic Domain Imaging of Thin Metallic Layers Using PEEM

Photoemission electron microscopy (PEEM) in combination with resonant excitation by circularly polarized soft X-rays has proven to be a powerful analytical tool for the study of magnetic microstructures and multilayers. In this type of electron microscope the lateral intensity distribution of the emitted low-energy secondary or photoelectrons is imaged by an electron-optical system. Owing to its fast parallel image acquisition, its wide zoom range allowing fields of view from almost 1 mm down to a few µm combined with a high base-resolution of the order of 20 nm, the method offers a unique access to many aspects in surface and thin film magnetism on the mesoscopic length scale. Magnetic con…

Multi-MHz time-of-flight electronic bandstructure imaging of graphene on Ir(111)

In the quest for detailed spectroscopic insight into the electronic structure at solid surfaces in a large momentum range, we have developed an advanced experimental approach. It combines the 3D detection scheme of a time-of-flight momentum microscope with an optimized filling pattern of the BESSY II storage ring. Here, comprehensive data sets covering the full surface Brillouin zone have been used to study faint substrate-film hybridization effects in the electronic structure of graphene on Ir(111), revealed by a pronounced linear dichroism in angular distribution. The method paves the way to 3D electronic bandmapping with unprecedented data recording efficiency.

Preparation of thin films of the ternary heavy fermion system CeNi 2 Ge 2

Ge2 layers on W(110). In order to produce well-ordered and atomically clean surfaces of the Ce-based intermetallic system the growth was performed under UHV conditions (p<2×10-11 mbar). Both the polycrystalline CeNi2Ge2 compound and the individual elements Ce, Ni, and Ge were used as evaporants. The characterisation of the layers was made with LEED, SEM, and XPS. We find a significant influence of the substrate temperature and the evaporation power on the growth characteristics. The compound material CeNi2Ge2 exhibits complicated behaviour when evaporated. Under carefully selected growth conditions we obtain well-ordered films with a stoichiometry of Ce:Ni:Ge=1:2:2 and a (001) oriented surf…

Investigating surface magnetism by means of photoexcitation electron emission microscopy

The imaging of surfaces by means of photoexcitation electron emission microscopy (PEEM) has recently received considerable interest. This is mainly due to the extended use and availability of brilliant synchrotron radiation in the soft x-ray regime which generally facilitates studies with surface specificity and chemical selectivity. The most popular application of the x-ray PEEM (XPEEM) technique concerns studies of magnetic systems and phenomena. By exploiting the high degree of circular or linear polarization of the synchrotron light, the magnetic microstructure in both ferromagnets and antiferromagnets can be visualized. In this contribution we demonstrate the unique potential and the v…

Clean and ordered surfaces of CeNi 2 Ge 2 layers on W(110)

Investigations of the geometric and electronic properties of ternary Ce-based heavy fermion systems CeT2X2 (T : Ni,Pd,Rh; X : Ge,Si) were carried out by means of electron spectroscopic methods. The main problem for these surface-sensitive techniques is the preparation of well-ordered and atomically clean surfaces. The ternary substance CeNi2Ge2 was grown on a W(110) substrate by MBE with subsequent annealing. A nearly layer-by-layer growth mode was detected using MEED. The annealed layers are ordered, but show small Ni2Ge crystalline islands. The composition was characterised by means of AES in dependence of the substrate as well as the annealing temperature. Electronic properties are inves…

Mapováni spinů povrchových a bulkových Rashba stavů v tenkých vrstvách feroelektrického α-GeTe(111)

Rozbíjení inverzní symetrie ve fereeleRashba efekt; Fotoemisse; DFTktrickém polovodiči způsobuje děleni stavů, tzv Rashba efekt. V tomto článku ukazujeme kompletně mapování spinové polarizace těchto Rashba stavů za pomoci spinovo rozlišené fotoemisse. The breaking of bulk inversion symmetry in ferroelectric semiconductors causes a Rashba-type spin splitting of electronic bulk bands. This is shown by a comprehensive mapping of the spin polarization of the electronic bands in ferroelectric α- GeTe(111) films using a time-of-flight momentum microscope equipped with an imaging spin filter that enables a simultaneous measurement of more than 10 000 data points. The experiment reveals an opposite…

Electronic structure of terpene derivatives

Abstract He I photoelectron spectra of terpene derivatives and their preparative intermediates have been measured. The changes of the ionization potentials are discussed in relation to the corresponding variations of the electronic structure. Especially, the effect of methyl and oxygen substitution has been studied.

Néel Vector Induced Manipulation of Valence States in the Collinear Antiferromagnet Mn 2 Au

The coupling of real and momentum space is utilized to tailor electronic properties of the collinear metallic antiferromagnet Mn2Au by aligning the real space Neel vector indicating the direction o...

Orientation and substrate interaction of adsorbed CO and NO molecules probed by circular dichroism in the angular distribution of photoelectrons.

The sensitivity and utility of circular dichroism in the angular distribution of photoelectrons (CDAD) as a probe of molecular orientation is demonstrated for adsorbed CO and NO molecules. A comparison between measured CDAD spectra and calculated values for spatially oriented CO and NiCO clearly confirms the well-known perpendicular adsorption for CO on Ni(100), whereas for CO adsorbed on Fe(100) a tilted adsorption geometry was found. For NO/Ni(100) and for NO on the oxygen-preadsorbed Ni(100) surface, an average tilt angle of α=40±10° was observed. In the case of the oxygen-preadsorbed Ni(100) surface, a higher fraction of NO molecules was found to be in a tilted orientation than on the c…

NanoESCA: imaging UPS and XPS with high energy resolution

Abstract A novel imaging electron spectrometer has been used for laterally resolved ultraviolet photoelectron spectroscopy (UPS) and X-ray photoelectron spectroscopy (XPS) in the soft X-ray range. The instrument is based on a high-resolution emission microscope optics using a cathode lens and an imaging dispersive analyser. The analyser is corrected for the leading aberration term ( α 2 -term) by means of two hemispherical analysers in antisymmetric configuration with an appropriate transfer lens. Small-area spectra as well as energy-filtered images have been taken in the soft X-ray range for a meteorite sample and in the range of the d-band of a Cu polycrystal. An energy resolution of 106 …

Electron-TOF-analyser for complete momentum analysis in photoemission from surfaces

Abstract We present a new method for momentum-selective imaging by means of a time-of-flight (TOF) technique. The instrument employs a time- and space-resolving delayline detector in combination with a parabolic electrostatic field and a drift space. We use this kind of spectrometer, to raise the efficiency of experiments, which are total momentum resolved. The main difference to conventional photoemission experiments using a rotatable spectrometer is the simultaneous detection of all emitted photoelectrons. In addition to this feature, the angular distribution should be directly visible, to observe solid state symmetries. In order to facilitate these requirements, we use a delayline detect…

Dominance of the first excitation step for magnetic circular dichroism in near-threshold two-photon photoemission

Magnetic circular dichroism (MCD) in near-threshold photoemission is measured for a perpendicularly magnetized Cs/Co/Pt(111) film with work function adjusted by Cs adsorption. For one-photon photoe ...

Temperature-Dependent Change of the Electronic Structure in the Kondo Lattice System $YbRh_{2}Si_{2}$

Seminar, Deutschland; Journal of physics / Condensed matter 00(00), 1-20 (2021). doi:10.1088/1361-648X/abe479

Site-specific atomic order and band structure tailoring in the diluted magnetic semiconductor (In,Ga,Mn)As

Physical review / B 103(7), 075107 (1-13) (2021). doi:10.1103/PhysRevB.103.075107

Formation of an intermolecular charge-transfer compound in UHV codeposited tetramethoxypyrene and tetracyanoquinodimethane

Ultrahigh vacuum (UHV)-deposited films of the mixed phase of tetramethoxypyrene and tetracyanoquinodimethane $({\text{TMP}}_{1}{\text{-TCNQ}}_{1})$ on gold have been studied using ultraviolet photoelectron spectroscopy (UPS), x-ray diffraction (XRD), infrared (IR) spectroscopy, and scanning tunneling spectroscopy (STS). The formation of an intermolecular charge-transfer (CT) compound is evident from the appearance of new reflexes in XRD (${d}_{1}=0.894\text{ }\text{nm}$ and ${d}_{2}=0.677\text{ }\text{nm}$). A softening of the CN stretching vibration (redshift by $7\text{ }{\text{cm}}^{\ensuremath{-}1}$) of TCNQ is visible in the IR spectra, being indicative of a CT on the order of $0.3e$ f…

Magneto-optical linear dichroism in threshold photoemission electron microscopy of polycrystalline Fe films.

Magnetic linear dichroism in threshold photoemission has been exploited to obtain magnetic contrast in a photoemission electron microscope using a mercury arc lamp. The dichroism at threshold can be described similar to the magneto-optical Kerr effect in the region of visible light. The asymmetry of electron intensity observed for a 100 nm polycrystalline Fe film on silicon is A=(0.37+/-0.05)%. The asymmetry occurs for the geometry of the transverse Kerr effect. For unpolarized light the asymmetry was about half the value observed for linearly polarized light. Threshold photoemission microscopy has a large potential for high resolution magnetic domain imaging with fast data acquisition.

Electrical and emission properties of current-carrying silver nanocluster films investigated by emission electron microscopy

Water Influences on the Copper Active Site in Hemocyanin

Active metal sites play a key role in the biochemistry of oxygen transport by hemocyanins. Observing the changes in the local electronic structure of the copper sites upon oxygenation is thus essen...

Charakterisierung von dotierten Heusler-Verbindungen: Co2Cr1−xFexAl

The dependence of circular dichroism in photoemission on the optical properties of Cs monolayers on Pt(111)

We report on the dependence of dichroic photoemission excited by circularly polarised light on the angle of photon incidence. We measured the difference in the angle-resolved photoemission intensities from Cs 5p semi-core levels excited by photons of opposite helicity, which is known as CDAD. We found that the dependence of the measured differences on the angle of light incidence deviates strongly from the model of CDAD for free atoms, as expected. Using the Fresnel equations and a complex index of refraction, one finds that not only the third component but also the second component of the Stokes vector is responsible for the excitation process. Both Stokes components change sign if the ini…

Photoionization of Oriented Systems and Circular Dichroism

Circular dichroism (CD) spectroscopy is a modification of normal absorption spectroscopy using circularly polarized light instead of unpolarized light for determining the difference in the absorption coefficients for right and left circularly polarized light, respectively, in optically active samples. Thus, there is nothing mysterious about CD spectroscopy. However, relative to most other spectroscopic techniques there seems to be a large psychological barrier in its application and at least physicists often regard CD, and optical activity in general, as a rather obscure technique without any useful application. There are some understandable reasons for this attitude, manifesting themselves…

Dirakův kužel a pseudogapped hustota stavů v topologické polovině Heuslerovy sloučeniny YPtBi

Topologické izolátory (Tis) jsou zajímavé materiály, které vykazují nebývalé vlastnosti. . Zde jsme prozkoumali sloučeniny YPtBi jako příklad ze třídy polovu-Heuslerových materiálů. Topological insulators (TIs) are exciting materials, which exhibit unprecedented properties, such as helical spinmomentum locking, which leads to large torques for magnetic switching and highly efficient spin current detection. Here we explore the compound YPtBi, an example from the class of half-Heusler materials, for which the typical band inversion of topological insulators was predicted. We prepared this material as thin films by conventional cosputtering from elementary targets. By in situ time-of-flight mo…

Spin Polarimetry and Magnetic Dichroism on a Buried Magnetic Layer Using Hard X-ray Photoelectron Spectroscopy

The spin-resolved electronic structure of buried magnetic layers is studied by hard X-ray photoelectron spectroscopy (HAXPES) using a spin polarimeter in combination with a high-energy hemispherical electron analyzer at the high-brilliance BL47XU beamline (SPring-8, Japan). Spin-resolved photoelectron spectra are analyzed in comparison with the results of magnetic linear and circular dichroism in photoelectron emission in the case of buried Co2FeAl0.5Si0.5 layers. The relatively large inelastic mean free path (up to 20 nm) of fast photoelectrons enables us to extend the HAXPES technique with electron-spin polarimetry and to develop spin analysis techniques for buried magnetic multilayers a…

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

Journal of physics / Condensed matter 29(25), 255001 - (2017). doi:10.1088/1361-648X/aa7173

Iodine on a magnetized iron film evidence for a magnetic coupling

Abstract Spin-resolved photoelectron spectra of iodine chemisorbed on a magnetized iron (110) surface have been taken using unpolarized VUV light. The partial spin spectra reveal the I 5p x and 5p z signals being split by up to 0.35 eV. This exchange splitting occurs due to hybridization of adsorbate and substrate bands as a consequence of the chemical bond of the halogen atoms to the iron surface.

Compact setup for spin-, time-, and angle-resolved photoemission spectroscopy.

Review of scientific instruments 91(6), 063001 (2020). doi:10.1063/5.0004861

Investigation of Many‐Body Effects in the Quasi‐Two‐Dimensional Electronic System of Organic Charge‐Transfer Salts

Theoretical study of new acceptor and donor molecules based on polycyclic aromatic hydrocarbons

Functionalized polcyclic aromatic hydrocarbons (PAHs) are an interesting class of molecules in which the electronic state of the graphene-like hydrocarbon part is tuned by the functional group. Searching for new types of donor and acceptor molecules, a set of new PAHs has recently been investigated experimentally using ultraviolet photoelectron spectroscopy (UPS). In this work, the electronic structure of the PAHs is studied numerically with the help of B3LYP hybrid density functionals. Using the DELTA-SCF method, electron binding energies have been determined which affirm, specify and complement the UPS data. Symmetry properties of molecular orbitals are analyzed for a categorization and a…

Quantitative spin polarization analysis in photoelectron emission microscopy with an imaging spin filter.

Abstract Using a photoelectron emission microscope (PEEM), we demonstrate spin-resolved electron spectroscopic imaging of ultrathin magnetic Co films grown on Cu(100). The spin-filter, based on the spin-dependent reflection of low energy electrons from a W(100) crystal, is attached to an aberration corrected electrostatic energy analyzer coupled to an electrostatic PEEM column. We present a method for the quantitative measurement of the electron spin polarization at 4×10 3 points of the PEEM image, simultaneously. This approach uses the subsequent acquisition of two images with different scattering energies of the electrons at the W(100) target to directly derive the spin polarization witho…

Field Emission of Electrons Generated by the Near Field of Strongly Coupled Plasmons

Field emission of electrons is generated solely by the ultrastrong near-field of strongly coupled plasmons without the help of a noticeable dc field. Strongly coupled plasmons are excited at Au nanoparticles in subnanometer distance to a Au film by femtosecond laser pulses. Field-emitted electrons from individual nanoparticles are detected by means of photoelectron emission microscopy and spectroscopy. The dependence of total electron yield and kinetic energy on the laser power proves that field emission is the underlying emission process. We derive a dynamic version of the Fowler-Nordheim equation that yields perfect agreement with the experiment.

Hard x-ray photoelectron spectroscopy: a snapshot of the state-of-the-art in 2020

Journal of physics / Condensed matter 33(23), 233001 (1-44) (2021). doi:10.1088/1361-648X/abeacd

Imaging spin filter for electrons based on specular reflection from iridium (001)

Abstract 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 specul…

DICHROISM IN ANGLE-RESOLVED PHOTOEMISSION FROM Pt(111)

The angular dependence of the circular dichroism in photoemission from Pt(111) was investigated for excitation with VUV and soft X-ray radiation. VUV excitation was used to probe band structure and the circular dichroism for valence band emission. The measurements are compared to full relativistic single step photoemission calculations. XPS was used to investigate the circular dichroism in emission from the 4f core level. In this case, the dichroism is induced by photoelectron diffraction. First results from single step core level calculations are compared to the experimental observations.

Photoemission Electron Microscopy as a tool for the investigation of optical near fields

Photoemission electron microscopy was used to image the electrons photoemitted from specially tailored Ag nanoparticles deposited on a Si substrate (with its native oxide SiO$_{x}$). Photoemission was induced by illumination with a Hg UV-lamp (photon energy cutoff $\hbar\omega_{UV}=5.0$ eV, wavelength $\lambda_{UV}=250$ nm) and with a Ti:Sapphire femtosecond laser ($\hbar\omega_{l}=3.1$ eV, $\lambda_{l}=400$ nm, pulse width below 200 fs), respectively. While homogeneous photoelectron emission from the metal is observed upon illumination at energies above the silver plasmon frequency, at lower photon energies the emission is localized at tips of the structure. This is interpreted as a signat…

Time-resolved photoemission electron microscopy of magnetic field and magnetisation changes

Owing to its parallel image acquisition, photoemission electron microscopy is well suited for real-time observation of fast processes on surfaces. Pulsed excitation sources like synchrotron radiation or lasers, fast electric pulsers for the study of magnetic switching, and/or time-resolved detection can be utilised. A standard approach also being used in light optical imaging is stroboscopic illumination of a periodic (or quasi-periodic) process. Using this technique, the time dependence of the magnetic field in a pulsed microstrip line has been imaged in real time exploiting Lorentz-type contrast. Similarly, the corresponding field-induced changes in the magnetisation of cobalt microstruct…

Magnetization changes visualized using photoemission electron microscopy

Abstract Photoemission electron microscopy was used to visualize the motion of magnetic domains on a sub-nanosecond timescale. The technique exploits the imaging of magnetic domains using soft X-ray circular dichroism, with the special feature that the instrument utilizes a fast image acquisition system with intrinsic 125 ps time resolution. The overall time resolution used is about 500 ps. Different domains and domain movements have been observed in lithographically-produced Permalloy structures on a copper microstrip-line. A current pulse of I=0.5 A with rise times of about 300 ps switched the Permalloy islands from a Landau-Lifshitz type domain configuration into metastable s-state domai…

Crystal growth of new charge-transfer salts based on π-conjugated donor molecules

Abstract New charge transfer crystals of π-conjugated, aromatic molecules (phenanthrene and picene) as donors were obtained by physical vapor transport. The melting behavior, optimization of crystal growth and the crystal structure are reported for charge transfer salts with (fluorinated) tetracyanoquinodimethane (TCNQ-Fx, x=0, 2, 4), which was used as acceptor material. The crystal structures were determined by single-crystal X-ray diffraction. Growth conditions for different vapor pressures in closed ampules were applied and the effect of these starting conditions for crystal size and quality is reported. The process of charge transfer was investigated by geometrical analysis of the cryst…

4D texture of circular dichroism in soft-x-ray photoemission from tungsten

Brief treatment and crisis intervention 21(1), 013017 (2019). doi:10.1088/1367-2630/aaf4cd

Beyond the Heisenberg Model: Anisotropic Exchange Interaction between a Cu-Tetraazaporphyrin Monolayer andFe3O4(100)

The exchange coupling of a single spin localized at the central ion of Cu-tetraazaporphyrin on a magnetite(100) surface has been studied using x-ray magnetic circular dichroism (XMCD). Sum rule analysis of the XMCD spectra results in Cu spin and orbital magnetic moments as a function of the applied external field at low temperatures (20 K). The exchange coupling is positive for magnetization direction perpendicular to the surface (ferromagnetic) while it is negative for in-plane magnetization direction (antiferromagnetic). We attribute the anisotropy of the Heisenberg exchange coupling to an orbitally dependent exchange Hamiltonian.

Stroboscopic XMCD-PEEM Imaging

Abstract This article summarizes recent results on magnetization dynamics obtained with time-resolved photoemission electron microscopy (PEEM) using X-ray magnetic circular dichroism as contrast mechanism. Time resolution is performed by a stroboscopic technique that is exclusively sensitive to reversible processes, but offers a very high time resolution only limited by the X-ray pulse width. A time resolution of 20 ps in combination with a lateral resolution of 100 nm has been achieved.

Phase defect inspection of multilayer masks for 13.5 nm optical lithography using PEEM in a standing wave mode

We report on recent developments of an "at wavelength" full-field imaging technique for defect inspection of multilayer mask blanks for extreme ultraviolet lithography (EUVL). Our approach uses photoemission electron microscopy (PEEM) in a near normal incidence mode at 13.5 nut wavelength to image the photoemission induced by the EUV wave field on the multilayer blank surface. We analyze buried defects on Mo/Si multilayer samples down to a lateral size of 50 nm and report on first, results obtained from a six inches mask blank prototype as prerequisite for industrial usage. (c) 2007 Elsevier B.V. All rights reserved.

Narrow-band pulsed electron source based on near-threshold photoionization of Cs in a magneto-optical trap

The newly developed method of time-of-flight (ToF) momentum microscopy was used to analyse the cold electron emission from a Cs 3D magneto-optical trap (MOT). Three-step resonant photoionization was implemented via two intermediate states (6P3/2 pumped with 852 nm laser and 7S1/2 with 1470 nm) and a tuneable femtosecond Ti:sapphire laser for the final ionization step. The magnetic field of the MOT is switched off during the photoionization step. The natural bandwidth of the fs-laser is reduced to 4 meV using optical spectral filters. Precise tuning of the photon energy makes it possible to observe the transition regime between direct photoemission into the open continuum and field induced i…

Time-resolved X-ray photoemission electron microscopy: imaging magnetodynamics on the 100 ps scale and below

Abstract We present recent results of time-resolved X-ray photoemission electron microscopy (TR-XPEEM) investigations on magnetic systems. Our studies of microstructured permalloy particles employ a magnetic pump XPEEM probe approach. The stroboscopic experiments feature a time resolution of Δ τ ≤ 130  ps and yield magnetic domain images with a surprising richness of details. We observe a strong influence of incoherent magnetization rotation processes, which lead to complicated transient domain structures with a blocked relaxation behavior.

Growth and defect studies of CdTe particles

The paper reports the epitaxial growth of cadmium telluride (CdTe) particles by thermal deposition on cleaved planes of (001)NaCl and (001)KBr. Using high resolution transmission electron microscopy and electron diffraction it was shown that CdTe particles could have different orientation and phase (cubic or hexagonal) depending on the substrate temperature. Their most common defects are twins and stacking faults.

Magnetic dichroism in angle-resolved hard x-ray photoemission from buried layers

This work reports the measurement of magnetic dichroism in angular-resolved photoemission from in-plane magnetized buried thin films. The high bulk sensitivity of hard x-ray photoelectron spectroscopy (HAXPES) in combination with circularly polarized radiation enables the investigation of the magnetic properties of buried layers. HAXPES experiments with an excitation energy of 8 keV were performed on exchange-biased magnetic layers covered by thin oxide films. Two types of structures were investigated with the IrMn exchange-biasing layer either above or below the ferromagnetic layer: one with a CoFe layer on top and another with a Co${}_{2}$FeAl layer buried beneath the IrMn layer. A pronou…

Orbital mapping of carbon thin films by XANES-spectromicroscopy

Abstract A laterally resolved micro-XANES study (X-ray absorption near edge structure) of amorphous carbon, hydrogen terminated CVD-diamond (100) and highly oriented pyrolytic graphite (HOPG) is presented. The results were obtained by means of a photoemission electron microscope. Using this technique the well-known spectral features of carbon in its different chemical states (sp 2 , sp 3 ) could be recorded. The sp 2 /sp 3 content of the films was extracted from the spectra. Images, taken at X-ray energies corresponding to maxima (π*, C–H*) of the unoccupied density of states in these spectra, map the lateral distribution of the different orbitals at the sample surface. This study revealed …

Detailed study of defects in thin fullerite films

The structural investigations of fullerite films were performed using high-resolution electron microscopy, electron diffraction and electron energy loss spectroscopy and X-ray photoelectron spectroscopy. In particular defects such as dislocations, stacking faults and twins were studied in details. It was shown that fullerite films could be characterized by a face-centered cubic (f.c.c.) structure with lattice parameter a = 1.416 nm. They are distinguished for their rich polytypic structure that is caused by breaking of alteration of closely packed planes of (111) type. The quantitative method based on information theory using the “run-length encoding” algorithm was suggested to evaluate the…

Determining the optical properties of adsorbate covered surfaces by dichroism in VUV-photoemission

The dichroic effects of photoemission excited by polarised light depend on the angle of photon incidence. Measurements of the difference in the angle-resolved photoemission intensities from Cs 5p semi-corelevels excited by photons of opposite helicity, or of orthogonal linear polarisation are reported. It was thought that the dependence of dichroism on the angle of incidence cannot be described using equations omitting metal optics. A complete consideration of the vector potential of the exciting light is needed, including the phase shift between it's parallel and perpendicular components. The phase shift is produced by the complex index of refraction. Using the Fresnel equations for struct…

Temperature Dependence of Electronic and Magnetic Properties of (DOEO)&lt;sub&gt;4&lt;/sub&gt;[HgBr&lt;sub&gt;4&lt;/sub&gt;]·TCE Single Crystals

The temperature dependence of electronic and magnetic properties of the organic charge-transfer salt (DOEO)4[HgBr4]·TCE was investigated using magnetometry. The magnetic susceptibility shows a maximum at 40 K followed by an onset of a pronounced increase at 70 K and a constant behavior above 120 K. Implications on the charge carrier density are discussed. Combining the magnetometry with resistivity and ESR measurements we propose a sequence of insulating, metallic and semiconducting behavior with increasing temperature. Our results indicate that (DOEO)4[HgBr4]·TCE is close to the boundary between an insulating and conducting ground state.

Fast k-Space Mapping of Electronic Bands Using Time-of-Flight Based Cathode-Lens Microspectroscopy.

Formation of refractory metal nuggets and their link to the history of CAIs

Abstract Ca, Al-rich inclusions (CAIs) often contain numerous refractory metal nuggets (RMNs), consisting of elements like Os, Ir, Mo, Pt and Ru. The nuggets are usually thought to have formed by equilibrium condensation from a gas of solar composition, simultaneously with or prior to oxide and silicate minerals. However, the exact mechanisms responsible for their extremely variable compositions, small sizes and associations with CAI minerals remain puzzling. Expanding on previous work on chemically separated RMNs, we have studied a large number of RMNs within their host CAIs from three different meteorite types, i.e., the highly primitive chondrite Acfer 094 (C2-ungrouped), Allende (CV3 ox…

Multidimensional photoemission spectroscopy—the space-charge limit

New journal of physics 20(3), 033004 - (2018). doi:10.1088/1367-2630/aaa262

k-resolved electronic properties of ternary heavy fermion systems

Stroboscopic XMCD–PEEM imaging of standing and propagating spinwave modes in permalloy thin-film structures

Abstract Using synchrotron-based stroboscopic photoemission electron microscopy with X-ray circular dichroism as contrast method, we have investigated the high-frequency response of permalloy thin-film structures. Standing precessional modes have been studied in rectangular elements (16 × 32 μm 2 , 10 nm thick) with a high time resolution of about 15 ps in the low- α mode of BESSY. With increasing amplitude of the applied magnetic AC field the particle is driven from an initial symmetric Landau flux-closure state into an asymmetric state and finally into a single-domain state magnetized perpendicular to the applied field H AC . The electromagnetic microwave field thus can induces a net magn…

Magnetic Domain Imaging with a Photoemission Microscope

ABSTRACTPhotoelectron emission microscopy (PEEM) has proven to be a versatile analytical technique in surface science. When operated with circularly polarized light in the soft x-ray regime, however, photoemission microscopy offers a unique combination of magnetic and chemical information. Exploiting the high brilliance and circular polarization available at a helical undulator beamline, the lateral resolution in the imaging of magnetic domain structures may be pushed well into the sub-micrometer range. Using a newly designed photoemission microscope we show that under these circumstances not only domains, but also domain walls can be selectively investigated. The high sensitivity of the te…

Sub-nanosecond resolution x-ray magnetic circular dichroism photoemission electron microscopy of magnetization processes in a permalloy ring

Fast magnetization processes in a microstructured permalloy ring with 80 µm o.d. and 30 nm thickness have been observed by photoemission electron microscopy exploiting x-ray magnetic circular dichroism as the magnetic contrast mechanism. As a high speed probe we employed synchrotron radiation pulses at the ESRF (Grenoble) operated in 16-bunch mode, yielding photon pulses of 105 ps FWHM with a period of 176 ns. Fast magnetic field pulses have been generated by means of current pulses through coplanar waveguides with the magnetic structure being lithographically prepared on their surface. A stroboscopic pump–probe set-up with a variable time delay between the field pulse and photon pulse allo…

Nondestructive full-field imaging XANES-PEEM analysis of cosmic grains

For chemical analysis of submicron particles, mass spectrometric methods have the disadvantage of being destructive. Thus, a nondestructive elemental and chemical mapping with a high spatial resolution prior to mass analysis is extremely valuable to precharacterize the sample. Here, first results are presented of combined XANES (x-ray absorption near-edge structure) and PEEM (photoemission electron microscopy) measurements on a cosmic grain fraction from the Murchison meteorite. This nondestructive full-field imaging method is well suited for a quantitative analysis and for a preselection prior to detailed mass spectrometric investigations with isotopic resolution/selectivity. A spectral un…

A spatially resolved investigation of the local, micro-magnetic domain structure of single and polycrystalline Co2FeSi

The Heusler compound Co2FeSi is a promising material for magneto-electronic devices. With a Curie temperature of 1100?K and a saturation magnetization of 6?Bohr magnetons and a high spin polarization at the Fermi edge it fulfils the essential requirements for magnetic sensors or spin valve structures. An essential feature for such devices is the micro-magnetic domain structure. X-ray magnetic circular dichroism?photo emission electron microscopy has been used for a direct observation of the domain structure of single- and polycrystalline samples. The polycrystalline material exhibits a micro-magnetic ripple structure, as it is well known for pure Co and other polycrystalline Heusler compoun…

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 A(-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 dispersi…

Three-dimensional characterization of extreme ultraviolet mask blank defects by interference contrast photoemission electron microscopy

A photoemission electron microscope based on a new contrast mechanism "interference contrast" is applied to characterize extreme ultraviolet lithography mask blank defects. Inspection results show that positioning of interference destructive condition (node of standing wave field) on surface of multilayer in the local region of a phase defect is necessary to obtain best visibility of the defect on mask blank. A comparative experiment reveals superiority of the interference contrast photoemission electron microscope (Extreme UV illumination) over a topographic contrast one (UV illumination with Hg discharge lamp) in detecting extreme ultraviolet mask blank phase defects. A depth-resolved det…

Analysis of Optical Systems, Contrast Depth, and Measurement of Electric and Magnetic Field Distribution on the Object's Surface in Mirror Electron Microscopy

Abstract The contrast depth is analyzed as well, that is the sensitivity of electron mirror microscope to disorders of homogeneity on the object (local magnetic and electric fields, surface relief). Because of the latter ones, electron trajectories feel disturbances (electrons acquire additional increment velocity in radial and azimuthal directions), which leads to the shift of the observed point on the screen and, as a consequence, to the image contrast. Since the electron energy, when reflected, tends to zero, electrons are influenced by heterogeneities for a long time. It causes high sensitivity to heterogeneities, up to the crossing of electron trajectories (caustics are generated). The…

Robustness of plasmonic angular momentum confinement in cross resonant optical antennas

Using a combination of photoemission electron microscopy and numerical simulations, we investigated the angular moment transfer in strongly enhanced optical near-fields of artificially fabricated optical antennas. The polarization dependence of the optical near-field enhancement has been measured in a maximum symmetric geometry, i.e., excitation by a normal incident planar wave. Finite-difference time-domain simulations for the realistic antenna geometries as determined by high-resolution electron microscopy reveal a very good agreement with experimental data. The agreement confirms that the geometrical asymmetries and inhomogeneities due to the nanoscale fabrication process preserve the ci…

The spatial distribution of non-linear effects in multi-photon photoemission from metallic adsorbates on Si(1 1 1)

Multi-photon excitations from thin metallic films on silicon substrates have been observed utilising photoemission electron microscopy. The photoelectrons have been excited by means of high power femtosecond laser pulses with a photon energy below the work function threshold. The strong spatial variations of the non-linear effects became directly visible in electron emission from the adsorbed thin films. Centres of enhanced photoelectron yield, so-called hot spots, were observed on the surfaces of various samples. The multi-photon electron yield of the metallic films (permalloy and lead) depends strongly on the sample topography and the photon polarisation.

Spin-polarized photoelectrons resonantly excited by circularly polarized light from a fractional Ag film on GaAs(100)

We demonstrate a finite spin polarization of photoelectrons emitted from GaAs(100) covered by a fractional Ag film. The photoemission yield shows a sharp maximum for intermediate coverage and the spin polarization increases with increasing laser intensity. Photoelectrons are excited by circularly polarized 100 fs laser pulses of 800 nm wavelength. We recorded the photoemitted electrons using a photoemission electron microscope combined with a Mott spin polarimeter. The spin polarization is analyzed in dependence on the excitation frequency and intensity and on the average thickness of the silver film. The results are explained by a model combining multiphoton photoemission and optical field…

Direct 3D mapping of the Fermi surface and Fermi velocity.

Time-of-flight momentum microscopy is developed. It enables direct three-dimensional mapping of the topology of the Fermi surface, identification of electron and hole pockets, and quantification of Fermi velocity as a function of wavevector.

Defektanalyse von a-C- und CNx-Schichten mittels Röntgen-Photoemissions-Elektronenmikroskopie (X-PEEM)Characterization of stoichiometric defects in diamond, a-C and CNx thin films with Soft X-ray photoelectron microscopy (X-PEEM)

Amorphe Kohlenstoff- und Kohlenstoffnitridschichten werden vielseitig als Schutzschichten in der Industrie verwandt. Insbesondere werden in der Magnetfestplattenspeicherindustrie verschleisfeste sauerstoffundurchlassige Schutzschichten von wenigen Nanometern Dicke benotigt. Rontgen-Photoemissions-Elektronenmikroskopie (X-PEEM) stellt eine Analysetechnik zur Charakterisierung u.a. von Kohlenstoffschutzschichten dar, da sich Informationen uber die lokale Bindungsumgebung aus der Rontgenabsorptions-Nahkantenstruktur (XANES) gewinnen lassen. CVD-DLC- sowie a-C- und CNx-Schichten wurden analysiert. Fur die a-C-Schichten auf Si (100) wurde der Anteil sp2-hybridisierter Atome bestimmt und mit den …

Magnetic dichroism in photoemission with unpolarized light.

A magnetic dichroism in photoemission from ferromagnets induced by unpolarized light is observed for the first time in the valence band region as well as for surface states. The study was carried out with magnetized Fe(110), Co(0001), and Gd(0001) films grown epitaxially on W(110). This phenomenon leads to an intensity asymmetry for opposite directions of the sample magnetization. It can be easily used for a routine laboratory diagnostic of magnetic behavior. A simple theoretical interpretation of the phenomenon based on the atomic model is given.

Linear Dichroism in Photoemission from Oriented Molecules

It is shown that oriented molecules reveal both Linear Dichroism (LD) and Linear Dichroism in the Angular Distribution (LDAD) of photoelectrons, which means a difference between photoelectron currents ejected at a definite angle by linearly polarized light of two mutually perpendicular polarizations. Measurements of LD and LDAD enable one to investigate the orientation of molecules and to make an essential step towards the complete quantummechanical experiment. As an example, LDAD in a model case of oriented heteronuclear diatomic molecules is presented.

Accessing fast magnetization dynamics by XPEEM: Status and perspectives

Abstract Being already well established as a versatile technique for high-resolution static magnetic domain imaging, X-ray photoemission electron microscopy (XPEEM) is now also capturing the field of time-resolved magnetic investigations. Using appropriate operation modes at synchrotron radiation sources, a time resolution of 10 ps and less can be achieved in recent magnetodynamics studies, giving access even to phenomena involving precessional processes.

Spin-polarization effects for electrons passing through thin iron and cobalt films

Abstract Spin-dependent effects of the inelastic mean free path (IMFP) are evident for low-energy electrons passing through magnetized ferromagnetic films caused by a different attenuation within the layer. Values of IMFP for both spin components were determined for ultrathin iron and cobalt layers on W(1 1 0) by means of spin-resolving photoelectron spectroscopy.

Spin polarisation and dichroism in ARUPS from thin rare earth films

Abstract In the present study, spin polarisation and dichroism were investigated in angular resolved VUV photoemission ARUPS from magnetised as well as paramagnetic rare earth surfaces. Thin Gd(0001) films were prepared epitaxially on W(110). The photoelectrons were excited by polarised synchrotron radiation from the BESSY I synchrotron radiation source. A SPLEED detector attached to an electron spectrometer mounted on a single axis goniometer was used for angular resolved spin analysis. The main part of this work focused on the characteristic surface state of Gd(0001) which shows a splitting, as previously observed by linear magnetic dichroism and spin polarised photoemission. The spin ana…

Detekcia vektora spinovej polarizácie vo viackanálovej spinovo rozlýšenej fotoemissie za použitia spinového filtra založeného na Ir(001)

Physical review / B 95(10), 104423 (2017). doi:10.1103/PhysRevB.95.104423

Enhanced orbital magnetic moments in the Heusler compounds ,,

Abstract Using the magnetic circular dichroism in X-ray absorption at the L2,3-edges of the 3d-transition metals, we determined the element specific ratio between orbital and spin magnetic moment of the Heusler compounds Co 2 CrAl , Co 2 Cr 0.6 Fe 0.4 Al and Co2FeAl. The orbital magnetic moment per spin is large (0.1–0.2) compared to bulk values of Fe and Co metals.

Time- and energy resolved photoemission electron microscopy-imaging of photoelectron time-of-flight analysis by means of pulsed excitations

Abstract The present work enlightens the developments in time- and energy resolved photoemission electron microscopy over the past few years. We describe basic principles of the technique and demonstrate different applications. An energy- and time-filtering photoemission electron microscopy (PEEM) for real-time spectroscopic imaging can be realized either by a retarding field or hemispherical energy analyzer or by using time-of-flight optics with a delay line detector. The latter method has the advantage of no data loss at all as all randomly incoming particles are measured not only by position but also by time. This is of particular interest for pump–probe experiments in the femtosecond an…

MAGNETIC COUPLING OF ALKALI AND RARE-GAS FILMS ADSORBED ON A FERROMAGNETIC SURFACE

The observation of magnetic circular dichroism in the angular distribution of photoelectrons (MCDAD) from alkali and rare-gas films adsorbed on a thin remanently magnetized Co layer is reported. The observation of an antisymmetric MCDAD near normal emission for Co(0001)–Cs 5p semi core level is shown. The reversed magnetization leads to a mirror-image-like distribution. The second system under investigation, physisorbed Co(0001)–Xe 5p, does not give such an but shows significant differences in the MCDAD signal for both directions of magnetization, in particular in the |mj| substates of the p3/2 level. A magnetic coupling between Xe and Co is evident when we take results of spin-resolved ph…

Trace element analysis in pre-solar stardust grains via full-field imaging XPS (Nano-ESCA)

An acid-resistant, SiC-rich, residue from the Murchison meteorite was investigated by means of a novel imaging XPS instrument. The micrometer-sized grains were deposited on a Si wafer from an aqueous suspension. Energy filtered ESCA images have been taken in the kinetic energy range from the threshold up to about 400 eV for various photon energies. A lateral resolution of the order of 120 nm along with a high energy resolution in the range of 100 meV provides the basis for chemical trace element analysis with maximum sensitivity. Apart from major (Si, C) and minor (N, Mg, Al, Fe) elements, the energy filtered images and local microspectra revealed the presence of a variety of heavy trace el…

Extraction dynamics of electrons from magneto-optically trapped atoms

Pulsed photoionization of laser-cooled atoms in a magneto-optical trap (MOT) has the potential to create cold electron beams of few meV bandwidths and few ps pulse lengths. Such a source would be highly attractive for the study of fast low-energy processes like coherent phonon excitation. To study the suitability of MOT-based sources for the production of simultaneously cold and fast electrons, we study the photoionization dynamics of trapped Cs atoms. A momentum-microscope-like setup with a delay-line detector allows for the simultaneous measurement of spatial and temporal electron distributions. The measured patterns are complex, due to the Lorentz force inducing spiral trajectories. Ray-…

Image enhancement in photoemission electron microscopy by means of imaging time-of-flight analysis

Abstract Photoemission electron microscopy (PEEM) is widely used in combination with synchrotron sources as a powerful tool to observe chemical and magnetic properties of metal and semiconductor surfaces. Presently, the resolution limit of these instruments using soft-X-ray excitation is limited to about 50 nm, because of the chromatic aberation of the electron optics used. Various sophisticated approaches have thus been reported for enhancing the spatial resolution in photoemission electron microscopy. This work demonstrates the use of a simple imaging energy filter based on electron time-of-flight (ToF) selection. The spatial resolution could be improved dramatically, even though the inst…

Electron-spectroscopic investigations on ternary HFS: CeT2X2

Investigations of the electronic properties were carried out for ternary Ce-based heavy fermion systems. The well-ordered surfaces of HFS were prepared by MBE on W (110) with subsequent annealing. The layers are characterised by MEED, LEED, AES and XPS. For the electron-spectroscopic investigations, ARUPS and SPEELS were used. In the photoemission spectra, dispersion effects could be detected. By means of SPEELS, the dipole-forbidden Ce f-f transitions could be observed. The comparison of the energy loss spectra above and below the characteristic temperature T∗ reveals differences in the energy losses as well as in the asymmetries.

Microspectroscopy and spectromicroscopy with photoemission electron microscopy using a new kind of imaging energy filter

The use of an imaging retarding field analyser attached to the FOCUS IS-PEEM is described. This kind of energy filter is a simple, powerful tool to obtain microspectra from areas of down to about 1 μm using (V)UV and X-ray excitation sources. First results of microspectroscopy measured by excitation with a laboratory as well as a synchrotron X-ray source are presented.

Peculiarities of imaging one- and two-dimensional structures in an emission electron microscope. 1. theory

Local changes in work function cause deviations of the electrical microfield near a sample surface as a result of the uniform accelerating field distribution between the sample (cathode) and the extractor electrode (anode). This results in a change in the electron trajectories. As a consequence, the microscope image shows remarkable changes in position, size, intensity and lateral resolution of distinct details, which can be quantitatively described by the calculations presented here. Analysing these effects in the image gives an opportunity to determine the real lateral size of the observed structures and the distribution of local contact potentials.

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.

High-resolution hard-x-ray photoelectron diffraction in a momentum microscope—the model case of graphite

New journal of physics 21(11), 113031 - (2019). doi:10.1088/1367-2630/ab51fe

Emission Electron Microscopy of Nanoparticles in Strong fs Laser Fields

Heusler compounds as ternary intermetallic nanoparticles: Co2FeGa

This work describes the preparation of ternary nanoparticles based on the Heusler compound Co2FeGa. Nanoparticles with sizes of about 20?nm were synthesized by reducing a methanol impregnated mixture of CoCl2 ? 6H2O, Fe(NO3)3 ? 9H2O and Ga(NO3)3 ? xH2O after loading on fumed silica. The dried samples were heated under pure H2 gas at 900??C. The obtained nanoparticles?embedded in silica?were investigated by means of x-ray diffraction (XRD), transmission electron microscopy, temperature dependent magnetometry and M??bauer spectroscopy. All methods clearly revealed the Heusler-type L21 structure of the nanoparticles. In particular, anomalous XRD data demonstrate the correct composition in addi…

Investigation of a Ge nanoparticle film by means of electron stimulated photon emission spectroscopy

Abstract Electron stimulated photon emission spectroscopy was used for the study of the electronic structure of Ge nanoparticles. A nanoparticle film was prepared by thermal deposition on a quartz substrate. Photon emission was stimulated by electron bombardment at energies of several hundred electron volts. Electron field emission from a W-tip was used at tip voltage U t  = 100–600 eV. A spectrometer in combination with a liquid nitrogen cooled charge-coupled device (CCD) camera was used for light detection. Light emission spectra were measured in the energy range 1.18–4.2 eV. They are characterized by features at ∼1.6 and ∼3.1 eV. A comparison with light emission spectra obtained with ano…

Adsorbates on thin iron(100) films

The electronic and magnetic properties of different kinds of adsorbates on thin magnetized Fe(100) films have been investigated by means of spin resolving photoelectron spectroscopy. The study has been carried out with atomically physisorbed xenon, the molecule carbon monoxide, and metallic gold. The spin splitting of the Xe 5p signal can be explained by magnetic interactions with the final ionic hole state. By spin analysis, it could be shown that at room temperature for low exposures the adsorption of CO is dissociative and with increasing exposure additionally molecular. The Au related features for the monolayer show different line shapes in both spin channels but no splittings due to an…

Dichroism in VUV photoemission from the (0001)-surfaces of ultrathin Gd and Nd films on W(110)

Abstract Ultrathin layers of Gd and Nd epitaxially grown on W(110) have been investigated using linearly and circularly polarised light at the 6.5 m NIM beamline at the BESSY storage ring in Berlin. The high quality of the films was monitored by the sharp and dispersionless surface state just below the Fermi energy. The CDAD (circular dichroism in the angular distribution of photoelectrons) measurements showed strong effects in the surface states as well as in the valence bands. The LMDAD (linear magnetic dichroism in…) from Gd(0001) showed a small, but significant splitting of the surface state. This splitting can be reproduced by numerical one-step calculations based on spin-dependent sur…

Electronic structure of adsorbed organic molecules

We report on investigations of chiral organic molecules in the gas phase and physisorbed on graphite. The measurements were carried out by means of angle-resolving VUV photoelectron spectroscopy. The emission from specific orbitals in oriented molecules can be forbidden because of dipole selection rules. Due to the lack of certain features in the spectra, it was possible to determine the adsorption geometry of cyclohexanone and camphor as being with their ring system parallel to the surface. By comparison of gas-phase and adsorbate spectra of ethyl benzene derivatives, adsorption could be proved to be molecular without decomposition. For amino acids on graphite, the occurrence of characteri…

Emitter-site specificity of hard x-ray photoelectron Kikuchi-diffraction

New journal of physics 22(10), 103002 (1-13) (2020). doi:10.1088/1367-2630/abb68b

High-pass energy-filtered photoemission electron microscopy imaging of dopants in silicon.

Differently doped areas in silicon can show strong electron-optical contrast in dependence on the dopant concentration and surface conditions. Photoemission electron microscopy is a powerful surface-sensitive technique suitable for fast imaging of doping-induced contrast in semiconductors. We report on the observation of Si (100) samples with n- and p-type doped patterns (with the dopant concentration varied from 10(16) to 10(19) cm(-3)) on a p- and n-type substrate (doped to 10(15) cm(-3)), respectively. A high-pass energy filter of the entire image enabled us to obtain spectroscopic information, i.e. quantified photo threshold and related photoyield differences depending on the doping lev…

Test of band structure calculations for Heusler compounds by spin-resolved photoemission spectroscopy

The electronic density of states of epitaxial thin films of the Heusler compound Co${}_{2}$MnGa is probed in situ by spin-resolved ultraviolet photoemission spectroscopy. The experiments reveal several characteristic features in the intensity spectrum and a clear Fermi edge signature. A high spin polarization of $\ensuremath{\simeq}\phantom{\rule{-0.16em}{0ex}}55%$ at the Fermi edge is followed by a sign change at the binding energy of $\ensuremath{\simeq}$0.8 eV. Corresponding calculations of the band structure and the photoemission spectrum were performed employing a spin-polarized relativistic Korringa-Kohn-Rostoker code. Good agreement between the experimental data and calculations was …

Size dependence of magnetic domain patterns in exchange-biased Permalloy/NiO microstructures

The magnetic domain structure in Permalloy (Ni81Fe19) micropatterns (10?100??m) on NiO has been investigated by means of soft x-ray photoemission electron microscopy. The exchange anisotropy between the Ni81Fe19 patterns and the NiO layer results in the formation of complex domain structures which markedly differ from the simple Landau?Lifshitz configurations. The domain structures reflect the competition between the exchange anisotropy and the dipole?dipole interaction in a weakly coupled system. The observed domain structures change with the feature size, as the domain patterns lose complexity in the smaller structures.

Time-resolved photoemission electron microscopy

The excellent time structure of Synchrotron radiation and short-pulse lasers has opened the door to a novel way of time-resolved imaging using PEEM. Periodic or repetitive processes can be studied by stroboscopic illumination with the pulsed photon beam. Since the first experiments in 2003, two fields of applications have been established in several groups. One concerns the investigation of fast magnetisation processes like precessional switching, Gigahertz-eigenmodes of ferromagnetic nanostructures or travelling spin waves in thin films. More recently, femtosecond lasers have been used for imaging of localised surface plasmons in nanoparticles and their temporal behaviour in the femtosecon…

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

Journal of synchrotron radiation 28(6), 1891 - 1908 (2021). doi:10.1107/S1600577521010511

Periodic unmixing of a binary metallic vapor

We report on a type of surface structuring after short pulse laser ablation of a binary alloy. We observe the emergence of a concentric ring structure with changing elemental composition. The composition changes are interpreted by condensation of the ambient ablation vapor due to stress wave excitations in the ablation spot.

Correlation in the transition-metal-based Heusler compoundsCo2MnSiandCo2FeSi

Half-metallic ferromagnets, such as the Heusler compounds with formula ${X}_{2}YZ$, are expected to show an integer value for the spin magnetic moment. In contrast to experiments, calculations give noninteger values in certain cases where the compounds are based on $X=\mathrm{Co}$. In order to explain deviations of the magnetic moment calculated for such compounds, the dependence of the electronic structure on the lattice parameter was studied theoretically. In the local density approximation (LDA), the minimum total energy of ${\mathrm{Co}}_{2}\mathrm{FeSi}$ is found for the experimental lattice parameter, but the calculated magnetic moment is approximately 12% too low. In addition, half-m…

Near Field of Strongly Coupled Plasmons: Uncovering Dark Modes

Strongly coupled plasmons in a system of individual gold nanoparticles placed at subnanometer distance to a gold film (nanoparticle-on-plane, NPOP) are investigated using two complementary single particle spectroscopy techniques. Optical scattering spectroscopy exclusively detects plasmon modes that couple to the far field via their dipole moment (bright modes). By using photoemission electron microscopy (PEEM), we detect in the identical NPOPs near-field modes that do not couple to the scattered far field (dark modes) and are characterized by a strongly enhanced nonlinear electron emission process. To our knowledge, this is the first time that both far- and near-field spectroscopy are carr…

Statistical mechanics of fullerene coalescence growth

Among the different carbon allotropes fullerenes are exceptionally intriguing for their spheroidal topology out of pentagons and hexagons. However, the dominant formation mode is still ambiguous. Here, we analyze the fullerene formation process by the statistical analysis of fullerene sizes produced in a laser-induced microplasma finding that a simple two-parameter lognormal distribution describes impressively well the cluster frequencies under various conditions. Our findings clearly reveal coalescent growth following a classical collision dynamics and disagree with several earlier assumptions.

Multipole WIEN-filter for a high-resolution X-PEEM

Abstract The development and construction of an X-PEEM with integral multipole WIEN-filter for spectromicroscopy with high lateral resolution is presented. All relevant electron-optical properties of the filter have been examined by field and trajectory calculations. Electric and magnetic multipole components (dipole, quadrupole and hexapole) can be chosen independently from each other, thus allowing electron-optical corrections. Theoretical values for the lateral resolution are in the range of 10 nm, experimental values of ≤25 nm have been achieved using the column without filter. The instrument is designed in particular for the use of Sychrotron radiation as well as new, high-brilliance l…

Circular dichroism in X-ray photoemission from Pd(111) and CO/Pd(111)

It is shown experimentally that in the soft X-ray region a large circular dichroism in the photoelectron angular distribution (CDAD) exists for both valence orbitals and core levels of CO molecules adsorbed on Pd(111). From theoretical consideration it follows that in the case of a spherically symmetric ground state wave function, like the 1σ and 2σ orbitals of CO, CDAD appears due to the lack of spherical symmetry in the final state. For carbonK-shell experimental results are compared to model calculations. Investigations at the Pd core levels proved that CDAD does also arise in X-ray photo-emission from non-magnetic crystals.

Ferromagnetism at the summit: A perspective on: “Spin polarized field emission from Fe and co-coated W tips” by Y.R. Niu and M.S. Altman

PEEM with high time resolution—imaging of transient processes and novel concepts of chromatic and spherical aberration correction

The potential of time-resolved photoemission electron microscopy (PEEM) for imaging ultrafast processes and for aberration correction in full-field imaging is discussed. In particular, we focus on stroboscopic imaging of precessional magnetic excitations via XMCD-PEEM exploiting the time structure of synchrotron radiation (magnetic field pulse pump–X-ray probe). In a special bunch-compression mode at BESSY, a time resolution of about 15 ps has been obtained. Further, we discuss an all-optical pump–probe technique using femtosecond laser excitation. A highly promising alternative to stroboscopic imaging is an approach using time-resolved image detection. As a second application of time-resol…

Composition and clues to the origin of refractory metal nuggets extracted from chondritic meteorites

Refractory metal nuggets (RMNs) contain elements, such as Os, Ir, Mo, and Ru, which are predicted to condense from a cooling gas of solar composition simultaneously with CAI-minerals. Berg et al. (2009) identified a large number of RMNs in acid-resistant residues of the Murchison meteorite and suggested that they are pristine condensates. In extending the work of these authors, we have improved the chemical extraction process to enrich the concentration of RMNs in the residue sample and prepared three additional RMN-rich residues from the chondritic meteorites Murchison, Allende, and Leoville. The results show that, while their origin is clearly solar, the compositions in detail of RMNs fro…

Development of hard x-ray photoelectron SPLEED-based spectrometer applicable for probing of buried magnetic layer valence states

Abstract A novel design of high-voltage compatible polarimeter for spin-resolved hard X-ray photoelectron spectroscopy (Spin-HAXPES) went into operation at beamline BL09XU of SPring-8 in Hyogo, Japan. The detector is based on the well-established principle of electron diffraction from a W(001) single-crystal at a scattering energy of 103.5 eV. It's special feature is that it can be operated at a high negative bias potential up to 10 kV, necessary to access the HAXPES range. The polarimeter is operated behind a large hemispherical analyzer (Scienta R-4000). It was optimized for high transmission of the transfer optics. A delay-line detector (20 mm dia.) is positioned at the exit plane of the…

CCDC 1448360: Experimental Crystal Structure Determination

Related Article: Antonia Morherr, Sebastian Witt, Alisa Chernenkaya, Jan-Peter Bäcker, Gerd Schönhense, Michael Bolte, Cornelius Krellner|2016|Physica B: Condensed Matter(Amsterdam)|496|98|doi:10.1016/j.physb.2016.05.023

CCDC 1448362: Experimental Crystal Structure Determination

Related Article: Antonia Morherr, Sebastian Witt, Alisa Chernenkaya, Jan-Peter Bäcker, Gerd Schönhense, Michael Bolte, Cornelius Krellner|2016|Physica B: Condensed Matter(Amsterdam)|496|98|doi:10.1016/j.physb.2016.05.023

CCDC 1448363: Experimental Crystal Structure Determination

Related Article: Antonia Morherr, Sebastian Witt, Alisa Chernenkaya, Jan-Peter Bäcker, Gerd Schönhense, Michael Bolte, Cornelius Krellner|2016|Physica B: Condensed Matter(Amsterdam)|496|98|doi:10.1016/j.physb.2016.05.023

CCDC 1448361: Experimental Crystal Structure Determination

Related Article: Antonia Morherr, Sebastian Witt, Alisa Chernenkaya, Jan-Peter Bäcker, Gerd Schönhense, Michael Bolte, Cornelius Krellner|2016|Physica B: Condensed Matter(Amsterdam)|496|98|doi:10.1016/j.physb.2016.05.023