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…

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…

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

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…

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…

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…

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…

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…

Photoelectron-holography using circularly polarized light

Abstract Circular dichroism in the angular distribution of photoelectrons (CDAD) is not only observed from aligned initial states, but also as a consequence of the scattering of photoelectrons at the surrounding atoms in a solid or an adsorbate. Using the analytical result for the CDAD, we show that it is an integral transformation of the product of the angular momentum of the emitted electron and the Fourier-transformed scattering potential of the surrounding atoms. Therefore, we interpret the CDAD pattern as photoelectron-hologram. The real space distribution of atoms can be reconstructed by an inverse integral transformation of the CDAD pattern, which carries the full phase-information. …

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…

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…

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…

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 …

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…

Development of a scanning electron microscopy with polarization analysis system for magnetic imaging with ns time resolution and phase-sensitive detection.

Scanning electron microscopy with polarization analysis is a powerful lab-based magnetic imaging technique offering simultaneous imaging of multiple magnetization components and a very high spatial resolution. However, one drawback of the technique is the long required acquisition time resulting from the low inherent efficiency of spin detection, which has limited the applicability of the technique to certain quasi-static measurement schemes and materials with high magnetic contrast. Here we demonstrate the ability to improve the signal-to-noise ratio for particular classes of measurements involving periodic excitation of the magnetic structure via the implementation of a digital phase-sens…

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…

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…

Actinic EUVL mask blank defect inspection by EUV photoelectron microscopy

A new method for the actinic at-wavelength inspection of defects inside and ontop of Extreme Ultraviolet Lithography (EUVL) multilayer-coated mask blanks is presented. The experimental technique is based on PhotoElectron Emission Microscopy (PEEM) supported by the generation of a standing wave field inside and above the multilayer mask blank when illuminated near the resonance Bragg wavelength at around 13.5 nm wavelength. Experimental results on programmed defect samples based on e-beam lithographic structures or PSL equivalent silica balls overcoated with an EUV multilayer show that buried defects scaling down to 50 nm in lateral size are detectable with further scalability down to 30 nm …

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.

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…

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

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.

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.

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…

The dependence of dichroism in VUV-photoemission on the optical properties of adsorbates: Cs-monolayer on W(110)

Abstract We report on the dependence of dichroic photoemission excited by polarised light on the angle of photon incidence. We measured the difference in the angle-resolved photoemission intensities from Cs-5p semi-corelevels excited by photons of opposite helicity, known as CDAD and of orthogonal linear polarisation—LDAD. We found that the dependence of dichroism on the angle of incidence can not be described by the equations used in the photoemission model for free atomic states. A complex consideration of the parallel and perpendicular components of the vector potential of the exciting light is needed, including the phase shift between these components. The phase shift is produced by the…

Multidimensional photoemission spectroscopy—the space-charge limit

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

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…

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…

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.

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 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…

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…

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…

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.

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.

Emission Electron Microscopy of Nanoparticles in Strong fs Laser Fields

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…

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-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.