Alkali antimonides are well established as high efficiency, low intrinsic emittance photocathodes for accelerators and photon detectors. However, conventionally grown alkali antimonide films are polycrystalline with surface disorder and roughness that can limit achievable beam brightness. Ordering the crystalline structure of alkali antimonides has the potential to deliver higher brightness electron beams by reducing surface disorder and enabling the engineering of material properties at the level of atomic layers. In this report, we demonstrate the growth of ordered Cs3Sb films on single crystal substrates 3C-SiC and graphene-coated 4H-SiC using pulsed laser deposition and conventional thermal evaporation growth techniques. The crystalline structures of the Cs3Sb films were examined using reflection high energy electron diffraction and x-ray diffraction diagnostics, while film thickness and roughness estimates were made using x-ray reflectivity. With these tools, we observed ordered domains in less than 10 nm thick films with quantum efficiencies greater than 1% at 530 nm. Moreover, we identify structural features such as Laue oscillations indicative of highly ordered films. We found that Cs3Sb films grew with flat, fiber-textured surfaces on 3C-SiC and with multiple ordered domains and sub-nanometer surface roughness on graphene-coated 4H-SiC under our growth conditions. We identify the crystallographic orientations of Cs3Sb grown on graphene-coated 4H-SiC substrates and discuss the significance of examining the crystal structure of these films for growing epitaxial heterostructures in future experiments.

Van der Waals heterostacks can exhibit emergent properties as a result of the coupling between the individual layers stacked. Here we focus on heterostacks of graphene and hBN, and study both coherent electron resonances (or unoccupied states) and inelastic losses. For this, we measure electron reflection and transmission spectra of the stack, as a function of electron energy. Special attention is paid to the symmetry upon flipping the heterostack, i.e., whether the electrons are first incident on the graphene or on the hBN surface: whereas electron reflection may be sensitive to sample orientation, electron transmission should not. Experimentally, we compare LEEM (reflection) and eV-TEM (transmission) IV spectra measured on free-standing graphene-hBN heterostacks with either the graphene or hBN side facing the LEEM objective lens. Resonances and inelastic loss are first modeled with the help of a simple wave interference toy model inspired by optics. More advanced calculations are performed to obtain the spatially resolved density of unoccupied states in the heterostack. We relate these calculations to the measured spectra, taking into account the finite probing depth of the reflected electron beam.

The development of high-brightness electron sources is critical to state-of-the-art electron accelerator applications like X-ray free electron laser (XFEL) and ultra-fast electron microscopy. Cesium telluride is chosen as the electron source material for multiple cutting-edge XFEL facilities worldwide. This manuscript presents the first demonstration of the growth of highly crystalized and epitaxial cesium telluride thin films on 4H-SiC and graphene/4H-SiC substrates with ultrasmooth film surfaces. The ordering of the film was characterized by in situ reflection high energy electron diffraction and multiple X-ray diagnostics. The results of the quantum efficiency performance for epitaxial cesium telluride photocathodes are also reported.

Ultra-flat, ultra-thin alkali antimonide photocathodes with high crystallinity can exhibit high quantum efficiency and low mean transverse energy of outgoing electrons, which are essential requirements for a variety of applications for photocathode materials. Here, we investigate the growth of Cs3Sb on graphene-coated 4H–SiC (Gr/4H–SiC), 3C–SiC, and Si3N4 substrates. Sb is deposited using pulsed laser deposition, while Cs is deposited thermally and simultaneously. We demonstrate, employing x-ray analysis and quantum efficiency measurements, that this growth method yields atomically smooth Cs3Sb photocathodes with a high quantum efficiency (>10%), even in the ultra-thin limit (<30 nm). For the Si3N4 substrate, film growth is shown to be polycrystalline, while films grown on Gr/4H–SiC show a high degree of ordering with signs of epitaxy.

1 Abstract Detailing the physical basis of neural circuits with large-volume serial electron microscopy (EM), ‘connectomics’, has emerged as an invaluable tool in the neuroscience armamentarium. However, imaging synaptic resolution connectomes is currently limited to either transmission electron microscopy (TEM) or scanning electron microscopy (SEM). Here, we describe a third way, using photoemission electron microscopy (PEEM) which illuminates ultra-thin brain slices collected on solid substrates with UV light and images the photoelectron emission pattern with a wide-field electron microscope. PEEM works with existing sample preparations for EM and routinely provides sufficient resolution and contrast to reveal myelinated axons, somata, dendrites, and sub-cellular organelles. Under optimized conditions, PEEM provides synaptic resolution; and simulation and experiments show that PEEM can be transformatively fast, at Gigahertz pixel rates. We conclude that PEEM imaging leverages attractive aspects of SEM and TEM, namely reliable sample collection on robust substrates combined with fast wide-field imaging, and could enable faster data acquisition for next-generation circuit mapping.

Energy-Dispersive X-Ray Spectroscopy (EDS) is a technique frequently used in Scanning and Transmission Electron Microscopes to study the elemental composition of a sample. Briefly, high energy electrons of the incident electron beam may ionize an electron from a core shell. The decay of this excited state may result in the emission of a characteristic X-ray photon or Auger-Meitner electron. A solid-state EDS detector captures the X-ray photon and determines its energy. The energy spectrum thus contains information on the elemental make-up of the sample. Low Energy Electron Microscopy (LEEM) typically utilizes incident electrons with energies in the range 0-100 eV, insufficient for the generation of elemental X-rays. In general, LEEM does therefore not allow for elemental characterization of the sample under study. Here we show how relatively simple modifications and additions to the LEEM instrument make in-situ EDS spectroscopy possible, and how high-quality EDS spectra can be obtained, thus enabling elemental analysis in LEEM instruments for the first time.

Electron states above the vacuum level are known to play an important role in secondary electron processes, such as photoelectron emission and secondary electron emission where they act as ``final'' (or better ``intermediate'') states from which an electron is emitted to the vacuum. However, despite their relevance, these states are typically not well known, nor independently investigated, mostly due to a lack of proper spectroscopic techniques. Here, we present a spectroscopy study on crystalline pentacene, used as a model system to investigate the influence of these states on secondary electron processes. Using low-energy electron (LEE) spectroscopy, we first gauge the spectrum of such states in few-monolayer pentacene films. We, subsequently, relate these states to photoelectron and secondary electron emission. Specifically, photoemission experiments (Hg lamp) show a decrease in intensity with each additional pentacene layer grown. Given an absence of increase in the ionization energy or change in the crystal structure with increasing layer count, we relate the decrease in photoemission intensity to the emergence of a band gap just above the vacuum level as observed in LEE reflectivity spectra. Second, we study the energy distribution of secondary electrons. We use electron-beam damage to cause controlled changes in the band structure, and find a clear correlation between the evolution of the LEE spectra and the distribution of secondary electrons.

Terrace-sized, single-orientation graphene can be grown on top of a carbon buffer layer on silicon carbide by thermal decomposition. Despite its homogeneous appearance, a surprisingly large variation in electron transport properties is observed. Here, we employ Aberration-Corrected Low-Energy Electron Microscopy (AC-LEEM) to study a possible cause of this variability. We characterize the morphology of stacking domains between the graphene and the buffer layer of high-quality samples. Similar to the case of twisted bilayer graphene, the lattice mismatch between the graphene layer and the buffer layer at the growth temperature causes a moir\'e pattern with domain boundaries between AB and BA stackings. We analyze this moir\'e pattern to characterize the relative strain and to count the number of edge dislocations. Furthermore, we show that epitaxial graphene on silicon carbide is close to a phase transition, causing intrinsic disorder in the form of co-existence of anisotropic stripe domains and isotropic trigonal domains. Using adaptive geometric phase analysis, we determine the precise relative strain variation caused by these domains. We observe that the step edges of the SiC substrate influence the orientation of the domains and we discuss which aspects of the growth process influence these effects by comparing samples from different sources.

Stacking domain boundaries occur in Van der Waals heterostacks whenever there is a twist angle or lattice mismatch between subsequent layers. Not only can these domain boundaries host topological edge states, imaging them has been instrumental to determine local variations in twisted bilayer graphene. Here, we analyse the mechanisms causing stacking domain boundary contrast in Bright Field Low-Energy Electron Microscopy (BF-LEEM) for both graphene on SiC, where domain boundaries are caused by strain and for twisted few layer graphene. We show that when domain boundaries are between the top two graphene layers, BF-LEEM contrast is observed due to amplitude contrast and corresponds well to calculations of the contrast based purely on the local stacking in the domain boundary. Conversely, for deeper-lying domain boundaries, amplitude contrast only provides a weak distinction between the inequivalent stackings in the domains themselves. However, for small domains phase contrast, where electrons from different parts of the unit cell interfere causes a very strong contrast. We derive a general rule-of-thumb of expected BF-LEEM contrast for domain boundaries in Van der Waals materials.

In van der Waals (vdW) materials, the electron mean free path (MFP) is largely influenced by the discrete states in the unoccupied band structure. So far, the influence of these states has only been measured in graphene, while all measurements on other vdW materials lack energy resolution. Here, we present reflection and transmission spectra of freestanding, few-layered molybdenum disulfide (MoS2) samples in the 0-55 eV electron range. Our measurements reveal states of enhanced electron transmissivity above the vacuum level, that correspond to the (unoccupied) density of states. We also show a full quantum-mechanical calculation that confirms a good understanding of the elastic scattering in MoS2. A model is developed to extract the inelastic MFP spectrum, which is a measure of the inelastic scattering cross section. As MoS2 is a complicated system of different atomic planes, we expect that our methods generalize well to other van der Waals materials and heterostacks thereof.

A new, complementary technique based on Photo Emission Electron Microscopy (PEEM) is demonstrated. In contrast to PEEM, the sample is placed on a transparent substrate and is illuminated from the back side while electrons are collected from the other (front) side. In this paper, the working principle of this technique, coined back-illuminated PEEM (BIPEEM), is described. In BIPEEM, the electron intensity is strongly thickness-dependent. This dependence can be described by a simple model which contains the optical attenuation length and the electron mean free path. Electrons forming an image in BIPEEM hence carry information of the inner part of the sample, as well as of the surface, as we demonstrate experimentally.

The LEEM-IV spectra of few-layer graphene show characteristic minima at specific energies, which depend on the number of graphene layers. For the same samples, low-energy TEM (eV-TEM) spectra exhibit transmission maxima at energies corresponding to those of the reflection minima in LEEM. Both features can be understood from interferences of the electron wave function in a purely elastic model. Inelastic scattering processes in turn lead to a finite, energy-dependent inelastic Mean Free Path (MFP) and a lower finesse of the interference features. Here we develop a model that introduces both an elastic and inelastic scattering parameter on the wave-function level, thus reconciling the models considered previously. Fitting to published data, we extract the elastic and inelastic MFP self-consistently and compare these to recent reports.

We describe a cryogenic sample chamber for low energy electron microscopy (LEEM), and present first experimental results. Modifications to our IBM/SPECS aberration-corrected LEEM instrument are presented first. These include incorporation of mechanisms for cooling the sample and its surroundings, and reduction of various sources of heat load. Using both liquid nitrogen and liquid helium, we have reached sample temperatures down to about 15 K. We also present first results for low-temperature LEEM, obtained on a three-monolayer pentacene film. Specifically, we observe a reduction of the electron beam irradiation damage cross-section at 15 eV by more than a factor of five upon cooling from 300 K down to 52 K. We also observe changes in the LEEM-IV spectra of the sample upon cooling, and discuss possible causes.

In a Low Energy Electron Microscope (LEEM) the sample is illuminated with an electron beam with typical electron landing energies from 0-100 eV. The energy spread of the electron beam is determined by the characteristics of the electron source. For the two most commonly used electron sources, LaB6 and cold field emission W, typical energy spreads Delta E are 0.75 and 0.25 eV at full width half maximum, respectively. Here we present a design for a LEEM gun energy filter, that reduces Delta E to similar to 100 meV. Such a filter has been incorporated in the IBM/SPECS AC-LEEM system at IBM. Experimental results are presented and found to be in excellent agreement with expectations.

In 'magic angle' twisted bilayer graphene (TBG) a flat band forms, yielding correlated insulator behavior and superconductivity. In general, the moiré structure in TBG varies spatially, influencing the overall conductance properties of devices. Hence, to understand the wide variety of phase diagrams observed, a detailed understanding of local variations is needed. Here, we study spatial and temporal variations of the moiré pattern in TBG using aberration-corrected Low Energy Electron Microscopy (AC-LEEM). We find a smaller spatial variation than reported previously. Furthermore, we observe thermal fluctuations corresponding to collective atomic displacements over 70 pm on a timescale of seconds. Remarkably, no untwisting is found up to 600 ∘C. We conclude that thermal annealing can be used to decrease local disorder. Finally, we observe edge dislocations in the underlying atomic lattice, the moiré structure acting as a magnifying glass. These topological defects are anticipated to exhibit unique local electronic properties.

Transmission electron microscopy at very low energy is a promising way to avoid damaging delicate biological samples with the incident electrons, a known problem in conventional transmission electron microscopy. For imaging in the 0-30 eV range, we added a second electron source to a low energy electron microscopy (LEEM) setup, enabling imaging and spectroscopy in both transmission and reflection mode at nanometer (nm) resolution. The latter is experimentally demonstrated for free-standing graphene. Exemplary eV-TEM micrographs of gold nanoparticles suspended on graphene and of DNA origami rectangles on graphene oxide further establish the capabilities of the technique. The long and short axes of the DNA origami rectangles are discernable even after an hour of illumination with low energy electrons. In combination with recent developments in 2D membranes, allowing for versatile sample preparation, eV-TEM is paving the way to damage-free imaging of biological samples at nm resolution.

Tobias A. de Jong, Tjerk Benschop, Xing Chen, R.M. Tromp, M. de Dood, D. Efetov, F. Baumberger, M. Allan, S.J. van der Molen Leiden Institute of Physics, Niels Bohrweg 2, Leiden, The Netherlands IBM T.J. Watson Research Center, Yorktown Heights, New York 10598, USA Institut de Ciencies Fotoniques, The Barcelona Institute of Science and Technology, Castelldefels, Barcelona, Spain Department of Quantum Matter Physics, University of Geneva, 24 Quai Ernest-Ansermet, 1211 Geneva 4, Switzerland Swiss Light Source, Paul Scherrer Institute, CH-5232 Villigen PSI, Switzerland

Crystalline films of pentacene molecules, two to four monolayers in thickness, are grown via in situ sublimation on silicon substrates in the ultrahigh vacuum chamber of a low-energy electron microscope. It is observed that the diffraction pattern of the pentacene layers fades upon irradiation with low-energy electrons. The damage cross section is found to increase by more than an order of magnitude for electron energies from 0 to 10 eV and by another order of magnitude from 10 to 40 eV. Close to 0 eV, damage is virtually nil. Creation of chemically reactive atomic centers after electron attachment or impact ionization is thought to trigger chemical reactions between neighboring molecules that gradually transform the layer into a disordered carbon nanomembrane. Additionally, diminishing spectroscopic features related to the unoccupied band structure of the layers, accompanied by loss of definition in real-space images, and an increase in the background intensity of diffraction images during irradiation point to chemical changes and formation of a disordered layer.

Imaging dynamical processes at interfaces and on the nanoscale is of great importance throughout science and technology. While light-optical imaging techniques often cannot provide the necessary spatial resolution, electron-optical techniques damage the specimen and cause dose-induced artefacts. Here, Optical Near-field Electron Microscopy (ONEM) is proposed, an imaging technique that combines non-invasive probing with light, with a high spatial resolution read-out via electron optics. Close to the specimen, the optical near-fields are converted into a spatially varying electron flux using a planar photocathode. The electron flux is imaged using low energy electron microscopy, enabling label-free nanometric resolution without the need to scan a probe across the sample. The specimen is never exposed to damaging electrons.