Back illuminated photo emission electron microscopy (BIPEEM).

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.

Flat Γ Moiré Bands in Twisted Bilayer WSe_{2}.

The recent observation of correlated phases in transition metal dichalcogenide moiré systems at integer and fractional filling promises new insight into metal-insulator transitions and the unusual states of matter that can emerge near such transitions. Here, we combine real- and momentum-space mapping techniques to study moiré superlattice effects in 57.4° twisted WSe_{2} (tWSe_{2}). Our data reveal a split-off flat band that derives from the monolayer Γ states. Using advanced data analysis, we directly quantify the moiré potential from our data. We further demonstrate that the global valence band maximum in tWSe_{2} is close in energy to this flat band but derives from the monolayer K states which show weaker superlattice effects. These results constrain theoretical models and open the perspective that Γ-valley flat bands might be involved in the correlated physics of twisted WSe_{2}.

Low-Energy Electron Irradiation Damage in Few-Monolayer Pentacene Films.

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.

Quantitative analysis of spectroscopic low energy electron microscopy data: High-dynamic range imaging, drift correction and cluster analysis.

For many complex materials systems, low-energy electron microscopy (LEEM) offers detailed insights into morphology and crystallography by naturally combining real-space and reciprocal-space information. Its unique strength, however, is that all measurements can easily be performed energy-dependently. Consequently, one should treat LEEM measurements as multi-dimensional, spectroscopic datasets rather than as images to fully harvest this potential. Here we describe a measurement and data analysis approach to obtain such quantitative spectroscopic LEEM datasets with high lateral resolution. The employed detector correction and adjustment techniques enable measurement of true reflectivity values over four orders of magnitudes of intensity. Moreover, we show a drift correction algorithm, tailored for LEEM datasets with inverting contrast, that yields sub-pixel accuracy without special computational demands. Finally, we apply dimension reduction techniques to summarize the key spectroscopic features of datasets with hundreds of images into two single images that can easily be presented and interpreted intuitively. We use cluster analysis to automatically identify different materials within the field of view and to calculate average spectra per material. We demonstrate these methods by analyzing bright-field and dark-field datasets of few-layer graphene grown on silicon carbide and provide a high-performance Python implementation.

Nonuniversal Transverse Electron Mean Free Path through Few-layer Graphene.

In contrast to the in-plane transport electron mean-free path in graphene, the transverse mean-free path has received little attention and is often assumed to follow the "universal" mean-free path (MFP) curve broadly adopted in surface and interface science. Here we directly measure transverse electron scattering through graphene from 0 to 25 eV above the vacuum level both in reflection using low energy electron microscopy and in transmission using electronvolt transmission electron microscopy. From these data, we obtain quantitative MFPs for both elastic and inelastic scattering. Even at the lowest energies, the total MFP is just a few graphene layers and the elastic MFP oscillates with graphene layer number, both refuting the universal curve. A full theoretical calculation taking the graphene band structure into consideration agrees well with experiment, while the key experimental results are reproduced even by a simple optical toy model.

Charge Catastrophe and Dielectric Breakdown During Exposure of Organic Thin Films to Low-Energy Electron Radiation.

The effects of exposure to ionizing radiation are central in many areas of science and technology, including medicine and biology. Absorption of UV and soft-x-ray photons releases photoelectrons, followed by a cascade of lower energy secondary electrons with energies down to 0 eV. While these low energy electrons give rise to most chemical and physical changes, their interactions with soft materials are not well studied or understood. Here, we use a low energy electron microscope to expose thin organic resist films to electrons in the range 0-50 eV, and to analyze the energy distribution of electrons returned to the vacuum. We observe surface charging that depends strongly and nonlinearly on electron energy and electron beam current, abruptly switching sign during exposure. Charging can even be sufficiently severe to induce dielectric breakdown across the film. We provide a simple but comprehensive theoretical description of these phenomena, identifying the presence of a cusp catastrophe to explain the sudden switching phenomena seen in the experiments. Surprisingly, the films undergo changes at all incident electron energies, starting at ∼0 eV.

Imaging pulsed laser deposition growth of homo-epitaxial SrTiO3 by low-energy electron microscopy.

By combining low-energy electron microscopy with in situ pulsed laser deposition we have developed a new technique for film growth analysis, making use of both diffraction and real-space information. Working at the growth temperature, we can use: the intensity and profile variations of the specular beam to follow the coverage in a layer-by-layer fashion; real-space microscopy to follow e.g. atomic steps at the surface; and electron reflectivity to probe the unoccupied band structure of the grown material. Here, we demonstrate our methodology for homo-epitaxial growth of SrTiO3. Interestingly, the same combination of techniques will also be applicable to hetero-epitaxial oxide growth, largely extending the scope of research possibilities.

Low-Energy Electron Potentiometry: Contactless Imaging of Charge Transport on the Nanoscale.

Charge transport measurements form an essential tool in condensed matter physics. The usual approach is to contact a sample by two or four probes, measure the resistance and derive the resistivity, assuming homogeneity within the sample. A more thorough understanding, however, requires knowledge of local resistivity variations. Spatially resolved information is particularly important when studying novel materials like topological insulators, where the current is localized at the edges, or quasi-two-dimensional (2D) systems, where small-scale variations can determine global properties. Here, we demonstrate a new method to determine spatially-resolved voltage maps of current-carrying samples. This technique is based on low-energy electron microscopy (LEEM) and is therefore quick and non-invasive. It makes use of resonance-induced contrast, which strongly depends on the local potential. We demonstrate our method using single to triple layer graphene. However, it is straightforwardly extendable to other quasi-2D systems, most prominently to the upcoming class of layered van der Waals materials.

Intrinsic instability of aberration-corrected electron microscopes.

Aberration-corrected microscopes with subatomic resolution will impact broad areas of science and technology. However, the experimentally observed lifetime of the corrected state is just a few minutes. Here we show that the corrected state is intrinsically unstable; the higher its quality, the more unstable it is. Analyzing the contrast transfer function near optimum correction, we define an "instability budget" which allows a rational trade-off between resolution and stability. Unless control systems are developed to overcome these challenges, intrinsic instability poses a fundamental limit to the resolution practically achievable in the electron microscope.

Controlling the interparticle distance in a 2D molecule-nanoparticle network.

Mechanically controllable break junctions allow for an impressive level of control over the distance between two electrodes, but lack stability at room temperature. On the other hand, two-dimensional (2D) networks of nanoparticles bridged by molecules form a stable device structure for investigating molecular conductance properties. Here, we combine both techniques to create a robust platform for molecular charge transport with control over the inter-electrode distance on the picometer scale. The resistance change due to bending of our structures is dependent on the molecular species present between the nanoparticles.

Transition voltage spectroscopy and the nature of vacuum tunneling.

Transition voltage spectroscopy (TVS) has been proposed as a tool to analyze charge transport through molecular junctions. We extend TVS to Au-vacuum-Au junctions and study the distance dependence of the transition voltage V(t)(d) for clean electrodes in cryogenic vacuum. On the one hand, this allows us to provide an important reference for V(t)(d) measurements on molecular junctions. On the other hand, we show that TVS forms a simple and powerful test for vacuum tunneling models.

Universal scaling in highly doped conducting polymer films.

Electrical transport of a highly doped disordered conducting polymer, viz. poly-3,4-ethylenedioxythiophene stabilized with poly-4-styrenesulphonic acid, is investigated as a function of bias and temperature. The transport shows universal power-law scaling with both bias and temperature. All measurements constitute a single universal curve, and the complete J(V,T) characteristics are described by a single equation. We relate this scaling to dissipative tunneling processes, such as Coulomb blockade.

Medipix 2 detector applied to low energy electron microscopy.

Low energy electron microscopy (LEEM) and photo-emission electron microscopy (PEEM) traditionally use microchannel plates (MCPs), a phosphor screen and a CCD-camera to record images and diffraction patterns. In recent years, however, MCPs have become a limiting factor for these types of microscopy. Here, we report on a successful test series using a solid state hybrid pixel detector, Medipix 2, in LEEM and PEEM. Medipix 2 is a background-free detector with an infinite dynamic range, making it very promising for both real-space imaging and spectroscopy. We demonstrate a significant enhancement of both image contrast and resolution, as compared to MCPs. Since aging of the Medipix 2 detector is negligible for the electron energies used in LEEM/PEEM, we expect Medipix to become the detector of choice for a new generation of systems.

Conductance switching in Ag(2)S devices fabricated by in situ sulfurization.

We report a simple and reproducible method to fabricate switchable Ag(2)S devices. The alpha-Ag(2)S thin films are produced by a sulfurization process after silver deposition on an Si substrate. Structure and composition of the Ag(2)S are characterized using XRD and RBS. Our samples show semiconductor behaviour at low bias voltages, whereas they exhibit reproducible bipolar resistance switching at higher bias voltages. The transition between both types of behaviour is observed by hysteresis in the I-V curves, indicating decomposition of the Ag(2)S, increasing the Ag(+) ion mobility. The as-fabricated Ag(2)S samples are a good candidate for future solid state memory devices, as they show reproducible memory resistive properties and they are fabricated by an accessible and reliable method.

Single atom adhesion in optimized gold nanojunctions.

We study the interaction between single apex atoms in a metallic contact, using the break junction geometry. By carefully training our samples, we create stable junctions in which no further atomic reorganization takes place. This allows us to study the relation between the so-called jump out of contact (from contact to tunneling regime) and jump to contact (from tunneling to contact regime) in detail. Our data can be fully understood within a relatively simple elastic model, where the elasticity k of the electrodes is the only free parameter. We find 5

One-way optoelectronic switching of photochromic molecules on gold.

We investigate photochromic molecular switches that are self-assembled on gold. We use two experimental techniques; namely, the mechanically controllable break-junction technique to measure electronic transport, and UV/Vis spectroscopy to measure absorption. We observe switching of the molecules from the conducting to the insulating state when illuminated with visible light (lambda=546 nm), in spite of the gold surface plasmon absorption present around this wavelength. However, we fail to observe the reverse process which should occur upon illumination with UV light (lambda=313 nm). We attribute this to quenching of the excited state of the molecule in the open form by the presence of gold.