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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.

Extreme ultraviolet (EUV) lithography (13.5 nm) is the newest technology that allows high-throughput fabrication of electronic circuitry in the sub-20 nm scale. It is commonly assumed that low-energy electrons (LEEs) generated in the resist materials by EUV photons are mostly responsible for the solubility switch that leads to nanopattern formation. Yet, reliable quantitative information on this electron-induced process is scarce. In this work, we combine LEE microscopy (LEEM), electron energy loss spectroscopy (EELS), and atomic force microscopy (AFM) to study changes induced by electrons in the 0–40 eV range in thin films of a state-of-the-art molecular organometallic EUV resist known as tin-oxo cage. LEEM–EELS uniquely allows to correct for surface charging and thus to accurately determine the electron landing energy. AFM postexposure analyses revealed that irradiation of the resist with LEEs leads to the densification of the resist layer because of carbon loss. Remarkably, electrons with energies as low as 1.2 eV can induce chemical reactions in the Sn-based resist. Electrons with higher energies are expected to cause electronic excitation or ionization, opening up more pathways to enhanced conversion. However, we do not observe a substantial increase of chemical conversion (densification) with the electron energy increase in the 2–40 eV range. Based on the dose-dependent thickness profiles, a simplified reaction model is proposed where the resist undergoes sequential chemical reactions, first yielding a sparsely cross-linked network and then a more densely cross-linked network. This model allows us to estimate a maximum reaction volume on the initial material of 0.15 nm3 per incident electron in the energy range studied, which means that about 10 LEEs per molecule on average are needed to turn the material insoluble and thus render a pattern. Our observations are consistent with the observed EUV sensitivity of tin-oxo cages.

Transport experiments in twisted bilayer graphene have revealed multiple superconducting domes separated by correlated insulating states1–5. These properties are generally associated with strongly correlated states in a flat mini-band of the hexagonal moire superlattice as was predicted by band structure calculations6–8. Evidence for the existence of a flat band comes from local tunnelling spectroscopy9–13 and electronic compressibility measurements14, which report two or more sharp peaks in the density of states that may be associated with closely spaced Van Hove singularities. However, direct momentum-resolved measurements have proved to be challenging15. Here, we combine different imaging techniques and angle-resolved photoemission with simultaneous real- and momentum-space resolution (nano-ARPES) to directly map the band dispersion in twisted bilayer graphene devices near charge neutrality. Our experiments reveal large areas with a homogeneous twist angle that support a flat band with a spectral weight that is highly localized in momentum space. The flat band is separated from the dispersive Dirac bands, which show multiple moire hybridization gaps. These data establish the salient features of the twisted bilayer graphene band structure. Spectroscopic measurements using nano-ARPES on twisted bilayer graphene directly highlight the presence of the flat bands.

The two-dimensional electron liquid which forms between the band insulators LaAlO3 (LAO) and SrTiO3 (STO) is a promising component for oxide electronics, but the requirement of using single crystal SrTiO3 substrates for the growth limits its applications in terms of device fabrication. It is therefore important to find ways to deposit these materials on other substrates, preferably Si, or Si-based, in order to facilitate integration with existing technology. Interesting candidates are micron-sized nanosheets of Ca2Nb3O10 which can be used as seed layers for perovskite materials on any substrate. We have used low-energy electron microscopy (LEEM) with in-situ pulsed laser deposition to study the subsequent growth of STO and LAO on such flakes which were deposited on Si. We can follow the morphology and crystallinity of the layers during growth, as well as fingerprint their electronic properties with angle resolved reflected electron spectroscopy. We find that STO layers, deposited on the nanosheets, can be made crystalline and flat; that LAO can be grown in a layer-by-layer fashion; and that the full heterostructure shows the signature of the formation of a conducting interface., 11 pages, 7 figures

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.

The properties of Van der Waals (VdW) heterostructures are determined by the twist angle and the interface between adjacent layers as well as their polytype and stacking. Here, the use of spectroscopic low energy electron microscopy (LEEM) and micro low energy electron diffraction (µLEED) methods to measure these properties locally is described. The authors present results on a MoS2/hBN heterostructure, but the methods are applicable to other materials. Diffraction spot analysis is used to assess the benefits of using hBN as a substrate. In addition, by making use of the broken rotational symmetry of the lattice, the cleaving history of the MoS2 flake is determined, that is, which layer stems from where in the bulk.

Graphene on silicon carbide (SiC) bears great potential for future graphene electronic applications because it is available on the wafer scale and its properties can be custom tailored by inserting various atoms into the graphene/SiC interface. It remains unclear, however, how atoms can cross the impermeable graphene layer during this widely used intercalation process. Here we demonstrate that in contrast to the current consensus, graphene layers grown in argon atmosphere on SiC are not homogeneous, but instead are composed of domains of different crystallographic stacking as they have been observed in other systems. We show that these domains are intrinsically formed during growth and that dislocations between domains dominate the (de)intercalation dynamics. Tailoring these dislocation networks, e.g., through substrate engineering, will increase the control over the intercalation process and could open a playground for topological and correlated electron phenomena in two-dimensional superstructures.

We live in an age of nanomaterials in which new materials are discovered almost every day. Moreover, we are starting to engineer material properties at the nanoscale. Hence, we need new tools to investigate different materials routinely and on small length scales.

In a lot of systems, charge transport is governed by local features rather than being a global property as suggested by extracting a single resistance value. Consequently, techniques that resolve local structure in the electronic potential are crucial for a detailed understanding of electronic transport in realistic devices. Recently, we have introduced a new potentiometry method based on low-energy electron microscopy (LEEM) that utilizes characteristic features in the reflectivity spectra of layered materials [1]. Performing potentiometry experiments in LEEM has the advantage of being fast, offering a large field of view and the option to zoom in and out easily, and of being non-invasive compared to scanning-probe methods. However, not all materials show clear features in their reflectivity spectra. Here we, therefore, focus on a different version of low-energy electron potentiometry (LEEP) that uses the mirror mode transition, i.e. the drop in electron reflectivity around zero electron landing energy when they start to interact with the sample rather than being reflected in front of it. This transition is universal and sensitive to the local electrostatic surface potential (either workfunction or applied potential). It can consequently be used to perform LEEP experiments on a broader range of material compared to the method described in Ref. [1]. We provide a detailed description of the experimental setup and demonstrate LEEP on workfunction-related intrinsic potential variations on the Si(111) surface and for a metal-semiconductor-metal junction with an external bias applied. In the latter, we visualize the Schottky effect at the metal-semiconductor interface. Finally, we compare how robust the two LEEP techniques discussed above are against image distortions due to sample inhomogeneities or contamination.

The properties of any material are fundamentally determined by its electronic band structure. Each band represents a series of allowed states inside a material, relating electron energy and momentum. The occupied bands, that is, the filled electron states below the Fermi level, can be routinely measured. However, it is remarkably difficult to characterize the empty part of the band structure experimentally. Here, we present direct measurements of unoccupied bands of monolayer, bilayer and trilayer graphene. To obtain these, we introduce a technique based on low-energy electron microscopy. It relies on the dependence of the electron reflectivity on incidence angle and energy and has a spatial resolution ∼10 nm. The method can be easily applied to other nanomaterials such as van der Waals structures that are available in small crystals only., The electronic properties of a material depend on both the filled and the unoccupied electron states. Here, the authors present a technique based on low-energy electron microscopy that is able to directly probe the unoccupied bands of few-layer graphene, as well as other materials.

In the visible to infrared spectral range, highly-reflective silver mirrors are applied in the manufacture of optical instruments such as telescopes. However, it is still difficult to combine high reflectivity and long-term stability of the protected silver coating. We show that the deposition of impervious protective layers is necessary but often not sufficient for long-term environmental stability. Hygroscopic air borne particles absorbed by the protections surface attract water molecules and form a solution. This solution first damages the protection, subsequently permeates the protection and finally damages the silver whereby the reflectivity is reduced. We demonstrate this particular damage mechanism with different experiments and describe this mechanism in detail.

The direct wafer bonding technology is applied to join glass substrates for optical devices in high power laser applications. Uncoated as well as coated fused silica substrates were bonded to each other by hydrophilic direct bonding and -for comparison- sodium silicate-solution bonding. Both technologies are expected to generate materials-adapted Si-O-Si bonds at uncoated interfaces. Optical transmission and reflection in the spectral range of 200 nm to 1200 nm were measured and reveal superior transmission for the direct bonding technology in the ultra-violet range. Even in the near infrared at 980 nm, better performance with direct bonding as compared to silicate-solution bonding is evidenced by laser induced damage threshold measurements. For all coated samples, a distinct reduction in bonding strength relative to uncoated ones is observed in 3-point bending tests.

We present a technique to tune the charge density of epitaxial graphene via an electrostatic gate that is buried in the silicon carbide substrate. The result is a device in which graphene remains accessible for further manipulation or investigation. Via nitrogen or phosphor implantation into a silicon carbide wafer and subsequent graphene growth, devices can routinely be fabricated using standard semiconductor technology. We have optimized samples for room temperature as well as for cryogenic temperature operation. Depending on implantation dose and temperature we operate in two gating regimes. In the first, the gating mechanism is similar to a MOSFET, the second is based on a tuned space charge region of the silicon carbide semiconductor. We present a detailed model that describes the two gating regimes and the transition in between., Manuscript submitted to Journal of Physics D

Graphene, a single monolayer of graphite, has recently attracted considerable interest owing to its novel magneto-transport properties, high carrier mobility and ballistic transport up to room temperature. It has the potential for technological applications as a successor of silicon in the post Moore's law era, as a single-molecule gas sensor, in spintronics, in quantum computing or as a terahertz oscillator. For such applications, uniform ordered growth of graphene on an insulating substrate is necessary. The growth of graphene on insulating silicon carbide (SiC) surfaces by high-temperature annealing in vacuum was previously proposed to open a route for large-scale production of graphene-based devices. However, vacuum decomposition of SiC yields graphene layers with small grains (30-200 nm; refs 14-16). Here, we show that the ex situ graphitization of Si-terminated SiC(0001) in an argon atmosphere of about 1 bar produces monolayer graphene films with much larger domain sizes than previously attainable. Raman spectroscopy and Hall measurements confirm the improved quality of the films thus obtained. High electronic mobilities were found, which reach mu=2,000 cm (2) V(-1) s(-1) at T=27 K. The new growth process introduced here establishes a method for the synthesis of graphene films on a technologically viable basis.

Low Energy Electron Microscopy (LEEM) is a specialized surface-sensitive microscopy technique utilizing electron with energies more than 1000 times lower than regular EM. This provides unique measurement opportunities, but also challenges in the analysis of the data. Here, we showcase how we utilize Numpy, Scipy, Dask and Scikit Learn and other parts of the scientific python stack to implement image analysis techniques, previously described for other microscopy techniques, but adapted to the specific challenges of LEEM [1,2]. Amongst others, we implement fast, parallelized, image (stack) registration and image stitching using Dask. We show that the image registration algorithm is, in the best-case, accurate to the sub-pixel level results and fast enough to enable registration of 500 images within 7 minutes on a regular desktop CPU, enabling per-pixel analysis of spectroscopic datasets, where energy is added to the images as a third dimension. Similarly, the stitching algorithm allows for the creation of 100Mpixel+ overview images from tiles with estimated positions. In summary, we show that the use of the scientific python stack allows for easy adoption to specific peculiarities of different imaging techniques and even individual datasets. We anticipate the code from this work can be adapted to be applied to other forms of electron microscopy such as PEEM, scanning tunneling microscopy, and others, providing a open source, Python alternative to existing closed source / undisclosed implementations in often proprietary languages. [1] T.A. de Jong et al., Quantitative analysis of spectroscopic Low Energy Electron Microscopy data: High-dynamic range imaging, drift correction and cluster analysis, Ultramicroscopy, Volume 213, 2020, https://doi.org/10.1016/j.ultramic.2019.112913. [2] https://github.com/TAdeJong/LEEM-analysis, This work was financially supported by the Netherlands Organisation for Scientific Research (NWO/OCW) as part of the Frontiers of Nanoscience (NanoFront) program.