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... Show moreStacking 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. Show less
Jong, T.A. de; Visser, L.; Jobst, J.; Tromp, R.M.; Molen, S.J. van der 2022
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... Show moreTerrace-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 moiré pattern with domain boundaries between AB and BA stackings.We analyze this moiré 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. Show less
In twisted bilayer graphene (TBG) a moiré pattern forms that introduces a new length scale to the material. At the 'magic' twist angle of 1.1°, this causes a flat band to form, yielding emergent... Show moreIn twisted bilayer graphene (TBG) a moiré pattern forms that introduces a new length scale to the material. At the 'magic' twist angle of 1.1°, this causes a flat band to form, yielding emergent properties such as correlated insulator behavior and superconductivity [1-4]. In general, the moiré structure in TBG varies spatially, influencing the local electronic properties [5-9] and hence the outcome of macroscopic charge transport experiments. In particular, to understand the wide variety observed in the phase diagrams and critical temperatures, a more detailed understanding of the local moiré variation is needed [10]. Here, we study spatial and temporal variations of the moiré pattern in TBG using aberration-corrected Low Energy Electron Microscopy (AC-LEEM) [11,12]. The spatial variation we find is lower than reported previously. At 500°C, we observe thermal fluctuations of the moiré lattice, corresponding to collective atomic displacements of less than 70pm on a time scale of seconds [13], homogenizing the sample. Despite previous concerns, no untwisting of the layers is found, even at temperatures as high as 600°C [14,15]. From these observations, we conclude that thermal annealing can be used to decrease the local disorder in TBG samples. Finally, we report the existence of individual edge dislocations in the atomic and moiré lattice. These topological defects break translation symmetry and are anticipated to exhibit unique local electronic properties. Show less
Tebyani, A.; Baalbergen, F.B.; Tromp, R.M.; Molen, S.J. van der 2021
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... Show moreFor 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. Show less
Jobst, J.; Boers, L.M.; Yin, C.; Aarts, J.; Tromp, R.M.; Molen, S.J. van der 2019
For many applications, it is important to measure the local work function of a surface with high lateral resolution. Low-energy electron microscopy is regularly employed to this end since it is, in... Show moreFor many applications, it is important to measure the local work function of a surface with high lateral resolution. Low-energy electron microscopy is regularly employed to this end since it is, in principle, very well suited as it combines high-resolution imaging with high sensitivity to local electrostatic potentials. For surfaces with areas of different work function, however, lateral electrostatic fields inevitably associated with work function discontinuities deflect the low-energy electrons and thereby cause artifacts near these discontinuities. We use ray-tracing simulations to show that these artifacts extend over hundreds of nanometers and cause an overestimation of the true work function difference near the discontinuity by a factor of 1.6 if the standard image analysis methods are used. We demonstrate on a mixed-terminated strontium titanate surface that comparing LEEM data with detailed ray-tracing simulations leads to much a more robust estimate of the work function difference. Show less
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... Show moreGraphene 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. Show less
Jobst, J.; Kautz, J.; Mytiliniou, M.; Tromp, R.M.; Molen, S.J. van der 2017
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... Show moreIn 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 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. Show less
