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
Transport experiments in twisted bilayer graphene haverevealed multiple superconducting domes separated by cor-related insulating states 1–5 . These properties are generallyassociated with strongly... Show moreTransport experiments in twisted bilayer graphene haverevealed multiple superconducting domes separated by cor-related insulating states 1–5 . These properties are generallyassociated with strongly correlated states in a flat mini-bandof the hexagonal moiré superlattice as was predicted by bandstructure calculations 6–8 . Evidence for the existence of a flatband comes from local tunnelling spectroscopy 9–13 and elec-tronic compressibility measurements 14 , which report two ormore sharp peaks in the density of states that may be asso-ciated with closely spaced Van Hove singularities. However,direct momentum-resolved measurements have proved to bechallenging 15 . Here, we combine different imaging techniquesand angle-resolved photoemission with simultaneous real- andmomentum-space resolution (nano-ARPES) to directly mapthe band dispersion in twisted bilayer graphene devices nearcharge neutrality. Our experiments reveal large areas with ahomogeneous twist angle that support a flat band with a spec-tral weight that is highly localized in momentum space. The flatband is separated from the dispersive Dirac bands, which showmultiple moiré hybridization gaps. These data establish thesalient features of the twisted bilayer graphene band structure. Show less
Bespalov, I.; Zhang, Y.; Haitjema, J.; Tromp, R.M.; Molen, S.J. van der; Brouwer, A.M.; ... ; Castellanos, S. 2020
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... Show moreThe 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. Show less
Jong, T.A. de; Kok, D.N.L.; Torren, A.J.H. van der; Schopmans, H.; Tromp, R.M.; Molen, S.J. van der; Jobst, J. 2019
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
Torren, A.J.H. van der; Yuan, H.; Liao, Z.; Elshof, J.E. ten; Koster, G.; Huijben, M.; ... ; Aarts, J. 2019
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... Show moreThe 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. Show less
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... Show moreThe 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. Show less
Jong, T.A. de; Krasovskii, E.E.; Ott, C.; Tromp, R.M.; Molen, S.J. van der; Jobst, J. 2018
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
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
Kisslinger, F.; Popp, M.; Jobst, J.; Weber, H.B. 2017
High electron mobility is one of graphene’s key properties, exploited for applications and fundamental research alike. Highest mobility values are found in heterostructures of graphene and... Show moreHigh electron mobility is one of graphene’s key properties, exploited for applications and fundamental research alike. Highest mobility values are found in heterostructures of graphene and hexagonal boron nitride, which consequently are widely used. However, surprisingly little is known about the interaction between the electronic states of these layered systems. Rather pragmatically, it is assumed that these do not couple significantly. Here we study the unoccupied band structure of graphite, boron nitride and their heterostructures using angle-resolved reflected-electron spectroscopy. We demonstrate that graphene and boron nitride bands do not interact over a wide energy range, despite their very similar dispersions. The method we use can be generally applied to study interactions in van der Waals systems, that is, artificial stacks of layered materials. With this we can quantitatively understand the ‘chemistry of layers’ by which novel materials are created via electronic coupling between the layers they are composed of. Show less
Jobst, J.; Kautz, J.; Geelen, D.; Tromp, R.M.; Molen, S.J. van der 2015
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... Show moreThe 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. Show less
Kautz, J.; Jobst, J.; Sorger, C.; Tromp, R.M.; Weber, H.B.; Molen, S.J. van der 2015
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,... Show moreCharge 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. Show less
