arXiv subjects

Sense Jan van der Molen

Publications and source records attributed to Sense Jan van der Molen.

17 recordsLinked to original sources

arXiv2023

Sharp zero-phonon lines of single organic molecules on a hexagonal boron-nitride surface

Single fluorescent molecules embedded in the bulk of host crystals have proven to be excellent probes of the dynamics in their nano environment, thanks to their narrow (about 0.1 μeV) optical linewidth of the 0-0 zero-phonon line (0-0 ZPL) at cryogenic temperatures. However, the optical linewidths of the 0-0 ZPL have been found to increase dramatically as the single molecules are located closer to a surface or interface, while no 0-0 ZPL has been detected for organic molecules on any surface. Here, we study single fluorescent terrylene molecules adsorbed on the surface of hexagonal boron-nitride (hBN) substrates. Our low-temperature results show for the first time the observation of the 0-0 ZPL of fluorescent molecules on a surface. With resonant excitation, we find 0-0 ZPL linewidths down to values that are about 10 times larger than the Fourier limit of 45 +/- 3 MHz, dictated by the fluorescence lifetime. We compare our results for molecules deposited on the surfaces of annealed and non-annealed hBN flakes and we see a marked improvement in the spectral stability of the emitters after annealing. Our high-resolution spectra obtained on terrylene suggest the possibility of employing hBN in combination with a wide variety of single molecule emitters for investigation of physical phenomena at surfaces or for use in nanophotonic devices.

physics.chem-ph↗

arXiv2022

Observation of 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$^{\circ}$ 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$_2$.

cond-mat.str-el↗

arXiv2022

Low-Energy Electron Microscopy contrast of stacking boundaries: comparing twisted few-layer graphene and strained epitaxial graphene on silicon carbide

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.

cond-mat.mes-hall↗

arXiv2022

Stacking domain morphology in epitaxial graphene on silicon carbide

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 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.

cond-mat.mes-hall↗

arXiv2021

Imaging moiré deformation and dynamics in twisted bilayer graphene

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 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.

cond-mat.mes-hall↗

arXiv2021

Measuring local moiré lattice heterogeneity of twisted bilayer graphene

We introduce a new method to continuously map inhomogeneities of a moiré lattice and apply it to large-area topographic images we measure on open-device twisted bilayer graphene (TBG). We show that the variation in the twist angle of a TBG device, which is frequently conjectured to be the reason for differences between devices with a supposed similar twist angle, is about 0.08° around the average of 2.02° over areas of several hundred nm, comparable to devices encapsulated between hBN slabs. We distinguish between an effective twist angle and local anisotropy and relate the latter to heterostrain. Our results imply that for our devices, twist angle heterogeneity has a roughly equal effect to the electronic structure as local strain. The method introduced here is applicable to results from different imaging techniques, and on different moiré materials.

cond-mat.mes-hall↗

arXiv2020

Complementary LEEM and eV-TEM for imaging and spectroscopy

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 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.

cond-mat.mtrl-sci↗

arXiv2020

Direct evidence for flat bands in twisted bilayer graphene from nano-ARPES

Transport experiments in twisted bilayer graphene revealed multiple superconducting domes separated by correlated insulating states. These properties are generally associated with strongly correlated states in a flat mini-band of the hexagonal moiré superlattice as it was predicted by band structure calculations. Evidence for such a flat band comes from local tunneling spectroscopy and electronic compressibility measurements, reporting two or more sharp peaks in the density of states that may be associated with closely spaced van Hove singularities. Direct momentum resolved measurements proved difficult though. 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 homogeneous twist angle that support a flat band with spectral weight that is highly localized in momentum space. The flat band is separated from the dispersive Dirac bands which show multiple moiré hybridization gaps. These data establish the salient features of the twisted bilayer graphene band structure.

cond-mat.str-el↗

arXiv2019

Patterning Sn-based EUV resists with low-energy electrons

Extreme Ultraviolet (EUV) lithography is the newest technology that will be used in the semiconductor industry for printing circuitry in the sub-20 nm scale. Low-energy electrons (LEEs) produced upon illumination of resist materials with EUV photons (92 eV) play a central role in the formation of the nanopatterns. However, up to now the details of this process are not well understood. In this work, a novel experimental approach that combines Low-Energy Electron Microscopy (LEEM), Electron Energy Loss Spectroscopy (EELS), and Atomic Force Microscopy (AFM) is used to study changes induced by electrons in the 0-40 eV range in thin films of molecular organometallic EUV resists known as tin-oxo cages. LEEM-EELS spectroscopic experiments were used to detect surface charging upon electron exposure and to estimate the electron landing energy. AFM post-exposure analyses revealed that irradiation of the resist with LEEs leads to the densification of the resist layer associated to carbon loss. The same chemical processes that yield densification render the solubility change responsible for the pattern formation in the lithographic application. Remarkably, electrons as low as 1.2 eV are able to induce chemical reactions in the Sn-based resist. Based on the thickness profiles resulting from LEE exposures in the 3-48 mC/cm 2 dose range, a simplified reaction model is proposed where the resist undergoes sequential chemical reactions, yielding first a sparsely cross-linked network, followed by the formation of a denser cross-linked network. This model allows us to estimate a maximum reaction volume on the initial material of 0.15 nm 3 per incident electron in the energy range studied, which means that less than 10 LEEs per molecule on average are needed to turn the material insoluble and thus render a pattern.

physics.app-ph↗

arXiv2019

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.

cond-mat.mtrl-sci↗

arXiv2018

Quantifying work function differences using low-energy electron microscopy: the case of mixed-terminated strontium titanate

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 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.

cond-mat.mtrl-sci↗

arXiv2018

Measuring the Local Twist Angle and Layer Arrangement in Van der Waals Heterostructures

The properties of Van der Waals heterostructures are determined by the twist angle and the interface between adjacent layers as well as their polytype and stacking. Here we describe the use of spectroscopic Low Energy Electron Microscopy (LEEM) and micro Low Energy Electron Diffraction (μLEED) methods to measure these properties locally. We present results on a MoS$_{2}$/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, we determine the cleaving history of the MoS$_{2}$ flake, i.e., which layer stems from where in the bulk.

cond-mat.mtrl-sci↗

arXiv2014

Optical tracing of multiple charges in single-electron devices

Single molecules that exhibit narrow optical transitions at cryogenic temperatures can be used as local electric-field sensors. We derive the single charge sensitivity of aromatic organic dye molecules, based on first principles. Through numerical modeling, we demonstrate that by using currently available technologies it is possible to optically detect charging events in a granular network with a sensitivity better than $10^{-5}e/\sqrt{\textrm{Hz}}$ and track positions of multiple electrons, simultaneously, with nanometer spatial resolution. Our results pave the way for minimally-invasive optical inspection of electronic and spintronic nanodevices and building hybrid optoelectronic interfaces that function at both single-photon and single-electron levels.

cond-mat.mes-hall↗

arXiv2011

Observation of Quantum Interference in Molecular Charge Transport

As the dimensions of a conductor approach the nano-scale, quantum effects will begin to dominate its behavior. This entails the exciting possibility of controlling the conductance of a device by direct manipulation of the electron wave function. Such control has been most clearly demonstrated in mesoscopic semiconductor structures at low temperatures. Indeed, the Aharanov-Bohm effect, conductance quantization and universal conductance fluctuations are direct manifestations of the electron wave nature. However, an extension of this concept to more practical emperatures has not been achieved so far. As molecules are nano-scale objects with typical energy level spacings (~eV) much larger than the thermal energy at 300 K (~25 meV), they are natural candidates to enable such a break-through. Fascinating phenomena including giant magnetoresistance, Kondo effects and conductance switching, have previously been demonstrated at the molecular level. Here, we report direct evidence for destructive quantum interference in charge transport through two-terminal molecular junctions at room temperature. Furthermore, we show that the degree of interference can be controlled by simple chemical modifications of the molecule. Not only does this provide the experimental demonstration of a new phenomenon in quantum charge transport, it also opens the road for a new type of molecular devices based on chemical or electrostatic control of quantum interference.

cond-mat.mes-hall↗

arXiv2011

Opportunities and limitations of transition voltage spectroscopy: a theoretical analysis

In molecular charge transport, transition voltage spectroscopy (TVS) holds the promise that molecular energy levels can be explored at bias voltages lower than required for resonant tunneling. We investigate the theoretical basis of this novel tool, using a generic model. In particular, we study the length dependence of the conducting frontier orbital and of the 'transition voltage' as a function of length. We show that this dependence is influenced by the amount of screening of the electrons in the molecule, which determines the voltage drop to be located at the contacts or across the entire molecule. We observe that the transition voltage depends significantly on the length, but that the ratio between the transition voltage and the conducting frontier orbital is approximately constant only in strongly screening (conjugated) molecules. Uncertainty about the screening within a molecule thus limits the predictive power of TVS. We furthermore argue that the relative length independence of the transition voltage for non-conjugated chains is due to strong localization of the frontier orbitals on the end groups ensuring binding of the rods to the metallic contacts. Finally, we investigate the characteristics of TVS in asymmetric molecular junctions. If a single level dominates the transport properties, TVS can provide a good estimate for both the level position and the degree of junction asymmetry. If more levels are involved the applicability of TVS becomes limited.

cond-mat.mes-hall↗

arXiv2011

Charge transport in a single superconducting tin nanowire encapsulated in a multiwalled carbon nanotube

The charge transport properties of single superconducting tin nanowires, encapsulated by multiwalled carbon nanotubes have been investigated by multi-probe measurements. The multiwalled carbon nanotube protects the tin nanowire from oxidation and shape fragmentation and therefore allows us to investigate the electronic properties of stable wires with diameters as small as 25 nm. The transparency of the contact between the Ti/Au electrode and nanowire can be tuned by argonion etching the multiwalled nanotube. Application of a large electrical current results in local heating at the contact which in turn suppresses superconductivity.

cond-mat.mes-hall↗

arXiv2007

Feedback controlled electromigration in four-terminal nano-junctions

We have developed a fast, yet highly reproducible method to fabricate metallic electrodes with nanometer separation using electromigration (EM). We employ four-terminal instead of two-terminal devices in combination with an analog feedback to maintain the voltage $U$ over the junction constant. After the initialization phase ($U < 0.2V), during which the temperature $T$ increases by 80-150 degs C, EM sets in shrinking the wire locally. This quickly leads to a transition from the diffusive to a quasi-ballistic regime ($0.2V < U < 0.6V). At the end of this second regime, a gap forms (U > 0.6V). Remarkably, controlled electromigration is still possible in the quasi-ballistic regime.

cond-mat.mes-hall↗