arXiv subjects

Johan Verbeeck

Publications and source records attributed to Johan Verbeeck.

At least 19 recordsLinked to original sources

arXiv2026

Navigating the Landscape of Hierarchical Multi-Component Strategies: GPC, DOOR, and MOST

There is a growing recognition of the importance to involve patients in every stage of drug development. This shift acknowledges that patients' perspectives, experiences, and preferences are essential for ensuring that treatments meet real-world needs. In this context, a new body of statistical literature has emerged, focusing not only on the simultaneous consideration of multiple outcomes that reflect patients' overall experiences, but also on their structured prioritization. We refer to this class of approaches as hierarchical multi-component statistical methods. Among these, two influential frameworks - generalized pairwise comparisons (GPC) and desirability of outcome ranking (DOOR) - have emerged in the last decade, each aiming to offer a comprehensive approach to evaluating treatment effects. A new methodology, referred to here as the Markov ordinal state transition model (MOST), has recently been introduced without focusing on an explicit link with GPC nor DOOR. This paper seeks to fill this gap by offering a comprehensive and comparative analysis of the three approaches. Through examples and an exploration of the structural and philosophical differences between the methods, our aim is to provide guidance and encourage lines of research in the rapidly-evolving landscape of hierarchical multi-component statistical methodologies.

stat.ME↗

arXiv2026

A 4D-STEM Tomographic Framework Assisted by Object Tracking for Nanoparticle Structure Determination

Three-dimensional electron diffraction (3D ED) has emerged as a powerful method for solving the structures of sub-micron-sized particles down to nanoparticles. However, it faces technical challenges when applied to beam-sensitive samples or agglomerated nanoparticles. This study presents a novel approach that combines 4D-STEM tomography with object tracking and segmentation algorithms to overcome these limitations and achieve single-crystalline 3D ED datasets from nanopowder samples. The method and data quality are assessed on brookite TiO2 nanorods and beam-sensitive CsPbBr3 nanoparticles. To finely sample the reciprocal-space, the data acquisition was automated to acquire hundreds of 4D-STEM scans at fine tilt steps using a slightly convergent beam (0.6 to 1 mrad). Compared to conventional 3D ED methodologies, the proposed method provides enhanced signal-to-noise ratio, low illumination time for reducing beam damage, and the ability to analyze multiple particles from a single tomographic dataset. The procedure is optimized to be feasible using commercially available desktops and detectors. This extends the method applicability to systems and samples that were very challenging for conventional 3D ED methods, by eliminating several technical challenges for the data acquisition.

physics.ins-det↗

arXiv2025

Secondary electron topographical contrast formation in scanning transmission electron microscopy

Secondary electron (SE) imaging offers a powerful complementary capabilities to conventional scanning transmission electron microscopy (STEM) by providing surface-sensitive, pseudo-3D topographic information. However, contrast interpretation of such images remains empirical due to complex interactions of emitted SE with the magnetic field in the objective field of TEM. Here, we propose an analytical physical model that takes into account the physics of SE emission and interaction of the emitted SEs with magnetic field. This enables more reliable image interpretation and potentially lay the foundation for novel 3D surface reconstruction algorithms.

physics.app-ph↗

arXiv2025

Sub-unit cell engineering of CrVO$_3$ superlattice thin films

Ordered corundum oxides introduce new prospects in the field of functional oxides thin films, complementing the more widely studied class of ABO$_3$ perovskites. In this work, we take advantage of the layer-by-layer growth regime to fabricate epitaxial CrVO$_3$ superlattice thin films with atomic-scale accuracy on the periodic arrangement of Cr and V layers. By means of X-ray diffraction, scanning transmission electron microscopy and Raman spectroscopy, we confirm the thickness control in the sub-unit cell scale, alternating 3, 2 or 1 single atomic layers of Cr$_2$O$_3$ and V$_2$O$_3$. For the first time, we stabilize the ilmenite phase of CrVO$_3$ (space group R-3) and compare the functional properties of the thin film with those calculated by density functional theory. This novel approach to the growth of ordered corundum oxides opens the path towards the stabilization of new complex oxides with tailored properties by varying the composition and the superlattice period, ultimately broadening the family of functional rhombohedral oxides.

cond-mat.mtrl-sci↗

arXiv2025

Roadmap for Quantum Nanophotonics with Free Electrons

Over the past century, continuous advancements in electron microscopy have enabled the synthesis, control, and characterization of high-quality free-electron beams. These probes carry an evanescent electromagnetic field that can drive localized excitations and provide high-resolution information on material structures and their optical responses, currently reaching the sub-{\aa}ngstr\"om and few-meV regime. Moreover, combining free electrons with pulsed light sources in ultrafast electron microscopy adds temporal resolution in the sub-femtosecond range while offering enhanced control of the electron wave function. Beyond their exceptional capabilities for time-resolved spectromicroscopy, free electrons are emerging as powerful tools in quantum nanophotonics, on par with photons in their ability to carry and transfer quantum information, create entanglement within and with a specimen, and reveal previously inaccessible details on nanoscale quantum phenomena. This Roadmap outlines the current state of this rapidly evolving field, highlights key challenges and opportunities, and discusses future directions through a collection of topical sections prepared by leading experts.

cond-mat.mes-hall↗

arXiv2024

Edge-Detected 4DSTEM -- effective low-dose diffraction data acquisition method for nanopowder samples in a SEM instrument

The appearance of direct electron detectors marked a new era for electron diffraction. Their high sensitivity and low noise opens the possibility to extend electron diffraction from transmission electron microscopes (TEM) to lower energies such as those found in commercial scanning electron microscopes (SEM).The lower acceleration voltage does however put constraints on the maximum sample thickness and it is a-priori unclear how useful such a diffraction setup could be. On the other hand, nanoparticles are increasingly appearing in consumer products and could form an attractive class of naturally thin samples to investigate with this setup.In this work we present such a diffraction setup and discuss methods to effectively collect and process diffraction data from dispersed crystalline nanoparticles in a commercial SEM instrument. We discuss ways to drastically reduce acquisition time while at the same time lowering beam damage and contamination issues as well as providing significant data reduction leading to fast processing and modest data storage needs. These approaches are also amenable to TEM and could be especially useful in the case of beam-sensitive objects.

physics.app-ph↗

arXiv2024

Coexistence of high electron-mobility, unpaired spins, and superconductivity at high carrier density SrTiO$_3$-based interfaces

The $t_{2g}$ band-structure of SrTiO$_3$-based two-dimensional electron gasses (2DEGs), have been found to play a role in features such as the superconducting dome, high-mobility transport, and the magnitude of spin-orbit coupling. This adds to the already very diverse range of phenomena, including magnetism and extreme magnetoresistance, exhibited by this particular material platform. Tuning and/or combining these intriguing attributes could yield significant progress within quantum and spintronics technologies. Doing so demands precise control of the parameters, which requires a better understanding of the factors that affect them. Here we present effects of the $t_{2g}$ band-order inversion, stemming from the growth of spinel-structured $\gamma$-Al$_2$O$_3$ onto perovskite SrTiO$_3$. Electronic transport measurements show that with LaAlO$_3$/SrTiO$_3$ as the reference, the carrier density and electron mobility are enhanced, and the sample displays a reshaping of the superconducting dome. Additionally, unpaired spins are evidenced by increasing Anomalous Hall Effect with decreasing temperature, entering the same temperature range as the superconducting transition, and a Kondo-like upturn in the sheet resistance. Finally, it is argued that the high-mobility $d_{xz/yz}$-band is more likely than the $d_{xy}$-band to host the supercurrent.

cond-mat.mtrl-sci↗

arXiv2024

Improving the Accuracy of Temperature Measurement on TEM samples using Plasmon Energy Expansion Thermometry (PEET): Addressing Sample Thickness Effects

Advances in analytical scanning transmission electron microscopy (STEM) and microelectronic mechanical systems (MEMS) based microheaters have enabled in-situ materials characterization at the nanometer scale at elevated temperature. In addition to resolving the structural information at elevated temperatures, detailed knowledge of the local temperature distribution inside the sample is essential to reveal thermally induced phenomena and processes. Here, we investigate the accuracy of plasmon energy expansion thermometry (PEET) as a method to map the local temperature in a tungsten (W) lamella in a range between room temperature and 700 degC. In particular, we address the influence of sample thickness in the range of a typical electron-transparent TEM sample (from 30 nm to 70 nm) on the temperature-dependent plasmon energy. The shift in plasmon energy, used to determine the local sample temperature, is not only temperature-dependent, but in case of W also thickness-dependent in sample thicknesses below approximately 60 nm. The results highlight the importance of considering sample thickness (and especially thickness variations) when analyzing the local bulk plasmon energy for temperature measurement using PEET. However, in case of W, an increasing beam broadening (FWHM) of the bulk plasmon peak with decreasing sample thickness can be used to improve the accuracy of PEET in TEM lamellae with varying sample thickness.

cond-mat.mtrl-sci↗

arXiv2024

Automated detection and mapping of crystal tilt using thermal diffuse scattering in transmission electron microscopy

Quantitative interpretation of transmission electron microscopy (TEM) data of crystalline specimens often requires the accurate knowledge of the local crystal orientation. A method is presented which exploits momentum-resolved scanning TEM (STEM) data to determine the local mistilt from a major zone axis. It is based on a geometric analysis of Kikuchi bands within a single diffraction pattern, yielding the centre of the Laue circle. Whereas the approach is not limited to convergent illumination, it is here developed using unit-cell averaged diffraction patterns corresponding to high-resolution STEM settings. In simulation studies, an accuracy of approximately 0.1mrad is found. The method is implemented in automated software and applied to crystallographic tilt and in-plane rotation mapping in two experimental cases. In particular, orientation maps of high-Mn steel and an epitaxially grown La$_{\text{0.7}}$Sr$_{\text{0.3}}$MnO$_{\text{3}}$-SrTiO$_{\text{3}}$ interface are presented. The results confirm the estimates of the simulation study and indicate that tilt mapping can be performed consistently over a wide field of view with diameters well above 100nm at unit cell real space sampling.

cond-mat.mtrl-sci↗

arXiv2024

Unveiling the 3D Morphology of Epitaxial GaAs/AlGaAs Quantum Dots

Strain-free GaAs/AlGaAs semiconductor quantum dots (QDs) grown by droplet etching and nanohole infilling (DENI) are highly promising candidates for the on-demand generation of indistinguishable and entangled photon sources. The spectroscopic fingerprint and quantum optical properties of QDs are significantly influenced by their morphology. The effects of nanohole geometry and infilled material on the exciton binding energies and fine structure splitting are well understood. However, a comprehensive understanding of GaAs/AlGaAs QD morphology remains elusive. To address this, we employ high-resolution scanning transmission electron microscopy (STEM) and reverse engineering through selective chemical etching and atomic force microscopy (AFM). Cross-sectional STEM of uncapped QDs reveals an inverted conical nanohole with Al-rich sidewalls and defect-free interfaces. Subsequent selective chemical etching and AFM measurements further reveal asymmetries in element distribution. This study enhances the understanding of DENI QD morphology and provides a fundamental three-dimensional structural model for simulating and optimizing their optoelectronic properties.

quant-ph↗

arXiv2024

Relativistic EELS scattering cross-sections for microanalysis based on Dirac solutions

The rich information of electron energy-loss spectroscopy (EELS) comes from the complex inelastic scattering process whereby fast electrons transfer energy and momentum to atoms, exciting bound electrons from their ground states to higher unoccupied states. To quantify EELS, the common practice is to compare the cross-sections integrated within an energy window or fit the observed spectrum with theoretical differential cross-sections calculated from a generalized oscillator strength (GOS) database with experimental parameters. The previous Hartree-Fock-based and DFT-based GOS are calculated from Schr\"odinger's solution of atomic orbitals, which does not include the full relativistic effects. Here, we attempt to go beyond the limitations of the Schr\"odinger solution in the GOS tabulation by including the full relativistic effects using the Dirac equation within the local density approximation, which is particularly important for core-shell electrons of heavy elements with strong spin-orbit coupling. This has been done for all elements in the periodic table (up to Z = 118) for all possible excitation edges using modern computing capabilities and parallelization algorithms. The relativistic effects of fast incoming electrons were included to calculate cross-sections that are specific to the acceleration voltage. We make these tabulated GOS available under an open-source license to the benefit of both academic users as well as allowing integration into commercial solutions.

physics.atom-ph↗

arXiv2023

Imaging the suppression of ferromagnetism in LaMnO$_3$ by metallic overlayers

LaMnO$_3$ (LMO) thin films epitaxially grown on SrTiO$_3$ (STO) usually exhibit ferromagnetism above a critical layer thickness. We report the use of scanning SQUID microscopy (SSM) to study the suppression of the ferromagnetism in STO/LMO/metal structures. By partially covering the LMO surface with a metallic layer, both covered and uncovered LMO regions can be studied simultaneously. While Au does not significantly influence the ferromagnetic order of the underlying LMO film, a thin Ti layer induces a strong suppression of the ferromagnetism, over tens of nanometers, which increases with time on a timescale of days. Detailed EELS analysis of the Ti-LaMnO$_3$ interface reveals \textcolor{black}{the presence of Mn$^{2+}$ and} an evolution of the Ti valence state from Ti$^0$ to Ti$^{4+}$ over approximately 5 nanometers. Furthermore, we demonstrate that by patterning Ti/Au overlayers, we can locally suppress the ferromagnetism and define ferromagnetic structures down to sub-micrometer scales.

cond-mat.mtrl-sci↗

arXiv2023

Quantum Wavefront Shaping with a 48-element Programmable Phase Plate for Electrons

We present a 48-element programmable phase plate for coherent electron waves produced by a combination of photolithography and focused ion beam. This brings the highly successful concept of wavefront shaping from light optics into the realm of electron optics and provides an important new degree of freedom to prepare electron quantum states. The phase plate chip is mounted on an aperture rod placed in the C2 plane of a transmission electron microscope operating in the 100-300 kV range. The phase plate's behavior is characterized by a Gerchberg-Saxton algorithm, showing a phase sensitivity of 0.075rad/mV at 300kV, with a phase resolution of approximately $3\cdot10^{-3}\pi$. In addition, we provide a brief overview of possible use cases and support it with both simulated and experimental results.

physics.ins-det↗

arXiv2023

Pattern Formation by Electric-field Quench in Mott Crystal

The control of Mott phase is intertwined with the spatial reorganization of the electronic states. Out-of-equilibrium driving forces typically lead to electronic patterns that are absent at equilibrium, whose nature is however often elusive. Here, we unveil a nanoscale pattern formation in the Ca$_2$RuO$_4$ Mott insulator. We demonstrate how an applied electric field spatially reconstructs the insulating phase that, uniquely after switching off the electric field, exhibits nanoscale stripe domains. The stripe pattern has regions with inequivalent octahedral distortions that we directly observe through high-resolution scanning transmission electron microscopy. The nanotexture depends on the orientation of the electric field, it is non-volatile and rewritable. We theoretically simulate the charge and orbital reconstruction induced by a quench dynamics of the applied electric field providing clear-cut mechanisms for the stripe phase formation. Our results open the path for the design of non-volatile electronics based on voltage-controlled nanometric phases.

cond-mat.str-el↗

arXiv2022

High-strain-induced local modification of the electronic properties of VO$_2$ thin films

Vanadium dioxide (VO2) is a popular candidate for electronic and optical switching applications due to its well-known semiconductor-metal transition. Its study is notoriously challenging due to the interplay of long and short range elastic distortions, as well as the symmetry change, and the electronic structure changes. The inherent coupling of lattice and electronic degrees of freedom opens the avenue towards mechanical actuation of single domains. In this work, we show that we can manipulate and monitor the reversible semiconductor-to-metal transition of VO2 while applying a controlled amount of mechanical pressure by a nanosized metallic probe using an atomic force microscope. At a critical pressure, we can reversibly actuate the phase transition with a large modulation of the conductivity. Direct tunneling through the VO2-metal contact is observed as the main charge carrier injection mechanism before and after the phase transition of VO2. The tunneling barrier is formed by a very thin but persistently insulating surfacelayer of the VO2. The necessary pressure to induce the transition decreases with temperature. In addition, we measured the phase coexistence line in a hitherto unexplored regime. Our study provides valuable information on pressure-induced electronic modifications of the VO2 properties, as well as on nanoscale metal-oxide contacts, which can help in the future design of oxide electronics.

cond-mat.mtrl-sci↗

arXiv2022

Can a Programmable Phase Plate Serve as an Aberration Corrector in the Transmission Electron Microscope (TEM)?

Current progress in programmable electrostatic phase plates raises questions about their usefulness for specific applications. Here, we explore different designs for such phase plates with the specific goal of correcting spherical aberration in the Transmission Electron Microscope (TEM). We numerically investigate whether a phase plate could provide down to 1 $\r{A}$ngstr\"om spatial resolution on a conventional uncorrected TEM. Different design aspects (fill-factor, pixel pattern, symmetry) were evaluated to understand their effect on the electron probe size and current density. Some proposed designs show a probe size ($d_{50}$) down to 0.66$\r{A}$, proving that it should be possible to correct spherical aberration well past the 1\AA~ limit using a programmable phase plate consisting of an array of electrostatic phase shifting elements.

physics.app-ph↗

arXiv2021

Real Time Integration Centre of Mass (riCOM) Reconstruction for 4D-STEM

A real-time image reconstruction method for scanning transmission electron microscopy (STEM) is proposed. With an algorithm requiring only the center of mass (COM) of the diffraction pattern at one probe position at a time, it is able to update the resulting image each time a new probe position is visited without storing any intermediate diffraction patterns. The results show clear features at higher spatial frequency, such as atomic column positions. It is also demonstrated that some common post processing methods, such as band pass filtering, can be directly integrated in the real time processing flow. Compared with other reconstruction methods, the proposed method produces high quality reconstructions with good noise robustness at extremely low memory and computational requirements. An efficient, interactive open source implementation of the concept is further presented, which is compatible with frame-based, as well as event-based camera/file types. This method provides the attractive feature of immediate feedback that microscope operators have become used to, e.g. conventional high angle annular dark field STEM imaging, allowing for rapid decision making and fine tuning to obtain the best possible images for beam sensitive samples at the lowest possible dose.

cond-mat.mtrl-sci↗

arXiv2021

Reducing electron beam damage through alternative STEM scanning strategies. Part I -- Experimental findings

The highly energetic electrons in a transmission electron microscope (TEM) can alter or even completely destroy the structure of samples before sufficient information can be obtained. This is especially problematic in the case of zeolites, organic and biological materials. As this effect depends on both the electron beam and the sample and can involve multiple damage pathways, its study remained difficult and is plagued with irreproducibity issues, circumstantial evidence, rumours, and a general lack of solid data. Here we take on the experimental challenge to investigate the role of the STEM scan pattern on the damage behaviour of a commercially available zeolite sample with the clear aim to make our observations as reproducible as possible. We make use of a freely programmable scan engine that gives full control over the tempospatial distribution of the electron probe on the sample and we use its flexibility to obtain mutliple repeated experiments under identical conditions comparing the difference in beam damage between a conventional raster scan pattern and a newly proposed interleaved scan pattern that provides exactly the same dose and dose rate and visits exactly the same scan points. We observe a significant difference in beam damage for both patterns with up to 11 % reduction in damage (measured from mass loss). These observations demonstrate without doubt that electron dose, dose rate and acceleration voltage are not the only parameters affecting beam damage in (S)TEM experiments and invite the community to rethink beam damage as an unavoidable consequence of applied electron dose.

cond-mat.mtrl-sci↗