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In this paper convexity constraints are derived for a background model of electron energy loss spectra (EELS) that is linear in the fitting parameters. The model outperforms a power-law both on experimental and simulated backgrounds, especially for wide energy ranges, and thus improves elemental quantification results. Owing to the model's linearity, the constraints can be imposed through fitting by quadratic programming. This has important advantages over conventional nonlinear power-law fitting such as high speed and a guaranteed unique solution without need for initial parameters. As such, the need for user input is significantly reduced, which is essential for unsupervised treatment of large data sets. This is demonstrated on a demanding spectrum image of a semiconductor device sample with a high number of elements over a wide energy range., Comment: Updated version

Microplasmas can be used for a wide range of technological applications and to improve our understanding of fundamental physics. Scanning electron microscopy, on the other hand, provides insights into the sample morphology and chemistry of materials from the mm-down to the nm-scale. Combining both would provide direct insight into plasma-sample interactions in real-time and at high spatial resolution. Up till now, very few attempts in this direction have been made, and significant challenges remain. This work presents a stable direct current glow discharge microplasma setup built inside a scanning electron microscope. The experimental setup is capable of real-time in-situ imaging of the sample evolution during plasma operation and it demonstrates localized sputtering and sample oxidation. Further, the experimental parameters such as varying gas mixtures, electrode polarity, and field strength are explored and experimental $V$-$I$ curves under various conditions are provided. These results demonstrate the capabilities of this setup in potential investigations of plasma physics, plasma-surface interactions, and materials science and its practical applications. The presented setup shows the potential to have several technological applications, e.g., to locally modify the sample surface (e.g., local oxidation and ion implantation for nanotechnology applications) on the $\mu$m-scale., Comment: LG, DC, and RDM contributed equally to this work. The videos mentioned in the manuscript can be found in the Zenodo repository linked in the paper

We present a detailed atomistic picture of the oxidation mechanism of Co nanoparticles and its impact on magnetism by experimentally following the evolution of the structure, chemical composition, and magnetism of individual, gas-phase grown Co nanoparticles during controlled oxidation. The early stage oxidation occurs in a twostep process characterized by (i) the initial formation of small CoO crystallites randomly distributed across the nanoparticle surface, until their coalescence leads to structural completion of the oxide shell and passivation of the metallic core; (ii) progressive conversion of the CoO shell to Co3O4, accompanied by void formation due to the nanoscale Kirkendall effect. The Co nanoparticles remain highly reactive toward oxygen during phase (i), demonstrating the absence of a pressure gap whereby a low reactivity at low pressures is postulated. Our results provide an important benchmark for an improved understanding of the magnetism of oxidized cobalt nanoparticles, with potential implications on their performance in catalytic reactions., Comment: 34 pages, 5 figures

In this study we explore the possibility to use deep learning for the reconstruction of phase images from 4D scanning transmission electron microscopy (4D-STEM) data. The process can be divided into two main steps. First, the complex electron wave function is recovered for a convergent beam electron diffraction pattern (CBED) using a convolutional neural network (CNN). Subsequently a corresponding patch of the phase object is recovered using the phase object approximation (POA). Repeating this for each scan position in a 4D-STEM dataset and combining the patches by complex summation yields the full phase object. Each patch is recovered from a kernel of 3x3 adjacent CBEDs only, which eliminates common, large memory requirements and enables live processing during an experiment. The machine learning pipeline, data generation and the reconstruction algorithm are presented. We demonstrate that the CNN can retrieve phase information beyond the aperture angle, enabling super-resolution imaging. The image contrast formation is evaluated showing a dependence on thickness and atomic column type. Columns containing light and heavy elements can be imaged simultaneously and are distinguishable. The combination of super-resolution, good noise robustness and intuitive image contrast characteristics makes the approach unique among live imaging methods in 4D-STEM.

Four dimensional scanning transmission electron microscopy (4D STEM) records the scattering of electrons in a material in great detail. The benefits offered by 4D STEM are substantial, with the wealth of data it provides facilitating for instance high precision, high electron dose efficiency phase imaging via center of mass or ptychography based analysis. However the requirement for a 2D image of the scattering to be recorded at each probe position has long placed a severe bottleneck on the speed at which 4D STEM can be performed. Recent advances in camera technology have greatly reduced this bottleneck, with the detection efficiency of direct electron detectors being especially well suited to the technique. However even the fastest frame driven pixelated detectors still significantly limit the scan speed which can be used in 4D STEM, making the resulting data susceptible to drift and hampering its use for low dose beam sensitive applications. Here we report the development of the use of an event driven Timepix3 direct electron camera that allows us to overcome this bottleneck and achieve 4D STEM dwell times down to 100~ns; orders of magnitude faster than what has been possible with frame based readout. We characterise the detector for different acceleration voltages and show that the method is especially well suited for low dose imaging and promises rich datasets without compromising dwell time when compared to conventional STEM imaging.

Electron tomography is a widely used experimental technique for analyzing nanometer-scale structures of a large variety of materials in three dimensions. Unfortunately, the acquisition of conventional electron tomography tilt series can easily take up one hour or more, depending on the complexity of the experiment. Using electron tomography, it is therefore far from straightforward to obtain statistically meaningful 3D data, to investigate samples that do not withstand long acquisition, or to perform in situ 3D characterization using this technique. Various acquisition strategies have been proposed to accelerate the tomographic acquisition, and reduce the required electron dose. These methods include tilting the holder continuously while acquiring a projection movie and a hybrid, incremental, methodology which combines the benefits of the conventional and continuous technique. In this paper, the different acquisition strategies will be experimentally compared in terms of speed, resolution and electron dose, based on experimental tilt series acquired for various metallic nanoparticles.

Laser-induced manipulation of magnetism at the nanoscale is a rapidly growing research topic with potential for applications in spintronics. In this work, we address the role of the scattering cross section, thermal effects, and laser fluence on the magnetic, structural, and chemical stability of individual magnetic nanoparticles excited by single femtosecond laser pulses. We find that the energy transfer from the fs laser pulse to the nanoparticles is limited by the Rayleigh scattering cross section, which in combination with the light absorption of the supporting substrate and protective layers determines the increase in the nanoparticle temperature. We investigate individual Co nanoparticles (8 to 20 nm in size) as a prototypical model system, using x-ray photoemission electron microscopy and scanning electron microscopy upon excitation with single femtosecond laser pulses of varying intensity and polarization. In agreement with calculations, we find no deterministic or stochastic reversal of the magnetization in the nanoparticles up to intensities where ultrafast demagnetization or all-optical switching is typically reported in thin films. Instead, at higher fluences, the laser pulse excitation leads to photo-chemical reactions of the nanoparticles with the protective layer, which results in an irreversible change in the magnetic properties. Based on our findings, we discuss the conditions required for achieving laser-induced switching in isolated nanomagnets., Comment: 36 pages, 7 figures

We report charge-transfer up to a single electron per interfacial unit cell across non-polar heterointerfaces from the Mott insulator LaTiO3 to the charge transfer insulator LaCoO3. In high-quality bi- and tri-layer systems grown using pulsed laser deposition, soft X-ray absorption, dichroism and STEM-EELS are used to probe the cobalt 3d-electron count and provide an element-specific investigation of the magnetic properties. The experiments prove a deterministically-tunable charge transfer process acting in the LaCoO3 within three unit cells of the heterointerface, able to generate full conversion to 3d7 divalent Co, which displays a paramagnetic ground state. The number of LaTiO3 / LaCoO3 interfaces, the thickness of an additional "break" layer between the LaTiO3 and LaCoO3, and the LaCoO3 film thickness itself in tri-layers provide a trio of sensitive control knobs for the charge transfer process, illustrating the efficacy of O2p-band alignment as a guiding principle for property design in complex oxide heterointerfaces.

A topological insulating phase has theoretically been predicted for the thermodynamically unstable perovskite phase of YBiO$_{3}$. Here, it is shown that the crystal structure of the Y-Bi-O system can be controlled by using a BaBiO$_{3}$ buffer layer. The BaBiO$_{3}$ film overcomes the large lattice mismatch of 12% with the SrTiO$_{3}$ substrate by forming a rocksalt structure in between the two perovskite structures. Depositing an YBiO$_{3}$ film directly on a SrTiO$_{3}$ substrate gives a fluorite structure. However, when the Y-Bi-O system is deposited on top of the buffer layer with the correct crystal phase and comparable lattice constant, a single oriented perovskite structure with the expected lattice constants is observed., Comment: 8 pages, 7 figures + 4 pages supporting information

Strain has a strong effect on the properties of materials and the performance of electronic devices. Their ever shrinking size translates into a constant demand for accurate and precise measurement methods with very high spatial resolution. In this regard, transmission electron microscopes are key instruments thanks to their ability to map strain with sub-nanometer resolution. Here we present a novel method to measure strain at the nanometer scale based on the diffraction of electron Bessel beams. We demonstrate that our method offers a strain sensitivity better than $2.5 \cdot 10^{-4}$ and an accuracy of $1.5 \cdot 10^{-3}$, competing with, or outperforming, the best existing methods with a simple and easy to use experimental setup., Comment: This article may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing. This article appeared in Appl. Phys. Lett. 114, 243501 (2019) and may be found at https://aip.scitation.org/doi/abs/10.1063/1.5096245 Data available at: https://doi.org/10.5281/zenodo.2566137 and code available at: https://bitbucket.org/lutosensis/tem-thesis/src

We report on the fabrication of conducting interfaces between LaAlO$_3$ and SrTiO$_3$ by 90$^o$ off-axis sputtering in an Ar atmosphere. At a growth pressure of 0.04 mbar the interface is metallic, with a carrier density of the order of $10^{13}$ cm$^{-2}$ at 3 K. By increasing the growth pressure, we observe an increase of the out-of-plane lattice constants of the LaAlO$_3$ films while the in-plane lattice constants do not change. Also, the low-temperature sheet resistance increases with increasing growth pressure, leading to an insulating interface when the growth pressure reaches 0.10 mbar. We attribute the structural variations to an increase of the La/Al ratio, which also explains the transition from metallic behavior to insulating behavior of the interfaces. Our research emphasizes the key role of the cation stoichiometry of LaAlO$_3$ in the formation of the conducting interface, and also the control which is furnished by the Ar pressure in the growth process., Comment: 4 pages, 4 figures; manuscript under review

First results on the experimental realisation of a 2x2 programmable phase plate for electrons are presented. The design consists of an array of electrostatic einzel lenses that influence the phase of electron waves passing through 4 separately controllable aperture holes. This functionality is demonstrated in a conventional transmission electron microscope operating at 300~kV and results are in very close agreement with theoretical predictions. The dynamic creation of a set of electron probes with different phase symmetry is demonstrated, thereby bringing adaptive optics in TEM one step closer to reality. The limitations of the current design and how to overcome these in the future are discussed. Simulations show how further evolved versions of the current proof of concept might open new and exciting application prospects for beam shaping and aberration correction.

A technique to measure the band gap of dielectric materials with high refractive index by means of energy electron loss spectroscopy (EELS) is presented. The technique relies on the use of a circular (Bessel) aperture and suppresses Cherenkov losses and surface-guided light modes by enforcing a momentum transfer selection. The technique also strongly suppresses the elastic zero loss peak, making the acquisition, interpretation and signal to noise ratio of low loss spectra considerably better, especially for excitations in the first few eV of the EELS spectrum. Simulations of the low loss inelastic electron scattering probabilities demonstrate the beneficial influence of the Bessel aperture in this setup even for high accelerating voltages. The importance of selecting the optimal experimental convergence and collection angles is highlighted. The effect of the created off-axis acquisition conditions on the selection of the transitions from valence to conduction bands is discussed in detail on a simplified isotropic two band model. This opens the opportunity for deliberately selecting certain transitions by carefully tuning the microscope parameters. The suggested approach is experimentally demonstrated and provides good signal to noise ratio and interpretable band gap signals on reference samples of diamond, GaN and AlN while offering spatial resolution in the nm range., Comment: 17 pages, 6 figures

Magnetic nanoparticles are important building blocks for future technologies ranging from nano-medicine to spintronics. Many related applications require nanoparticles with tailored magnetic properties. However, despite significant efforts undertaken towards this goal, a broad and poorly-understood dispersion of magnetic properties is reported, even within mono-disperse samples of the canonical ferromagnetic 3d transition metals. We address this issue by investigating the magnetism of a large number of size- and shape-selected, individual nanoparticles of Fe, Co, and Ni using a unique set of complementary characterization techniques. At room temperature only superparamagnetic behavior is observed in our experiments for all Ni nanoparticles within the investigated sizes, which range from 8 to 20 nm. However, Fe and Co nanoparticles can exist in two distinct magnetic states at any size in this range: (i) a superparamagnetic state as expected from the bulk and surface anisotropies known for the respective materials and as observed for Ni; and (ii) a state with unexpected stable magnetization at room temperature. This striking state is assigned to significant modifications of the magnetic properties arising from metastable lattice defects in the core of the nanoparticles as concluded by calculations and atomic structural characterization. Also related with the structural defects, we find that the magnetic state of Fe and Co nanoparticles can be tuned by thermal treatment enabling one to tailor their magnetic properties for applications. This work demonstrates the importance of complementary single particle investigations for a better understanding of nanoparticle magnetism and for full exploration of their potential for applications., Comment: 38 pages, 6 figures, Supplementary Material

Plasmonics, the science and technology of the interaction of light with metallic objects, is fundamentally changing the way we can detect, generate and manipulate light. Although the field is progressing swiftly, thanks to the availability of nanoscale manufacturing and analysis methods, fundamental properties such as the plasmonic excitations' symmetries cannot be accessed directly, leading to a partial, sometimes incorrect, understanding of their properties. Here we overcome this limitation by deliberately shaping the wave function of an electron beam to match a plasmonic excitations' symmetry in a modified transmission electron microscope. We show experimentally and theoretically that this offers selective detection of specific plasmon modes within metallic nanoparticles, while excluding modes with other symmetries. This method resembles the widespread use of polarized light for the selective excitation of plasmon modes with the advantage of locally probing the response of individual plasmonic objects and a far wider range of symmetry selection criteria.

Friedel's law states that the modulus of the Fourier transform of real functions is centrosymmetric, while the phase is antisymmetric. As a consequence of this, elastic scattering of plane wave photons or electrons within the first-order Born-approximation as well as Fraunhofer diffraction on any aperture, is bound to result in centrosymmetric diffraction patterns. Friedel's law, however, does not apply for vortex beams, and centrosymmetry in general is not present in their diffraction patterns. In this work we extend Friedel's law for vortex beams by showing that the diffraction patterns of vortex beams with opposite topological charge, scattered on the same two dimensional potential, always are centrosymmetric to one another, regardless of the symmetry of the scattering object. We verify our statement by means of numerical simulations and experimental data. Our research provides deeper understanding in vortex beam diffraction and can be used to design new experiments to measure the topological charge of vortex beams with diffraction gratings, or study general vortex beam diffraction., Comment: 7 pages, 3 figures

Homogeneous highly epitaxial LaSrMnO3 (LSMO) thin films have been grown on Yttria-stabilized-Zirconia (YsZ) / CeO2 buffer layers on technological relevant 4" silicon wafers using a Twente Solid State Technology B.V. (TSST) developed large area Pulsed Laser Deposition (PLD) setup. We study and show the results of the effect of an additional SrRuO3 buffer layer on the growth temperature dependent structural and magnetic properties of LSMO films. With the introduction of a thin SrRuO3 layer on top of the buffer stack, LSMO films show ferromagnetic behaviour for growth temperatures as low as 250C. We suggest that occurrence of epitaxial crystal growth of LSMO at these low growth temperatures can be understood by an improved surface diffusion, which ensures sufficient intermixing of surface species for formation of the correct phase. This intermixing is necessary because the full plume is collected on the 4" wafer resulting in a compositional varying flux of species on the wafer, in contrast to small scale experiments., Comment: 4 pages, 3 figures

The use of phase plates in the back focal plane of a microscope is a well established technique in optical microscopy to increase the contrast of weakly interacting samples and is gaining interest in electron microscopy as well. In this paper we study the spiral phase plate (SPP), also called helical, vortex, or two-dimensional Hilbert phase plate, that adds an angularly dependent phase of the form $e^{i\ell\phi}$ to the exit wave in Fourier space. In the limit of large collection angles, we analytically calculate that the average of a pair of $\ell=\pm1$ SPP images is directly proportional to the gradient squared of the exit wave, explaining the edge contrast previously seen in optical SPP work. The difference between a clockwise-anticlockwise pair of SPP images and conditions where this difference vanishes and the gradient of the exit wave can be seen from one single SPP image, are discussed. Finally, we demonstrate how with three images, one without and one with each of an $\ell=\pm1$ SPP, may give enough information to reconstruct both the amplitude and the phase of the exit wave. This work provides the theoretical background to interpret images obtained with a SPP and can help enable new experiments to study for example magnetic materials in an electron microscope., Comment: 7 pages, 4 figures

The orbital angular momentum (OAM) of light and matter waves is a parameter that is getting increasingly more attention over the past couple of years. Beams with a well defined OAM, the so-called vortex beams, are applied already in e.g. telecommunication, astrophysics, nanomanipulation and chiral measurements in optics and electron microscopy. Also the OAM of a wave induced by the interaction with a sample, shows great potential of interest. In all these experiments it is crucial to measure the exact (local) OAM content of the wave, whether it is an incoming vortex beam or an exit wave after interacting with a sample. In this work we investigate the use of spiral phase plates as an alternative to the programmable phase plates used in optics to measure OAM. We derive analytically how these can be used to study the local OAM components of any wave function. By means of numerical simulations we illustrate how the OAM of a pure vortex beam can be measured. We also look at a sum of misaligned vortex beams and show how using SPPs the position and the OAM of each individual beam can be detected. Finally we look at the OAM induced by a magnetic dipole on a free electron wave and show how the SPP can be used to localize the magnetic poles and measure their "magnetic charge". Although our findings can be applied to study the OAM of any wave function, they are of particular interest for electron microscopy where versatile programmable phase plates do not yet exist., Comment: 7 pages, 5 figures

The concept of compressive sensing was recently proposed to significantly reduce the electron dose in scanning transmission electron microscopy (STEM) while still maintaining the main features in the image. Here, an experimental setup based on an electromagnetic shutter placed in the condenser plane of a STEM is proposed. The shutter blanks the beam following a random pattern while the scanning coils are moving the beam in the usual scan pattern. Experimental images at both medium scale and high resolution are acquired and then reconstructed based on a discrete cosine algorithm. The obtained results confirm the predicted usefulness of compressive sensing in experimental STEM even though some remaining artifacts need to be resolved., Comment: 7 pages, 5 figures

In this work we present an alternative way to look at electron diffraction in a transmission electron microscope. In stead of writing the scattering amplitude in Fourier space as a set of plane waves, we use the cylindrical Fourier transform to describe the scattering amplitude in a basis of orbital angular momentum (OAM) eigenstates. We show how working in this framework can be very convenient when investigating e.g. rotation and screw axis symmetries. For the latter we find selection rules on the OAM-coefficients that unambiguously reveal the handedness of the screw axis. Detecting the OAM-coefficients of the scattering amplitude thus offers the possibility to detect the handedness of crystals without the need for dynamical simulations, the thickness of the sample nor the exact crystal structure. We propose an experimental setup to measure the OAM-components where an image of the crystal is taken after inserting a spiral phase plate in the diffraction plane and perform mulsti-slice simulations on $\alpha$-quartz to demonstrate how the method indeed reveals the chirality. Experimental feasibility of the technique is discussed together with its main advantages with respect to chirality determination of screw axes. The method shows how the use of a spiral phase plate can be extended from a simple phase imaging technique to a tool to measure the local OAM-decomposition of an electron wave, widening the field of interest well beyond chiral space group determination., Comment: 12 pages, 10 figures

In this paper we explore the desirability of a transmission electron microscope in which the phase of the electron wave can be freely controlled. We discuss different existing methods to manipulate the phase of the electron wave and their limitations. We show how with the help of current techniques the electron wave can already be crafted into specific classes of waves each having their own peculiar properties. Assuming a versatile phase modulation device is feasible, we explore possible benefits and methods that could come into existence borrowing from light optics where so-called spatial light modulators provide programmable phase plates for quite some time now. We demonstrate that a fully controllable phase plate building on Harald Rose's legacy in aberration correction and electron optics in general would open an exciting field of research and applications., Comment: 9 pages, 4 figures, special Ultramicroscopy issue for PICO2015 conference

We report the atomic layer deposition of titanium dioxide on carbon nanosheet templates and investigate the effects of post-deposition annealing in a helium environment using different characterization techniques. The crystallization of the titanium dioxide coating upon annealing is observed using in-situ X-ray diffraction. The (micro)-structural characterization of the films is carried out by scanning electron microscopy and advanced transmission electron microscopy techniques. Our study shows that the annealing of the atomic layer deposition processed and carbon nanosheets templated titanium dioxide layers in helium environment results in the formation of a porous, nanocrystalline and photocatalytically active titanium dioxide-carbon nanosheet composite film. Such composites are suitable for photocatalysis and dye-sensitized solar cells applications.

Recent theoretical and experimental developments in the field of electron vortex beam physics have raised questions on what exactly this novelty in the field of electron microscopy (and other fields, such as particle physics) really provides. An important part in the answer to those questions lies in scattering theory. The present investigation explores various aspects of inelastic quantum scattering theory for cylindrically symmetric beams with orbital angular momentum. The model system of Coulomb scattering on a hydrogen atom provides the setting to address various open questions: How is momentum transferred? Do vortex beams selectively excite atoms, and how can one employ vortex beams to detect magnetic transitions? The analytical approach presented here provides answers to these questions. OAM transfer is possible, but not through selective excitation; rather, by pre- and post-selection one can filter out the relevant contributions to a specific signal.

The phase problem can be considered as one of the cornerstones of quantum mechanics intimately connected to the detection process and the uncertainty relation. The latter impose fundamental limits on the manifold phase reconstruction schemes invented to date in particular at small magnitudes of the quantum wave. Here, we show that a rigorous solution of the Transport of Intensity Reconstruction (TIE) scheme in terms of a linear elliptic partial differential equation for the phase provides reconstructions even in the presence of wave zeros if particular boundary conditions (BCs) are given. We furthermore discuss how partial coherence hampers phase reconstruction and show that a modified version of the TIE reconstructs the curl-free current density at arbitrary (in-)coherence. This opens the way for a large variety of new applications in fields as diverse as astrophysics, geophysics, photonics, acoustics, and electron microscopy, where zeros in the respective wave field are a ubiquitous feature., Comment: 5 pages, 3 figures, includes correction as in https://journals.aps.org/prl/abstract/10.1103/PhysRevLett.111.199902

We investigate topological aspects of sub-nm electron vortex beams upon elastic propagation through atomic scattering potentials. Two main aspects can be distinguished: (i) Significantly reduced delocalization compared to a similar non-vortex beam if the beam centers on an atomic column and (ii) site symmetry dependent splitting of higher-order vortex beams. Furthermore, the results provide insight into the complex vortex line fabric within the elastically scattered wave containing characteristic vortex loops predominantly attached to atomic columns and characteristic twists of vortex lines around atomic columns., Comment: 10 pages, 6 figures

We investigate electron vortex beams elastically scattered on chiral crystals. After deriving a general expression for the scattering amplitude of a vortex electron, we study its diffraction on point scatterers arranged on a helix. We derive a relation between the handedness of the helix and the topological charge of the electron vortex on one hand, and the symmetry of the Higher Order Laue Zones in the diffraction pattern on the other for kinematically and dynamically scattered electrons. We then extend this to atoms arranged on a helix as found in crystals which belong to chiral space groups and propose a new method to determine the handedness of such crystals by looking at the symmetry of the diffraction pattern. Contrary to alternative methods, our technique does not require multiple scattering which makes it possible to also investigate extremely thin samples in which multiple scattering is suppressed. In order to verify the model, elastic scattering simulations are performed and an experimental demonstration on Mn$_2$Sb$_2$O$_7$ is given where we find the sample to belong to the right handed variant of its enantiomorphic pair. This demonstrates the usefulness of electron vortex beams to reveal the chirality of crystals in a transmission electron microscope and provides the required theoretical basis for further developments in this field.

In TEM, a typical goal consists of making a small electron probe in the sample plane in order to obtain high spatial resolution in scanning transmission electron microscopy. In order to do so, the phase of the electron wave is corrected to resemble a spherical wave compensating for aberrations in the magnetic lenses. In this contribution we discuss the advantage of changing the phase of an electron wave in a specific way in order to obtain fundamentally different electron probes opening up new application in the (S)TEM. We focus on electron vortex states as a specific family of waves with an azimuthal phase signature and discuss their properties, production and applications. The concepts presented here are rather general and also different classes of probes can be obtained in a similar fashion showing that electron probes can be tuned to optimise a specific measurement or interaction.

The recent demonstration of electron vortex beams has opened up the new possibility of studying orbital angular momentum (OAM) in the interaction between electron beams and matter. To this aim, methods to analyze the OAM of an electron beam are fundamentally important and a necessary next step. We demonstrate the measurement of electron beam OAM through a variety of techniques. The use of forked holographic masks, diffraction from geometric apertures, diffraction from a knife-edge and the application of an astigmatic lens are all experimentally demonstrated. The viability and limitations of each are discussed with supporting numerical simulations., Comment: 5 pages, 4 figurse

By considering a cylindrically symmetric generalization of a plane wave, the first Born approximation of screened Coulomb scattering unfolds two new dimensions in the scattering problem: transverse momentum and orbital angular momentum of the incoming beam. In this paper, the elastic Coulomb scattering amplitude is calculated analytically for incoming Bessel beams. This reveals novel features occurring for wide angle scattering when the incoming beam is correctly prepared. The result successfully generalizes the well known Rutherford formula, incorporating transverse and orbital angular momentum into the formalism., Comment: 9 pages, 5 figures

A \ce{(LaVO_3)_6/(SrVO_3)_3} superlattice is studied with a combination of sub-{\AA} resolved scanning transmission electron microscopy and monochromated electron energy-loss spectroscopy. The V oxidation state is mapped with atomic spatial resolution enabling to investigate electronic reconstruction at the \ce{LaVO_3}/\ce{SrVO_3} interfaces. Surprisingly, asymmetric charge distribution is found at adjacent chemically symmetric interfaces. The local structure is proposed and simulated with double channeling calculation which agrees qualitatively with our experiment. We demonstrate that local strain asymmetry is the likely cause of the electronic asymmetry of the interfaces. The electronic reconstruction at the interfaces extends much further than the chemical composition, varying from 0.5 to 1.2 nm. This distance corresponds to the length of charge transfer previously found in the \ce{(LaVO_3)_m}/\ce{(SrVO_3)_n} metal/insulating and the \ce{(LaAlO_3)_m}/\ce{(SrTiO_3)_n} insulating/insulating interfaces., Comment: 6 pages, 5 figures. Physical Review B, 2013

Kirchhoff's scalar diffraction theory is applied throughout photon and electron optics. It is based on the stationary electromagnetic or Schr\"odinger wave equation, and is useful in describing interference phenomena for both light and matter waves. Here, Kirchhoff's diffraction theory is derived from the relativistic Dirac equation, thus reformulated to work on Dirac spinors. The parallels with the "classic" scalar theory are highlighted, and a basic interpretation of the result obtained for the Fraunhofer diffraction limit is given. The goal of this paper is to emphasize the similarity between the two equations on the most fundamental level.

The recent experimental realization of electron vortex beams opens up a wide research domain previously unexplored. The present paper explores the relativistic properties of these electron vortex beams, and quantifies deviations from scalar wave theory. It is common in electron optics to use the Schr\"odinger equation neglecting spin. The present paper investigates the role of spin and the total angular momentum Jz and how it pertains to the vortex states. As an application, we also investigate if it is possible to use holographic reconstruction to create novel total angular momentum eigenstates in a Transmission Electron Microscope. It is demonstrated that relativistic spin coupling effects disappear in the paraxial limit, and spin effects in holographically created electron vortex beams can only be exploited by using specialized magnetic apertures., Comment: 6 pages, 2 figures

Electron vortex beams carrying intrinsic orbital angular momentum (OAM) are produced in electron microscopes where they are controlled and focused using magnetic lenses. We observe various rotational phenomena arising from the interaction between the OAM and magnetic lenses. First, the Zeeman coupling, proportional to the OAM and magnetic field strength, produces an OAM-independent Larmor rotation of a mode superposition inside the lens. Second, hen passing through the focal plane, the electron beam acquires an additional Gouy phase dependent on the absolute value of the OAM. This brings about the Gouy rotation of the superposition image proportional to the sign of the OAM. A combination of the Larmor and Gouy effects can result in the addition (or subtraction) of rotations, depending on the OAM sign. This behaviour is unique to electron vortex beams and has no optical counterpart, as Larmor rotation occurs only for charged particles. Our experimental results are in agreement with recent theoretical predictions., Comment: 5 pages, 5 figures

We examine the propagation of the recently-discovered electron vortex beams in a longitudinal magnetic field. We consider both the Aharonov-Bohm configuration with a single flux line and the Landau case of a uniform magnetic field. While stationary Aharonov-Bohm modes represent Bessel beams with flux- and vortex-dependent probability distributions, stationary Landau states manifest themselves as non-diffracting Laguerre-Gaussian beams. Furthermore, the Landau-state beams possess field- and vortex-dependent phases: (i) the Zeeman phase from coupling the quantized angular momentum to the magnetic field and (ii) the Gouy phase, known from optical Laguerre-Gaussian beams. Remarkably, together these phases determine the structure of Landau energy levels. This unified Zeeman-Landau-Gouy phase manifests itself in a nontrivial evolution of images formed by various superpositions of modes. We demonstrate that, depending on the chosen superposition, the image can rotate in a magnetic field with either (i) Larmor, (ii) cyclotron (double-Larmor), or (iii) zero frequency. At the same time, its centroid always follows the classical cyclotron trajectory, in agreement with the Ehrenfest theorem. Remarkably, the non-rotating superpositions reproduce stable multi-vortex configurations that appear in rotating superfluids. Our results open up an avenue for the direct electron-microscopy observation of fundamental properties of free quantum electron states in magnetic fields., Comment: 21 pages, 10 figures, 1 table, to appear in Phys. Rev. X

Perovskite oxide heteroepitaxy receives much attention because of the possibility to com- bine the diverse functionalities of perovskite oxide building blocks. A general boundary con- dition for the epitaxy is the presence of polar discontinuities at heterointerfaces. These polar discontinuities result in reconstructions, often creating new functionalities at the interface. However, for a significant number of materials these reconstructions are unwanted as they alter the intrinsic materials properties at the interface. Therefore, a strategy to eliminate this reconstruction of the polar discontinuity at the interfaces is required. We show that the use of compositional interface engineering can prevent the reconstruction at the La0.67Sr0.33MnO3/SrTiO3 (LSMO/STO) interface. The polar discontinuity at this interface can be removed by the insertion of a single La0.33Sr0.67O layer, resulting in improved interface magnetization and electrical conductivity., Comment: Advanced Functional Materials, online march 2012

When comparing a set of La0.67Sr0.33MnO3 (LSMO) samples, the Curie temperature (TC) of the samples is an important figure of merit for the sample quality. Therefore, a reliable method to determine TC is required. Here, a method based on the analysis of the magnetization loops is proposed., Comment: Supplementary information to Preventing the reconstruction of the polar discontinuity at oxide heterointerfaces, Advanced Functional Materials, online march 2012

Solution derived La2Zr2O7 films have drawn much attention for potential applications as thermal barriers or low-cost buffer layers for coated conductor technology. Annealing and coating parameters strongly affect the microstructure of La2Zr2O7, but different film processing methods can yield similar microstructural features such as nanovoids and nanometer-sized La2Zr2O7 grains. Nanoporosity is a typical feature found in such films and the implications for the functionality of the films is investigated by a combination of scanning transmission electron microscopy, electron energy-loss spectroscopy and quantitative electron tomography. Chemical solution based La2Zr2O7 films deposited on flexible Ni-5at.%W substrates with a {100}<001> biaxial texture were prepared for an in-depth characterization. A sponge-like structure composed of nanometer sized voids is revealed by high-angle annular dark-field scanning transmission electron microscopy in combination with electron tomography. A three-dimensional quantification of nanovoids in the La2Zr2O7 film is obtained on a local scale. Mostly non-interconnected highly facetted nanovoids compromise more than one-fifth of the investigated sample volume. The diffusion barrier efficiency of a 170 nm thick La2Zr2O7 film is investigated by STEM-EELS yielding a 1.8 \pm 0.2 nm oxide layer beyond which no significant nickel diffusion can be detected and intermixing is observed. This is of particular significance for the functionality of YBa2Cu3O7-{\delta} coated conductor architectures based on solution derived La2Zr2O7 films as diffusion barriers., Comment: Accepted for publication in Superconductor Science and Technology