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State-of-the-art electron microscopes such as scanning electron microscopes (SEM), scanning transmission electron microscopes (STEM) and transmission electron microscopes (TEM) have become increasingly sophisticated. However, the quality of experimental images is often hampered by stochastic and deterministic distortions arising from the instrument or its environment. These distortions can arise during any stage of the imaging process, including image acquisition, transmission, or visualization. In this paper, we will discuss the main sources of distortion in TEM and S(T)EM images, develop models to describe them and propose a method to correct these distortions using a convolutional neural network. We demonstrate the effectiveness of our approach on a variety of experimental images and show that it can significantly improve the signal-to-noise ratio resulting in an increase in the amount of quantitative structural information that can be extracted from the image. Overall, our findings provide a powerful framework for improving the quality of electron microscopy images and advancing the field of structural analysis and quantification in materials science and biology.

In oxide heterostructures, different materials are integrated into a single artificial crystal, resulting in a breaking of inversion-symmetry across the heterointerfaces. A notable example is the interface between polar and non-polar materials, where valence discontinuities lead to otherwise inaccessible charge and spin states. This approach paved the way to the discovery of numerous unconventional properties absent in the bulk constituents. However, control of the geometric structure of the electronic wavefunctions in correlated oxides remains an open challenge. Here, we create heterostructures consisting of ultrathin SrRuO$_3$, an itinerant ferromagnet hosting momentum-space sources of Berry curvature, and LaAlO$_3$, a polar wide-bandgap insulator. Transmission electron microscopy reveals an atomically sharp LaO/RuO$_2$/SrO interface configuration, leading to excess charge being pinned near the LaAlO$_3$/SrRuO$_3$ interface. We demonstrate through magneto-optical characterization, theoretical calculations and transport measurements that the real-space charge reconstruction modifies the momentum-space Berry curvature in SrRuO$_3$, driving a reorganization of the topological charges in the band structure. Our results illustrate how the topological and magnetic features of oxides can be manipulated by engineering charge discontinuities at oxide interfaces., Comment: 5 pages main text (4 figures), 29 pages of supplementary information

Recently, the maximum a posteriori (MAP) probability rule has been proposed as an objective and quantitative method to detect atom columns and even single atoms from high-resolution high-angle annular dark-field (HAADF) scanning transmission electron microscopy (STEM) images. The method combines statistical parameter estimation and model-order selection using a Bayesian framework and has been shown to be especially useful for the analysis of the structure of beam-sensitive nanomaterials. In order to avoid beam damage, images of such materials are usually acquired using a limited incoming electron dose resulting in a low contrast-to-noise ratio (CNR) which makes visual inspection unreliable. This creates a need for an objective and quantitative approach. The present paper describes the methodology of the MAP probability rule, gives its step-by-step derivation and discusses its algorithmic implementation for atom column detection. In addition, simulation results are presented showing that the performance of the MAP probability rule to detect the correct number of atomic columns from HAADF STEM images is superior to that of other model-order selection criteria, including the Akaike Information Criterion (AIC) and the Bayesian Information Criterion (BIC). Moreover, the MAP probability rule is used as a tool to evaluate the relation between STEM image quality measures and atom detectability resulting in the introduction of the so-called integrated CNR (ICNR) as a new image quality measure that better correlates with atom detectability than conventional measures such as signal-to-noise ratio (SNR) and CNR.

The atomic lensing model has been proposed as a promising method facilitating atom-counting in heterogeneous nanocrystals [KHW van den Bos et. al, Phys. Rev. Lett. 116 (2016) 246101] Here, image simulations will validate the model, which describes dynamical diffraction as a superposition of individual atoms focussing the incident electrons. It will be demonstrated that the model is reliable in the annular dark field regime for crystals having columns containing dozens of atoms. By using the principles of statistical detection theory, it will be shown that this model gives new opportunities for detecting compositional differences.

Geometric phases in condensed matter play a central role in topological transport phenomena such as the quantum, spin and anomalous Hall effect (AHE). In contrast to the quantum Hall effect - which is characterized by a topological invariant and robust against perturbations - the AHE depends on the Berry curvature of occupied bands at the Fermi level and is therefore highly sensitive to subtle changes in the band structure. A unique platform for its manipulation is provided by transition metal oxide heterostructures, where engineering of emergent electrodynamics becomes possible at atomically sharp interfaces. We demonstrate that the Berry curvature and its corresponding vector potential can be manipulated by interface engineering of the correlated itinerant ferromagnet SrRuO$_3$ (SRO). Measurements of the AHE reveal the presence of two interface-tunable spin-polarized conduction channels. Using theoretical calculations, we show that the tunability of the AHE at SRO interfaces arises from the competition between two topologically non-trivial bands. Our results demonstrate how reconstructions at oxide interfaces can be used to control emergent electrodynamics on a nanometer-scale, opening new routes towards spintronics and topological electronics., Comment: 8 pages, 4 figures, (+ Supplementary Information)

Atomically resolved electron energy-loss spectroscopy experiments are commonplace in modern aberrationcorrected transmission electron microscopes. Energy resolution has also been increasing steadily with the continuous improvement of electron monochromators. Electronic excitations however are known to be delocalised due to the long range interaction of the charged accelerated electrons with the electrons in a sample. This has made several scientists question the value of combined high spatial and energy resolution for mapping interband transitions and possibly phonon excitation in crystals. In this paper we demonstrate experimentally that atomic resolution information is indeed available at very low energy losses around 100 meV expressed as a modulation of the broadening of the zero loss peak. Careful data analysis allows us to get a glimpse of what are likely phonon excitations with both an energy loss and gain part. These experiments confirm recent theoretical predictions on the strong localisation of phonon excitations as opposed to electronic excitations and show that a combination of atomic resolution and recent developments in increased energy resolution will offer great benefit for mapping phonon modes in real space.

In this article, an overview of the fabrication and properties of high quality La0.67Sr0.33MnO3 (LSMO) thin films is given. A high quality LSMO film combines a smooth surface morphology with a large magnetization and a small residual resistivity, while avoiding precipitates and surface segregation. In literature, typically only a few of these issues are adressed. We therefore present a thorough characterization of our films, which were grown by pulsed laser deposition. The films were characterized with reflection high energy electron diffraction, atomic force microscopy, x-ray diffraction, magnetization and transport measurements, x-ray photoelectron spectroscopy and scanning transmission electron microscopy. The films have a saturation magnetization of 4.0 {\mu}B/Mn, a Curie temperature of 350 K and a residual resistivity of 60 {\mu}{\Omega}cm. These results indicate that high quality films, combining both large magnetization and small residual resistivity, were realized. A comparison between different samples presented in literature shows that focussing on a single property is insufficient for the optimization of the deposition process. For high quality films, all properties have to be adressed. For LSMO devices, the thin film quality is crucial for the device performance. Therefore, this research is important for the application of LSMO in devices., Comment: Accepted for publication in Journal of Physics D - Applied Physics

The synthesis of materials with well-controlled composition and structure improves our understanding of their intrinsic electrical transport properties. Recent developments in atomically controlled growth have been shown to be crucial in enabling the study of new physical phenomena in epitaxial oxide heterostructures. Nevertheless, these phenomena can be influenced by the presence of defects that act as extrinsic sources of both doping and impurity scattering. Control over the nature and density of such defects is therefore necessary, are we to fully understand the intrinsic materials properties and exploit them in future device technologies. Here, we show that incorporation of a strontium copper oxide nano-layer strongly reduces the impurity scattering at conducting interfaces in oxide LaAlO3-SrTiO3(001) heterostructures, opening the door to high carrier mobility materials. We propose that this remote cuprate layer facilitates enhanced suppression of oxygen defects by reducing the kinetic barrier for oxygen exchange in the hetero-interfacial film system. This design concept of controlled defect engineering can be of significant importance in applications in which enhanced oxygen surface exchange plays a crucial role., Comment: Advanced Functional Materials (2013)

Perovskite oxides exhibit a plethora of exceptional electronic properties, providing the basis for novel concepts of oxide-electronic devices. The interest in these materials is even extended by the remarkable characteristics of their interfaces. Studies on single epitaxial connections between the two wide-bandgap insulators LaAlO3 and SrTiO3 have revealed them to be either high-mobility electron conductors or insulating, depending on the atomic stacking sequences. In the latter case they are conceivably positively charged. For device applications, as well as for basic understanding of the interface conduction mechanism, it is important to investigate the electronic coupling of closely-spaced complementary interfaces. Here we report the successful realization of such electronically coupled complementary interfaces in SrTiO3 - LaAlO3 thin film multilayer structures, in which the atomic stacking sequence at the interfaces was confirmed by quantitative transmission electron microscopy. We found a critical separation distance of 6 perovskite unit cell layers, corresponding to approximately 2.3 nm, below which a decrease of the interface conductivity and carrier density occurs. Interestingly, the high carrier mobilities characterizing the separate electron doped interfaces are found to be maintained in coupled structures down to sub-nanometer interface spacing.