Characterization of structure and mixing in nanoparticle hetero-aggregates using convolutional neural networks: 3D-reconstruction versus 2D-projection.

Structural and chemical characterization of nanomaterials provides important information for understanding their functional properties. Nanomaterials with characteristic structure sizes in the nanometer range can be characterized by scanning transmission electron microscopy (STEM). In conventional STEM, two-dimensional (2D) projection images of the samples are acquired, information about the third dimension is lost.

Synergizing ICP-MS, STEM-EDXS, and SMPS single particle analytics exemplified by superlattice L1 Pt/Fe aerosol nanoparticles produced by spark ablation.

Spark ablation was used to continuously synthesize bimetallic L1 Pt/Fe nanoparticles in an aerosol process involving a furnace and hydrogen as a reducing process gas. For the formation of Pt/Fe in the favorable L1 crystal configuration, which is a promising electrocatalyst, the Pt-Fe ratio plays a crucial role. State-of-the-art analytics for such multi-element nanoparticles include, among others, electron microscopy (EM) with an element mapping function, such as scanning transmission electron microscopy with energy-dispersive X-ray spectroscopy (STEM-EDXS).

GaN atomic electric fields from a segmented STEM detector: Experiment and simulation.

Atomic electric fields in a thin GaN sample are measured with the centre-of-mass approach in 4D-scanning transmission electron microscopy (4D-STEM) using a 12-segmented STEM detector in a Spectra 300 microscope. The electric fields, charge density and potential are compared to simulations and an experimental measurement using a pixelated 4D-STEM detector. The segmented detector benefits from a high recording speed, which enables measurements at low radiation doses.

Origin of the spectral red-shift and polarization patterns of self-assembled InGaN nanostructures on GaN nanowires.

The luminescence of InGaN nanowires (NWs) is frequently reported with large red-shifts as compared to the theoretical value expected from the average In content. Both compositional fluctuations and radial built-in fields were considered accountable for this effect, depending on the size, structure, composition, and surrounding medium of the NWs. In the present work, the emission properties of InGaN/GaN NWs grown by plasma-assisted molecular beam epitaxy are investigated in a comprehensive study combining ultraviolet-Raman and photoluminescence spectroscopy (PL) on vertical arrays, polarization-dependent PL on bundles of a few NWs, scanning transmission electron microscopy, energy-dispersive X-ray spectroscopy, and calculations of the band profiles.

Correlative analysis on InGaN/GaN nanowires: structural and optical properties of self-assembled short-period superlattices.

The influence of self-assembled short-period superlattices (SPSLs) on the structural and optical properties of InGaN/GaN nanowires (NWs) grown by PAMBE on Si (111) was investigated by STEM, EDXS, µ-PL analysis and k·p simulations. STEM analysis on single NWs indicates that in most of the studied nanostructures, SPSLs self-assemble during growth. The SPSLs display short-range ordering of In-rich and In-poor InGaN regions with a period of 2-3 nm that are covered by a GaN shell and that transition to a more homogenous InGaN core.

Dose efficient annular bright field contrast with the ISTEM method: A proof of principle demonstration.

The ISTEM mode for TEM has been demonstrated to have several advantages in regard to resolution and precision. While previous works primarily focussed on the advantages due to the reduced spatial coherence, the actual image contrast, i.e.

Angle-dependence of ADF-STEM intensities for chemical analysis of InGaN/GaN.

In this paper we perform angular resolved annular-dark field (ADF) scanning-transmission electron microscopy (STEM) to study the scattered intensity in an InGaN layer buried in GaN as a function of the scattering angle. We achieved angular resolution with a motorized iris aperture in front of the ADF detector. Using this setup, we investigated how the intensities measured in various angular ranges agree with multislice simulations in the frozen-lattice approximation.

Towards the interpretation of a shift of the central beam in nano-beam electron diffraction as a change in mean inner potential.

The measurement of electric fields in scanning transmission electron microscopy (STEM) is a highly investigated field of research. The constant improvement of spatial resolution in STEM and the development of new hardware for the fast acquisition of diffraction patterns even paved the way for the measurement of atomic electric fields. Although the basic principle that an electric field leads to a tilt of the focussed electron probe that can be detected as a shift of the diffraction pattern in the back focal plane of the objective lens seems quite simple, many challenges arose in the measurement of fields in a quantitative way.

4D-STEM at interfaces to GaN: Centre-of-mass approach & NBED-disc detection.

4D-scanning transmission electron microscopy (4D-STEM) can be used to measure electric fields such as atomic fields or polarization-induced electric fields in crystal heterostructures. The paper focuses on effects occurring in 4D-STEM at interfaces, where two model systems are used: an AlN/GaN nanowire superlattice as well as a GaN/vacuum interface. Two different methods are applied: First, we employ the centre-of mass (COM) technique which uses the average momentum transfer evaluated from the intensity distribution in the diffraction pattern.

Accuracy and precision of position determination in ISTEM imaging of BaTiO.

In this paper we study the effect of lens aberrations (spherical aberration and astigmatism), beam tilt, contamination and shot noise on the accuracy and precision of position determination in imaging scanning transmission electron microscopy (ISTEM) on the example of BaTiO. ISTEM images are simulated as a function of sample thickness and defocus starting from a nearly perfect microscope setting. A defocus range was identified, in which atom column positions were reliably visible and could be decently measured.

Quantitative Characterization of Nanometer-Scale Electric Fields via Momentum-Resolved STEM.

Most of today's electronic devices, like solar cells and batteries, are based on nanometer-scale built-in electric fields. Accordingly, characterization of fields at such small scales has become an important task in the optimization of these devices. In this study, with GaAs-based p-n junctions as the example, key characteristics such as doping concentrations, polarity, and the depletion width are derived quantitatively using four-dimensional scanning transmission electron microscopy (4DSTEM).

Angle-resolved STEM using an iris aperture: Scattering contributions and sources of error for the quantitative analysis in Si.

The angle-resolved electron scattering is investigated in scanning-transmission electron microscopy (STEM) using a motorised iris aperture placed above a conventional annular detector. The electron intensity scattered into various angle ranges is compared with simulations that were carried out in the frozen-lattice approximation. As figure of merit for the agreement of experiment and simulation we evaluate the specimen thickness which is compared with the thickness obtained from position-averaged convergent beam electron diffraction (PACBED).

Accurate measurement of strain at interfaces in 4D-STEM: A comparison of various methods.

Strain analysis by nano-beam electron diffraction allows for measurements of strain with nanometre resolution in a large field of view. This is done by evaluating distances between diffraction discs in diffraction patterns acquired while a focussed electron beam is scanned across the sample in a transmission electron microscope. The bottleneck of this method is a precise determination of diffraction disc positions, which suffers from the inner structure of the discs caused by dynamical diffraction.

Influence of plasmon excitations on atomic-resolution quantitative 4D scanning transmission electron microscopy.

Scanning transmission electron microscopy (STEM) allows to gain quantitative information on the atomic-scale structure and composition of materials, satisfying one of todays major needs in the development of novel nanoscale devices. The aim of this study is to quantify the impact of inelastic, i.e.

Electrical Polarization in AlN/GaN Nanodisks Measured by Momentum-Resolved 4D Scanning Transmission Electron Microscopy.

We report the mapping of polarization-induced internal electric fields in AlN/GaN nanowire heterostructures at unit cell resolution as a key for the correlation of optical and structural phenomena in semiconductor optoelectronics. Momentum-resolved aberration-corrected scanning transmission electron microscopy is employed as a new imaging mode that simultaneously provides four-dimensional data in real and reciprocal space. We demonstrate how internal mesoscale and atomic electric fields can be separated in an experiment, which is verified by comprehensive dynamical simulations of multiple electron scattering.

Influence of distortions of recorded diffraction patterns on strain analysis by nano-beam electron diffraction.

Images acquired in transmission electron microscopes can be distorted for various reasons such as e.g. aberrations of the lenses of the imaging system or inaccuracies of the image recording system.

Strain analysis from nano-beam electron diffraction: Influence of specimen tilt and beam convergence.

Strain analyses from experimental series of nano-beam electron diffraction (NBED) patterns in scanning transmission electron microscopy are performed for different specimen tilts. Simulations of NBED series are presented for which strain analysis gives results that are in accordance with experiment. This consequently allows to study the relation between measured strain and actual underlying strain.

Using molecular dynamics for multislice TEM simulation of thermal diffuse scattering in AlGaN.

For simulation of transmission electron microscopic images and diffraction patterns, the accurate inclusion of thermal diffuse scattering by phonons is important. In the frozen phonon multislice algorithm, this is possible, if thermal displacements according to the realistic, quantum mechanical distribution can be generated. For pure crystals, quantum mechanical calculations based on DFT yield those displacements.

Ultrathin Au-Alloy Nanowires at the Liquid-Liquid Interface.

Ultrathin bimetallic nanowires are of importance and interest for applications in electronic devices such as sensors and heterogeneous catalysts. In this work, we have designed a new, highly reproducible and generalized wet chemical method to synthesize uniform and monodispersed Au-based alloy (AuCu, AuPd, and AuPt) nanowires with tunable composition using microwave-assisted reduction at the liquid-liquid interface. These ultrathin alloy nanowires are below 4 nm in diameter and about 2 μm long.

Quantitative HAADF STEM of SiGe in presence of amorphous surface layers from FIB preparation.

The chemical composition of four SiGe layers grown on silicon was determined from quantitative scanning transmission electron microscopy (STEM). The chemical analysis was performed by a comparison of the high-angle annular dark field (HAADF) intensity with multislice simulations. It could be shown that amorphous surface layers originating from the preparation process by focused-ion beam (FIB) at 30 kV have a strong influence on the quantification: the local specimen thickness is overestimated by approximately a factor of two, and the germanium concentration is substantially underestimated.

Screening Precursor-Solvent Combinations for LiTiO Energy Storage Material Using Flame Spray Pyrolysis.

The development and industrial application of advanced lithium based energy-storage materials are directly related to the innovative production techniques and the usage of inexpensive precursor materials. Flame spray pyrolysis (FSP) is a promising technique that overcomes the challenges in the production processes such as scalability, process control, material versatility, and cost. In the present study, phase pure anode material LiTiO (LTO) was designed using FSP via extensive systematic screening of lithium and titanium precursors dissolved in five different organic solvents.

Bias-Controlled Optical Transitions in GaN/AlN Nanowire Heterostructures.

We report on the control and modification of optical transitions in 40× GaN/AlN heterostructure superlattices embedded in GaN nanowires by an externally applied bias. The complex band profile of these multi-nanodisc heterostructures gives rise to a manifold of optical transitions, whose emission characteristic is strongly influenced by polarization-induced internal electric fields. We demonstrate that the superposition of an external axial electric field along a single contacted nanowire leads to specific modifications of each photoluminescence emission, which allows to investigate and identify their origin and to control their characteristic properties in terms of transition energy, intensity and decay time.

Optimization of NBED simulations for disc-detection measurements.

Nano-beam electron diffraction (NBED) is a method which can be applied to measure lattice strain and polarisation fields in strained layer heterostructures and transistors. To investigate precision, accuracy and spatial resolution of such measurements in dependence of properties of the specimen as well as electron optical parameters, simulations of NBED patterns are required which allow to predict the result of common disc-detection algorithms. In this paper we demonstrate by focusing on the detection of the central disc in crystalline silicon that such simulations require to take several experimental characteristics into account in order to obtain results which are comparable to those from experimental NBED patterns.

Materials characterisation by angle-resolved scanning transmission electron microscopy.

Solid-state properties such as strain or chemical composition often leave characteristic fingerprints in the angular dependence of electron scattering. Scanning transmission electron microscopy (STEM) is dedicated to probe scattered intensity with atomic resolution, but it drastically lacks angular resolution. Here we report both a setup to exploit the explicit angular dependence of scattered intensity and applications of angle-resolved STEM to semiconductor nanostructures.