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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. This results in inaccuracies of measures obtained from the distorted images. Here we report on measurement and correction of elliptical distortions of diffraction patterns. The effect of this correction on the measurement of crystal lattice strain is investigated. We show that the effect of the distortions is smaller than the precision of the measurement in cases where the strain is obtained from shifts of diffracted discs with respect to their positions in images acquired in an unstrained reference area of the sample. This can be explained by the fact that diffraction patterns acquired in the strain free reference area of the sample are distorted in the same manner as the diffraction patterns acquired in the strained region of interest. In contrast, for samples without a strain free reference region such as nanoparticles or nanoporous structures, where we evaluate ratios of lattice plane distances along different directions, the distortions are usually not negligible. Furthermore, two techniques for the detection of diffraction disc positions are compared showing that for samples in which the crystal orientation changes over the investigated area it is more precise to detect the positions of many diffraction discs simultaneously instead of detecting each disc position independently.

Single atom detection is of key importance to solving a wide range of scientific and technological problems. The strong interaction of electrons with matter makes transmission electron microscopy one of the most promising techniques. In particular, aberration correction using scanning transmission electron microscopy has made a significant step forward toward detecting single atoms. However, to overcome radiation damage, related to the use of high-energy electrons, the incoming electron dose should be kept low enough. This results in images exhibiting a low signal-to-noise ratio and extremely weak contrast, especially for light-element nanomaterials. To overcome this problem, a combination of physics-based model fitting and the use of a model-order selection method is proposed, enabling one to detect single atoms with high reliability

The charge density is among the most fundamental solid state properties determining bonding, electrical characteristics, and adsorption or catalysis at surfaces. While atomic-scale charge densities have as yet been retrieved by solid state theory, we demonstrate both charge density and electric field mapping across a mono-/bilayer boundary in 2D MoS2 by momentum-resolved scanning transmission electron microscopy. Based on consistency of the four-dimensional experimental data, statistical parameter estimation and dynamical electron scattering simulations using strain-relaxed supercells, we are able to identify an AA-type bilayer stacking and charge depletion at the Mo-terminated layer edge. Published version

Results for the development and detailed analysis of self-organized InAs/InAlGaAs/InP quantum dots suitable for single-photon emission at the $1.55\phantom{\rule{0.28em}{0ex}}\ensuremath{\mu}\mathrm{m}$ telecom wavelength are reported. The structural and compositional properties of the system are obtained from high-resolution scanning transmission electron microscopy of individual quantum dots. The system is composed of almost pure InAs quantum dots embedded in quaternary InAlGaAs barrier material, which is lattice matched to the InP substrate. When using the measured results for a representative quantum-dot geometry as well as experimentally reconstructed alloy concentrations, a combination of strain-field and electronic-state calculations is able to reproduce the quantum-dot emission wavelength in agreement with the experimentally determined photoluminescence spectrum. The inhomogeneous broadening of the latter can be related to calculated variations of the emission wavelength for the experimentally deduced In-concentration fluctuations and size variations.

Measurement of lattice strain is important to characterize semiconductor nanostructures. As strain has large influence on the electronic band structure, methods for the measurement of strain with high precision, accuracy and spatial resolution in a large field of view are mandatory. In this paper we present a theoretical study of precision and accuracy of measurement of strain by convergent nano-beam electron diffraction. It is found that the accuracy of the evaluation suffers from halos in the diffraction pattern caused by a variation of strain within the area covered by the focussed electron beam. This effect, which is expected to be strong at sharp interfaces between materials with different lattice plane distances, will be discussed for convergent-beam electron diffraction patterns using a conventional probe and for patterns formed by a precessing electron beam. Furthermore, we discuss approaches to optimize the accuracy of strain measured at interfaces. The study is based on the evaluation of diffraction patterns simulated for different realistic structures that have been investigated experimentally in former publications. These simulations account for thermal diffuse scattering using the frozen-lattice approach and the modulation-transfer function of the image-recording system. The influence of Poisson noise is also investigated.

Piezoelectric and spontaneous polarization play an essential role in GaN-based devices. InGaN quantum wells (QWs) in GaN host material, especially grown along the polar c-direction, exhibit strong internal fields in the QW region due to the indium-induced strain. An exact knowledge of the electric fields is essential, since they are one of the factors limiting the performance of green LDs and LEDs. Differential phase contrast in a scanning transmission electron microscope enables direct, local, and quantitative measurements of these electric fields. For a multiQW sample, it was possible to determine the piezoelectric field in the range of 43-67MVm(-1) with a resolution of 10MVm(-1) (= 10mVnm(-1)). (C) 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

The chemical composition of four Si1-xGex 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. By means of simulations, the effect of amorphous surface layers on the HAADF intensity of crystalline silicon and germanium is investigated. Based on these simulations, a method is developed to analyze the experimental HAADF-STEM images by taking the influence of the amorphous layers into account which is done by a reduction of the intensities by multiplication with a constant factor. This suggested modified HAADF analysis gives germanium concentrations which are in agreement with the nominal values. The same TEM lamella was treated with low-voltage ion milling which removed the amorphous surface layers completely. The results from subsequent quantitative HAADF analyses are in agreement with the nominal concentrations which validates the applicability of the used frozen-lattice based multislice simulations to describe the HAADF scattering of Si1-xGex in STEM. (C) 2017 Elsevier B.V. All rights reserved.

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. These experimental characteristics are the background intensity, the presence of Poisson noise caused by electron statistics and blurring caused by inelastic scattering and by the transfer quality of the microscope camera. By means of these optimized simulations, different effects of specimen properties on disc detection - such as strain, surface morphology and compositional changes on the nanometer scale - are investigated and discussed in the context of misinterpretation in experimental NBED evaluations. It is shown that changes in surface morphology and chemical composition lead to measured shifts of the central disc in the NBED pattern of tens to hundreds of grad. These shifts are of the same order of magnitude or even larger than shifts that could be caused by an electric polarisation field in the range of MV/cm. (C) 2017 Elsevier B.V. All rights reserved.

This study sheds light on the prerequisites, possibilities, limitations and interpretation of high-resolution differential phase contrast (DPC) imaging in scanning transmission electron microscopy (STEM). We draw particular attention to the well-established DPC technique based on segmented annular detectors and its relation to recent developments based on pixelated detectors. These employ the expectation value of the momentum transfer as a reliable measure of the angular deflection of the STEM beam induced by an electric field in the specimen. The influence of scattering and propagation of electrons within the specimen is initially discussed separately and then treated in terms of a two-state channeling theory. A detailed simulation study of GaN is presented as a function of specimen thickness and bonding. It is found that bonding effects are rather detectable implicitly, e.g., by characteristics of the momentum flux in areas between the atoms than by directly mapping electric fields and charge densities. For strontium titanate, experimental charge densities are compared with simulations and discussed with respect to experimental artifacts such as scan noise. Finally, we consider practical issues such as figures of merit for spatial and momentum resolution, minimum electron dose, and the mapping of larger-scale, built-in electric fields by virtue of data averaged over a crystal unit cell. We find that the latter is possible for crystals with an inversion center. Concerning the optimal detector design, this study indicates that a sampling of 5 mrad per pixel is sufficient in typical applications, corresponding to approximately 10 × 10 available pixels.

Nanoporous gold (npAu) has attracted a lot of attention during the last decade as it has interesting applications particularly in the field of catalysis [1]. It is prepared by corrosion of a suitable gold master alloy, e.g. gold/silver. The remaining material forms a sponge-like structure built of ligaments and pores still preserving a crystalline structure over several tens of nanometres. A high surface to volume ratio, open porosity making it permeable for gases and liquids and a strongly curved ligament surface providing surface atoms of different coordination are only some properties which qualify npAu as catalytic material with well adjustable and reproducible structure. One important structural property that is expected to have strong influence on the catalytic activity is lattice strain, because strain affects the electronic states [2]. Here we present measurements of strain in npAu. A measurement of lattice strain by means of high-resolution TEM for example by the analysis of lattice plane distances is possible only in a very small field of view for npAu. As the positions of intensity maxima in the images depend on several experimental parameters, such as defocus, orientation, composition, lens aberrations and especially specimen thickness, maxima detection in TEM micrographs succeeds only in small parts of the sample, because thickness is varying strongly. This can be seen in Fig. 1. Close to the surface intensity maxima can be detected and thus strain can be measured, in this case tensile strain up to 5% has been found. But as the ligament gets thicker and defects become visible, contrast changes and strain analysis fails. A method that overcomes these problems is strain analysis using nano-beam electron diffraction (NBED) [3]. Here a focussed electron probe is scanned across the sample and at each position of the scanning beam the corresponding diffraction pattern is recorded. As distances between the non-overlapping diffraction discs depend basically on the local lattice parameter according to Bragg's law, strain can be measured by comparing distances between diffraction discs at different positions of the scanning beam. By an analysis of distances between diffraction discs in two linearly independent directions strain as well as shear-strain and rotation can be measured. A further advantage of strain analysis by NBED is its large field of view, because at first sight it is limited only by the size of the scanned part of the sample. Hence strain and rotation of neighbouring ligaments in npAu can be measured. On the other hand a large field of view requires the acquisition of a large number of diffraction patterns in a short time to avoid effects of sample drift, beam induced sample damage and contamination. Here we present strain and rotation maps of npAu measured using a delay-line detector for the acquisition of the diffraction patterns. With this detector strain maps at a scanning raster of e.g. 100x100 pixels can be recorded, allowing measurements in a field of view of several hundreds of nanometers (Fig. 2) still preserving a sampling limited spatial resolution of about 1.6 nm [4]. Furthermore we show by evaluation of simulations that two important aspects concerning the precision of the measurement have to be taken into account. As the precision of the measurement suffers from noise in the diffraction pattern, the precision degrades for shorter image integration times. On the other hand the precision can be increased using a precessing [5, 6] electron beam, as the diffraction discs are illuminated more homogeneously and hence their positions can be detected more precisely. In this way a compromise between precision and speed / size of the measurement has to be found. Keywords: nanoporous gold; strain measurement; NBED; precision

The preadsorption of Ag on Si(111) drastically changes the growth of Ge. In a temperature range from $400{\phantom{\rule{0.16em}{0ex}}}^{\ensuremath{\circ}}\mathrm{C}$ to $650{\phantom{\rule{0.16em}{0ex}}}^{\ensuremath{\circ}}\mathrm{C}$, Ag adsorption on Si leads to the formation of a $\sqrt{3}\ifmmode\times\else\texttimes\fi{}\sqrt{3}$-R ${30}^{\ensuremath{\circ}}$ reconstruction that exhibits a maze-like morphology on the mesoscopic scale, as observed by low-energy electron diffraction (LEED) and low-energy electron microscopy. This maze morphology can be attributed to a surface roughening on an atomic scale, induced by the re-arrangement of top layer atoms during the $7\ifmmode\times\else\texttimes\fi{}7$ to $\sqrt{3}\ifmmode\times\else\texttimes\fi{}\sqrt{3}$-R ${30}^{\ensuremath{\circ}}$ transition. The subsequent deposition of Ge results in the formation of a wetting layer, the evolution of which has been found to be governed by the Ag/Si(111)-$\sqrt{3}\ifmmode\times\else\texttimes\fi{}\sqrt{3}$-R ${30}^{\ensuremath{\circ}}$ template's maze structure, as the latter offers a high density of heterogeneous nucleation sites. Upon further Ge growth, three-dimensional islands with diameters in the micrometer range are formed, which exhibit a large and flat (111) top facet. X-ray photoemission electron microscopy reveals that during Ge growth, Ag is segregating to the surface very efficiently. Grazing-incidence x-ray diffraction and transmission electron microscopy have been used to study the composition, strain state and defect structure of the Ge islands in dependence of the growth temperature. The strain induced by lattice mismatch is found to be largely relaxed (80--90% relaxation) in the investigated growth temperature range from 400 to $600{\phantom{\rule{0.16em}{0ex}}}^{\ensuremath{\circ}}\mathrm{C}$, which is confirmed by high-resolution LEED measurements. As a main relaxation mechanism, the formation of interfacial misfit dislocations has been identified. Interdiffusion of Si into the Ge islands becomes more and more pronounced for increasing growth temperature, whereas the formation of twinned Ge regions can drastically be suppressed at higher temperature.

Nitride-based three-dimensional core-shell nanorods (NRs) are promising candidates for the achievement of highly efficient optoelectronic devices. For a detailed understanding of the complex core-shell layer structure of InGaN/GaN NRs, a systematic determination and correlation of the structural, compositional, and optical properties on a nanometer-scale is essential. In particular, the combination of low-temperature cathodoluminescence (CL) spectroscopy directly performed in a scanning transmission electron microscope (STEM), and quantitative high-angle annular dark field imaging enables a comprehensive study of the nanoscopic attributes of the individual shell layers. The investigated InGaN/GaN core-shell NRs, which were grown by metal-organic vapor-phase epitaxy using selective-area growth exhibit an exceptionally low density of extended defects. Using highly spatially resolved CL mapping of single NRs performed in cross-section, we give a direct insight into the optical properties of the individual core-shell layers. Most interesting, we observe a red shift of the InGaN single quantum well from 410 to 471 nm along the nonpolar side wall. Quantitative STEM analysis of the active region reveals an increasing thickness of the single quantum well (SQW) from 6 to 13 nm, accompanied by a slight increase of the indium concentration along the nonpolar side wall from 11% to 13%. Both effects, the increased quantum-well thickness and the higher indium incorporation, are responsible for the observed energetic shift of the InGaN SQW luminescence. Furthermore, compositional mappings of the InGaN quantum well reveal the formation of locally indium rich regions with several nanometers in size, leading to potential fluctuations in the InGaN SQW energy landscape. This is directly evidenced by nanometer-scale resolved CL mappings that show strong localization effects of the excitonic SQW emission.

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. Our method is applied to measure nitrogen content and specimen thickness in a GaNxAs1−x layer independently at atomic resolution by evaluating two dedicated angular intervals. We demonstrate contrast formation due to strain and composition in a Si- based metal-oxide semiconductor field effect transistor (MOSFET) with GexSi1−x stressors as a function of the angles used for imaging. To shed light on the validity of current theoretical approaches this data is compared with theory, namely the Rutherford approach and contemporary multislice simulations. Inconsistency is found for the Rutherford model in the whole angular range of 16–255 mrad. Contrary, the multislice simulations are applicable for angles larger than 35 mrad whereas a significant mismatch is observed at lower angles. This limitation of established simulations is discussed particularly on the basis of inelastic scattering.

The built-in piezoelectric fields in group III-nitrides can act as road blocks on the way to maximizing the efficiency of opto-electronic devices. In order to overcome this limitation, a proper characterization of these fields is necessary. In this work nano-beam electron diffraction in scanning transmission electron microscopy mode has been used to simultaneously measure the strain state and the induced piezoelectric fields in a GaN/AlN multiple quantum well system, The authors thank the FEI company for the EDX measurements and HR-BF-STEM data. This work was supported by the MAT2010-15206 (CICYT, Spain), EU-COST Action MP0805, and P09-TEP-5403 (Junta de Andalucía with EU-FEDER participation). We acknowledge support by FCT Portugal (PTDC/FIS NAN/0973/2012, SFRH/BPD/74095/2010, Investigador FCT), and Juan de la Cierva program (JCI-2012-14509). K.M. acknowledges support from the Deutsche Forschungsgemeinschaft (DFG) under contract No. MU 3660/1-1. T.G: acknowledges support from DFG (R02051/11-1)

The electronic properties of quaternary AlInGaN devices significantly depend on the homogeneity of the alloy. The identification of compositional fluctuations or verification of random-alloy distribution is hence of grave importance. Here, a comprehensive multiprobe study of composition and compositional homogeneity is presented, investigating AlInGaN layers with indium concentrations ranging from 0 to 17 at% and aluminium concentrations between 0 and 39 at% employing high-angle annular dark field scanning electron microscopy (HAADF STEM), energy dispersive X-ray spectroscopy (EDX) and atom probe tomography (APT). EDX mappings reveal distributions of local concentrations which are in good agreement with random alloy atomic distributions. This was hence investigated with HAADF STEM by comparison with theoretical random alloy expectations using statistical tests. To validate the performance of these tests, HAADF STEM image simulations were carried out for the case of a random-alloy distribution of atoms and for the case of In-rich clusters with nanometer dimensions. The investigated samples, which were grown by metal-organic vapor phase epitaxy (MOVPE), were thereby found to be homogeneous on this nanometer scale. Analysis of reconstructions obtained from APT measurements yielded matching results. Though HAADF STEM only allows for the reduction of possible combinations of indium and aluminium concentrations to the proximity of isolines in the two-dimensional composition space. The observed ranges of composition are in good agreement with the EDX and APT results within the respective precisions.

Dank der enormen Weiterentwicklung aberrationskorrigierter Elektronenoptik erreicht die Raster-Transmissionselektronenmikroskopie (STEM) heute eine Auflosung von 50 pm (1 pm = 10–12 m). Damit eroffnet sich der Blick in subatomare Details, wie atomare elektrische Felder oder Ladungstransfers bei chemischen Bindungen.

GaN nanotubes with coaxial InGaN quantum wells were analyzed by scanning transmission electron microscopy in order to determine their structural properties as well as the indium distribution across the InGaN quantum wells. For the latter, two process steps are necessary. First, a technique to prepare cross-sectional slices out of the nanotubes has been developed. Second, an existing scanning transmission electron microscopy analysis technique has been extended with respect to the special crystallographic orientation of this type of specimen. In particular, the shape of the nanotubes, their defect structure, and the incorporation of indium on different facets were investigated. The quantum wells preferentially grow on m-planes of the dodecagonally shaped nanotubes and on semipolar top facets while no significant indium signal was found on a-planes. An averaged indium concentration of 6% to 7% was found by scanning transmission electron microscopy analysis and could be confirmed by cathodoluminescence measu...

We report on a new camera that is based on a pnCCD sensor for applications in scanning transmission electron microscopy. Emerging new microscopy techniques demand improved detectors with regards to readout rate, sensitivity and radiation hardness, especially in scanning mode. The pnCCD is a 2D imaging sensor that meets these requirements. Its intrinsic radiation hardness permits direct detection of electrons. The pnCCD is read out at a rate of 1,150 frames per second with an image area of 264 x 264 pixel. In binning or windowing modes, the readout rate is increased almost linearly, for example to 4000 frames per second at 4× binning (264 x 66 pixel). Single electrons with energies from 300 keV down to 5 keV can be distinguished due to the high sensitivity of the detector. Three applications in scanning transmission electron microscopy are highlighted to demonstrate that the pnCCD satisfies experimental requirements, especially fast recording of 2D images. In the first application, 65536 2D diffraction patterns were recorded in 70 s. STEM images corresponding to intensities of various diffraction peaks were reconstructed. For the second application, the microscope was operated in a Lorentz-like mode. Magnetic domains were imaged in an area of 256 x 256 sample points in less than 37 seconds for a total of 65536 images each with 264 x 132 pixels. Due to information provided by the two-dimensional images, not only the amplitude but also the direction of the magnetic field could be determined. In the third application, millisecond images of a semiconductor nanostructure were recorded to determine the lattice strain in the sample. A speed-up in measurement time by a factor of 200 could be achieved compared to a previously used camera system.

Advanced materials 2207130 (2022). doi:10.1002/adma.202207130, Published by Wiley-VCH, Weinheim