“Electron Bessel beam diffraction for precise and accurate nanoscale strain mapping”. Guzzinati G, Ghielens W, Mahr C, Béché, A, Rosenauer A, Calders T, Verbeeck J, Applied physics letters 114, 243501 (2019). http://doi.org/10.1063/1.5096245
Abstract: 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 a very high spatial resolution. In this regard, transmission electron microscopes are key instruments thanks to their ability to map strain with a subnanometer resolution. Here, we present a 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 × 10−4 and an accuracy of 1.5 × 10−3, competing with, or outperforming, the best existing methods with a simple and easy to use experimental setup.
Keywords: A1 Journal article; ADReM Data Lab (ADReM); Electron microscopy for materials research (EMAT)
Impact Factor: 3.411
Times cited: 17
DOI: 10.1063/1.5096245
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“Electrical Polarization in AlN/GaN Nanodisks Measured by Momentum-Resolved 4D Scanning Transmission Electron Microscopy”. Müller-Caspary K, Grieb T, Müßener J, Gauquelin N, Hille P, Schörmann J, Verbeeck J, Van Aert S, Eickhoff M, Rosenauer A, Physical review letters 122, 106102 (2019). http://doi.org/10.1103/PhysRevLett.122.106102
Abstract: 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. A mean difference of 5.3 +- 1.5 MV/cm is found for the polarization-induced electric fields in AlN and GaN, being in accordance with dedicated simulations and photoluminescence measurements in previous publications.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 8.462
Times cited: 26
DOI: 10.1103/PhysRevLett.122.106102
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“Comparison of first moment STEM with conventional differential phase contrast and the dependence on electron dose”. Müller-Caspary K, Krause FF, Winkler F, Béché, A, Verbeeck J, Van Aert S, Rosenauer A, Ultramicroscopy 203, 95 (2019). http://doi.org/10.1016/J.ULTRAMIC.2018.12.018
Abstract: This study addresses the comparison of scanning transmission electron microscopy (STEM) measurements of momentum transfers using the first moment approach and the established method that uses segmented annular detectors. Using an ultrafast pixelated detector to acquire four-dimensional, momentum-resolved STEM signals, both the first moment calculation and the calculation of the differential phase contrast (DPC) signals are done for the same experimental data. In particular, we investigate the ability to correct the segment-based signal to yield a suitable approximation of the first moment for cases beyond the weak phase object approximation. It is found that the measurement of momentum transfers using segmented detectors can approach the first moment measurement as close as 0.13 h/nm in terms of a root mean square (rms) difference in 10 nm thick SrTiO3 for a detector with 16 segments. This amounts to 35% of the rms of the momentum transfers. In addition, we present a statistical analysis of the precision of first moment STEM as a function of dose. For typical experimental settings with recent hardware such as a Medipix3 Merlin camera attached to a probe-corrected STEM, we find that the precision of the measurement of momentum transfers stagnates above certain doses. This means that other instabilities such as specimen drift or scan noise have to be taken into account seriously for measurements that target, e.g., the detection of bonding effects in the charge density.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.843
Times cited: 25
DOI: 10.1016/J.ULTRAMIC.2018.12.018
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Guzzinati G, Ghielens W, Mahr C, Bé,ché, A, Rosenauer A, Calders T, Verbeeck J (2019) Electron Bessel beam diffraction patterns, line scan of Si/SiGe multilayer
Keywords: Dataset; ADReM Data Lab (ADReM); Electron microscopy for materials research (EMAT)
DOI: 10.5281/ZENODO.2566137
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“Atomic-scale quantification of charge densities in two-dimensional materials”. Müller-Caspary K, Duchamp M, Roesner M, Migunov V, Winkler F, Yang H, Huth M, Ritz R, Simson M, Ihle S, Soltau H, Wehling T, Dunin-Borkowski RE, Van Aert S, Rosenauer A, Physical review B 98, 121408 (2018). http://doi.org/10.1103/PHYSREVB.98.121408
Abstract: 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.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.836
Times cited: 10
DOI: 10.1103/PHYSREVB.98.121408
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“Strain analysis from nano-beam electron diffraction : influence of specimen tilt and beam convergence”. Grieb T, Krause FF, Schowalter M, Zillmann D, Sellin R, Müller-Caspary K, Mahr C, Mehrtens T, Bimberg D, Rosenauer A, Ultramicroscopy 190, 45 (2018). http://doi.org/10.1016/J.ULTRAMIC.2018.03.013
Abstract: 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. A two-tilt method which can be seen as lowest-order electron beam precession is suggested and experimentally implemented. Strain determination from NBED series with increasing beam convergence is performed in combination with the experimental realization of a probe-forming aperture with a cross inside. It is shown that using standard evaluation techniques, the influence of beam convergence on spatial resolution is lower than the influence of sharp rings around the diffraction disc which occur at interfaces and which are caused by the tails of the intensity distribution of the electron probe. (C) 2018 Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.843
Times cited: 1
DOI: 10.1016/J.ULTRAMIC.2018.03.013
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“Measurement of local crystal lattice strain variations in dealloyed nanoporous gold”. Mahr C, Müller-Caspary K, Graf M, Lackmann A, Grieb T, Schowalter M, Krause FF, Mehrtens T, Wittstock A, Weissmueller J, Rosenauer A, Materials research letters 6, 84 (2018). http://doi.org/10.1080/21663831.2017.1396263
Abstract: Reversible macroscopic length changes in nanoporous structures can be achieved by applying electric potentials or by exposing them to different gases or liquids. Thus, these materials are interesting candidates for applications as sensors or actuators. Macroscopic length changes originate from microscopic changes of crystal lattice parameters. In this report, we show spatially resolved measurements of crystal lattice strain in dealloyed nanoporous gold. The results confirm theory by indicating a compression of the lattice along the axis of cylindrically shaped ligaments and an expansion in radial direction. Furthermore, we show that curved npAu surfaces show inward relaxation of the surface layer. [GRAPHICS] .
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.773
Times cited: 4
DOI: 10.1080/21663831.2017.1396263
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“Quantitative HAADF STEM of SiGe in presence of amorphous surface layers from FIB preparation”. Grieb T, Tewes M, Schowalter M, Müller-Caspary K, Krause FF, Mehrtens T, Hartmann J-M, Rosenauer A, Ultramicroscopy 184, 29 (2018). http://doi.org/10.1016/J.ULTRAMIC.2017.09.012
Abstract: <script type='text/javascript'>document.write(unpmarked('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.'));
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.843
Times cited: 7
DOI: 10.1016/J.ULTRAMIC.2017.09.012
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“Interplay of morphology, composition, and optical properties of InP-based quantum dots emitting at the 1.55 \mum telecom wavelength”. Carmesin C, Schowalter M, Lorke M, Mourad D, Grieb T, Müller-Caspary K, Yacob M, Reithmaier JP, Benyoucef M, Rosenauer A, Jahnke F, Physical review B 96, 235309 (2017). http://doi.org/10.1103/PHYSREVB.96.235309
Abstract: <script type='text/javascript'>document.write(unpmarked('Results for the development and detailed analysis of self-organized InAs/InAlGaAs/InP quantum dots suitable for single-photon emission at the 1.55 mu 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.'));
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.836
Times cited: 3
DOI: 10.1103/PHYSREVB.96.235309
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“Determining oxygen relaxations at an interface: A comparative study between transmission electron microscopy techniques”. Gauquelin N, van den Bos KHW, Béché, A, Krause FF, Lobato I, Lazar S, Rosenauer A, Van Aert S, Verbeeck J, Ultramicroscopy 181, 178 (2017). http://doi.org/10.1016/j.ultramic.2017.06.002
Abstract: Nowadays, aberration corrected transmission electron microscopy (TEM) is a popular method to characterise nanomaterials at the atomic scale. Here, atomically resolved images of nanomaterials are acquired, where the contrast depends on the illumination, imaging and detector conditions of the microscope. Visualization of light elements is possible when using low angle annular dark field (LAADF) STEM, annular bright field (ABF) STEM, integrated differential phase contrast (iDPC) STEM, negative spherical aberration imaging (NCSI) and imaging STEM (ISTEM). In this work, images of a NdGaO3-La0.67Sr0.33MnO3 (NGO-LSMO) interface are quantitatively evaluated by using statistical parameter estimation theory. For imaging light elements, all techniques are providing reliable results, while the techniques based on interference contrast, NCSI and ISTEM, are less robust in terms of accuracy for extracting heavy column locations. In term of precision, sample drift and scan distortions mainly limits the STEM based techniques as compared to NCSI. Post processing techniques can, however, partially compensate for this. In order to provide an outlook to the future, simulated images of NGO, in which the unavoidable presence of Poisson noise is taken into account, are used to determine the ultimate precision. In this future counting noise limited scenario, NCSI and ISTEM imaging will provide more precise values as compared to the other techniques, which can be related to the mechanisms behind the image recording.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.843
Times cited: 34
DOI: 10.1016/j.ultramic.2017.06.002
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“Quantitative determination of residual silver distribution in nanoporous gold and its influence on structure and catalytic performance”. Mahr C, Kundu P, Lackmann A, Zanaga D, Thiel K, Schowalter M, Schwan M, Bals S, Wittstock A, Rosenauer A, Journal of catalysis 352, 52 (2017). http://doi.org/10.1016/j.jcat.2017.05.002
Abstract: Large efforts have been made trying to understand the origin of the high catalytic activity of dealloyed nanoporous gold as a green catalyst for the selective promotion of chemical reactions at low temperatures. Residual silver, left in the sample after dealloying of a gold-silver alloy, has been shown to have a strong influence on the activity of the catalyst. But the question of how the silver is distributed within the porous structure has not finally been answered yet. We show by quantitative energy dispersive X-ray tomography measurements that silver forms clusters that are distributed irregularly, both on the surface and inside the ligaments building up the porous structure. Furthermore, we find that the role of the residual silver is ambiguous. Whereas CO oxidation is supported by more residual silver, methanol oxidation to methyl formate is hindered. Structural characterisation reveals larger ligaments and pores for decreasing residual silver concentration.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 6.844
Times cited: 42
DOI: 10.1016/j.jcat.2017.05.002
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“Optimization of NBED simulations for disc-detection measurements”. Grieb T, Krause FF, Mahr C, Zillmann D, Müller-Caspary K, Schowalter M, Rosenauer A, Ultramicroscopy 181, 50 (2017). http://doi.org/10.1016/J.ULTRAMIC.2017.04.015
Abstract: 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.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.843
Times cited: 6
DOI: 10.1016/J.ULTRAMIC.2017.04.015
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“How precise can atoms of a nanocluster be located in 3D using a tilt series of scanning transmission electron microscopy images?”.Alania M, De Backer A, Lobato I, Krause FF, Van Dyck D, Rosenauer A, Van Aert S, Ultramicroscopy 181, 134 (2017). http://doi.org/10.1016/j.ultramic.2016.12.013
Abstract: In this paper, we investigate how precise atoms of a small nanocluster can ultimately be located in three dimensions (3D) from a tilt series of images acquired using annular dark field (ADF) scanning transmission electron microscopy (STEM). Therefore, we derive an expression for the statistical precision with which the 3D atomic position coordinates can be estimated in a quantitative analysis. Evaluating this statistical precision as a function of the microscope settings also allows us to derive the optimal experimental design. In this manner, the optimal angular tilt range, required electron dose, optimal detector angles, and number of projection images can be determined.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Vision lab
Impact Factor: 2.843
Times cited: 3
DOI: 10.1016/j.ultramic.2016.12.013
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“Locating light and heavy atomic column positions with picometer precision using ISTEM”. van den Bos KHW, Krause FF, Béché, A, Verbeeck J, Rosenauer A, Van Aert S, Ultramicroscopy 172, 75 (2016). http://doi.org/10.1016/j.ultramic.2016.10.003
Abstract: Recently, imaging scanning transmission electron microscopy (ISTEM) has been proposed as a promising new technique combining the advantages of conventional TEM (CTEM) and STEM [1]. The ability to visualize light and heavy elements together makes it a particularly interesting new, spatially incoherent imaging mode. Here, we evaluate this technique in term of precision with which atomic column locations can be measured. By using statistical parameter estimation theory, we will show that these locations can be accurately measured with a precision in the picometer range. Furthermore, a quantitative comparison is made with HAADF STEM imaging to investigate the advantages of ISTEM.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.843
Times cited: 8
DOI: 10.1016/j.ultramic.2016.10.003
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“Measurement of atomic electric fields and charge densities from average momentum transfers using scanning transmission electron microscopy”. Muller-Caspary K, Krause FF, Grieb T, Loffler S, Schowalter M, Béché, A, Galioit V, Marquardt D, Zweck J, Schattschneider P, Verbeeck J, Rosenauer A, Ultramicroscopy 178, 62 (2016). http://doi.org/10.1016/j.ultramic.2016.05.004
Abstract: 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 5mrad per pixel is sufficient in typical applications, corresponding to approximately 10x10 available pixels.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.843
Times cited: 93
DOI: 10.1016/j.ultramic.2016.05.004
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“Homogeneity and composition of AlInGaN : a multiprobe nanostructure study”. Krause FF, Ahl JP, Tytko D, Choi PP, Egoavil R, Schowalter M, Mehrtens T, Müller-Caspary K, Verbeeck J, Raabe D, Hertkorn J, Engl K, Rosenauer A, Ultramicroscopy 156, 29 (2015). http://doi.org/10.1016/j.ultramic.2015.04.012
Abstract: 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.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.843
Times cited: 11
DOI: 10.1016/j.ultramic.2015.04.012
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“Atomic electric fields revealed by a quantum mechanical approach to electron picodiffraction”. Mueller K, Krause FF, Béché, A, Schowalter M, Galioit V, Loeffler S, Verbeeck J, Zweck J, Schattschneider P, Rosenauer A, Nature communications 5, 5653 (2014). http://doi.org/10.1038/ncomms6653
Abstract: By focusing electrons on probes with a diameter of 50 pm, aberration-corrected scanning transmission electron microscopy (STEM) is currently crossing the border to probing subatomic details. A major challenge is the measurement of atomic electric fields using differential phase contrast (DPC) microscopy, traditionally exploiting the concept of a field- induced shift of diffraction patterns. Here we present a simplified quantum theoretical interpretation of DPC. This enables us to calculate the momentum transferred to the STEM probe from diffracted intensities recorded on a pixel array instead of conventional segmented bright- field detectors. The methodical development yielding atomic electric field, charge and electron density is performed using simulations for binary GaN as an ideal model system. We then present a detailed experimental study of SrTiO3 yielding atomic electric fields, validated by comprehensive simulations. With this interpretation and upgraded instrumentation, STEM is capable of quantifying atomic electric fields and high-contrast imaging of light atoms.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 12.124
Times cited: 197
DOI: 10.1038/ncomms6653
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“Optimal experimental design for the detection of light atoms from high-resolution scanning transmission electron microscopy images”. Gonnissen J, de Backer A, den Dekker AJ, Martinez GT, Rosenauer A, Sijbers J, Van Aert S, Applied physics letters 105, 063116 (2014). http://doi.org/10.1063/1.4892884
Abstract: We report an innovative method to explore the optimal experimental settings to detect light atoms from scanning transmission electron microscopy (STEM) images. Since light elements play a key role in many technologically important materials, such as lithium-battery devices or hydrogen storage applications, much effort has been made to optimize the STEM technique in order to detect light elements. Therefore, classical performance criteria, such as contrast or signal-to-noise ratio, are often discussed hereby aiming at improvements of the direct visual interpretability. However, when images are interpreted quantitatively, one needs an alternative criterion, which we derive based on statistical detection theory. Using realistic simulations of technologically important materials, we demonstrate the benefits of the proposed method and compare the results with existing approaches.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Vision lab
Impact Factor: 3.411
Times cited: 12
DOI: 10.1063/1.4892884
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“A memory efficient method for fully three-dimensional object reconstruction with HAADF STEM”. Van den Broek W, Rosenauer A, Van Aert S, Sijbers J, van Dyck D, Ultramicroscopy 141, 22 (2014). http://doi.org/10.1016/j.ultramic.2014.03.008
Abstract: The conventional approach to object reconstruction through electron tomography is to reduce the three-dimensional problem to a series of independent two-dimensional slice-by-slice reconstructions. However, at atomic resolution the image of a single atom extends over many such slices and incorporating this image as prior knowledge in tomography or depth sectioning therefore requires a fully three-dimensional treatment. Unfortunately, the size of the three-dimensional projection operator scales highly unfavorably with object size and readily exceeds the available computer memory. In this paper, it is shown that for incoherent image formation the memory requirement can be reduced to the fundamental lower limit of the object size, both for tomography and depth sectioning. Furthermore, it is shown through multislice calculations that high angle annular dark field scanning transmission electron microscopy can be sufficiently incoherent for the reconstruction of single element nanocrystals, but that dynamical diffraction effects can cause classification problems if more than one element is present. (C) 2014 Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Vision lab
Impact Factor: 2.843
Times cited: 6
DOI: 10.1016/j.ultramic.2014.03.008
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“The effect of probe inaccuracies on the quantitative model-based analysis of high angle annular dark field scanning transmission electron microscopy images”. Martinez GT, de Backer A, Rosenauer A, Verbeeck J, Van Aert S, Micron 63, 57 (2014). http://doi.org/10.1016/j.micron.2013.12.009
Abstract: Quantitative structural and chemical information can be obtained from high angle annular dark field scanning transmission electron microscopy (HAADF STEM) images when using statistical parameter estimation theory. In this approach, we assume an empirical parameterized imaging model for which the total scattered intensities of the atomic columns are estimated. These intensities can be related to the material structure or composition. Since the experimental probe profile is assumed to be known in the description of the imaging model, we will explore how the uncertainties in the probe profile affect the estimation of the total scattered intensities. Using multislice image simulations, we analyze this effect for Cs corrected and non-Cs corrected microscopes as a function of inaccuracies in cylindrically symmetric aberrations, such as defocus and spherical aberration of third and fifth order, and non-cylindrically symmetric aberrations, such as 2-fold and 3-fold astigmatism and coma.
Keywords: A1 Journal article; Engineering Management (ENM); Electron microscopy for materials research (EMAT)
Impact Factor: 1.98
Times cited: 25
DOI: 10.1016/j.micron.2013.12.009
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“Quantitative composition determination at the atomic level using model-based high-angle annular dark field scanning transmission electron microscopy”. Martinez GT, Rosenauer A, de Backer A, Verbeeck J, Van Aert S, Ultramicroscopy 137, 12 (2014). http://doi.org/10.1016/j.ultramic.2013.11.001
Abstract: High angle annular dark field scanning transmission electron microscopy (HAADF STEM) images provide sample information which is sensitive to the chemical composition. The image intensities indeed scale with the mean atomic number Z. To some extent, chemically different atomic column types can therefore be visually distinguished. However, in order to quantify the atomic column composition with high accuracy and precision, model-based methods are necessary. Therefore, an empirical incoherent parametric imaging model can be used of which the unknown parameters are determined using statistical parameter estimation theory (Van Aert et al., 2009, [1]). In this paper, it will be shown how this method can be combined with frozen lattice multislice simulations in order to evolve from a relative toward an absolute quantification of the composition of single atomic columns with mixed atom types. Furthermore, the validity of the model assumptions are explored and discussed.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.843
Times cited: 74
DOI: 10.1016/j.ultramic.2013.11.001
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“Atom counting in HAADF STEM using a statistical model-based approach : methodology, possibilities, and inherent limitations”. de Backer A, Martinez GT, Rosenauer A, Van Aert S, Ultramicroscopy 134, 23 (2013). http://doi.org/10.1016/j.ultramic.2013.05.003
Abstract: In the present paper, a statistical model-based method to count the number of atoms of monotype crystalline nanostructures from high resolution high-angle annular dark-field (HAADF) scanning transmission electron microscopy (STEM) images is discussed in detail together with a thorough study on the possibilities and inherent limitations. In order to count the number of atoms, it is assumed that the total scattered intensity scales with the number of atoms per atom column. These intensities are quantitatively determined using model-based statistical parameter estimation theory. The distribution describing the probability that intensity values are generated by atomic columns containing a specific number of atoms is inferred on the basis of the experimental scattered intensities. Finally, the number of atoms per atom column is quantified using this estimated probability distribution. The number of atom columns available in the observed STEM image, the number of components in the estimated probability distribution, the width of the components of the probability distribution, and the typical shape of a criterion to assess the number of components in the probability distribution directly affect the accuracy and precision with which the number of atoms in a particular atom column can be estimated. It is shown that single atom sensitivity is feasible taking the latter aspects into consideration.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.843
Times cited: 48
DOI: 10.1016/j.ultramic.2013.05.003
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“Procedure to count atoms with trustworthy single-atom sensitivity”. Van Aert S, de Backer A, Martinez GT, Goris B, Bals S, Van Tendeloo G, Rosenauer A, Physical review : B : condensed matter and materials physics 87, 064107 (2013). http://doi.org/10.1103/PhysRevB.87.064107
Abstract: We report a method to reliably count the number of atoms from high-angle annular dark field scanning transmission electron microscopy images. A model-based analysis of the experimental images is used to measure scattering cross sections at the atomic level. The high sensitivity of these measurements in combination with a thorough statistical analysis enables us to count atoms with single-atom sensitivity. The validity of the results is confirmed by means of detailed image simulations. We will show that the method can be applied to nanocrystals of arbitrary shape, size, and atom type without the need for a priori knowledge about the atomic structure.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.836
Times cited: 106
DOI: 10.1103/PhysRevB.87.064107
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“Correction of non-linear thickness effects in HAADF STEM electron tomography”. van den Broek W, Rosenauer A, Goris B, Martinez GT, Bals S, Van Aert S, van Dyck D, Ultramicroscopy 116, 8 (2012). http://doi.org/10.1016/j.ultramic.2012.03.005
Abstract: In materials science, high angle annular dark field scanning transmission electron microscopy is often used for tomography at the nanometer scale. In this work, it is shown that a thickness dependent, non-linear damping of the recorded intensities occurs. This results in an underestimated intensity in the interior of reconstructions of homogeneous particles, which is known as the cupping artifact. In this paper, this non-linear effect is demonstrated in experimental images taken under common conditions and is reproduced with a numerical simulation. Furthermore, an analytical derivation shows that these non-linearities can be inverted if the imaging is done quantitatively, thus preventing cupping in the reconstruction.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Vision lab
Impact Factor: 2.843
Times cited: 67
DOI: 10.1016/j.ultramic.2012.03.005
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“Computational aspects in quantitative EELS”. Verbeeck J, Van Aert S, Zhang L, Haiyan T, Schattschneider P, Rosenauer A, Microscopy and microanalysis 16, 240 (2010). http://doi.org/10.1017/S143192761005511X
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 1.891
DOI: 10.1017/S143192761005511X
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“Refinement of chemically sensitive structure factors using parallel and convergent beam electron nanodiffraction”. Müller K, Schowalter M, Rosenauer A, Jansen J, Tsuda K, Titantah JT, Lamoen D, Journal of physics : conference series 209, 012025 (2010). http://doi.org/10.1088/1742-6596/209/1/012025
Abstract: We introduce a new method to measure structure factors from parallel beam electron diffraction (PBED) patterns. Bloch wave refinement routines were developed which can minimise the difference between simulated and experimental Bragg intensities via variation of structure factors, Debye parameters, specimen thickness and -orientation. Due to plane wave illumination, the PBED refinement is highly efficient not only in computational respect, but also concerning the experimental effort since energy filtering is shown to have no significant effect on the refinement results. The PBED method was applied to simulated GaAs diffraction patterns to derive systematic errors and rules for the identification of plausible refinement results. The evaluation of experimental GaAs PBED patterns yields a 200 X-ray structure factor of -6.33±0.14. Additionally, we obtained -6.35±0.13 from two-dimensional convergent beam electron diffraction refinements. Both results confirm density functional theory calculations published by Rosenauer et al. and indicate the inaccuracy of isolated atom scattering data, which is crucial e.g. for the composition evaluation by lattice fringe analysis.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
DOI: 10.1088/1742-6596/209/1/012025
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“Ab initio based atomic scattering amplitudes and {002} electron structure factors of InxGa1-xAs/GaAs quantum wells”. Titantah JT, Lamoen D, Schowalter M, Rosenauer A, Journal of physics : conference series 209, 012040 (2010). http://doi.org/10.1088/1742-6596/209/1/012040
Abstract: The atomic scattering amplitudes of the various atoms of the systems Ga1−xInxAs, GaAs1−xNx and InAs1−xNx are calculated using the density functional theory (DFT) approach. The scattering amplitudes of N, Ga, As and In in the model systems are compared with the frequently used Doyle and Turner values. Deviation from the latter values is found for small scattering vectors (s<0.3Å−1) and for these scattering vectors dependence on the orientation of the scattering vector and the chemical environment is reported. We suggest a parametrization of these modified scattering amplitudes (MASAs) for small scattering vectors (s<1.0Å−1). The MASAs are exploited within zero pressure classical Metropolis Monte Carlo (MC), finite temperature calculations to investigate the effect of quantum well size on the electron {002} structure factor (SF) of Ga1−xInxAs quantum wells.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
DOI: 10.1088/1742-6596/209/1/012040
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“Density-functional theory calculations of the electron energy-loss near-edge structure of Li-intercalated graphite”. Titantah JT, Lamoen D, Schowalter M, Rosenauer A, Carbon 47, 2501 (2009). http://doi.org/10.1016/j.carbon.2009.05.002
Abstract: We have studied the structural and electronic properties of lithium-intercalated graphite (LIG) for various Li content. Atomic relaxation shows that Li above the center of the carbon hexagon in a AAAA stacked graphite is the only stable Li configuration in stage 1 intercalated graphite. Lithium and Carbon 1s energy-loss near-edge structure (ELNES) calculations are performed on the Li-intercalated graphite using the core-excited density-functional theory formulation. Several features of the Li 1s ELNES are correlated with reported experimental features. The ELNES spectra of Li is found to be electron beam orientation sensitive and this property is used to assign the origin of the various Li 1s ELNES features. Information about core-hole screening by the valence electrons and charge transfer in the LIG systems is obtained from the C 1s ELNES and valence charge density difference calculations, respectively.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 6.337
Times cited: 12
DOI: 10.1016/j.carbon.2009.05.002
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“Modified atomic scattering amplitudes and size effects on the 002 and 220 electron structure factors of multiple Ga1-xInxAs/GaAs quantum wells”. Titantah JT, Lamoen D, Schowalter M, Rosenauer A, Journal of applied physics 105, 084310 (2009). http://doi.org/10.1063/1.3115407
Abstract: The modified atomic scattering amplitudes (MASAs) of mixed Ga<sub>1-x</sub>In<sub>x</sub>As, GaAs<sub>1-x</sub>N<sub>x</sub>, and InAs<sub>1-x</sub>N<sub>x</sub> are calculated using the density functional theory approach and the results are compared with those of the binary counterparts. The MASAs of N, Ga, As, and In for various scattering vectors in various chemical environments and in the zinc-blende structure are compared with the frequently used Doyle and Turner values. Deviation from the Doyle and Turner results is found for small scattering vectors (s<0.3 Å<sup>-1</sup>) and for these scattering vectors the MASAs are found to be sensitive to the orientation of the scattering vector and on the chemical environment. The chemical environment sensitive MASAs are used within zero pressure classical Metropolis Monte Carlo, finite temperature calculations to investigate the effect of well size on the electron 002 and 220 structure factors (SFs). The implications of the use of the 002 (200) spot for the quantification of nanostructured Ga<sub>1-x</sub>In<sub>x</sub>As systems are examined while the 220 SF across the well is evaluated and is found to be very sensitive to the in-plane static displacements.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.068
DOI: 10.1063/1.3115407
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“Refinement of the 200 structure factor for GaAs using parallel and convergent beam electron nanodiffraction data”. Müller K, Schowalter M, Jansen J, Tsuda K, Titantah J, Lamoen D, Rosenauer A, Ultramicroscopy 109, 802 (2009). http://doi.org/10.1016/j.ultramic.2009.03.029
Abstract: We present a new method to measure structure factors from electron spot diffraction patterns recorded under almost parallel illumination in transmission electron microscopes. Bloch wave refinement routines have been developed to refine the crystal thickness, its orientation and structure factors by comparison of experimentally recorded and calculated intensities. Our method requires a modicum of computational effort, making it suitable for contemporary personal computers. Frozen lattice and Bloch wave simulations of GaAs diffraction patterns are used to derive optimised experimental conditions. Systematic errors are estimated from the application of the method to simulated diffraction patterns and rules for the recognition of physically reasonable initial refinement conditions are derived. The method is applied to the measurement of the 200 structure factor for GaAs. We found that the influence of inelastically scattered electrons is negligible. Additionally, we measured the 200 structure factor from zero loss filtered two-dimensional convergent beam electron diffraction patterns. The precision of both methods is found to be comparable and the results agree well with each other. A deviation of more than 20% from isolated atom scattering data is observed, whereas close agreement is found with structure factors obtained from density functional theory [A. Rosenauer, M. Schowalter, F. Glas, D. Lamoen, Phys. Rev. B 72 (2005), 085326-1], which account for the redistribution of electrons due to chemical bonding via modified atomic scattering amplitudes.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.843
Times cited: 8
DOI: 10.1016/j.ultramic.2009.03.029
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