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Author | De Backer, A.; Van Aert, S.; Faes, C.; Arslan Irmak, E.; Nellist, P.D.; Jones, L. | ||||
Title | Experimental reconstructions of 3D atomic structures from electron microscopy images using a Bayesian genetic algorithm | Type | A1 Journal article | ||
Year | 2022 | Publication | N P J Computational Materials | Abbreviated Journal | npj Comput Mater |
Volume | 8 | Issue | 1 | Pages | 216 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | We introduce a Bayesian genetic algorithm for reconstructing atomic models of monotype crystalline nanoparticles from a single projection using Z-contrast imaging. The number of atoms in a projected atomic column obtained from annular dark field scanning transmission electron microscopy images serves as an input for the initial three-dimensional model. The algorithm minimizes the energy of the structure while utilizing a priori information about the finite precision of the atom-counting results and neighbor-mass relations. The results show promising prospects for obtaining reliable reconstructions of beam-sensitive nanoparticles during dynamical processes from images acquired with sufficiently low incident electron doses. | ||||
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Language | Wos | 000866500900001 | Publication Date | 2022-10-12 | |
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ISSN | 2057-3960 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | Times cited | Open Access | OpenAccess | ||
Notes | This work was supported by the European Research Council (Grant 770887 PICOMETRICS to S.V.A. and Grant 823717 ESTEEM3). The authors acknowledge financial support from the Research Foundation Flanders (FWO, Belgium) through project fundings (G.0267.18N, G.0502.18N, G.0346.21N) and a postdoctoral grant to A.D.B. L.J. acknowledges Science Foundation Ireland (SFI – grant number URF/RI/191637), the Royal Society, and the AMBER Centre. The authors acknowledge Aakash Varambhia for his assistance and expertise with the experimental recording and use of characterization facilities within the David Cockayne Centre for Electron Microscopy, Department of Materials, University of Oxford, and in particular the EPSRC (EP/K040375/1 South of England Analytical Electron Microscope).; esteem3reported; esteem3JRA | Approved | Most recent IF: NA | ||
Call Number | EMAT @ emat @c:irua:191398 | Serial | 7114 | ||
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Author | De wael, A.; De Backer, A.; Yu, C.-P.; Sentürk, D.G.; Lobato, I.; Faes, C.; Van Aert, S. | ||||
Title | Three Approaches for Representing the Statistical Uncertainty on Atom-Counting Results in Quantitative ADF STEM | Type | A1 Journal article | ||
Year | 2022 | Publication | Microscopy and microanalysis | Abbreviated Journal | Microsc Microanal |
Volume | Issue | Pages | 1-9 | ||
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | A decade ago, a statistics-based method was introduced to count the number of atoms from annular dark-field scanning transmission electron microscopy (ADF STEM) images. In the past years, this method was successfully applied to nanocrystals of arbitrary shape, size, and composition (and its high accuracy and precision has been demonstrated). However, the counting results obtained from this statistical framework are so far presented without a visualization of the actual uncertainty about this estimate. In this paper, we present three approaches that can be used to represent counting results together with their statistical error, and discuss which approach is most suited for further use based on simulations and an experimental ADF STEM image. | ||||
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Language | Wos | 000854930500001 | Publication Date | 2022-09-19 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1431-9276 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 2.8 | Times cited | Open Access | OpenAccess | |
Notes | This project has received funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation programme (Grant Agreement No. 770887 and No. 823717 ESTEEM3). The authors acknowledge financial support from the Research Foundation Flanders (FWO, Belgium) through grants to A.D.w. and A.D.B. and projects G.0502.18N, G.0267.18N, and EOS 30489208. S.V.A. acknowledges TOP BOF funding from the University of Antwerp. The authors are grateful to L.M. Liz-Marzán (CIC biomaGUNE and Ikerbasque) for providing the samples. esteem3reported; esteem3jra | Approved | Most recent IF: 2.8 | ||
Call Number | EMAT @ emat @c:irua:190585 | Serial | 7119 | ||
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Author | Sentürk, D.G.; De Backer, A.; Friedrich, T.; Van Aert, S. | ||||
Title | Optimal experiment design for element specific atom counting using multiple annular dark field scanning transmission electron microscopy detectors | Type | A1 Journal article | ||
Year | 2022 | Publication | Ultramicroscopy | Abbreviated Journal | Ultramicroscopy |
Volume | 242 | Issue | Pages | 113626 | |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | This paper investigates the possible benefits for counting atoms of different chemical nature when analysing multiple 2D scanning transmission electron microscopy (STEM) images resulting from independent annular dark field (ADF) detector regimes. To reach this goal, the principles of statistical detection theory are used to quantify the probability of error when determining the number of atoms in atomic columns consisting of multiple types of elements. In order to apply this theory, atom-counting is formulated as a statistical hypothesis test, where each hypothesis corresponds to a specific number of atoms of each atom type in an atomic column. The probability of error, which is limited by the unavoidable presence of electron counting noise, can then be computed from scattering-cross sections extracted from multiple ADF STEM images. Minimisation of the probability of error as a function of the inner and outer angles of a specified number of independent ADF collection regimes results in optimal experimental designs. Based on simulations of spherical Au@Ag and Au@Pt core–shell nanoparticles, we investigate how the combination of two non-overlapping detector regimes helps to improve the probability of error when unscrambling two types of atoms. In particular, the combination of a narrow low angle ADF detector with a detector formed by the remaining annular collection regime is found to be optimal. The benefit is more significant if the atomic number Z difference becomes larger. In addition, we show the benefit of subdividing the detector regime into three collection areas for heterogeneous nanostructures based on a structure consisting of three types of elements, e.g., a mixture of Au, Ag and Al atoms. Finally, these results are compared with the probability of error resulting when one would ultimately use a pixelated 4D STEM detector and how this could help to further reduce the incident electron dose. |
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000873778100001 | Publication Date | 0000-00-00 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0304-3991 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 2.2 | Times cited | Open Access | OpenAccess | |
Notes | This work was supported by the European Research Council (Grant 770887 PICOMETRICS to S. Van Aert and Grant 823717 ESTEEM3). The authors acknowledge financial support from the Research Foundation Flanders (FWO, Belgium) through project fundings (G.0346.21N and EOS 30489208) and a postdoctoral grant to A. De Backer. S. Van Aert acknowledges funding from the University of Antwerp Research fund (BOF).; esteem3reported; esteem3jra | Approved | Most recent IF: 2.2 | ||
Call Number | EMAT @ emat @c:irua:190925 | Serial | 7118 | ||
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Author | Liu, P.; Arslan Irmak, E.; De Backer, A.; De wael, A.; Lobato, I.; Béché, A.; Van Aert, S.; Bals, S. | ||||
Title | Three-dimensional atomic structure of supported Au nanoparticles at high temperature | Type | A1 Journal article | ||
Year | 2021 | Publication | Nanoscale | Abbreviated Journal | Nanoscale |
Volume | 13 | Issue | Pages | ||
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | Au nanoparticles (NPs) deposited on CeO2 are extensively used as thermal catalysts since the morphology of the NPs is expected to be stable at elevated temperatures. Although it is well known that the activity of Au NPs depends on their size and surface structure, their three-dimensional (3D) structure at the atomic scale has not been completely characterized as a function of temperature. In this paper, we overcome the limitations of conventional electron tomography by combining atom counting applied to aberration-corrected scanning transmission electron microscopy images and molecular dynamics relaxation. In this manner, we are able to perform an atomic resolution 3D investigation of supported Au NPs. Our results enable us to characterize the 3D equilibrium structure of single NPs as a function of temperature. Moreover, the dynamic 3D structural evolution of the NPs at high temperatures, including surface layer jumping and crystalline transformations, has been studied. | ||||
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Language | Wos | 000612999200029 | Publication Date | 2020-12-29 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2040-3364 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 7.367 | Times cited | 13 | Open Access | OpenAccess |
Notes | This work was supported by the European Research Council (Grant 815128 REALNANO to SB, Grant 770887 PICOMETRICS to SVA, Grant 823717 ESTEEM3). The authors acknowledge financial support from the Research Foundation Flanders (FWO, Belgium) through grants to A. D. w. and A. D. B. and project funding G.0267.18N.; sygma; esteem3JRA; esteem3reported | Approved | Most recent IF: 7.367 | ||
Call Number | EMAT @ emat @c:irua:174858 | Serial | 6665 | ||
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Author | Albrecht, W.; Van Aert, S.; Bals, S. | ||||
Title | Three-Dimensional Nanoparticle Transformations Captured by an Electron Microscope | Type | A1 Journal article | ||
Year | 2021 | Publication | Accounts Of Chemical Research | Abbreviated Journal | Accounts Chem Res |
Volume | 54 | Issue | 5 | Pages | 1189-1199 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000626269900011 | Publication Date | 2021-03-02 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0001-4842 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 20.268 | Times cited | 12 | Open Access | OpenAccess |
Notes | The authors acknowledge funding from the European Research Council under the European Union’s Horizon 2020 research and innovation program (ERC Consolidator Grants No. 815128–REALNANO and No. 770887–PICOMETRICS), the Research Foundation Flanders (FWO, G.0267.18N), and the European Commission (EUSMI). The authors furthermore acknowledge funding from the European Union’s Horizon 2020 research and innovation program, ESTEEM3. The authors also acknowledge contributions from all co-workers that have contributed over the years: Thomas Altantzis, Annick De Backer, Joost Batenburg and co-workers, Armand Béché, Eva Bladt, Lewys Jones and co-workers, Luis Liz-Marzán and co-workers, Ivan Lobato, Thais Milagres de Oliveira, Peter Nellist and co-workers, Hugo Pérez Garza and co-workers, Alexander Skorikov, Sara Skrabalak and co-workers, Sandra Van Aert, Alfons van Blaaderen and co-workers, Hans Vanrompay, Staf Van Tendeloo, and Johan Verbeeck.; sygmaSB; | Approved | Most recent IF: 20.268 | ||
Call Number | EMAT @ emat @c:irua:177644 | Serial | 6752 | ||
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Author | Fatermans, J.; de Backer, A.; den Dekker, A.J.; Van Aert, S. | ||||
Title | Atom column detection | Type | H2 Book chapter | ||
Year | 2021 | Publication | Advances in imaging and electron physics T2 – Advances in imaging and electron physics | Abbreviated Journal | |
Volume | Issue | Pages | 177-214 | ||
Keywords | H2 Book chapter; Electron microscopy for materials research (EMAT); Vision lab | ||||
Abstract | By combining statistical parameter estimation and model-order selection using a Bayesian framework, the maximum a posteriori (MAP) probability rule is proposed in this chapter as an objective and quantitative method to detect atom columns from high-resolution scanning transmission electron microscopy (HRSTEM) images. The validity and usefulness of this approach is demonstrated to both simulated and experimental annular dark-field (ADF) STEM images, but also to simultaneously acquired annular bright-field (ABF) and ADF STEM image data. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2021-03-06 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | 217 | Series Issue | Edition | ||
ISSN | ISBN | 978-0-12-824607-8; 1076-5670 | Additional Links | UA library record | |
Impact Factor | Times cited | Open Access | Not_Open_Access | ||
Notes | ERC Consolidator project funded by the European Union grant #770887 Picometrics | Approved | Most recent IF: NA | ||
Call Number | UA @ admin @ c:irua:177531 | Serial | 6775 | ||
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Author | de Backer, A.; Fatermans, J.; den Dekker, A.J.; Van Aert, S. | ||||
Title | Atom counting | Type | H2 Book chapter | ||
Year | 2021 | Publication | Advances in imaging and electron physics T2 – Advances in imaging and electron physics | Abbreviated Journal | |
Volume | Issue | Pages | 91-144 | ||
Keywords | H2 Book chapter; Electron microscopy for materials research (EMAT); Vision lab | ||||
Abstract | In this chapter, a statistical model-based method to count the number of atoms of monotype crystalline nanostructures from high-resolution annular dark-field (ADF) scanning transmission electron microscopy (STEM) images is discussed in detail together with a thorough study on the possibilities and inherent limitations. We show that this method can be applied to nanocrystals of arbitrary shape, size, and atom type. The validity of the atom-counting results is confirmed by means of detailed image simulations and it is shown that the high sensitivity of our method enables us to count atoms with single atom sensitivity. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2021-03-06 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | 217 | Series Issue | Edition | ||
ISSN | ISBN | 978-0-12-824607-8; 1076-5670 | Additional Links | UA library record | |
Impact Factor | Times cited | Open Access | Not_Open_Access | ||
Notes | ERC Consolidator project funded by the European Union grant #770887 Picometrics | Approved | Most recent IF: NA | ||
Call Number | UA @ admin @ c:irua:177529 | Serial | 6776 | ||
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Author | de Backer, A.; Fatermans, J.; den Dekker, A.J.; Van Aert, S. | ||||
Title | Efficient fitting algorithm | Type | H2 Book chapter | ||
Year | 2021 | Publication | Advances in imaging and electron physics T2 – Advances in imaging and electron physics | Abbreviated Journal | |
Volume | Issue | Pages | 73-90 | ||
Keywords | H2 Book chapter; Electron microscopy for materials research (EMAT) | ||||
Abstract | An efficient model-based estimation algorithm is introduced to quantify the atomic column positions and intensities from atomic-resolution (scanning) transmission electron microscopy ((S)TEM) images. This algorithm uses the least squares estimator on image segments containing individual columns fully accounting for overlap between neighboring columns, enabling the analysis of a large field of view. To provide end-users with this well-established quantification method, a user friendly program, StatSTEM, is developed which is freely available under a GNU public license. In this chapter, this efficient algorithm is applied to three different nanostructures for which the analysis of a large field of view is required. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2021-03-06 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | 217 | Series Issue | Edition | ||
ISSN | ISBN | 978-0-12-824607-8; 1076-5670 | Additional Links | UA library record | |
Impact Factor | Times cited | Open Access | Not_Open_Access | ||
Notes | ERC Consolidator project funded by the European Union grant #770887 Picometrics | Approved | Most recent IF: NA | ||
Call Number | UA @ admin @ c:irua:177528 | Serial | 6778 | ||
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Author | de Backer, A.; Fatermans, J.; den Dekker, A.J.; Van Aert, S. | ||||
Title | General conclusions and future perspectives | Type | H2 Book chapter | ||
Year | 2021 | Publication | Advances in imaging and electron physics T2 – Advances in imaging and electron physics | Abbreviated Journal | |
Volume | Issue | Pages | 243-253 | ||
Keywords | H2 Book chapter; Electron microscopy for materials research (EMAT); Vision lab | ||||
Abstract | This chapter provides an overview of statistical and quantitative methodologies that have pushed (scanning) transmission electron microscopy ((S)TEM) toward accurate and precise measurements of unknown structure parameters for understanding the relation between the structure of a material and its properties. Hereby, statistical parameter estimation theory has extensively been used which enabled not only measuring atomic column positions, but also quantifying the number of atoms, and detecting atomic columns as accurately and precisely as possible from experimental images. As a general conclusion, it can be stated that advanced statistical techniques are ideal tools to perform quantitative electron microscopy at the atomic scale. In the future, statistical methods will continue to be developed and novel quantification procedures will open up new possibilities for studying material structures at the atomic scale. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2021-03-06 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | 217 | Series Issue | Edition | ||
ISSN | ISBN | 978-0-12-824607-8; 1076-5670 | Additional Links | UA library record | |
Impact Factor | Times cited | Open Access | Not_Open_Access | ||
Notes | ERC Consolidator project funded by the European Union grant #770887 Picometrics | Approved | Most recent IF: NA | ||
Call Number | UA @ admin @ c:irua:177533 | Serial | 6781 | ||
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Author | Fatermans, J.; de Backer, A.; den Dekker, A.J.; Van Aert, S. | ||||
Title | Image-quality evaluation and model selection with maximum a posteriori probability | Type | H2 Book chapter | ||
Year | 2021 | Publication | Advances in imaging and electron physics T2 – Advances in imaging and electron physics | Abbreviated Journal | |
Volume | Issue | Pages | 215-242 | ||
Keywords | H2 Book chapter; Electron microscopy for materials research (EMAT); Vision lab | ||||
Abstract | The maximum a posteriori (MAP) probability rule for atom column detection can also be used as a tool to evaluate the relation between scanning transmission electron microscopy (STEM) image quality and atom detectability. In this chapter, a new image-quality measure is proposed that correlates well with atom detectability, namely the integrated contrast-to-noise ratio (ICNR). Furthermore, the working principle of the MAP probability rule is described in detail showing a close relation to the principles of model-selection methods. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2021-03-06 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | 217 | Series Issue | Edition | ||
ISSN | ISBN | 978-0-12-824607-8; 1076-5670 | Additional Links | UA library record | |
Impact Factor | Times cited | Open Access | Not_Open_Access | ||
Notes | ERC Consolidator project funded by the European Union grant #770887 Picometrics | Approved | Most recent IF: NA | ||
Call Number | UA @ admin @ c:irua:177532 | Serial | 6782 | ||
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Author | de Backer, A.; Fatermans, J.; den Dekker, A.J.; Van Aert, S. | ||||
Title | Introduction | Type | H2 Book chapter | ||
Year | 2021 | Publication | Advances in imaging and electron physics T2 – Advances in imaging and electron physics | Abbreviated Journal | |
Volume | Issue | Pages | 1-28 | ||
Keywords | H2 Book chapter; Electron microscopy for materials research (EMAT) | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2021-03-06 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | 217 | Series Issue | Edition | ||
ISSN | ISBN | 978-0-12-824607-8; 1076-5670 | Additional Links | UA library record | |
Impact Factor | Times cited | Open Access | Not_Open_Access | ||
Notes | ERC Consolidator project funded by the European Union grant #770887 Picometrics | Approved | Most recent IF: NA | ||
Call Number | UA @ admin @ c:irua:177525 | Serial | 6784 | ||
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Author | de Backer, A.; Fatermans, J.; den Dekker, A.J.; Van Aert, S. | ||||
Title | Optimal experiment design for nanoparticle atom counting from ADF STEM images | Type | H2 Book chapter | ||
Year | 2021 | Publication | Advances in imaging and electron physics T2 – Advances in imaging and electron physics | Abbreviated Journal | |
Volume | Issue | Pages | 145-175 | ||
Keywords | H2 Book chapter; Electron microscopy for materials research (EMAT); Vision lab | ||||
Abstract | In this chapter, the principles of detection theory are used to quantify the probability of error for atom counting from high-resolution scanning transmission electron microscopy (HRSTEM) images. Binary and multiple hypothesis testing have been investigated in order to determine the limits to the precision with which the number of atoms in a projected atomic column can be estimated. The probability of error has been calculated when using STEM images, scattering cross-sections or peak intensities as a criterion to count atoms. Based on this analysis, we conclude that scattering cross-sections perform almost equally well as images and perform better than peak intensities. Furthermore, the optimal STEM detector design can be derived for atom counting using the expression of the probability of error. We show that for very thin objects the low-angle annular dark-field (LAADF) regime is optimal and that for thicker objects the optimal inner detector angle increases. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2021-03-06 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | 217 | Series Issue | Edition | ||
ISSN | ISBN | 978-0-12-824607-8; 1076-5670 | Additional Links | UA library record | |
Impact Factor | Times cited | Open Access | Not_Open_Access | ||
Notes | ERC Consolidator project funded by the European Union grant #770887 Picometrics | Approved | Most recent IF: NA | ||
Call Number | UA @ admin @ c:irua:177530 | Serial | 6785 | ||
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Author | de Backer, A.; Fatermans, J.; den Dekker, A.J.; Van Aert, S. | ||||
Title | Statistical parameter estimation theory : principles and simulation studies | Type | H2 Book chapter | ||
Year | 2021 | Publication | Advances in imaging and electron physics T2 – Advances in imaging and electron physics | Abbreviated Journal | |
Volume | Issue | Pages | 29-72 | ||
Keywords | H2 Book chapter; Electron microscopy for materials research (EMAT); Vision lab | ||||
Abstract | In this chapter, the principles of statistical parameter estimation theory for a quantitative analysis of atomic-resolution electron microscopy images are introduced. Within this framework, electron microscopy images are described by a parametric statistical model. Here, parametric models are introduced for different types of electron microscopy images: reconstructed exit waves, annular dark-field (ADF) scanning transmission electron microscopy (STEM) images, and simultaneously acquired ADF and annular bright-field (ABF) STEM images. Furthermore, the Cramér-Rao lower bound (CRLB) is introduced, i.e. a theoretical lower bound on the variance of any unbiased estimator. This CRLB is used to quantify the precision of the structure parameters of interest, such as the atomic column positions and the integrated atomic column intensities. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2021-03-06 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | 217 | Series Issue | Edition | ||
ISSN | ISBN | 978-0-12-824607-8; 1076-5670 | Additional Links | UA library record | |
Impact Factor | Times cited | Open Access | Not_Open_Access | ||
Notes | ERC Consolidator project funded by the European Union grant #770887 Picometrics | Approved | Most recent IF: NA | ||
Call Number | UA @ admin @ c:irua:177527 | Serial | 6788 | ||
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Author | Albrecht, W.; Arslan Irmak, E.; Altantzis, T.; Pedrazo‐Tardajos, A.; Skorikov, A.; Deng, T.‐S.; van der Hoeven, J.E.S.; van Blaaderen, A.; Van Aert, S.; Bals, S. | ||||
Title | 3D Atomic‐Scale Dynamics of Laser‐Light‐Induced Restructuring of Nanoparticles Unraveled by Electron Tomography | Type | A1 Journal article | ||
Year | 2021 | Publication | Advanced Materials | Abbreviated Journal | Adv Mater |
Volume | Issue | Pages | 2100972 | ||
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) | ||||
Abstract | Understanding light–matter interactions in nanomaterials is crucial for optoelectronic, photonic, and plasmonic applications. Specifically, metal nanoparticles (NPs) strongly interact with light and can undergo shape transformations, fragmentation and ablation upon (pulsed) laser excitation. Despite being vital for technological applications, experimental insight into the underlying atomistic processes is still lacking due to the complexity of such measurements. Herein, atomic resolution electron tomography is performed on the same mesoporous-silica-coated gold nanorod, before and after femtosecond laser irradiation, to assess the missing information. Combined with molecular dynamics (MD) simulations based on the experimentally determined 3D atomic-scale morphology, the complex atomistic rearrangements, causing shape deformations and defect generation, are unraveled. These rearrangements are simultaneously driven by surface diffusion, facet restructuring, and strain formation, and are influenced by subtleties in the atomic distribution at the surface. |
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Language | Wos | 000671662000001 | Publication Date | 2021-07-11 | |
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Series Volume | Series Issue | Edition | |||
ISSN | 0935-9648 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 19.791 | Times cited | 8 | Open Access | OpenAccess |
Notes | W.A. and E.A.I. contributed equally to this work. The authors acknowledge funding from the European Research Council under the European Union’s Horizon 2020 research and innovation program (ERC Consolidator Grants No. 815128 – REALNANO and No. 770887 – PICOMETRICS), the European Union’s Seventh Framework Programme (ERC Advanced Grant No. 291667 – HierarSACol), and the European Commission (EUSMI). W.A. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in the Horizon2020 program (Grant 797153, SOPMEN). T.-S.D. acknowledges financial support from the National Science Foundation of China (NSFC, Grant No. 61905056). The authors also acknowledge financial support by the Research Foundation Flanders (FWO Grant G.0267.18N).; sygmaSB | Approved | Most recent IF: 19.791 | ||
Call Number | EMAT @ emat @c:irua:179781 | Serial | 6805 | ||
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Author | De wael, A.; De Backer, A.; Lobato, I.; Van Aert, S. | ||||
Title | Modelling ADF STEM images using elliptical Gaussian peaks and its effects on the quantification of structure parameters in the presence of sample tilt | Type | A1 Journal article | ||
Year | 2021 | Publication | Ultramicroscopy | Abbreviated Journal | Ultramicroscopy |
Volume | Issue | Pages | 113391 | ||
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | A small sample tilt away from a main zone axis orientation results in an elongation of the atomic columns in ADF STEM images. An often posed research question is therefore whether the ADF STEM image intensities of tilted nanomaterials should be quantified using a parametric imaging model consisting of elliptical rather than the currently used symmetrical peaks. To this purpose, simulated ADF STEM images corresponding to different amounts of sample tilt are studied using a parametric imaging model that consists of superimposed 2D elliptical Gaussian peaks on the one hand and symmetrical Gaussian peaks on the other hand. We investigate the quantification of structural parameters such as atomic column positions and scattering cross sections using both parametric imaging models. In this manner, we quantitatively study what can be gained from this elliptical model for quantitative ADF STEM, despite the increased parameter space and computational effort. Although a qualitative improvement can be achieved, no significant quantitative improvement in the estimated structure parameters is achieved by the elliptical model as compared to the symmetrical model. The decrease in scattering cross sections with increasing sample tilt is even identical for both types of parametric imaging models. This impedes direct comparison with zone axis image simulations. Nonetheless, we demonstrate how reliable atom-counting can still be achieved in the presence of small sample tilt. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000704334200001 | Publication Date | 2021-09-24 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0304-3991 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 2.843 | Times cited | Open Access | OpenAccess | |
Notes | This project has received funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (Grant Agreement No. 770887 and No. 823717 ESTEEM3). The authors acknowledge financial support from the Research Foundation Flanders (FWO, Belgium) through grants to A.D.w. and A.D.B. and projects G.0502.18N, G.0267.18N, and EOS 30489208. S.V.A. acknowledges TOP BOF funding from the University of Antwerp.; esteem3JRA; esteem3reported | Approved | Most recent IF: 2.843 | ||
Call Number | EMAT @ emat @c:irua:181462 | Serial | 6810 | ||
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Author | Hudry, D.; De Backer, A.; Popescu, R.; Busko, D.; Howard, I.A.; Bals, S.; Zhang, Y.; Pedrazo‐Tardajos, A.; Van Aert, S.; Gerthsen, D.; Altantzis, T.; Richards, B.S. | ||||
Title | Interface Pattern Engineering in Core‐Shell Upconverting Nanocrystals: Shedding Light on Critical Parameters and Consequences for the Photoluminescence Properties | Type | A1 Journal article | ||
Year | 2021 | Publication | Small | Abbreviated Journal | Small |
Volume | Issue | Pages | 2104441 | ||
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) | ||||
Abstract | Advances in controlling energy migration pathways in core-shell lanthanide (Ln)-based hetero-nanocrystals (HNCs) have relied heavily on assumptions about how optically active centers are distributed within individual HNCs. In this article, it is demonstrated that different types of interface patterns can be formed depending on shell growth conditions. Such interface patterns are not only identified but also characterized with spatial resolution ranging from the nanometer- to the atomic-scale. In the most favorable cases, atomic-scale resolved maps of individual particles are obtained. It is also demonstrated that, for the same type of core-shell architecture, the interface pattern can be engineered with thicknesses of just 1 nm up to several tens of nanometers. Total alloying between the core and shell domains is also possible when using ultra-small particles as seeds. Finally, with different types of interface patterns (same architecture and chemical composition of the core and shell domains) it is possible to modify the output color (yellow, red, and green-yellow) or change (improvement or degradation) the absolute upconversion quantum yield. The results presented in this article introduce an important paradigm shift and pave the way toward the emergence of a new generation of core-shell Ln-based HNCs with better control over their atomic-scale organization. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000710758000001 | Publication Date | 2021-10-25 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1613-6810 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.643 | Times cited | 17 | Open Access | OpenAccess |
Notes | The authors would like to acknowledge the financial support provided by the Helmholtz Recruitment Initiative Fellowship (B.S.R.) and the Helmholtz Association's Research Field Energy (Materials and Technologies for the Energy Transition program, Topic 1 Photovoltaics and Wind Energy). The authors would like to thank the Karlsruhe Nano Micro Facility (KNMF) for STEM access. This project has received funding from the European Research Council (ERC) under the European Union's Horizon 2020 Research and Innovation Programme (Grant agreement no. 770887 PICOMETRICS to S.V.A. and Grant agreement no. 815128 REALNANO to S.B.). The authors acknowledge financial support from the Research Foundation Flanders (FWO, Belgium) through Projects no. G.0502.18N, G.0267.18N, and a postdoctoral grant to A.D.B. T.A. acknowledges funding from the University of Antwerp Research fund (BOF). This project had received funding (EUSMI proposal #E181100205) from the European Union's Horizon 2020 Research and Innovation Programme under Grant agreement no 731019 (EUSMI). D.H. would like to thank “CGFigures” for helpful tutorials on 3D graphics with Blender.; sygmaSB | Approved | Most recent IF: 8.643 | ||
Call Number | EMAT @ emat @c:irua:183285 | Serial | 6817 | ||
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Author | Arslan Irmak, E.; Liu, P.; Bals, S.; Van Aert, S. | ||||
Title | 3D Atomic Structure of Supported Metallic Nanoparticles Estimated from 2D ADF STEM Images: A Combination of Atom – Counting and a Local Minima Search Algorithm | Type | A1 Journal article | ||
Year | 2021 | Publication | Small methods | Abbreviated Journal | Small Methods |
Volume | Issue | Pages | 2101150 | ||
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | Determining the three-dimensional (3D) atomic structure of nanoparticles (NPs) is critical to understand their structure-dependent properties. It is hereby important to perform such analyses under conditions relevant for the envisioned application. Here, we investigate the 3D structure of supported Au NPs at high temperature, which is of importance to understand their behavior during catalytic reactions. To overcome limitations related to conventional high-resolution electron tomography at high temperature, 3D characterization of NPs with atomic resolution has been performed by applying atom-counting using atomic resolution annular darkfield scanning transmission electron microscopy (ADF STEM) images followed by structural relaxation. However, at high temperatures, thermal displacements, which affect the ADF STEM intensities, should be taken into account. Moreover, it is very likely that the structure of a NP investigated at elevated temperature deviates from a ground state configuration, which is difficult to determine using purely computational energy minimization approaches. In this paper, we therefore propose an optimized approach using an iterative local minima search algorithm followed by molecular dynamics (MD) structural relaxation of candidate structures associated with each local minimum. In this manner, it becomes possible to investigate the 3D atomic structure of supported NPs, which may deviate from their ground state configuration. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000716511600001 | Publication Date | 2021-11-10 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2366-9608 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | Times cited | 12 | Open Access | OpenAccess | |
Notes | This work was supported by the European Research Council (Grant 815128 REALNANO to SB, Grant 770887 PICOMETRICS to SVA, Grant 823717 ESTEEM3). The authors acknowledge financial support from the Research Foundation Flanders (FWO, Belgium) through project funding (G.0267.18N, G.0502.18N, G.0346.21N).; sygmaSB; esteem3jra; esteem3reported | Approved | Most recent IF: NA | ||
Call Number | EMAT @ emat @c:irua:183289 | Serial | 6820 | ||
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Author | van Thiel, T. c.; Brzezicki, W.; Autieri, C.; Hortensius, J. r.; Afanasiev, D.; Gauquelin, N.; Jannis, D.; Janssen, N.; Groenendijk, D. j.; Fatermans, J.; Van Aert, S.; Verbeeck, J.; Cuoco, M.; Caviglia, A. d. | ||||
Title | Coupling Charge and Topological Reconstructions at Polar Oxide Interfaces | Type | A1 Journal article | ||
Year | 2021 | Publication | Physical Review Letters | Abbreviated Journal | Phys Rev Lett |
Volume | 127 | Issue | 12 | Pages | 127202 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | 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 nonpolar materials, where valence discontinuities lead to otherwise inaccessible charge and spin states. This approach paved the way for the discovery of numerous unconventional properties absent in the bulk constituents. However, control of the geometric structure of the electronic wave functions in correlated oxides remains an open challenge. Here, we create heterostructures consisting of ultrathin SrRuO3, an itinerant ferromagnet hosting momentum-space sources of Berry curvature, and LaAlO3, a polar wide-band-gap insulator. Transmission electron microscopy reveals an atomically sharp LaO/RuO2/SrO interface configuration, leading to excess charge being pinned near the LaAlO3/SrRuO3 interface. We demonstrate through magneto-optical characterization, theoretical calculations and transport measurements that the real-space charge reconstruction drives a reorganization of the topological charges in the band structure, thereby modifying the momentum-space Berry curvature in SrRuO3. Our results illustrate how the topological and magnetic features of oxides can be manipulated by engineering charge discontinuities at oxide interfaces. |
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000704665000010 | Publication Date | 2021-09-16 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0031-9007 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.462 | Times cited | 17 | Open Access | OpenAccess |
Notes | The authors thank E. Lesne, M. Lee, H. Barakov, M. Matthiesen and U. Filippozzi for discussions. The authors are grateful to E.J.S. van Thiel for producing the illustration in Fig. 4a. This work was supported by the European Research Council under the European Unions Horizon 2020 programme/ERC Grant agreements No. [677458], [770887] and No. [731473] (Quantox of QuantERA ERA-NET Cofund in Quantum Technologies) and by the Netherlands Organisation for Scientific Research (NWO/OCW) as part of the Frontiers of Nanoscience (NanoFront) and VIDI program. The authors acknowledge funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No. [823717] – ESTEEM3. N. G., J. V., and S. V. A. acknowledge funding from the University of Antwerp through the Concerted Research Actions (GOA) project Solarpaint and the TOP project. C. A. and W. B. are supported by the Foundation for Polish Science through the International Research Agendas program co-financed by the European Union within the Smart Growth Operational Programme. C. A. acknowledges access to the computing facilities of the Interdisciplinary Center of Modeling at the University of Warsaw, Grant No. G73-23 and G75-10. W.B. acknowledges support from the Narodowe Centrum Nauk (NCN, National Science Centre, Poland) Project No. 2019/34/E/ST3/00404'; esteem3TA; esteem3reported | Approved | Most recent IF: 8.462 | ||
Call Number | EMAT @ emat @c:irua:182595 | Serial | 6824 | ||
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Author | Zheng, Y.-R.; Vernieres, J.; Wang, Z.; Zhang, K.; Hochfilzer, D.; Krempl, K.; Liao, T.-W.; Presel, F.; Altantzis, T.; Fatermans, J.; Scott, S.B.; Secher, N.M.; Moon, C.; Liu, P.; Bals, S.; Van Aert, S.; Cao, A.; Anand, M.; Nørskov, J.K.; Kibsgaard, J.; Chorkendorff, I. | ||||
Title | Monitoring oxygen production on mass-selected iridium–tantalum oxide electrocatalysts | Type | A1 Journal article | ||
Year | 2021 | Publication | Nature Energy | Abbreviated Journal | Nat Energy |
Volume | Issue | Pages | |||
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) | ||||
Abstract | Development of low-cost and high-performance oxygen evolution reaction catalysts is key to implementing polymer electrolyte membrane water electrolyzers for hydrogen production. Iridium-based oxides are the state-of-the-art acidic oxygen evolution reactio catalysts but still suffer from inadequate activity and stability, and iridium's scarcity motivates the discovery of catalysts with lower iridium loadings. Here we report a mass-selected iridium-tantalum oxide catalyst prepared by a magnetron-based cluster source with considerably reduced noble-metal loadings beyond a commercial IrO2 catalyst. A sensitive electrochemistry/mass-spectrometry instrument coupled with isotope labelling was employed to investigate the oxygen production rate under dynamic operating conditions to account for the occurrence of side reactions and quantify the number of surface active sites. Iridium-tantalum oxide nanoparticles smaller than 2 nm exhibit a mass activity of 1.2 ± 0.5 kA “g” _“Ir” ^“-1” and a turnover frequency of 2.3 ± 0.9 s-1 at 320 mV overpotential, which are two and four times higher than those of mass-selected IrO2, respectively. Density functional theory calculations reveal that special iridium coordinations and the lowered aqueous decomposition free energy might be responsible for the enhanced performance. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000728458000001 | Publication Date | 2021-12-09 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2058-7546 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | Times cited | 95 | Open Access | OpenAccess | |
Notes | Y.-R.Z. and Z.W acknowledge funding from the Toyota Research Institute. This project has received funding from VILLUM FONDEN (grant no. 9455) and the European Research Council under the European Union’s Horizon 2020 research and innovation programme (grants no. 741860-CLUNATRA, no. 815128−REALNANO and no. 770887−PICOMETRICS). S.B. and S.V.A. acknowledge funding from the Research Foundation Flanders (FWO, G026718N and G050218N). T.A. acknowledges the University of Antwerp Research Fund (BOF). STEM measurements were supported by the European Union's Horizon 2020 Research Infrastructure-Integrating Activities for Advanced Communities under grant agreement No 823717 – ESTEEM3.; sygmaSB | Approved | Most recent IF: NA | ||
Call Number | EMAT @ emat @c:irua:184794 | Serial | 6903 | ||
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Author | Friedrich, T.; Yu, C.-P.; Verbeek, J.; Pennycook, T.; Van Aert, S. | ||||
Title | Phase retrieval from 4-dimensional electron diffraction datasets | Type | P1 Proceeding | ||
Year | 2021 | Publication | Proceedings T2 – IEEE International Conference on Image Processing (ICIP), SEP 19-22, 2021, Electr. network | Abbreviated Journal | |
Volume | Issue | Pages | 3453-3457 | ||
Keywords | P1 Proceeding; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | We present a computational imaging mode for large scale electron microscopy data, which retrieves a complex wave from noisy/sparse intensity recordings using a deep learning approach and subsequently reconstructs an image of the specimen from the Convolutional Neural Network (CNN) predicted exit waves. We demonstrate that an appropriate forward model in combination with open data frameworks can be used to generate large synthetic datasets for training. In combination with augmenting the data with Poisson noise corresponding to varying dose-values, we effectively eliminate overfitting issues. The U-NET[1] based architecture of the CNN is adapted to the task at hand and performs well while maintaining a relatively small size and fast performance. The validity of the approach is confirmed by comparing the reconstruction to well-established methods using simulated, as well as real electron microscopy data. The proposed method is shown to be effective particularly in the low dose range, evident by strong suppression of noise, good spatial resolution, and sensitivity to different atom types, enabling the simultaneous visualisation of light and heavy elements and making different atomic species distinguishable. Since the method acts on a very local scale and is comparatively fast it bears the potential to be used for near-real-time reconstruction during data acquisition. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000819455103114 | Publication Date | 2021-08-23 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 978-1-6654-4115-5 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | Times cited | Open Access | OpenAccess | ||
Notes | Approved | Most recent IF: NA | |||
Call Number | UA @ admin @ c:irua:189462 | Serial | 7089 | ||
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Author | De wael, A.; De Backer, A.; Jones, L.; Varambhia, A.; Nellist, P.D.; Van Aert, S. | ||||
Title | Measuring Dynamic Structural Changes of Nanoparticles at the Atomic Scale Using Scanning Transmission Electron Microscopy | Type | A1 Journal article | ||
Year | 2020 | Publication | Physical Review Letters | Abbreviated Journal | Phys Rev Lett |
Volume | 124 | Issue | 10 | Pages | 106105 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | We propose a new method to measure atomic scale dynamics of nanoparticles from experimental high-resolution annular dark field scanning transmission electron microscopy images. By using the so-called hidden Markov model, which explicitly models the possibility of structural changes, the number of atoms in each atomic column can be quantified over time. This newly proposed method outperforms the current atom-counting procedure and enables the determination of the probabilities and cross sections for surface diffusion. This method is therefore of great importance for revealing and quantifying the atomic structure when it evolves over time via adatom dynamics, surface diffusion, beam effects, or during in situ experiments. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000519718100015 | Publication Date | 2020-03-13 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0031-9007 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.6 | Times cited | Open Access | OpenAccess | |
Notes | This project has received funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation programme (Grant Agreement No. 770887 and No. 823717 ESTEEM3). The authors acknowledge financial support from the Research Foundation Flanders (FWO, Belgium) through grants to A.D.w. and A.D.B. and projects G.0502.18N and EOS 30489208. L.J. acknowledges the SFI AMBER Centre for support. A.V. and P.D.N. acknowledge the UK Engineering and Physical Sciences Council (EPSRC) for support (EP/K040375/1 and 1772738). A.V. also acknowledges Johnson-Matthey for support. We would like to thank Brian Theobald and Jonathan Sharman from JMTC Sonning for provision of the Pt sample. | Approved | Most recent IF: 8.6; 2020 IF: 8.462 | ||
Call Number | EMAT @ emat @c:irua:167148 | Serial | 6347 | ||
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Author | Fatermans, J.; den Dekker, Aj.; Müller-Caspary, K.; Gauquelin, N.; Verbeeck, J.; Van Aert, S. | ||||
Title | Atom column detection from simultaneously acquired ABF and ADF STEM images | Type | A1 Journal article | ||
Year | 2020 | Publication | Ultramicroscopy | Abbreviated Journal | Ultramicroscopy |
Volume | 219 | Issue | Pages | 113046 | |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT); Vision lab | ||||
Abstract | In electron microscopy, the maximum a posteriori (MAP) probability rule has been introduced as a tool to determine the most probable atomic structure from high-resolution annular dark-field (ADF) scanning transmission electron microscopy (STEM) images exhibiting low contrast-to-noise ratio (CNR). Besides ADF imaging, STEM can also be applied in the annular bright-field (ABF) regime. The ABF STEM mode allows to directly visualize light-element atomic columns in the presence of heavy columns. Typically, light-element nanomaterials are sensitive to the electron beam, limiting the incoming electron dose in order to avoid beam damage and leading to images exhibiting low CNR. Therefore, it is of interest to apply the MAP probability rule not only to ADF STEM images, but to ABF STEM images as well. In this work, the methodology of the MAP rule, which combines statistical parameter estimation theory and model-order selection, is extended to be applied to simultaneously acquired ABF and ADF STEM images. For this, an extension of the commonly used parametric models in STEM is proposed. Hereby, the effect of specimen tilt has been taken into account, since small tilts from the crystal zone axis affect, especially, ABF STEM intensities. Using simulations as well as experimental data, it is shown that the proposed methodology can be successfully used to detect light elements in the presence of heavy elements. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000594768500005 | Publication Date | 2020-06-01 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0304-3991 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 2.2 | Times cited | 9 | Open Access | OpenAccess |
Notes | The authors acknowledge financial support from the Research Foundation Flanders (FWO, Belgium) through project fundings (No. W.O.010.16N, No. G.0368.15N, No. G.0502.18N, EOS 30489208). This project has received funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (Grant Agreement No. 770887). The authors acknowledge funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No. 823717 – ESTEEM3. The direct electron detector (Medipix3, Quantum Detectors) was funded by the Hercules fund from the Flemish Government. K. M. C. acknowledges funding from the Initiative and Network Fund of the Helmholtz Association (Germany) under contract VH-NG-1317. The authors thank Mark Huijben from the University of Twente (Enschede, The Netherlands) for providing the LiMn2O4 sample used in section 4.2 of this study. N. G., J. V., and S. V. A. acknowledge funding from the University of Antwerp through the Concerted Research Actions (GOA) project Solarpaint and the TOP project. | Approved | Most recent IF: 2.2; 2020 IF: 2.843 | ||
Call Number | EMAT @ emat @c:irua:169706 | Serial | 6373 | ||
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Author | Groenendijk, D.J.; Autieri, C.; van Thiel, T.C.; Brzezicki, W.; Hortensius, J.R.; Afanasiev, D.; Gauquelin, N.; Barone, P.; van den Bos, K.H.W.; van Aert, S.; Verbeeck, J.; Filippetti, A.; Picozzi, S.; Cuoco, M.; Caviglia, A.D. | ||||
Title | Berry phase engineering at oxide interfaces | Type | A1 Journal article | ||
Year | 2020 | Publication | Abbreviated Journal | Phys. Rev. Research | |
Volume | 2 | Issue | 2 | Pages | 023404 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Three-dimensional strontium ruthenate (SrRuO3) is an itinerant ferromagnet that features Weyl points acting as sources of emergent magnetic fields, anomalous Hall conductivity, and unconventional spin dynamics. Integrating SrRuO3 in oxide heterostructures is potentially a novel route to engineer emergent electrodynamics, but its electronic band topology in the two-dimensional limit remains unknown. Here we show that ultrathin SrRuO3 exhibits spin-polarized topologically nontrivial bands at the Fermi energy. Their band anticrossings show an enhanced Berry curvature and act as competing sources of emergent magnetic fields. We control their balance by designing heterostructures with symmetric (SrTiO3/SrRuO3/SrTiO3 and SrIrO3/SrRuO3/SrIrO3) and asymmetric interfaces (SrTiO3/SrRuO3/SrIrO3). Symmetric structures exhibit an interface-tunable single-channel anomalous Hall effect, while ultrathin SrRuO3 embedded in asymmetric structures shows humplike features consistent with multiple Hall contributions. The band topology of two-dimensional SrRuO3 proposed here naturally accounts for these observations and harmonizes a large body of experimental results. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000603642700008 | Publication Date | 2020-06-25 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2643-1564 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | Times cited | 58 | Open Access | OpenAccess | |
Notes | Nederlandse Organisatie voor Wetenschappelijk Onderzoek; Fonds Wetenschappelijk Onderzoek; European Research Council; Horizon 2020, 677458 770887 731473 ; Fondazione Cariplo, 2013-0726 ; Narodowe Centrum Nauki, 2016/23/B/ST3/00839 ; Fundacja na rzecz Nauki Polskiej; Universiteit Antwerpen; Vlaamse regering; | Approved | Most recent IF: NA | ||
Call Number | EMAT @ emat @c:irua:172462 | Serial | 6401 | ||
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Author | De wael, A.; De Backer, A.; Van Aert, S. | ||||
Title | Hidden Markov model for atom-counting from sequential ADF STEM images: Methodology, possibilities and limitations | Type | A1 Journal article | ||
Year | 2020 | Publication | Ultramicroscopy | Abbreviated Journal | Ultramicroscopy |
Volume | 219 | Issue | Pages | 113131 | |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | We present a quantitative method which allows us to reliably measure dynamic changes in the atomic structure of monatomic crystalline nanomaterials from a time series of atomic resolution annular dark field scanning transmission electron microscopy images. The approach is based on the so-called hidden Markov model and estimates the number of atoms in each atomic column of the nanomaterial in each frame of the time series. We discuss the origin of the improved performance for time series atom-counting as compared to the current state-of-the-art atom-counting procedures, and show that the so-called transition probabilities that describe the probability for an atomic column to lose or gain one or more atoms from frame to frame are particularly important. Using these transition probabilities, we show that the method can also be used to estimate the probability and cross section related to structural changes. Furthermore, we explore the possibilities for applying the method to time series recorded under variable environmental conditions. The method is shown to be promising for a reliable quantitative analysis of dynamic processes such as surface diffusion, adatom dynamics, beam effects, or in situ experiments. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000594770500003 | Publication Date | 2020-10-03 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0304-3991 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 2.2 | Times cited | Open Access | OpenAccess | |
Notes | This project has received funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (Grant Agreement No. 770887 and No. 823717 ESTEEM3). The authors acknowledge financial support from the Research Foundation Flanders (FWO, Belgium) through grants to A.D.w. and A.D.B. and projects G.0502.18N and EOS 30489208. | Approved | Most recent IF: 2.2; 2020 IF: 2.843 | ||
Call Number | EMAT @ emat @c:irua:172449 | Serial | 6417 | ||
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Author | Milagres de Oliveira, T.; Albrecht, W.; González-Rubio, G.; Altantzis, T.; Lobato Hoyos, I.P.; Béché, A.; Van Aert, S.; Guerrero-Martínez, A.; Liz-Marzán, L.M.; Bals, S. | ||||
Title | 3D Characterization and Plasmon Mapping of Gold Nanorods Welded by Femtosecond Laser Irradiation | Type | A1 Journal article | ||
Year | 2020 | Publication | Acs Nano | Abbreviated Journal | Acs Nano |
Volume | 14 | Issue | Pages | acsnano.0c02610 | |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) | ||||
Abstract | Ultrafast laser irradiation can induce morphological and structural changes in plasmonic nanoparticles. Gold nanorods (Au NRs), in particular, can be welded together upon irradiation with femtosecond laser pulses, leading to dimers and trimers through the formation of necks between individual nanorods. We used electron tomography to determine the 3D (atomic) structure at such necks for representative welding geometries and to characterize the induced defects. The spatial distribution of localized surface plasmon modes for different welding configurations was assessed by electron energy loss spectroscopy. Additionally, we were able to directly compare the plasmon line width of single-crystalline and welded Au NRs with single defects at the same resonance energy, thus making a direct link between the structural and plasmonic properties. In this manner, we show that the occurrence of (single) defects results in significant plasmon broadening. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000586793400016 | Publication Date | 2020-08-19 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1936-0851 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 17.1 | Times cited | 25 | Open Access | OpenAccess |
Notes | This project has received funding from the European Research Council under the European Union's Horizon 2020 research and innovation program (ERC Consolidator Grants #815128 – REALNANO and #770887 – PICOMETRICS). The authors gratefully acknowledge funding from the Research Foundation Flanders (FWO, Belgium) through project funding G.0381.16N and G.0267.18N. W.A. acknowledges an Individual Fellowship funded by the Marie 27 Sklodowska-Curie Actions (MSCA) in Horizon 2020 program (grant 797153, SOPMEN). G.G.-R. acknowledge receipt of FPI Fellowship from the Spanish MINECO. This work has been funded by the Spanish Ministry of Science, Innovation and Universities (MICIU) (Grants RTI2018-095844-B-I00 and MAT2017-86659-R) and the Madrid Regional Government (Grant P2018/NMT-4389). A.B. acknowledges funding from FWO project G093417N and from the European Union's Horizon 2020 research and innovation programme under grant agreement No 823717 – ESTEEM3. L.M.L.-M. acknowledges the Maria de Maeztu Units of Excellence Program from the Spanish State Research Agency (Grant No. MDM-2017-0720); Comunidad de Madrid, P2018/NMT-4389 ; Ministerio de Ciencia, Innovación y Universidades, MAT2017-86659-R RTI2018-095844-B-I00 ; Ministerio de Economía y Competitividad; H2020 Marie Sklodowska-Curie Actions, 797153 ; Fonds Wetenschappelijk Onderzoek, G.0267.18N G.0381.16N G093417N ; H2020 Research Infrastructures, 823717 ; H2020 European Research Council, 770887 815128 ; Agencia Estatal de Investigación, Ministerio de Ciencia, Innovación y Universidades, MDM-2017-0720 ; sygma | Approved | Most recent IF: 17.1; 2020 IF: 13.942 | ||
Call Number | EMAT @ emat @c:irua:172440 | Serial | 6426 | ||
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Author | Imran, M.; Ramade, J.; Di Stasio, F.; De Franco, M.; Buha, J.; Van Aert, S.; Goldoni, L.; Lauciello, S.; Prato, M.; Infante, I.; Bals, S.; Manna, L. | ||||
Title | Alloy CsCdxPb1–xBr3Perovskite Nanocrystals: The Role of Surface Passivation in Preserving Composition and Blue Emission | Type | A1 Journal article | ||
Year | 2020 | Publication | Chemistry Of Materials | Abbreviated Journal | Chem Mater |
Volume | 32 | Issue | Pages | acs.chemmater.0c03825 | |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Various strategies have been proposed to engineer the band gap of metal halide perovskite nanocrystals (NCs) while preserving their structure and composition and thus ensuring spectral stability of the emission color. An aspect that has only been marginally investigated is how the type of surface passivation influences the structural/color stability of AMX3 perovskite NCs composed of two different M2+ cations. Here, we report the synthesis of blue-emitting Cs-oleate capped CsCdxPb1–xBr3 NCs, which exhibit a cubic perovskite phase containing Cd-rich domains of Ruddlesden–Popper phases (RP phases). The RP domains spontaneously transform into pure orthorhombic perovskite ones upon NC aging, and the emission color of the NCs shifts from blue to green over days. On the other hand, postsynthesis ligand exchange with various Cs-carboxylate or ammonium bromide salts, right after NC synthesis, provides monocrystalline NCs with cubic phase, highlighting the metastability of RP domains. When NCs are treated with Cs-carboxylates (including Cs-oleate), most of the Cd2+ ions are expelled from NCs upon aging, and the NCs phase evolves from cubic to orthorhombic and their emission color changes from blue to green. Instead, when NCs are coated with ammonium bromides, the loss of Cd2+ ions is suppressed and the NCs tend to retain their blue emission (both in colloidal dispersions and in electroluminescent devices), as well as their cubic phase, over time. The improved compositional and structural stability in the latter cases is ascribed to the saturation of surface vacancies, which may act as channels for the expulsion of Cd2+ ions from NCs. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000603288800034 | Publication Date | 2020-12-04 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0897-4756 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.6 | Times cited | 44 | Open Access | OpenAccess |
Notes | European Commission; Fonds Wetenschappelijk Onderzoek, G.0267.18N ; H2020 European Research Council, 770887 815128 851794 ; We acknowledge funding from the FLAG-ERA JTC2019 project PeroGas. S.B., and S.V.A. acknowledges funding from the European Research Council under the European Union’s Horizon 2020 research and innovation program (ERC Consolidator Grants #815128REALNANO and #770887PICOMETRICS) and from the Research Foundation Flanders (FWO, Belgium) through project funding G.0267.18N. F.D.S. acknowledges the funding from ERC starting grant NANOLED (851794). The computational work was carried out on the Dutch National e-infrastructure with the support of the SURF Cooperative; sygma | Approved | Most recent IF: 8.6; 2020 IF: 9.466 | ||
Call Number | EMAT @ emat @c:irua:174004 | Serial | 6659 | ||
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Author | Altantzis, T.; Lobato, I.; De Backer, A.; Béché, A.; Zhang, Y.; Basak, S.; Porcu, M.; Xu, Q.; Sánchez-Iglesias, A.; Liz-Marzán, L.M.; Van Tendeloo, G.; Van Aert, S.; Bals, S. | ||||
Title | Three-Dimensional Quantification of the Facet Evolution of Pt Nanoparticles in a Variable Gaseous Environment | Type | A1 Journal article | ||
Year | 2019 | Publication | Nano letters | Abbreviated Journal | Nano Lett |
Volume | 19 | Issue | 19 | Pages | 477-481 |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | Pt nanoparticles play an essential role in a wide variety of catalytic reactions. The activity of the particles strongly depends on their three-dimensional (3D) structure and exposed facets, as well as on the reactive environment. High-resolution electron microscopy has often been used to characterize nanoparticle catalysts but unfortunately most observations so far have been either performed in vacuum and/or using conventional (2D) in situ microscopy. The latter however does not provide direct 3D morphological information. We have implemented a quantitative methodology to measure variations of the 3D atomic structure of nanoparticles under the flow of a selected gas. We were thereby able to quantify refaceting of Pt nanoparticles with atomic resolution during various oxidation−reduction cycles. In a H2 environment, a more faceted surface morphology of the particles was observed with {100} and {111} planes being dominant. On the other hand, in O2 the percentage of {100} and {111} facets decreased and a significant increase of higher order facets was found, resulting in a more rounded morphology. This methodology opens up new opportunities toward in situ characterization of catalytic nanoparticles because for the first time it enables one to directly measure 3D morphology variations at the atomic scale in a specific gaseous reaction environment. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000455561300061 | Publication Date | 2019-01-09 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1530-6984 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 12.712 | Times cited | 82 | Open Access | OpenAccess |
Notes | This work was supported by the European Research Council (Grant 335078 COLOURATOM to S.B. and Grant 770887 PICOMETRICS to S.V.A.). The authors acknowledge funding from the European Commission Grant (EUSMI 731019 to S.B., L.M.L.-M., and Q.X. and MUMMERING 765604 to S.B. and Q.X.). The authors gratefully acknowledge funding from the Research Foundation Flanders (FWO, Belgium) through project fundings (G.0368.15N, G.0369.15N, and G.0267.18N), postdoctoral grants to T.A. and A.D.B, and an FWO [PEGASUS]2 Marie Sklodowska-Curie fellowship to Y.Z. (12U4917N). L.M.L.-M. acknowledges funding from the Spanish Ministerio de Economía y Competitividad (Grant MAT2017-86659-R). We gratefully acknowledge the support of NVIDIA Corporation with the donation of the Titan X Pascal GPU used for this research. ecas_sara Realnano 815128; sygma | Approved | Most recent IF: 12.712 | ||
Call Number | EMAT @ emat @UA @ admin @ c:irua:156390 | Serial | 5150 | ||
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Author | van den Bos, K.H.W.; Janssens, L.; De Backer, A.; Nellist, P.D.; Van Aert, S. | ||||
Title | The atomic lensing model: new opportunities for atom-by-atom metrology of heterogeneous nanomaterials | Type | A1 Journal article | ||
Year | 2019 | Publication | Ultramicroscopy | Abbreviated Journal | Ultramicroscopy |
Volume | 203 | Issue | Pages | 155 | |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | The atomic lensing model has been proposed as a promising method facilitating atom-counting in heterogeneous nanocrystals [1]. 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. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000465021000020 | Publication Date | 2018-12-06 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0304-3991 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 2.843 | Times cited | 4 | Open Access | OpenAccess |
Notes | The authors acknowledge financial support from the Research Foundation Flanders (FWO, Belgium) through project fundings (G.0369.15N, G.0502.18N and WO.010.16N), and by personal grants to K.H.W. van den Bos and A. De Backer. This project has received funding from the European Research Council (ERC) under the European Unions Horizon 2020 research and innovation programme (grant agreement No. 770887). | Approved | Most recent IF: 2.843 | ||
Call Number | EMAT @ emat @UA @ admin @ c:irua:155721 | Serial | 5074 | ||
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Author | Fatermans, J.; Van Aert, S.; den Dekker, A.J. | ||||
Title | The maximum a posteriori probability rule for atom column detection from HAADF STEM images | Type | A1 Journal article | ||
Year | 2019 | Publication | Ultramicroscopy | Abbreviated Journal | Ultramicroscopy |
Volume | 201 | Issue | Pages | 81-91 | |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT); Vision lab | ||||
Abstract | 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. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000466343800009 | Publication Date | 2019-02-04 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0304-3991 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 2.843 | Times cited | 1 | Open Access | OpenAccess |
Notes | The authors acknowledge financial support from the Research Foundation Flanders (FWO, Belgium) through project fundings (No. W.O.010.16N, No. G.0368.15N, No. G.0502.18N). This project has received funding from the European Research Council (ERC) under the European Unions Horizon 2020 research and innovation programme (Grant Agreement No. 770887). | Approved | Most recent IF: 2.843 | ||
Call Number | EMAT @ emat @UA @ admin @ c:irua:157176 | Serial | 5153 | ||
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Author | Van Aert, S.; De Backer, A.; Jones, L.; Martinez, G.T.; Béché, A.; Nellist, P.D. | ||||
Title | Control of Knock-On Damage for 3D Atomic Scale Quantification of Nanostructures: Making Every Electron Count in Scanning Transmission Electron Microscopy | Type | A1 Journal article | ||
Year | 2019 | Publication | Physical review letters | Abbreviated Journal | Phys Rev Lett |
Volume | 122 | Issue | 6 | Pages | 066101 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Understanding nanostructures down to the atomic level is the key to optimizing the design of advancedmaterials with revolutionary novel properties. This requires characterization methods capable of quantifying the three-dimensional (3D) atomic structure with the highest possible precision. A successful approach to reach this goal is to count the number of atoms in each atomic column from 2D annular dark field scanning transmission electron microscopy images. To count atoms with single atom sensitivity, a minimum electron dose has been shown to be necessary, while on the other hand beam damage, induced by the high energy electrons, puts a limit on the tolerable dose. An important challenge is therefore to develop experimental strategies to optimize the electron dose by balancing atom-counting fidelity vs the risk of knock-on damage. To achieve this goal, a statistical framework combined with physics-based modeling of the dose-dependent processes is here proposed and experimentally verified. This model enables an investigator to theoretically predict, in advance of an experimental measurement, the optimal electron dose resulting in an unambiguous quantification of nanostructures in their native state with the highest attainable precision. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000458824200008 | Publication Date | 2019-02-13 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0031-9007 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.462 | Times cited | 3 | Open Access | OpenAccess |
Notes | This project has received funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (Grant Agreement No. 770887). The authors acknowledge financial support from the Research Foundation Flanders (FWO, Belgium) through project fundings (WO.010.16N, G.0934.17N, G.0502.18N, G.0267.18N), and a grant to A. D. B. The research leading to these results has received funding from the European Union Seventh Framework Programme under Grant Agreement No. 312483— ESTEEM2 (Integrated Infrastructure Initiative-I3) and the UK EPSRC (Grant No. EP/M010708/1). | Approved | Most recent IF: 8.462 | ||
Call Number | EMAT @ emat @UA @ admin @ c:irua:157175 | Serial | 5156 | ||
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