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Author | Duarte, M.; Daems, N.; Hereijgers, J.; Arenas Esteban, D.; Bals, S.; Breugelmans, T. | ||||
Title | Enhanced CO2 electroreduction with metal-nitrogen-doped carbons in a continuous flow reactor | Type | A1 Journal article | ||
Year | 2021 | Publication | Journal Of Co2 Utilization | Abbreviated Journal | J Co2 Util |
Volume | 50 | Issue | Pages | 101583-12 | |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) | ||||
Abstract | As part of a mitigation and adaptation approach to increasing carbon dioxide atmospheric concentrations, we report superior performance of various metal-nitrogen-doped carbon catalysts, synthesized using an easily up-scalable method, for the electrochemical reduction to carbon monoxide and/or formate at industrially relevant current densities up to 200 mAcm−2. Altering the embedded transition metal (i.e. Sn, Co, Fe, Mn and Ni) allowed to tune the selectivity towards the desired product. Mn-N-C and Fe-N-C performance was compromised by its high CO* binding energy, while Co-N-C catalyzed preferentially the HER. Ni-N-C and Sn-N-C revealed to be promising electrocatalysts, the latter being evaluated for the first time in a flow reactor. A productivity of 589 L CO m-2 h-1 at -1.39 VRHE with Ni-N-C and 751 g HCOO- m-2 h-1 at -1.47 VRHE with Sn-N-C was achieved with no signs of degradation detected after 24 h of operation at industrially relevant current densities (100 mAcm−2). Stable operation at 200 mAcm−2 led to turnover frequencies for the production of carbon products of up to 5176 h-1. These enhanced productivities, in combination with high stability, constitute an essential step towards the scalability and ultimately towards the economical valorization of CO2 electrolyzers using metal-containing nitrogen-doped catalysts. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000670316000002 | Publication Date | 2021-05-28 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2212-9820 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 4.292 | Times cited | 14 | Open Access | OpenAccess |
Notes | The authors acknowledge sponsoring from the Research Foundation – Flanders (FWO) in the frame of a post-doctoral grant (12Y3919N – ND). This project was co-funded by the Interreg 2 Seas-Program 2014-2020, co-financed by the European Fund for Regional Development in the frame of subsidiary contract nr. 2S03-019. This work was further performed in the framework of the Catalisti MOT project D2M (“Dioxide to Monoxide (D2M): Innovative catalysis for CO2 to CO conversion”). We thank Lien Pacquets for analyzing the samples with SEM-EDX, Saskia Defoss´e for helping with the N2 physisorption measurements and Kitty Baert (VUB) for analyzing the samples with XPS and Raman. | Approved | Most recent IF: 4.292 | ||
Call Number | UA @ admin @ c:irua:178151 | Serial | 6779 | ||
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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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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: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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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: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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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:177530 | Serial | 6785 | ||
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Author | Borah, R.; Ninakanti, R.; Nuyts, G.; Peeters, H.; Pedrazo-Tardajos, A.; Nuti, S.; Vande Velde, C.; De Wael, K.; Lenaerts, S.; Bals, S.; Verbruggen, S. | ||||
Title | Selectivity in ligand functionalization of photocatalytic metal oxide nanoparticles for phase transfer and self‐assembly applications | Type | A1 Journal article | ||
Year | 2021 | Publication | Chemistry-A European Journal | Abbreviated Journal | Chem-Eur J |
Volume | Issue | Pages | chem.202100029-15 | ||
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Sustainable Energy, Air and Water Technology (DuEL); Intelligence in PRocesses, Advanced Catalysts and Solvents (iPRACS) | ||||
Abstract | Functionalization of photocatalytic metal oxide nanoparticles of TiO 2 , ZnO, WO 3 and CuO with amine‐terminated (oleylamine) and thiol‐terminated (1‐dodecanethiol) alkyl chained ligands was studied under ambient conditions. A high selectivity was observed in the binding specificity of a ligand towards nanoparticles of these different oxides. It was observed that oleylamine binds stably to only TiO 2 and WO 3 , while 1‐dodecanethiol binds stably only to ZnO and CuO. Similarly, polar to non‐polar solvent phase transfer of TiO 2 and WO 3 nanoparticles could be achieved by using oleylamine, but not by 1‐dodecanethiol, while the contrary holds for ZnO and CuO. The surface chemistry of ligand functionalized nanoparticles was probed by ATR‐FTIR spectroscopy, that enabled to elucidate the occupation of the ligands at the active sites. The photo‐stability of the ligands on the nanoparticle surface was determined by the photocatalytic self‐cleaning properties of the material. While TiO 2 and WO 3 degrade the ligands within 24 hours under both UV and visible light, ligands on ZnO and CuO remain unaffected. The gathered insights are also highly relevant from an application point of view. As an example, since the ligand functionalized nanoparticles are hydrophobic in nature, they can thus be self‐assembled at the air‐water interface, for obtaining nanoparticle films with demonstrated photocatalytic as well as anti‐fogging properties. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000652651400001 | Publication Date | 2021-04-21 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0947-6539 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 5.317 | Times cited | 15 | Open Access | OpenAccess |
Notes | R.B. and S.W.V. acknowledge financial support from the University of Antwerp Special Research Fund (BOF) for a DOCPRO4 doctoral scholarship. S.B. and A.P.-T. acknowledge financial support from the European Commission under the Horizon 2020 Program by means of the grant agreement no. 731019 EUSMI and the ERC Consolidator grant no. 815128 REALNANO.; sygmaSB | Approved | Most recent IF: 5.317 | ||
Call Number | UA @ admin @ c:irua:177495 | Serial | 6787 | ||
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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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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:177527 | Serial | 6788 | ||
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Author | Xi, J.; Yang, S.; Silvioli, L.; Cao, S.; Liu, P.; Chen, Q.; Zhao, Y.; Sun, H.; Hansen, J.N.; Haraldsted, J.-P.B.; Kibsgaard, J.; Rossmeisl, J.; Bals, S.; Wang, S.; Chorkendorff, I. | ||||
Title | Highly active, selective, and stable Pd single-atom catalyst anchored on N-doped hollow carbon sphere for electrochemical H₂O₂ synthesis under acidic conditions | Type | A1 Journal article | ||
Year | 2021 | Publication | Journal Of Catalysis | Abbreviated Journal | J Catal |
Volume | 393 | Issue | Pages | 313-323 | |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Single-atom catalysts (SACs) have recently attracted broad scientific interests due to their unique structural feature, the single-atom dispersion. Optimized electronic structure as well as high stability are required for single-atom catalysts to enable efficient electrochemical production of H2O2. Herein, we report a facile synthesis method that stabilizes atomic Pd species on the reduced graphene oxide/Ndoped carbon hollow carbon nanospheres (Pd1/N-C). Pd1/N-C exhibited remarkable electrochemical H2O2 production rate with high faradaic efficiency, reaching 80%. The single-atom structure and its high H2O2 production rate were maintained even after 10,000 cycle stability test. The existence of single-atom Pd as well as its coordination with N species is responsible for its high activity, selectivity, and stability. The N coordination number and substrate doping around Pd atoms are found to be critical for an optimized adsorption energy of intermediate *OOH, resulting in efficient electrochemical H2O2 production. (C) 2020 Elsevier Inc. All rights reserved. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000640923500003 | Publication Date | 2020-11-26 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0021-9517 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 6.844 | Times cited | 40 | Open Access | Not_Open_Access |
Notes | This research was financially supported by the National Natural Science Foundation of China (No. 51772110), Natural Science Foundation of Hubei Province (No. 2019CFB539), Danmarks Innovationsfond within the ProActivE project (5160-00003B), Villum Foundation V-SUSTAIN grant 9455 to the Villum Center for the Science of Sustainable Fuels and Chemicals, the Carlsberg Foundation grant CF18-0435, the Institutional Research Program (2E30220) of the Korea Institute of Science and Technology (KIST), Shenzhen Science and Technology Plan under Grant (JCYJ20170818160751460) and the Open Project of Key Laboratory of Green Chemical Engineering Process of Ministry of Education (No. GCP20200205). The authors would like to acknowledge the Analytical and Testing Center of Huazhong University of Science and Technology and the Wuhan National Laboratory for Optoelectronics for SEM, TEM, Raman and XPS measurements. | Approved | Most recent IF: 6.844 | ||
Call Number | UA @ admin @ c:irua:178321 | Serial | 6796 | ||
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Author | Skorikov, A.; Heyvaert, W.; Albecht, W.; Pelt, D.M.; Bals, S. | ||||
Title | Deep learning-based denoising for improved dose efficiency in EDX tomography of nanoparticles | Type | A1 Journal article | ||
Year | 2021 | Publication | Nanoscale | Abbreviated Journal | Nanoscale |
Volume | 13 | Issue | Pages | 12242-12249 | |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | The combination of energy-dispersive X-ray spectroscopy (EDX) and electron tomography is a powerful approach to retrieve the 3D elemental distribution in nanomaterials, providing an unprecedented level of information for complex, multi-component systems, such as semiconductor devices, as well as catalytic and plasmonic nanoparticles. Unfortunately, the applicability of EDX tomography is severely limited because of extremely long acquisition times and high electron irradiation doses required to obtain 3D EDX reconstructions with an adequate signal-to-noise ratio. One possibility to address this limitation is intelligent denoising of experimental data using prior expectations about the objects of interest. Herein, this approach is followed using the deep learning methodology, which currently demonstrates state-of-the-art performance for an increasing number of data processing problems. Design choices for the denoising approach and training data are discussed with a focus on nanoparticle-like objects and extremely noisy signals typical for EDX experiments. Quantitative analysis of the proposed method demonstrates its significantly enhanced performance in comparison to classical denoising approaches. This allows for improving the tradeoff between the reconstruction quality, acquisition time and radiation dose for EDX tomography. The proposed method is therefore especially beneficial for the 3D EDX investigation of electron beam-sensitive materials and studies of nanoparticle transformations. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000671395800001 | Publication Date | 2021-07-08 | |
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 | 11 | Open Access | OpenAccess |
Notes | Nederlandse Organisatie voor Wetenschappelijk Onderzoek, 016.Veni.192.235 ; H2020 European Research Council, 815128 ; H2020 Marie Skłodowska-Curie Actions, 797153 ; H2020 Research Infrastructures, 731019; realnano; sygmaSB | Approved | Most recent IF: 7.367 | ||
Call Number | EMAT @ emat @c:irua:179756 | Serial | 6799 | ||
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Author | Mychinko, M.; Skorikov, A.; Albrecht, W.; Sánchez‐Iglesias, A.; Zhuo, X.; Kumar, V.; Liz‐Marzán, L.M.; Bals, S. | ||||
Title | The Influence of Size, Shape, and Twin Boundaries on Heat‐Induced Alloying in Individual Au@Ag Core–Shell Nanoparticles | Type | A1 Journal article | ||
Year | 2021 | Publication | Small | Abbreviated Journal | Small |
Volume | Issue | Pages | 2102348 | ||
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | Environmental conditions during real-world application of bimetallic core–shell nanoparticles (NPs) often include the use of elevated temperatures, which are known to cause elemental redistribution, in turn significantly altering the properties of these nanomaterials. Therefore, a thorough understanding of such processes is of great importance. The recently developed combination of fast electron tomography with in situ heating holders is a powerful approach to investigate heat-induced processes at the single NP level, with high spatial resolution in 3D. In combination with 3D finite-difference diffusion simulations, this method can be used to disclose the influence of various NP parameters on the diffusion dynamics in Au@Ag core–shell systems. A detailed study of the influence of heating on atomic diffusion and alloying for Au@Ag NPs with varying core morphology and crystallographic details is carried out. Whereas the core shape and aspect ratio of the NPs play a minor role, twin boundaries are found to have a strong influence on the elemental diffusion. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000673326600001 | Publication Date | 2021-07-14 | |
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 | 8 | Open Access | OpenAccess |
Notes | The funding for this project was provided by European Research Council (ERC Consolidator Grant 815128, REALNANO) and European Commission (grant 731019, EUSMI and grant 26019, ESTEEM). This work was performed under the Maria de Maeztu Units of Excellence Programme-Grant No. MDM-2017-0720, Ministry of Science and Innovation.; sygmaSB | Approved | Most recent IF: 8.643 | ||
Call Number | EMAT @ emat @c:irua:179856 | Serial | 6804 | ||
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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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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000671662000001 | Publication Date | 2021-07-11 | |
Series Editor | Series Title | Abbreviated Series Title | |||
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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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 | Velazco, A.; Béché, A.; Jannis, D.; Verbeeck, J. | ||||
Title | Reducing electron beam damage through alternative STEM scanning strategies, Part I: Experimental findings | Type | A1 Journal article | ||
Year | 2022 | Publication | Ultramicroscopy | Abbreviated Journal | Ultramicroscopy |
Volume | 232 | Issue | Pages | 113398 | |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | The highly energetic electrons in a transmission electron microscope (TEM) can alter or even completely destroy the structure of samples before sufficient information can be obtained. This is especially problematic in the case of zeolites, organic and biological materials. As this effect depends on both the electron beam and the sample and can involve multiple damage pathways, its study remained difficult and is plagued with irreproducibility issues, circumstantial evidence, rumors, and a general lack of solid data. Here we take on the experimental challenge to investigate the role of the STEM scan pattern on the damage behavior of a commercially available zeolite sample with the clear aim to make our observations as reproducible as possible. We make use of a freely programmable scan engine that gives full control over the tempospatial distribution of the electron probe on the sample and we use its flexibility to obtain multiple repeated experiments under identical conditions comparing the difference in beam damage between a conventional raster scan pattern and a newly proposed interleaved scan pattern that provides exactly the same dose and dose rate and visits exactly the same scan points. We observe a significant difference in beam damage for both patterns with up to 11 % reduction in damage (measured from mass loss). These observations demonstrate without doubt that electron dose, dose rate and acceleration voltage are not the only parameters affecting beam damage in (S)TEM experiments and invite the community to rethink beam damage as an unavoidable consequence of applied electron dose. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000714819200002 | Publication Date | 2021-10-02 | |
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 | 18 | Open Access | OpenAccess |
Notes | A.V., D.J., A.B. and J.V. acknowledge funding from FWO project G093417N (’Compressed sensing enabling low dose imaging in transmission electron microscopy’) and G042920N (’Coincident event detection for advanced spectroscopy in transmission electron microscopy’). This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 823717 ESTEEM3. The Qu-Ant-EM microscope was partly funded by the Hercules fund from the Flemish Government. J.V. acknowledges funding from GOA project “Solarpaint” of the University of Antwerp.; JRA; reported | Approved | Most recent IF: 2.2 | ||
Call Number | EMAT @ emat @c:irua:183282 | Serial | 6818 | ||
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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 | Koo, J.; Dahl, A.B.; Bærentzen, J.A.; Chen, Q.; Bals, S.; Dahl, V.A. | ||||
Title | Shape from projections via differentiable forward projector for computed tomography | Type | A1 Journal article | ||
Year | 2021 | Publication | Ultramicroscopy | Abbreviated Journal | Ultramicroscopy |
Volume | 224 | Issue | Pages | 113239 | |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | In computed tomography, the reconstruction is typically obtained on a voxel grid. In this work, however, we propose a mesh-based reconstruction method. For tomographic problems, 3D meshes have mostly been studied to simulate data acquisition, but not for reconstruction, for which a 3D mesh means the inverse process of estimating shapes from projections. In this paper, we propose a differentiable forward model for 3D meshes that bridge the gap between the forward model for 3D surfaces and optimization. We view the forward projection as a rendering process, and make it differentiable by extending recent work in differentiable rendering. We use the proposed forward model to reconstruct 3D shapes directly from projections. Experimental results for single-object problems show that the proposed method outperforms traditional voxel-based methods on noisy simulated data. We also apply the proposed method on electron tomography images of nanoparticles to demonstrate the applicability of the method on real data. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000744576800008 | Publication Date | 2021-03-11 | |
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 | 3 | Open Access | OpenAccess |
Notes | EU Horizon 2020 MSCA Innovative Training Network MUMMERING Grant Number 765604. | Approved | Most recent IF: 2.843 | ||
Call Number | EMAT @ emat @c:irua:183267 | Serial | 6825 | ||
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Author | Jannis, D.; Hofer, C.; Gao, C.; Xie, X.; Béché, A.; Pennycook, Tj.; Verbeeck, J. | ||||
Title | Event driven 4D STEM acquisition with a Timepix3 detector: Microsecond dwell time and faster scans for high precision and low dose applications | Type | A1 Journal article | ||
Year | 2022 | Publication | Ultramicroscopy | Abbreviated Journal | Ultramicroscopy |
Volume | 233 | Issue | Pages | 113423 | |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | Four dimensional scanning transmission electron microscopy (4D STEM) records the scattering of electrons in a material in great detail. The benefits offered by 4D STEM are substantial, with the wealth of data it provides facilitating for instance high precision, high electron dose efficiency phase imaging via centre of mass or ptychography based analysis. However the requirement for a 2D image of the scattering to be recorded at each probe position has long placed a severe bottleneck on the speed at which 4D STEM can be performed. Recent advances in camera technology have greatly reduced this bottleneck, with the detection efficiency of direct electron detectors being especially well suited to the technique. However even the fastest frame driven pixelated detectors still significantly limit the scan speed which can be used in 4D STEM, making the resulting data susceptible to drift and hampering its use for low dose beam sensitive applications. Here we report the development of the use of an event driven Timepix3 direct electron camera that allows us to overcome this bottleneck and achieve 4D STEM dwell times down to 100 ns; orders of magnitude faster than what has been possible with frame based readout. We characterize the detector for different acceleration voltages and show that the method is especially well suited for low dose imaging and promises rich datasets without compromising dwell time when compared to conventional STEM imaging. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000734396800003 | Publication Date | 2021-11-13 | |
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 | 31 | Open Access | OpenAccess |
Notes | This project has received funding from the Euro- pean Union’s Horizon 2020 Research Infrastructure – Integrating Activities for Advanced Communities under grant agreement No 823717 – ESTEEM3. J.V. and A.B. acknowledge funding from FWO project G093417N (‘Compressed sensing enabling low dose imaging in transmission electron microscopy’). J.V. and D.J. ac- knowledge funding from FWO project G042920N ‘Co- incident event detection for advanced spectroscopy in transmission electron microscopy’. We acknowledge funding under the European Union’s Horizon 2020 re- search and innovation programme (J.V. and D.J un- der grant agreement No 101017720, FET-Proactive EBEAM, and C.H., C.G., X.X. and T.J.P. from the Eu- ropean Research Council (ERC) Grant agreement No. 802123-HDEM).; esteem3JRA; esteem3reported | Approved | Most recent IF: 2.2 | ||
Call Number | EMAT @ emat @c:irua:183948 | Serial | 6828 | ||
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Author | Feng, X.; Jena, H.S.; Krishnaraj, C.; Arenas-Esteban, D.; Leus, K.; Wang, G.; Sun, J.; Rüscher, M.; Timoshenko, J.; Roldan Cuenya, B.; Bals, S.; Voort, P.V.D. | ||||
Title | Creation of Exclusive Artificial Cluster Defects by Selective Metal Removal in the (Zn, Zr) Mixed-Metal UiO-66 | Type | A1 Journal article | ||
Year | 2021 | Publication | Journal Of The American Chemical Society | Abbreviated Journal | J Am Chem Soc |
Volume | Issue | Pages | jacs.1c05357 | ||
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | The differentiation between missing linker defects and missing cluster defects in MOFs is difficult, thereby limiting the ability to correlate materials properties to a specific type of defects. Herein, we present a novel and easy synthesis strategy for the creation of solely “missing cluster defects” by preparing mixed-metal (Zn, Zr)-UiO-66 followed by a gentle acid wash to remove the Zn nodes. The resulting material has the reo UiO-66 structure, typical for well-defined missing cluster defects. The missing clusters are thoroughly characterized, including low-pressure Ar-sorption, iDPCSTEM at a low dose (1.5 pA), and XANES/EXAFS analysis. We show that the missing cluster UiO-66 has a negligible number of missing linkers. We show the performance of the missing cluster UiO-66 in CO2 sorption and heterogeneous catalysis. |
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000730569500001 | Publication Date | 2021-12-07 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0002-7863 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 13.858 | Times cited | 29 | Open Access | OpenAccess |
Notes | Agentschap Innoveren en Ondernemen, HBC.2019.0110 HBC.2021.0254 ; Universiteit Gent; Fonds Wetenschappelijk Onderzoek, 665501 ; Dalian University of Technology; China Scholarship Council, 201507565009 ; National Natural Science Foundation of China, 22101039 ; H2020 European Research Council, 815128 REALNANO ; sygmaSB | Approved | Most recent IF: 13.858 | ||
Call Number | EMAT @ emat @c:irua:183951 | Serial | 6833 | ||
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Author | Mustonen, K.; Hofer, C.; Kotrusz, P.; Markevich, A.; Hulman, M.; Mangler, C.; Susi, T.; Pennycook, T.J.; Hricovini, K.; Richter, C.M.; Meyer, J.C.; Kotakoski, J.; Skákalová, V. | ||||
Title | Towards Exotic Layered Materials: 2D Cuprous Iodide | Type | A1 Journal article | ||
Year | 2021 | Publication | Advanced materials | Abbreviated Journal | Adv Mater |
Volume | Issue | Pages | 2106922 | ||
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | Heterostructures composed of two-dimensional (2D) materials are already opening many new possibilities in such fields of technology as electronics and magnonics, but far more could be achieved if the number and diversity of 2D materials is increased. So far, only a few dozen 2D crystals have been extracted from materials that exhibit a layered phase in ambient conditions, omitting entirely the large number of layered materials that may exist in other temperatures and pressures. Here, we demonstrate how these structures can be stabilized in 2D van der Waals stacks under room temperature via growing them directly in graphene encapsulation by using graphene oxide as the template material. Specifically, we produce an ambient stable 2D structure of copper and iodine, a material that normally only occurs in layered form at elevated temperatures between 645 and 675 K. Our results establish a simple route to the production of more exotic phases of materials that would otherwise be difficult or impossible to stabilize for experiments in ambient. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000744012500001 | Publication Date | 2021-12-07 | |
Series Editor | Series Title | Abbreviated Series Title | |||
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 | Open Access | OpenAccess | |
Notes | We acknowledge funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme Grant agreements No.~756277-ATMEN (A.M. and T.S.) and No.802123-HDEM (C.H. and T.J.P.). Computational resources from the Vienna Scientific Cluster (VSC) are gratefully acknowledged. V.S. was supported by the Austrian Science Fund (FWF) (project no. I2344-N36), the Slovak Research and Development Agency (APVV-16-0319), the project CEMEA of the Slovak Academy of Sciences, ITMS project code 313021T081 of the Research & Innovation Operational Programme and from the V4-Japan Joint Research Program (BGapEng). J.K. acknowledges the FWF funding within project P31605-N36 and M.H. the funding from Slovak Research and Development Agency via the APVV-15-0693 and APVV-19-0365 project grants. Danubia NanoTech s.r.o. has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 101008099 (CompSafeNano project) and also thanks Mr. Kamil Bernath for his support. | Approved | Most recent IF: 19.791 | ||
Call Number | EMAT @ emat @c:irua:183956 | Serial | 6834 | ||
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Author | Hofer, C.; Pennycook, T.J. | ||||
Title | Reliable phase quantification in focused probe electron ptychography of thin materials | Type | A1 Journal Article | ||
Year | 2023 | Publication | Ultramicroscopy | Abbreviated Journal | Ultramicroscopy |
Volume | 254 | Issue | Pages | 113829 | |
Keywords | A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; | ||||
Abstract | Electron ptychography provides highly sensitive, dose efficient phase images which can be corrected for aberrations after the data has been acquired. This is crucial when very precise quantification is required, such as with sensitivity to charge transfer due to bonding. Drift can now be essentially eliminated as a major impediment to focused probe ptychography, which benefits from the availability of easily interpretable simultaneous Z-contrast imaging. However challenges have remained when quantifying the ptychographic phases of atomic sites. The phase response of a single atom has a negative halo which can cause atoms to reduce in phase when brought closer together. When unaccounted for, as in integrating methods of quantification, this effect can completely obscure the effects of charge transfer. Here we provide a new method of quantification that overcomes this challenge, at least for 2D materials, and is robust to experimental parameters such as noise, sample tilt. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 001071608700001 | Publication Date | 2023-08-18 | |
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 | ||
Notes | FWO, G013122N ; Horizon 2020 Framework Programme; Horizon 2020; European Research Council, 802123-HDEM ; European Research Council; | Approved | Most recent IF: 2.2; 2023 IF: 2.843 | ||
Call Number | EMAT @ emat @c:irua:200272 | Serial | 8987 | ||
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Author | Ding, L.; Zhao, M.; Ehlers, F.J.H.; Jia, Z.; Zhang, Z.; Weng, Y.; Schryvers, D.; Liu, Q.; Idrissi, H. | ||||
Title | “Branched” structural transformation of the L12-Al3Zr phase manipulated by Cu substitution/segregation in the Al-Cu-Zr alloy system | Type | A1 Journal article | ||
Year | 2024 | Publication | Journal of materials science & technology | Abbreviated Journal | Journal of Materials Science & Technology |
Volume | 185 | Issue | Pages | 186-206 | |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | The effect of Cu on the evolution of the Al3Zr phase in an Al-Cu-Zr cast alloy during solution treatment at 500 °C has been thoroughly studied by combining atomic resolution high-angle annular dark-field scanning transmission electron microscopy, energy-dispersive X-ray spectroscopy and first-principles cal- culations. The heat treatment initially produces a pure L12-Al3Zr microstructure, allowing for about 13 % Cu to be incorporated in the dispersoid. Cu incorporation increases the energy barrier for anti-phase boundary (APB) activation, thus stabilizing the L12 structure. Additional heating leads to a Cu-induced “branched”path for the L12 structural transformation, with the latter process accelerated once the first APB has been created. Cu atoms may either (i) be repelled by the APBs, promoting the transformation to a Cu-poor D023 phase, or (ii) they may segregate at one Al-Zr layer adjacent to the APB, promoting a transformation to a new thermodynamically favored phase, Al4CuZr, formed when these segregation layers are periodically arranged. Theoretical studies suggest that the branching of the L12 transformation path is linked to the speed at which an APB is created, with Cu attraction triggered by a comparatively slow process. This unexpected transformation behavior of the L12-Al3Zr phase opens a new path to understanding, and potentially regulating the Al3Zr dispersoid evolution for high temperature applications. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 001154261100001 | Publication Date | 2023-12-24 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1005-0302 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 10.9 | Times cited | Open Access | Not_Open_Access | |
Notes | This work was supported by the National Key Research and Development Program (No. 2020YFA0405900), the National Natural Science Foundation of China (Grant No. 52371111 and U2141215 ), the Natural Science Foundation of Jiangsu Province (No. BE2022159 ). We are grateful to the High Performance Computing Center of Nanjing Tech University for supporting the computational resources. H. Idrissi is mandated by the Belgian National Fund for Scientific Research (FSR- FNRS). | Approved | Most recent IF: 10.9; 2024 IF: 2.764 | ||
Call Number | EMAT @ emat @c:irua:202392 | Serial | 8981 | ||
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Author | Robert, Hl.; Lobato, I.; Lyu, Fj.; Chen, Q.; Van Aert, S.; Van Dyck, D.; Müller-Caspary, K. | ||||
Title | Dynamical diffraction of high-energy electrons investigated by focal series momentum-resolved scanning transmission electron microscopy at atomic resolution | Type | A1 Journal article | ||
Year | 2022 | Publication | Ultramicroscopy | Abbreviated Journal | Ultramicroscopy |
Volume | 233 | Issue | Pages | 113425 | |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT); Vision lab | ||||
Abstract | We report a study of scattering dynamics in crystals employing momentum-resolved scanning transmission electron microscopy under varying illumination conditions. As we perform successive changes of the probe focus, multiple real-space signals are obtained in dependence of the shape of the incident electron wave. With support from extensive simulations, each signal is shown to be characterised by an optimum focus for which the contrast is maximum and which differs among different signals. For instance, a systematic focus mismatch is found between images formed by high-angle scattering, being sensitive to thickness and chemical composition, and the first moment in diffraction space, being sensitive to electric fields. It follows that a single recording at one specific probe focus is usually insufficient to characterise materials comprehensively. Most importantly, we demonstrate in experiment and simulation that the second moment ( |
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000734396800009 | Publication Date | 2021-11-13 | |
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 | We thank Dr. Florian Winkler for valuable discussions and experimental work at the early stages of this study. This work was supported by the Initiative and Network Fund of the Helmholtz Association (Germany) under contracts VH-NG-1317 and ZT-I-0025. This project furthermore received funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (grant agreement No. 770887). | Approved | Most recent IF: 2.2 | ||
Call Number | EMAT @ emat @c:irua:184833 | Serial | 6898 | ||
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Author | Chen, B.; Gauquelin, N.; Green, R.J.; Verbeeck, J.; Rijnders, G.; Koster, G. | ||||
Title | Asymmetric Interfacial Intermixing Associated Magnetic Coupling in LaMnO3/LaFeO3 Heterostructures | Type | A1 Journal article | ||
Year | 2021 | Publication | Frontiers in physics | Abbreviated Journal | Front. Phys. |
Volume | 9 | Issue | Pages | ||
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | The structural and magnetic properties of LaMnO<sub>3</sub>/LaFeO<sub>3</sub>(LMO/LFO) heterostructures are characterized using a combination of scanning transmission electron microscopy, electron energy-loss spectroscopy, bulk magnetometry, and resonant x-ray reflectivity. Unlike the relatively abrupt interface when LMO is deposited on top of LFO, the interface with reversed growth order shows significant cation intermixing of Mn<sup>3+</sup>and Fe<sup>3+</sup>, spreading ∼8 unit cells across the interface. The asymmetric interfacial chemical profiles result in distinct magnetic properties. The bilayer with abrupt interface shows a single magnetic hysteresis loop with strongly enhanced coercivity, as compared to the LMO plain film. However, the bilayer with intermixed interface shows a step-like hysteresis loop, associated with the separate switching of the “clean” and intermixed LMO sublayers. Our study illustrates the key role of interfacial chemical profile in determining the functional properties of oxide heterostructures. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000745284500001 | Publication Date | 2021-12-14 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2296-424X | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | Times cited | 1 | Open Access | OpenAccess | |
Notes | This work is supported by the international M-ERA.NET project SIOX (project 4288) and H2020 project ULPEC (project 732642). The X-Ant-EM microscope and the direct electron detector were partly funded by the Hercules fund from the Flemish Government. NG and JV acknowledge funding from GOA project “Solarpaint” of the University of Antwerp. RG was supported by the Natural Sciences and Engineering Research Council of Canada (NSERC). Part of the research described in this paper was performed at the Canadian Light Source, a national research facility of the University of Saskatchewan, which is supported by the Canada Foundation for Innovation (CFI), NSERC, the National Research Council (NRC), the Canadian Institutes of Health Research (CIHR), the Government of Saskatchewan, and the University of Saskatchewan. | Approved | Most recent IF: NA | ||
Call Number | EMAT @ emat @c:irua:185176 | Serial | 6901 | ||
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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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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 | Veronesi, S.; Pfusterschmied, G.; Fabbri, F.; Leitgeb, M.; Arif, O.; Esteban, D.A.; Bals, S.; Schmid, U.; Heun, S. | ||||
Title | 3D arrangement of epitaxial graphene conformally grown on porousified crystalline SiC | Type | A1 Journal article | ||
Year | 2022 | Publication | Carbon | Abbreviated Journal | Carbon |
Volume | 189 | Issue | Pages | 210-218 | |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | |||||
Address | |||||
Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000760358800008 | Publication Date | 2021-12-17 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0008-6223 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 10.9 | Times cited | 3 | Open Access | OpenAccess |
Notes | Horizon 2020; European Commission; Horizon 2020 Framework Programme; European Research Council, 128 731 019 ; European Research Council, REALNANO 815 128 ; sygmaSB | Approved | Most recent IF: 10.9 | ||
Call Number | EMAT @ emat @c:irua:186583 | Serial | 6952 | ||
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Author | Stuyck, W.; Bugaev, A.L.; Nelis, T.; de Oliveira-Silva, R.; Smolders, S.; Usoltsev, O.A.; Arenas Esteban, D.; Bals, S.; Sakellariou, D.; De Vos, D. | ||||
Title | Sustainable formation of tricarballylic acid from citric acid over highly stable Pd/Nb2O5.nH2O catalysts | Type | A1 Journal article | ||
Year | 2022 | Publication | Journal of catalysis | Abbreviated Journal | J Catal |
Volume | Issue | Pages | |||
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | |||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000792492100009 | Publication Date | 2022-02-17 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0021-9517 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 7.3 | Times cited | 5 | Open Access | OpenAccess |
Notes | Fonds Wetenschappelijk Onderzoek; Russian Science Foundation, 20-43-01015 ; KU Leuven, METU14/04 MK-5853.2021.1.2 ; | Approved | Most recent IF: 7.3 | ||
Call Number | EMAT @ emat @c:irua:186580 | Serial | 6954 | ||
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Author | Van Everbroeck, T.; Wu, J.; Arenas-Esteban, D.; Ciocarlan, R.-G.; Mertens, M.; Bals, S.; Dujardin, C.; Granger, P.; Seftel, E.M.; Cool, P. | ||||
Title | ZnAl layered double hydroxide based catalysts (with Cu, Mn, Ti) used as noble metal-free three-way catalysts | Type | A1 Journal article | ||
Year | 2022 | Publication | Applied clay science | Abbreviated Journal | Appl Clay Sci |
Volume | 217 | Issue | Pages | 106390 | |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA) | ||||
Abstract | |||||
Address | |||||
Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000795870100004 | Publication Date | 2022-01-02 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0169-1317 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 5.6 | Times cited | 6 | Open Access | OpenAccess |
Notes | The authors acknowledge financial support by theEuropean Union’s Horizon 2020 Project Partial-PGMs (H2020-NMP-686086). R-G C. and P.C. acknowledge the FWO-Flanders (project no. G038215N) for financial support. S⋅B and D.A.E thank the financial support of the European Research Council (ERC-CoG-2019 815128). The authors are grateful to Johnson Matthey, UK, for supplying the commercial benchmark catalysts; realnano; sygmaSB | Approved | Most recent IF: 5.6 | ||
Call Number | EMAT @ emat @c:irua:186956 | Serial | 6955 | ||
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Author | Heyvaert, W.; Pedrazo-Tardajos, A.; Kadu, A.; Claes, N.; González-Rubio, G.; Liz-Marzán, L.M.; Albrecht, W.; Bals, S. | ||||
Title | Quantification of the Helical Morphology of Chiral Gold Nanorods | Type | A1 Journal article | ||
Year | 2022 | Publication | ACS materials letters | Abbreviated Journal | ACS Materials Lett. |
Volume | 4 | Issue | Pages | 642-649 | |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Chirality in inorganic nanoparticles and nanostructures has gained increasing scientific interest, because of the possibility to tune their ability to interact differently with left- and right-handed circularly polarized light. In some cases, the optical activity is hypothesized to originate from a chiral morphology of the nanomaterial. However, quantifying the degree of chirality in objects with sizes of tens of nanometers is far from straightforward. Electron tomography offers the possibility to faithfully retrieve the three-dimensional morphology of nanomaterials, but only a qualitative interpretation of the morphology of chiral nanoparticles has been possible so far. We introduce herein a methodology that enables us to quantify the helicity of complex chiral nanomaterials, based on the geometrical properties of a helix. We demonstrate that an analysis at the single particle level can provide significant insights into the origin of chiroptical properties. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000784490000013 | Publication Date | 2022-03-08 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2639-4979 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | Times cited | 11 | Open Access | OpenAccess | |
Notes | S.B. and A.P.-T. gratefully acknowledge funding by the European Research Council (ERC Consolidator Grant #815128-REALNANO) the European Union’s Horizon 2020 research and innovation program under grant agreement #823717ESTEEM3. L.M.L.-M. acknowledges funding from MCIN/ AEI /10.13039/501100011033, grant # PID2020- 117779RB-I00 and the Maria de Maeztu Units of Excellence Program from the Spanish State Research Agency (Grant No. MDM-2017-0720). G.G.-R. thanks the Spanish Spanish Ministerio de Ciencia e Innovación for an FPI (BES-2014- 068972) fellowship.; SygmaSB; esteem3reported; esteem3jra | Approved | Most recent IF: NA | ||
Call Number | EMAT @ emat @c:irua:186959 | Serial | 6956 | ||
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Author | Ning, S.; Xu, W.; Ma, Y.; Loh, L.; Pennycook, T.J.; Zhou, W.; Zhang, F.; Bosman, M.; Pennycook, S.J.; He, Q.; Loh, N.D. | ||||
Title | Accurate and Robust Calibration of the Uniform Affine Transformation Between Scan-Camera Coordinates for Atom-Resolved In-Focus 4D-STEM Datasets | Type | A1 Journal article | ||
Year | 2022 | Publication | Microscopy and microanalysis | Abbreviated Journal | Microsc Microanal |
Volume | Issue | Pages | 1-11 | ||
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Accurate geometrical calibration between the scan coordinates and the camera coordinates is critical in four-dimensional scanning transmission electron microscopy (4D-STEM) for both quantitative imaging and ptychographic reconstructions. For atomic-resolved, in-focus 4D-STEM datasets, we propose a hybrid method incorporating two sub-routines, namely a J-matrix method and a Fourier method, which can calibrate the uniform affine transformation between the scan-camera coordinates using raw data, without a priori knowledge about the crystal structure of the specimen. The hybrid method is found robust against scan distortions and residual probe aberrations. It is also effective even when defects are present in the specimen, or the specimen becomes relatively thick. We will demonstrate that a successful geometrical calibration with the hybrid method will lead to a more reliable recovery of both the specimen and the electron probe in a ptychographic reconstruction. We will also show that, although the elimination of local scan position errors still requires an iterative approach, the rate of convergence can be improved, and the residual errors can be further reduced if the hybrid method can be firstly applied for initial calibration. The code is made available as a simple-to-use tool to correct affine transformations of the scan-camera coordinates in 4D-STEM experiments. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000767045700001 | Publication Date | 2022-03-09 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1431-9276 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 2.8 | Times cited | Open Access | OpenAccess | |
Notes | N. D. Loh kindly acknowledges support from NUS Early Career Research Award (R-154-000-B35-133), MOE’s AcRF Tier 1 grant nr. R-284-000-172-114 and NRF CRP grant number NRF-CRP16-2015-05. Q. He would also like to acknowledge the support of the National Research Foundation (NRF) Singapore, under its NRF Fellowship (NRF-NRFF11-2019-0002). W. Zhou acknowledges the support from Beijing Outstanding Young Scientist Program (BJJWZYJH01201914430039). F. Zhang acknowledges the support of the National Natural Science Foundation of China (11775105, 12074167). T. J. Pennycook acknowledges funding under the European Union’s Horizon 2020 research and innovation programme from the European Research Council (ERC) Grant agreement No. 802123-HDEM. | Approved | Most recent IF: 2.8 | ||
Call Number | EMAT @ emat @c:irua:186958 | Serial | 6957 | ||
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Author | Zillner, J.; Boyen, H.-G.; Schulz, P.; Hanisch, J.; Gauquelin, N.; Verbeeck, J.; Kueffner, J.; Desta, D.; Eisele, L.; Ahlswede, E.; Powalla, M. | ||||
Title | The role of SnF₂ additive on interface formation in all lead-free FASnI₃ perovskite solar cells | Type | A1 Journal article | ||
Year | 2022 | Publication | Advanced functional materials | Abbreviated Journal | Adv Funct Mater |
Volume | Issue | Pages | 2109649-9 | ||
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | Tin-based perovskites are promising alternative absorber materials for leadfree perovskite solar cells but need strategies to avoid fast tin (Sn) oxidation. Generally, this reaction can be slowed down by the addition of tin fluoride (SnF2) to the perovskite precursor solution, which also improves the perovskite layer morphology. Here, this work analyzes the spatial distribution of the additive within formamidinium tin triiodide (FASnI(3)) films deposited on top of poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) hole transporting layers. Employing time-of-flight secondary ion mass spectrometry and a combination of hard and soft X-ray photoelectron spectroscopy, it is found that Sn F2 preferably accumulates at the PEDOT:PSS/perovskite interface, accompanied by the formation of an ultrathin SnS interlayer with an effective thickness of approximate to 1.2 nm. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000779891000001 | Publication Date | 0000-00-00 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1616-301x | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 19 | Times cited | 22 | Open Access | OpenAccess |
Notes | J.Z. and H.-G.B. contributed equally to this work. This project received funding from the European Union's Horizon 2020 research and innovation programme under grant agreement No. 850937 (PERCISTAND). H.-G.B. and D.D. are very grateful to the Research Foundation Flanders (FWO) for funding the HAXPES-lab instrument within the HERCULES program for Large Research Infrastructure of the Flemish government. P.S. thanks the French Agence Nationale de la Recherche for funding under the contract number ANR-17-MPGA-0012. This work was supported by the Federal Ministry for Economic Affairs and Energy (BMWi) Germany under the contract number 03EE1038A (CAPITANO) and financed by the Ministry of Science, Research and the Arts of Baden-Württemberg as part of the sustainability financing of the projects of the Excellence Initiative II (KSOP). | Approved | Most recent IF: 19 | ||
Call Number | UA @ admin @ c:irua:187969 | Serial | 7067 | ||
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