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Author De Backer, A.; Zhang, Z.; van den Bos, K.H.W.; Bladt, E.; Sánchez‐Iglesias, A.; Liz‐Marzán, L.M.; Nellist, P.D.; Bals, S.; Van Aert, S. url  doi
openurl 
  Title Element Specific Atom Counting at the Atomic Scale by Combining High Angle Annular Dark Field Scanning Transmission Electron Microscopy and Energy Dispersive X‐ray Spectroscopy Type A1 Journal article
  Year 2022 Publication Small methods Abbreviated Journal Small Methods  
  Volume Issue Pages 2200875  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract A new methodology is presented to count the number of atoms in multimetallic nanocrystals by combining energy dispersive X-ray spectroscopy (EDX) and high angle annular dark field scanning transmission electron microscopy (HAADF STEM). For this purpose, the existence of a linear relationship between the incoherent HAADF STEM and EDX images is exploited. Next to the number of atoms for each element in the atomic columns, the method also allows quantification of the error in the obtained number of atoms, which is of importance given the noisy nature of the acquired EDX signals. Using experimental images of an Au@Ag core–shell nanorod, it is demonstrated that 3D structural information can be extracted at the atomic scale. Furthermore, simulated data of an Au@Pt core–shell nanorod show the prospect to characterize heterogeneous nanostructures with adjacent atomic numbers.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000862072700001 Publication Date 2022-09-30  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  ISSN 2366-9608 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 12.4 Times cited 5 Open Access OpenAccess  
  Notes This work was supported by the European Research Council (Grant 770887 PICOMETRICS to S.V.A., Grant 815128 REALNANO to S.B., 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.; esteem3reported; esteem3JRA Approved Most recent IF: 12.4  
  Call Number EMAT @ emat @c:irua:191570 Serial 7109  
Permanent link to this record
 

 
Author De Backer, A.; Van Aert, S.; Faes, C.; Arslan Irmak, E.; Nellist, P.D.; Jones, L. url  doi
openurl 
  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.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000866500900001 Publication Date 2022-10-12  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  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 Ni, B.; Mychinko, M.; Gómez‐Graña, S.; Morales‐Vidal, J.; Obelleiro‐Liz, M.; Heyvaert, W.; Vila‐Liarte, D.; Zhuo, X.; Albrecht, W.; Zheng, G.; González‐Rubio, G.; Taboada, J.M.; Obelleiro, F.; López, N.; Pérez‐Juste, J.; Pastoriza‐Santos, I.; Cölfen, H.; Bals, S.; Liz‐Marzán, L.M. url  doi
openurl 
  Title Chiral Seeded Growth of Gold Nanorods Into 4‐Fold Twisted Nanoparticles with Plasmonic Optical Activity Type A1 Journal article
  Year 2022 Publication Advanced materials Abbreviated Journal Adv Mater  
  Volume Issue Pages 2208299  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract A robust and reproducible methodology to prepare stable inorganic nanoparticles with chiral morphology might hold the key to the practical utilization of these materials. We describe herein an optimized chiral growth method to prepare 4-fold twisted gold nanorods, where the amino acid cysteine is used as a dissymmetry inducer. Four tilted ridges were found to develop on the surface of single-crystal nanorods upon repeated reduction of HAuCl4, in the presence of cysteine as the chiral inducer and ascorbic acid as a reducing agent. From detailed electron microscopy analysis of the crystallographic structures, we propose that dissymmetry results from the development of chiral facets in the form of protrusions (tilted ridges) on the initial nanorods, eventually leading to a twisted shape. The role of cysteine is attributed to assisting enantioselective facet evolution, which is supported by density functional theory simulations of the surface energies, modified upon adsorption of the chiral molecule. The development of R-type and S-type chiral structures (small facets, terraces, or kinks) would thus be non-equal, removing the mirror symmetry of the Au NR and in turn resulting in a markedly chiral morphology with high plasmonic optical activity.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000888886000001 Publication Date 2022-10-14  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  ISSN 0935-9648 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 29.4 Times cited 35 Open Access OpenAccess  
  Notes This work was supported by the MCIN/AEI/10.13039/501100011033 (Grants PID2019-108954RB-I00, PID2020-117371RA-I00, PID2020-117779RB-I00, and Maria de Maeztu Units of Excellence Program from the Spanish State Research Agency Grant No. MDM-2017-0720), Xunta de Galicia/FEDER (Grant GRC ED431C 2020/09) and the European Regional Development Fund (ERDF). M.M., W.H. and S.B. acknowledge financial support from the European Commission under the Horizon 2020 Programme by ERC Consolidator grant no. 815128 (REALNANO). W.A. acknowledges financial support from the research program of AMOLF, which is partly financed by the Dutch Research Council (NWO). J. M.-V. and N. L. thank the Spanish Ministry of Science and Innovation for financial support (RTI2018- 101394-B-I00 and Severo Ochoa Grant MCIN/AEI/10.13039/501100011033 CEX2019-000925-S) and the Barcelona Supercomputing Center-MareNostrum (BSC-RES) for providing generous computer resources. S.G.-G. acknowledges the MCIN. B. N. acknowledges a postdoctoral fellowship of the Alexander von Humboldt Foundation. G. G.-R. acknowledges the Deutsche Forschungsgemeinschaft (GO 3526/1-1) for financial support. H.C. thanks Deutsche Forschungsgemeinschaft (DFG) SFB 1214 project B1 for funding. G.C-Z. acknowledges National Natural Science Foundation of China (Grant No. 21902148). Approved Most recent IF: 29.4  
  Call Number EMAT @ emat @c:irua:191808 Serial 7115  
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Author Zhuo, X.; Mychinko, M.; Heyvaert, W.; Larios, D.; Obelleiro-Liz, M.; Taboada, J.M.; Bals, S.; Liz-Marzán, L.M. url  doi
openurl 
  Title Morphological and Optical Transitions during Micelle-Seeded Chiral Growth on Gold Nanorods Type A1 Journal article
  Year 2022 Publication ACS nano Abbreviated Journal Acs Nano  
  Volume Issue Pages  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Chiral plasmonics is a rapidly developing field where breakthroughs and unsolved problems coexist. We have recently reported binary surfactant-assisted seeded growth of chiral gold nanorods (Au NRs) with high chiroptical activity. Such a seeded-growth process involves the use of a chiral cosurfactant that induces micellar helicity, in turn driving the transition from achiral to chiral Au NRs, from both the morphological and the optical points of view. We report herein a detailed study on both transitions, which reveals intermediate states that were hidden so far. The correlation between structure and optical response is carefully analyzed, including the (linear and CD) spectral evolution over time, electron tomography, the impact of NR dimensions on their optical response, the variation of the absorption-to-scattering ratio during the evolution from achiral to chiral Au NRs, and the near-field enhancement related to chiral plasmon modes. Our findings provide further understanding of the growth process of chiral Au NRs and the associated optical changes, which will facilitate further study and applications of chiral nanomaterials.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000878324400001 Publication Date 2022-10-26  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 17.1 Times cited 17 Open Access OpenAccess  
  Notes This work was supported by the European Research Council (ERC-AdG-4DbioSERS-787510 to L.M.L.-M. and ERC-CoG-REALNANO-815128 to S.B.) and the MCIN/AEI/10.13039/501100011033 (Grant PID2020-117779RB-I00). X.Z. acknowledges funding from the Juan de la Cierva fellowship (FJC2018-036104-I) and the University Development Fund (UDF01002665, CUHK-Shenzhen). D.L., M.O.-L., and J.M.T. acknowledge funding from the European Regional Development Fund (ERDF) and the Spanish Ministerio de Ciencia, Innovación y Universidades, under Projects PID2020-116627RB-C21 and PID2020-116627RB-C22, as well as from the ERDF/Galician Regional Government as part of the agreement for funding the Atlantic Research Center for Information and Communication Technologies (atlanTTic) and ERDF/Extremadura Regional Government under Projects IB18073 and GR18055. This work was performed in the framework of the Maria de Maeztu Units of Excellence Program from the Spanish State Research Agency (Grant No. MDM-2017-0720). The authors acknowledge Dr. Guillermo González-Rubio for providing suggestions for synthesis and Dr. Irantzu Llarena for assisting with the CD measurements. Approved Most recent IF: 17.1  
  Call Number EMAT @ emat @c:irua:191815 Serial 7116  
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Author Gao, C.; Hofer, C.; Jannis, D.; Béché, A.; Verbeeck, J.; Pennycook, T.J. pdf  url
doi  openurl
  Title Overcoming contrast reversals in focused probe ptychography of thick materials: An optimal pipeline for efficiently determining local atomic structure in materials science Type A1 Journal article
  Year 2022 Publication Applied physics letters Abbreviated Journal Appl Phys Lett  
  Volume 121 Issue 8 Pages 081906  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract Ptychography provides highly efficient imaging in scanning transmission electron microscopy (STEM), but questions have remained over its applicability to strongly scattering samples such as those most commonly seen in materials science. Although contrast reversals can appear in ptychographic phase images as the projected potentials of the sample increase, we show here how these can be easily overcome by a small amount of defocus. The amount of defocus is small enough that it not only can exist naturally when focusing using the annular dark field (ADF) signal but can also be adjusted post acquisition. The ptychographic images of strongly scattering materials are clearer at finite doses than other STEM techniques and can better reveal light atomic columns within heavy lattices. In addition, data for ptychography can now be collected simultaneously with the fastest of ADF scans. This combination of sensitivity and interpretability presents an ideal workflow for materials science.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000844403300006 Publication Date 2022-08-22  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  ISSN 0003-6951 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 4 Times cited 9 Open Access OpenAccess  
  Notes European Research Council, 802123-HDEM ; HORIZON EUROPE European Research Council, 823717-ESTEEM3 ; Fonds Wetenschappelijk Onderzoek, G042920N ; Fonds Wetenschappelijk Onderzoek, G042820N ; Horizon 2020 Framework Programme, 101017720 ; Fonds Wetenschappelijk Onderzoek, G013122N ; esteem3reported; esteem3jra Approved Most recent IF: 4  
  Call Number EMAT @ emat @c:irua:190670 Serial 7120  
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Author De wael, A.; De Backer, A.; Yu, C.-P.; Sentürk, D.G.; Lobato, I.; Faes, C.; Van Aert, S. pdf  url
doi  openurl
  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.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000854930500001 Publication Date 2022-09-19  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) 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. pdf  url
doi  openurl
  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.
 
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000873778100001 Publication Date 0000-00-00  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) 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  
Permanent link to this record
 

 
Author Arseenko, M.; Hannard, F.; Ding, L.; Zhao, L.; Maire, E.; Villanova, J.; Idrissi, H.; Simar, A. pdf  doi
openurl 
  Title A new healing strategy for metals : programmed damage and repair Type A1 Journal article
  Year 2022 Publication Acta materialia Abbreviated Journal Acta Mater  
  Volume 238 Issue Pages 118241-10  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Self-healing strategies aim at avoiding part repair or even replacement, which is time consuming, expen-sive and generates waste. However, strategies for metallic systems are still under-developed and solid-state solutions for room temperature service are limited to nano-scale damage repair. Here we propose a new healing strategy of micron-sized damage requiring only short and low temperature heating. This new strategy is based on damage localization particles, which can be healed by fast diffusing atoms of the matrix activated during heat treatment. The healing concept was successfully validated with a com-mercial aluminum alloy and manufactured by Friction Stir Processing (FSP). Damage was demonstrated to initiate on particles that were added to the matrix during material processing. In situ 2D and 3D nano -imaging confirmed healing of the damaged material and showed that heating this material for 10 min at 400 degrees C is sufficient to heal incipient damage with complete filling of 70% of all damage (and up to 90% when their initial size is below 0.2 mu m). Furthermore, strength is retained and the work of fracture of the alloy is improved by about 40% after healing. The proposed Programmed Damage and Repair healing strategy could be extended to other metal based systems presenting precipitation. (C) 2022 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000843502700006 Publication Date 2022-08-03  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  ISSN 1359-6454 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 9.4 Times cited Open Access Not_Open_Access  
  Notes Approved Most recent IF: 9.4  
  Call Number UA @ admin @ c:irua:190561 Serial 7121  
Permanent link to this record
 

 
Author Zhang, H.; Pryds, N.; Park, D.-S.; Gauquelin, N.; Santucci, S.; Christensen, D., V.; Jannis, D.; Chezganov, D.; Rata, D.A.; Insinga, A.R.; Castelli, I.E.; Verbeeck, J.; Lubomirsky, I.; Muralt, P.; Damjanovic, D.; Esposito, V. pdf  url
doi  openurl
  Title Atomically engineered interfaces yield extraordinary electrostriction Type A1 Journal article
  Year 2022 Publication Nature Abbreviated Journal  
  Volume 609 Issue 7928 Pages 695-700  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Electrostriction is a property of dielectric materials whereby an applied electric field induces a mechanical deformation proportional to the square of that field. The magnitude of the effect is usually minuscule (<10(-19) m(2) V-2 for simple oxides). However, symmetry-breaking phenomena at the interfaces can offer an efficient strategy for the design of new properties(1,2). Here we report an engineered electrostrictive effect via the epitaxial deposition of alternating layers of Gd2O3-doped CeO2 and Er2O3-stabilized delta-Bi2O3 with atomically controlled interfaces on NdGaO3 substrates. The value of the electrostriction coefficient achieved is 2.38 x 10(-14) m(2) V-2, exceeding the best known relaxor ferroelectrics by three orders of magnitude. Our theoretical calculations indicate that this greatly enhanced electrostriction arises from coherent strain imparted by interfacial lattice discontinuity. These artificial heterostructures open a new avenue for the design and manipulation of electrostrictive materials and devices for nano/micro actuation and cutting-edge sensors.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000859073900001 Publication Date 2022-09-21  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  ISSN 1476-4687 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor Times cited 12 Open Access OpenAccess  
  Notes This research was supported by the BioWings project, funded by the European Union’s Horizon 2020, Future and Emerging Technologies programme (grant no. 801267), and by the Danish Council for Independent Research Technology and Production Sciences for the DFF—Research Project 2 (grant no. 48293). N.P. and D.V.C. acknowledge funding from Villum Fonden for the NEED project (no. 00027993) and from the Danish Council for Independent Research Technology and Production Sciences for the DFF—Research Project 3 (grant no. 00069 B). V.E. acknowledges funding from Villum Fonden for the IRIDE project (no. 00022862). N.G. and J.V. acknowledge funding from the GOA project ('Solarpaint') of the University of Antwerp. The microscope used in this work was partly funded by the Hercules Fund from the Flemish Government. D.J. acknowledges funding from the FWO Project (no. G093417N) from the Flemish Fund for Scientific Research. D.C. acknowledges TOP/BOF funding from the University of Antwerp. This project has received funding from the European Union’s Horizon 2020 Research Infrastructure—Integrating Activities for Advanced Communities—under grant agreement no. 823717-ESTEEM3. We thank T. D. Pomar and A. J. Bergne for English proofreading.; esteem3reported; esteem3TA Approved Most recent IF: NA  
  Call Number UA @ admin @ c:irua:190576 Serial 7129  
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Author Vega Ibañez, F.; Béché, A.; Verbeeck, J. url  doi
openurl 
  Title Can a programmable phase plate serve as an aberration corrector in the transmission electron microscope (TEM)? Type A1 Journal article
  Year 2022 Publication Microscopy and microanalysis Abbreviated Journal Microsc Microanal  
  Volume Issue Pages Pii S1431927622012260-10  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract Current progress in programmable electrostatic phase plates raises questions about their usefulness for specific applications. Here, we explore different designs for such phase plates with the specific goal of correcting spherical aberration in the transmission electron microscope (TEM). We numerically investigate whether a phase plate could provide down to 1 angstrom ngstrom spatial resolution on a conventional uncorrected TEM. Different design aspects (fill factor, pixel pattern, symmetry) were evaluated to understand their effect on the electron probe size and current density. Some proposed designs show a probe size () down to 0.66 angstrom, proving that it should be possible to correct spherical aberration well past the 1 angstrom limit using a programmable phase plate consisting of an array of electrostatic phase-shifting elements.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000849975400001 Publication Date 2022-09-21  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  ISSN 1431-9276 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 2.8 Times cited 3 Open Access OpenAccess  
  Notes All authors acknowledge funding from the Flemish Research Fund under contract G042820N “Exploring adaptive optics in transmission electron microscopy”. J.V. acknowledges funding from the European Union’s Horizon 2020 Research Infrastructure – Integrating Activities for Advanced Communities under grant agreement No 823717 – ESTEEM3 and from the University of Antwerp through a TOP BOF project.; esteem3reported; esteem3jra Approved Most recent IF: 2.8  
  Call Number UA @ admin @ c:irua:190627 Serial 7134  
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Author Penders, A.G.; Konstantinović, M.J.; Van Renterghem, W.; Bosch, R.-W.; Schryvers, D.; Somville, F. pdf  url
doi  openurl
  Title Characterization of IASCC crack tips extracted from neutron-irradiated flux thimble tube specimens in view of a probabilistic fracture model Type A1 Journal article
  Year 2022 Publication Journal of nuclear materials Abbreviated Journal J Nucl Mater  
  Volume 571 Issue Pages 154015-154016  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract This study reports the properties of irradiation assisted stress corrosion crack tips extracted by means of focused-ion beam from 60 to 80 dpa neutron-irradiated O-ring specimens tested under straining conditions under a pressurized-water reactor environment. Various crack tip morphologies and surrounding deformation features were analyzed as a function of applied stress, surface oxidation state and loading form – constant versus cyclic. All investigated cracks exhibit grain boundary oxidation in front of the crack tip, with the extent of oxidation being proportional to applied stress. These findings clearly demonstrate that, under the subcritical crack propagation regime, the grain boundary oxide grows faster than the crack. On the other hand, crack tips appertaining to specimens with removed oxide layer at the outer surface show comparatively less oxidation at the crack tip, which could indicate towards crack initiation from regions that exemplify lower stress, such as the O-ring inner surface. Cyclic loading is found to have a more pronounced effect on the crack tip microstructure, demonstrating increased deformation twinning and -martensitic transformation, which signifies towards an increased susceptibility to intergranular failure. Still, the extent of crack tip grain boundary oxidation in this case agrees well with expected values for maximum stress applied during cyclic loading. All results are interpreted based on the probabilistic subcritical crack propagation mechanism and provide strong support to a stress-driven internal oxidation model.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000872389200009 Publication Date 2022-09-06  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  ISSN 0022-3115 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 3.1 Times cited Open Access OpenAccess  
  Notes Approved Most recent IF: 3.1  
  Call Number UA @ admin @ c:irua:190375 Serial 7135  
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Author Yang, T.; Kong, Y.; Du, Y.; Li, K.; Schryvers, D. url  doi
openurl 
  Title Discovery of core-shell quasicrystalline particles Type A1 Journal article
  Year 2023 Publication Scripta materialia Abbreviated Journal  
  Volume 222 Issue Pages 115040-115046  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Submicron-sized quasicrystalline particles were obtained in an Al-Zn-Mg-Cu alloy produced by traditional melting. These particles consist of an Al-Fe-Ni core and a Mg-Cu-Zn shell and were found to be stable and embedded randomly in the Al matrix. The diffraction patterns of these core-shell particles reveal a decagonal core and an icosahedral shell with, respectively, ten- and five-fold axes aligned. High resolution scanning transmission electron microscopy of the Mg-Cu-Zn shell confirms the five-fold symmetry atomic arrangement and the icosahedral structure. It can therefore be concluded that Fe and Ni impurities play an important role in mediating the formation of such an unusual ternary core-shell quasicrystalline particle. These findings provide some novel insights in the formation of quasicrystals in traditional industrial Al alloys.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000864491400005 Publication Date 2022-09-11  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  ISSN 1359-6462 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 6 Times cited Open Access OpenAccess  
  Notes Approved Most recent IF: 6; 2023 IF: 3.747  
  Call Number UA @ admin @ c:irua:191489 Serial 7144  
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Author Lopez-Garcia, C.; Canossa, S.; Hadermann, J.; Gorni, G.; Oropeza, F.E.; de la Pena O'Shea, V.A.; Iglesias, M.; Monge, M.A.; Gutierrez-Puebla, E.; Gandara, F. url  doi
openurl 
  Title Heterometallic molecular complexes act as messenger building units to encode desired metal-atom combinations to multivariate metal-organic frameworks Type A1 Journal article
  Year 2022 Publication Journal of the American Chemical Society Abbreviated Journal J Am Chem Soc  
  Volume 144 Issue 36 Pages 16262-16266  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract A novel synthetic approach is described for the targeted preparation of multivariate metal-organic frameworks (MTV-MOFs) with specific combinations of metal elements. This methodology is based on the use of molecular complexes that already comprise desired metal-atom combinations, as building units for the MTV-MOF synthesis. These units are transformed into the MOF structural constituents through a ligand/linker exchange process that involves structural modifications while preserving their origina l l y encoded atomic combination. Thus, through the use of heterometalli c ring-shaped molecules combining gallium and nickel or cobalt, we have obtained MOFs with identical combinations of the metal elements, now incorporated in the rod-shaped secondary building unit, as confirmed with a combination of X-ray and electron diffraction, electron microscopy, and X-ray absorption spectroscopy techniques.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000841435900001 Publication Date 2022-08-12  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  ISSN 0002-7863 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 15 Times cited Open Access OpenAccess  
  Notes Approved Most recent IF: 15  
  Call Number UA @ admin @ c:irua:190023 Serial 7169  
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Author Hao, Y. url  openurl
  Title A joint experimental-modeling study of the structure and properties of functional molecular monolayers for the control of organic crystal growth Type Doctoral thesis
  Year 2022 Publication Abbreviated Journal  
  Volume Issue Pages xiii, 174 p.  
  Keywords Doctoral thesis; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Among all types of discovered crystals, those formed by organic molecules show the greatest diversity, which results from the intrinsic complexity of the organic molecules and the weak interactions between them. Even for a given compound, different crystal structures can exist. This feature is referred to as polymorphism in the modern crystallographic context and those different crystal forms are called polymorphs. In reality, the crystallization of organic molecules is often performed at the surface of a substrate, giving rise to heterogeneous crystallization. Except for the well-known catalyzing effects, the existence of substrates brings more possibilities to the polymorphic behaviors of organic molecules, promoting the formation of new polymorphs that are only stable in the vicinity of the substrates. For this reason, these new polymorphic forms are often described as substrate-induced polymorphs (SIPs). It is of great importance to understand the formation of SIPs for organic molecules as it has been reported that SIPs can show superior properties with respect to their bulk form counterparts. Up to now, most studies focus on the identifying and characterizing the presence of SIPs, which relies mainly on X-ray diffraction techniques. However, a detailed explanation about the origin of SIPs is still missing. In this work, we have combined several powerful experimental characterization techniques, including X-ray diffraction, transmission electron microscopy (TEM) and scanning tunneling microscopy (STM) in order to reach an integrated view over the formation of SIPs. These experimental studies are strongly supported by computational chemistry simulations, such as density functional theory and molecular dynamics. A big advantage of using atomistic simulations is that it enables the possibility to predict a priori the crystal structures of SIPs and to establish a posteriori the general rules for the formation of SIPs. In practice, this thesis employs state-of-art atomistic simulation approaches in order to bridge substrate-induced polymorphism with a conceptually-connected research area: the self-assembly of molecular networks (SAMNs), also called 2D crystallization. Unlike SIPs, which extend at least several molecular layers, SAMNs are composed of a single layer of molecules with ordered packing. Our simulations have enabled a more comprehensive understanding about the role of substrate during the formation of SIPs and we elucidate how the positional and orientational order of molecules propagates from the substrate to the upper 2D and even 3D crystal layers. In this way, a fundamental understanding of the substrate-induced crystallization is gained by connecting 2D and 3D crystallization using substrate-induced approaches.  
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  Corporate Author Thesis  
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  Language Wos Publication Date  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  ISSN ISBN Additional Links UA library record  
  Impact Factor Times cited Open Access  
  Notes Approved Most recent IF: NA  
  Call Number UA @ admin @ c:irua:191758 Serial 7176  
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Author Frolov, A.S.; Callaert, C.; Batuk, M.; Hadermann, J.; Volykhov, A.A.; Sirotina, A.P.; Amati, M.; Gregoratti, L.; Yashina, L.V. doi  openurl
  Title Nanoscale phase separation in the oxide layer at GeTe (111) surfaces Type A1 Journal article
  Year 2022 Publication Nanoscale Abbreviated Journal Nanoscale  
  Volume 14 Issue 35 Pages 12918-12927  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract As a semiconductor ferroelectric, GeTe has become a focus of renewed attention due to the recent discovery of giant Rashba splitting. It already has a wide range of applications, from thermoelectricity to data storage. Its stability in ambient air, as well as the structure and properties of an oxide layer, define the processing media for device production and operation. Here, we studied a reaction between the GeTe (111) surface and molecular oxygen for crystals having solely inversion domains. We evaluated the reaction kinetics both ex situ and in situ using NAP XPS. The structure of the oxide layer is extensively discussed, where, according to HAADF-STEM and STEM-EDX, nanoscale phase separation of GeO2 and Te is observed, which is unusual for semiconductors. We believe that such behaviour is closely related to the ferroelectric properties and the domain structure of GeTe.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000847743300001 Publication Date 2022-08-25  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  ISSN 2040-3364; 2040-3372 ISBN Additional Links UA library record; WoS full record  
  Impact Factor 6.7 Times cited Open Access Not_Open_Access  
  Notes Approved Most recent IF: 6.7  
  Call Number UA @ admin @ c:irua:190665 Serial 7181  
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Author Idrissi, H.; Béché, A.; Gauquelin, N.; Ul-Haq, I.; Bollinger, C.; Demouchy, S.; Verbeeck, J.; Pardoen, T.; Schryvers, D.; Cordier, P. url  doi
openurl 
  Title On the formation mechanisms of intragranular shear bands in olivine by stress-induced amorphization Type A1 Journal article
  Year 2022 Publication Acta materialia Abbreviated Journal Acta Mater  
  Volume 239 Issue Pages 118247-118249  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Intragranular amorphization shear lamellae are found in deformed olivine aggregates. The detailed trans-mission electron microscopy analysis of intragranular lamella arrested in the core of a grain provides novel information on the amorphization mechanism. The deformation field is complex and heteroge-neous, corresponding to a shear crack type instability involving mode I, II and III loading components. The formation and propagation of the amorphous lamella is accompanied by the formation of crystal defects ahead of the tip. These defects are geometrically necessary [001] dislocations, characteristics of high-stress deformation in olivine, and rotational nanodomains which are tentatively interpreted as disclinations. We show that these defects play an important role in dictating the path followed by the amorphous lamella. Stress-induced amorphization in olivine would thus result from a direct crystal-to -amorphous transformation associated with a shear instability and not from a mechanical destabilization due to the accumulation of high number of defects from an intense preliminary deformation. The pref-erential alignment of some lamellae along (010) is a proof of the lower ultimate mechanical strength of these planes.(c) 2022 The Authors. Published by Elsevier Ltd on behalf of Acta Materialia Inc. This is an open access article under the CC BY license ( http://creativecommons.org/licenses/by/4.0/ )  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000861076600004 Publication Date 2022-08-05  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  ISSN 1359-6454 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 9.4 Times cited 5 Open Access OpenAccess  
  Notes The QuanTEM microscope was partially funded by the Flemish government. The K2 camera was funded by FWO Hercules fund G0H4316N 'Direct electron detector for soft matter TEM'. A. Beche acknowledges funding from FWO project G093417N ('Compressed sensing enabling low dose imaging in transmission electron microscopy'). H. Idrissi is mandated by the Belgian National Fund for Scientific Research (FSR-FNRS). This work was supported by the FNRS under Grant PDR – T011322F and by the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation programme under grant agreement No 787,198 Time Man. J-L Rouviere is acknowledged for his support with the GPA softawre. Approved Most recent IF: 9.4  
  Call Number UA @ admin @ c:irua:191432 Serial 7186  
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Author Borah, R.; Ninakanti, R.; Bals, S.; Verbruggen, S.W. url  doi
openurl 
  Title Plasmon resonance of gold and silver nanoparticle arrays in the Kretschmann (attenuated total reflectance) vs. direct incidence configuration Type A1 Journal article
  Year 2022 Publication Scientific reports Abbreviated Journal Sci Rep-Uk  
  Volume 12 Issue 1 Pages 15738-19  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Sustainable Energy, Air and Water Technology (DuEL)  
  Abstract While the behaviour of plasmonic solid thin films in the Kretschmann (also known as Attenuated Total Reflection, ATR) configuration is well-understood, the use of discrete nanoparticle arrays in this optical configuration is not thoroughly explored. It is important to do so, since close packed plasmonic nanoparticle arrays exhibit exceptionally strong light-matter interactions by plasmonic coupling. The present work elucidates the optical properties of plasmonic Au and Ag nanoparticle arrays in both the direct normal incidence and Kretschmann configuration by numerical models, that are validated experimentally. First, hexagonal close packed Au and Ag nanoparticle films/arrays are obtained by air–liquid interfacial assembly. The numerical models for the rigorous solution of the Maxwell’s equations are validated using experimental optical spectra of these films before systematically investigating various parameters. The individual far-field/near-field optical properties, as well as the plasmon relaxation mechanism of the nanoparticles, vary strongly as the packing density of the array increases. In the Kretschmann configuration, the evanescent fields arising from p – and s -polarized (or TM and TE polarized) incidence have different directional components. The local evanescent field intensity and direction depends on the polarization, angle of incidence and the wavelength of incidence. These factors in the Kretschmann configuration give rise to interesting far-field as well as near-field optical properties. Overall, it is shown that plasmonic nanoparticle arrays in the Kretschmann configuration facilitate strong broadband absorptance without transmission losses, and strong near-field enhancement. The results reported herein elucidate the optical properties of self-assembled nanoparticle films, pinpointing the ideal conditions under which the normal and the Kretschmann configuration can be exploited in multiple light-driven applications.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000858344700048 Publication Date 2022-09-21  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  ISSN 2045-2322 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 4.6 Times cited 11 Open Access OpenAccess  
  Notes R.B. acknowledges financial support from the University of Antwerp Special Research Fund (BOF) for a DOCPRO4 doctoral scholarship (Grant FN541100001). Approved Most recent IF: 4.6  
  Call Number UA @ admin @ c:irua:190864 Serial 7194  
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Author Guo, A.; Bai, H.; Liang, Q.; Feng, L.; Su, X.; Van Tendeloo, G.; Wu, J. pdf  doi
openurl 
  Title Resistive switching in Ag₂Te semiconductor modulated by Ag+-ion diffusion and phase transition Type A1 Journal article
  Year 2022 Publication Advanced Electronic Materials Abbreviated Journal Adv Electron Mater  
  Volume Issue Pages 2200850-2200858  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Memristors are considered to be the fourth circuit element and have great potential in areas like logic operations, information storage, and neuromorphic computing. The functional material in a memristor, which has a nonlinear resistance, is the key component to be developed. Herein, resistive switching is demonstrated and the structural evolutions in Ag2Te are examined under an external electric field. It is shown that the electroresistance effect is originating from an electronically triggered phase transition together with directional Ag+-ion diffusion. Using in situ transmission electron microscopy, the phase transition from the monoclinic alpha-Ag2Te into the face-centered cubic beta-Ag2Te, accompanied by a change in resistance, is directly observed. Diffusion of Ag+-ions modulates the localized density of Ag+-ion vacancies, leading to a change in electrical conductivity and influences the threshold voltage to trigger the phase transition. During the electric field-driven phase transition, the spontaneous and localized multiple polarizations from the low-symmetry alpha-Ag2Te (referring to an antiferroelectric structure) are vanishing in the cubic beta-Ag2Te (referring to a paraelectric structure). The abrupt resistance change of thin Ag2Te caused by the phase transition and modulated by the applied electric field demonstrates its great potential as functional material in volatile memory and memristors with a low-energy consumption.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000855728500001 Publication Date 2022-09-21  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  ISSN 2199-160x ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 6.2 Times cited Open Access Not_Open_Access  
  Notes Approved Most recent IF: 6.2  
  Call Number UA @ admin @ c:irua:190582 Serial 7203  
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Author Cunha, D.M.; Gauquelin, N.; Xia, R.; Verbeeck, J.; Huijben, M. url  doi
openurl 
  Title Self-assembled epitaxial cathode-electrolyte nanocomposites for 3D microbatteries Type A1 Journal article
  Year 2022 Publication ACS applied materials and interfaces Abbreviated Journal Acs Appl Mater Inter  
  Volume 14 Issue 37 Pages 42208-42214  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract The downscaling of electronic devices requires rechargeable microbatteries with enhanced energy and power densities. Here, we evaluate self-assembled vertically aligned nano-composite (VAN) thin films as a platform to create high-performance three-dimensional (3D) microelectrodes. This study focuses on controlling the VAN formation to enable interface engineering between the LiMn2O4 cathode and the (Li,La)TiO3 solid electrolyte. Electrochemical analysis in a half cell against lithium metal showed the absence of sharp redox peaks due to the confinement in the electrode pillars at the nanoscale. The (100)-oriented VAN thin films showed better rate capability and stability during extensive cycling due to the better alignment to the Li-diffusion channels. However, an enhanced pseudocapacitive contribution was observed for the increased total surface area within the (110)-oriented VAN thin films. These results demonstrate for the first time the electrochemical behavior of cathode-electrolyte VANs for lithium-ion 3D microbatteries while pointing out the importance of control over the vertical interfaces.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000852647100001 Publication Date 2022-09-06  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  ISSN 1944-8244 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 9.5 Times cited 4 Open Access OpenAccess  
  Notes This research was carried out with the support from the Netherlands Organization for Scientific Research (NWO) under VIDI grant no. 13456. Approved Most recent IF: 9.5  
  Call Number UA @ admin @ c:irua:190619 Serial 7206  
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Author Wang, D.; Hermes, M.; Najmr, S.; Tasios, N.; Grau-Carbonell, A.; Liu, Y.; Bals, S.; Dijkstra, M.; Murray, C.B.; van Blaaderen, A. url  doi
openurl 
  Title Structural diversity in three-dimensional self-assembly of nanoplatelets by spherical confinement Type A1 Journal article
  Year 2022 Publication Nature communications Abbreviated Journal Nat Commun  
  Volume 13 Issue 1 Pages 6001-6012  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Nanoplatelets offer many possibilities to construct advanced materials due to new properties associated with their (semi)two-dimensional shapes. However, precise control of both positional and orientational order of the nanoplatelets in three dimensions, which is required to achieve emerging and collective properties, is challenging to realize. Here, we combine experiments, advanced electron tomography and computer simulations to explore the structure of supraparticles self-assembled from nanoplatelets in slowly drying emulsion droplets. We demonstrate that the rich phase behaviour of nanoplatelets, and its sensitivity to subtle changes in shape and interaction potential can be used to guide the self-assembly into a wide range of different structures, offering precise control over both orientation and position order of the nanoplatelets. Our research is expected to shed light on the design of hierarchically structured metamaterials with distinct shape- and orientation- dependent properties. Nanoplatelets can be used as anisotropic building blocks for constructing novel optoelectronic materials. Here, Wang et al. show a route of assembling nanoplatelets with controllable positional and orientational order in three dimensions facilitated by the surface tension of drying emulsion droplets.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000867312100031 Publication Date 2022-10-12  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  ISSN 2041-1723 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 16.6 Times cited 7 Open Access OpenAccess  
  Notes We thank A. Kadu, M. Chiappini, F. Rabouw, S. Paliwal, X. Xie, C. Xia and Z. Wang for fruitful discussions. D.W. and A.v.B. acknowledge partial financial support from the European Research Council under the European Union's Seventh Framework Programme (FP-2007-2013)/ERC Advanced Grant Agreement 291667 HierarSACol. M.H. was supported by the Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC). D.W. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020 program (grant 894254 SuprAtom). Y.L. acknowledges the Sustainability project between the faculties of Science and Geosciences of Utrecht University. M.D. acknowledges financial support from European Research Council (Grant No. ERC-2019-ADV-H2020 884902 SoftML). S.B. acknowledges financial support from ERC Consolidator Grant No. 815128 REALNANO. C.B.M. acknowledges support for materials synthesis from the Office of Naval Research Multidisciplinary University Research Initiative Award ONR N00014-18-1-2497. The authors acknowledge the EM square center at Utrecht University for the access to the microscopes. Approved Most recent IF: 16.6  
  Call Number UA @ admin @ c:irua:191387 Serial 7214  
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Author Sheath, B.C.; Xu, X.; Manuel, P.; Hadermann, J.; Batuk, M.; O'Sullivan, J.; Bonilla, R.S.; Clarke, S.J. url  doi
openurl 
  Title Structures and magnetic ordering in layered Cr oxide arsenides Sr₂CrO₂Cr₂OAs₂ and Sr₂CrO₃CrAs Type A1 Journal article
  Year 2022 Publication Inorganic chemistry Abbreviated Journal Inorg Chem  
  Volume 61 Issue 31 Pages 10-12385  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract Two novel chromium oxide arsenide materials have been synthesized, Sr2CrO2Cr2OAs2 (i.e., Sr2Cr3As2O3) and Sr2CrO3CrAs (i.e., Sr2Cr2AsO3), both of which contain chromium ions in two distinct layers. Sr2CrO2Cr2OAs2 was targeted following electron microscopy measurements on a related phase. It crystallizes in the space group P4/mmm and accommodates distorted CrO4As2 octahedra containing Cr2+ and distorted CrO(2)As(4 )octahedra containing Cr3+. In contrast, Sr2CrO3CrAs incorporates Cr3+ in CrO5 square-pyramidal coordination in [Sr2CrO3](+) layers and Cr2+ ions in CrAs(4 )tetrahedra in [CrAs](-) layers and crystallizes in the space group P4/nmm. Powder neutron diffraction data reveal antiferromagnetic ordering in both compounds. In Sr2CrO3CrAs the Cr2+ moments in the [CrAs](-) layers exhibit long-range ordering, while the Cr3+ moments in the [Sr2CrO3](+) layers only exhibit short-range ordering. However, in Sr2CrO2Cr2OAs2, both the Cr(2+ )moments in the CrO4As2 environments and the Cr3+ moments in the CrO2As4 polyhedra are long-range-ordered below 530(10) K. Above this temperature, only the Cr3+ moments are ordered with a Neel temperature slightly in excess of 600 K. A subtle structural change is evident in Sr2CrO2Cr2OAs2 below the magnetic ordering transitions.  
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  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000841943600001 Publication Date 2022-07-27  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  ISSN 0020-1669 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 4.6 Times cited Open Access OpenAccess  
  Notes Approved Most recent IF: 4.6  
  Call Number UA @ admin @ c:irua:190007 Serial 7215  
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Author Pacquets, L. url  openurl
  Title Towards stable Cu-Ag bimetallic nanoparticles to boost the electrocatalytic CO2 reduction Type Doctoral thesis
  Year 2022 Publication Abbreviated Journal  
  Volume Issue Pages xvi, 188 p.  
  Keywords Doctoral thesis; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)  
  Abstract Ever since the industrial revolution, the emission of greenhouse gasses dramatically increased, resulting in high CO2 concentration in the atmosphere. The electrochemical conversion of CO2 to value added products, such as carbon monoxide, formic acid, methane, ethylene and ethanol is a very promising strategy to inhibit CO2 emissions. Nevertheless, at the moment, the electrochemical CO2 reduction (eCO2R) is not yet industrially viable, mainly due to the lack of good electrocatalysts. On the other hand, core-shell nanoparticles (NPs) have emerged over the last couple of years as promising candidates. It is believed that bimetallic enhancement effects are behind the improved performance of these core-shell NPs when compared to the individual metals. Although widely investigated, there are still some remaining issues and/or open questions. Indeed, the development of a robust and straightforward synthesis method along with fundamental insight into their resistance towards electrochemical stress remains absent. A good control over morphology, size and composition is key in determining which properties are beneficial for the eCO2R. Since these catalysts are designed to be implemented in electrolyzers, they have to maintain long-term performance. This makes the design of a reproducible method, unveiling structure-performance relationships the effect of electrochemical stress, a crucial aspect. Exploring and modifying existing synthesis methods, have led to the acquisition of a robust and reproducible synthesis method where thermal decomposition of the Cu core is combined with the galvanic replacement of Ag in organic solvents. The implementation of this method has led to the design of a wide variety of Cu-Ag bimetallic NPs and enabled to investigate their composition-selectivity profile. Introducing Ag on Cu suppressed hydrogen and increased the CO formation. CO production was boosted by using Cu@Ag core-shells and was promoted even more by changing the type of electrolyte. As these nanoparticles suffered from degradation, the 3D mapping of the structural changes of Cu@Ag core-shells under operating conditions led to the hypothesis of a two-step degradation mechanism where initially Cu leaching was observed with the subsequent sintering of the Ag shells. One approach to avoid this electrochemical degradation, investigated in this research, was the application of an ultrathin carbon layer to protect the active layer. This ultrathin carbon layer operated as a protective layer, suppressing hydrogen production and increasing the stability of the electrocatalyst. In conclusion, the product selectivity can be tuned by using different Cu-Ag bimetallic nanoparticles synthesized through a robust method. Their unique degradation pathway of Cu@Ag core-shell nanoparticles has led to the proposition of a more accurate stabilization strategy. These findings can contribute significantly in the quest for improved electrocatalysts for the eCO2R.  
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  ISSN ISBN Additional Links UA library record  
  Impact Factor Times cited Open Access  
  Notes Approved Most recent IF: NA  
  Call Number UA @ admin @ c:irua:190236 Serial 7221  
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Author Yang, S.; An, H.; Anastasiadou, D.; Xu, W.; Wu, L.; Wang, H.; de Ruiter, J.; Arnouts, S.; Figueiredo, M.C.; Bals, S.; Altantzis, T.; van der Stam, W.; Weckhuysen, B.M. url  doi
openurl 
  Title Waste-derived copper-lead electrocatalysts for CO₂ reduction Type A1 Journal article
  Year 2022 Publication ChemCatChem Abbreviated Journal Chemcatchem  
  Volume 14 Issue 18 Pages e202200754-11  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)  
  Abstract It remains a real challenge to control the selectivity of the electrocatalytic CO2 reduction (eCO(2)R) reaction to valuable chemicals and fuels. Most of the electrocatalysts are made of non-renewable metal resources, which hampers their large-scale implementation. Here, we report the preparation of bimetallic copper-lead (CuPb) electrocatalysts from industrial metallurgical waste. The metal ions were extracted from the metallurgical waste through simple chemical treatment with ammonium chloride, and CuxPby electrocatalysts with tunable compositions were fabricated through electrodeposition at varying cathodic potentials. X-ray spectroscopy techniques showed that the pristine electrocatalysts consist of Cu-0, Cu1+ and Pb2+ domains, and no evidence for alloy formation was found. We found a volcano-shape relationship between eCO(2)R selectivity toward two electron products, such as CO, and the elemental ratio of Cu and Pb. A maximum Faradaic efficiency towards CO was found for Cu9.00Pb1.00, which was four times higher than that of pure Cu, under the same electrocatalytic conditions. In situ Raman spectroscopy revealed that the optimal amount of Pb effectively improved the reducibility of the pristine Cu1+ and Pb2+ domains to metallic Cu and Pb, which boosted the selectivity towards CO by synergistic effects. This work provides a framework of thinking to design and tune the selectivity of bimetallic electrocatalysts for CO2 reduction through valorization of metallurgical waste.  
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  Language Wos 000853941300001 Publication Date 2022-06-28  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  ISSN 1867-3880; 1867-3899 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 4.5 Times cited 7 Open Access OpenAccess  
  Notes S.Y and B.M.W. acknowledge support from the EU Framework Programme for Research and Innovation Horizon 2020 (SOCRATES-721385; project website: http://etn-socrates.eu/). W.v.d.S., M.C.F. and B.M.W. acknowledge support from the Strategic UU-TU/e Alliance project 'Joint Centre for Chemergy Research'. S.B. acknowledges support from the European Research Council (ERC Consolidator Grant #815128 REALNANO). S.A. and T.A. acknowledge funding from the University of Antwerp Research fund (BOF). The Beijing Synchrotron Radiation Facility (1W1B, BSRF) is acknowledged for the beamtime. We are grateful to Annelies van der Bok and Bas Salzmann (Condensed Matter and Interfaces, Utrecht University, UU) for the support with the ICP-OES measurements. The authors thank dr. Robin Geitenbeek, Nikos Nikolopoulos, Ioannis Nikolopoulos, Jochem Wijten and Joris Janssens (Inorganic Chemistry and Catalysis, UU) for helpful discussions and technical support. The authors also thank Yuang Piao (Materials Chemistry and Catalysis, UU) for the help in the preparation of the figures of the article. Approved Most recent IF: 4.5  
  Call Number UA @ admin @ c:irua:190703 Serial 7226  
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Author Batuk, M.; Vandemeulebroucke, D.; Ceretti, M.; Paulus, W.; Hadermann, J. url  doi
openurl 
  Title Topotactic redox cycling in SrFeO2.5+δ explored by 3D electron diffraction in different gas atmospheres Type A1 Journal article
  Year 2022 Publication Journal of materials chemistry A : materials for energy and sustainability Abbreviated Journal J Mater Chem A  
  Volume Issue Pages  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract For oxygen conducting materials applied in solid oxide fuel cells and chemical-looping processes, the understanding of the oxygen diffusion mechanism and the materials’ crystal structure at different stages of the redox reactions is a key parameter to control their performance. In this paper we report the first ever in situ 3D ED experiment in a gas environment and with it uncover the structure evolution of SrFeO2.5 as notably different from that reported from in situ X-ray and in situ neutron powder diffraction studies in gas environments. Using in situ 3D ED on submicron sized single crystals obtained from a high quality monodomain SrFeO2.5 single crystal , we observe the transformation under O2 flow of SrFeO2.5 with an intra- and interlayer ordering of the left and right twisted (FeO4) tetrahedral chains (space group Pcmb) into consecutively SrFeO2.75 with space group Cmmm (at 350°C, 33% O2) and SrFeO3-δ with space group Pm3 ̅m (at 400°C, 100% O2). Upon reduction in H2 flow, the crystals return to the brownmillerite structure with intralayer order, but without regaining the interlayer order of the pristine crystals. Therefore, redox cycling of SrFeO2.5 crystals in O2 and H2 introduces stacking faults into the structure, resulting in an I2/m(0βγ)0s symmetry with variable β.  
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  Language Wos 000891928400001 Publication Date 0000-00-00  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  ISSN 2050-7488 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 11.9 Times cited Open Access OpenAccess  
  Notes Financial support is acknowledged from the FWO-Hercules fund I003218N ‘Infrastructure for imaging nanoscale processes in gas/vapor or liquid environments’, from the University of Antwerp through grant BOF TOP 38689. This work was supported by the European Commission Horizon 2020 NanED grant number 956099. Financial support from the French National Research Agency (ANR) through the project “Structural induced Electronic Complexity controlled by low temperature Topotactic Reaction” (SECTOR No. ANR-14-CE36- 0006-01) is gratefully acknowledged. Approved Most recent IF: 11.9  
  Call Number EMAT @ emat @c:irua:192325 Serial 7229  
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Author Parastaev, A.; Muravev, V.; Osta, E.H.; Kimpel, T.F.; Simons, J.F.M.; van Hoof, A.J.F.; Uslamin, E.; Zhang, L.; Struijs, J.J.C.; Burueva, D.B.; Pokochueva, E.V.; Kovtunov, K.V.; Koptyug, I.V.; Villar-Garcia, I.J.; Escudero, C.; Altantzis, T.; Liu, P.; Béché, A.; Bals, S.; Kosinov, N.; Hensen, E.J.M. url  doi
openurl 
  Title Breaking structure sensitivity in CO2 hydrogenation by tuning metal–oxide interfaces in supported cobalt nanoparticles Type A1 Journal article
  Year 2022 Publication Nature Catalysis Abbreviated Journal Nat Catal  
  Volume 5 Issue 11 Pages 1051-1060  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)  
  Abstract A high dispersion of the active metal phase of transition metals on oxide supports is important when designing efficient heterogeneous catalysts. Besides nanoparticles, clusters and even single metal atoms can be attractive for a wide range of reactions. However, many industrially relevant catalytic transformations suffer from structure sensitivity, where reducing the size of the metal particles below a certain size substantially lowers catalytic performance. A case in point is the low activity of small cobalt nanoparticles in the hydrogenation of CO and CO2. Here we show how engineering of catalytic sites at the metal–oxide interface in cerium oxide–zirconium dioxide (ceria–zirconia)-supported cobalt can overcome this structure sensitivity. Few-atom cobalt clusters dispersed on 3 nm cobalt(II)-oxide particles stabilized by ceria–zirconia yielded a highly active CO2 methanation catalyst with a specific activity higher than that of larger particles under the same conditions.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000884939300006 Publication Date 2022-11-17  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  ISSN 2520-1158 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 37.8 Times cited 32 Open Access OpenAccess  
  Notes This research was supported by the Applied and Engineering Sciences division of the Netherlands Organization for Scientific Research through the Alliander (now Qirion) Perspective program on Plasma Conversion of CO2. We acknowledge Diamond Light Source for time on beamline B18 under proposal SP20715-1. This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 823717 – ESTEEM3. S.B. acknowledges support from the European Research Council (ERC Consolidator Grant #815128 REALNANO) and T.A. acknowledges funding from the University of Antwerp Research fund (BOF). A.B. received funding from the European Union under grant agreement No 823717 – ESTEEM3. The authors acknowledge funding through the Hercules grant (FWO, University of Antwerp) I003218N “Infrastructure for imaging nanoscale processes in gas/vapour or liquid environments”. I.V.K., D.B.B., and E.V.P. acknowledge the Russian Ministry of Science and Higher Education (contract 075-15-2021-580) for financial support of parahydrogen-based studies. Experiments using synchrotron radiation XPS were performed at the CIRCE beamline at ALBA Synchrotron with the collaboration of ALBA staff. F. Oropeza Palacio and Rim C.J. van de Poll are acknowledged for the help with RPES measurements.; esteem3reported; esteem3jra Approved Most recent IF: 37.8  
  Call Number EMAT @ emat @c:irua:192068 Serial 7230  
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Author Martin, É.; Gossuin, Y.; Bals, S.; Kavak, S.; Vuong, Q.L. pdf  url
doi  openurl
  Title Monte Carlo simulations of the magnetic behaviour of iron oxide nanoparticle ensembles: taking size dispersion, particle anisotropy, and dipolar interactions into account Type A1 Journal article
  Year 2022 Publication European physical journal : B : condensed matter and complex systems Abbreviated Journal Eur Phys J B  
  Volume 95 Issue 12 Pages 201  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract In this work, the magnetic properties of superparamagnetic iron oxide nanoparticles (SPIONs) submitted to an external magnetic field are studied using a Metropolis algorithm. The influence on the M(B) curves of the size distribution of the nanoparticles, of uniaxial anisotropy, and of dipolar interaction between the cores are examined, as well as the influence of drying the samples under a zero or non-zero magnetic field. It is shown that the anisotropy impacts the shape of the magnetization curves, which then deviate from a pure Langevin behaviour, whereas the dipolar interaction has no influence on the curves at 300 K for small particles (with a radius of 3 nm). The fitting of the magnetization curves of particles with magnetic anisotropy to a Langevin model (including a size distribution of the particles) can then lead to erroneous values of the distribution parameters. The simulation results are qualitatively compared to experimental results obtained for iron oxide nanoparticles (with a 3.21 nm median radius).  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000901937400001 Publication Date 2022-12-21  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  ISSN 1434-6028 ISBN Additional Links UA library record; WoS full record  
  Impact Factor 1.6 Times cited Open Access OpenAccess  
  Notes The authors would like to thank Sophie Laurent from the University of Mons for the access to the Dynamic Light Scattering equipment. Computational resources have been provided by the Consortium des Equipements de Calcul Intensif (C ´ ECI), funded by the ´ Fonds de la Recherche Scientifique de Belgique (F.R.S.- FNRS) under Grant No. 2.5020.11 and by the Walloon Region. Approved Most recent IF: 1.6  
  Call Number EMAT @ emat @c:irua:192706 Serial 7232  
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Author Wang, J.; Zhang, K.; Kavak, S.; Bals, S.; Meynen, V. pdf  url
doi  openurl
  Title Modifying the Stöber Process: Is the Organic Solvent Indispensable? Type A1 Journal Article
  Year 2022 Publication Chemistry-A European Journal Abbreviated Journal Chem-Eur J  
  Volume Issue Pages  
  Keywords A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;  
  Abstract The Stöber method is one of the most important and fundamental processes for the synthesis of inorganic (nano)materials but has the drawback of using a large amount of organic solvent. Herein, ethanol was used as an example to explore if the organic solvent in a typical Stöber method can be omitted. It was found that ethanol increases the particle size of the obtained silica spheres and aids the formation of uniform silica particles rather than forming a gel. Nevertheless, the results indicated that an organic solvent in the initial synthesis mixture is not indispensable. An initially immiscible synthesis method was discovered, which can replace the organic solvent-based Stöber method to successfully synthesize silica particles with the same size ranges as the original Stöber process without addition of organic solvents. Moreover, this process can be of further value for the extension to synthesis processes of other materials based on the Stöber process.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000898283500001 Publication Date 2022-12-14  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  ISSN 0947-6539 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 4.3 Times cited 3 Open Access OpenAccess  
  Notes The authors are grateful to Alexander Vansant and Dr. Steven Mullens of VITO for their contributions to the DLS measurements in this paper. J.W acknowledges the State Scholarship funded by the China Scholarship Council (201806060123). K.Z acknowledges the EASiCHEM project funded by the Flemish Strategic Basic Research Program of the Catalisti cluster and Flanders Innovation & Entrepreneurship (HBC.2018.0484). S.K acknowledges the Flemish Fund for Scientific Research (FWO Flanders) through a PhD research grant (1181122N). Approved Most recent IF: 4.3  
  Call Number EMAT @ emat @c:irua:191646 Serial 7233  
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Author De Backer, A.; Bals, S.; Van Aert, S. pdf  url
doi  openurl
  Title A decade of atom-counting in STEM: From the first results toward reliable 3D atomic models from a single projection Type A1 Journal article
  Year 2023 Publication Ultramicroscopy Abbreviated Journal  
  Volume Issue Pages 113702  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract Quantitative structure determination is needed in order to study and understand nanomaterials at the atomic scale. Materials characterisation resulting in precise structural information is a crucial point to understand the structure–property relation of materials. Counting the number of atoms and retrieving the 3D atomic structure of nanoparticles plays an important role here. In this paper, an overview will be given of the atom-counting methodology and its applications over the past decade. The procedure to count the number of atoms will be discussed in detail and it will be shown how the performance of the method can be further improved. Furthermore, advances toward mixed element nanostructures, 3D atomic modelling based on the atom-counting results, and quantifying the nanoparticle dynamics will be highlighted.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000953765800001 Publication Date 2023-02-10  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  ISSN 0304-3991 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 2.2 Times cited 3 Open Access OpenAccess  
  Notes This work was supported by the European Research Council (Grant 770887 PICOMETRICS to S. Van Aert, Grant 815128 REALNANO to S. Bals, 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 EOS 30489208) and a postdoctoral grant to A. De Backer. S. Van Aert acknowledges funding from the University of Antwerp Research fund (BOF) . The authors also thank the colleagues who have contributed to this work over the years, including T. Altantzis, E. Arslan Irmak, K.J. Batenburg, E. Bladt, A. De wael, R. Erni, C. Faes, B. Goris, L. Jones, L.M. Liz-Marzán, I. Lobato, G.T. Martinez, P.D. Nellist, M.D. Rosell, A. Rosenauer, K.H.W. van den Bos, A. Varambhia, and Z. Zhang.; esteem3reported; esteem3JRA Approved Most recent IF: 2.2; 2023 IF: 2.843  
  Call Number EMAT @ emat @c:irua:195896 Serial 7236  
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Author Marchetti, A.; Gori, A.; Ferretti, A.M.; Esteban, D.A.; Bals, S.; Pigliacelli, C.; Metrangolo, P. url  doi
openurl 
  Title Templated Out‐of‐Equilibrium Self‐Assembly of Branched Au Nanoshells Type A1 Journal article
  Year 2023 Publication Small Abbreviated Journal  
  Volume Issue Pages 2206712  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Out-of-equilibrium self-assembly of metal nanoparticles (NPs) has been devised using different types of strategies and fuels, but the achievement of finite 3D structures with a controlled morphology through this assembly mode is still rare. Here we used a spherical peptide-gold superstructure (PAuSS) as a template to control the out-of-equilibrium self-assembly of Au NPs, obtaining a transient 3D branched Au-nanoshell (BAuNS) stabilized by sodium dodecyl sulphate (SDS). The BAuNS dismantled upon concentration gradient equilibration over time in the solution, leading to NPs disassembly. Notably, BAuNS assembly and disassembly favoured temporary interparticle plasmonic coupling, leading to a remarkable oscillation of their optical properties.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000914725800001 Publication Date 2023-01-17  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  ISSN 1613-6810 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 13.3 Times cited 1 Open Access OpenAccess  
  Notes European Research Council, ERC‐2017‐PoC MINIRES 789815 ERC‐2012‐StG_20111012 FOLDHALO 307108 815128 ; Approved Most recent IF: 13.3; 2023 IF: 8.643  
  Call Number EMAT @ emat @c:irua:194299 Serial 7247  
Permanent link to this record
 

 
Author Chowdhury, M.S.; Rösch, E.L.; Esteban, D.A.; Janssen, K.-J.; Wolgast, F.; Ludwig, F.; Schilling, M.; Bals, S.; Viereck, T.; Lak, A. url  doi
openurl 
  Title Decoupling the Characteristics of Magnetic Nanoparticles for Ultrahigh Sensitivity Type A1 Journal article
  Year 2023 Publication Nano letters Abbreviated Journal  
  Volume 23 Issue 1 Pages 58-65  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Immunoassays exploiting magnetization dynamics of magnetic nanoparticles are highly promising for mix-and-measure, quantitative, and point-of-care diagnostics. However, how single-core magnetic nanoparticles can be employed to reduce particle concentration and concomitantly maximize assay sensitivity is not fully understood. Here, we design monodisperse Néel and Brownian relaxing magnetic nanocubes (MNCs) of different sizes and compositions. We provide insights into how to decouple physical properties of these MNCs to achieve ultrahigh sensitivity. We find that tri-component-based Zn0.06 Co0.80Fe2.14 O4 particles, with out-of-phase to initial magnetic susceptibility χ /χ ratio of 0.47 out of 0.50 for magnetically blocked ideal particles, show the ultrahigh magnetic sensitivity by providing rich magnetic particle spectroscopy (MPS) harmonics spectrum despite bearing lower saturation magnetization than di-component Zn0.1Fe2.9O4 having high saturation magnetization. The Zn0.06Co0.80Fe2.14O4 MNCs, coated with catechol-based polyethylene glycol ligands, measured by our benchtop MPS show three orders of magnitude better particle LOD than that of commercial nanoparticles of comparable size.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000907816300001 Publication Date 2023-01-11  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume (down) Series Issue Edition  
  ISSN 1530-6984 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 10.8 Times cited 1 Open Access OpenAccess  
  Notes Deutsche Forschungsgemeinschaft, DFG RTG 1952 ; Joachim Herz Stiftung; H2020 Research Infrastructures, 823717 ; Approved Most recent IF: 10.8; 2023 IF: 12.712  
  Call Number EMAT @ emat @c:irua:193406 Serial 7248  
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