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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. | ||||
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. | ||||
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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 | 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 | Batuk, M.; Vandemeulebroucke, D.; Ceretti, M.; Paulus, W.; Hadermann, J. | ||||
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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Publisher | Place of Publication | Editor | |||
Language | Wos | 000891928400001 | Publication Date | 0000-00-00 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | 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 | Martin, É.; Gossuin, Y.; Bals, S.; Kavak, S.; Vuong, Q.L. | ||||
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). | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000901937400001 | Publication Date | 2022-12-21 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | 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 | Chowdhury, M.S.; Rösch, E.L.; Esteban, D.A.; Janssen, K.-J.; Wolgast, F.; Ludwig, F.; Schilling, M.; Bals, S.; Viereck, T.; Lak, A. | ||||
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. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000907816300001 | Publication Date | 2023-01-11 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1530-6984 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 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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Author | Marchetti, A.; Gori, A.; Ferretti, A.M.; Esteban, D.A.; Bals, S.; Pigliacelli, C.; Metrangolo, P. | ||||
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. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000914725800001 | Publication Date | 2023-01-17 | |
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 | 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 | ||
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Author | Daele, K.V.; Arenas‐Esteban, D.; Choukroun, D.; Hoekx, S.; Rossen, A.; Daems, N.; Pant, D.; Bals, S.; Breugelmans, T. | ||||
Title | Enhanced Pomegranate‐Structured SnO2Electrocatalysts for the Electrochemical CO2Reduction to Formate | Type | A1 Journal article | ||
Year | 2023 | Publication | ChemElectroChem | Abbreviated Journal | |
Volume | Issue | Pages | |||
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) | ||||
Abstract | Although most state-of-the-art Sn-based electrocatalysts yield promising results in terms of selectivity and catalyst activity, their stability remains insufficient to date. Here, we demonstrate the successful application of the recently developed pomegranate-structured SnO2 (Pom. SnO2) and SnO2@C (Pom. SnO2@C) nanocomposite electrocatalysts for the efficient electrochemical conversion of CO2 to formate. With an initial selectivity of 83 and 86% towards formate and an operating potential of -0.72 V and -0.64 V vs. RHE, respectively, these pomegranate SnO2 electrocatalysts are able to compete with most of the current state-of-the-art Sn-based electrocatalysts in terms of activity and selectivity. Given the importance of electrocatalyst stability, long-term experiments (24 h) were performed and a temporary loss in selectivity for the Pom. SnO2@C electrocatalyst was largely restored to its initial selectivity upon drying and exposure to air. Of all the used (24 h) electrocatalysts, the pomegranate SnO2@C had the highest selectivity over a time period of one hour, reaching an average recovered FE of 85%, while the commercial SnO2 and bare pomegranate SnO2 electrocatalysts reached an average of 79 and 80% FE towards formate, respectively. Furthermore, the pomegranate structure of Pom. SnO2@C was largely preserved due to the presence of the heterogeneous carbon shell, which acts as a protective layer, physically inhibiting particle segregation/pulverisation and agglomeration. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000936694800001 | Publication Date | 2023-02-15 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2196-0216 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 4 | Times cited | Open Access | OpenAccess | |
Notes | European Regional Development Fund, E2C 2S03-019 ; | Approved | Most recent IF: 4; 2023 IF: 4.136 | ||
Call Number | EMAT @ emat @c:irua:195228 | Serial | 7249 | ||
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Author | Craig, T.M.; Kadu, A.A.; Batenburg, K.J.; Bals, S. | ||||
Title | Real-time tilt undersampling optimization during electron tomography of beam sensitive samples using golden ratio scanning and RECAST3D | Type | A1 Journal article | ||
Year | 2023 | Publication | Nanoscale | Abbreviated Journal | |
Volume | 15 | Issue | 11 | Pages | 5391-5402 |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | Electron tomography is a widely used technique for 3D structural analysis of nanomaterials, but it can cause damage to samples due to high electron doses and long exposure times. To minimize such damage, researchers often reduce beam exposure by acquiring fewer projections through tilt undersampling. However, this approach can also introduce reconstruction artifacts due to insufficient sampling. Therefore, it is important to determine the optimal number of projections that minimizes both beam exposure and undersampling artifacts for accurate reconstructions of beam-sensitive samples. Current methods for determining this optimal number of projections involve acquiring and post-processing multiple reconstructions with different numbers of projections, which can be time-consuming and requires multiple samples due to sample damage. To improve this process, we propose a protocol that combines golden ratio scanning and quasi-3D reconstruction to estimate the optimal number of projections in real-time during a single acquisition. This protocol was validated using simulated and realistic nanoparticles, and was successfully applied to reconstruct two beam-sensitive metal–organic framework complexes. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000937908900001 | Publication Date | 2023-02-13 | |
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 | 6.7 | Times cited | 1 | Open Access | OpenAccess |
Notes | H2020 European Research Council, 815128 ; H2020 Marie Skłodowska-Curie Actions, 860942 ; | Approved | Most recent IF: 6.7; 2023 IF: 7.367 | ||
Call Number | EMAT @ emat @c:irua:195235 | Serial | 7260 | ||
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Author | de la Encarnación, C.; Jungwirth, F.; Vila-Liarte, D.; Renero-Lecuna, C.; Kavak, S.; Orue, I.; Wilhelm, C.; Bals, S.; Henriksen-Lacey, M.; Jimenez de Aberasturi, D.; Liz-Marzán, L.M. | ||||
Title | Hybrid core–shell nanoparticles for cell-specific magnetic separation and photothermal heating | Type | A1 Journal article | ||
Year | 2023 | Publication | Journal of materials chemistry B : materials for biology and medicine | Abbreviated Journal | |
Volume | Issue | Pages | |||
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Hyperthermia, as the process of heating a malignant site above 42 °C to trigger cell death, has emerged as an effective and selective cancer therapy strategy. Various modalities of hyperthermia have been proposed, among which magnetic and photothermal hyperthermia are known to benefit from the use of nanomaterials. In this context, we introduce herein a hybrid colloidal nanostructure comprising plasmonic gold nanorods (AuNRs) covered by a silica shell, onto which iron oxide nanoparticles (IONPs) are subsequently grown. The resulting hybrid nanostructures are responsive to both external magnetic fields and near-infrared irradiation. As a result, they can be applied for the targeted magnetic separation of selected cell populations – upon targeting by antibody functionalization – as well as for photothermal heating. Through this combined functionality, the therapeutic effect of photothermal heating can be enhanced. We demonstrate both the fabrication of the hybrid system and its application for targeted photothermal hyperthermia of human glioblastoma cells. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000968908400001 | Publication Date | 2023-04-05 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2050-750X | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 7 | Times cited | 1 | Open Access | OpenAccess |
Notes | Ministerio de Ciencia e Innovación, PID2019-108854RA-I00 ; H2020 European Research Council, ERC AdG 787510, 4DBIOSERS ERC CoG 815128, REALNANO ; Fonds Wetenschappelijk Onderzoek, PhD research grant 1181122N ; | Approved | Most recent IF: 7; 2023 IF: 4.543 | ||
Call Number | EMAT @ emat @c:irua:195879 | Serial | 7261 | ||
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Author | Vlasov, E.; Denisov, N.; Verbeeck, J. | ||||
Title | Low-cost electron detector for scanning electron microscope | Type | A1 Journal article | ||
Year | 2023 | Publication | HardwareX | Abbreviated Journal | HardwareX |
Volume | 14 | Issue | Pages | e00413 | |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Electron microscopy is an indispensable tool for the characterization of (nano) materials. Electron microscopes are typically very expensive and their internal operation is often shielded from the user. This situation can provide fast and high quality results for researchers focusing on e.g. materials science if they have access to the relevant instruments. For researchers focusing on technique development, wishing to test novel setups, however, the high entry price can lead to risk aversion and deter researchers from innovating electron microscopy technology further. The closed attitude of commercial entities about how exactly the different parts of electron microscopes work, makes it even harder for newcomers in this field. Here we propose an affordable, easy-to-build electron detector for use in a scanning electron microscope (SEM). The aim of this project is to shed light on the functioning of such detectors as well as show that even a very modest design can lead to acceptable performance while providing high flexibility for experimentation and customization. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 001042486000001 | Publication Date | 2023-03-10 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2468-0672 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | Times cited | 1 | Open Access | OpenAccess | |
Notes | The authors acknowledge the financial support of the Research Foundation Flanders (FWO, Belgium) project SBO [Grant No. S000121N]. JV acknowledges funding from the HORIZON-INFRA-2022-TECH-01-01 project IMPRESS [Grant No. 101094299]. | Approved | Most recent IF: NA | ||
Call Number | EMAT @ emat @c:irua:195886 | Serial | 7252 | ||
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Author | Zhang, Z.; Lobato, I.; De Backer, A.; Van Aert, S.; Nellist, P. | ||||
Title | Fast generation of calculated ADF-EDX scattering cross-sections under channelling conditions | Type | A1 Journal article | ||
Year | 2023 | Publication | Ultramicroscopy | Abbreviated Journal | |
Volume | 246 | Issue | Pages | 113671 | |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Advanced materials often consist of multiple elements which are arranged in a complicated structure. Quantitative scanning transmission electron microscopy is useful to determine the composition and thickness of nanostructures at the atomic scale. However, significant difficulties remain to quantify mixed columns by comparing the resulting atomic resolution images and spectroscopy data with multislice simulations where dynamic scattering needs to be taken into account. The combination of the computationally intensive nature of these simulations and the enormous amount of possible mixed column configurations for a given composition indeed severely hamper the quantification process. To overcome these challenges, we here report the development of an incoherent non-linear method for the fast prediction of ADF-EDX scattering cross-sections of mixed columns under channelling conditions. We first explain the origin of the ADF and EDX incoherence from scattering physics suggesting a linear dependence between those two signals in the case of a high-angle ADF detector. Taking EDX as a perfect incoherent reference mode, we quantitatively examine the ADF longitudinal incoherence under different microscope conditions using multislice simulations. Based on incoherent imaging, the atomic lensing model previously developed for ADF is now expanded to EDX, which yields ADF-EDX scattering cross-section predictions in good agreement with multislice simulations for mixed columns in a core–shell nanoparticle and a high entropy alloy. The fast and accurate prediction of ADF-EDX scattering cross-sections opens up new opportunities to explore the wide range of ordering possibilities of heterogeneous materials with multiple elements. | ||||
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Corporate Author | Zezhong Zhang | Thesis | |||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000995063900001 | Publication Date | 2022-12-28 | |
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 | European Research Council 770887 PICOMETRICS; Fonds Wetenschappelijk Onderzoek No.G.0502.18N; Horizon 2020, 770887 ; Horizon 2020 Framework Programme; European Research Council, 823717 ESTEEM3 ; esteem3reported; esteem3JRa | Approved | Most recent IF: 2.2; 2023 IF: 2.843 | ||
Call Number | EMAT @ emat @c:irua:195890 | Serial | 7251 | ||
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Author | van der Sluijs, M.M.; Salzmann, B.B.V.; Arenas Esteban, D.; Li, C.; Jannis, D.; Brafine, L.C.; Laning, T.D.; Reinders, J.W.C.; Hijmans, N.S.A.; Moes, J.R.; Verbeeck, J.; Bals, S.; Vanmaekelbergh, D. | ||||
Title | Study of the Mechanism and Increasing Crystallinity in the Self-Templated Growth of Ultrathin PbS Nanosheets | Type | A1 Journal article | ||
Year | 2023 | Publication | Chemistry of materials | Abbreviated Journal | |
Volume | Issue | Pages | |||
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Colloidal 2D semiconductor nanocrystals, the analogue of solid-state quantum wells, have attracted strong interest in material science and physics. Molar quantities of suspended quantum objects with spectrally pure absorption and emission can be synthesized. For the visible region, CdSe nanoplatelets with atomically precise thickness and tailorable emission have been (almost) perfected. For the near-infrared region, PbS nanosheets (NSs) hold strong promise, but the photoluminescence quantum yield is low and many questions on the crystallinity, atomic structure, intriguing rectangular shape, and formation mechanism remain to be answered. Here, we report on a detailed investigation of the PbS NSs prepared with a lead thiocyanate single source precursor. Atomically resolved HAADF-STEM imaging reveals the presence of defects and small cubic domains in the deformed orthorhombic PbS crystal lattice. Moreover, variations in thickness are observed in the NSs, but only in steps of 2 PbS monolayers. To study the reaction mechanism, a synthesis at a lower temperature allowed for the study of reaction intermediates. Specifically, we studied the evolution of pseudo-crystalline templates towards mature, crystalline PbS NSs. We propose a self-induced templating mechanism based on an oleylamine-lead-thiocyanate (OLAM-Pb-SCN) complex with two Pb-SCN units as a building block; the interactions between the long-chain ligands regulate the crystal structure and possibly the lateral dimensions. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000959572100001 | Publication Date | 2023-03-25 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0897-4756 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.6 | Times cited | 2 | Open Access | OpenAccess |
Notes | H2020 Research Infrastructures, 731019 ; H2020 European Research Council, 692691 815128 ; Nederlandse Organisatie voor Wetenschappelijk Onderzoek, 715.016.002 ; | Approved | Most recent IF: 8.6; 2023 IF: 9.466 | ||
Call Number | EMAT @ emat @c:irua:195894 | Serial | 7255 | ||
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Author | De Backer, A.; Bals, S.; Van Aert, S. | ||||
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. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000953765800001 | Publication Date | 2023-02-10 | |
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 | 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 | Jain, N.; Hao, Y.; Parekh, U.; Kaltenegger, M.; Pedrazo-Tardajos, A.; Lazzaroni, R.; Resel, R.; Geerts, Y.H.; Bals, S.; Van Aert, S. | ||||
Title | Exploring the effects of graphene and temperature in reducing electron beam damage: A TEM and electron diffraction-based quantitative study on Lead Phthalocyanine (PbPc) crystals | Type | A1 Journal article | ||
Year | 2023 | Publication | Micron | Abbreviated Journal | |
Volume | 169 | Issue | Pages | 103444 | |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | High-resolution transmission electron microscopy (TEM) of organic crystals, such as Lead Phthalocyanine (PbPc), is very challenging since these materials are prone to electron beam damage leading to the breakdown of the crystal structure during investigation. Quantification of the damage is imperative to enable high-resolution imaging of PbPc crystals with minimum structural changes. In this work, we performed a detailed electron diffraction study to quantitatively measure degradation of PbPc crystals upon electron beam irradiation. Our study is based on the quantification of the fading intensity of the spots in the electron diffraction patterns. At various incident dose rates (e/Å2/s) and acceleration voltages, we experimentally extracted the decay rate (1/s), which directly correlates with the rate of beam damage. In this manner, a value for the critical dose (e/Å2) could be determined, which can be used as a measure to quantify beam damage. Using the same methodology, we explored the influence of cryogenic temperatures, graphene TEM substrates, and graphene encapsulation in prolonging the lifetime of the PbPc crystal structure during TEM investigation. The knowledge obtained by diffraction experiments is then translated to real space high-resolution TEM imaging of PbPc. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000965998800001 | Publication Date | 2023-03-21 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0968-4328 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 2.4 | Times cited | 1 | Open Access | OpenAccess |
Notes | This work is supported by FWO and FNRS within the 2Dto3D network of the EOS (Excellence of Science) program (grant number 30489208) and ERC-CoGREALNANO-815128 (to Prof. Dr. Sara Bals). N.J. would like to thank Dr. Kunal S. Mali and Dr. Da Wang for useful and interesting discussions on sample preparation procedures. | Approved | Most recent IF: 2.4; 2023 IF: 1.98 | ||
Call Number | EMAT @ emat @c:irua:196069 | Serial | 7379 | ||
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Author | Benedoue, S.; Benedet, M.; Gasparotto, A.; Gauquelin, N.; Orekhov, A.; Verbeeck, J.; Seraglia, R.; Pagot, G.; Rizzi, G.A.; Balzano, V.; Gavioli, L.; Noto, V.D.; Barreca, D.; Maccato, C. | ||||
Title | Insights into the Photoelectrocatalytic Behavior of gCN-Based Anode Materials Supported on Ni Foams | Type | A1 Journal article | ||
Year | 2023 | Publication | Nanomaterials | Abbreviated Journal | Nanomaterials-Basel |
Volume | 13 | Issue | 6 | Pages | 1035 |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | Graphitic carbon nitride (gCN) is a promising n-type semiconductor widely investigated for photo-assisted water splitting, but less studied for the (photo)electrochemical degradation of aqueous organic pollutants. In these fields, attractive perspectives for advancements are offered by a proper engineering of the material properties, e.g., by depositing gCN onto conductive and porous scaffolds, tailoring its nanoscale morphology, and functionalizing it with suitable cocatalysts. The present study reports on a simple and easily controllable synthesis of gCN flakes on Ni foam substrates by electrophoretic deposition (EPD), and on their eventual decoration with Co-based cocatalysts [CoO, CoFe2O4, cobalt phosphate (CoPi)] via radio frequency (RF)-sputtering or electrodeposition. After examining the influence of processing conditions on the material characteristics, the developed systems are comparatively investigated as (photo)anodes for water splitting and photoelectrocatalysts for the degradation of a recalcitrant water pollutant [potassium hydrogen phthalate (KHP)]. The obtained results highlight that while gCN decoration with Co-based cocatalysts boosts water splitting performances, bare gCN as such is more efficient in KHP abatement, due to the occurrence of a different reaction mechanism. The related insights, provided by a multi-technique characterization, may provide valuable guidelines for the implementation of active nanomaterials in environmental remediation and sustainable solar-to-chemical energy conversion. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000960297000001 | Publication Date | 2023-03-13 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2079-4991 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 5.3 | Times cited | 3 | Open Access | OpenAccess |
Notes | The present work was financially supported by CNR (Progetti di Ricerca @CNR—avviso 2020—ASSIST), Padova University (P-DiSC#04BIRD2020-UNIPD EUREKA, DOR 2020–2022), AMGA Foundation (NYMPHEA project), INSTM Consortium (INSTM21PDGASPAROTTO—NANOMAT, INSTM21PDBARMAC—ATENA) and the European Union’s Horizon 2020 research and innovation program under grant agreement No. 823717—ESTEEM3. The FWO-Hercules fund G0H4316N ‘Direct electron detector for soft matter TEM’ is also acknowledged. Many thanks are also due to Dr. Riccardo Lorenzin for his support to experimental activities.; esteem3reported; esteem3TA | Approved | Most recent IF: 5.3; 2023 IF: 3.553 | ||
Call Number | EMAT @ emat @c:irua:196115 | Serial | 7378 | ||
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Author | Verdierre, G.; Gauquelin, N.; Jannis, D.; Birkhölzer, Y.A.; Mallik, S.; Verbeeck, J.; Bibes, M.; Koster, G. | ||||
Title | Epitaxial growth of the candidate ferroelectric Rashba material SrBiO3by pulsed laser deposition | Type | A1 Journal article | ||
Year | 2023 | Publication | APL materials | Abbreviated Journal | |
Volume | 11 | Issue | 3 | Pages | 031109 |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | Among oxides, bismuthates have been gaining much interest due to their unique features. In addition to their superconducting properties, they show potential for applications as topological insulators and as possible spin-to-charge converters. After being first investigated in their bulk form in the 1980s, bismuthates have been successfully grown as thin films. However, most efforts have focused on BaBiO<sub>3</sub>, with SrBiO<sub>3</sub>receiving only little attention. Here, we report the growth of epitaxial films of SrBiO<sub>3</sub>on both TiO<sub>2</sub>-terminated SrTiO<sub>3</sub>and NdO-terminated NdScO<sub>3</sub>substrates by pulsed laser deposition. SrBiO<sub>3</sub>has a pseudocubic lattice constant of ∼4.25 Å and grows relaxed on NdScO<sub>3</sub>. Counter-intuitively, it grows with a slight tensile strain on SrTiO<sub>3</sub>despite a large lattice mismatch, which should induce compressive strain. High-resolution transmission electron microscopy reveals that this occurs as a consequence of structural domain matching, with blocks of 10 SrBiO<sub>3</sub>unit planes matching blocks of 11 SrTiO<sub>3</sub>unit planes. This work provides a framework for the synthesis of high quality perovskite bismuthates films and for the understanding of their interface interactions with homostructural substrates. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000953363800004 | Publication Date | 2023-03-01 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2166-532X | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 6.1 | Times cited | Open Access | OpenAccess | |
Notes | This work received support from the ERC Advanced grant (Grant No. 833973) “FRESCO” and funding from the European Union’s Horizon 2020 Research and Innovation Program under Grant Agreement No. 823717—ESTEEM3, Van Gogh travel grant, Nuffic, The Netherlands (CF No. 42582SB).; esteem3reported; esteem3TA | Approved | Most recent IF: 6.1; 2023 IF: 4.335 | ||
Call Number | EMAT @ emat @c:irua:196135 | Serial | 7377 | ||
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Author | Benedet, M.; Andrea Rizzi, G.; Gasparotto, A.; Gauquelin, N.; Orekhov, A.; Verbeeck, J.; Maccato, C.; Barreca, D. | ||||
Title | Functionalization of graphitic carbon nitride systems by cobalt and cobalt-iron oxides boosts solar water oxidation performances | Type | A1 Journal article | ||
Year | 2023 | Publication | Applied surface science | Abbreviated Journal | |
Volume | 618 | Issue | Pages | 156652 | |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | The ever-increasing energy demand from the world population has made the intensive use of fossil fuels an overarching threat to global environment and human health. An appealing alternative is offered by sunlight-assisted photoelectrochemical water splitting to yield carbon-free hydrogen fuel, but kinetic limitations associated to the oxygen evolution reaction (OER) render the development of cost-effective, eco-friendly and stable electrocatalysts an imperative issue. In the present work, OER catalysts based on graphitic carbon nitride (g-C3N4) were deposited on conducting glass substrates by a simple decantation procedure, followed by functionalization with low amounts of nanostructured CoO and CoFe2O4 by radio frequency (RF)-sputtering, and final annealing under inert atmosphere. A combination of advanced characterization tools was used to investigate the interplay between material features and electrochemical performances. The obtained results highlighted the formation of a p-n junction for the g-C3N4-CoO system, whereas a Z-scheme junction accounted for the remarkable performance enhancement yielded by g-C3N4-CoFe2O4. The intimate contact between the system components also afforded an improved electrocatalyst stability in comparison to various bare and functionalized g-C3N4-based systems. These findings emphasize the importance of tailoring g-C3N4 chemico-physical properties through the dispersion of complementary catalysts to fully exploit its applicative potential. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000950654300001 | Publication Date | 2023-02-04 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0169-4332 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 6.7 | Times cited | 11 | Open Access | OpenAccess |
Notes | The authors gratefully acknowledge financial support from CNR (Progetti di Ricerca @CNR – avviso 2020 – ASSIST), Padova University (P-DiSC#04BIRD2020-UNIPD EUREKA, DOR 2020–2022), AMGA Foundation (NYMPHEA project), INSTM Consortium (INSTM21PDGASPAROTTO – NANOMAT, INSTM21PDBARMAC – ATENA) and the European Union's Horizon 2020 research and innovation program under grant agreement No 823717 – ESTEEM3. The FWO-Hercules fund G0H4316N 'Direct electron detector for soft matter TEM' is also acknowledged. Many thanks are due to Prof. Luca Gavioli (Università Cattolica del Sacro Cuore, Brescia, Italy) and Dr. Riccardo Lorenzin (Department of Chemical Sciences, Padova University, Italy) for their invaluable technical support.; esteem3reported; esteem3TA | Approved | Most recent IF: 6.7; 2023 IF: 3.387 | ||
Call Number | EMAT @ emat @c:irua:196150 | Serial | 7376 | ||
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Author | Vijayakumar, J.; Savchenko, T.M.; Bracher, D.M.; Lumbeeck, G.; Béché, A.; Verbeeck, J.; Vajda, Š.; Nolting, F.; Vaz, Ca.f.; Kleibert, A. | ||||
Title | Absence of a pressure gap and atomistic mechanism of the oxidation of pure Co nanoparticles | Type | A1 Journal article | ||
Year | 2023 | Publication | Nature communications | Abbreviated Journal | Nat Commun |
Volume | 14 | Issue | 1 | Pages | 174 |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | Understanding chemical reactivity and magnetism of 3<italic>d</italic>transition metal nanoparticles is of fundamental interest for applications in fields ranging from spintronics to catalysis. Here, we present an atomistic picture of the early stage of the oxidation mechanism and its impact on the magnetism of Co nanoparticles. Our experiments reveal a two-step process characterized by (i) the initial formation of small CoO crystallites across the nanoparticle surface, until their coalescence leads to structural completion of the oxide shell passivating the metallic core; (ii) progressive conversion of the CoO shell to Co<sub>3</sub>O<sub>4</sub>and void formation due to the nanoscale Kirkendall effect. The Co nanoparticles remain highly reactive toward oxygen during phase (i), demonstrating the absence of a pressure gap whereby a low reactivity at low pressures is postulated. Our results provide an important benchmark for the development of theoretical models for the chemical reactivity in catalysis and magnetism during metal oxidation at the nanoscale. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000955726400021 | Publication Date | 2023-01-12 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2041-1723 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 16.6 | Times cited | 1 | Open Access | OpenAccess |
Notes | Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung, 200021160186 2002153540 ; EC | Horizon 2020 Framework Programme, 810310 823717 ; University of Basel | Swiss Nanoscience Institute, P1502 ; This work is funded by Swiss National Foundation (SNF) (Grants. No 200021160186 and 2002153540) and the Swiss Nanoscience Institut (SNI) (Grant No. SNI P1502). S.V. acknowledges support from the European Union’s Horizon 2020 research and innovation programme under grant agreement no. 810310, which corresponds to the J. Heyrovsky Chair project (“ERA Chair at J. Heyrovský Institute of Physical Chemistry AS CR – The institutional approach towards ERA”). The funders had no role in the preparation of the article. Part of this work was performed at the Surface/Interface: Microscopy (SIM) beamline of the Swiss Light Source (SLS), Paul Scherrer Institut, Villigen, Switzerland. We kindly acknowledge Anja Weber and Elisabeth Müller from PSI for their help in fabricating the sample markers. A.B. and J. Verbeeck received funding from the European Union’s Horizon 2020 Research Infrastructure – Integrating Activities for Advanced Communities under grant agreement No. 823717 – ESTEEM3 reported | Approved | Most recent IF: 16.6; 2023 IF: 12.124 | ||
Call Number | EMAT @ emat @c:irua:196738 | Serial | 8804 | ||
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Author | Mary Joy, R.; Pobedinskas, P.; Bourgeois, E.; Chakraborty, T.; Görlitz, J.; Herrmann, D.; Noël, C.; Heupel, J.; Jannis, D.; Gauquelin, N.; D'Haen, J.; Verbeeck, J.; Popov, C.; Houssiau, L.; Becher, C.; Nesládek, M.; Haenen, K. | ||||
Title | Germanium vacancy centre formation in CVD nanocrystalline diamond using a solid dopant source | Type | A3 Journal article | ||
Year | 2023 | Publication | Science talks | Abbreviated Journal | Science Talks |
Volume | 5 | Issue | Pages | 100157 | |
Keywords | A3 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | |||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2023-02-09 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2772-5693 | ISBN | Additional Links | UA library record | |
Impact Factor | Times cited | Open Access | OpenAccess | ||
Notes | Approved | Most recent IF: NA | |||
Call Number | EMAT @ emat @c:irua:196969 | Serial | 8791 | ||
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Author | Gauquelin, N.; Forte, F.; Jannis, D.; Fittipaldi, R.; Autieri, C.; Cuono, G.; Granata, V.; Lettieri, M.; Noce, C.; Miletto-Granozio, F.; Vecchione, A.; Verbeeck, J.; Cuoco, M. | ||||
Title | Pattern Formation by Electric-Field Quench in a Mott Crystal | Type | A1 Journal article | ||
Year | 2023 | Publication | Nano letters | Abbreviated Journal | |
Volume | Issue | Pages | |||
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | The control of Mott phase is intertwined with the spatial reorganization of the electronic states. Out-of-equilibrium driving forces typically lead to electronic patterns that are absent at equilibrium, whose nature is however often elusive. Here, we unveil a nanoscale pattern formation in the Ca2 RuO4 Mott insulator. We demonstrate how an applied electric field spatially reconstructs the insulating phase that, uniquely after switching off the electric field, exhibits nanoscale stripe domains. The stripe pattern has regions with inequivalent octahedral distortions that we directly observe through high-resolution scanning transmission electron microscopy. The nanotexture depends on the orientation of the electric field, it is non-volatile and rewritable. We theoretically simulate the charge and orbital reconstruction induced by a quench dynamics of the applied electric field providing clear-cut mechanisms for the stripe phase formation. Our results open the path for the design of non-volatile electronics based on voltage-controlled nanometric phases. |
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Publisher | Place of Publication | Editor | |||
Language | Wos | 001012061600001 | Publication Date | 2023-05-18 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1530-6984 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 10.8 | Times cited | 2 | Open Access | OpenAccess |
Notes | This project has received funding from the European Union’s Horizon 2020 research and innova- tion programme under grant agreement No 823717 – ESTEEM3. The Merlin camera used in the experiment received funding from the FWO-Hercules fund G0H4316N ’Direct electron detector 15for soft matter TEM’. C. A. and G. C. are supported by the Foundation for Polish Science through the International Research Agendas program co-financed by the European Union within the Smart Growth Operational Programme. C. A. and G. C. acknowledge the access to the computing facil- ities of the Interdisciplinary Center of Modeling at the University of Warsaw, Grant No. GB84-0, GB84-1 and GB84-7 and GB84-7 and Poznan Supercomputing and Networking Center Grant No. 609.. C. A. and G. C. acknowledge the CINECA award under the ISCRA initiative IsC85 “TOP- MOST” Grant, for the availability of high-performance computing resources and support. We acknoweldge A. Guarino and C. Elia for providing support about the electrical characterization of the sample. M.C., R.F., and A.V. acknowledge support from the EU’s Horizon 2020213 research and innovation program under Grant Agreement No. 964398 (SUPERGATE). | Approved | Most recent IF: 10.8; 2023 IF: 12.712 | ||
Call Number | EMAT @ emat @c:irua:196970 | Serial | 8789 | ||
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Author | Kavak, S.; Kadu, A.A.; Claes, N.; Sánchez-Iglesias, A.; Liz-Marzán, L.M.; Batenburg, K.J.; Bals, S. | ||||
Title | Quantitative 3D Investigation of Nanoparticle Assemblies by Volumetric Segmentation of Electron Tomography Data Sets | Type | A1 Journal article | ||
Year | 2023 | Publication | The journal of physical chemistry: C : nanomaterials and interfaces | Abbreviated Journal | |
Volume | 127 | Issue | 20 | Pages | 9725-9734 |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | Morphological characterization of nanoparticle assemblies and hybrid nanomaterials is critical in determining their structure-property relationships as well as in the development of structures with desired properties. Electron tomography has become a widely utilized technique for the three-dimensional characterization of nanoparticle assemblies. However, the extraction of quantitative morphological parameters from the reconstructed volume can be a complex and labor-intensive task. In this study, we aim to overcome this challenge by automating the volumetric segmentation process applied to three-dimensional reconstructions of nanoparticle assemblies. The key to enabling automated characterization is to assess the performance of different volumetric segmentation methods in accurately extracting predefined quantitative descriptors for morphological characterization. In our methodology, we compare the quantitative descriptors obtained through manual segmentation with those obtained through automated segmentation methods, to evaluate their accuracy and effectiveness. To show generality, our study focuses on the characterization of assemblies of CdSe/CdS quantum dots, gold nanospheres and CdSe/CdS encapsulated in polymeric micelles, and silica-coated gold nanorods decorated with both CdSe/CdS or PbS quantum dots. We use two unsupervised segmentation algorithms: the watershed transform and the spherical Hough transform. Our results demonstrate that the choice of automated segmentation method is crucial for accurately extracting the predefined quantitative descriptors. Specifically, the spherical Hough transform exhibits superior performance in accurately extracting quantitative descriptors, such as particle size and interparticle distance, thereby allowing for an objective, efficient, and reliable volumetric segmentation of complex nanoparticle assemblies. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000991752700001 | Publication Date | 2023-05-25 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1932-7447 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 3.7 | Times cited | 2 | Open Access | OpenAccess |
Notes | Fonds Wetenschappelijk Onderzoek, 1181122N ; Horizon 2020 Framework Programme, 861950 ; H2020 European Research Council, 815128 ; | Approved | Most recent IF: 3.7; 2023 IF: 4.536 | ||
Call Number | EMAT @ emat @c:irua:196971 | Serial | 8793 | ||
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Author | Samal, D.; Gauquelin, N.; Takamura, Y.; Lobato, I.; Arenholz, E.; Van Aert, S.; Huijben, M.; Zhong, Z.; Verbeeck, J.; Van Tendeloo, G.; Koster, G. | ||||
Title | Unusual structural rearrangement and superconductivity in infinite layer cuprate superlattices | Type | A1 Journal article | ||
Year | 2023 | Publication | Physical review materials | Abbreviated Journal | |
Volume | 7 | Issue | 5 | Pages | 054803 |
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 | 001041792100007 | Publication Date | 2023-05-30 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2475-9953 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 3.4 | Times cited | Open Access | OpenAccess | |
Notes | Air Force Office of Scientific Research; European Office of Aerospace Research and Development, FA8655-10-1-3077 ; Office of Science, DE-AC02-05CH11231 ; National Science Foundation, DMR-1745450 ; Seventh Framework Programme, 278510 ; Bijzonder Onderzoeksfonds UGent; | Approved | Most recent IF: 3.4; 2023 IF: NA | ||
Call Number | EMAT @ emat @c:irua:196973 | Serial | 8790 | ||
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Author | Vlasov, E.; Skorikov, A.; Sánchez-Iglesias, A.; Liz-Marzán, L.M.; Verbeeck, J.; Bals, S. | ||||
Title | Secondary electron induced current in scanning transmission electron microscopy: an alternative way to visualize the morphology of nanoparticles | Type | A1 Journal article | ||
Year | 2023 | Publication | ACS materials letters | Abbreviated Journal | ACS Materials Lett. |
Volume | Issue | Pages | 1916-1921 | ||
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Electron tomography (ET) is a powerful tool to determine the three-dimensional (3D) structure of nanomaterials in a transmission electron microscope. However, the acquisition of a conventional tilt series for ET is a time-consuming process and can therefore not provide 3D structural information in a time-efficient manner. Here, we propose surface-sensitive secondary electron (SE) imaging as an alternative to ET for the investigation of the morphology of nanomaterials. We use the SE electron beam induced current (SEEBIC) technique that maps the electrical current arising from holes generated by the emission of SEs from the sample. SEEBIC imaging can provide valuable information on the sample morphology with high spatial resolution and significantly shorter throughput times compared with ET. In addition, we discuss the contrast formation mechanisms that aid in the interpretation of SEEBIC data. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 001006191600001 | Publication Date | 2023-06-12 | |
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 | 1 | Open Access | OpenAccess | |
Notes | The funding for this project was provided by European Research Council (ERC Consolidator Grant 815128, REALNANO). J.V. acknowledges the eBEAM project, which is supported by the European Union’s Horizon 2020 research and innovation program under grant agreement no. 101017720 (FET-Proactive EBEAM). L.M.L.-M. acknowledges funding from MCIN/AEI/10.13039/501100011033 (grant # PID2020-117779RB-I00). | Approved | Most recent IF: NA | ||
Call Number | EMAT @ emat @c:irua:197004 | Serial | 8795 | ||
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Author | Saniz, R.; Baldinozzi, G.; Arts, I.; Lamoen, D.; Leinders, G.; Verwerft, M. | ||||
Title | Charge order, frustration relief, and spin-orbit coupling in U3O8 | Type | A1 Journal article | ||
Year | 2023 | Publication | Physical review materials | Abbreviated Journal | |
Volume | 7 | Issue | 5 | Pages | 054410 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Research efforts on the description of the low-temperature magnetic order and electronic properties of U3O8 have been inconclusive so far. Reinterpreting neutron scattering results, we use group representation theory to show that the ground state presents collinear out-of-plane magnetic moments, with antiferromagnetic coupling both in-layer and between layers. Charge order relieves the initial geometric frustration, generating a slightly distorted honeycomb sublattice with Néel-type order. The precise knowledge of the characteristics of this magnetic ground state is then used to explain the fine features of the band gap. In this system, spin-orbit coupling (SOC) is of critical importance, as it strongly affects the electronic structure, narrowing the gap by ∼38%, compared to calculations neglecting SOC. The predicted electronic structure actually explains the salient features of recent optical absorption measurements, further demonstrating the excellent agreement between the calculated ground state properties and experiment. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 001041429800007 | Publication Date | 2023-05-31 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2475-9953 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 3.4 | Times cited | Open Access | OpenAccess | |
Notes | Financial support for this research was partly provided by the Energy Transition Fund of the Belgian FPS Economy (Project SF-CORMOD Spent Fuel CORrosion MODeling).Fonds Wetenschappelijk Onderzoek; Vlaams Supercomputer Centrum; Universiteit Antwerpen; Vlaamse regering; | Approved | Most recent IF: 3.4; 2023 IF: NA | ||
Call Number | EMAT @ emat @c:irua:197043 | Serial | 8796 | ||
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Author | Carrasco, S.; Orcajo, G.; Martínez, F.; Imaz, I.; Kavak, S.; Arenas-Esteban, D.; Maspoch, D.; Bals, S.; Calleja, G.; Horcajada, P. | ||||
Title | Hf/porphyrin-based metal-organic framework PCN-224 for CO2 cycloaddition with epoxides | Type | A1 Journal article | ||
Year | 2023 | Publication | Materials Today Advances | Abbreviated Journal | |
Volume | 19 | Issue | Pages | 100390 | |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Herein, we describe for the first time the synthesis of the highly porous Hf-tetracarboxylate porphyrin-based metal-organic framework (MOF) (Hf)PCN-224(M) (M = H2, Co2+). (Hf)PCN-224(H2) was easily and efficiently prepared following a simple microwave-assisted procedure with good yields (56–67%; space-time yields: 1100–1270 kg m−3·day−1), high crystallinity and phase purity by using trifluoromethanesulfonic acid and benzoic acid as modulators in less than 30 min. By simply introducing a preliminary step (10 min), 5,10,15,20-(tetra-4-carboxyphenyl)porphyrin linker (TCPP) was quantitatively metalated with Co2+ without additional purification and/or time consuming protection/deprotection steps to further obtain (Hf)PCN-224(Co). (Hf)PCN-224(Co) was then tested as catalyst in CO2 cycloaddition reaction with different epoxides to yield cyclic carbonates, showing the best catalytic performance described to date compared to other PCNs, under mild conditions (1 bar CO2, room temperature, 18–24 h). Twelve epoxides were tested, obtaining from moderate to excellent conversions (35–96%). Moreover, this reaction was gram scaled-up (x50) without significant loss of yield to cyclic carbonates. (Hf)PCN-224(Co) maintained its integrity and crystallinity even after 8 consecutive runs, and poisoning was efficiently reverted by a simple thermal treatment (175 °C, 6 h), fully recovering the initial catalytic activity. | ||||
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Language | Wos | 001025764000001 | Publication Date | 2023-06-19 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2590-0498 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 10 | Times cited | 1 | Open Access | OpenAccess |
Notes | S.C. acknowledges the European Union's Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie (MSCA-COFUND) grant agreement No 754382 (GOT Energy Talent). S.C. and P.H. acknowledge “Comunidad de Madrid” and European Regional Development Fund-FEDER 2014-2020-OE REACT-UE 1 for their financial support to VIRMOF-CM project associated to R&D projects in response to COVID-19. The authors acknowledge H2020-MSCA-ITN-2019 HeatNMof (ref. 860942), the M-ERA-NET C-MOF-cell (grant PCI2020-111998 funded by MCIN/AEI /10.13039/501100011033 and European Union NextGenerationEU/PRTR) project, and Retos Investigación MOFSEIDON (grant PID2019-104228RB-I00 funded by MCIN/AEI/10.13039/501100011033) project. This work has been also supported by the Regional Government of Madrid (Project ACES2030-CM, S2018/EMT-4319) and the Universidad Rey Juan Carlos IMPULSO Project (grant MATER M − 3000). S.K acknowledges the Flemish Fund for Scientific Research (FWO Vlaanderen) through a PhD research grant (1181122 N). | Approved | Most recent IF: 10; 2023 IF: NA | ||
Call Number | EMAT @ emat @c:irua:197198 | Serial | 8800 | ||
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Author | Muravev, V.; Parastaev, A.; van den Bosch, Y.; Ligt, B.; Claes, N.; Bals, S.; Kosinov, N.; Hensen, E.J.M. | ||||
Title | Size of cerium dioxide support nanocrystals dictates reactivity of highly dispersed palladium catalysts | Type | A1 Journal article | ||
Year | 2023 | Publication | Science | Abbreviated Journal | |
Volume | 380 | Issue | 6650 | Pages | 1174-1179 |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | The catalytic performance of heterogeneous catalysts can be tuned by modulation of the size and structure of supported transition metals, which are typically regarded as the active sites. In single-atom metal catalysts, the support itself can strongly affect the catalytic properties. Here, we demonstrate that the size of cerium dioxide (CeO2) support governs the reactivity of atomically dispersed palladium (Pd) in carbon monoxide (CO) oxidation. Catalysts with small CeO2 nanocrystals (~4 nanometers) exhibit unusually high activity in a CO-rich reaction feed, whereas catalysts with medium-size CeO2 (~8 nanometers) are preferred for lean conditions. Detailed spectroscopic investigations reveal support size–dependent redox properties of the Pd-CeO2 interface. | ||||
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Language | Wos | 001010846100008 | Publication Date | 2023-06-16 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0036-8075 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 56.9 | Times cited | 22 | Open Access | OpenAccess |
Notes | We thank the staff of the MAX IV Laboratory for time on beamline SPECIES under proposals 20200412 and 20190983; E. Kokkonen and A. Klyushin for assistance with NAP-XPS and RPES experiments conducted at SPECIES; staff of the MAX IV Laboratory for time on beamline BALDER under proposal 20200378; K. Klementiev for assistance with XAS measurements; J. Drnec at the ESRF for providing assistance in using beamline ID31; and V. Perez-Dieste and I. Villar Garcia at the CIRCE beamline at ALBA Synchrotron for help with acquiring preliminary RPES data obtained under proposal 2020024219. The synchrotron-based XRD measurements were performed on beamline ID31 at the European Synchrotron Radiation Facility (ESRF), Grenoble, France. Funding: This work was supported by the Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), a NWO Gravitation program funded by the Ministry of Education, Culture and Science of the Government of the Netherlands (V.M. and E.J.M.H.); the European Research Council (ERC consolidator grant 815128 REALNANO to S.B. and N.C.); and the European Union’s Horizon 2020 Research and Innovation Program (grant 823717–ESTEEM to S.B. and N.C). Research conducted at MAX IV, a Swedish national user facility, is supported by the Swedish Research council under contract 2018-07152, the Swedish Governmental Agency for Innovation Systems under contract 2018-04969, and Formas under contract 2019-02496 (VM). | Approved | Most recent IF: 56.9; 2023 IF: 37.205 | ||
Call Number | EMAT @ emat @c:irua:197199 | Serial | 8801 | ||
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Author | Lobato, I.; De Backer, A.; Van Aert, S. | ||||
Title | Real-time simulations of ADF STEM probe position-integrated scattering cross-sections for single element fcc crystals in zone axis orientation using a densely connected neural network | Type | A1 Journal article | ||
Year | 2023 | Publication | Ultramicroscopy | Abbreviated Journal | Ultramicroscopy |
Volume | 251 | Issue | Pages | 113769 | |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Quantification of annular dark field (ADF) scanning transmission electron microscopy (STEM) images in terms of composition or thickness often relies on probe-position integrated scattering cross sections (PPISCS). In order to compare experimental PPISCS with theoretically predicted ones, expensive simulations are needed for a given specimen, zone axis orientation, and a variety of microscope settings. The computation time of such simulations can be in the order of hours using a single GPU card. ADF STEM simulations can be efficiently parallelized using multiple GPUs, as the calculation of each pixel is independent of other pixels. However, most research groups do not have the necessary hardware, and, in the best-case scenario, the simulation time will only be reduced proportionally to the number of GPUs used. In this manuscript, we use a learning approach and present a densely connected neural network that is able to perform real-time ADF STEM PPISCS predictions as a function of atomic column thickness for most common face-centered cubic (fcc) crystals (i.e., Al, Cu, Pd, Ag, Pt, Au and Pb) along [100] and [111] zone axis orientations, root-mean-square displacements, and microscope parameters. The proposed architecture is parameter efficient and yields accurate predictions for the PPISCS values for a wide range of input parameters that are commonly used for aberration-corrected transmission electron microscopes. |
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Language | Wos | 001011617200001 | Publication Date | 2023-06-01 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0304-3991 | ISBN | Additional Links | UA library record; WoS full record | |
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). The authors acknowledge financial support from the Research Foundation Flanders (FWO, Belgium) through project fundings (G034621N and G0A7723N) and a postdoctoral grant to A. De Backer. S. Van Aert acknowledges funding from the University of Antwerp Research fund (BOF), Belgium. | Approved | Most recent IF: 2.2; 2023 IF: 2.843 | ||
Call Number | EMAT @ emat @c:irua:197275 | Serial | 8812 | ||
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Author | Sa, J.; Hu, N.; Heyvaert, W.; Van Gordon, K.; Li, H.; Wang, L.; Bals, S.; Liz-Marzán, L.M.; Ni, W. | ||||
Title | Spontaneous Chirality Evolved at the Au–Ag Interface in Plasmonic Nanorods | Type | A1 Journal article | ||
Year | 2023 | Publication | Chemistry of materials | Abbreviated Journal | Chem. Mater. |
Volume | Issue | Pages | |||
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Chiral ligands are considered a required ingredient during the synthesis of dissymmetric plasmonic metal nanocrystals. The mechanism behind the generation of chiral structures involves the formation of high Miller index chiral facets, induced by the adsorption of such chiral ligands. We found however that, chirality can also evolve spontaneously, without the involvement of any chiral ligands, during the co-deposition of Au and Ag on Au nanorods. When using a specific Au/Ag ratio, phase segregation of the two metals leads to an interface within the obtained AuAg shell, which can be exposed by removing the Ag component via oxidative etching. Although a close-to-racemic mixture of chiral Au nanorods with right and left handedness is found in solution, electron tomography analysis evidences left- and righthanded helicities, both at the Au-Ag interface and at the exposed surface of Au NRs after Ag etching. The helicity profile of the NRs indicates dominating inclination angles in a range from 30° to 60°. Single-particle optical characterization also reveals random handedness in the plasmonic response of individual nanorods. We hypothesize that, the origin of chirality is related with symmetry breaking during the co-deposition of Au and Ag, through an initial perturbation in a small region on the Au-Ag interface that eventually leads to chiral segregation throughout the nanocrystal. | ||||
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Language | Wos | 001052093300001 | Publication Date | 2023-08-21 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0897-4756 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 8.6 | Times cited | Open Access | OpenAccess | |
Notes | The authors acknowledge the financial support from the National Natural Science Foundation of China (grant 22074102). LMLM acknowledges funding from 26 MCIN/AEI/10.13039/501100011033 and “ESF Investing in your future” (Grant PID2020- 117779RB-I00). This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 823717 – ESTEEM3.; Ministerio de Ciencia e Innovaci?n, PID2020-117779RB-I00 ; H2020 Research Infrastructures, 823717 ; European Social Fund, PID2020-117779RB-I00 ; National Natural Science Foundation of China, 22074102 ; | Approved | Most recent IF: 8.6; 2023 IF: 9.466 | ||
Call Number | EMAT @ emat @c:irua:198151 | Serial | 8810 | ||
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Author | Arteaga Cardona, F.; Jain, N.; Popescu, R.; Busko, D.; Madirov, E.; Arús, B.A.; Gerthsen, D.; De Backer, A.; Bals, S.; Bruns, O.T.; Chmyrov, A.; Van Aert, S.; Richards, B.S.; Hudry, D. | ||||
Title | Preventing cation intermixing enables 50% quantum yield in sub-15 nm short-wave infrared-emitting rare-earth based core-shell nanocrystals | Type | A1 Journal article | ||
Year | 2023 | Publication | Nature communications | Abbreviated Journal | Nat Commun |
Volume | 14 | Issue | 1 | Pages | 4462 |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | Short-wave infrared (SWIR) fluorescence could become the new gold standard in optical imaging for biomedical applications due to important advantages such as lack of autofluorescence, weak photon absorption by blood and tissues, and reduced photon scattering coefficient. Therefore, contrary to the visible and NIR regions, tissues become translucent in the SWIR region. Nevertheless, the lack of bright and biocompatible probes is a key challenge that must be overcome to unlock the full potential of SWIR fluorescence. Although rare-earth-based core-shell nanocrystals appeared as promising SWIR probes, they suffer from limited photoluminescence quantum yield (PLQY). The lack of control over the atomic scale organization of such complex materials is one of the main barriers limiting their optical performance. Here, the growth of either homogeneous (α-NaYF<sub>4</sub>) or heterogeneous (CaF<sub>2</sub>) shell domains on optically-active α-NaYF<sub>4</sub>:Yb:Er (with and without Ce<sup>3+</sup>co-doping) core nanocrystals is reported. The atomic scale organization can be controlled by preventing cation intermixing only in heterogeneous core-shell nanocrystals with a dramatic impact on the PLQY. The latter reached 50% at 60 mW/cm<sup>2</sup>; one of the highest reported PLQY values for sub-15 nm nanocrystals. The most efficient nanocrystals were utilized for in vivo imaging above 1450 nm. | ||||
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Language | Wos | 001037058500022 | Publication Date | 2023-07-25 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2041-1723 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 16.6 | Times cited | 1 | Open Access | OpenAccess |
Notes | D.H. would like to thank Dominique Ectors (Bruker AXS GmbH, Karlsruhe, Germany) for assistance and discussion on the PXRD data and TOPAS evaluations. The authors would like to acknowledge the financial support provided by the Helmholtz Association via: i) the Professorial Recruitment Initiative Funding (B.S.R.); ii) the Research Field Energy – Program Materials and Technologies for the Energy Transition – Topic 1 Photovoltaics (F.A.C., D.B., E.M., B.S.R., D.H.). This project received funding from the European Union’s Horizon 2020 innovation programme under grant agreement 823717. This work was supported by the European Research Council (grant 770887-PICOMETRICS to S.V.A. and Grant 815128-REALNANO to S.B.). The authors acknowledge financial support from the ResearchFoundation Flanders (FWO, Belgium) through project fundings (G.0346.21 N to S.V.A. and S.B.) and a postdoctoral grant (A.D.B.). The authors (B.A.A., O.T.B. and A.C.) acknowledge funding from the Helmholtz Zentrum München, the DFG-Emmy Noether program (BR 5355/2-1) and from the CZI Deep Tissue Imaging (DTI-0000000248). The authors (O.T.B. and D.H.) would like to thank the Helmholtz Imaging (ZT-I-PF-4-038-BENIGN). | Approved | Most recent IF: 16.6; 2023 IF: 12.124 | ||
Call Number | EMAT @ emat @c:irua:198158 | Serial | 8808 | ||
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Author | Paulus, A.; Hendrickx, M.; Mayda, S.; Batuk, M.; Reekmans, G.; von Holst, M.; Elen, K.; Abakumov, A.M.; Adriaensens, P.; Lamoen, D.; Partoens, B.; Hadermann, J.; Van Bael, M.K.; Hardy, A. | ||||
Title | Understanding the Activation of Anionic Redox Chemistry in Ti4+-Substituted Li2MnO3as a Cathode Material for Li-Ion Batteries | Type | A1 Journal article | ||
Year | 2023 | Publication | ACS applied energy materials | Abbreviated Journal | ACS Appl. Energy Mater. |
Volume | 6 | Issue | 13 | Pages | 6956-6971 |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT) | ||||
Abstract | Layered Li-rich oxides, demonstrating both cationic and anionic redox chemistry being used as positive electrodes for Li-ion batteries,have raised interest due to their high specific discharge capacities exceeding 250 mAh/g. However, irreversible structural transformations triggered by anionic redox chemistry result in pronounced voltagefade (i.e., lowering the specific energy by a gradual decay of discharge potential) upon extended galvanostatic cycling. Activating or suppressing oxygen anionic redox through structural stabilization induced by redox-inactivecation substitution is a well-known strategy. However, less emphasishas been put on the correlation between substitution degree and theactivation/suppression of the anionic redox. In this work, Ti4+-substituted Li2MnO3 was synthesizedvia a facile solution-gel method. Ti4+ is selected as adopant as it contains no partially filled d-orbitals. Our study revealedthat the layered “honeycomb-ordered” C2/m structure is preserved when increasing the Ticontent to x = 0.2 in the Li2Mn1-x Ti (x) O-3 solidsolution, as shown by electron diffraction and aberration-correctedscanning transmission electron microscopy. Galvanostatic cycling hintsat a delayed oxygen release, due to an improved reversibility of theanionic redox, during the first 10 charge-discharge cyclesfor the x = 0.2 composition compared to the parentmaterial (x = 0), followed by pronounced oxygen redoxactivity afterward. The latter originates from a low activation energybarrier toward O-O dimer formation and Mn migration in Li2Mn0.8Ti0.2O3, as deducedfrom first-principles molecular dynamics (MD) simulations for the“charged” state. Upon lowering the Ti substitution to x = 0.05, the structural stability was drastically improvedbased on our MD analysis, stressing the importance of carefully optimizingthe substitution degree to achieve the best electrochemical performance. | ||||
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Language | Wos | 001018266700001 | Publication Date | 2023-07-10 | |
Series Editor | Series Title | Abbreviated Series Title | |||
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ISSN | 2574-0962 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 6.4 | Times cited | Open Access | Not_Open_Access: Available from 24.12.2023 | |
Notes | Universiteit Hasselt, AUHL/15/2 – GOH3816N ; Russian Science Foundation, 20-43-01012 ; Fonds Wetenschappelijk Onderzoek, AUHL/15/2 – GOH3816N G040116N ; The computational resources and services used in this work were provided by the VSC (Flemish Supercomputer Center) and the HPC infrastructure of the University of Antwerp (CalcUA), both funded by the FWO Vlaanderen and the Flemish Government-department EWI. | Approved | Most recent IF: 6.4; 2023 IF: NA | ||
Call Number | EMAT @ emat @c:irua:198160 | Serial | 8809 | ||
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Author | Denisov, N.; Jannis, D.; Orekhov, A.; Müller-Caspary, K.; Verbeeck, J. | ||||
Title | Characterization of a Timepix detector for use in SEM acceleration voltage range | Type | A1 Journal article | ||
Year | 2023 | Publication | Ultramicroscopy | Abbreviated Journal | Ultramicroscopy |
Volume | 253 | Issue | Pages | 113777 | |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Hybrid pixel direct electron detectors are gaining popularity in electron microscopy due to their excellent properties. Some commercial cameras based on this technology are relatively affordable which makes them attractive tools for experimentation especially in combination with an SEM setup. To support this, a detector characterization (Modulation Transfer Function, Detective Quantum Efficiency) of an Advacam Minipix and Advacam Advapix detector in the 15–30 keV range was made. In the current work we present images of Point Spread Function, plots of MTF/DQE curves and values of DQE(0) for these detectors. At low beam currents, the silicon detector layer behaviour should be dominant, which could make these findings transferable to any other available detector based on either Medipix2, Timepix or Timepix3 provided the same detector layer is used. | ||||
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Language | Wos | 001026912700001 | Publication Date | 2023-06-08 | |
Series Editor | Series Title | Abbreviated Series Title | |||
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ISSN | 0304-3991 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 2.2 | Times cited | Open Access | OpenAccess | |
Notes | The authors acknowledge the financial support of the Research Foundation Flanders (FWO, Belgium) project SBO S000121N. The authors are grateful to Dr. Lobato for productive discussion of methods. | Approved | Most recent IF: 2.2; 2023 IF: 2.843 | ||
Call Number | EMAT @ emat @c:irua:198258 | Serial | 8815 | ||
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