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Author |
Mulder, J.T.T.; Jenkinson, K.; Toso, S.; Prato, M.; Evers, W.H.H.; Bals, S.; Manna, L.; Houtepen, A.J.J. |
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Title |
Nucleation and growth of bipyramidal Yb:LiYF₄ nanocrystals : growing up in a hot environment |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Chemistry of materials |
Abbreviated Journal |
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Volume |
35 |
Issue |
14 |
Pages |
5311-5321 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Lanthanide-doped LiYF4 (Ln:YLF) is commonlyused fora broad variety of optical applications, such as lasing, photon upconversionand optical refrigeration. When synthesized as nanocrystals (NCs),this material is also of interest for biological applications andfundamental physical studies. Until now, it was unclear how Ln:YLFNCs grow from their ionic precursors into tetragonal NCs with a well-defined,bipyramidal shape and uniform dopant distribution. Here, we studythe nucleation and growth of ytterbium-doped LiYF4 (Yb:YLF),as a template for general Ln:YLF NC syntheses. We show that the formationof bipyramidal Yb:YLF NCs is a multistep process starting with theformation of amorphous Yb:YLF spheres. Over time, these spheres growvia Ostwald ripening and crystallize, resulting in bipyramidal Yb:YLFNCs. We further show that prolonged heating of the NCs results inthe degradation of the NCs, observed by the presence of large LiFcubes and small, irregular Yb:YLF NCs. Due to the similarity in chemicalnature of all lanthanide ions our work sheds light on the formationstages of Ln:YLF NCs in general. |
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Wos |
001021474500001 |
Publication Date |
2023-07-03 |
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Series Issue |
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Edition |
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ISSN |
0897-4756; 1520-5002 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
8.6 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
This project has received funding from the European Union's Horizon 2020 research and innovation program under Grant Agreement No. 766900 (Testing the large-scale limit of quantum mechanics). The authors thank Niranjan Saikumar for proof reading the manuscript. |
Approved |
Most recent IF: 8.6; 2023 IF: 9.466 |
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Call Number |
UA @ admin @ c:irua:197787 |
Serial |
8907 |
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Permanent link to this record |
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Author |
Ramesha, B.M.; Pawlak, B.; Arenas Esteban, D.; Reekmans, G.; Bals, S.; Marchal, W.; Carleer, R.; Adriaensens, P.; Meynen, V. |
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Title |
Partial hydrolysis of diphosphonate ester during the formation of hybrid Tio₂ nanoparticles : role of acid concentration |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
ChemPhysChem : a European journal of chemical physics and physical chemistry |
Abbreviated Journal |
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Volume |
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Issue |
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Pages |
e202300437-13 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA) |
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Abstract |
In the present work, a method was utilized to control the in‐situ partial hydrolysis of a diphosphonate ester in presence of a titania precursor and in function of acid content and its impact on the hybrid nanoparticles was assessed. The hydrolysis degree of organodiphosphonate ester linkers during the formation of hybrid organic‐inorganic metal oxide nanoparticles, are relatively underexplored . Quantitative solution NMR spectroscopy revealed that during the synthesis of TiO2 nanoparticles, an increase in acid concentration introduces a higher degree of partial hydrolysis of the TEPD linker into diverse acid/ester derivatives of TEPD. Increasing the HCl/Ti ratio from 1 to 3, resulted in an increase in degree of partial hydrolysis of the TEPD linker in solution from 4% to 18.8% under the here applied conditions. As a result of the difference in partial hydrolysis, the linker‐TiO2 bonding was altered. Upon subsequent drying of the colloidal TiO2 solution, different textures, at nanoscale and macroscopic scale, were obtained dependent on the HCl/Ti ratio and thus the degree of hydrolysis of TEPD. Understanding such linker‐TiO2 nanoparticle surface dynamics is crucial for making hybrid organic‐inorganic materials (i.e. (porous) metal phosphonates) employed in applications such as electronic/photonic devices, separation technology and heterogeneous catalysts. |
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Wos |
001071673900001 |
Publication Date |
2023-09-05 |
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Abbreviated Series Title |
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Series Issue |
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Edition |
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ISSN |
1439-4235; 1439-7641 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
2.9 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
This work was supported by the Research Foundation-Flanders (FWO Vlaanderen) Project G.0121.17 N. The work was further supported by Hasselt University and the Research Foundation – Flanders (FWO Vlaanderen) via the Hercules project AUHL/15/2 – GOH3816 N. V. M. acknowledges the Research Foundation Flanders (FWO) for project K801621 N. B. M. R. acknowledges, Prof. Dr. Christophe Detavernier and Dr. Davy Deduystche (COCOON, Ghent University) for PXRD and VT-XRD measurements, Prof. Dr. Christophe Van De Velde (iPRACS, University of Antwerp) and Dr. Radu Ciocarlan (LADCA, University of Antwerp) for helpful discussions on PXRD measurements and Dr. Nick Gys (University of Antwerp and VITO) for ICP-OES measurements. |
Approved |
Most recent IF: 2.9; 2023 IF: 3.075 |
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Call Number |
UA @ admin @ c:irua:198934 |
Serial |
8911 |
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Permanent link to this record |
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Author |
Teunissen, J.L.; Braeckevelt, T.; Skvortsova, I.; Guo, J.; Pradhan, B.; Debroye, E.; Roeffaers, M.B.J.; Hofkens, J.; Van Aert, S.; Bals, S.; Rogge, S.M.J.; Van Speybroeck, V. |
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Title |
Additivity of Atomic Strain Fields as a Tool to Strain-Engineering Phase-Stabilized CsPbI3Perovskites |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
The Journal of Physical Chemistry C |
Abbreviated Journal |
J. Phys. Chem. C |
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Volume |
127 |
Issue |
48 |
Pages |
23400-23411 |
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Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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Abstract |
CsPbI3 is a promising perovskite material for photovoltaic applications in its photoactive perovskite or black phase. However, the material degrades to a photovoltaically inactive or yellow phase at room temperature. Various mitigation strategies are currently being developed to increase the lifetime of the black phase, many of which rely on inducing strains in the material that hinder the black-to-yellow phase transition. Physical insight into how these strategies exactly induce strain as well as knowledge of the spatial extent over which these strains impact the material is crucial to optimize these approaches but is still lacking. Herein, we combine machine learning potential-based molecular dynamics simulations with our in silico strain engineering approach to accurately quantify strained large-scale atomic structures on a nanosecond time scale. To this end, we first model the strain fields introduced by atomic substitutions as they form the most elementary strain sources. We demonstrate that the magnitude of the induced strain fields decays exponentially with the distance from the strain source, following a decay rate that is largely independent of the specific substitution. Second, we show that the total strain field induced by multiple strain sources can be predicted to an excellent approximation by summing the strain fields of each individual source. Finally, through a case study, we illustrate how this additive character allows us to explain how complex strain fields, induced by spatially extended strain sources, can be predicted by adequately combining the strain fields caused by local strain sources. Hence, the strain additivity proposed here can be adopted to further our insight into the complex strain behavior in perovskites and to design strain from the atomic level onward to enhance their sought-after phase stability. |
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Wos |
001116862000001 |
Publication Date |
2023-12-07 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
3.7 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
This work was supported by iBOF-21-085 PERsist (Special Research Fund of Ghent University, KU Leuven Research Fund, and the Research Fund of the University of Antwerp). S.M.J.R., T.B., and B.P. acknowledge financial support from the Research Foundation-Flanders (FWO) through two postdoctoral fellow- ships [grant nos. 12T3522N (S.M.J.R.) and 1275521N (B.P.)] and an SB-FWO fellowship [grant no. 1SC1319 (T.B.)]. E.D., M.B.J.R., and J.H. acknowledge financial support from the Research Foundation-Flanders (FWO, grant nos. G.0B39.15, G.0B49.15, G098319N, S002019N, S004322N, and ZW15_09- GOH6316). J.H. acknowledges support from the Flemish government through long-term structural funding Methusalem (CASAS2, Meth/15/04) and the MPI as an MPI fellow. S.V.A. and S.B. acknowledge financial support from the Research Foundation-Flanders (FWO, grant no. G0A7723N). S.M.J.R. and V.V.S. acknowledge funding from the Research Board of Ghent University (BOF). The computational resources and services used in this work were provided by the VSC (Flemish Supercomputer Center), funded by the Research Foundation- Flanders (FWO) and the Flemish Government�department EWI.; KU Leuven, iBOF-21-085 PERsist ; Universiteit Antwerpen, iBOF-21-085 PERsist ; Universiteit Gent, iBOF-21-085 PERsist ; Vlaamse regering, CASAS2, Meth/15/04 ; Fonds Wetenschappelijk Onderzoek, G.0B39.15 G098319N G.0B49.15 1SC1319 12T3522N ZW15 09-GOH6316 G0A7723N 1275521N S004322N S002019N ; |
Approved |
Most recent IF: 3.7; 2023 IF: 4.536 |
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Call Number |
EMAT @ emat @c:irua:202124 |
Serial |
8985 |
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Permanent link to this record |
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Author |
Ghasemitarei, M.; Ghorbi, T.; Yusupov, M.; Zhang, Y.; Zhao, T.; Shali, P.; Bogaerts, A. |
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Title |
Effects of Nitro-Oxidative Stress on Biomolecules: Part 1—Non-Reactive Molecular Dynamics Simulations |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
Biomolecules |
Abbreviated Journal |
Biomolecules |
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Volume |
13 |
Issue |
9 |
Pages |
1371 |
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Keywords |
A1 Journal Article; plasma medicine; reactive oxygen and; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
Plasma medicine, or the biomedical application of cold atmospheric plasma (CAP), is an expanding field within plasma research. CAP has demonstrated remarkable versatility in diverse biological applications, including cancer treatment, wound healing, microorganism inactivation, and skin disease therapy. However, the precise mechanisms underlying the effects of CAP remain incompletely understood. The therapeutic effects of CAP are largely attributed to the generation of reactive oxygen and nitrogen species (RONS), which play a crucial role in the biological responses induced by CAP. Specifically, RONS produced during CAP treatment have the ability to chemically modify cell membranes and membrane proteins, causing nitro-oxidative stress, thereby leading to changes in membrane permeability and disruption of cellular processes. To gain atomic-level insights into these interactions, non-reactive molecular dynamics (MD) simulations have emerged as a valuable tool. These simulations facilitate the examination of larger-scale system dynamics, including protein-protein and protein-membrane interactions. In this comprehensive review, we focus on the applications of non-reactive MD simulations in studying the effects of CAP on cellular components and interactions at the atomic level, providing a detailed overview of the potential of CAP in medicine. We also review the results of other MD studies that are not related to plasma medicine but explore the effects of nitro-oxidative stress on cellular components and are therefore important for a broader understanding of the underlying processes. |
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Wos |
001071356400001 |
Publication Date |
2023-09-11 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2218-273X |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
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Times cited |
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Open Access |
Not_Open_Access |
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Notes |
This research received no external funding. |
Approved |
Most recent IF: NA |
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Call Number |
PLASMANT @ plasmant @c:irua:200380 |
Serial |
8958 |
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Permanent link to this record |
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Author |
Meng, S.; Wu, L.; Liu, M.; Cui, Z.; Chen, Q.; Li, S.; Yan, J.; Wang, L.; Wang, X.; Qian, J.; Guo, H.; Niu, J.; Bogaerts, A.; Yi, Y. |
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Title |
Plasma‐driven<scp>CO2</scp>hydrogenation to<scp>CH3OH</scp>over<scp>Fe2O3</scp>/<scp>γ‐Al2O3</scp>catalyst |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
AIChE Journal |
Abbreviated Journal |
AIChE Journal |
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Volume |
69 |
Issue |
10 |
Pages |
e18154 |
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Keywords |
A1 Journal Article; chemisorbed oxygen, CO2 hydrogenation, iron-based catalyst, methanol production, plasma catalysis; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
We report a plasma‐assisted CO<sub>2</sub>hydrogenation to CH<sub>3</sub>OH over Fe<sub>2</sub>O<sub>3</sub>/γ‐Al<sub>2</sub>O<sub>3</sub>catalysts, achieving 12% CO<sub>2</sub>conversion and 58% CH<sub>3</sub>OH selectivity at a temperature of nearly 80°C atm pressure. We investigated the effect of various supports and loadings of the Fe‐based catalysts, as well as optimized reaction conditions. We characterized catalysts by X‐ray powder diffraction (XRD), hydrogen temperature programmed reduction (H<sub>2</sub>‐TPR), CO<sub>2</sub>and CO temperature programmed desorption (CO<sub>2</sub>/CO‐TPD), high‐resolution transmission electron microscopy (HRTEM), scanning transmission electron microscopy (STEM), x‐ray photoelectron spectroscopy (XPS), Mössbauer, and Fourier transform infrared<bold>(</bold>FTIR). The XPS results show that the enhanced CO<sub>2</sub>conversion and CH<sub>3</sub>OH selectivity are attributed to the chemisorbed oxygen species on Fe<sub>2</sub>O<sub>3</sub>/γ‐Al<sub>2</sub>O<sub>3</sub>. Furthermore, the diffuse reflectance infrared Fourier transform spectroscopy (DRIFTs) and TPD results illustrate that the catalysts with stronger CO<sub>2</sub>adsorption capacity exhibit a higher reaction performance.<italic>In situ</italic>DRIFTS gain insight into the specific reaction pathways in the CO<sub>2</sub>/H<sub>2</sub>plasma. This study reveals the role of chemisorbed oxygen species as a key intermediate, and inspires to design highly efficient catalysts and expand the catalytic systems for CO<sub>2</sub>hydrogenation to CH<sub>3</sub>OH. |
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Wos |
001022420000001 |
Publication Date |
2023-07-07 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0001-1541 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.7 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
Fundamental Research Funds for the Central Universities, DUT18JC42 ; National Natural Science Foundation of China, 21908016 21978032 ; |
Approved |
Most recent IF: 3.7; 2023 IF: 2.836 |
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Call Number |
PLASMANT @ plasmant @c:irua:197829 |
Serial |
8959 |
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Permanent link to this record |
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Author |
Marchetti, A.; Gori, A.; Ferretti, A.M.; Esteban, D.A.; Bals, S.; Pigliacelli, C.; Metrangolo, P. |
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Title |
Templated Out‐of‐Equilibrium Self‐Assembly of Branched Au Nanoshells (Small 12/2023) |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
Small |
Abbreviated Journal |
Small |
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Volume |
19 |
Issue |
12 |
Pages |
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Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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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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Wos |
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Publication Date |
2023-03-23 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1613-6810 |
ISBN |
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Additional Links |
UA library record |
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Impact Factor |
13.3 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
P.M. is grateful to the European Research Council (ERC) for the Starting Grant ERC-2012- StG_20111012 FOLDHALO (Grant Agreement no. 307108) and the Proof-of-Concept Grant ERC-2017-PoC MINIRES (Grant Agreement no.789815). A. M. and P. M. are thankful to the project Hydrogex funded by Cariplo Foundation (grant no. 2018-1720). D.A.E. and S.B. acknowledges financial support from ERC Consolidator Grant Number 815128 REALNANO and Grant Agreement No. 731019 (EUSMI). |
Approved |
Most recent IF: 13.3; 2023 IF: 8.643 |
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Call Number |
EMAT @ emat @c:irua:200859 |
Serial |
8960 |
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Permanent link to this record |
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Author |
Van den Broek, W.; Jannis, D.; Verbeeck, J. |
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Title |
Convexity constraints on linear background models for electron energy-loss spectra |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
Ultramicroscopy |
Abbreviated Journal |
Ultramicroscopy |
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Volume |
254 |
Issue |
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Pages |
113830 |
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Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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Abstract |
In this paper convexity constraints are derived for a background model of electron energy loss spectra (EELS) that is linear in the fitting parameters. The model outperforms a power-law both on experimental and simulated backgrounds, especially for wide energy ranges, and thus improves elemental quantification results. Owing to the model’s linearity, the constraints can be imposed through fitting by quadratic programming. This has important advantages over conventional nonlinear power-law fitting such as high speed and a guaranteed unique solution without need for initial parameters. As such, the need for user input is significantly reduced, which is essential for unsupervised treatment of large datasets. This is demonstrated on a demanding spectrum image of a semiconductor device sample with a high number of elements over a wide energy range. |
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Wos |
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Publication Date |
2023-08-15 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0304-3991 |
ISBN |
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Additional Links |
UA library record |
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Impact Factor |
2.2 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
ECSEL, 875999 ; Horizon 2020; Horizon 2020 Framework Programme; Electronic Components and Systems for European Leadership; |
Approved |
Most recent IF: 2.2; 2023 IF: 2.843 |
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Call Number |
EMAT @ emat @c:irua:200588 |
Serial |
8961 |
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Permanent link to this record |
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Author |
Bercx, M.; Mayda, S.; Depla, D.; Partoens, B.; Lamoen, D. |
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Title |
Plasmonic effects in the neutralization of slow ions at a metallic surface |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
Contributions to Plasma Physics |
Abbreviated Journal |
Contrib. Plasma Phys |
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Pages |
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Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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Abstract |
Secondary electron emission is an important process that plays a significant role in several plasma‐related applications. As measuring the secondary electron yield experimentally is very challenging, quantitative modelling of this process to obtain reliable yield data is critical as input for higher‐scale simulations. Here, we build upon our previous work combining density functional theory calculations with a model originally developed by Hagstrum to extend its application to metallic surfaces. As plasmonic effects play a much more important role in the secondary electron emission mechanism for metals, we introduce an approach based on Poisson point processes to include both surface and bulk plasmon excitations to the process. The resulting model is able to reproduce the yield spectra of several available experimental results quite well but requires the introduction of global fitting parameters, which describe the strength of the plasmon interactions. Finally, we use an in‐house developed workflow to calculate the electron yield for a list of elemental surfaces spanning the periodic table to produce an extensive data set for the community and compare our results with more simplified approaches from the literature. |
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Wos |
001067651300001 |
Publication Date |
2023-09-16 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0863-1042 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
1.6 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
We acknowledge the financial support of FWO-Vlaanderen through project G.0216.14N. 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: 1.6; 2023 IF: 1.44 |
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Call Number |
EMAT @ emat @c:irua:200330 |
Serial |
8962 |
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Permanent link to this record |
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Author |
Van Gordon, K.; Baúlde, S.; Mychinko, M.; Heyvaert, W.; Obelleiro-Liz, M.; Criado, A.; Bals, S.; Liz-Marzán, L.M.; Mosquera, J. |
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Title |
Tuning the Growth of Chiral Gold Nanoparticles Through Rational Design of a Chiral Molecular Inducer |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
Nano Letters |
Abbreviated Journal |
Nano Lett. |
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Volume |
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Issue |
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Pages |
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Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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Abstract |
The bottom-up production of chiral gold nanomaterials holds great potential for the advancement of biosensing and nano-optics, among other applications. Reproducible preparations of colloidal nanomaterials with chiral morphology have been reported, using cosurfactants or chiral inducers such as thiolated amino acids. However, the underlying growth mechanisms for these nanomaterials remain insufficiently understood. We introduce herein a purposely devised chiral inducer, a cysteine modified with a hydrophobic chain, as a versatile chiral inducer. The amphiphilic and chiral features of this molecule provide control over the chiral morphology and the chiroptical signature of the obtained nanoparticles by simply varying the concentration of chiral inducer. These results are supported by circular dichroism and electromagnetic modeling as well as electron tomography to analyze structural evolution at the facet scale. Our observations suggest complex roles for the factors involved in chiral synthesis: the chemical nature of the chiral inducers and the influence of cosurfactants. |
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Place of Publication |
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Wos |
001092787000001 |
Publication Date |
2023-10-25 |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1530-6984 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
10.8 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
J.M. Taboada and F. Obelleiro are thanked for support with electromagnetic simulations. The authors acknowledge financial support by the European Research Council (ERC CoG No. 815128 REALNANO to S. Bals; ERC AdG No. 787510, 4DbioSERS to L.M.L.-M.) and from MCIN/AEI/10.13039/501100011033 and “ESF Investing in your future” (Grant PID2020-117779RB-I00 to L.M.L.-M., Grant RYC2020-030183-I to A.C., and Grants RYC2019-027842-I, PID2020-117885GA-I00 to J.M.). |
Approved |
Most recent IF: 10.8; 2023 IF: 12.712 |
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Call Number |
EMAT @ emat @c:irua:200590 |
Serial |
8963 |
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Permanent link to this record |
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Author |
Li, S.; Sun, J.; Gorbanev, Y.; van’t Veer, K.; Loenders, B.; Yi, Y.; Kenis, T.; Chen, Q.; Bogaerts, A. |
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Title |
Plasma-Assisted Dry Reforming of CH4: How Small Amounts of O2Addition Can Drastically Enhance the Oxygenate Production─Experiments and Insights from Plasma Chemical Kinetics Modeling |
Type |
A1 Journal Article |
|
Year |
2023 |
Publication |
ACS Sustainable Chemistry & Engineering |
Abbreviated Journal |
ACS Sustainable Chem. Eng. |
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Volume |
11 |
Issue |
42 |
Pages |
15373-15384 |
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Keywords |
A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
Plasma-based dry reforming of methane (DRM) into
high-value-added oxygenates is an appealing approach to enable
otherwise thermodynamically unfavorable chemical reactions at
ambient pressure and near room temperature. However, it suffers
from coke deposition due to the deep decomposition of CH4. In this
work, we assess the DRM performance upon O2 addition, as well as
varying temperature, CO2/CH4 ratio, discharge power, and gas
residence time, for optimizing oxygenate production. By adding O2,
the main products can be shifted from syngas (CO + H2) toward
oxygenates. Chemical kinetics modeling shows that the improved
oxygenate production is due to the increased concentration of
oxygen-containing radicals, e.g., O, OH, and HO2, formed by electron
impact dissociation [e + O2 → e + O + O/O(1D)] and subsequent
reactions with H atoms. Our study reveals the crucial role of oxygen-coupling in DRM aimed at oxygenates, providing practical
solutions to suppress carbon deposition and at the same time enhance the oxygenates production in plasma-assisted DRM. |
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Place of Publication |
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Wos |
001082603900001 |
Publication Date |
2023-10-23 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2168-0485 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
8.4 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
Fonds Wetenschappelijk Onderzoek, S001619N ; China Scholarship Council, 202006060029 ; National Natural Science Foundation of China, 21975018 ; H2020 European Research Council, 810182 ; |
Approved |
Most recent IF: 8.4; 2023 IF: 5.951 |
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Call Number |
PLASMANT @ plasmant @c:irua:201013 |
Serial |
8966 |
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Permanent link to this record |
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Author |
de la Croix, T.; Claes, N.; Eyley, S.; Thielemans, W.; Bals, S.; De Vos, D. |
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Title |
Heterogeneous Pt-catalyzed transfer dehydrogenation of long-chain alkanes with ethylene |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
Catalysis Science & Technology |
Abbreviated Journal |
Catal. Sci. Technol. |
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Volume |
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Issue |
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Pages |
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Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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Abstract |
The dehydrogenation of long-chain alkanes to olefins and alkylaromatics is a challenging endothermic reaction, typically requiring harsh conditions which can lead to low selectivity and coking. More favorable thermodynamics can be achieved by using a hydrogen acceptor, such as ethylene. In this work, the potential of heterogeneous platinum catalysts for the transfer dehydrogenation of long-chain alkanes is investigated, using ethylene as a convenient hydrogen acceptor. Pt/C and Pt–Sn/C catalysts were prepared<italic>via</italic>a simple polyol method and characterized with CO pulse chemisorption, HAADF-STEM, and EDX measurements. Conversion of ethylene was monitored<italic>via</italic>gas-phase FTIR, and distribution of liquid products was analyzed<italic>via</italic>GC-FID, GC-MS, and 1H-NMR. Compared to unpromoted Pt/C, Sn-promoted catalysts show lower initial reaction rates, but better resistance to catalyst deactivation, while increasing selectivity towards alkylaromatics. Both reaction products and ethylene were found to inhibit the reaction significantly. At 250 °C for 22 h, TON up to 28 and 86 mol per mol Pt were obtained for Pt/C and PtSn<sub>2</sub>/C, respectively, with olefin selectivities of 94% and 53%. The remaining products were mainly unbranched alkylaromatics. These findings show the potential of simple heterogeneous catalysts in alkane transfer dehydrogenation, for the preparation of valuable olefins and alkylaromatics, or as an essential step in various tandem reactions. |
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Place of Publication |
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Wos |
001104905100001 |
Publication Date |
2023-11-09 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2044-4753 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
5 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
T. de la Croix gratefully acknowledges the support of the Flanders Research Foundation (FWO) under project 11F6622N. D. De Vos is grateful to FWO for support of project G0D3721N, and to KU Leuven for the iBOF project 21/016/C3. S. Bals and N. Claes acknowledge funding from the European Research Council under the European Union’s Horizon 2020 research and innovation program (ERC Consolidator Grant No. 815128- REALNANO). W. Thielemans and S. Eyley thank KU Leuven (grant C14/18/061) and FWO (G0A1219N) for financial support. |
Approved |
Most recent IF: 5; 2023 IF: 5.773 |
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Call Number |
EMAT @ emat @c:irua:201010 |
Serial |
8968 |
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Permanent link to this record |
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Author |
Claes, J.; Partoens, B.; Lamoen, D. |
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Title |
Decoupled DFT-1/2 method for defect excitation energies |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
Physical Review B |
Abbreviated Journal |
Phys. Rev. B |
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Volume |
108 |
Issue |
12 |
Pages |
125306 |
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Keywords |
A1 Journal Article; Condensed Matter Theory (CMT) ; |
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Abstract |
The DFT-1/2 method is a band-gap correction with GW precision at a density functional theory (DFT) computational cost. The method was also extended to correct the gap between defect levels, allowing for the calculation of optical transitions. However, this method fails when the atomic character of the occupied and unoccupied defect levels is similar as we illustrate by two examples, the tetrahedral hydrogen interstitial and the negatively charged vacancy in diamond. We solve this problem by decoupling the effect of the occupied and unoccupied defect levels and call this the decoupled DFT-1/2 method for defects. |
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Place of Publication |
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Wos |
001089302800003 |
Publication Date |
2023-09-25 |
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Series Editor |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2469-9950 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
3.7 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
This work was supported by the FWO (Research Foundation-Flanders), Project No. G0D1721N. This work was performed in part using HPC resources from 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 (Economie, Wetenschap & Innovatie). |
Approved |
Most recent IF: 3.7; 2023 IF: 3.836 |
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Call Number |
CMT @ cmt @c:irua:201287 |
Serial |
8976 |
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Permanent link to this record |
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Author |
Bogaerts, A. |
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Title |
Special Issue on “Dielectric Barrier Discharges and their Applications” in Commemoration of the 20th Anniversary of Dr. Ulrich Kogelschatz’s Work |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
Plasma Chemistry and Plasma Processing |
Abbreviated Journal |
Plasma Chem Plasma Process |
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Volume |
43 |
Issue |
6 |
Pages |
1281-1285 |
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Keywords |
A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
n/a |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Wos |
001110371000001 |
Publication Date |
2023-11-30 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0272-4324 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
3.6 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
n/a |
Approved |
Most recent IF: 3.6; 2023 IF: 2.355 |
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Call Number |
PLASMANT @ plasmant @c:irua:201387 |
Serial |
8969 |
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Permanent link to this record |
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Author |
Lin, A.; Gromov, M.; Nikiforov, A.; Smits, E.; Bogaerts, A. |
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Title |
Characterization of Non-Thermal Dielectric Barrier Discharges for Plasma Medicine: From Plastic Well Plates to Skin Surfaces |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
Plasma Chemistry and Plasma Processing |
Abbreviated Journal |
Plasma Chem Plasma Process |
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Volume |
43 |
Issue |
6 |
Pages |
1587-1612 |
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Keywords |
A1 Journal Article; Non-thermal plasma · Plasma medicine · Dielectric barrier discharge · Plasma diagnostics · Plasma surface interaction · In situ plasma monitoring; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
technologies have been expanding, and one of the most exciting and rapidly growing
applications is in biology and medicine. Most biomedical studies with DBD plasma systems are performed in vitro, which include cells grown on the surface of plastic well plates, or in vivo, which include animal research models (e.g. mice, pigs). Since many DBD systems use the biological target as the secondary electrode for direct plasma generation and treatment, they are sensitive to the surface properties of the target, and thus can be altered based on the in vitro or in vivo system used. This could consequently affect biological response from plasma treatment. Therefore, in this study, we investigated the DBD plasma behavior both in vitro (i.e. 96-well flat bottom plates, 96-well U-bottom plates, and 24-well flat bottom plates), and in vivo (i.e. mouse skin). Intensified charge coupled device (ICCD) imaging was performed and the plasma discharges were visually distinguishable between the different systems. The geometry of the wells did not affect DBD plasma generation for low application distances (≤ 2 mm), but differentially affected plasma uniformity on the bottom of the well at greater distances. Since DBD plasma treatment in vitro is rarely performed in dry wells for plasma medicine experiments, the effect of well wetness was also investigated. In all in vitro cases, the uniformity of the DBD plasma was affected when comparing wet versus dry wells, with the plasma in the wide-bottom wells appearing the most similar to plasma generated on mouse skin. Interestingly, based on quantification of ICCD images, the DBD plasma intensity per surface area demonstrated an exponential one-phase decay with increasing application distance, regardless of the in vitro or in vivo system. This trend is similar to that of the energy per pulse of plasma, which is used to determine the total plasma treatment energy for biological systems. Optical emission spectroscopy performed on the plasma revealed similar trends in radical species generation between the plastic well plates and mouse skin. Therefore, taken together, DBD plasma intensity per surface area may be a valuable parameter to be used as a simple method for in situ monitoring during biological treatment and active plasma treatment control, which can be applied for in vitro and in vivo systems. |
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Place of Publication |
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Wos |
001072607700001 |
Publication Date |
2023-09-27 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0272-4324 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.6 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
This work was partially funded by the Research Foundation—Flanders (FWO) and supported by the following Grants: 12S9221N (A. L.), G044420N (A. L. and A. B.), and G033020N (A.B.). We would also like to thank several patrons, as part of this research was funded by donations from different donors, including Dedert Schilde vzw, Mr Willy Floren, and the Vereycken family. We would also like to acknowledge the support from the European Cooperation in Science & Technology (COST) Action on “Therapeutical applications of Cold Plasmas” (CA20114; PlasTHER). |
Approved |
Most recent IF: 3.6; 2023 IF: 2.355 |
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Call Number |
PLASMANT @ plasmant @c:irua:200285 |
Serial |
8970 |
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Permanent link to this record |
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Author |
Bhatia, H.; Keshavarz, M.; Martin, C.; Van Gaal, L.; Zhang, Y.; de Coen, B.; Schrenker, N.J.; Valli, D.; Ottesen, M.; Bremholm, M.; Van de Vondel, J.; Bals, S.; Hofkens, J.; Debroye, E. |
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Title |
Achieving High Moisture Tolerance in Pseudohalide Perovskite Nanocrystals for Light-Emitting Diode Application |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
ACS Applied Optical Materials |
Abbreviated Journal |
ACS Appl. Opt. Mater. |
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Volume |
1 |
Issue |
6 |
Pages |
1184-1191 |
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Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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Abstract |
The addition of potassium thiocyanate (KSCN) to the FAPbBr3 structure and subsequent post-treatment of nanocrystals (NCs) lead to high quantum confinement, resulting in a photoluminescent quantum yield (PLQY) approaching unity and microsecond decay times. This synergistic approach demonstrated exceptional stability under humid conditions, retaining 70% of the PLQY for over a month, while the untreated NCs degrade within 24 h. Additionally, the devices incorporating the post-treated NCs displayed 1.5% external quantum efficiency (EQE), a 5-fold improvement over untreated devices. These results provide promising opportunities for the use of perovskites in moisture-stable optoelectronics. |
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Place of Publication |
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Wos |
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Publication Date |
2023-06-23 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2771-9855 |
ISBN |
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Additional Links |
UA library record |
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Impact Factor |
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Times cited |
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Open Access |
OpenAccess |
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Notes |
Hercules Foundation, HER/11/14 ; European Commission; Ministerio de Ciencia e Innovaci?n, PID2021-128761OA-C22 ; European Regional Development Fund; Vlaamse regering, CASAS2 Meth/15/04 ; Fonds Wetenschappelijk Onderzoek, 1238622N 1514220N 1S45223N G.0B39.15 G.0B49.15 G098319N S002019N ZW15_09-GOH6316 ; Onderzoeksraad, KU Leuven, C14/19/079 db/21/006/bm iBOF-21-085 STG/21/010 ; Junta de Comunidades de Castilla-La Mancha, SBPLY/21/180501/000127 ; H2020 European Research Council, 642196 815128 ; |
Approved |
Most recent IF: NA |
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Call Number |
EMAT @ emat @c:irua:201011 |
Serial |
8975 |
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Permanent link to this record |
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Author |
Delfino, C.L.; Hao, Y.; Martin, C.; Minoia, A.; Gopi, E.; Mali, K.S.; Van der Auweraer, M.; Geerts, Y.H.; Van Aert, S.; Lazzaroni, R.; De Feyter, S. |
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Title |
Conformation-Dependent Monolayer and Bilayer Structures of an Alkylated TTF Derivative Revealed using STM and Molecular Modeling |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
The Journal of Physical Chemistry C |
Abbreviated Journal |
J. Phys. Chem. C |
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Volume |
127 |
Issue |
47 |
Pages |
23023-23033 |
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Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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Abstract |
In this study, the multi-layer self-assembled molecular network formation of an alkylated tetrathiafulvalene compound is studied at the liquid-solid interface between 1-phenyloctane and graphite. A combined theoretical/experimental approach associating force-field and quantum-chemical calculations with scanning tunnelling microscopy is used to determine the two-dimensional self-assembly beyond the monolayer, but also to further the understanding of the molecular adsorption conformation and its impact on the molecular packing within the assemblies at the monolayer and bilayer level. |
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Place of Publication |
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Wos |
001111637100001 |
Publication Date |
2023-11-30 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
3.7 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
Financial support from the Research Foundation-Flanders (FWO G081518N, G0A3220N) and KU Leuven–Internal Funds (C14/19/079) is acknowledged. This work was in part supported by FWO and F. R. S.-FNRS under the Excellence of Science EOS program (project 30489208 and 40007495). C.M. acknowledges the financial support: Grants PID2021-128761OA-C22 and CNS2022-136052 funded by MCIN/AEI/10.13039/501100011033 by the “European Union” and SBPLY/21/180501/000127 funded by JCCM and by the EU through “Fondo Europeo de Desarollo Regional” (FEDER). Research in Mons is also supported by the Belgian National Fund for Scientific Research (FRS-FNRS) within the Consortium des Équipements de Calcul Intensif – CÉCI, under Grant 2.5020.11, and by the Walloon Region (ZENOBE Tier-1 supercomputer, under grant 1117545). |
Approved |
Most recent IF: 3.7; 2023 IF: 4.536 |
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Call Number |
EMAT @ emat @c:irua:201671 |
Serial |
8974 |
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Permanent link to this record |
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Author |
Mayda, S.; Monico, L.; Krishnan, D.; De Meyer, S.; Cotte, M.; Garrevoet, J.; Falkenberg, G.; Sandu, I.C.A.; Partoens, B.; Lamoen, D.; Romani, A.; Miliani, C.; Verbeeck, J.; Janssens, K. |
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Title |
A combined experimental and computational approach to understanding CdS pigment oxidation in a renowned early 20th century painting |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Chemistry of materials |
Abbreviated Journal |
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Volume |
35 |
Issue |
24 |
Pages |
10403-10415 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT); Antwerp X-ray Imaging and Spectroscopy (AXIS) |
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Abstract |
Cadmium sulfide (CdS)-based yellow pigments have been used in a number of early 20th century artworks, including The Scream series painted by Edvard Munch. Some of these unique paintings are threatened by the discoloration of these CdS-based yellow oil paints because of the oxidation of the original sulfides to sulfates. The experimental data obtained here prove that moisture and cadmium chloride compounds play a key role in promoting such oxidation. To clarify how these two factors effectively prompt the process, we studied the band alignment between CdS, CdCl2, and Cd-(OH)Cl as well as the radicals center dot OH and H3O center dot by density functional theory (DFT) methods. Our results show that a stack of several layers of Cd-(OH)Cl creates a pocket of positive holes at the Cl-terminated surface and a pocket of electrons at the OH-terminated surface by leading in a difference in ionization energy at both surfaces. The resulting band alignment indicates that Cd-(OH)Cl can indeed play the role of an oxidative catalyst for CdS in a moist environment, thus providing an explanation for the experimental evidence. |
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Place of Publication |
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Wos |
001133000900001 |
Publication Date |
2023-12-08 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756; 1520-5002 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
8.6 |
Times cited |
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Open Access |
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Notes |
The experimental research on the cadmium yellow powders/paint mock-ups and The Scream (ca. 1910) was financially supported by the European Union, research projects IPERION-CH (H2020-INFRAIA-2014-2015, GA no. 654028) and IPERION-HS (H2020-INFRAIA-2019-1, GA no. 871034) and the project AMIS within the program Dipartimenti di Eccellenza 2018-2022 (funded by MUR and the University of Perugia). For the beamtime grants received, the authors thank the ESRF-ID21 beamline (experiments HG64 and HG95), the DESY-P06 beamline, a member of the Helmholtz Association HGF (experiments I-20130221 EC and I-20160126 EC), and the project CALIPSOplus under the GA no. 730872 from the E.U. Framework Programme for Research and Innovation Horizon 2020. All of the staff of the MUNCH Museum (Conservation Department) is acknowledged for their collaboration. 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: 8.6; 2023 IF: 9.466 |
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Call Number |
UA @ admin @ c:irua:202836 |
Serial |
8999 |
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Permanent link to this record |
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Author |
Duran, T.A.; Yayak, Y.O.; Aydin, H.; Peeters, F.M.; Yagmurcukardes, M. |
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|
Title |
A perspective on the state-of-the-art functionalized 2D materials |
Type |
A1 Journal article |
|
Year |
2023 |
Publication |
Journal of applied physics |
Abbreviated Journal |
|
|
|
Volume |
134 |
Issue |
12 |
Pages |
120901-120929 |
|
|
Keywords |
A1 Journal article; Condensed Matter Theory (CMT) |
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|
Abstract |
Two-dimensional (2D) ultra-thin materials are more crucial than their bulk counterparts for the covalent functionalization of their surface owing to atomic thinness, large surface-to-volume ratio, and high reactivity of surface atoms having unoccupied orbitals. Since the surface of a 2D material is composed of atoms having unoccupied orbitals, covalent functionalization enables one to improve or precisely modify the properties of the ultra-thin materials. Chemical functionalization of 2D materials not only modifies their intrinsic properties but also makes them adapted for nanotechnology applications. Such engineered materials have been used in many different applications with their improved properties. In the present Perspective, we begin with a brief history of functionalization followed by the introduction of functionalized 2D materials. Our Perspective is composed of the following sections: the applications areas of 2D graphene and graphene oxide crystals, transition metal dichalcogenides, and in-plane anisotropic black phosphorus, all of which have been widely used in different nanotechnology applications. Finally, our Perspectives on the future directions of applications of functionalized 2D materials are given. The present Perspective sheds light on the current progress in nanotechnological applications of engineered 2D materials through surface functionalization. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
001087770500008 |
Publication Date |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
|
|
|
ISSN |
0021-8979; 1089-7550 |
ISBN |
|
Additional Links |
UA library record; WoS full record |
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Impact Factor |
3.2 |
Times cited |
|
Open Access |
|
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|
Notes |
|
Approved |
Most recent IF: 3.2; 2023 IF: 2.068 |
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Call Number |
UA @ admin @ c:irua:201281 |
Serial |
9000 |
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Permanent link to this record |
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Author |
Jenkinson, K.; Spadaro, M.C.; Golovanova, V.; Andreu, T.; Morante, J.R.; Arbiol, J.; Bals, S. |
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Title |
Direct operando visualization of metal support interactions induced by hydrogen spillover during CO₂ hydrogenation |
Type |
A1 Journal article |
|
Year |
2023 |
Publication |
Advanced materials |
Abbreviated Journal |
|
|
|
Volume |
35 |
Issue |
51 |
Pages |
2306447-10 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
The understanding of catalyst active sites is a fundamental challenge for the future rational design of optimized and bespoke catalysts. For instance, the partial reduction of Ce4+ surface sites to Ce3+ and the formation of oxygen vacancies are critical for CO2 hydrogenation, CO oxidation, and the water gas shift reaction. Furthermore, metal nanoparticles, the reducible support, and metal support interactions are prone to evolve under reaction conditions; therefore a catalyst structure must be characterized under operando conditions to identify active states and deduce structure-activity relationships. In the present work, temperature-induced morphological and chemical changes in Ni nanoparticle-decorated mesoporous CeO2 by means of in situ quantitative multimode electron tomography and in situ heating electron energy loss spectroscopy, respectively, are investigated. Moreover, operando electron energy loss spectroscopy is employed using a windowed gas cell and reveals the role of Ni-induced hydrogen spillover on active Ce3+ site formation and enhancement of the overall catalytic performance. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
001106139400001 |
Publication Date |
2023-10-22 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0935-9648 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
29.4 |
Times cited |
|
Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 29.4; 2023 IF: 19.791 |
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Call Number |
UA @ admin @ c:irua:201143 |
Serial |
9022 |
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Permanent link to this record |
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Author |
Huang, S.; Griffin, E.; Cai, J.; Xin, B.; Tong, J.; Fu, Y.; Kravets, V.; Peeters, F.M.; Lozada-Hidalgo, M. |
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Title |
Gate-controlled suppression of light-driven proton transport through graphene electrodes |
Type |
A1 Journal article |
|
Year |
2023 |
Publication |
Nature communications |
Abbreviated Journal |
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|
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Volume |
14 |
Issue |
1 |
Pages |
6932-6937 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT) |
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Abstract |
Recent experiments demonstrated that proton transport through graphene electrodes can be accelerated by over an order of magnitude with low intensity illumination. Here we show that this photo-effect can be suppressed for a tuneable fraction of the infra-red spectrum by applying a voltage bias. Using photocurrent measurements and Raman spectroscopy, we show that such fraction can be selected by tuning the Fermi energy of electrons in graphene with a bias, a phenomenon controlled by Pauli blocking of photo-excited electrons. These findings demonstrate a dependence between graphene's electronic and proton transport properties and provide fundamental insights into molecularly thin electrode-electrolyte interfaces and their interaction with light. Recent experiments have shown that proton transport through graphene electrodes can be promoted by light, but the understanding of this phenomenon remains unclear. Here, the authors report the electrical tunability of this photo-effect, showing a connection between graphene electronic and proton transport properties. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
001094448600003 |
Publication Date |
2023-10-31 |
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Series Editor |
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Series Title |
|
Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
|
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ISSN |
2041-1723 |
ISBN |
|
Additional Links |
UA library record; WoS full record |
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Impact Factor |
16.6 |
Times cited |
|
Open Access |
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Notes |
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Approved |
Most recent IF: 16.6; 2023 IF: 12.124 |
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Call Number |
UA @ admin @ c:irua:201185 |
Serial |
9041 |
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Permanent link to this record |
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Author |
Hugenschmidt, M.; Jannis, D.; Kadu, A.A.; Grünewald, L.; De Marchi, S.; Perez-Juste, J.; Verbeeck, J.; Van Aert, S.; Bals, S. |
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Title |
Low-dose 4D-STEM tomography for beam-sensitive nanocomposites |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
ACS materials letters |
Abbreviated Journal |
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Volume |
6 |
Issue |
1 |
Pages |
165-173 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Electron tomography is essential for investigating the three-dimensional (3D) structure of nanomaterials. However, many of these materials, such as metal-organic frameworks (MOFs), are extremely sensitive to electron radiation, making it difficult to acquire a series of projection images for electron tomography without inducing electron-beam damage. Another significant challenge is the high contrast in high-angle annular dark field scanning transmission electron microscopy that can be expected for nanocomposites composed of a metal nanoparticle and an MOF. This strong contrast leads to so-called metal artifacts in the 3D reconstruction. To overcome these limitations, we here present low-dose electron tomography based on four-dimensional scanning transmission electron microscopy (4D-STEM) data sets, collected using an ultrafast and highly sensitive direct electron detector. As a proof of concept, we demonstrate the applicability of the method for an Au nanostar embedded in a ZIF-8 MOF, which is of great interest for applications in various fields, including drug delivery. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
001141178500001 |
Publication Date |
2023-12-11 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2639-4979 |
ISBN |
|
Additional Links |
UA library record; WoS full record |
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Impact Factor |
|
Times cited |
|
Open Access |
Not_Open_Access |
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Notes |
This work was supported by the European Research Council (Grant 815128 REALNANO to S.B., Grant 770887 PICOMETRICS to S.V.A.). J.P.-J. and S.M. acknowledge financial support from the MCIN/AEI/10.13039/501100011033 (Grants No. PID2019-108954RB-I00) and EU Horizon 2020 research and innovation program under grant agreement no. 883390 (SERSing). J.V., S.B., S.V.A., and L.G. acknowledge funding from the Flemish government (iBOF-21-085 PERsist). |
Approved |
Most recent IF: NA |
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Call Number |
UA @ admin @ c:irua:202771 |
Serial |
9053 |
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Permanent link to this record |
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Author |
Liu, J.; Xu, W.; Xiao, Y.M.; Ding, L.; Li, H.W.; Peeters, F.M. |
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Title |
Optical spectrum of n-type and p-type monolayer MoS₂ in the presence of proximity-induced interactions |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Journal of applied physics |
Abbreviated Journal |
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Volume |
134 |
Issue |
22 |
Pages |
224301-224307 |
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Keywords |
A1 Journal article; Condensed Matter Theory (CMT) |
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Abstract |
In this paper, we examined the effects of proximity-induced interactions such as Rashba spin-orbit coupling and effective Zeeman fields (EZFs) on the optical spectrum of n-type and p-type monolayer (ML)-MoS2. The optical conductivity is evaluated using the standard Kubo formula under random-phase approximation by including the effective electron-electron interaction. It has been found that there exist two absorption peaks in n-type ML-MoS2 and two knife shaped absorptions in p-type ML-MoS2, which are contributed by the inter-subband spin-flip electronic transitions within conduction and valence bands at valleys K and K ' with a lifted valley degeneracy. The optical absorptions in n-type and p-type ML-MoS 2 occur in THz and infrared radiation regimes and the position, height, and shape of them can be effectively tuned by Rashba parameter, EZF parameters, and carrier density. The interesting theoretical predictions in this study would be helpful for the experimental observation of the optical absorption in infrared to THz bandwidths contributed by inter-subband spin-flip electronic transitions in a lifted valley degeneracy monolayer transition metal dichalcogenides system. The obtained results indicate that ML-MoS2 with the platform of proximity interactions make it a promising infrared and THz material for optics and optoelectronics. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
001135684400003 |
Publication Date |
2023-12-11 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0021-8979; 1089-7550 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
3.2 |
Times cited |
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Open Access |
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Notes |
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Approved |
Most recent IF: 3.2; 2023 IF: 2.068 |
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Call Number |
UA @ admin @ c:irua:202777 |
Serial |
9069 |
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Permanent link to this record |
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Author |
Marchetti, A.; Gori, A.; Ferretti, A.M.; Esteban, D.A.; Bals, S.; Pigliacelli, C.; Metrangolo, P. |
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Title |
Templated Out‐of‐Equilibrium Self‐Assembly of Branched Au Nanoshells |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Small |
Abbreviated Journal |
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Volume |
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Issue |
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Pages |
2206712 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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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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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000914725800001 |
Publication Date |
2023-01-17 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1613-6810 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.3 |
Times cited |
1 |
Open Access |
OpenAccess |
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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 |
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Call Number |
EMAT @ emat @c:irua:194299 |
Serial |
7247 |
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Permanent link to this record |
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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. |
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Title |
Decoupling the Characteristics of Magnetic Nanoparticles for Ultrahigh Sensitivity |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Nano letters |
Abbreviated Journal |
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Volume |
23 |
Issue |
1 |
Pages |
58-65 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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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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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000907816300001 |
Publication Date |
2023-01-11 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1530-6984 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
10.8 |
Times cited |
1 |
Open Access |
OpenAccess |
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Notes |
Deutsche Forschungsgemeinschaft, DFG RTG 1952 ; Joachim Herz Stiftung; H2020 Research Infrastructures, 823717 ; |
Approved |
Most recent IF: 10.8; 2023 IF: 12.712 |
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Call Number |
EMAT @ emat @c:irua:193406 |
Serial |
7248 |
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Permanent link to this record |
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Author |
Vlasov, E.; Denisov, N.; Verbeeck, J. |
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Title |
Low-cost electron detector for scanning electron microscope |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
HardwareX |
Abbreviated Journal |
HardwareX |
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Volume |
14 |
Issue |
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Pages |
e00413 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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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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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
001042486000001 |
Publication Date |
2023-03-10 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2468-0672 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
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Times cited |
1 |
Open Access |
OpenAccess |
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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 |
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Call Number |
EMAT @ emat @c:irua:195886 |
Serial |
7252 |
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Permanent link to this record |
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Author |
Craig, T.M.; Kadu, A.A.; Batenburg, K.J.; Bals, S. |
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Title |
Real-time tilt undersampling optimization during electron tomography of beam sensitive samples using golden ratio scanning and RECAST3D |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Nanoscale |
Abbreviated Journal |
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Volume |
15 |
Issue |
11 |
Pages |
5391-5402 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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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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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000937908900001 |
Publication Date |
2023-02-13 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2040-3364 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
6.7 |
Times cited |
1 |
Open Access |
OpenAccess |
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Notes |
H2020 European Research Council, 815128 ; H2020 Marie Skłodowska-Curie Actions, 860942 ; |
Approved |
Most recent IF: 6.7; 2023 IF: 7.367 |
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Call Number |
EMAT @ emat @c:irua:195235 |
Serial |
7260 |
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Permanent link to this record |
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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. |
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Title |
Hybrid core–shell nanoparticles for cell-specific magnetic separation and photothermal heating |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Journal of materials chemistry B : materials for biology and medicine |
Abbreviated Journal |
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Volume |
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Issue |
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Pages |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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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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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000968908400001 |
Publication Date |
2023-04-05 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2050-750X |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7 |
Times cited |
1 |
Open Access |
OpenAccess |
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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 |
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Call Number |
EMAT @ emat @c:irua:195879 |
Serial |
7261 |
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Permanent link to this record |
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Author |
Miranda, L.P.; da Costa, D.R.; Peeters, F.M.; Costa Filho, R.N. |
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Title |
Vacancy clustering effect on the electronic and transport properties of bilayer graphene nanoribbons |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Nanotechnology |
Abbreviated Journal |
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Volume |
34 |
Issue |
5 |
Pages |
055706-55710 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT) |
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Abstract |
Experimental realizations of two-dimensional materials are hardly free of structural defects such as e.g. vacancies, which, in turn, modify drastically its pristine physical defect-free properties. In this work, we explore effects due to point defect clustering on the electronic and transport properties of bilayer graphene nanoribbons, for AA and AB stacking and zigzag and armchair boundaries, by means of the tight-binding approach and scattering matrix formalism. Evident vacancy concentration signatures exhibiting a maximum amplitude and an universality regardless of the system size, stacking and boundary types, in the density of states around the zero-energy level are observed. Our results are explained via the coalescence analysis of the strong sizeable vacancy clustering effect in the system and the breaking of the inversion symmetry at high vacancy densities, demonstrating a similar density of states for two equivalent degrees of concentration disorder, below and above the maximum value. |
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Wos |
000886630000001 |
Publication Date |
2022-11-02 |
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ISSN |
0957-4484 |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.5 |
Times cited |
1 |
Open Access |
OpenAccess |
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Approved |
Most recent IF: 3.5; 2023 IF: 3.44 |
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Call Number |
UA @ admin @ c:irua:192030 |
Serial |
7350 |
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Author |
Andelkovic, M.; Rakhimov, K.Y.; Chaves, A.; Berdiyorov, G.R.; Milošević, M.V. |
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Title |
Wave-packet propagation in a graphene geometric diode |
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A1 Journal article |
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Year |
2023 |
Publication |
Physica. E: Low-dimensional systems and nanostructures |
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Volume |
147 |
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Pages |
115607-4 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT) |
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Abstract |
Dynamics of electron wave-packets is studied using the continuum Dirac model in a graphene geometric diode where the propagation of the wave packet is favored in certain direction due to the presence of geometric constraints. Clear rectification is obtained in the THz frequency range with the maximum rectification level of 3.25, which is in good agreement with recent experiments on graphene ballistic diodes. The rectification levels are considerably higher for systems with narrower channels. In this case, the wave packet transmission probabilities and rectification rate also strongly depend on the energy of the incident wave packet, as a result of the quantum nature of energy levels along such channels. These findings can be useful for fundamental understanding of the charge carrier dynamics in graphene geometry diodes. |
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Wos |
000903737000003 |
Publication Date |
2022-12-10 |
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ISSN |
1386-9477 |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.3 |
Times cited |
1 |
Open Access |
OpenAccess |
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Approved |
Most recent IF: 3.3; 2023 IF: 2.221 |
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Call Number |
UA @ admin @ c:irua:193497 |
Serial |
7351 |
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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. |
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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 |
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Year |
2023 |
Publication |
Micron |
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169 |
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Pages |
103444 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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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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Wos |
000965998800001 |
Publication Date |
2023-03-21 |
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ISSN |
0968-4328 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
2.4 |
Times cited |
1 |
Open Access |
OpenAccess |
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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 |
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Call Number |
EMAT @ emat @c:irua:196069 |
Serial |
7379 |
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