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Author Pramanik, G.; Kvakova, K.; Thottappali, M.A.; Rais, D.; Pfleger, J.; Greben, M.; El-Zoka, A.; Bals, S.; Dracinsky, M.; Valenta, J.; Cigler, P.
Title Inverse heavy-atom effect in near infrared photoluminescent gold nanoclusters Type A1 Journal Article
Year 2021 Publication Nanoscale Abbreviated Journal (up) Nanoscale
Volume 13 Issue 23 Pages 10462-10467
Keywords A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;
Abstract Fluorophores functionalized with heavy elements show enhanced intersystem crossing due to increased spin–orbit coupling, which in turn shortens the fluorescence decay lifetime (<italic>τ</italic><sup>PL</sup>). This phenomenon is known as the heavy-atom effect (HAE). Here, we report the observation of increased<italic>τ</italic><sup>PL</sup>upon functionalisation of near-infrared photoluminescent gold nanoclusters with iodine. The heavy atom-mediated increase in<italic>τ</italic><sup>PL</sup>is in striking contrast with the HAE and referred to as inverse HAE. Femtosecond and nanosecond transient absorption spectroscopy revealed overcompensation of a slight decrease in lifetime of the transition associated with the Au core (ps) by a large increase in the long-lived triplet state lifetime associated with the Au shell, which contributed to the observed inverse HAE. This unique observation of inverse HAE in gold nanoclusters provides the means to enhance the triplet excited state lifetime.
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Publisher Place of Publication Editor
Language Wos Publication Date 2021-05-24
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2040-3364 ISBN Additional Links
Impact Factor 7.367 Times cited 7 Open Access OpenAccess
Notes The authors acknowledge support from GACR project Nr.18- 12533S. G. P. acknowledges support from EUSMI project No. E180200060; J.P. from the Ministry of Education, Youth and Sports of the Czech Republic – Program INTER-EXCELLENCE (LTAUSA19066). Approved Most recent IF: 7.367
Call Number EMAT @ emat @ Serial 6950
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Author Fatermans, J.; Romolini, G.; Altantzis, T.; Hofkens, J.; Roeffaers, M.B.J.; Bals, S.; Van Aert, S.
Title Atomic-scale detection of individual lead clusters confined in Linde Type A zeolites Type A1 Journal article
Year 2022 Publication Nanoscale Abbreviated Journal (up) Nanoscale
Volume Issue Pages
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Abstract Structural analysis of metal clusters confined in nanoporous materials is typically performed by X-ray-driven techniques. Although X-ray analysis has proved its strength in the characterization of metal clusters, it provides averaged structural information. Therefore, we here present an alternative workflow for bringing the characterization of confined metal clusters towards the local scale. This workflow is based on the combination of aberration-corrected transmission electron microscopy (TEM), TEM image simulations, and powder X-ray diffraction (XRD) with advanced statistical techniques. In this manner, we were able to characterize the clustering of Pb atoms in Linde Type A (LTA) zeolites with Pb loadings as low as 5 wt%. Moreover, individual Pb clusters could be directly detected. The proposed methodology thus enables a local-scale characterization of confined metal clusters in zeolites. This is important for further elucidation of the connection between the structure and the physicochemical properties of such systems.
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Publisher Place of Publication Editor
Language Wos 000809619900001 Publication Date 0000-00-00
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2040-3364 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.7 Times cited 2 Open Access OpenAccess
Notes The authors acknowledge the Research Foundation Flanders through project fundings (FWO, G026718N, G050218N, ZW15_09-G0H6316N, and W002221N) and through a PhD scholarship to G.R. (grant 11C6920N), as well as iBOF-21-085 PERSIST. T.A. and S.V.A. acknowledge funding from the University of Antwerp Research fund (BOF). J.H. acknowledges the Flemish government through long-term structural funding Methusalem (CASAS2, Meth/15/04) and the MPI as MPI fellow. M.R. acknowledges funding by the KU Leuven Research Fund (C14/19/079). S.B. and S.V.A. acknowledge funding from the European Research Council under the European Union’s Horizon 2020 research and innovation program (ERC Consolidator Grants No. 815128−REALNANO and No. 770887−PICOMETRICS). The authors thank Dr. D. Chernyshov for the collection of XRD measurements. Approved Most recent IF: 6.7
Call Number EMAT @ emat @c:irua:189061 Serial 7076
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Author Wang, Y.; Sztranyovszky, Z.; Zilli, A.; Albrecht, W.; Bals, S.; Borri, P.; Langbein, W.
Title Quantitatively linking morphology and optical response of individual silver nanohedra Type A1 Journal article
Year 2022 Publication Nanoscale Abbreviated Journal (up) Nanoscale
Volume 14 Issue 30 Pages 11028-11037
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract The optical response of metal nanoparticles is governed by plasmonic resonances, which are dictated by the particle morphology. A thorough understanding of the link between morphology and optical response requires quantitatively measuring optical and structural properties of the same particle. Here we present such a study, correlating electron tomography and optical micro-spectroscopy. The optical measurements determine the scattering and absorption cross-section spectra in absolute units, and electron tomography determines the 3D morphology. Numerical simulations of the spectra for the individual particle geometry, and the specific optical set-up used, allow for a quantitative comparison including the cross-section magnitude. Silver nanoparticles produced by photochemically driven colloidal synthesis, including decahedra, tetrahedra and bi-tetrahedra are investigated. A mismatch of measured and simulated spectra is found in some cases when assuming pure silver particles, which is explained by the presence of a few atomic layers of tarnish on the surface, not evident in electron tomography. The presented method tightens the link between particle morphology and optical response, supporting the predictive design of plasmonic nanomaterials.
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Publisher Place of Publication Editor
Language Wos 000828704000001 Publication Date 2022-07-15
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2040-3364; 2040-3372 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.7 Times cited 1 Open Access OpenAccess
Notes Z.S. acknowledges the UK Engineering and Physical Sciences Research Council (EPSRC) for his Ph.D. studentship award (grant EP/R513003/1). Y.W. acknowledges Iwan Moreels (University of Ghent) for training in nanoparticle synthesis. Y.W. acknowledges the Biotechnology and Biological Sciences Research Council (BBSRC) for his Ph.D. studentship award (grant BB/L015889/1). This work was supported by the UK EPSRC (grants EP/I005072/1 and EP/M028313/1), and by the European Commission (EUSMI E191000350). W.A. acknowledges an Individual Fellowship from the Marie Skodowska-Curie actions (MSCA) under the EU's Horizon 2020 program (Grant 797153, SOPMEN). We thank Lukas Payne and Iestyn Pope for contributions to the development of the hardware and software used for the optical measurements. Approved Most recent IF: 6.7
Call Number UA @ admin @ c:irua:189578 Serial 7092
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Author Parastaev, A.; Muravev, V.; Osta, E.H.; Kimpel, T.F.; Simons, J.F.M.; van Hoof, A.J.F.; Uslamin, E.; Zhang, L.; Struijs, J.J.C.; Burueva, D.B.; Pokochueva, E.V.; Kovtunov, K.V.; Koptyug, I.V.; Villar-Garcia, I.J.; Escudero, C.; Altantzis, T.; Liu, P.; Béché, A.; Bals, S.; Kosinov, N.; Hensen, E.J.M.
Title Breaking structure sensitivity in CO2 hydrogenation by tuning metal–oxide interfaces in supported cobalt nanoparticles Type A1 Journal article
Year 2022 Publication Nature Catalysis Abbreviated Journal (up) Nat Catal
Volume 5 Issue 11 Pages 1051-1060
Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Abstract A high dispersion of the active metal phase of transition metals on oxide supports is important when designing efficient heterogeneous catalysts. Besides nanoparticles, clusters and even single metal atoms can be attractive for a wide range of reactions. However, many industrially relevant catalytic transformations suffer from structure sensitivity, where reducing the size of the metal particles below a certain size substantially lowers catalytic performance. A case in point is the low activity of small cobalt nanoparticles in the hydrogenation of CO and CO2. Here we show how engineering of catalytic sites at the metal–oxide interface in cerium oxide–zirconium dioxide (ceria–zirconia)-supported cobalt can overcome this structure sensitivity. Few-atom cobalt clusters dispersed on 3 nm cobalt(II)-oxide particles stabilized by ceria–zirconia yielded a highly active CO2 methanation catalyst with a specific activity higher than that of larger particles under the same conditions.
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Publisher Place of Publication Editor
Language Wos 000884939300006 Publication Date 2022-11-17
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2520-1158 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 37.8 Times cited 32 Open Access OpenAccess
Notes This research was supported by the Applied and Engineering Sciences division of the Netherlands Organization for Scientific Research through the Alliander (now Qirion) Perspective program on Plasma Conversion of CO2. We acknowledge Diamond Light Source for time on beamline B18 under proposal SP20715-1. This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 823717 – ESTEEM3. S.B. acknowledges support from the European Research Council (ERC Consolidator Grant #815128 REALNANO) and T.A. acknowledges funding from the University of Antwerp Research fund (BOF). A.B. received funding from the European Union under grant agreement No 823717 – ESTEEM3. The authors acknowledge funding through the Hercules grant (FWO, University of Antwerp) I003218N “Infrastructure for imaging nanoscale processes in gas/vapour or liquid environments”. I.V.K., D.B.B., and E.V.P. acknowledge the Russian Ministry of Science and Higher Education (contract 075-15-2021-580) for financial support of parahydrogen-based studies. Experiments using synchrotron radiation XPS were performed at the CIRCE beamline at ALBA Synchrotron with the collaboration of ALBA staff. F. Oropeza Palacio and Rim C.J. van de Poll are acknowledged for the help with RPES measurements.; esteem3reported; esteem3jra Approved Most recent IF: 37.8
Call Number EMAT @ emat @c:irua:192068 Serial 7230
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Author Zhou, Y.; Che, F.; Liu, M.; Zou, C.; Liang, Z.; De Luna, P.; Yuan, H.; Li, J.; Wang, Z.; Xie, H.; Li, H.; Chen, P.; Bladt, E.; Quintero-Bermudez, R.; Sham, T.-K.; Bals, S.; Hofkens, J.; Sinton, D.; Chen, G.; Sargent, E.H.
Title Dopant-induced electron localization drives CO2 reduction to C2 hydrocarbons Type A1 Journal article
Year 2018 Publication Nature chemistry Abbreviated Journal (up) Nat Chem
Volume 10 Issue 10 Pages 974-980
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The electrochemical reduction of CO2 to multi-carbon products has attracted much attention because it provides an avenue to the synthesis of value-added carbon-based fuels and feedstocks using renewable electricity. Unfortunately, the efficiency of CO2 conversion to C-2 products remains below that necessary for its implementation at scale. Modifying the local electronic structure of copper with positive valence sites has been predicted to boost conversion to C-2 products. Here, we use boron to tune the ratio of Cu delta+ to Cu-0 active sites and improve both stability and C-2-product generation. Simulations show that the ability to tune the average oxidation state of copper enables control over CO adsorption and dimerization, and makes it possible to implement a preference for the electrosynthesis of C-2 products. We report experimentally a C-2 Faradaic efficiency of 79 +/- 2% on boron-doped copper catalysts and further show that boron doping leads to catalysts that are stable for in excess of similar to 40 hours while electrochemically reducing CO2 to multi-carbon hydrocarbons.
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Language Wos 000442395200013 Publication Date 2018-07-13
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1755-4330; 1755-4349 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 25.87 Times cited 700 Open Access OpenAccess
Notes ; This work was supported financially by funding from TOTAL S.A., the Ontario Research Fund: Research Excellence Program, the Natural Sciences and Engineering Research Council of Canada, the CIFAR Bio-Inspired Solar Energy programme, a University of Toronto Connaught grant, the Ministry of Science, Natural Science Foundation of China (21471040, 21271055 and 21501035), the Innovation-Driven Plan in Central South University project (2017CX003), a project from State Key Laboratory of Powder Metallurgy in Central South University, the Thousand Youth Talents Plan of China and Hundred Youth Talents Program of Hunan and the China Scholarship Council programme. This work benefited from the soft X-ray microcharacterization beamline at CLS, sector 20BM at the APS and the Ontario Centre for the Characterisation of Advanced Materials at the University of Toronto. H.Y. acknowledges financial support from the Research Foundation-Flanders (FWO postdoctoral fellowship). C.Z. acknowledges support from the International Academic Exchange Fund for Joint PhD Students from Tianjin University. P.D.L. acknowledges financial support from the Natural Sciences and Engineering Research Council in the form of the Canada Graduate Scholarship-Doctoral award. S.B. and E.B. acknowledge financial support from the European Research Council (ERC Starting Grant # 335078-COLOURATOMS). The authors thank B. Zhang, N. Wang, C. T. Dinh, T. Zhuang, J. Li and Y. Zhao for fruitful discussions, as well as Y. Hu and Q. Xiao from CLS, and Z. Finfrock and M. Ward from APS for their help during the course of study. Computations were performed on the SOSCIP Consortium's Blue Gene/Q computing platform. SOSCIP is funded by the Federal Economic Development Agency of Southern Ontario, the Province of Ontario, IBM Canada, Ontario Centres of Excellence, Mitacs and 15 Ontario academic member institutions. ; ecas_sara Approved Most recent IF: 25.87
Call Number UA @ lucian @ c:irua:153693UA @ admin @ c:irua:153693 Serial 5091
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Author Bals, S.; Van Aert, S.; Romero, C.P.; Lauwaet, K.; Van Bael, M.J.; Schoeters, B.; Partoens, B.; Yuecelen, E.; Lievens, P.; Van Tendeloo, G.
Title Atomic scale dynamics of ultrasmall germanium clusters Type A1 Journal article
Year 2012 Publication Nature communications Abbreviated Journal (up) Nat Commun
Volume 3 Issue 897 Pages 897
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT)
Abstract Starting from the gas phase, small clusters can be produced and deposited with huge flexibility with regard to composition, materials choice and cluster size. Despite many advances in experimental characterization, a detailed morphology of such clusters is still lacking. Here we present an atomic scale observation as well as the dynamical behaviour of ultrasmall germanium clusters. Using quantitative scanning transmission electron microscopy in combination with ab initio calculations, we are able to characterize the transition between different equilibrium geometries of a germanium cluster consisting of less than 25 atoms. Seven-membered rings, trigonal prisms and some smaller subunits are identified as possible building blocks that stabilize the structure.
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Language Wos 000306099900024 Publication Date 2012-06-12
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2041-1723; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 12.124 Times cited 90 Open Access
Notes Fwo; Iap; Iwt Approved Most recent IF: 12.124; 2012 IF: 10.015
Call Number UA @ lucian @ c:irua:100340 Serial 183
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Author Willhammar, T.; Sentosun, K.; Mourdikoudis, S.; Goris, B.; Kurttepeli, M.; Bercx, M.; Lamoen, D.; Partoens, B.; Pastoriza-Santos, I.; Pérez-Juste, J.; Liz-Marzán, L.M.; Bals, S.; Van Tendeloo, G.
Title Structure and vacancy distribution in copper telluride nanoparticles influence plasmonic activity in the near-infrared Type A1 Journal article
Year 2017 Publication Nature communications Abbreviated Journal (up) Nat Commun
Volume 8 Issue 8 Pages 14925
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT)
Abstract Copper chalcogenides find applications in different domains including photonics, photothermal therapy and photovoltaics. CuTe nanocrystals have been proposed as an alternative to noble metal particles for plasmonics. Although it is known that deviations from stoichiometry are a prerequisite for plasmonic activity in the near-infrared, an accurate description of the material and its (optical) properties is hindered by an insufficient understanding of the atomic structure and the influence of defects, especially for materials in their nanocrystalline form. We demonstrate that the structure of Cu1.5±xTe nanocrystals canbe determined using electron diffraction tomography. Real-space high-resolution electron tomography directly reveals the three-dimensional distribution of vacancies in the structure. Through first-principles density functional theory, we furthermore demonstrate that the influence of these vacancies on the optical properties of the nanocrystals is determined. Since our methodology is applicable to a variety of crystalline nanostructured materials, it is expected to provide unique insights concerning structure–property correlations.
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Publisher Place of Publication Editor
Language Wos 000397799700001 Publication Date 2017-03-30
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2041-1723 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 12.124 Times cited 37 Open Access OpenAccess
Notes The work was financially supported by the European Research Council through an ERC Starting Grant (#335078-COLOURATOMS). T.W. acknowledges the Swedish Research Council for an international postdoc grant. We acknowledge financial support of FWO-Vlaanderen through project G.0216.14N, G.0369.15N and a postdoctoral research grant to B.G. 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. The work was further supported by the Spanish MINECO (MAT2013-45168-R). S.M. thanks the Action ooSupporting Postdoctoral Researchers44 of the Operational Program ‘Education and Lifelong Learning’ (Action’s Beneficiary: General Secretariat for Research and Technology of Greece), which was co-financed by the European Social Fund (ESF) and the Greek State. (ROMEO:green; preprint:; postprint:can ; pdfversion:can); ECAS_Sara Approved Most recent IF: 12.124
Call Number EMAT @ emat @ c:irua:142203UA @ admin @ c:irua:142203 Serial 4538
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Author Dendooven, J.; Ramachandran, R.K.; Solano, E.; Kurttepeli, M.; Geerts, L.; Heremans, G.; Ronge, J.; Minjauw, M.M.; Dobbelaere, T.; Devloo-Casier, K.; Martens, J.A.; Vantomme, A.; Bals, S.; Portale, G.; Coati, A.; Detavernier, C.
Title Independent tuning of size and coverage of supported Pt nanoparticles using atomic layer deposition Type A1 Journal article
Year 2017 Publication Nature communications Abbreviated Journal (up) Nat Commun
Volume 8 Issue 8 Pages 1074
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Synthetic methods that allow for the controlled design of well-defined Pt nanoparticles are highly desirable for fundamental catalysis research. In this work, we propose a strategy that allows precise and independent control of the Pt particle size and coverage. Our approach exploits the versatility of the atomic layer deposition (ALD) technique by combining two ALD processes for Pt using different reactants. The particle areal density is controlled by tailoring the number of ALD cycles using trimethyl(methylcyclopentadienyl) platinum and oxygen, while subsequent growth using the same Pt precursor in combination with nitrogen plasma allows for tuning of the particle size at the atomic level. The excellent control over the particle morphology is clearly demonstrated by means of in situ and ex situ X-ray fluorescence and grazing incidence small angle X-ray scattering experiments, providing information about the Pt loading, average particle dimensions, and mean center-to-center particle distance.
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Publisher Place of Publication Editor
Language Wos 000413353500023 Publication Date 2017-10-16
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2041-1723 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 12.124 Times cited 88 Open Access OpenAccess
Notes ; This research was funded by the Research Foundation-Flanders (FWO), the Special Research Fund BOF of Ghent University (GOA 01G01513) and the Flemish Government (Medium-scale research infrastructure funding-Hercules funding). J. D., T. D. and M. M. M. acknowledge the FWO for a research fellowship. S. B. acknowledges the European Research Council, ERC grant no. 335078-Colouratom. For the GISAXS and XRF measurements at SOLEIL, the authors received funding from the European Community's Trans National Access Program CALIPSO. We are also grateful to the SOLEIL and ESRF staff for smoothly running the facilities. The authors thank G. Verellen for his help with drawing the 3D sketches. ; ecas_Sara Approved Most recent IF: 12.124
Call Number UA @ lucian @ c:irua:146668UA @ admin @ c:irua:146668 Serial 4786
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Author Quan, L.N.; Ma, D.; Zhao, Y.; Voznyy, O.; Yuan, H.; Bladt, E.; Pan, J.; de Arquer, F.P.G.; Sabatini, R.; Piontkowski, Z.; Emwas, A.-H.; Todorovic, P.; Quintero-Bermudez, R.; Walters, G.; Fan, J.Z.; Liu, M.; Tan, H.; Saidaminov, M., I; Gao, L.; Li, Y.; Anjum, D.H.; Wei, N.; Tang, J.; McCamant, D.W.; Roeffaers, M.B.J.; Bals, S.; Hofkens, J.; Bakr, O.M.; Lu, Z.-H.; Sargent, E.H.
Title Edge stabilization in reduced-dimensional perovskites Type A1 Journal article
Year 2020 Publication Nature Communications Abbreviated Journal (up) Nat Commun
Volume 11 Issue 1 Pages 170
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Reduced-dimensional perovskites are attractive light-emitting materials due to their efficient luminescence, color purity, tunable bandgap, and structural diversity. A major limitation in perovskite light-emitting diodes is their limited operational stability. Here we demonstrate that rapid photodegradation arises from edge-initiated photooxidation, wherein oxidative attack is powered by photogenerated and electrically-injected carriers that diffuse to the nanoplatelet edges and produce superoxide. We report an edge-stabilization strategy wherein phosphine oxides passivate unsaturated lead sites during perovskite crystallization. With this approach, we synthesize reduced-dimensional perovskites that exhibit 97 +/- 3% photoluminescence quantum yields and stabilities that exceed 300 h upon continuous illumination in an air ambient. We achieve green-emitting devices with a peak external quantum efficiency (EQE) of 14% at 1000 cd m(-2); their maximum luminance is 4.5 x 10(4) cd m(-2) (corresponding to an EQE of 5%); and, at 4000 cd m(-2), they achieve an operational half-lifetime of 3.5 h.
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Publisher Place of Publication Editor
Language Wos 000551458200001 Publication Date 2020-01-10
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2041-1723 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 16.6 Times cited 147 Open Access OpenAccess
Notes ; This publication is based in part on work supported by an award (KUS-11-009-21) from the King Abdullah University of Science and Technology (KAUST), by the Ontario Research Fund Research Excellence Program, by the Ontario Research Fund (ORF), by the Natural Sciences and Engineering Research Council (NSERC) of Canada, and by the US Department of Navy, Office of Naval Research (Grant Award No. N00014-17-12524). H.Y. acknowledges the Research Foundation-Flanders (FWO Vlaanderen) for a postdoctoral fellowship. E.B. gratefully acknowledges financial support by the Research Foundation-Flanders (FWO Vlaanderen). S.B. acknowledges financial support from European Research Council (ERC Starting Grant #815128-REALNANO). M.B.J.R. and J.H. acknowledge the Research Foundation-Flanders (FWO, Grants G.0962.13, G.0B39.15, AKUL/11/14 and G0H6316N), KU Leuven Research Fund (C14/15/053) and the European Research Council under the European Union's Seventh Framework Programme (FP/2007-2013)/ ERC Grant Agreement No. [307523], ERC-Stg LIGHT to M.B.J.R. DFT calculations were performed on the IBM BlueGene Q supercomputer with support from the Southern Ontario Smart Computing Innovation Platform (SOSCIP). M.I.S. acknowledges the Banting Postdoctoral Fellowship program from the Natural Sciences and Engineering Research Council of Canada (NSERC). H.T. acknowledges the Netherlands Organisation for Scientific Research (NWO) for a Rubicon grant (680-50-1511). ; sygma Approved Most recent IF: 16.6; 2020 IF: 12.124
Call Number UA @ admin @ c:irua:171327 Serial 6496
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Author Boschker, H.T.S.; Cook, P.L.M.; Polerecky, L.; Eachambadi, R.T.; Lozano, H.; Hidalgo-Martinez, S.; Khalenkow, D.; Spampinato, V.; Claes, N.; Kundu, P.; Wang, D.; Bals, S.; Sand, K.K.; Cavezza, F.; Hauffman, T.; Bjerg, J.T.; Skirtach, A.G.; Kochan, K.; McKee, M.; Wood, B.; Bedolla, D.; Gianoncelli, A.; Geerlings, N.M.J.; Van Gerven, N.; Remaut, H.; Geelhoed, J.S.; Millan-Solsona, R.; Fumagalli, L.; Nielsen, L.P.; Franquet, A.; Manca, J.V.; Gomila, G.; Meysman, F.J.R.
Title Efficient long-range conduction in cable bacteria through nickel protein wires Type A1 Journal article
Year 2021 Publication Nature Communications Abbreviated Journal (up) Nat Commun
Volume 12 Issue 1 Pages 3996
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Filamentous cable bacteria display long-range electron transport, generating electrical currents over centimeter distances through a highly ordered network of fibers embedded in their cell envelope. The conductivity of these periplasmic wires is exceptionally high for a biological material, but their chemical structure and underlying electron transport mechanism remain unresolved. Here, we combine high-resolution microscopy, spectroscopy, and chemical imaging on individual cable bacterium filaments to demonstrate that the periplasmic wires consist of a conductive protein core surrounded by an insulating protein shell layer. The core proteins contain a sulfur-ligated nickel cofactor, and conductivity decreases when nickel is oxidized or selectively removed. The involvement of nickel as the active metal in biological conduction is remarkable, and suggests a hitherto unknown form of electron transport that enables efficient conduction in centimeter-long protein structures.
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Language Wos 000669944900006 Publication Date 2021-06-28
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2041-1723 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 12.124 Times cited 23 Open Access OpenAccess
Notes The authors thank Marlies Neiemeisland for assistance with Raman microscopy, Michiel Kienhuis for assistance with NanoSIMS analysis, Peter Hildebrandt and Diego Millo for helping with the interpretation of the Raman spectra, IONTOF for the Orbitrap Hybrid- SIMS analysis, and Rene Fabregas for helping with finite-element numerical modeling for SDM. H.T.S.B. and F.J.R.M. were financially supported by the Netherlands Organization for Scientific Research (VICI grant 016.VICI.170.072). Research Foundation Flanders supported F.J.R.M., J.V.M., and R.T.E. through FWO grant G031416N, and F.J.R.M. and J.S.G. through FWO grant G038819N. N.M.J.G. is the recipient of a Ph.D. scholarship for teachers from NWO in the Netherlands (grant 023.005.049). The NanoSIMS facility at Utrecht University was financed through a large infrastructure grant by the Netherlands Organization for Scientific Research (NWO, grant no. 175.010.2009.011) and through a Research Infrastructure Fund by the Utrecht University Board. A.G.S. is supported by the Special Research Fund (BOF) of Ghent University (BOF14/IOP/003, BAS094-18, 01IO3618) and FWO (G043219). The ToF-SIMS was funded by FWO Hercules grant (ZW/13/07) to J.V.M. and A.F. H.L., R.M.S., and G.G. were funded by the European Union H2020 Framework Programme (MSCA-ITN-2016) under grant agreement n 721874.EU, the Spanish Agencia Estatal de Investigación and EU FEDER under grant agreements TEC2016-79156-P and TEC2015-72751-EXP, the Generalitat de Catalunya through 2017-SGR1079 grant and CERCA Program. G.G. was recipient of an ICREA Academia Award, and H.L. of a FPI fellowship (BES-2015-074799) from the Agencia Estatal de Investigación/Fondo Social Europeo. L.F. received funding from the European Research Council (grant agreement No. 819417) under the European Union’s Horizon 2020 research and innovation programme. Approved Most recent IF: 12.124
Call Number EMAT @ emat @c:irua:179813 Serial 6803
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Author Wang, D.; van der Wee, E.B.; Zanaga, D.; Altantzis, T.; Wu, Y.; Dasgupta, T.; Dijkstra, M.; Murray, C.B.; Bals, S.; van Blaaderen, A.
Title Quantitative 3D real-space analysis of Laves phase supraparticles Type A1 Journal article
Year 2021 Publication Nature Communications Abbreviated Journal (up) Nat Commun
Volume 12 Issue 1 Pages 3980
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Abstract 3D real-space analysis of thick nanoparticle crystals is non-trivial. Here, the authors demonstrate the structural analysis of a bulk-like Laves phase by imaging an off-stoichiometric binary mixture of hard-sphere-like nanoparticles in spherical confinement by electron tomography, enabling defect analysis on the single-particle level. Assembling binary mixtures of nanoparticles into crystals, gives rise to collective properties depending on the crystal structure and the individual properties of both species. However, quantitative 3D real-space analysis of binary colloidal crystals with a thickness of more than 10 layers of particles has rarely been performed. Here we demonstrate that an excess of one species in the binary nanoparticle mixture suppresses the formation of icosahedral order in the self-assembly in droplets, allowing the study of bulk-like binary crystal structures with a spherical morphology also called supraparticles. As example of the approach, we show single-particle level analysis of over 50 layers of Laves phase binary crystals of hard-sphere-like nanoparticles using electron tomography. We observe a crystalline lattice composed of a random mixture of the Laves phases. The number ratio of the binary species in the crystal lattice matches that of a perfect Laves crystal. Our methodology can be applied to study the structure of a broad range of binary crystals, giving insights into the structure formation mechanisms and structure-property relations of nanomaterials.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000687320200032 Publication Date 2021-06-25
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2041-1723 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 12.124 Times cited 10 Open Access OpenAccess
Notes M. Hermes is sincerely thanked for providing interactive views of the structures in this work. The authors thank I. Lobato, S. Dussi, L. Filion, E. Boattini, S. Paliwal, B. van der Meer and X. Xie for fruitful discussions. D.W., E.B.v.d.W. and A.v.B. acknowledge partial financial support from the European Research Council under the European Union’s Seventh Framework Program (FP-2007-2013)/ERC Advanced Grant Agreement 291667 HierarSACol. T.D. and M.D. acknowledge financial support from the Industrial Partnership Program, “Computational Sciences for Energy Research” (Grant no. 13CSER025), of the Netherlands Organization for Scientific Research (NWO), which was co-financed by Shell Global Solutions International B.V. S.B. acknowledges financial support from ERC Consolidator Grant No. 815128 REALNANO. T.A. acknowledges a post-doctoral grant from the Research Foundation Flanders (FWO, Belgium). C.B.M and Y.W. acknowledge support for materials synthesis from the Office of Naval Research Multidisciplinary University Research Initiative Award ONR N00014-18-1-2497. The authors acknowledge EM Square center at Utrecht University for the access to the microscopes.; sygmaSB Approved Most recent IF: 12.124
Call Number UA @ admin @ c:irua:181662 Serial 6845
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Author Toso, S.; Imran, M.; Mugnaioli, E.; Moliterni, A.; Caliandro, R.; Schrenker, N.J.; Pianetti, A.; Zito, J.; Zaccaria, F.; Wu, Y.; Gemmi, M.; Giannini, C.; Brovelli, S.; Infante, I.; Bals, S.; Manna, L.
Title Halide perovskites as disposable epitaxial templates for the phase-selective synthesis of lead sulfochloride nanocrystals Type A1 Journal article
Year 2022 Publication Nature communications Abbreviated Journal (up) Nat Commun
Volume 13 Issue 1 Pages 3976-10
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Colloidal chemistry grants access to a wealth of materials through simple and mild reactions. However, even few elements can combine in a variety of stoichiometries and structures, potentially resulting in impurities or even wrong products. Similar issues have been long addressed in organic chemistry by using reaction-directing groups, that are added to a substrate to promote a specific product and are later removed. Inspired by such approach, we demonstrate the use of CsPbCl3 perovskite nanocrystals to drive the phase-selective synthesis of two yet unexplored lead sulfochlorides: Pb3S2Cl2 and Pb4S3Cl2. When homogeneously nucleated in solution, lead sulfochlorides form Pb3S2Cl2 nanocrystals. Conversely, the presence of CsPbCl3 triggers the formation of Pb4S3Cl2/CsPbCl3 epitaxial heterostructures. The phase selectivity is guaranteed by the continuity of the cationic subnetwork across the interface, a condition not met in a hypothetical Pb3S2Cl2/CsPbCl3 heterostructure. The perovskite domain is then etched, delivering phase-pure Pb4S3Cl2 nanocrystals that could not be synthesized directly. Phase-selective approaches, such using reaction-directing groups, are often seen in traditional organic chemistry and catalysis. Here authors use perovskite nanocrystals as disposable templates to drive the phase-selective synthesis of two colloidal nanomaterials, the lead sulfohalides Pb3S2Cl2 and Pb4S3Cl2.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000825867200003 Publication Date 2022-07-08
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2041-1723 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 16.6 Times cited 15 Open Access OpenAccess
Notes The authors would like to acknowledge Dr. Joka Buha for the help with preliminary tests preceding this project, and Dr. B. M. Aresta and Dr. L. Cassano for their administrative support. The authors acknowledge financial support from the Research Foundation Flanders (FWO) through a postdoctoral fellowship to N.J.S. (FWO Grant No. 1238622N, N.J.S). S.B. acknowledges financial support from the European Commission by ERC Consolidator grant REALNANO (No. 815128, S.B.). L.M. acknowledges financial support from the Italian Ministry of University and Research (MIUR) through the Flag-Era JTC2019 project “Solution-Processed Perovskite/Graphene Nanocomposites for SelfPowered Gas Sensors” (PeroGaS, L.M.). The access to the National Synchrotron Light Source, Brookhaven National Laboratory, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC0298CH10886 (NSLS-II Proposal Number 307441). Approved Most recent IF: 16.6
Call Number UA @ admin @ c:irua:189684 Serial 7085
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Author Wang, D.; Hermes, M.; Najmr, S.; Tasios, N.; Grau-Carbonell, A.; Liu, Y.; Bals, S.; Dijkstra, M.; Murray, C.B.; van Blaaderen, A.
Title Structural diversity in three-dimensional self-assembly of nanoplatelets by spherical confinement Type A1 Journal article
Year 2022 Publication Nature communications Abbreviated Journal (up) Nat Commun
Volume 13 Issue 1 Pages 6001-6012
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Nanoplatelets offer many possibilities to construct advanced materials due to new properties associated with their (semi)two-dimensional shapes. However, precise control of both positional and orientational order of the nanoplatelets in three dimensions, which is required to achieve emerging and collective properties, is challenging to realize. Here, we combine experiments, advanced electron tomography and computer simulations to explore the structure of supraparticles self-assembled from nanoplatelets in slowly drying emulsion droplets. We demonstrate that the rich phase behaviour of nanoplatelets, and its sensitivity to subtle changes in shape and interaction potential can be used to guide the self-assembly into a wide range of different structures, offering precise control over both orientation and position order of the nanoplatelets. Our research is expected to shed light on the design of hierarchically structured metamaterials with distinct shape- and orientation- dependent properties. Nanoplatelets can be used as anisotropic building blocks for constructing novel optoelectronic materials. Here, Wang et al. show a route of assembling nanoplatelets with controllable positional and orientational order in three dimensions facilitated by the surface tension of drying emulsion droplets.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000867312100031 Publication Date 2022-10-12
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2041-1723 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 16.6 Times cited 7 Open Access OpenAccess
Notes We thank A. Kadu, M. Chiappini, F. Rabouw, S. Paliwal, X. Xie, C. Xia and Z. Wang for fruitful discussions. D.W. and A.v.B. acknowledge partial financial support from the European Research Council under the European Union's Seventh Framework Programme (FP-2007-2013)/ERC Advanced Grant Agreement 291667 HierarSACol. M.H. was supported by the Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC). D.W. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020 program (grant 894254 SuprAtom). Y.L. acknowledges the Sustainability project between the faculties of Science and Geosciences of Utrecht University. M.D. acknowledges financial support from European Research Council (Grant No. ERC-2019-ADV-H2020 884902 SoftML). S.B. acknowledges financial support from ERC Consolidator Grant No. 815128 REALNANO. C.B.M. acknowledges support for materials synthesis from the Office of Naval Research Multidisciplinary University Research Initiative Award ONR N00014-18-1-2497. The authors acknowledge the EM square center at Utrecht University for the access to the microscopes. Approved Most recent IF: 16.6
Call Number UA @ admin @ c:irua:191387 Serial 7214
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Author Chen, H.; Xiong, Y.; Li, J.; Abed, J.; Wang, D.; Pedrazo-Tardajos, A.; Cao, Y.; Zhang, Y.; Wang, Y.; Shakouri, M.; Xiao, Q.; Hu, Y.; Bals, S.; Sargent, E.H.H.; Su, C.-Y.; Yang, Z.
Title Epitaxially grown silicon-based single-atom catalyst for visible-light-driven syngas production Type A1 Journal article
Year 2023 Publication Nature communications Abbreviated Journal (up) Nat Commun
Volume 14 Issue 1 Pages 1719-11
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Despite the natural abundance and promising properties of Si, there are few examples of crystalline Si-based catalysts. Here, the authors report an epitaxial growth method to construct Co single atoms on Si for light driven CO2 reduction to syngas. Improving the dispersion of active sites simultaneous with the efficient harvest of photons is a key priority for photocatalysis. Crystalline silicon is abundant on Earth and has a suitable bandgap. However, silicon-based photocatalysts combined with metal elements has proved challenging due to silicon's rigid crystal structure and high formation energy. Here we report a solid-state chemistry that produces crystalline silicon with well-dispersed Co atoms. Isolated Co sites in silicon are obtained through the in-situ formation of CoSi2 intermediate nanodomains that function as seeds, leading to the production of Co-incorporating silicon nanocrystals at the CoSi2/Si epitaxial interface. As a result, cobalt-on-silicon single-atom catalysts achieve an external quantum efficiency of 10% for CO2-to-syngas conversion, with CO and H-2 yields of 4.7 mol g((Co))(-1) and 4.4 mol g((Co))(-1), respectively. Moreover, the H-2/CO ratio is tunable between 0.8 and 2. This photocatalyst also achieves a corresponding turnover number of 2 x 10(4) for visible-light-driven CO2 reduction over 6 h, which is over ten times higher than previously reported single-atom photocatalysts.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000962607600018 Publication Date 2023-03-28
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2041-1723 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 16.6 Times cited 6 Open Access OpenAccess
Notes This work was supported by the National Natural Science Foundation of China (21821003, 21890380, 21905316), Guangdong Natural Science Foundation (2019A1515011748), the Science and Technology Planning Project of Guangdong Province (2019A050510018), Pearl River Recruitment Program of Talent (2019QN01C108), the EU Infrastructure Project EUSMI (Grant No. E190700310), and Sun Yat-sen University. D.W. acknowledges an Individual Fellowship funded by the Marie-Sklodowska-Curie Actions (MSCA) in Horizon 2020 program (grant 894254 SuprAtom). S.B. and A.P.-T. acknowledge financial support from the European Commission under the Horizon 2020 Programme by grant no. 731019 (EUSMI) and ERC Consolidator grant no. 815128 (REALNANO). This project has received funding from the European Commission Grant (EUSMI E190700310). Synchrotron XAS data described in this paper was performed at the Canadian Light Source, a national research facility of the University of Saskatchewan, which is supported by the Canada Foundation for Innovation (CFI), the Natural Sciences and Engineering Research Council (NSERC), the National Research Council (NRC), the Canadian Institutes of Health Research (CIHR), the Government of Saskatchewan, and the University of Saskatchewan. Approved Most recent IF: 16.6; 2023 IF: 12.124
Call Number UA @ admin @ c:irua:196062 Serial 7932
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Author Arteaga Cardona, F.; Jain, N.; Popescu, R.; Busko, D.; Madirov, E.; Arús, B.A.; Gerthsen, D.; De Backer, A.; Bals, S.; Bruns, O.T.; Chmyrov, A.; Van Aert, S.; Richards, B.S.; Hudry, D.
Title Preventing cation intermixing enables 50% quantum yield in sub-15 nm short-wave infrared-emitting rare-earth based core-shell nanocrystals Type A1 Journal article
Year 2023 Publication Nature communications Abbreviated Journal (up) Nat Commun
Volume 14 Issue 1 Pages 4462
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Short-wave infrared (SWIR) fluorescence could become the new gold standard in optical imaging for biomedical applications due to important advantages such as lack of autofluorescence, weak photon absorption by blood and tissues, and reduced photon scattering coefficient. Therefore, contrary to the visible and NIR regions, tissues become translucent in the SWIR region. Nevertheless, the lack of bright and biocompatible probes is a key challenge that must be overcome to unlock the full potential of SWIR fluorescence. Although rare-earth-based core-shell nanocrystals appeared as promising SWIR probes, they suffer from limited photoluminescence quantum yield (PLQY). The lack of control over the atomic scale organization of such complex materials is one of the main barriers limiting their optical performance. Here, the growth of either homogeneous (α-NaYF<sub>4</sub>) or heterogeneous (CaF<sub>2</sub>) shell domains on optically-active α-NaYF<sub>4</sub>:Yb:Er (with and without Ce<sup>3+</sup>co-doping) core nanocrystals is reported. The atomic scale organization can be controlled by preventing cation intermixing only in heterogeneous core-shell nanocrystals with a dramatic impact on the PLQY. The latter reached 50% at 60 mW/cm<sup>2</sup>; one of the highest reported PLQY values for sub-15 nm nanocrystals. The most efficient nanocrystals were utilized for in vivo imaging above 1450 nm.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001037058500022 Publication Date 2023-07-25
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2041-1723 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 16.6 Times cited 1 Open Access OpenAccess
Notes D.H. would like to thank Dominique Ectors (Bruker AXS GmbH, Karlsruhe, Germany) for assistance and discussion on the PXRD data and TOPAS evaluations. The authors would like to acknowledge the financial support provided by the Helmholtz Association via: i) the Professorial Recruitment Initiative Funding (B.S.R.); ii) the Research Field Energy – Program Materials and Technologies for the Energy Transition – Topic 1 Photovoltaics (F.A.C., D.B., E.M., B.S.R., D.H.). This project received funding from the European Union’s Horizon 2020 innovation programme under grant agreement 823717. This work was supported by the European Research Council (grant 770887-PICOMETRICS to S.V.A. and Grant 815128-REALNANO to S.B.). The authors acknowledge financial support from the ResearchFoundation Flanders (FWO, Belgium) through project fundings (G.0346.21 N to S.V.A. and S.B.) and a postdoctoral grant (A.D.B.). The authors (B.A.A., O.T.B. and A.C.) acknowledge funding from the Helmholtz Zentrum München, the DFG-Emmy Noether program (BR 5355/2-1) and from the CZI Deep Tissue Imaging (DTI-0000000248). The authors (O.T.B. and D.H.) would like to thank the Helmholtz Imaging (ZT-I-PF-4-038-BENIGN). Approved Most recent IF: 16.6; 2023 IF: 12.124
Call Number EMAT @ emat @c:irua:198158 Serial 8808
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Author Zheng, Y.-R.; Vernieres, J.; Wang, Z.; Zhang, K.; Hochfilzer, D.; Krempl, K.; Liao, T.-W.; Presel, F.; Altantzis, T.; Fatermans, J.; Scott, S.B.; Secher, N.M.; Moon, C.; Liu, P.; Bals, S.; Van Aert, S.; Cao, A.; Anand, M.; Nørskov, J.K.; Kibsgaard, J.; Chorkendorff, I.
Title Monitoring oxygen production on mass-selected iridium–tantalum oxide electrocatalysts Type A1 Journal article
Year 2021 Publication Nature Energy Abbreviated Journal (up) Nat Energy
Volume Issue Pages
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Abstract Development of low-cost and high-performance oxygen evolution reaction catalysts is key to implementing polymer electrolyte membrane water electrolyzers for hydrogen production. Iridium-based oxides are the state-of-the-art acidic oxygen evolution reactio catalysts but still suffer from inadequate activity and stability, and iridium's scarcity motivates the discovery of catalysts with lower iridium loadings. Here we report a mass-selected iridium-tantalum oxide catalyst prepared by a magnetron-based cluster source with considerably reduced noble-metal loadings beyond a commercial IrO2 catalyst. A sensitive electrochemistry/mass-spectrometry instrument coupled with isotope labelling was employed to investigate the oxygen production rate under dynamic operating conditions to account for the occurrence of side reactions and quantify the number of surface active sites. Iridium-tantalum oxide nanoparticles smaller than 2 nm exhibit a mass activity of 1.2 ± 0.5 kA “g” _“Ir” ^“-1” and a turnover frequency of 2.3 ± 0.9 s-1 at 320 mV overpotential, which are two and four times higher than those of mass-selected IrO2, respectively. Density functional theory calculations reveal that special iridium coordinations and the lowered aqueous decomposition free energy might be responsible for the enhanced performance.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000728458000001 Publication Date 2021-12-09
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2058-7546 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor Times cited 95 Open Access OpenAccess
Notes Y.-R.Z. and Z.W acknowledge funding from the Toyota Research Institute. This project has received funding from VILLUM FONDEN (grant no. 9455) and the European Research Council under the European Union’s Horizon 2020 research and innovation programme (grants no. 741860-CLUNATRA, no. 815128−REALNANO and no. 770887−PICOMETRICS). S.B. and S.V.A. acknowledge funding from the Research Foundation Flanders (FWO, G026718N and G050218N). T.A. acknowledges the University of Antwerp Research Fund (BOF). STEM measurements were supported by the European Union's Horizon 2020 Research Infrastructure-Integrating Activities for Advanced Communities under grant agreement No 823717 – ESTEEM3.; sygmaSB Approved Most recent IF: NA
Call Number EMAT @ emat @c:irua:184794 Serial 6903
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Author Goris, B.; Bals, S.; van den Broek, W.; Carbó-Argibay, E.; Gómez-Graña, S.; Liz-Marzán, L.M.; Van Tendeloo, G.
Title Atomic-scale determination of surface facets in gold nanorods Type A1 Journal article
Year 2012 Publication Nature materials Abbreviated Journal (up) Nat Mater
Volume 11 Issue 11 Pages 930-935
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract It is widely accepted that the physical properties of nanostructures depend on the type of surface facets1, 2. For Au nanorods, the surface facets have a major influence on crucial effects such as reactivity and ligand adsorption and there has been controversy regarding facet indexing3, 4. Aberration-corrected electron microscopy is the ideal technique to study the atomic structure of nanomaterials5, 6. However, these images correspond to two-dimensional (2D) projections of 3D nano-objects, leading to an incomplete characterization. Recently, much progress was achieved in the field of atomic-resolution electron tomography, but it is still far from being a routinely used technique. Here we propose a methodology to measure the 3D atomic structure of free-standing nanoparticles, which we apply to characterize the surface facets of Au nanorods. This methodology is applicable to a broad range of nanocrystals, leading to unique insights concerning the connection between the structure and properties of nanostructures.
Address
Corporate Author Thesis
Publisher Place of Publication London Editor
Language Wos 000310434600015 Publication Date 2012-10-19
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1476-1122;1476-4660; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 39.737 Times cited 261 Open Access
Notes 262348 ESMI; Hercules 3; 24691 COUNTATOMS; 267867 PLASMAQUO Approved Most recent IF: 39.737; 2012 IF: 35.749
Call Number UA @ lucian @ c:irua:101778 Serial 182
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Author Verheyen, E.; Joos, L.; Van Havenbergh, K.; Breynaert, E.; Kasian, N.; Gobechiya, E.; Houthoofd, K.; Martineau, C.; Hinterstein, M.; Taulelle, F.; Van Speybroeck, V.; Waroquier, M.; Bals, S.; Van Tendeloo, G.; Kirschhock, C.E.A.; Martens, J.A.;
Title Design of zeolite by inverse sigma transformation Type A1 Journal article
Year 2012 Publication Nature materials Abbreviated Journal (up) Nat Mater
Volume 11 Issue 12 Pages 1059-1064
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Although the search for new zeolites has traditionally been based on trial and error, more rational methods are now available. The theoretical concept of inverse transformation of a zeolite framework to generate a new structure by removal of a layer of framework atoms and contraction has for the first time been achieved experimentally. The reactivity of framework germanium atoms in strong mineral acid was exploited to selectively remove germanium-containing four-ring units from an UTL type germanosilicate zeolite. Annealing of the leached framework through calcination led to the new all-silica COK-14 zeolite with intersecting 12- and 10-membered ring channel systems. An intermediate stage of this inverse transformation with dislodged germanate four-rings still residing in the pores could be demonstrated. Inverse transformation involving elimination of germanium-containing structural units opens perspectives for the synthesis of many more zeolites.
Address
Corporate Author Thesis
Publisher Place of Publication London Editor
Language Wos 000311432600025 Publication Date 2012-10-19
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1476-1122;1476-4660; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 39.737 Times cited 140 Open Access
Notes Fwo Approved Most recent IF: 39.737; 2012 IF: 35.749
Call Number UA @ lucian @ c:irua:101783 Serial 661
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Author Huijben, M.; Rijnders, G.; Blank, D.H.A.; Bals, S.; Van Aert, S.; Verbeeck, J.; Van Tendeloo, G.; Brinkman, A.; Hilgenkamp, H.
Title Electronically coupled complementary interfaces between perovskite band insulators Type A1 Journal article
Year 2006 Publication Nature materials Abbreviated Journal (up) Nat Mater
Volume 5 Issue Pages 556-560
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract
Address
Corporate Author Thesis
Publisher Place of Publication London Editor
Language Wos 000238708900021 Publication Date 2006-06-18
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1476-1122;1476-4660; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 39.737 Times cited 315 Open Access
Notes Fwo Approved Most recent IF: 39.737; 2006 IF: 19.194
Call Number UA @ lucian @ c:irua:59713UA @ admin @ c:irua:59713 Serial 1019
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Author Geuchies, J.J.; van Overbeek, C.; Evers, W.H.; Goris, B.; de Backer, A.; Gantapara, A.P.; Rabouw, F.T.; Hilhorst, J.; Peters, J.L.; Konovalov, O.; Petukhov, A.V.; Dijkstra, M.; Siebbeles, L.D.A.; van Aert, S.; Bals, S.; Vanmaekelbergh, D.
Title In situ study of the formation mechanism of two-dimensional superlattices from PbSe nanocrystals Type A1 Journal article
Year 2016 Publication Nature materials Abbreviated Journal (up) Nat Mater
Volume 15 Issue 15 Pages 1248-1254
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Oriented attachment of PbSe nanocubes can result in the formation of two-dimensional (2D) superstructures with long-range nanoscale and atomic order. This questions the applicability of classic models in which the superlattice grows by first forming a nucleus, followed by sequential irreversible attachment of nanocrystals, as one misaligned attachment would disrupt the 2D order beyond repair. Here, we demonstrate the formation mechanism of 2D PbSe superstructures with square geometry by using in situ grazing-incidence X-ray scattering (small angle and wide angle), ex situ electron microscopy, and Monte Carlo simulations. We observed nanocrystal adsorption at the liquid/gas interface, followed by the formation of a hexagonal nanocrystal monolayer. The hexagonal geometry transforms gradually through a pseudo-hexagonal phase into a phase with square order, driven by attractive interactions between the {100} planes perpendicular to the liquid substrate, which maximize facet-to-facet overlap. The nanocrystals then attach atomically via a necking process, resulting in 2D square superlattices.
Address Condensed Matter and Interfaces, Debye Institute for Nanomaterials Science, Utrecht University, 3584 CC Utrecht, The Netherlands
Corporate Author Thesis
Publisher Place of Publication Editor
Language English Wos 000389104400011 Publication Date 2016-09-05
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1476-1122 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 39.737 Times cited 182 Open Access OpenAccess
Notes This research is part of the programme ‘Designing Dirac Carriers in semiconductor honeycomb superlattices (DDC13),’ which is supported by the Foundation for Fundamental Research on Matter (FOM), which is part of the Dutch Research Council (NWO). J.J.G. acknowledges funding from the Debye and ESRF Graduate Programs. The authors gratefully acknowledge funding from the Research Foundation Flanders (G.036915 G.037413 and funding of postdoctoral grants to B.G. and A.d.B). S.B. acknowledges the European Research Council, ERC grant No 335078—Colouratom. The authors gratefully acknowledge I. Swart and M. van Huis for fruitful discussions. We acknowledge funding from NWO-CW TOPPUNT ‘Superficial Superstructures’. The X-ray scattering measurements were performed at the ID10 beamline at ESRF under proposal numbers SC-4125 and SC-3786. The authors thank G. L. Destri and F. Zontone for their support during the experiments.; ECAS_Sara; (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:cannot); Approved Most recent IF: 39.737
Call Number EMAT @ emat @ c:irua:136165 Serial 4289
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Author Wang, D.; Dasgupta, T.; van der Wee, E.B.; Zanaga, D.; Altantzis, T.; Wu, Y.; Coli, G.M.; Murray, C.B.; Bals, S.; Dijkstra, M.; van Blaaderen, A.
Title Binary icosahedral clusters of hard spheres in spherical confinement Type A1 Journal article
Year 2020 Publication Nature Physics Abbreviated Journal (up) Nat Phys
Volume Issue Pages 1-9
Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Abstract The influence of geometry on the local and global packing of particles is important to many fundamental and applied research themes, such as the structure and stability of liquids, crystals and glasses. Here we show by experiments and simulations that a binary mixture of hard-sphere-like nanoparticles crystallizing into a MgZn(2)Laves phase in bulk spontaneously forms icosahedral clusters in slowly drying droplets. Using advanced electron tomography, we are able to obtain the real-space coordinates of all the spheres in the icosahedral clusters of up to about 10,000 particles. The local structure of 70-80% of the particles became similar to that of the MgCu(2)Laves phase. These observations are important for photonic applications. In addition, we observed in simulations that the icosahedral clusters nucleated away from the spherical boundary, which is distinctly different from that of the single species clusters. Our findings open the way for particle-level studies of nucleation and growth of icosahedral clusters, and of binary crystallization. The authors investigate out-of-equilibrium crystallization of a binary mixture of sphere-like nanoparticles in small droplets. They observe the spontaneous formation of an icosahedral structure with stable MgCu(2)phases, which are promising for photonic applications.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000564497300002 Publication Date 2020-08-31
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1745-2473; 1745-2481 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 19.6 Times cited 38 Open Access OpenAccess
Notes ; D.W., E.B.v.d.W. and A.v.B. acknowledge partial financial support from the European Research Council under the European Union's Seventh Framework Programme (FP-2007-2013)/ERC Advanced Grant Agreement 291667 HierarSACol. T.D. and M. D. acknowledge financial support from the Industrial Partnership Programme, 'Computational Sciences for Energy Research' (grant number 13CSER025), of the Netherlands Organization for Scientific Research (NWO), which was co-financed by Shell Global Solutions International BV G.M.C. was also financially supported by NWO. S.B. acknowledges financial support from ERC Consolidator Grant Number 815128 REALNANO. T.A. acknowledges a post-doctoral grant from the Research Foundation Flanders (FWO, Belgium). C.B.M. and Y.W. acknowledge support for materials synthesis from the Office of Naval Research Multidisciplinary University Research Initiative Award ONR N00014-18-1-2497. G. A. Blab is gratefully acknowledged for 3D printing numerous truncated tetrahedra, which increased our understanding of the connection between the binary icosahedral cluster and Laves phase structures. N. Tasios is sincerely thanked for providing the code for the diffraction pattern calculation. M. Hermes is sincerely thanked for providing interactive views of the structures in this work. We thank G. van Tendeloo, M. Engel, J. Wang, S. Dussi, L. Filion, E. Boattini, S. Paliwal, N. Tasios, B. van der Meer, I. Lobato, J. Wu and L. Laurens for fruitful discussions. We acknowledge the EM Square centre at Utrecht University for the access to the microscopes. ; sygma Approved Most recent IF: 19.6; 2020 IF: 22.806
Call Number UA @ admin @ c:irua:172044 Serial 6460
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Author Yuan, R.; Claes, N.; Verheyen, E.; Tuel, A.; Bals, S.; Breynaert, E.; Martens, J.; Kirschhock, C.E.A.
Title Synthesis of IWW-type germanosilicate zeolite using 5-azonia-spiro[4, 4]nonane as structure directing agent Type A1 Journal article
Year 2016 Publication New journal of chemistry Abbreviated Journal (up) New J Chem
Volume 40 Issue 40 Pages 4319-4324
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract IWW-type zeolite with Si/Ge of 4.9 is obtained using 5-azonia-spiro[4,4]nonane as template in fluoride-free medium under hydrothermal conditions at 175 °C. In an otherwise identical synthesis, using the related 5-azonia-spiro[4,5]decane as structure directing agent, a mixture of IWW and NON zeolite types was formed. In absence of GeO2 from the reactant mixture, pure NON formed. The IWW zeolite was characterized by XRD, SEM, and HRTEM. IWW zeolite displayed a unique morphology and could be calcined at 600 °C without loss of crystallinity. The Si/Ge ratio of the IWW zeolite was increased by postsynthesis modification. Part of the germanium could be eliminated from the as-synthesized IWW zeolite by acid leaching using 6 M HCl solution. Also the calcined material could be degermanated. Here the presence of a silicon source in the acidic leaching solution minimized structural damage. This way the Si/Ge ratio of the IWW zeolite was increased from 4.9 up to 10.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000375586400038 Publication Date 2016-02-19
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1144-0546 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.269 Times cited 8 Open Access OpenAccess
Notes The authors acknowledge FWO/NWO and ESRF for providing beam time at the DUBBLE and SNBL beamlines (ESRF, Grenoble) and P. Abdala for her assistance during the use of the beamline. The authors are grateful to L. Van Tendeloo for taking SEM images. I. Cuppens and K. Houthoofd are thanked for the ICP and AAS measurements. R.Y. acknowledges Chinese Scholarship Council for a CSC doctoral fellowship. JAM and CEAK acknowledge the Flemish government for long-term structural funding (Methusalem). N.C. and S.B. acknowledge financial support from European Research Council (ERC Starting Grant #335078-COLOURATOMS).; ECAS_Sara; (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:cannot); Approved Most recent IF: 3.269
Call Number c:irua:133671 Serial 4027
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Author Mayer, J.A.; Offermans, T.; Chrapa, M.; Pfannmöller, M.; Bals, S.; Ferrini, R.; Nisato, G.
Title Optical enhancement of a printed organic tandem solar cell using diffractive nanostructures Type A1 Journal article
Year 2018 Publication Optics express Abbreviated Journal (up) Opt Express
Volume 26 Issue 26 Pages A240
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Solution processable organic tandem solar cells offer a promising approach to achieve cost-effective, lightweight and flexible photovoltaics. In order to further enhance the efficiency of optimized organic tandem cells, diffractive light-management nanostructures were designed for an optimal redistribution of the light as function of both wavelength and propagation angles in both sub-cells. As the fabrication of these optical structures is compatible with roll-to-roll production techniques such as hot-embossing or UV NIL imprinting, they present an optimal cost-effective solution for printed photovoltaics. Tandem cells with power conversion efficiencies of 8-10% were fabricated in the ambient atmosphere by doctor blade coating, selected to approximate the conditions during roll-to-roll manufacturing. Application of the light management structure onto an 8.7% efficient encapsulated tandem cell boosted the conversion efficiency of the cell to 9.5%. (C) 2018 Optical Society of America under the terms of the OSA Open Access Publishing Agreement
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000427900400003 Publication Date 2018-02-26
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1094-4087 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.307 Times cited 9 Open Access OpenAccess
Notes ; FP7 European collaborative project SUNFLOWER (FP7-ICT-2011-7, grant number 287594); German Federal Ministry of Education and Research (BMBF) (03xEK3504, project TAURUS); FP7 European project ESTEEM2 (grant number 312483); HEiKA centre FunTECH-3D. ; Approved Most recent IF: 3.307
Call Number UA @ lucian @ c:irua:150839UA @ admin @ c:irua:150839 Serial 4975
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Author Prabhakara, V.; Nuytten, T.; Bender, H.; Vandervorst, W.; Bals, S.; Verbeeck, J.
Title Linearized radially polarized light for improved precision in strain measurements using micro-Raman spectroscopy Type A1 Journal article
Year 2021 Publication Optics Express Abbreviated Journal (up) Opt Express
Volume 29 Issue 21 Pages 34531
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Strain engineering in semiconductor transistor devices has become vital in the semiconductor industry due to the ever-increasing need for performance enhancement at the nanoscale. Raman spectroscopy is a non-invasive measurement technique with high sensitivity to mechanical stress that does not require any special sample preparation procedures in comparison to characterization involving transmission electron microscopy (TEM), making it suitable for inline strain measurement in the semiconductor industry. Indeed, at present, strain measurements using Raman spectroscopy are already routinely carried out in semiconductor devices as it is cost effective, fast and non-destructive. In this paper we explore the usage of linearized radially polarized light as an excitation source, which does provide significantly enhanced accuracy and precision as compared to linearly polarized light for this application. Numerical simulations are done to quantitatively evaluate the electric field intensities that contribute to this enhanced sensitivity. We benchmark the experimental results against TEM diffraction-based techniques like nano-beam diffraction and Bessel diffraction. Differences between both approaches are assigned to strain relaxation due to sample thinning required in TEM setups, demonstrating the benefit of Raman for nondestructive inline testing.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000708940500144 Publication Date 2021-10-11
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1094-4087 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.307 Times cited 2 Open Access OpenAccess
Notes Horizon 2020 Framework Programme, 823717 – ESTEEM3 ; GOA project, “Solarpaint” ; Herculesstichting;; esteem3jra; esteem3reported; Approved Most recent IF: 3.307
Call Number EMAT @ emat @c:irua:182472 Serial 6816
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Author Krsmanovic, R.; Bals, S.; Bertoni, G.; Van Tendeloo, G.
Title Structural characterization of Er-doped Li2O-Al2O3-SiO2 glass ceramics Type A1 Journal article
Year 2008 Publication Optical materials Abbreviated Journal (up) Opt Mater
Volume 30 Issue 7 Pages 1183-1188
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Particularly favourable properties of glass ceramics are developed on the basis of two key advantages of these materials: the variation of chemical composition and of microstructure. Therefore, detailed structural and chemical information are necessary to get insight in novel glass ceramic materials. We present here two examples of Er-doped Li2O-Al2O3-SiO2, with different quantities of ZrO2, both obtained with sol-gel synthesis. Different transmission electron microscopy techniques: conventional TEM, HRTEM, and EELS are used and the results are compared with those previously obtained with XRD and Rietveld analysis. We also demonstrate the 3D reconstruction, obtained from HAADF-STEM imaging, to determine the morphology of nanosize precipitates in these composites. (c) 2007 Elsevier B.V. All rights reserved.
Address
Corporate Author Thesis
Publisher Place of Publication Amsterdam Editor
Language Wos 000254419100035 Publication Date 2007-07-11
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0925-3467; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 2.238 Times cited 12 Open Access
Notes Iap-V1; Esteem Approved Most recent IF: 2.238; 2008 IF: 1.714
Call Number UA @ lucian @ c:irua:70004 Serial 3219
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Author Ata, I.; Ben Dkhil, S.; Pfannmoeller, M.; Bals, S.; Duche, D.; Simon, J.-J.; Koganezawa, T.; Yoshimoto, N.; Videlot-Ackermann, C.; Margeat, O.; Ackermann, J.; Baeuerle, P.
Title The influence of branched alkyl side chains in A-D-A oligothiophenes on the photovoltaic performance and morphology of solution-processed bulk-heterojunction solar cells Type A1 Journal article
Year 2017 Publication Organic chemistry frontiers : an international journal of organic chemistry Abbreviated Journal (up) Org Chem Front
Volume 4 Issue 4 Pages 1561-1573
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Besides providing sufficient solubility, branched alkyl chains also affect the film-forming and packing properties of organic semiconductors. In order to avoid steric hindrance as it is present in wide-spread alkyl chains comprising a branching point position at the C2-position, i.e., 2-ethylhexyl, the branching point can be moved away from the pi-conjugated backbone. In this report, we study the influence of the modification of the branching point position from the C2-position in 2-hexyldecylamine (1) to the C4-position in 4-hexyldecylamine (2) connected to the central dithieno[3,2-b: 2', 3'-d] pyrrole (DTP) moiety in a well-studied A-D-A oligothiophene on the optoelectronic properties and photovoltaic performance in solution- processed bulk heterojunction solar cells (BHJSCs) with [6,6]-phenyl-C71-butyric acid methyl ester (PC71BM) as the acceptor material. Post-treatment of the photoactive layers is performed via solvent vapor annealing (SVA) in order to improve the film microstructure of the bulk heterojunction. The time evolution of nanoscale morphological changes is followed by combining scanning transmission electron microscopy with low-energy-loss spectroscopic imaging (STEM-SI), solid-state absorption spectroscopy, and two-dimensional grazing incidence X-ray diffraction (2D-GIXRD). Our results show an improvement of the photovoltaic performance that is dependent on the branching point position in the donor oligomer. Optical spacers are utilized to increase light absorption inside the co-oligomer 2-based BHJSCs leading to increased power conversion efficiencies (PCEs) of 8.2% when compared to the corresponding co-oligomer 1-based devices. A STEM-SI analysis of the respective device cross-sections of active layers containing 1 and 2 as donor materials indeed reveals significant differences in their respective active layer morphologies.
Address
Corporate Author Thesis
Publisher RSC Publishing Place of Publication London Editor
Language Wos 000406374800013 Publication Date 2017-05-02
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2052-4129 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.955 Times cited 24 Open Access OpenAccess
Notes ; We acknowledge financial support by the European Commission under the project “SUNFLOWER” (FP7-ICT-2011-7, grant number: 287594) and S.B. acknowledges the ERC Starting Grant Colouratoms (335078). ; Approved Most recent IF: 4.955
Call Number UA @ lucian @ c:irua:145176UA @ admin @ c:irua:145176 Serial 4727
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Author Guerrero, A.; Pfannmöller, M.; Kovalenko, A.; Ripolles, T.S.; Heidari, H.; Bals, S.; Kaufmann, L.-D.; Bisquert, J.; Garcia-Belmonte, G.
Title Nanoscale mapping by electron energy-loss spectroscopy reveals evolution of organic solar cell contact selectivity Type A1 Journal article
Year 2015 Publication Organic electronics: physics, materials, applications Abbreviated Journal (up) Org Electron
Volume 16 Issue 16 Pages 227-233
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Organic photovoltaic (OPV) devices are on the verge of commercialization being long-term stability a key challenge. Morphology evolution during lifetime has been suggested to be one of the main pathways accounting for performance degradation. There is however a lack of certainty on how specifically the morphology evolution relates to individual electrical parameters on operating devices. In this work a case study is created based on a thermodynamically unstable organic active layer which is monitored over a period of one year under non-accelerated degradation conditions. The morphology evolution is revealed by compositional analysis of ultrathin cross-sections using nanoscale imaging in scanning transmission electron microscopy (STEM) coupled with electron energy-loss spectroscopy (EELS). Additionally, devices are electrically monitored in real-time using the non-destructive electrical techniques capacitance-voltage (C-V) and Impedance Spectroscopy (IS). By comparison of imaging and electrical techniques the relationship between nanoscale morphology and individual electrical parameters of device operation can be conclusively discerned. It is ultimately observed how the change in the cathode contact properties occurring after the migration of fullerene molecules explains the improvement in the overall device performance. (C) 2014 Elsevier B.V. All rights reserved.
Address
Corporate Author Thesis
Publisher Place of Publication London Editor
Language Wos 000345649500029 Publication Date 2014-11-17
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1566-1199; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.399 Times cited 24 Open Access OpenAccess
Notes 287594 Sunflower; 335078 Colouratom; ECAS_Sara; (ROMEO:green; preprint:; postprint:can ; pdfversion:cannot); Approved Most recent IF: 3.399; 2015 IF: 3.827
Call Number c:irua:122169 Serial 2267
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Author Kumar, J.; Eraña, H.; López-Martínez, E.; Claes, N.; Martín, V.F.; Solís, D.M.; Bals, S.; Cortajarena, A.L.; Castilla, J.; Liz-Marzán, L.M.
Title Detection of amyloid fibrils in Parkinson’s disease using plasmonic chirality Type A1 Journal article
Year 2018 Publication Proceedings of the National Academy of Sciences of the United States of America Abbreviated Journal (up) P Natl Acad Sci Usa
Volume 115 Issue 115 Pages 3225-3230
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Amyloid fibrils, which are closely associated with various neurodegenerative

diseases, are the final products in many protein aggregation pathways. The identification of fibrils at low concentration is, therefore, pivotal in disease diagnosis and development of therapeutic strategies. We report a methodology for the specific identification of amyloid fibrils using chiroptical effects in plasmonic nanoparticles. The formation of amyloid fibrils based on α-synuclein was probed using gold nanorods, which showed no

apparent interaction with monomeric proteins but effective adsorption onto fibril structures via noncovalent interactions. The amyloid structure drives a helical nanorod arrangement, resulting in intense optical activity at the surface plasmon resonance wavelengths. This sensing technique was successfully applied to human brain homogenates of patients affected by Parkinson’s disease,

wherein protein fibrils related to the disease were identified through chiral signals from Au nanorods in the visible and near IR, whereas healthy brain samples did not exhibit any meaningful optical activity. The technique was additionally extended to the specific detection of infectious amyloids formed by prion proteins, thereby confirming the wide potential of the technique. The intense chiral response driven by strong dipolar coupling in helical Au nanorod arrangements allowed us to detect amyloid fibrils down to nanomolar concentrations.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000428382400032 Publication Date 2018-03-12
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0027-8424 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.661 Times cited 187 Open Access OpenAccess
Notes We thank Prof. Dr. J.-P. Timmermans and the Antwerp Centre of Advanced Microscopy for providing access to the Tecnai G2 Spirit BioTWIN TEM. We also thank the Basque Biobank (Basque Foundation for Health Innovation and Research, BIOEF) for providing us with Parkinson’s disease-affected brain samples. J.K. acknowledges financial support from the European Commission under Marie Sklodowska-Curie Program H2020- MSCA-IF-2015708321. S.B. and A.L.C. acknowledge European Research Council Grants 335078 COLOURATOM and 648071 ProNANO. S.B. and L.M.L.-M. acknowledge funding from European Commission Grant EUSMI 731019. A.L.C., J.C., and L.M.L.-M. acknowledge funding from Spanish Ministry of Economy and Competitiveness (MINECO) Grants MAT2013-46101- R, AGL2015-65046-C2-1-R, and BIO2016-77367-C2-1-R. (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:restricted); saraecas; ECASSara; Approved Most recent IF: 9.661
Call Number EMAT @ emat @c:irua:150355UA @ admin @ c:irua:150355 Serial 4918
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Author Sentosun, K.; Sanz Ortiz, M.N.; Batenburg, K.J.; Liz-Marzán, L.M.; Bals, S.
Title Combination of HAADF-STEM and ADF-STEM Tomography for Core-Shell Hybrid Materials Type A1 Journal article
Year 2015 Publication Particle and particle systems characterization Abbreviated Journal (up) Part Part Syst Char
Volume 32 Issue 32 Pages 1063-1067
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Vision lab
Abstract Characterization of core-shell type nanoparticles in 3D by transmission electron microscopy (TEM) can be very challenging. Especially when both heavy and light elements co-exist within the same nanostructure, artefacts in the 3D reconstruction are often present. A representative example would be a particle comprising an anisotropic metallic (Au) nanoparticle coated with a (mesoporous) silica shell. To obtain a reliable 3D characterization of such an object, we propose a dose-efficient strategy to simultaneously acquire high angle annular dark field scanning TEM and annular dark field tilt series for tomography. The 3D reconstruction is further improved by applying an advanced masking and interpolation approach to the acquired data. This new methodology enables us to obtain high quality reconstructions from which also quantitative information can be extracted. This approach is broadly applicable to investigate hybrid core-shell materials.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000368446800003 Publication Date 2015-10-13
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0934-0866; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.474 Times cited 13 Open Access OpenAccess
Notes S.B. acknowledges financial support from European Research Council (ERC) (ERC Starting Grant #335078-COLOURATOM). L.M. acknowledges funding from the EU, Grant# 310651-2 Self-Assembly in Confined Space (SACS). K.J.B acknowledges financial support from the Netherlands Organisation for Scientific Research (NWO), project number 639.072.005 and NWO CW 700.57.026. Networking support was provided by COST Action MP1207. The authors acknowledge the European Union under the Seventh Framework Program under a contract for an Integrated Infrastructure Initiative, Reference No. 312483-ESTEEM2 for financial support.; esteem2jra4; ECASSara; (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:cannot); Approved Most recent IF: 4.474; 2015 IF: 3.081
Call Number c:irua:129590 c:irua:129590 Serial 3967
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Author Altantzis, T.; Goris, B.; Sánchez-Iglesias, A.; Grzelczak, M.; Liz-Marzán, L.M.; Bals, S.
Title Quantitative structure determination of large three-dimensional nanoparticle assemblies Type A1 Journal article
Year 2013 Publication Particle and particle systems characterization Abbreviated Journal (up) Part Part Syst Char
Volume 30 Issue 1 Pages 84-88
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Thumbnail image of graphical abstract To investigate nanoassemblies in three dimensions, electron tomography is an important tool. For large nanoassemblies, it is not straightforward to obtain quantitative results in three dimensions. An optimized acquisition technique, incoherent bright field scanning transmission electron microscopy, is combined with an advanced 3D reconstruction algorithm. The approach is applied to quantitatively analyze large nanoassemblies in three dimensions.
Address
Corporate Author Thesis
Publisher Place of Publication Weinheim Editor
Language Wos 000310806000008 Publication Date 2012-11-07
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0934-0866; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.474 Times cited 23 Open Access
Notes Goa; Fwo; 267867 Plasmaquo; 262348 Esmi Approved Most recent IF: 4.474; 2013 IF: 0.537
Call Number UA @ lucian @ c:irua:101776 Serial 2763
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