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Author Berends, A.C.; van der Stam, W.; Hofmann, J.P.; Bladt, E.; Meeldijk, J.D.; Bals, S.; de Donega, C.M.
  Title Interplay between surface chemistry, precursor reactivity, and temperature determines outcome of ZnS shelling reactions on CuInS2 nanocrystals Type A1 Journal article
  Year 2018 Publication Chemistry of materials Abbreviated Journal Chem Mater
  Volume 30 Issue 30 Pages 2400-2413
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract ZnS shelling of I-III-VI(2 )nanocrystals (NCs) invariably leads to blue-shifts in both the absorption and photoluminescence spectra. These observations imply that the outcome of ZnS shelling reactions on I-III-VI2 colloidal NCs results from a complex interplay between several processes taking place in solution, at the surface of, and within the seed NC. However, a fundamental understanding of the factors determining the balance between these different processes is still lacking. In this work, we address this need by investigating the impact of precursor reactivity, reaction temperature, and surface chemistry (due to the washing procedure) on the outcome of ZnS shelling reactions on CuInS2 NCs using a seeded growth approach. We demonstrate that low reaction temperatures (150 degrees C) favor etching, cation exchange, and alloying regardless of the precursors used. Heteroepitaxial shell overgrowth becomes the dominant process only if reactive S- and Zn-precursors (S-ODE/OLAM and ZnI2 ) and high reaction temperatures (210 degrees C) are used, although a certain degree of heterointerfacial alloying still occurs. Remarkably, the presence of residual acetate at the surface of CIS seed NCs washed with ethanol is shown to facilitate heteroepitaxial shell overgrowth, yielding for the first time CIS/ZnS core/shell NCs displaying red-shifted absorption spectra, in agreement with the spectral shifts expected for a type-I band alignment. The insights provided by this work pave the way toward the design of improved synthesis strategies to CIS/ZnS core/shell and alloy NCs with tailored elemental distribution profiles, allowing precise tuning of the optoelectronic properties of the resulting materials.
  Address
  Corporate Author Thesis
  Publisher American Chemical Society Place of Publication Washington, D.C Editor
  Language Wos 000430023700027 Publication Date 2018-03-25
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 9.466 Times cited 85 Open Access OpenAccess
  Notes ; Annelies van der Bok is gratefully acknowledged for performing the ICP measurements. A.C.B. and C.d.M.D. acknowledge financial support from the division of Chemical Sciences (CW) of The Netherlands Organization for Scientific Research (NWO) under Grant No. ECHO.712.014.001. S.B. and E.B. acknowledge financial support from European Research Council (ERC Starting Grant No. 335078-COLOURATOMS). ; Ecas_Sara Approved Most recent IF: 9.466
  Call Number UA @ lucian @ c:irua:150772UA @ admin @ c:irua:150772 Serial 4972
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Author Pearce, P.E.; Rousse, G.; Karakulina, O.M.; Hadermann, J.; Van Tendeloo, G.; Foix, D.; Fauth, F.; Abakumov, A.M.; Tarascon, J.-M.
  Title β-Na1.7IrO3: A Tridimensional Na-Ion Insertion Material with a Redox Active Oxygen Network Type A1 Journal article
  Year 2018 Publication Chemistry of materials Abbreviated Journal Chem Mater
  Volume 30 Issue 10 Pages 3285-3293
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract The revival of the Na-ion battery concept has prompted an intense search for new high capacity Na-based positive electrodes. Recently, emphasis has been placed on manipulating Na-based layered compounds to trigger the participation of the anionic network. We further explored this direction and show the feasibility of achieving anionic-redox activity in three-dimensional Na-based compounds. A new 3D β-Na1.7IrO3 phase was synthesized in a two-step process, which involves first the electrochemical removal of Li from β-Li2IrO3 to produce β-IrO3, which is subsequently reduced by electrochemical Na insertion. We show that β-Na1.7IrO3 can reversibly uptake nearly 1.3 Na+ per formula unit through an uneven voltage profile characterized by the presence of four plateaus related to structural transitions. Surprisingly, the β-Na1.7IrO3 phase was found to be stable up to 600 °C, while it could not be directly synthesized via conventional synthetic methods. Although these Na-based iridate phases are of limited practical interest, they help to understand how introducing highly polarizable guest ions (Na+) into host rocksalt-derived oxide structures affects the anionic redox mechanism.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000433403800014 Publication Date 2018-05-22
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 9.466 Times cited 6 Open Access OpenAccess
  Notes The authors thank A. Perez for fruitful discussions and his valuable help in synchrotron XRD experiment and Matthieu Courty for carrying out the DSC measurements. The authors also greatly thank Matthieu Saubanère and Marie-Liesse Doublet for valuable discussions on theoretical aspects of this work. This work is based on experiments performed on the Materials Science and Powder Diffraction Beamline at ALBA synchrotron (Proposal 2016091814), Cerdanyola del Vallès, E- 08290 Barcelona, Spain. J.-M.T. acknowledges funding from the European Research Council (ERC) (FP/2014)/ERC Grant- Project 670116-ARPEMA. G.R. acknowledges funding from ANR DeliRedox. O.M.K., J.H., and A.M.A. are grateful to FWO Vlaanderen for financial support under Grant G040116N. Approved Most recent IF: 9.466
  Call Number EMAT @ emat @c:irua:152048 Serial 4996
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Author Peters, J.L.; Altantzis, T.; Lobato, I.; Jazi, M.A.; van Overbeek, C.; Bals, S.; Vanmaekelbergh, D.; Sinai, S.B.
  Title Mono- and Multilayer Silicene-Type Honeycomb Lattices by Oriented Attachment of PbSe Nanocrystals: Synthesis, Structural Characterization, and Analysis of the Disorder Type A1 Journal article
  Year 2018 Publication Chemistry of materials Abbreviated Journal Chem Mater
  Volume 30 Issue 30 Pages 4831-4837
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract Nanocrystal (NC) solids are commonly prepared from nonpolar organic NC suspensions. In many cases, the capping on the NC surface is preserved and forms a barrier between the NCs. More recently, superstructures with crystalline connections between the NCs, implying the removal of the capping, have been reported, too. Here, we present large-scale uniform superstructures of attached PbSe NCs with a silicene-type honeycomb geometry, resulting from solvent evaporation under nearly reversible conditions. We also prepared multilayered silicene honeycomb structures by using larger amounts of PbSe NCs. We show that the two-dimensional silicene superstructures can be seen as a crystallographic slice from a 3-D simple cubic structure. We describe the disorder in the silicene lattices in terms of the nanocrystals position and their atomic alignment. The silicene honeycomb sheets are large enough to be used in transistors and optoelectronic devices.
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  Publisher Place of Publication Editor
  Language Wos 000440105500042 Publication Date 2018-07-24
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 9.466 Times cited 33 Open Access OpenAccess
  Notes The authors acknowledge funding from the European Commission (Grant EUSMI 731019). S.B. acknowledges funding from the European Research Council (Grant 335078 COLOURATOM). T.A. acknowledges a postdoctoral grant from the Research Foundation Flanders (FWO). The authors acknowledge financial support from the European Commission under the Horizon 2020 Programme by means of the Grant Agreement No. 731019 EUSMI. (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); ecas_sara Approved Most recent IF: 9.466
  Call Number EMAT @ emat @c:irua:152997UA @ admin @ c:irua:152997 Serial 5011
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Author Grimaud, A.; Iadecola, A.; Batuk, D.; Saubanere, M.; Abakumov, A.M.; Freeland, J.W.; Cabana, J.; Li, H.; Doublet, M.-L.; Rousse, G.; Tarascon, J.-M.
  Title Chemical activity of the peroxide/oxide redox couple : case study of Ba5Ru2O11 in aqueous and organic solvents Type A1 Journal article
  Year 2018 Publication Chemistry of materials Abbreviated Journal Chem Mater
  Volume 30 Issue 11 Pages 3882-3893
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract The finding that triggering the redox activity of oxygen ions within the lattice of transition metal oxides can boost the performances of materials used in energy storage and conversion devices such as Li-ion batteries or oxygen evolution electrocatalysts has recently spurred intensive and innovative research in the field of energy. While experimental and theoretical efforts have been critical in understanding the role of oxygen nonbonding states in the redox activity of oxygen ions, a clear picture of the redox chemistry of the oxygen species formed upon this oxidation process is still missing. This can be, in part, explained by the complexity in stabilizing and studying these species once electrochemically formed. In this work, we alleviate this difficulty by studying the phase Ba5Ru2O11, which contains peroxide O-2(2-) groups, as oxygen evolution reaction electrocatalyst and Li-ion battery material. Combining physical characterization and electrochemical measurements, we demonstrate that peroxide groups can easily be oxidized at relatively low potential, leading to the formation of gaseous dioxygen and to the instability of the oxide. Furthermore, we demonstrate that, owing to the stabilization at high energy of peroxide, the high-lying energy of the empty sigma* antibonding O-O states limits the reversibility of the electrochemical reactions when the O-2(2-)/O2- redox couple is used as redox center for Li-ion battery materials or as OER redox active sites. Overall, this work suggests that the formation of true peroxide O-2(2-) states are detrimental for transition metal oxides used as OER catalysts and Li-ion battery materials. Rather, oxygen species with O-O bond order lower than 1 would be preferred for these applications.
  Address
  Corporate Author Thesis
  Publisher American Chemical Society Place of Publication Washington, D.C Editor
  Language Wos 000435416600038 Publication Date 2018-05-21
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 9.466 Times cited 2 Open Access Not_Open_Access
  Notes ; We thank S. Belin of the ROCK beamline (financed by the French National Research Agency (ANR) as a part of the “Investissements d'Avenir” program, reference: ANR-10-EQPX-45; proposal no. 20160095) of synchrotron SOLEIL for her assistance during XAS measurements. Authors would also like to thank V. Nassif for her assistance on the D1B beamline. A.G, G.R, and J.-M.T. acknowledge funding from the European Research Council (ERC) (FP/2014)/ERC Grant Project 670116-ARPEMA. ; Approved Most recent IF: 9.466
  Call Number UA @ lucian @ c:irua:151980 Serial 5016
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Author Quintanilla, M.; Zhang, Y.; Liz-Marzan, L.M.
  Title Subtissue plasmonic heating monitored with CaF2:Nd3+,Y3+ nanothermometers in the second biological window Type A1 Journal article
  Year 2018 Publication Chemistry of materials Abbreviated Journal Chem Mater
  Volume 30 Issue 8 Pages 2819-2828
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract Measuring temperature in biological environments is an ambitious goal toward supporting medical treatment and diagnosis. Minimally invasive techniques based on optical probes require very specific properties that are difficult to combine within a single material. These include high chemical stability in aqueous environments, optical signal stability, low toxicity, high emission intensity, and, essential, working at wavelengths within the biological transparency windows so as to minimize invasiveness while maximizing penetration depth. We propose CaF2:Nd3+,Y3+ as a candidate for thermometry based on an intraband ratiometric approach, fully working within the biological windows (excitation at 808 nm; emission around 1050 nm). We optimized the thermal probes through the addition of Y3+ as a dopant to improve both emission intensity and thermal sensitivity. To define the conditions under which the proposed technique can be applied, gold nanorods were used to optically generate subtissue hot areas, while the resulting temperature variation was monitored with the new nanothermometers.
  Address
  Corporate Author Thesis
  Publisher American Chemical Society Place of Publication Washington, D.C Editor
  Language Wos 000431088400038 Publication Date 2018-03-27
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 9.466 Times cited 28 Open Access Not_Open_Access
  Notes ; The authors would like to thank Dr. Guillermo Gonzalez Rubio for the kind support with the synthesis of gold nanorods. M.Q and L.M.L.-M. acknowledge financial support from the European Commission under the Marie Sklodowska-Curie program (H2020-MSCA-IF-2014_659021 – PHELLINI). Y.Z. acknowledges financial support from the European Union's Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie Grant Agreement No. 665501 through a FWO [PEGASUS]^2 Marie Sklodowska-Curie fellowship (12U4917N). ; Approved Most recent IF: 9.466
  Call Number UA @ lucian @ c:irua:151576 Serial 5042
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Author Van Tendeloo, L.; Wangermez, W.; Vandekerkhove, A.; Willhammar, T.; Bals, S.; Maes, A.; Martens, J.A.; Kirschhock, C.E.A.; Breynaert, E.
  Title Postsynthetic high-alumina zeolite crystal engineering in organic free hyper-alkaline media Type A1 Journal article
  Year 2017 Publication Chemistry of materials Abbreviated Journal Chem Mater
  Volume 29 Issue 29 Pages 629-638
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract Postsynthetic modification of high -alumina zeolites in hyper alkaline media can be tailored toward alteration of framework topology, crystal size and morphology, or desired Si/A1 ratio. FAU, EMT, MAZ, KFI, HEU, and LTA starting materials were treated with 1.2 M MOH (M = Na, K, RE, or Cs), leading to systematic ordered porosity or fully transformed frameworks with new topology and adjustable Si/Al ratio. In addition to the versatility of this tool for zeolite crystal engineering, these alterations improve understanding of the crystal chemistry. Such knowledge can guide further development in zeolite crystal engineering. Postsynthetic alteration also provides insight on the long-term stability of aluminosilicate zeolites that are used as a sorption sink in concrete -based waste disposal facilities in harsh alkaline conditions.
  Address
  Corporate Author Thesis
  Publisher American Chemical Society Place of Publication Washington, D.C Editor
  Language Wos 000392891700021 Publication Date 2016-12-20
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 9.466 Times cited 16 Open Access OpenAccess
  Notes ; This work was supported by long-term structural funding by the Flemish Government (Methusalem grant of Prof. J. Martens) and by ONDRAF/NIRAS, the Belgian Agency for Radioactive Waste and Fissile Materials, as part of the program on surface disposal of Belgian Category A waste. The Belgian government is acknowledged for financing the interuniversity poles of attraction (IAP-PAI). S.B. acknowledges financial support from European Research Council (ERC Advanced Grant No. 24691-COUNTATOMS, ERC Starting Grant No. 335078-COLOURATOMS). ; Ecas_Sara Approved Most recent IF: 9.466
  Call Number UA @ lucian @ c:irua:152674UA @ admin @ c:irua:152674 Serial 5145
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Author Tessier, M.D.; Baquero, E.A.; Dupont, D.; Grigel, V.; Bladt, E.; Bals, S.; Coppel, Y.; Hens, Z.; Nayral, C.; Delpech, F.
  Title Interfacial oxidation and photoluminescence of InP-Based core/shell quantum dots Type A1 Journal article
  Year 2018 Publication Chemistry of materials Abbreviated Journal Chem Mater
  Volume 30 Issue 30 Pages 6877-6883
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract Indium phosphide colloidal quantum dots (QDs) are emerging as an efficient cadmium-free alternative for optoelectronic applications. Recently, syntheses based on easy-to-implement aminophosphine precursors have been developed. We show by solid-state nuclear magnetic resonance spectroscopy that this new approach allows oxide-free indium phosphide core or core/shell quantum dots to be made. Importantly, the oxide-free core/shell interface does not help in achieving higher luminescence efficiencies. We demonstrate that in the case of InP/ZnS and InP/ZnSe QDs, a more pronounced oxidation concurs with a higher photoluminescence efficiency. This study suggests that a II-VI shell on a III-V core generates an interface prone to defects. The most efficient InP/ZnS or InP/ZnSe QDs are therefore made with an oxide buffer layer between the core and the shell: it passivates these interface defects but also results in a somewhat broader emission line width.
  Address
  Corporate Author Thesis
  Publisher American Chemical Society Place of Publication Washington, D.C Editor
  Language Wos 000447237800031 Publication Date 2018-09-12
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 9.466 Times cited 74 Open Access OpenAccess
  Notes ; The authors thank L. Biadala and C. Delerue for fruitful discussion. Z.H. acknowledges support by the European Commission via the Marie-Sklodowska Curie action Phonsi (H2020-MSCA-ITN-642656), by Research Foundation Flanders (Project 17006602), and by Ghent University (GOA No. 01G01513). Z.H., M.D.T., and D.D. acknowledge the Strategisch Initiatief Materialen in Vlaanderen of Agentschap Innoveren en Ondernemen (SIM VLAIO), vzw (SBO-QDOCCO, ICON-QUALIDI). This work was supported by the Universite Paul Sabatier, the Region Midi-Pyrenees, the CNRS, the Institut National des Sciences Appliquees of Toulouse, and the Agence Nationale pour la Recherche (Project ANR-13-IS10-0004-01). E.A.B. is grateful to Marie Curie Actions and Campus France for a PRESTIGE postdoc fellowship (FP7 /2007-2013) under REA Grant Agreement PCOFUND-GA-2013-609102. E.B. acknowledges financial support from Research Foundation Flanders (FWO). ; Approved Most recent IF: 9.466
  Call Number UA @ lucian @ c:irua:154732UA @ admin @ c:irua:154732 Serial 5109
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Author Morozov, V.; Deyneko, D.; Basoyich, O.; Khaikina, E.G.; Spassky, D.; Morozov, A.; Chernyshev, V.; Abakumov, A.; Hadermann, J.
  Title Incommensurately modulated structures and luminescence properties of the AgxSm(2-x)/3WO4 (x=0.286, 0.2) scheelites as thermographic phosphors Type A1 Journal article
  Year 2018 Publication Chemistry of materials Abbreviated Journal Chem Mater
  Volume 30 Issue 14 Pages 4788-4798
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract Ag+ for Sm3+ substitution in the scheelite-type AgxSm(2-x)/3 square(1-2x)/3WO4 tungstates has been investigated for its influence on the cation-vacancy ordering and luminescence properties. A solid state method was used to synthesize the x = 0.286 and x = 0.2 compounds, which exhibited (3 + 1)D incommensurately modulated structures in the transmission electron microscopy study. Their structures were refined using high resolution synchrotron powder X-ray diffraction data. Under near-ultraviolet light, both compounds show the characteristic emission lines for (4)G(5/2) -> H-6(J) (J = 5/2, 7/2, 9/2, and 11/2) transitions of the Sm3+ ions in the range 550-720 nm, with the J = 9/2 transition at the similar to 648 nm region being dominant for all photoluminescence spectra. The intensities of the (4)G(5/2) -> H-6(9/2) and (4)G(5/2) -> H-6(7/2) bands have different temperature dependencies. The emission intensity ratios (R) for these bands vary reproducibly with temperature, allowing the use of these materials as thermographic phosphors.
  Address
  Corporate Author Thesis
  Publisher American Chemical Society Place of Publication Washington, D.C Editor
  Language Wos 000440105500037 Publication Date 2018-06-21
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 9.466 Times cited 2 Open Access Not_Open_Access
  Notes ; This research was supported by FWO (Project G039211N), Flanders Research Foundation. The research was carried out within the state assignment of FASO of Russia (Themes No. 0339-2016-0007). V.M. thanks the Russian Foundation for Basic Research (Grant 18-03-00611) for financial support. E.G.K. and O.B. acknowledge financial support from the Russian Foundation for Basic Research (Grant 16-03-00510). D.D. thanks the Foundation of the Russian Federation President (Grant MK-3502.2018.5) for financial support. We are grateful to the ESRF for granting the beamtime. V.C. is grateful for the financial support of the Russian Ministry of Science and Education (Project No. RFMEFI61616X0069). We are grateful to the ESRF for the access to ID22 station (experiment MA-3313). ; Approved Most recent IF: 9.466
  Call Number UA @ lucian @ c:irua:153156 Serial 5107
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Author De Sloovere, D.; Safari, M.; Elen, K.; D'Haen, J.; Drozhzhin, O.A.; Abakumov, A.M.; Simenas, M.; Banys, J.; Bekaert, J.; Partoens, B.; Van Bael, M.K.; Hardy, A.
  Title Reduced Na2+xTi4O9 composite : a durable anode for sodium-ion batteries Type A1 Journal article
  Year 2018 Publication Chemistry of materials Abbreviated Journal Chem Mater
  Volume 30 Issue 23 Pages 8521-8527
  Keywords A1 Journal article; Condensed Matter Theory (CMT)
  Abstract Sodium-ion batteries (SIBs) are potential cost-effective solutions for stationary energy storage applications. Unavailability of suitable anode materials, however, is one of the important barriers to the maturity of SIBs. Here, we report a Na2+xTi4O9/C composite as a promising anode candidate for SIBs with high capacity and cycling stability. This anode is characterized by a capacity of 124 mAh g(-1) (plus 11 mAh g(-1) contributed by carbon black), an average discharge potential of 0.9 V vs Na/Na+, a good rate capability and a high stability (89% capacity retention after 250 cycles at a rate of 1 degrees C). The mechanisms of sodium insertion/deinsertion and of the formation of Na2+xTi4O9/C are investigated with the aid of various ex/in situ characterization techniques. The in situ formed carbon is necessary for the formation of the reduced sodium titanate. This synthesis method may enable the convenient synthesis of other composites of crystalline phases with amorphous carbon.
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  Publisher Place of Publication Editor
  Language Wos 000453489300014 Publication Date 2018-11-29
  Series Editor Series Title Abbreviated Series Title
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  ISSN (down) 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 9.466 Times cited 7 Open Access
  Notes ; This work was supported by the FWO (Research Foundation Flanders, project G040116). O.A.D. and A.M.A. are grateful to the Russian Science Foundation for financial support (Grant 17-73-30006). The authors acknowledge Pieter Samyn for Raman spectroscopy, Fulya Ulu Okudur for preliminary TEM, Bart Ruttens for XRD, Hilde Pellaers for SEM, Tom Haeldermans for elemental analysis, and Karen Leyssen and Vera Meynen for physisorption measurements. ; Approved Most recent IF: 9.466
  Call Number UA @ admin @ c:irua:156235 Serial 5227
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Author Akkerman, Q.A.; Bladt, E.; Petralanda, U.; Dang, Z.; Sartori, E.; Baranov, D.; Abdelhady, A.L.; Infante, I.; Bals, S.; Manna, L.
  Title Fully inorganic Ruddlesden-Popper double CI-I and triple CI-Br-I lead halide perovskite nanocrystals Type A1 Journal article
  Year 2019 Publication Chemistry of materials Abbreviated Journal Chem Mater
  Volume 31 Issue 31 Pages 2182-2190
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract The vast majority of lead halide perovskite (LHP) nanocrystals (NCs) are currently based on either a single halide composition (CsPbCl3, CsPbBr3, and CsPbI3) or an alloyed mixture of bromide with either Cl- or I- [i.e., CsPb(Br:Cl)(3) or CsPb(Br:I)(3)]. In this work, we present the synthesis as well as a detailed optical and structural study of two halide alloying cases that have not previously been reported for LHP NCs: Cs2PbI2Cl2 NCs and triple halide CsPb(Cl:Br:I)(3) NCs. In the case of Cs2PbI2Cl2, we observe for the first time NCs with a fully inorganic Ruddlesden-Popper phase (RPP) crystal structure. Unlike the well-explored organic-inorganic RPP, here, the RPP formation is triggered by the size difference between the halide ions. These NCs exhibit a strong excitonic absorption, albeit with a weak photoluminescence quantum yield (PLQY). In the case of the triple halide CsPb(Cl:Br:I)(3) composition, the NCs comprise a CsPbBr2Cl perovskite crystal lattice with only a small amount of incorporated iodide, which segregates at RPP planes' interfaces within the CsPb(Cl:Br:I)(3) NCs. Supported by density functional theory calculations and postsynthetic surface treatments to enhance the PLQY, we show that the combination of iodide segregation and defective RPP interfaces are most likely linked to the strong PL quenching observed in these nanostructures. In summary, this work demonstrates the limits of halide alloying in LHP NCs because a mixture that contains halide ions of very different sizes leads to the formation of defective RPP interfaces and a severe quenching of LHP NC's optical properties.
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  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000462950400038 Publication Date 2019-03-04
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 9.466 Times cited 58 Open Access OpenAccess
  Notes ; Q.A.A. and L.M. acknowledge funding from the European Union Seventh Framework Programme under grant agreement no. 614897 (ERC Consolidator Grant “TRANS-NANO”). The work of D.B. was supported by the European Union's Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie grant agreement no. 794560. E.B. and S.B. acknowledge funding from the Research Foundation Flanders (G.038116N, G.03691, and funding of a postdoctoral grant to E.B.). I.I. acknowledges The Netherlands Organization of Scientific Research (NWO) for financial support through the Innovational Research Incentive (Vidi) Scheme (grant no. 723.013.002). The computational work was carried out on the Dutch national e-infrastructure with the support of the SURF Cooperative. ; Approved Most recent IF: 9.466
  Call Number UA @ admin @ c:irua:159414 Serial 5250
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Author Tan, X.; Stephens, P.W.; Hendrickx, M.; Hadermann, J.; Segre, C.U.; Croft, M.; Kang, C.-J.; Deng, Z.; Lapidus, S.H.; Kim, S.W.; Jin, C.; Kotliar, G.; Greenblatt, M.
  Title Tetragonal Cs1.17In0.81Cl3 : a charge-ordered indium halide perovskite derivative Type A1 Journal article
  Year 2019 Publication Chemistry of materials Abbreviated Journal Chem Mater
  Volume 31 Issue 6 Pages 1981-1989
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract Polycrystalline samples of Cs1.17In0.81Cl3 were prepared by annealing a mixture of CsCl, InCl, and InCl3, stoichiometric for the targeted CsInCl3. Synchrotron powder X-ray diffraction refinement and chemical analysis by energy dispersive X-ray indicated that Cs1.17In0.81Cl3, a tetragonal distorted perovskite derivative (I4/m), is the thermodynamically stable product. The refined unit cell parameters and space group were confirmed by electron diffraction. In the tetragonal structure, In+ and In3+ are located in four different crystallographic sites, consistent with their corresponding bond lengths. In1, In2, and In3 are octahedrally coordinated, whereas In4 is at the center of a pentagonal bipyramid of Cl because of the noncooperative octahedral tilting of In4Cl6. The charged-ordered In+ and In3+ were also confirmed by X-ray absorption and Raman spectroscopy. Cs1.17In0.81Cl3 is the first example of an inorganic halide double perovskite derivative with charged-ordered In+ and In3+. Band structure and optical conductivity calculations were carried out with both generalized gradient approximation (GGA) and modified Becke-Johnson (mBJ) approach; the GGA calculations estimated the band gap and optical band gap to be 2.27 eV and 2.4 eV, respectively. The large and indirect band gap suggests that Cs1.17In0.81Cl3 is not a good candidate for photovoltaic application.
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  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000462950400017 Publication Date 2019-02-19
  Series Editor Series Title Abbreviated Series Title
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  ISSN (down) 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 9.466 Times cited 6 Open Access OpenAccess
  Notes ; M.G. and X.T. were supported by the Center for Computational Design of Functional Strongly Correlated Materials and Theoretical Spectroscopy under DOE Grant No. DE-FOA-0001276. M.G. also acknowledges support of NSF-DMR-1507252 grant. G.K. and C.-J.K. were supported by the Air Force Office of Scientific Research. MRCAT operations are supported by the Department of Energy and the MRCAT member institutions. The use of the Advanced Photon Source at the Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. The works at IOPCAS were supported by NSF & MOST of China through research projects. ; Approved Most recent IF: 9.466
  Call Number UA @ admin @ c:irua:159413 Serial 5262
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Author Choudhary, K.; Bercx, M.; Jiang, J.; Pachter, R.; Lamoen, D.; Tavazza, F.
  Title Accelerated Discovery of Efficient Solar Cell Materials Using Quantum and Machine-Learning Methods Type A1 Journal article
  Year 2019 Publication Chemistry of materials Abbreviated Journal Chem Mater
  Volume 31 Issue 15 Pages 5900-5908
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract Solar energy plays an important role in solving serious environmental

problems and meeting the high energy demand. However, the lack of suitable

materials hinders further progress of this technology. Here, we present the largest

inorganic solar cell material search till date using density functional theory (DFT) and

machine-learning approaches. We calculated the spectroscopic limited maximum

efficiency (SLME) using the Tran−Blaha-modified Becke−Johnson potential for 5097

nonmetallic materials and identified 1997 candidates with an SLME higher than 10%,

including 934 candidates with a suitable convex-hull stability and an effective carrier

mass. Screening for two-dimensional-layered cases, we found 58 potential materials

and performed G0W0 calculations on a subset to estimate the prediction uncertainty. As the above DFT methods are still computationally expensive, we developed a high accuracy machine-learning model to prescreen efficient materials and applied it to over a million materials. Our results provide a general framework and universal strategy for the design of high-efficiency solar

cell materials. The data and tools are publicly distributed at: https://www.ctcms.nist.gov/~knc6/JVASP.html, https://www.

ctcms.nist.gov/jarvisml/, https://jarvis.nist.gov/, and https://github.com/usnistgov/jarvis.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000480826900060 Publication Date 2019-08-13
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 9.466 Times cited 6 Open Access
  Notes ; ; Approved Most recent IF: 9.466
  Call Number EMAT @ emat @c:irua:161814 Serial 5291
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Author Ramachandran, R.K.; Filez, M.; Solano, E.; Poelman, H.; Minjauw, M.M.; Van Daele, M.; Feng, J.-Y.; La Porta, A.; Altantzis, T.; Fonda, E.; Coati, A.; Garreau, Y.; Bals, S.; Marin, G.B.; Detavernier, C.; Dendooven, J.
  Title Chemical and Structural Configuration of Pt Doped Metal Oxide Thin Films Prepared by Atomic Layer Deposition Type A1 Journal article
  Year 2019 Publication Chemistry of materials Abbreviated Journal Chem Mater
  Volume 31 Issue 31 Pages 9673-9683
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
  Abstract Pt doped semiconducting metal oxides and Pt metal clusters embedded in an oxide matrix are of interest for applications such as catalysis and gas sensing, energy storage and memory devices. Accurate tuning of the dopant level is crucial for adjusting the properties of these materials. Here, a novel atomic layer deposition (ALD) based method for doping Pt into In2O3 in specific, and metals in metal oxides in general, is demonstrated. This approach combines alternating exposures of Pt and In2O3 ALD processes in a single ‘supercycle’, followed by supercycle repetition leading to multilayered nanocomposites. The atomic level control of ALD and its conformal nature make the method suitable for accurate dopant control even on high surface area supports. Oxidation state, local structural environment and crystalline phase of the embedded Pt dopants were obtained by means of X-ray characterization methods and high angle annular dark-field scanning transmission electron microscopy (HAADF-STEM). In addition, this approach allows characterization of the nucleation stages of metal ALD processes, by stacking those states multiple times in an oxide matrix. Regardless of experimental conditions, a few Pt ALD cycles leads to the formation of oxidized Pt species due to their highly dispersed nature, as proven by X-ray absorption spectroscopy (XAS). Grazing-incidence small-angle X-ray scattering (GISAXS) and highresolution scanning transmission electron microscopy, combined with energy dispersive X-ray spectroscopy (HR-STEM/EDXS) show that Pt is evenly distributed in the In2O3 metal oxide matrix without the formation of clusters. For a larger number of Pt ALD

cycles, typ. > 10, the oxidation state gradually evolves towards fully metallic, and metallic Pt clusters are obtained within the In2O3 metal oxide matrix. This work reveals how tuning of the ALD supercycle approach for Pt doping allows controlled engineering of the Pt compositional and structural configuration within a metal oxide matrix.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000502418000010 Publication Date 2019-11-11
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 9.466 Times cited 6 Open Access OpenAccess
  Notes This research was supported by the Flemish Research Foundation (FWO-Vlaanderen), the Flemish Government (Long term structural funding – Methusalem funding and Medium scale research infrastructure funding-Hercules funding), the Special Research Fund BOF of Ghent University (GOA 01G01513) and the CALIPSO Trans National Access Program funded by the European Commission in supplying financing of travel costs. We are grateful to the SIXS and SAMBA-SOLEIL staff for smoothly running the beamline facilities. J.D. and R.K.R. are postdoctoral fellows of the FWO. Approved Most recent IF: 9.466
  Call Number EMAT @ emat @c:irua:164056 Serial 5380
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Author Kirkwood, N.; De Backer, A.; Altantzis, T.; Winckelmans, N.; Longo, A.; Antolinez, F.V.; Rabouw, F.T.; De Trizio, L.; Geuchies, J.J.; Mulder, J.T.; Renaud, N.; Bals, S.; Manna, L.; Houtepen, A.J.
  Title Locating and controlling the Zn content in In(Zn)P quantum dots Type A1 Journal article
  Year 2019 Publication Chemistry of materials Abbreviated Journal Chem Mater
  Volume 32 Issue 32 Pages 557-565
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract Zinc is routinely employed in the synthesis of InP quantum dots (QDs) to improve the photoluminescence efficiency and carrier mobility of the resulting In(Zn)P alloy nanostructures. The exact location of Zn in the final structures and the mechanism by which it enhances the optoelectronic properties of the QDs is debated. We use synchrotron X-ray absorbance spectroscopy to show that the majority of Zn in In(Zn)P QDs is located at their surface as Zn-carboxylates. However, a small amount of Zn is present inside the bulk of the QDs with the consequent contraction of their lattice, as confirmed by combining high resolution high-angle annular dark-field imaging scanning transmission electron microscopy (HAADF-STEM) with statistical parameter estimation theory. We further demonstrate that the Zn content and its incorporation into the QDs can be tuned by the ligation of commonly employed Zn carboxylate precursors: the use of highly reactive Zn-acetate leads to the formation of undesired Zn3P2 and the final nanostructures being characterized by broad optical features, whereas Zn-carboxylates with longer carbon chains lead to InP crystals with much lower zinc content and narrow optical features. These results can explain the differences between structural and optical properties of In(Zn)P samples reported across the literature, and provide a rational method to tune the amount of Zn in InP nanocrystals and to drive the incorporation of Zn either as surface Zn-carboxylate, as a substitutional dopant inside the InP crystal lattice, or even predominantly as Zn3P2.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000507721600056 Publication Date 2019-12-13
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 9.466 Times cited 39 Open Access OpenAccess
  Notes A.J.H. acknowledges support from the European Research Council Horizon 2020 ERC Grant Agreement No. 678004 (Doping on Demand). This research is supported by the Dutch Technology Foundation TTW, which is part of The Netherlands Organization for Scientific Research (NWO), and which is partly funded by Ministry of Economic Affairs. SB acknowledges funding from the European Research Council (grant 815128 REALNANO). The authors gratefully acknowledge funding from the Research Foundation Flanders (FWO, Belgium) through project funding G.0381.16N and a postdoctoral grant to A.D.B. AJH, LM and JM acknowledge support from the H2020 Collaborative Project TEQ (Grant No. 766900).; sygma Approved Most recent IF: 9.466
  Call Number EMAT @ emat @c:irua:165234 Serial 5438
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Author Minjauw, M.M.; Solano, E.; Sree, S.P.; Asapu, R.; Van Daele, M.; Ramachandran, R.K.; Heremans, G.; Verbruggen, S.W.; Lenaerts, S.; Martens, J.A.; Detavernier, C.; Dendooven, J.
  Title Plasma-enhanced atomic layer deposition of silver using Ag(fod)(PEt3) and NH3-plasma Type A1 Journal article
  Year 2017 Publication Chemistry of materials Abbreviated Journal Chem Mater
  Volume 29 Issue 17 Pages 7114-7121
  Keywords A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL)
  Abstract A plasma-enhanced atomic layer deposition (ALD) process using the Ag(fod)(PEt3) precursor [(triethylphosphine)(6,6,7,7,8,8,8-heptafluoro-2,2-dimethy1-3,5-octanedionate)silver(I)] in combination with NH3-plasma is reported. The steady growth rate of the reported process (0.24 +/- 0.03 nm/cycle) was found to be 6 times larger than that of the previously reported Ag ALD process based on the same precursor in combination with H-2-plasma (0.04 +/- 0.02 nm/cycle). The ALD characteristics of the H-2-plasma and NH3-plasma processes were verified. The deposited Ag films were polycrystalline face-centered cubic Ag for both processes. The film morphology was investigated by ex situ scanning electron microscopy and grazing-incidence small-angle X-ray scattering, and it was found that films grown with the NH3-plasma process exhibit a much higher particle areal density and smaller particle sizes on oxide substrates compared to those deposited using the H-2-plasma process. This control over morphology of the deposited Ag is important for applications in catalysis and plasmonics. While films grown with the H-2-plasma process had oxygen impurities (similar to 9 atom %) in the bulk, the main impurity for the NH3-plasma process was nitrogen (similar to 7 atom %). In situ Fourier transform infrared spectroscopy experiments suggest that these nitrogen impurities are derived from NH surface groups generated during the NH3-plasma, which interact with the precursor molecules during the precursor pulse. We propose that the reaction of these surface groups with the precursor leads to additional deposition of Ag atoms during the precursor pulse compared to the H-2-plasma process, which explains the enhanced growth rate of the NH3-plasma process.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000410868600012 Publication Date 2017-08-09
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 9.466 Times cited 9 Open Access
  Notes ; M.M.M. and J.D. acknowledge the Fonds Wetenschappelijk Onderzoek Vlaanderen (FWO Vlaanderen) for financial support through a personal research grant. We also acknowledge FWO Vlaanderen for providing project funding for this work. We are grateful to the ESRF staff for smoothly running the synchrotron and beamline facilities. We also thank Olivier Janssens for performing the SEM measurements and Stefaan Broekaert for mechanical assistance. J.A.M. acknowledges the Flemish Government for long-term structural funding (Methusalem). ; Approved Most recent IF: 9.466
  Call Number UA @ admin @ c:irua:146757 Serial 5983
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Author Marchetti, A.; Saniz, R.; Krishnan, D.; Rabbachin, L.; Nuyts, G.; De Meyer, S.; Verbeeck, J.; Janssens, K.; Pelosi, C.; Lamoen, D.; Partoens, B.; De Wael, K.
  Title Unraveling the Role of Lattice Substitutions on the Stabilization of the Intrinsically Unstable Pb2Sb2O7Pyrochlore: Explaining the Lightfastness of Lead Pyroantimonate Artists’ Pigments Type A1 Journal article
  Year 2020 Publication Chemistry Of Materials Abbreviated Journal Chem Mater
  Volume 32 Issue 7 Pages 2863-2873
  Keywords A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT)
  Abstract The pyroantimonate pigments Naples yellow and lead tin antimonate yellow are recognized as some of the most stable synthetic yellow pigments in the history of art. However, this exceptional lightfastness is in contrast with experimental evidence suggesting that this class of mixed oxides is of semiconducting nature. In this study the electronic structure and light-induced behavior of the lead pyroantimonate pigments were determined by means of a combined multifaceted analytical and computational approach (photoelectrochemical measurements, UV-vis diffuse reflectance spectroscopy, STEM-EDS, STEM-HAADF, and density functional theory calculations). The results demonstrate both the semiconducting nature and the lightfastness of these pigments. Poor optical absorption and minority carrier mobility are the main properties responsible for the observed stability. In addition, novel fundamental insights into the role played by Na atoms in the stabilization of the otherwise intrinsically unstable Pb2Sb2O7 pyrochlore were obtained.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000526394000016 Publication Date 2020-04-14
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 8.6 Times cited 8 Open Access OpenAccess
  Notes Universiteit Antwerpen; Belgian Federal Science Policy Office; Approved Most recent IF: 8.6; 2020 IF: 9.466
  Call Number EMAT @ emat @c:irua:168819 Serial 6363
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Author Imran, M.; Ramade, J.; Di Stasio, F.; De Franco, M.; Buha, J.; Van Aert, S.; Goldoni, L.; Lauciello, S.; Prato, M.; Infante, I.; Bals, S.; Manna, L.
  Title Alloy CsCdxPb1–xBr3Perovskite Nanocrystals: The Role of Surface Passivation in Preserving Composition and Blue Emission Type A1 Journal article
  Year 2020 Publication Chemistry Of Materials Abbreviated Journal Chem Mater
  Volume 32 Issue Pages acs.chemmater.0c03825
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract Various strategies have been proposed to engineer the band gap of metal halide perovskite nanocrystals (NCs) while preserving their structure and composition and thus ensuring spectral stability of the emission color. An aspect that has only been marginally investigated is how the type of surface passivation influences the structural/color stability of AMX3 perovskite NCs composed of two different M2+ cations. Here, we report the synthesis of blue-emitting Cs-oleate capped CsCdxPb1–xBr3 NCs, which exhibit a cubic perovskite phase containing Cd-rich domains of Ruddlesden–Popper phases (RP phases). The RP domains spontaneously transform into pure orthorhombic perovskite ones upon NC aging, and the emission color of the NCs shifts from blue to green over days. On the other hand, postsynthesis ligand exchange with various Cs-carboxylate or ammonium bromide salts, right after NC synthesis, provides monocrystalline NCs with cubic phase, highlighting the metastability of RP domains. When NCs are treated with Cs-carboxylates (including Cs-oleate), most of the Cd2+ ions are expelled from NCs upon aging, and the NCs phase evolves from cubic to orthorhombic and their emission color changes from blue to green. Instead, when NCs are coated with ammonium bromides, the loss of Cd2+ ions is suppressed and the NCs tend to retain their blue emission (both in colloidal dispersions and in electroluminescent devices), as well as their cubic phase, over time. The improved compositional and structural stability in the latter cases is ascribed to the saturation of surface vacancies, which may act as channels for the expulsion of Cd2+ ions from NCs.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000603288800034 Publication Date 2020-12-04
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 8.6 Times cited 44 Open Access OpenAccess
  Notes European Commission; Fonds Wetenschappelijk Onderzoek, G.0267.18N ; H2020 European Research Council, 770887 815128 851794 ; We acknowledge funding from the FLAG-ERA JTC2019 project PeroGas. S.B., and S.V.A. acknowledges funding from the European Research Council under the European Union’s Horizon 2020 research and innovation program (ERC Consolidator Grants #815128REALNANO and #770887PICOMETRICS) and from the Research Foundation Flanders (FWO, Belgium) through project funding G.0267.18N. F.D.S. acknowledges the funding from ERC starting grant NANOLED (851794). The computational work was carried out on the Dutch National e-infrastructure with the support of the SURF Cooperative; sygma Approved Most recent IF: 8.6; 2020 IF: 9.466
  Call Number EMAT @ emat @c:irua:174004 Serial 6659
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Author van der Sluijs, M.M.; Salzmann, B.B.V.; Arenas Esteban, D.; Li, C.; Jannis, D.; Brafine, L.C.; Laning, T.D.; Reinders, J.W.C.; Hijmans, N.S.A.; Moes, J.R.; Verbeeck, J.; Bals, S.; Vanmaekelbergh, D.
  Title Study of the Mechanism and Increasing Crystallinity in the Self-Templated Growth of Ultrathin PbS Nanosheets Type A1 Journal article
  Year 2023 Publication Chemistry of materials Abbreviated Journal
  Volume Issue Pages
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract Colloidal 2D semiconductor nanocrystals, the analogue of solid-state quantum wells, have attracted strong interest in material science and physics. Molar quantities of suspended quantum objects with spectrally pure absorption and emission can be synthesized. For the visible region, CdSe nanoplatelets with atomically precise thickness and tailorable emission have been (almost) perfected. For the near-infrared region, PbS nanosheets (NSs) hold strong promise, but the photoluminescence quantum yield is low and many questions on the crystallinity, atomic structure, intriguing rectangular shape, and formation mechanism remain to be answered. Here, we report on a detailed investigation of the PbS NSs prepared with a lead thiocyanate single source precursor. Atomically resolved HAADF-STEM imaging reveals the presence of defects and small cubic domains in the deformed orthorhombic PbS crystal lattice. Moreover, variations in thickness are observed in the NSs, but only in steps of 2 PbS monolayers. To study the reaction mechanism, a synthesis at a lower temperature allowed for the study of reaction intermediates. Specifically, we studied the evolution of pseudo-crystalline templates towards mature, crystalline PbS NSs. We propose a self-induced templating mechanism based on an oleylamine-lead-thiocyanate (OLAM-Pb-SCN) complex with two Pb-SCN units as a building block; the interactions between the long-chain ligands regulate the crystal structure and possibly the lateral dimensions.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000959572100001 Publication Date 2023-03-25
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 8.6 Times cited 2 Open Access OpenAccess
  Notes H2020 Research Infrastructures, 731019 ; H2020 European Research Council, 692691 815128 ; Nederlandse Organisatie voor Wetenschappelijk Onderzoek, 715.016.002 ; Approved Most recent IF: 8.6; 2023 IF: 9.466
  Call Number EMAT @ emat @c:irua:195894 Serial 7255
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Author Sa, J.; Hu, N.; Heyvaert, W.; Van Gordon, K.; Li, H.; Wang, L.; Bals, S.; Liz-Marzán, L.M.; Ni, W.
  Title Spontaneous Chirality Evolved at the Au–Ag Interface in Plasmonic Nanorods Type A1 Journal article
  Year 2023 Publication Chemistry of materials Abbreviated Journal Chem. Mater.
  Volume Issue Pages
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract Chiral ligands are considered a required ingredient during the synthesis of dissymmetric plasmonic metal nanocrystals. The mechanism behind the generation of chiral structures involves the formation of high Miller index chiral facets, induced by the adsorption of such chiral ligands. We found however that, chirality can also evolve spontaneously, without the involvement of any chiral ligands, during the co-deposition of Au and Ag on Au nanorods. When using a specific Au/Ag ratio, phase segregation of the two metals leads to an interface within the obtained AuAg shell, which can be exposed by removing the Ag component via oxidative etching. Although a close-to-racemic mixture of chiral Au nanorods with right and left handedness is found in solution, electron tomography analysis evidences left- and righthanded helicities, both at the Au-Ag interface and at the exposed surface of Au NRs after Ag etching. The helicity profile of the NRs indicates dominating inclination angles in a range from 30° to 60°. Single-particle optical characterization also reveals random handedness in the plasmonic response of individual nanorods. We hypothesize that, the origin of chirality is related with symmetry breaking during the co-deposition of Au and Ag, through an initial perturbation in a small region on the Au-Ag interface that eventually leads to chiral segregation throughout the nanocrystal.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 001052093300001 Publication Date 2023-08-21
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0897-4756 ISBN Additional Links UA library record; WoS full record
  Impact Factor 8.6 Times cited Open Access OpenAccess
  Notes The authors acknowledge the financial support from the National Natural Science Foundation of China (grant 22074102). LMLM acknowledges funding from 26 MCIN/AEI/10.13039/501100011033 and “ESF Investing in your future” (Grant PID2020- 117779RB-I00). This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 823717 – ESTEEM3.; Ministerio de Ciencia e Innovaci?n, PID2020-117779RB-I00 ; H2020 Research Infrastructures, 823717 ; European Social Fund, PID2020-117779RB-I00 ; National Natural Science Foundation of China, 22074102 ; Approved Most recent IF: 8.6; 2023 IF: 9.466
  Call Number EMAT @ emat @c:irua:198151 Serial 8810
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Author Vandemeulebroucke, D.; Batuk, M.; Hajizadeh, A.; Wastiaux, M.; Roussel, P.; Hadermann, J.
  Title Incommensurate Modulations and Perovskite Growth in LaxSr2–xMnO4−δAffecting Solid Oxide Fuel Cell Conductivity Type A1 Journal Article
  Year 2024 Publication Chemistry of Materials Abbreviated Journal Chem. Mater.
  Volume Issue Pages
  Keywords A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;
  Abstract Ruddlesden-Popper La????Sr2−????MnO4−???? materials are interesting symmetric solid oxide

fuel cell electrodes due to their good redox stability, mixed ionic and electronic conducting behavior and thermal expansion that matches well with common electrolytes. In reducing environments – as at a solid oxide fuel cell anode – the x = 0.5 member, i.e. La0.5Sr1.5MnO4−????, has a much higher total conductivity than compounds with a different La/Sr ratio, although all those compositions have the same K2NiF4-type I4/mmm structure. The origin for this conductivity difference is not yet known in literature. Now, a combination of in-situ and ex-situ 3D electron diffraction, high-resolution imaging, energy-dispersive X-ray analysis and electron energy-loss spectroscopy uncovered clear differences between x=0.25 and x=0.5 in the pristine structure, as well as in the transformations upon high-temperature reduction. In La0.5Sr1.5MnO4−????, Ruddlesden-Popper n=2 layer defects and an amorphous surface layer are present, but not in La0.25Sr1.75MnO4−????. After annealing at 700°C in 5% H2/Ar, La0.25Sr1.75MnO4−???? transforms to a tetragonal 2D incommensurately modulated structure with modulation vectors ⃗????1 = 0.2848(1) · (⃗????* +⃗????*) and ⃗????2 =0.2848(1) · (⃗????* – ⃗????*), whereas La0.5Sr1.5MnO4−???? only partially transforms to an orthorhombic 1D incommensurately modulated structure,

with ⃗???? = 0.318(2) · ⃗????*. Perovskite domains grow at the crystal edge at 700°C in 5%

H2 or vacuum, due to the higher La concentration on the surface compared to the bulk, which leads to a different thermodynamic equilibrium. Since it is known that a lower degree of oxygen vacancy ordering and a higher amount of perovskite blocks enhance oxygen mobility, those differences in defect structure and structural transformation upon reduction, might all contribute to the higher conductivity of La0.5Sr1.5MnO4−???? in solid oxide fuel cell anode conditions compared to other La/Sr ratios.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language English Wos 001174840900001 Publication Date 2024-02-20
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0897-4756 ISBN Additional Links UA library record; WoS full record
  Impact Factor 8.6 Times cited Open Access Not_Open_Access
  Notes Universiteit Antwerpen, BOF TOP 38689 ; Fonds Wetenschappelijk Onderzoek, I003218N ; European Commission NanED, 956099 ; Approved Most recent IF: 8.6; 2024 IF: 9.466
  Call Number EMAT @ emat @c:irua:204354 Serial 8997
Permanent link to this record
 

 
Author Ghica, C.; Nistor, L.; Bender, H.; Steegen, A.; Lauwers, A.; Maex, K.; van Landuyt, J.
  Title In situ transmission electron microscopy study of the silicidation process in Co thin films on patterned (001) Si substrates Type A1 Journal article
  Year 2001 Publication Journal of materials research Abbreviated Journal J Mater Res
  Volume 16 Issue 3 Pages 701-708
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract The results of an in situ transmission electron microscopy study of the formation of Co-silicides on patterned (001) Si substrates are discussed. It is shown that the results of the in situ heating experiments agreed very well with the data based on standard rapid thermal annealing experiments. Fast heating rates resulted in better definition of the silicide lines. Also, better lines were obtained for samples that received already a low-temperature ex situ anneal. A Ti cap layer gave rise to a higher degree of epitaxy in the CoSi2 silicide.
  Address
  Corporate Author Thesis
  Publisher Place of Publication New York, N.Y. Editor
  Language Wos 000167407200011 Publication Date 2008-03-06
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0884-2914;2044-5326; ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 1.673 Times cited 4 Open Access
  Notes Approved Most recent IF: 1.673; 2001 IF: 1.539
  Call Number UA @ lucian @ c:irua:103926 Serial 1588
Permanent link to this record
 

 
Author Lei, C.H.; Van Tendeloo, G.; Siegert, M.; Schubert, J.
  Title Microstructural investigation of BaTiO3 thin films deposited on (001) MgO Type A1 Journal article
  Year 2002 Publication Journal of materials research Abbreviated Journal J Mater Res
  Volume 17 Issue 8 Pages 1923-1931
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract The microstructure of BaTiO3 thin films, epitaxially deposited on (001) MgO by pulsed laser ablation, has been investigated by transmission electron microscopy. The films are always c-axis-orientated, but dislocations, {111} stacking faults, and antiphase boundaries are frequently observed. Conventional TEM and high-resolution microscopy allow one to deduce the Burgers vectors of dislocations as b(1) = <100> or b(2) = <110>, both being perfect dislocations. Most extrinsic stacking faults are ending at 1/3<112> or 1/3<111> partial dislocations; the displacement vector of the antiphase boundaries is 1/2<101>. Studying the interfacial structure by means of zone images taken along [100] and [110] shows that the misfit is mainly released by dislocations with Burgers vectors of 1/2<110> and 1/2<101>.
  Address
  Corporate Author Thesis
  Publisher Place of Publication New York, N.Y. Editor
  Language Wos 000177208800010 Publication Date 2008-03-06
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0884-2914;2044-5326; ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 1.673 Times cited 8 Open Access
  Notes Approved Most recent IF: 1.673; 2002 IF: 1.530
  Call Number UA @ lucian @ c:irua:103343 Serial 2044
Permanent link to this record
 

 
Author Ahonen, P.P.; Kauppinen, E.I.; Joubert, J.C.; Deschanvres, J.L.; Van Tendeloo, G.
  Title Preparation of nanocrystalline titania powder via aerosol pyrolysis of titanium tetrabutoxide Type A1 Journal article
  Year 1999 Publication Journal of materials research Abbreviated Journal J Mater Res
  Volume 14 Issue 10 Pages 3938-3948
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract Nanocrystalline titanium dioxide was prepared via aerosol pyrolysis of titanium alkoxide precursor at 200-580 degrees C in air and in nitrogen atmospheres. Powders were characterized by x-ray diffraction, thermogravimetric analysis, Brunauer-Emmett-Teller analysis, scanning electron microscopy, transmission electron microscopy, energy dispersive spectroscopy, x-ray fluorescence, Raman and infrared spectroscopy, and Berner-type low-pressure impactor. The anatase phase transition was initiated at 500 degrees C in nitrogen and at 580 degrees C in air. Under other conditions amorphous powders were observed and transformed to nanocrystalline TiO2 via thermal postannealing. In air, smooth and spherical particles with 2-4-mu m diameter were formed with an as-expected tendency to convert to rutile in the thermal postannealings. In nitrogen, a fraction of the titanium tetrabutoxide precursor evaporated and formed ultrafine particles via the gas-to-particle conversion. At 500 degrees C thermally stable anatase phase was formed in nitrogen. A specific surface area as high as 280 m(2) g(-1) was observed for an as-prepared powder.
  Address
  Corporate Author Thesis
  Publisher Place of Publication New York, N.Y. Editor
  Language Wos 000083163700019 Publication Date 2008-03-06
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0884-2914;2044-5326; ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 1.673 Times cited 38 Open Access
  Notes Approved Most recent IF: 1.673; 1999 IF: 1.574
  Call Number UA @ lucian @ c:irua:103485 Serial 2705
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Author Nistor, L.C.; Richard, O.; Zhao, C.; Bender, H.; Van Tendeloo, G.
  Title Thermal stability of atomic layer deposited Zr:Al mixed oxide thin films: an in situ transmission electron microscopy study Type A1 Journal article
  Year 2005 Publication Journal of materials research Abbreviated Journal J Mater Res
  Volume 20 Issue 7 Pages 1741-1750
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract
  Address
  Corporate Author Thesis
  Publisher Place of Publication New York, N.Y. Editor
  Language Wos 000230296100012 Publication Date 2005-07-12
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0884-2914;2044-5326; ISBN Additional Links UA library record; WoS full record
  Impact Factor 1.673 Times cited Open Access
  Notes Bil 01/73; IAP V-1 Approved Most recent IF: 1.673; 2005 IF: 2.104
  Call Number UA @ lucian @ c:irua:54884 Serial 3631
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Author Nistor, L.C.; van Landuyt, J.
  Title Structural studies of diamond thin films grown from the arc plasma Type A1 Journal article
  Year 1998 Publication Journal of materials research Abbreviated Journal J Mater Res
  Volume 12 Issue 10 Pages 2533-2542
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract
  Address
  Corporate Author Thesis
  Publisher Place of Publication New York, N.Y. Editor
  Language Wos A1997YD17000007 Publication Date 0000-00-00
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0884-2914 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 1.673 Times cited 13 Open Access
  Notes Approved Most recent IF: 1.673; 1998 IF: 1.539
  Call Number UA @ lucian @ c:irua:29674 Serial 3259
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Author Kahraman, Z.; Yagmurcukardes, M.; Sahin, H.
  Title Functionalization of single-layer TaS₂ and formation of ultrathin Janus structures Type A1 Journal article
  Year 2020 Publication Journal Of Materials Research Abbreviated Journal J Mater Res
  Volume 35 Issue 11 Pages 1397-1406
  Keywords A1 Journal article; Condensed Matter Theory (CMT)
  Abstract Ab initio calculations are performed to investigate the structural, vibrational, electronic, and piezoelectric properties of functionalized single layers of TaS2. We find that single-layer TaS2 is a suitable host material for functionalization via fluorination and hydrogenation. The one-side fluorinated (FTaS2) and hydrogenated (HTaS2) single layers display indirect gap semiconducting behavior in contrast to bare metallic TaS2. On the other hand, it is shown that as both surfaces of TaS2 are saturated anti-symmetrically, the formed Janus structure is a dynamically stable metallic single layer. In addition, it is revealed that out-of-plane piezoelectricity is created in all anti-symmetric structures. Furthermore, the Janus-type single-layer has the highest specific heat capacity to which longitudinal and transverse acoustical phonon modes have contribution at low temperatures. Our findings indicate that single-layer TaS2 is suitable for functionalization via H and F atoms that the formed, anti-symmetric structures display distinctive electronic, vibrational, and piezoelectric properties.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000540764300005 Publication Date 2020-04-08
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0884-2914 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 2.7 Times cited 1 Open Access
  Notes ; Computational resources were provided by TUBITAK ULAKBIM, High Performance and Grid Computing Center (TR-Grid e-Infrastructure). H.S. Acknowledges financial support from the TUBITAK under the project number 117F095. H.S. acknowledges support from Turkish Academy of Sciences under the GEBIP program. This work is supported by the Flemish Science Foundation (FWO-Vl) by a post-doctoral fellowship (M.Y.). ; Approved Most recent IF: 2.7; 2020 IF: 1.673
  Call Number UA @ admin @ c:irua:170185 Serial 6525
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Author Nistor, L.C.; van Landuyt, J.; Ralchenko, V.G.; Kononenko, T.V.; Obraztsova, E.D.; Strelnitsky, V.E.
  Title Direct observation of laser-induced crystallization of a-C : H films Type A1 Journal article
  Year 1994 Publication Applied physics A : materials science & processing Abbreviated Journal
  Volume 58 Issue 2 Pages 137-144
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract The post-growth modification of diamond-like amorphous hydrogenated carbon a-C:H films by laser treatment has been studied by transmission electron microscopy and Raman spectroscopy. a-C:H films grown on Si substrates by benzene decomposition in a rf glow discharge were irradiated with 15 ns pulses of a KrF-excimer laser with fluences in the ran e of E = 50-700 mJ/cm(2). At fluences below 100 mJ/cm(2) an increase in the number of graphitic clusters and in their ordering was evidenced from Raman spectra, while the film structure remained amorphous according to electron microscopy and electron diffraction observations. At higher fluences the appearance of diamond particles of 2-7 nm size, embedded into the lower crystallized graphitic matrix, was observed and simultaneously a progressive growth of graphite nanocrystals with dimensions from 2 nm to 4 nm was deduced from Raman measurements. The maximum thickness of the crystallized surface layer (approximate to 400 nm) and the degree of laser annealing are limited by the film ablation which starts at E > 250 mJ/cm(2). The laser-treated areas lose their chemical inertness. In particular, chemical etching in chromium acid becomes possible, which may be used for patterning the highly inert carbon films.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Heidelberg Editor
  Language Wos A1994MU87700005 Publication Date 2004-10-24
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0721-7250;1432-0630; ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor Times cited 73 Open Access
  Notes Approved no
  Call Number UA @ lucian @ c:irua:99924 Serial 718
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Author Cheng, K.; Leys, M.; Degroote, S.; van Daele, B.; Boeykens, S.; Derluyn, J.; Germain, M.; Van Tendeloo, G.; Engelen, J.; Borghs, G.
  Title Flat GaN epitaxial layers grown on Si(111) by metalorganic vapor phase epitaxy using step-graded AlGaN intermediate layers Type A1 Journal article
  Year 2006 Publication Journal of electronic materials Abbreviated Journal J Electron Mater
  Volume 35 Issue 4 Pages 592-598
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract
  Address
  Corporate Author Thesis
  Publisher Place of Publication Boston, Mass. Editor
  Language Wos 000237101800016 Publication Date 2007-04-16
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0361-5235;1543-186X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 1.579 Times cited 102 Open Access
  Notes Approved Most recent IF: 1.579; 2006 IF: 1.504
  Call Number UA @ lucian @ c:irua:58238 Serial 1223
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Author Callini, E.; Aguey-Zinsou, K.F.; Ahuja, R.; Ares, J.R.; Bals, S.; Biliškov, N.; Chakraborty, S.; Charalambopoulou, G.; Chaudhary, A.L.; Cuevas, F.; Dam, B.; de Jongh, P.; Dornheim, M.; Filinchuk, Y.; Grbović Novaković, J.; Hirscher, M.; Jensen, T.R.; Jensen, P.B.; Novaković, N.; Lai, Q.; Leardini, F.; Gattia, D.M.; Pasquini, L.; Steriotis, T.; Turner, S.; Vegge, T.; Züttel, A.; Montone, A.
  Title Nanostructured materials for solid-state hydrogen storage : a review of the achievement of COST Action MP1103 Type A1 Journal article
  Year 2016 Publication International journal of hydrogen energy T2 – E-MRS Fall Meeting / Symposium C on Hydrogen Storage in Solids -, Materials, Systems and Aplication Trends, SEP 15-18, 2015, Warsaw, POLAND Abbreviated Journal Int J Hydrogen Energ
  Volume 41 Issue 41 Pages 14404-14428
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
  Abstract In the framework of the European Cooperation in Science and Technology (COST) Action MP1103 Nanostructured Materials for Solid-State Hydrogen Storage were synthesized, characterized and modeled. This Action dealt with the state of the art of energy storage and set up a competitive and coordinated network capable to define new and unexplored ways for Solid State Hydrogen Storage by innovative and interdisciplinary research within the European Research Area. An important number of new compounds have been synthesized: metal hydrides, complex hydrides, metal halide ammines and amidoboranes. Tuning the structure from bulk to thin film, nanoparticles and nanoconfined composites improved the hydrogen sorption properties and opened the perspective to new technological applications. Direct imaging of the hydrogenation reactions and in situ measurements under operando conditions have been carried out in these studies. Computational screening methods allowed the prediction of suitable compounds for hydrogen storage and the modeling of the hydrogen sorption reactions on mono-, bi-, and three-dimensional systems. This manuscript presents a review of the main achievements of this Action. (C) 2016 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
  Address
  Corporate Author Thesis
  Publisher Pergamon-elsevier science ltd Place of Publication Oxford Editor
  Language Wos 000381950800051 Publication Date 2016-05-08
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0360-3199 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 3.582 Times cited 89 Open Access Not_Open_Access
  Notes All the authors greatly thank the COST Action MP1103 for financial support. Approved Most recent IF: 3.582
  Call Number UA @ lucian @ c:irua:135723 Serial 4307
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Author Van Tendeloo, G.; Lebedev, O.I.; Amelinckx, S.
  Title Atomic and microstructure of CMR materials Type A1 Journal article
  Year 2000 Publication Journal of magnetism and magnetic materials Abbreviated Journal J Magn Magn Mater
  Volume 211 Issue Pages 73-83
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract
  Address
  Corporate Author Thesis
  Publisher Place of Publication Amsterdam Editor
  Language Wos 000085772100013 Publication Date 2002-07-25
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN (down) 0304-8853; ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 2.63 Times cited 48 Open Access
  Notes Iuap 4-10 Approved Most recent IF: 2.63; 2000 IF: 0.996
  Call Number UA @ lucian @ c:irua:54773 Serial 165
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