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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. |
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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 |
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| |
Volume |
32 |
Issue |
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Pages |
acs.chemmater.0c03825 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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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. |
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Wos |
000603288800034 |
Publication Date |
2020-12-04 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
8.6 |
Times cited |
44 |
Open Access |
OpenAccess |
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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 #815128REALNANO and #770887PICOMETRICS) 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 |
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Call Number  |
EMAT @ emat @c:irua:174004 |
Serial |
6659 |
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| Permanent link to this record |
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Author |
Leemans, J.; Singh, S.; Li, C.; Ten Brinck, S.; Bals, S.; Infante, I.; Moreels, I.; Hens, Z. |
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Title |
Near-Edge Ligand Stripping and Robust Radiative Exciton Recombination in CdSe/CdS Core/Crown Nanoplatelets |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Journal Of Physical Chemistry Letters |
Abbreviated Journal |
J Phys Chem Lett |
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Volume |
11 |
Issue |
9 |
Pages |
3339-3344 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
We address the relation between surface chemistry and optoelectronic properties in semiconductor nanocrystals using core/crown CdSe/CdS nanoplatelets passivated by cadmium oleate (Cd(Ol)2) as model systems. We show that addition of butylamine to a nanoplatelet (NPL) dispersion maximally displaces ∼40% of the original Cd(Ol)2 capping. On the basis of density functional theory simulations, we argue that this behavior reflects the preferential displacement of Cd(Ol)2 from (near)-edge surface sites. Opposite from CdSe core NPLs, core/crown NPL dispersions can retain 45% of their initial photoluminescence efficiency after ligand displacement, while radiative exciton recombination keeps dominating the luminescent decay. Using electron microscopy observations, we assign this robust photoluminescence to NPLs with a complete CdS crown, which prevents charge carrier trapping in the near-edge surface sites created by ligand displacement. We conclude that Z-type ligands such as cadmium carboxylates can provide full electronic passivation of (100) facets yet are prone to displacement from (near)-edge surface sites. |
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Wos |
000535177500024 |
Publication Date |
2020-05-07 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1948-7185 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
5.7 |
Times cited |
24 |
Open Access |
OpenAccess |
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Notes |
Universiteit Gent, GOA 01G01019 ; Fonds Wetenschappelijk Onderzoek, 17006602 FWO17/PDO/184 ; H2020 European Research Council, 714876 Phocona 815128 Realnano ; SIM-Flanders, SBO-QDOCCO ; Z.H. and S.B. acknowledge support by SIM-Flanders (SBO-QDOCCO). Z.H. acknowledges support by FWO-Vlaanderen (research project 17006602). Z.H. and I.M. acknowledge support by Ghent University (GOA n◦ 01G01019). J.L. acknowledges FWO-vlaanderen for a fellowship (SB PhD fellow at FWO). Sh.S acknowledges FWO postdoctoral funding (FWO17/PDO/184). This project has further received funding from the European Research Counsil under the European Union’s Horizon 2020 research and innovation programme (ERC Consolidator grant no. 815128 REALNANO and starting grant no. 714876 PHOCONA).; sygma |
Approved |
Most recent IF: 5.7; 2020 IF: 9.353 |
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Call Number |
EMAT @ emat @c:irua:173994 |
Serial |
6657 |
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| Permanent link to this record |
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Author |
Albrecht, W.; Bals, S. |
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Title |
Fast Electron Tomography for Nanomaterials |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Journal Of Physical Chemistry C |
Abbreviated Journal |
J Phys Chem C |
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Volume |
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Issue |
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Pages |
acs.jpcc.0c08939 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Electron tomography (ET) has become a well-established technique to visualize nanomaterials in three dimensions. A vast richness in information can be gained by ET, but the conventional acquisition of a tomography series is an inherently slow process on the order of 1 h. The slow acquisition limits the applicability of ET for monitoring dynamic processes or visualizing nanoparticles, which are sensitive to the electron beam. In this Perspective, we summarize recent work on the development of emerging experimental and computational schemes to enhance the data acquisition process. We particularly focus on the application of these fast ET techniques for beam-sensitive materials and highlight insight into dynamic transformations of nanoparticles under external stimuli, which could be gained by fast in situ ET. Moreover, we discuss challenges and possible solutions for simultaneously increasing the speed and quality of fast ET. |
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Wos |
000608876900003 |
Publication Date |
2020-11-27 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.7 |
Times cited |
26 |
Open Access |
OpenAccess |
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Notes |
H2020 Research Infrastructures, 823717 ; H2020 European Research Council, 815128 ; The authors acknowledge funding from the European Research Council under the European Union’s Horizon 2020 research and innovation program (ERC Consolidator Grant No. 815128-REALNANO) and the European Commission (EUSMI). The authors furthermore acknowledge funding from the European Union’s Horizon 2020 research and innovation program, ESTEEM3. The authors also acknowledge contributions from all co-workers that have contributed over the years: J. Batenburg and co-workers, A. Béché, E. Bladt, L. Liz-Marzán and co-workers, H. Pérez Garza and co-workers, A. Skorikov, S. Skrabalak and co-workers, S. Van Aert, A. van Blaaderen and co-workers, H. Vanrompay, and J. Verbeeck.; sygma |
Approved |
Most recent IF: 3.7; 2020 IF: 4.536 |
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Call Number |
EMAT @ emat @c:irua:173965 |
Serial |
6656 |
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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. |
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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 |
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Year |
2020 |
Publication |
Chemistry Of Materials |
Abbreviated Journal |
Chem Mater |
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Volume |
32 |
Issue |
7 |
Pages |
2863-2873 |
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Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT) |
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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. |
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Wos |
000526394000016 |
Publication Date |
2020-04-14 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
8.6 |
Times cited |
8 |
Open Access |
OpenAccess |
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Notes |
Universiteit Antwerpen; Belgian Federal Science Policy Office; |
Approved |
Most recent IF: 8.6; 2020 IF: 9.466 |
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Call Number |
EMAT @ emat @c:irua:168819 |
Serial |
6363 |
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Author |
Paul, S.; Bladt, E.; Richter, A.F.; Döblinger, M.; Tong, Y.; Huang, H.; Dey, A.; Bals, S.; Debnath, T.; Polavarapu, L.; Feldmann, J. |
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Title |
Manganese‐Doping‐Induced Quantum Confinement within Host Perovskite Nanocrystals through Ruddlesden–Popper Defects |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Angewandte Chemie-International Edition |
Abbreviated Journal |
Angew Chem Int Edit |
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Volume |
59 |
Issue |
17 |
Pages |
6794-6799 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
The concept of doping Mn2+ ions into II–VI semiconductor nanocrystals (NCs) was recently extended to perovskite NCs. To date, most studies on Mn2+ doped NCs focus on enhancing the emission related to the Mn2+ dopant via an energy transfer mechanism. Herein, we found that the doping of Mn2+ ions into CsPbCl3 NCs not only results in a Mn2+‐related orange emission, but also strongly influences the excitonic properties of the host NCs. We observe for the first time that Mn2+ doping leads to the formation of Ruddlesden–Popper (R.P.) defects and thus induces quantum confinement within the host NCs. We find that a slight doping with Mn2+ ions improves the size distribution of the NCs, which results in a prominent excitonic peak. However, with increasing the Mn2+ concentration, the number of R.P. planes increases leading to smaller single‐crystal domains. The thus enhanced confinement and crystal inhomogeneity cause a gradual blue shift and broadening of the excitonic transition, respectively. |
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Corporate Author |
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Place of Publication |
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Wos |
000525279800024 |
Publication Date |
2020-04-20 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1433-7851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
16.6 |
Times cited |
64 |
Open Access |
OpenAccess |
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Notes |
Deutsche Forschungsgemeinschaft, EXC 2089/1-390776260 ; H2020 European Research Council, 815128-REALNANO ; Horizon 2020 Framework Programme, 839042 731019 ; Alexander von Humboldt-Stiftung; We acknowledge financial support by the Bavarian State Ministry of Science, Research, and Arts through the grant “Solar Technologies go Hybrid (SolTech)”, the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germanys Excellence Strategy—EXC 2089/1‐390776260 (“e‐conversion”), the Alexander von Humboldt Foundation (A.D. and T.D.), the European Union's Horizon 2020 research and innovation program under the Marie Sklodowska‐Curie grant agreement No. 839042 (H.H.). E.B. acknowledges a postdoctoral grant 12T2719N from the Research Foundation Flanders (FWO, Belgium). E.B. and S.B. acknowledge the financial support from the European Research Council ERC Consolidator Grants #815128‐REALNANO. L.P. thanks the EU Infrastructure Project EUSMI (European Union's Horizon 2020, grant No 731019). We thank local research center “Center for NanoScience (CeNS)” for providing communicative networking structure. We acknowledge the funding of Nanosystems Initiative Munich (NIM) for color figures.; sygma |
Approved |
Most recent IF: 16.6; 2020 IF: 11.994 |
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Call Number |
EMAT @ emat @c:irua:168535 |
Serial |
6399 |
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Author |
Canossa, S.; Gonzalez-Nelson, A.; Shupletsov, L.; Carmen Martin, M.; Van der Veen, M.A. |
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Title |
Overcoming Crystallinity Limitations of Aluminium Metal-Organic Frameworks by Oxalic Acid Modulated Synthesis |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Chemistry-A European Journal |
Abbreviated Journal |
Chem-Eur J |
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Volume |
26 |
Issue |
16 |
Pages |
3564-3570 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
A modulated synthesis approach based on the chelating properties of oxalic acid (H2C2O4) is presented as a robust and versatile method to achieve highly crystalline Al‐based metal‐organic frameworks. A comparative study on this method and the already established modulation by hydrofluoric acid was conducted using MIL‐53 as test system. The superior performance of oxalic acid modulation in terms of crystallinity and absence of undesired impurities is explained by assessing the coordination modes of the two modulators and the structural features of the product. The validity of our approach was confirmed for a diverse set of Al‐MOFs, namely X‐MIL‐53 (X=OH, CH3O, Br, NO2), CAU‐10, MIL‐69, and Al(OH)ndc (ndc=1,4‐naphtalenedicarboxylate), highlighting the potential benefits of extending the use of this modulator to other coordination materials. |
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Corporate Author |
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Thesis |
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Place of Publication |
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Wos |
000517650300001 |
Publication Date |
2020-03-18 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0947-6539 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.3 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
The Elettra Synchrotron facility (CNR Trieste, Basovizza, Italy) is acknowledged for granting beamtime at the single-crystal diffraction beamline XRD1 (Proposal ID 20185483) and the beamline staff is gratefully thanked for the precious assistance. This work was funded by the European Research Council (grant number 759 212) within the Horizon 2020 Framework Programme (H2020-EU.1.1). The work by A.G.-N. forms part of the research programme of DPI, NEWPOL project 731.015.506. |
Approved |
Most recent IF: 4.3; 2020 IF: 5.317 |
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Call Number |
EMAT @ emat @c:irua:167706 |
Serial |
6388 |
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Author |
Hendrickx, M.; Tang, Y.; Hunter, E.C.; Battle, P.D.; Cadogan, Jm.; Hadermann, J. |
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Title |
CaLa2FeCoSbO9 and ALa2FeNiSbO9 (A = Ca, Sr, Ba): cation-ordered, inhomogeneous, ferrimagnetic perovskites |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Journal Of Solid State Chemistry |
Abbreviated Journal |
J Solid State Chem |
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Volume |
285 |
Issue |
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Pages |
121226 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Polycrystalline samples of CaLa2FeCoSbO9 and ALa2FeNiSbO9 (A=Ca, Sr, Ba) have been prepared in solid-state reactions and studied by a combination of transmission electron microscopy, magnetometry, X-ray diffraction, neutron diffraction and Mössbauer spectroscopy. Diffraction and TEM showed that each shows 1:1 B-site ordering in which Co2+/Ni2+ and Sb5+ tend to occupy two distinct crystallographic sites while Fe3+ is distributed over both sites. While X-ray and neutron diffraction agreed that all four compositions are monophasic with space group P21/n, TEM revealed different levels of compositional inhomogeneity at the subcrystal scale, which, in the case of BaLa2FeNiSbO9, leads to the occurrence of both a P21/n and an I2/m phase. Magnetometry and neutron diffraction show that these perovskites are ferrimagnets with a G-type magnetic structure. Their relatively low magnetisation can be attributed to their inhomogeneity. This work demonstrates the importance of studying the microstructure of complex compositions. |
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Place of Publication |
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Language |
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Wos |
000521107900017 |
Publication Date |
2020-01-30 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0022-4596 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.3 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
PDB, ECH, and JH acknowledge support from EPSRC under grant EP/M0189954/1. We would also like to thank E. Suard at ILL and I. Da Silva at ISIS for the experimental assistance they provided. |
Approved |
Most recent IF: 3.3; 2020 IF: 2.299 |
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Call Number |
EMAT @ emat @c:irua:167137 |
Serial |
6345 |
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Author |
Smith, J.D.; Bladt, E.; Burkhart, J.A.C.; Winckelmans, N.; Koczkur, K.M.; Ashberry, H.M.; Bals, S.; Skrabalak, S.E. |
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Title |
Defect‐Directed Growth of Symmetrically Branched Metal Nanocrystals |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Angewandte Chemie (International ed. Print) |
Abbreviated Journal |
Angew. Chem. |
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Volume |
132 |
Issue |
132 |
Pages |
953-960 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Branched plasmonic nanocrystals (NCs) have attracted much attention due to electric field enhancements at their tips. Seeded growth provides routes to NCs with defined branching patterns and, in turn, near‐field distributions with defined symmetries. Here, a systematic analysis was undertaken in which seeds containing different distributions of planar defects were used to grow branched NCs in order to understand how their distributions direct the branching. Characterization of the products by multimode electron tomography and analysis of the NC morphologies at different overgrowth stages indicate that the branching patterns are directed by the seed defects, with the emergence of branches from the seed faces consistent with minimizing volumetric strain energy at the expense of surface energy. These results contrast with growth of branched NCs from single‐crystalline seeds and provide a new platform for the synthesis of symmetrically branched plasmonic NCs. |
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Place of Publication |
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Language |
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Wos |
000505279500063 |
Publication Date |
2020-01-07 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0044-8249 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
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Times cited |
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Open Access |
OpenAccess |
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Notes |
The authors thank Samantha Harvey for her initial observations of branched structures, Alexander Chen for his help with SAED, the staff of the Nanoscale Characterization Facility (Dr. Yi Yi),Electron Microscopy Center (Dr. David Morgan and Dr. Barry Stein), and Molecular Strucre Center at Indiana University. J.S. recognizes a fellowship provided by the Indiana Space Grant Consortium. E. B. acknowledges a post-doctoral grant from the Research Foundation Flanders (FWO, Belgium). This project has received funding from the National Science Foundation (award number: 1602476), Research Corporation for Scietific Advancement (2017 Frontiers in Research Excellence and Discovery Award), and the European Union’s Horizon 2020 research and innovation program under grant agreement No 731019 (EUSMI) and No 815128 (REALNANO).; sygma |
Approved |
Most recent IF: NA |
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Call Number |
EMAT @ emat @c:irua:166581 |
Serial |
6336 |
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Author |
González-Rubio, G.; Milagres de Oliveira, T.; Albrecht, W.; Díaz-Núñez, P.; Castro-Palacio, J.C.; Prada, A.; González, R.I.; Scarabelli, L.; Bañares, L.; Rivera, A.; Liz-Marzán, L.M.; Peña-Rodríguez, O.; Bals, S.; Guerrero-Martínez, A. |
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Title |
Formation of Hollow Gold Nanocrystals by Nanosecond Laser Irradiation |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Journal Of Physical Chemistry Letters |
Abbreviated Journal |
J Phys Chem Lett |
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Volume |
11 |
Issue |
11 |
Pages |
670-677 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
The irradiation of spherical gold nanoparticles (AuNPs) with nanosecond laser pulses induces shape transformations yielding nanocrystals with an inner cavity. The concentration of the stabilizing surfactant, the use of moderate pulse fluences, and the size of the irradiated AuNPs determine the efficiency of the process and the nature of the void. Hollow nanocrystals are obtained when molecules from the surrounding medium (e.g., water and organic matter derived from the surfactant) are trapped during laser pulse irradiation. These experimental observations suggest the existence of a subtle balance between the heating and cooling processes experienced by the nanocrystals, which induce their expansion and subsequent recrystallization keeping exogenous matter inside. The described approach provides valuable insight into the mechanism of interaction of pulsed nanosecond laser with AuNPs, along with interesting prospects for the development of hollow plasmonic nanoparticles with potential applications related to gas and liquid storage at the nanoscale. |
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Place of Publication |
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Editor |
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Language |
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Wos |
000512223400012 |
Publication Date |
2020-02-06 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1948-7185 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
5.7 |
Times cited |
15 |
Open Access |
OpenAccess |
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Notes |
This work has been funded by the Spanish Ministry of Science, Innovation and Universities (MICIU) (Grants RTI2018-095844-B-I00, PGC2018-096444-B-I00, ENE2015-70300-C3-3, and MAT2017-86659-R), the EUROfusion Consortium (Grant ENR-IFE19.CCFE-01) and the Madrid Regional Government (Grants P2018/NMT-4389 and P2018/EMT-4437). This project has received funding from the European Commission (grant 731019, EUSMI & grant 823717, ESTEEM3). The publication is based also upon work from COST Action TUMIEE (CA17126). The facilities provided by the Center for Ultrafast Lasers at Complutense University of Madrid are gratefully acknowledged. The authors also acknowledge the computer resources and technical assistance provided by the Centro de Supercomputacion y Visualizacion de Madrid (CeSViMa). L.M.L.-M. acknowledges the Maria de Maeztu Units of Excellence Program from the Spanish State Research Agency (Grant MDM-2017-0720). This project has also received funding from the European Research Council (ERC Consolidator Grant 815128, REALNANO). W.A. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020 program (Grant 797153, SOPMEN). A.P. and R.I.G. acknowledge the support of FONDECYT under Grants 3190123 and 11180557 and Financiamiento Basal para Centros Cientificos y Tecnologicos de Excelencia FB-0807. This research was partially supported by the supercomputing infrastructure of the NLHPC (ECM-02).; sygma; esteem3JRA; esteem3reported |
Approved |
Most recent IF: 5.7; 2020 IF: 9.353 |
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| |
Call Number |
EMAT @ emat @c:irua:166504 |
Serial |
6334 |
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| Permanent link to this record |
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Author |
Rumyantseva, M.N.; Vladimirova, S.A.; Platonov, V.B.; Chizhov, A.S.; Batuk, M.; Hadermann, J.; Khmelevsky, N.O.; Gaskov, A.M. |
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Title |
Sub-ppm H2S sensing by tubular ZnO-Co3O4 nanofibers |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Sensors And Actuators B-Chemical |
Abbreviated Journal |
Sensor Actuat B-Chem |
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| |
Volume |
307 |
Issue |
|
Pages |
127624 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Tubular ZnO – Co3O4 nanofibers were co-electrospun from polymer solution containing zinc and cobalt acetates. Phase composition, cobalt electronic state and element distribution in the fibers were investigated by XRD, SEM, HRTEM, HAADF-STEM with EDX mapping, and XPS. Bare ZnO has high selective sensitivity to NO and NO2, while ZnO-Co3O4 composites demonstrate selective sensitivity to H2S in dry and humid air. This effect is discussed in terms of transformation of cobalt oxides into cobalt sulfides and change in the acidity of ZnO oxide surface upon cobalt doping. Reduction in response and recovery time is attributed to the formation of a tubular structure facilitating gas transport through the sensitive layer. |
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Corporate Author |
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Place of Publication |
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Language |
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Wos |
000508110400059 |
Publication Date |
2019-12-24 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0925-4005 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
5.401 |
Times cited |
|
Open Access |
Not_Open_Access |
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| |
Notes |
This work was supported by RFBR grants No. 18-03-00091 and No. 18-03-00580. |
Approved |
Most recent IF: NA |
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| |
Call Number |
EMAT @ emat @c:irua:166449 |
Serial |
6343 |
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| Permanent link to this record |
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Author |
Chin, C.–M.; Battle, P.D.; Hunter, E.C.; Avdeev, M.; Hendrickx, M.; Hadermann, J. |
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Title |
Magnetic properties of La3Ni2Sb Ta Nb1––O9; from relaxor to spin glass |
Type |
A1 Journal article |
| |
Year |
2019 |
Publication |
Journal of solid state chemistry (Print) |
Abbreviated Journal |
Journal of Solid State Chemistry |
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| |
Volume |
273 |
Issue |
|
Pages |
175-185 |
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| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Neutron diffraction experiments conducted at 5 K in a magnetic field 0 < H/kOe < 50 have shown that the monoclinic perovskite La3Ni2TaO9 behaves as a relaxor ferromagnet. Compositions in the series La3Ni2SbxTayNb1–x–yO9 have been synthesized in polycrystalline form. Electron microscopy, X–ray diffraction and neutron diffraction have shown that the solid solutions are largely homogeneous and monophasic. Magnetometry and neutron diffraction have shown that the relaxor magnetisation persists in low fields when x + y = 1 but is rapidly diminished by the introduction of niobium. This change in magnetic behaviour is ascribed to the differences in the d–orbital energies of Sb5+, Nb5+ and Ta5+. |
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Wos |
000466261100026 |
Publication Date |
2019-03-02 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0022-4596 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
|
Times cited |
|
Open Access |
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Notes |
We thank EPSRC for funding through grant EP/M0189541. CMC thanks the Croucher Foundation and the University of Oxford for the award of a graduate scholarship. |
Approved |
no |
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| |
Call Number |
EMAT @ emat @c:irua:166445 |
Serial |
6346 |
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| Permanent link to this record |
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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. |
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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 |
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| |
Volume |
32 |
Issue |
32 |
Pages |
557-565 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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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. |
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Corporate Author |
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Thesis |
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Place of Publication |
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Editor |
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Language |
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Wos |
000507721600056 |
Publication Date |
2019-12-13 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
9.466 |
Times cited |
39 |
Open Access |
OpenAccess |
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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 |
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| |
Call Number |
EMAT @ emat @c:irua:165234 |
Serial |
5438 |
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| Permanent link to this record |
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Author |
Gvozdetskyi, V.; Bhaskar, G.; Batuk, M.; Zhao, X.; Wang, R.; Carnahan, S.L.; Hanrahan, M.P.; Ribeiro, R.A.; Canfield, P.C.; Rossini, A.J.; Wang, C.-Z.; Ho, K.-M.; Hadermann, J.; Zaikina, J.V. |
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Title |
Computationally Driven Discovery of a Family of Layered LiNiB Polymorphs |
Type |
A1 Journal article |
| |
Year |
2019 |
Publication |
Angewandte Chemie: international edition in English |
Abbreviated Journal |
Angew Chem Int Edit |
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| |
Volume |
58 |
Issue |
44 |
Pages |
15855-15862 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Two novel lithium nickel boride polymorphs RT-LiNiB and HT-LiNiB with layered crystal structures are reported. This family of compounds was theoretically predicted by using the adaptive genetic algorithm (AGA) and subsequently synthesized via a hydride route with LiH precursor as a lithium source. Being unique among the known ternary transition metal borides, the LiNiB structures feature Li layers alternating with nearly planar [NiB] layers, composed of Ni hexagonal rings centered by B-B pairs. A comprehensive study using a combination of single crystal/synchrotron powder X-ray diffraction data, solid-state 7Li and 11B NMR, scanning transmission electron microscopy, quantum chemistry calculations, and magnetism has shed light on the intrinsic features of these polymorphic compounds. The unique layered structures of LiNiB compounds make them ultimate precursors to further study their exfoliation, paving a way toward two-dimensional transition metal borides, MBenes. |
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Corporate Author |
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Thesis |
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Place of Publication |
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Language |
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Wos |
000491219600038 |
Publication Date |
2019-10-28 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1433-7851 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
11.994 |
Times cited |
|
Open Access |
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Notes |
the Gordon and Betty Moore Foundation’s EPiQS Initiative through Grant GBMF4411. The Ames Laboratory is operated for the U.S. Department of Energy by Iowa State University under contract #DE-AC02-07CH11358. Use of the Advanced Photon Source at 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. |
Approved |
Most recent IF: 11.994 |
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Call Number |
EMAT @ emat @c:irua:164752 |
Serial |
5433 |
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| Permanent link to this record |
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Author |
Jin, L.; Batuk, M.; Kirschner, F.K.K.; Lang, F.; Blundell, S.J.; Hadermann, J.; Hayward, M.A. |
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Title |
Exsolution of SrO during the Topochemical Conversion of LaSr3CoRuO8to the Oxyhydride LaSr3CoRuO4H4 |
Type |
A1 Journal article |
| |
Year |
2019 |
Publication |
Inorganic chemistry |
Abbreviated Journal |
Inorg Chem |
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| |
Volume |
58 |
Issue |
21 |
Pages |
14863-14870 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Reaction of the n = 1 Ruddlesden-Popper oxide LaSr3CoRuO8 with CaH2 yields the oxyhydride phase LaSr3CoRuO4H4 via topochemical anion-exchange. Close inspection of X-ray and neutron powder diffraction data in combination with HAADF-STEM images reveals that nanoparticles of SrO are exsolved from the system during the reaction, with the change in cation stoichiometry accommodated by the inclusion of n > 1 (Co/Ru)nOn+1H2n ‘perovskite’ layers into the Ruddlesden-Popper stacking sequence. This novel pseudo-topochemical process offers a new route for the formation of n > 1 Ruddlesden-Popper structured materials. Magnetization data are consistent with a LaSr3Co1+Ru2+O4H4 (Co1+, d8, S = 1; Ru2+, d6, S = 0) oxidation/spin state combination. Neutron diffraction and μ+SR data show no evidence for long-range magnetic order down to 2 K, suggesting the diamagnetic Ru2+ centers impede the Co-Co magnetic exchange interactions. |
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Corporate Author |
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Thesis |
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Place of Publication |
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Language |
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Wos |
000494894400062 |
Publication Date |
2019-11-04 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0020-1669 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.857 |
Times cited |
1 |
Open Access |
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Notes |
We thank P. Manuel for assistance collecting the neutron powder diffraction data. We thank The Leverhulme Trust grant award RPG-2014-366 “Topochemical reduction of 4d and 5d transition metal oxides” for supporting this work. Experiments at the Diamond Light Source were performed as part of the Block Allocation Group award “Oxford Solid State Chemistry BAG to probe composition-structure-property relationships in solids” (EE13284). Investigation by TEM was supported through the FWO grant G035619N. |
Approved |
Most recent IF: 4.857 |
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| |
Call Number |
EMAT @ emat @c:irua:164625 |
Serial |
5434 |
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| Permanent link to this record |
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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. |
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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 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
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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. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Wos |
000502418000010 |
Publication Date |
2019-11-11 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
6 |
Open Access |
OpenAccess |
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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 |
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Call Number |
EMAT @ emat @c:irua:164056 |
Serial |
5380 |
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Author |
Choudhary, K.; Bercx, M.; Jiang, J.; Pachter, R.; Lamoen, D.; Tavazza, F. |
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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 |
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Volume |
31 |
Issue |
15 |
Pages |
5900-5908 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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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. |
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Corporate Author |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000480826900060 |
Publication Date |
2019-08-13 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
6 |
Open Access |
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Notes |
; ; |
Approved |
Most recent IF: 9.466 |
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Call Number |
EMAT @ emat @c:irua:161814 |
Serial |
5291 |
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Author |
Barreca, D.; Gri, F.; Gasparotto, A.; Altantzis, T.; Gombac, V.; Fornasiero, P.; Maccato, C. |
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Title |
Insights into the Plasma-Assisted Fabrication and Nanoscopic Investigation of Tailored MnO2Nanomaterials |
Type |
A1 Journal Article |
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Year |
2018 |
Publication |
Inorganic Chemistry |
Abbreviated Journal |
Inorg Chem |
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Volume |
57 |
Issue |
23 |
Pages |
14564-14573 |
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Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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Abstract |
Among transition metal oxides, MnO2 is of considerable importance for various technological end-uses,from heterogeneous catalysis to gas sensing, owing to its
structural flexibility and unique properties at the nanoscale. In this work, we demonstrate the successful fabrication of supported MnO2 nanomaterials by a catalyst-free, plasmaassisted process starting from a fluorinated manganese(II)
molecular source in Ar/O2 plasmas. A thorough multitechnique characterization aimed at the systematic investigation of material structure, chemical composition, and
morphology revealed the formation of F-doped, oxygendeficient, MnO2-based nanomaterials, with a fluorine content tunable as a function of growth temperature (TG). Whereas phase-pure β-MnO2 was obtained for 100 °C ≤ TG ≤ 300 °C, the formation of mixed phase MnO2 + Mn2O3 nanosystems took place at 400 °C. In addition, the system nano-organization could be finely tailored, resulting in a controllable evolution from wheat-ear columnar arrays to high aspect ratio pointed-tip nanorod assemblies. Concomitantly, magnetic force microscopy analyses suggested the formation of spin domains with features dependent on material morphology. Preliminary tests in Vislight activated photocatalytic degradation of rhodamine B aqueous solutions pave the way to possible applications of the target materials in wastewater purification. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000452344400016 |
Publication Date |
2018-12-03 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0020-1669 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.857 |
Times cited |
|
Open Access |
Not_Open_Access |
|
| |
Notes |
The present work was financially supported by Padova University DOR 2016−2018 and P-DiSC #03BIRD2016- UNIPD projects. T.A. acknowledges a postdoctoral grant from the Research Foundation Flanders (FWO). Thanks are also due to Prof. Sara Bals (EMAT, University of Antwerp, Belgium) and to Dr. Giorgio Carraro (Department of Chemical Sciences, Padova University, Italy) for valuable support and experimental assistance. |
Approved |
Most recent IF: 4.857 |
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| |
Call Number |
EMAT @ emat @c:irua:156245 |
Serial |
5147 |
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| Permanent link to this record |
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Author |
Hasanli, N.; Gauquelin, N.; Verbeeck, J.; Hadermann, J.; Hayward, M.A. |
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| |
Title |
Small-moment paramagnetism and extensive twinning in the topochemically reduced phase Sr2ReLiO5.5 |
Type |
A1 Journal article |
| |
Year |
2018 |
Publication |
Journal of the Chemical Society : Dalton transactions |
Abbreviated Journal |
Dalton T |
|
| |
Volume |
47 |
Issue |
44 |
Pages |
15783-15790 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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| |
Abstract |
Reaction of the cation-ordered double perovskite Sr2ReLiO6 with dilute hydrogen at 475 degrees C leads to the topochemical deintercalation of oxide ions from the host lattice and the formation of a phase of composition Sr2ReLiO5.5, as confirmed by thermogravimetric and EELS data. A combination of neutron and electron diffraction data reveals the reduction process converts the -Sr2O2-ReLiO4-Sr2O2-ReLiO4- stacking sequence of the parent phase into a -Sr2O2-ReLiO3-Sr2O2-ReLiO4-, partially anion-vacant ordered sequence. Furthermore a combination of electron diffraction and imaging reveals Sr2ReLiO5.5 exhibits extensive twinning – a feature which can be attributed to the large, anisotropic volume expansion of the material on reduction. Magnetisation data reveal a strongly reduced moment of (eff) = 0.505(B) for the d(1) Re6+ centres in the phase, suggesting there remains a large orbital component to the magnetism of the rhenium centres, despite their location in low symmetry coordination environments. |
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Place of Publication |
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Language |
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Wos |
000450208000019 |
Publication Date |
2018-10-18 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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| |
ISSN |
1477-9226 |
ISBN |
|
Additional Links |
UA library record; WoS full record |
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| |
Impact Factor |
4.029 |
Times cited |
|
Open Access |
Not_Open_Access |
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Notes |
Experiments at the Diamond Light Source were performed as part of the Block Allocation Group award “Oxford Solid State Chemistry BAG to probe composition-structure-property relationships in solids” (EE13284). Experiments at the ISIS pulsed neutron facility were supported by a beam time allocation from the STFC. NH acknowledges funding from the “State Programme on Education of Azerbaijani Youth Abroad in 2007-2015” by the Ministry of Education of Azerbaijan. J. V. and N. G. acknowledge funding through the GOA project “Solarpaint” of the University of Antwerp. The microscope used in this work was partly funded by the Hercules Fund from the Flemish Government. |
Approved |
Most recent IF: 4.029 |
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| |
Call Number |
EMAT @ emat @c:irua:155771 |
Serial |
5137 |
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| Permanent link to this record |
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| |
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Author |
Serrano-Sevillano, J.; Reynaud, M.; Saracibar, A.; Altantzis, T.; Bals, S.; van Tendeloo, G.; Casas-Cabanas, M. |
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| |
Title |
Enhanced electrochemical performance of Li-rich cathode materials through microstructural control |
Type |
A1 Journal article |
| |
Year |
2018 |
Publication |
Physical chemistry, chemical physics |
Abbreviated Journal |
Phys Chem Chem Phys |
|
| |
Volume |
20 |
Issue |
20 |
Pages |
23112-23122 |
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| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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| |
Abstract |
The microstructural complexity of Li-rich cathode materials has so far hampered understanding the critical link between size, morphology and structural defects with both capacity and voltage fadings that this family of materials exhibits. Li2MnO3 is used here as a model material to extract reliable structure–property
relationships that can be further exploited for the development of high-performing and long-lasting Li-rich oxides. A series of samples with microstructural variability have been prepared and thoroughly characterized using the FAULTS software, which allows quantification of planar defects and extraction of
average crystallite sizes. Together with transmission electron microscopy (TEM) and density functional theory (DFT) results, the successful application of FAULTS analysis to Li2MnO3 has allowed rationalizing the synthesis conditions and identifying the individual impact of concurrent microstructural features on
both voltage and capacity fadings, a necessary step for the development of high-capacity Li-ion cathode materials with enhanced cycle life. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000445220500071 |
Publication Date |
2018-08-24 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
|
Edition |
|
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| |
ISSN |
1463-9076 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
4.123 |
Times cited |
36 |
Open Access |
OpenAccess |
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| |
Notes |
This work was supported by the Spanish Ministerio de la Economı´a y de la Competitividad through the project IONSTORE (MINECO ref. ENE2016-81020-R). The research leading to these results has received funding from the European Union Seventh Framework Programme under Grant Agreement 312483 – ESTEEM2 (Integrated Infrastructure Initiative-I3). JSS and AS are grateful for computing time provided by the Spanish i2Basque Centers. MR acknowledges the Spanish State for its financial support through her post-doctoral grant Juan de la Cierva – Formacio´n (MINECO ref. FJCI-2014-19990) and her international mobility grant Jose´ Castillejos (MECD ref. CAS15/00354). S. B. acknowledges funding from the European Research Council (ERC starting grant #335078 Colouratom) and T. A. a postdoctoral grant from the Research Foundation Flanders (FWO). (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:cannot); ecas_sara |
Approved |
Most recent IF: 4.123 |
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| |
Call Number |
EMAT @ emat @c:irua:154782UA @ admin @ c:irua:154782 |
Serial |
5062 |
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| Permanent link to this record |
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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. |
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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 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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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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Corporate Author |
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Place of Publication |
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Editor |
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Language |
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Wos |
000440105500042 |
Publication Date |
2018-07-24 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
|
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| |
ISSN |
0897-4756 |
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 |
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| |
Call Number |
EMAT @ emat @c:irua:152997UA @ admin @ c:irua:152997 |
Serial |
5011 |
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| Permanent link to this record |
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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. |
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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 |
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| |
Volume |
30 |
Issue |
10 |
Pages |
3285-3293 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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| |
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. |
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Corporate Author |
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Place of Publication |
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Language |
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Wos |
000433403800014 |
Publication Date |
2018-05-22 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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| |
ISSN |
0897-4756 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
9.466 |
Times cited |
6 |
Open Access |
OpenAccess |
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| |
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 |
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| |
Call Number |
EMAT @ emat @c:irua:152048 |
Serial |
4996 |
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| Permanent link to this record |
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Author |
Xia, C.; Winckelmans, N.; Prins, P.T.; Bals, S.; Gerritsen, H.C.; de Mello Donegá, C. |
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Title |
Near-Infrared-Emitting CuInS2/ZnS Dot-in-Rod Colloidal Heteronanorods by Seeded Growth |
Type |
A1 Journal article |
| |
Year |
2018 |
Publication |
Journal of the American Chemical Society |
Abbreviated Journal |
J Am Chem Soc |
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| |
Volume |
140 |
Issue |
140 |
Pages |
5755-5763 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Synthesis protocols for anisotropic CuInX2 (X = S, Se, Te)-based heteronanocrystals (HNCs) are scarce due to the difficulty in balancing the reactivities of multiple precursors and the high solid-state diffusion rates of the cations involved in the CuInX2 lattice. In this work, we report a multistep seeded growth synthesis protocol that yields colloidal wurtzite CuInS2/ZnS dot core/rod shell HNCs with photoluminescence in the NIR (∼800 nm). The wurtzite CuInS2 NCs used as seeds are obtained by topotactic partial Cu+ for In3+ cation exchange in template Cu2–xS NCs. The seed NCs are injected in a hot solution of zinc oleate and hexadecylamine in octadecene, 20 s after the injection of sulfur in octadecene. This results in heteroepitaxial growth of wurtzite ZnS primarily on the Sulfur-terminated polar facet of the CuInS2 seed NCs, the other facets being overcoated only by a thin (∼1 monolayer) shell. The fast (∼21 nm/min) asymmetric axial growth of the nanorod proceeds by addition of [ZnS] monomer units, so that the polarity of the terminal (002) facet is preserved throughout the growth. The delayed injection of the CuInS2 seed NCs is crucial to allow the concentration of [ZnS] monomers to build up, thereby maximizing the anisotropic heteroepitaxial growth rates while minimizing the rates of competing processes (etching, cation exchange, alloying). Nevertheless, a mild etching still occurred, likely prior to the onset of heteroepitaxial overgrowth, shrinking the core size from 5.5 to ∼4 nm. The insights provided by this work open up new possibilities in designing multifunctional Cu-chalcogenide based colloidal heteronanocrystals. |
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Corporate Author |
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Place of Publication |
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Language |
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Wos |
000431600000016 |
Publication Date |
2018-03-29 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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| |
ISSN |
0002-7863 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
13.858 |
Times cited |
43 |
Open Access |
OpenAccess |
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Notes |
Chenghui Xia acknowledges China Scholarship Council (CSC) for financial support (NO. 201406330055). S.B and N.W. acknowledge funding from the European Research Council (Starting Grant No. COLOURATOMS 335078). C.d.M.D. acknowledge financial support from the division of Chemical Sciences (CW) of The Netherlands Organization for Scientific Research (NWO) under Grant Number ECHO.712.014.001. The authors thank Xiaobin Xie and Da Wang for some TEM measurements, Donglong Fu for XRD measurements, Christina H. M. van Oversteeg for ICP-OES measurements, and Chun-Che Lin for suggestions regarding the synthesis. ECAS_Sara (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 13.858 |
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| |
Call Number |
EMAT @ emat @c:irua:150362UA @ admin @ c:irua:150362 |
Serial |
4917 |
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Author |
Sánchez-Iglesias, A.; Claes, N.; Solís, D.M.; Taboada, J.M.; Bals, S.; Liz-Marzán, L.M.; Grzelczak, M. |
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Title |
Reversible Clustering of Gold Nanoparticles under Confinement |
Type |
A1 Journal article |
| |
Year |
2018 |
Publication |
Angewandte Chemie: international edition in English |
Abbreviated Journal |
Angew Chem Int Edit |
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Volume |
57 |
Issue |
57 |
Pages |
3183-3186 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
A limiting factor of solvent-induced nanoparticle self-assembly is the need for constant sample dilution in assembly/disassembly cycles. Changes in the nanoparticle concentration alter the kinetics of the subsequent assembly process, limiting optical signal recovery. Herein, we show that upon confining hydrophobic nanoparticles in permeable silica nanocapsules, the number of nanoparticles participating in cyclic aggregation remains constant despite bulk changes in solution, leading to highly reproducible plasmon band shifts at different solvent compositions. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000426759900031 |
Publication Date |
2018-02-21 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1433-7851 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
11.994 |
Times cited |
53 |
Open Access |
OpenAccess |
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Notes |
L.M.L.-M. and M.G. acknowledge funding from the Spanish MINECO (Grant #MAT2013-46101R). N.C. and S.B. acknowledge financial support from European Research Council (ERC Starting Grant #335078-COLOURATOM). D.M.S., and J.M.T, acknowledge funding from the European Regional Development Fund (ERDF) and the Spanish MINECO (Projects TEC2017-85376-C2-1-R, TEC2017-85376-C2-2-R), and from the ERDF and the Galician Regional Government under agreement for funding the Atlantic Research Center for Information and Communication Technologies (AtlantTIC). (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:cannot); ECAS_Sara |
Approved |
Most recent IF: 11.994 |
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Call Number |
EMAT @ emat @c:irua:149558UA @ admin @ c:irua:149558 |
Serial |
4911 |
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| Permanent link to this record |
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Author |
Yang, Z.; Altantzis, T.; Bals, S.; Tendeloo, G.V.; Pileni, M.-P. |
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Title |
Do Binary Supracrystals Enhance the Crystal Stability? |
Type |
A1 Journal article |
| |
Year |
2018 |
Publication |
The journal of physical chemistry: C : nanomaterials and interfaces |
Abbreviated Journal |
J Phys Chem C |
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Volume |
122 |
Issue |
122 |
Pages |
13515-13521 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
We study the oxygen thermal stability of two binary
systems. The larger particles are magnetic amorphous Co (7.2 nm) or
Fe3O4 (7.5 nm) nanocrystals, whereas the smaller ones (3.7 nm) are
Au nanocrystals. The nanocrystal ordering as well as the choice of the
magnetic nanoparticles very much influence the stability of the binary
system. A perfect crystalline structure is obtained with the Fe3O4/Au
binary supracrystals. For the Co/Au binary system, oxidation of Co
results in the chemical transformation from Co to CoO, where the size
of the amorphous Co nanoparticles increases from 7.2 to 9.8 nm in
diameter. During the volume expansion of the Co nanoparticles, Au
nanoparticles within the binary assemblies coalesce and are at the
origin of the instability of the binary nanoparticle supracrystals. On the
other hand, for the Fe3O4/Au binary system, the oxidation of Fe3O4 to
γ-Fe2O3 does not lead to a size change of the nanoparticles, which
maintains the stability of the binary nanoparticle supracrystals. A similar behavior is observed for an AlB2-type Co−Ag binary
system: The crystalline structure is maintained, whereas in disordered assemblies, coalescence of Ag nanocrystals is observed. |
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Language |
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Wos |
000437811500035 |
Publication Date |
2018-01-30 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.536 |
Times cited |
5 |
Open Access |
OpenAccess |
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Notes |
The research leading to these results has been supported by an Advanced Grant of the European Research Council under Grant 267129. The authors appreciate financial support by the European Union under the Framework 7 program under a contract for an Integrated Infrastructure Initiative (Reference No. 262348 ESMI). S.B. acknowledges funding from ERC Starting Grant COLOURATOMS (335078). T.A. acknowledges a postdoctoral grant from the Research Foundation Flanders (FWO, Belgium). (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); ecas_sara |
Approved |
Most recent IF: 4.536 |
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Call Number |
EMAT @ emat @c:irua:149388UA @ admin @ c:irua:149388 |
Serial |
4812 |
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Author |
Winckelmans, N.; Altantzis, T.; Grzelczak, M.; Sánchez-Iglesias, A.; Liz-Marzán, L.M.; Bals, S. |
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Title |
Multimode Electron Tomography as a Tool to Characterize the Internal Structure and Morphology of Gold Nanoparticles |
Type |
A1 Journal article |
| |
Year |
2018 |
Publication |
The journal of physical chemistry: C : nanomaterials and interfaces |
Abbreviated Journal |
J Phys Chem C |
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Volume |
122 |
Issue |
122 |
Pages |
13522-13528 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Three dimensional (3D) characterization of structural defects in nanoparticles by transmission electron microscopy is far from straightforward. We propose the use of a dose-efficient approach, so-called multimode tomography, during which tilt series of low and high angle annular dark field scanning transmission electron microscopy projection images are acquired simultaneously. In this manner, not only reliable information can be obtained concerning the shape of the nanoparticles, but also the twin planes can be clearly visualized in 3D. As an example, we demonstrate the application of this approach to identify the position of the seeds with respect to the twinning planes in anisotropic gold nanoparticles synthesized using a seed mediated growth approach. |
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Place of Publication |
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Language |
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Wos |
000437811500036 |
Publication Date |
2018-01-16 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.536 |
Times cited |
23 |
Open Access |
OpenAccess |
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Notes |
S.B. and N.W. acknowledge funding from the European Research Council under the Seventh Framework Program (FP7), ERC Grant No. 335078 COLOURATOM. S.B. and T.A. acknowledge financial support from the Research Foundation Flanders (FWO, Belgium) through project fundings (G.0369.15N and G.0218.14N) and a postdoctoral research grant to T.A. L.M.L.-M. and M.G. acknowledge funding from the Spanish Ministerio de Economía y Competitividad (grant MAT2013-46101-R). L.M.L.-M. and S.B. acknowledge funding from the European Commission (grant EUSMI 731019). (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); saraecas; ECAS_Sara; |
Approved |
Most recent IF: 4.536 |
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| |
Call Number |
EMAT @ emat @c:irua:148164UA @ admin @ c:irua:148164 |
Serial |
4807 |
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Author |
Niu, H.; Pitcher, M.J.; Corkett, A.J.; Ling, S.; Mandal, P.; Zanella, M.; Dawson, K.; Stamenov, P.; Batuk, D.; Abakumov, A.M.; Bull, C.L.; Smith, R.I.; Murray, C.A.; Day, S.J.; Slater, B.; Cora, F.; Claridge, J.B.; Rosseinsky, M.J. |
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Title |
Room Temperature Magnetically Ordered Polar Corundum GaFeO3 Displaying Magnetoelectric Coupling |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
Journal of the American Chemical Society |
Abbreviated Journal |
J Am Chem Soc |
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Volume |
139 |
Issue |
4 |
Pages |
1520-1531 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
The polar corundum structure type offers a route to new room temperature multiferroic materials, as the partial LiNbO3-type cation ordering that breaks inversion symmetry may be combined with long-range magnetic ordering of high spin d(5) cations above room temperature in the AFeO(3) system. We report the synthesis of a polar corundum GaFeO3 by a high-pressure, high-temperature route and demonstrate that its polarity arises from partial LiNbO3 -type cation ordering by complementary use of neutron, X-ray, and electron diffraction methods. In situ neutron diffraction shows that the polar corundum forms directly from AlFeO3-type GaFeO3 under the synthesis conditions. The A(3+)/Fe3+ cations are shown to be more ordered in polar corundum GaFeO3 than in isostructural ScFeO3. This is explained by DFT calculations which indicate that the extent of ordering is dependent on the configurational entropy available to each system at the very different synthesis temperatures required to form their corundum structures. Polar corundum GaFeO3 exhibits weak ferromagnetism at room temperature that arises from its Fe2O3-like magnetic ordering, which persists to a temperature of 408 K. We demonstrate that the polarity and magnetization are coupled in this system with a measured linear magnetoelectric coupling coefficient of 0.057 ps/m. Such coupling is a prerequisite for potential applications of polar corundum materials in multiferroic/magnetoelectric devices. |
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Wos |
000393355600034 |
Publication Date |
2016-12-25 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0002-7863 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.858 |
Times cited |
12 |
Open Access |
OpenAccess |
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Notes |
This work was funded by the EPSRC under EP/N004884. We thank the STFC for provision of beam time at ISIS and Diamond Light Source. We thank the Materials Chemistry Consortium (EPSRC, EP/L000202) for access to computer time on the ARCHER UK National Supercomputing Service (http://www.archer.ac.uk). A.M.A. is grateful to the Russian Science Foundation (Grant 14-13-00680) for financial support. MJ.R is a Royal Society Research Professor. We wish to thank Dr. Ming Li (University of Nottingham, UK) for helpful discussion and advice. Original data is available at the University of Liverpool's DataCat repository at DOI: 10.17638/datacat.liverpool.ac.uk/235. The supporting crystallographic information file may also be obtained from FIZ Karlsruhe, 76344 Eggenstein-Leopoldshafen, Germany (e-mail: crysdata@fiz-karlsruhe.de), on quoting the deposition number CSD-432419. |
Approved |
Most recent IF: 13.858 |
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Call Number |
EMAT @ emat @c:irua:147507 |
Serial |
4777 |
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Author |
Jacquet, Q.; Perez, A.; Batuk, D.; Van Tendeloo, G.; Rousse, G.; Tarascon, J.-M. |
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Title |
The Li3RuyNb1-yO4 (0 ≤y≤ 1) System: Structural Diversity and Li Insertion and Extraction Capabilities |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
29 |
Issue |
12 |
Pages |
5331-5343 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Searching for novel high-capacity electrode materials combining cationic and anionic redox processes is an ever-growing activity within the field of Li-ion batteries. In this respect, we report on the exploration of the Li3RuyNb1-yO4 (O <= y <= 1) system with an O/M ratio of 4 to maximize the number of oxygen lone pairs, responsible for the anionic redox. We show that this system presents a very rich crystal chemistry with the existence of four structural types, which derive from the rocksalt structure but differ in their cationic arrangement, creating either zigzag, helical, jagged chains or clusters. From an electrochemical standpoint, these compounds are active on reduction via a classical cationic insertion process. The oxidation process is more complex, because of the instability of the delithiated phase. Our results promote the use of the rich Li3MO4 family as a viable platform for a better understanding of the relationships between structure and anionic redox activity. |
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Place of Publication |
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Wos |
000404493100036 |
Publication Date |
2017-06-27 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
17 |
Open Access |
Not_Open_Access |
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Notes |
The authors thank Paul Pearce, Alexis Grimaud, Matthieu Saubanere, and Marie-Liesse Doublet for fruitful discussions, Vivian Nassif for her help in neutron diffraction experiment at the D1B diffractometer at ILL, and Dominique Foix for XPS analysis. Use of the Advanced Photon Source at 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. Q.J. thanks the ANR “Deli-Redox” for Ph.D. funding. J.-M.T. and D.B. acknowledge funding from the European Research Council (ERC) (FP/2014)/ERC Grant -Project 670116-ARPEMA. |
Approved |
Most recent IF: 9.466 |
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Call Number |
EMAT @ emat @c:irua:147506 |
Serial |
4776 |
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Author |
Morozov, V.A.; Batuk, D.; Batuk, M.; Basovich, O.M.; Khaikina, E.G.; Deyneko, D.V.; Lazoryak, B.I.; Leonidov, I.I.; Abakumov, A.M.; Hadermann, J. |
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Title |
Luminescence Property Upgrading via the Structure and Cation Changing in AgxEu(2–x)/3WO4and AgxGd(2–x)/3–0.3Eu0.3WO4 |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
29 |
Issue |
20 |
Pages |
8811-8823 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
The creation and ordering of A-cation vacancies and the effect of cation substitutions in the scheelite-type framework are investigated as a factor for controlling the scheelite-type structure and luminescence properties. AgxEu3+(2−x)/3□(1−2x)/3WO4 and AgxGd(2−x)/3−0.3Eu3+0.3□(1−2x)/3WO4 (x = 0.5−0) scheelite-type phases were synthesized by a solid state method, and their structures were investigated using a combination of transmission electron microscopy techniques and powder synchrotron X-ray diffraction. Transmission electron microscopy also revealed the (3 + 1)D incommensurately modulated character of AgxEu3+(2−x)/3□(1−2x)/3WO4 (x = 0.286, 0.2) phases. The crystal structures of the scheelite-based AgxEu3+(2−x)/3□(1−2x)/3WO4 (x = 0.5, 0.286, 0.2) red phosphors have been refined from high resolution synchrotron powder X-ray diffraction data. The luminescence properties of all phases under near-ultraviolet (n-UV) light have been investigated. The excitation spectra of AgxEu3+(2−x)/3□(1−2x)/3WO4 (x = 0.5, 0.286,0.2) phosphors show the strongest absorption at 395 nm, which matches well with the commercially available n-UV-emitting GaN-based LED chip. The excitation spectra of the Eu2/3□1/3WO4 and Gd0.367Eu0.30□1/3WO4 phases exhibit the highest contribution of the charge transfer band at 250 nm and thus the most efficient energy transfer mechanism between the host and the luminescent ion as compared to direct excitation. The emission spectra of all samples indicate an intense red emission due to the 5D0 → 7F2 transition of Eu3+. Concentration dependence of the 5D0 → 7F2 emission for AgxEu(2−x)/3□(1−2x)/3WO4 samples differs from the same dependence for the earlier studied NaxEu3+(2−x)/3□(1−2x)/3MoO4 (0 ≤ x ≤ 0.5) phases. The intensity of the 5D0 → 7F2 emission is reduced almost 7 times with decreasing x from 0.5 to 0, but it practically does not change in the range from x = 0.286 to x = 0.200. The emission spectra of Gd-containing samples show a completely different trend as compared to only Eu-containing samples. The Eu3+ emission under excitation of Eu3+(5L6) level (λex = 395 nm) increases more than 2.5 times with the increasing Gd3+ concentration from 0.2 (x = 0.5) to 0.3 (x = 0.2) in the AgxGd(2−x)/3−0.3Eu3+0.3□(1−2x)/3WO4, after which it remains almost constant for higher Gd3+ concentrations. |
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Wos |
000413884900028 |
Publication Date |
2017-10-24 |
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Series Editor |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
7 |
Open Access |
Not_Open_Access |
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Notes |
This research was supported by FWO (project G039211N), Flanders Research Foundation. V.A.M. is grateful for financial support of the Russian Foundation for Basic Research (Grant 15-03-07741). E.G.K. and O.M.B. are grateful for financial support of the Russian Foundation for Basic Research (Grants 13-03-01020 and 16-03-00510). D.V.D. is grateful for financial support of the Russian Foundation for Basic Research (Grant 16-33-00197) and the Foundation of the President of the Russian Federation (Grant MK-7926.2016.5.). We are grateful to the ESRF for granting the beamtime. Experimental support of Andy Fitch at the ID31 beamline of ESRF is kindly acknowledged. |
Approved |
Most recent IF: 9.466 |
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Call Number |
EMAT @ emat @c:irua:147241 |
Serial |
4768 |
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Author |
Kus, M.; Altantzis, T.; Vercauteren, S.; Caretti, I.; Leenaerts, O.; Batenburg, K.J.; Mertens, M.; Meynen, V.; Partoens, B.; Van Doorslaer, S.; Bals, S.; Cool, P. |
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Title |
Mechanistic Insight into the Photocatalytic Working of Fluorinated Anatase {001} Nanosheets |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
The journal of physical chemistry: C : nanomaterials and interfaces |
Abbreviated Journal |
J Phys Chem C |
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Volume |
121 |
Issue |
121 |
Pages |
26275-26286 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT); Laboratory of adsorption and catalysis (LADCA) |
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Abstract |
Anatase nanosheets with exposed {001} facets
have gained increasing interest for photocatalytic applications. To
fully understand the structure-to-activity relation, combined
experimental and computational methods have been exploited.
Anatase nanosheets were prepared under hydrothermal conditions
in the presence of fluorine ions. High resolution scanning
transmission electron microscopy was used to fully characterize
the synthesized material, confirming the TiO2 nanosheet
morphology. Moreover, the surface structure and composition
of a single nanosheet could be determined by annular bright-field
scanning transmission electron microscopy (ABF-STEM) and
STEM electron energy loss spectroscopy (STEM-EELS). The photocatalytic activity was tested for the decomposition of organic
dyes rhodamine 6G and methyl orange and compared to a reference TiO2 anatase sample. The anatase nanosheets with exposed
{001} facets revealed a significantly lower photocatalytic activity compared to the reference. In order to understand the
mechanism for the catalytic performance, and to investigate the role of the presence of F−, light-induced electron paramagnetic
resonance (EPR) experiments were performed. The EPR results are in agreement with TEM, proving the presence of Ti3+
species close to the surface of the sample and allowing the analysis of the photoinduced formation of paramagnetic species.
Further, ab initio calculations of the anisotropic effective mass of electrons and electron holes in anatase show a very high effective
mass of electrons in the [001] direction, having a negative impact on the mobility of electrons toward the {001} surface and thus
the photocatalysis. Finally, motivated by the experimental results that indicate the presence of fluorine atoms at the surface, we
performed ab initio calculations to determine the position of the band edges in anatase slabs with different terminations of the
{001} surface. The presence of fluorine atoms near the surface is shown to strongly shift down the band edges, which indicates
another reason why it can be expected that the prepared samples with a large amount of {001} surface, but with fluorine atoms
near the surface, show only a low photocatalytic activity. |
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Wos |
000417228500017 |
Publication Date |
2017-11-30 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.536 |
Times cited |
20 |
Open Access |
OpenAccess |
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Notes |
The authors acknowledge the University of Antwerp for financial support in the frame of a GOA project. S.B. acknowledges funding from the European Research Council under the Seventh Framework Program (FP7), ERC Grant No. 335078 COLOURATOM. S.V.D. and V.M. acknowledge funding from the Fund for Scientific Research-Flanders (G.0687.13). T.A. acknowledges financial support from the Research Foundation Flanders (FWO, Belgium) through a postdoctoral grant. (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); saraecas; ECAS_Sara; |
Approved |
Most recent IF: 4.536 |
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Call Number |
EMAT @ emat @c:irua:147240UA @ admin @ c:irua:147240 |
Serial |
4771 |
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Author |
Momot, A.; Amini, M.N.; Reekmans, G.; Lamoen, D.; Partoens, B.; Slocombe, D.R.; Elen, K.; Adriaensens, P.; Hardy, A.; Van Bael, M.K. |
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Title |
A novel explanation for the increased conductivity in annealed Al-doped ZnO: an insight into migration of aluminum and displacement of zinc |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
Physical chemistry, chemical physics |
Abbreviated Journal |
Phys Chem Chem Phys |
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Volume |
19 |
Issue |
40 |
Pages |
27866-27877 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
A combined experimental and first-principles study is performed to study the origin of conductivity in
ZnO:Al nanoparticles synthesized under controlled conditions via a reflux route using benzylamine as a
solvent. The experimental characterization of the samples by Raman, nuclear magnetic resonance (NMR)
and conductivity measurements indicates that upon annealing in nitrogen, the Al atoms at interstitial
positions migrate to the substitutional positions, creating at the same time Zn interstitials. We provide
evidence for the fact that the formed complex of AlZn and Zni corresponds to the origin of the Knight
shifted peak (KS) we observe in 27Al NMR. As far as we know, the role of this complex has not been
discussed in the literature to date. However, our first-principles calculations show that such a complex is
indeed energetically favoured over the isolated Al interstitial positions. In our calculations we also
address the charge state of the Al interstitials. Further, Zn interstitials can migrate from Al_Zn and possibly
also form Zn clusters, leading to the observed increased conductivity. |
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Place of Publication |
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Wos |
000413290500073 |
Publication Date |
2017-10-09 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1463-9076 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.123 |
Times cited |
26 |
Open Access |
OpenAccess |
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Notes |
We want to thank the Interuniversity Attraction Poles Programme (P7/05) initiated by the Belgian Science Policy Office (BELSPO) for the financial support. We also acknowledge the Research Foundation Flanders (FWO-Vlaanderen) for support via the MULTIMAR WOG project and under project No. G018914. The computational parts were carried out using the HPC infrastructure at the University of Antwerp (CalcUA), a division of the Flemish Supercomputer Center VSC, supported financially by the Hercules foundation and the Flemish Government (EWI Department). |
Approved |
Most recent IF: 4.123 |
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Call Number |
EMAT @ emat @c:irua:146878 |
Serial |
4760 |
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