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Author Abakumov, A.M.; Erni, R.; Tsirlin, A.A.
Title Reply to Comment on “Frustrated octahedral tilting distortion in the incommensurately modulated Li3xNd2/3-xTiO3 perovskites” Type Editorial
Year 2014 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 26 Issue 2 Pages 1288
Keywords Editorial; Electron microscopy for materials research (EMAT)
Abstract
Address
Corporate Author Thesis
Publisher Place of Publication Washington, D.C. Editor
Language Wos 000330543600051 Publication Date 2014-01-03
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756;1520-5002; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.466 Times cited 1 Open Access
Notes Approved (up) Most recent IF: 9.466; 2014 IF: 8.354
Call Number UA @ lucian @ c:irua:115730 Serial 2874
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Author Ustarroz, J.; Altantzis, T.; Hammons, J.A.; Hubin, A.; Bals, S.; Terryn, H.
Title The role of nanocluster aggregation, coalescence, and recrystallization in the electrochemical deposition of platinum nanostructures Type A1 Journal article
Year 2014 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 26 Issue 7 Pages 2396-2406
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract By using an optimized characterization approach that combines aberration-corrected transmission electron microscopy, electron tomography, and in situ ultrasmall angle X-ray scattering (USAXS), we show that the early stages of Pt electrochemical growth on carbon substrates may be affected by the aggregation, self-alignment, and partial coalescence of nanoclusters of d ≈ 2 nm. The morphology of the resulting nanostructures depends on the degree of coalescence and recrystallization of nanocluster aggregates, which in turn depends on the electrodeposition potential. At low overpotentials, a self-limiting growth mechanism may block the epitaxial growth of primary nanoclusters and results in loose dendritic aggregates. At more negative potentials, the extent of nanocluster coalescence and recrystallization is larger and further growth by atomic incorporation may be allowed. On one hand, this suggests a revision of the VolmerWeber island growth mechanism. Whereas this theory has traditionally assumed direct attachment as the only growth mechanism, it is suggested that nanocluster self-limiting growth, aggregation, and coalescence should also be taken into account during the early stages of nanoscale electrodeposition. On the other hand, depending on the deposition potential, ultrahigh porosities can be achieved, turning electrodeposition in an ideal process for highly active electrocatalyst production without the need of using high surface area carbon supports.
Address
Corporate Author Thesis
Publisher Place of Publication Washington, D.C. Editor
Language Wos 000334572300026 Publication Date 2014-03-10
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756;1520-5002; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.466 Times cited 55 Open Access Not_Open_Access
Notes FWO; contract no. FWOAL527 Approved (up) Most recent IF: 9.466; 2014 IF: 8.354
Call Number UA @ lucian @ c:irua:116956 Serial 2916
Permanent link to this record
 
 
Author Kerkhofs, S.; Willhammar, T.; Van Den Noortgate, H.; Kirschhock, C.E.A.; Breynaert, E.; Van Tendeloo, G.; Bals, S.; Martens, J.A.
Title Self-Assembly of Pluronic F127—Silica Spherical Core–Shell Nanoparticles in Cubic Close-Packed Structures Type A1 Journal article
Year 2015 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 27 Issue 27 Pages 5161-5169
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract A new ordered mesoporous silica material (COK-19) with cubic symmetry is synthesized by silicate polycondensation in a citric acid/citrate buffered micellar solution of Pluronic F127 triblock copolymer near neutral pH. SAXS, nitrogen adsorption, TEM, and electron tomography reveal the final material has a cubic close packed symmetry (Fm3̅m) with isolated spherical mesopores interconnected through micropores. Heating of the synthesis medium from room temperature to 70 °C results in a mesopore size increase from 7.0 to 11.2 nm. Stepwise addition of the silicate source allows isolation of a sequence of intermediates that upon characterization with small-angle X-ray scattering uncovers the formation process via formation and aggregation of individual silica-covered Pluronic micelles.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000359499100003 Publication Date 2015-07-24
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.466 Times cited 39 Open Access OpenAccess
Notes J.A.M. acknowledges the Flemish government for long-term structural funding (Methusalem, METH/08/04). The Belgian government is acknowledged for financing the interuniversity poles of attraction (IAP-PAI, P7/05 FS2). G.V.T., S.B. and T.W. acknowledge financial support from European Research Council (ERC Starting Grant no. 335078-COLOURATOMS). E.B. acknowledges financial support the Flemish FWO for a postdoctoral fellowship (1265013N). The authors gratefully thank Kristof Houthoofd for performing the NMR experiments.; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); Approved (up) Most recent IF: 9.466; 2015 IF: 8.354
Call Number c:irua:127758 Serial 3977
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Author Wang, Y.; Sentosun, K.; Li, A.; Coronado-Puchau, M.; Sánchez-Iglesias, A.; Li, S.; Su, X.; Bals, S.; Liz-Marzán, L.M.
Title Engineering Structural Diversity in Gold Nanocrystals by Ligand-Mediated Interface Control Type A1 Journal article
Year 2015 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 27 Issue 27 Pages 8032-8040
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Surface and interface control is fundamentally important for crystal growth engineering, catalysis, surface enhanced spectroscopies, and self-assembly, among other processes and applications. Understanding the role of ligands in regulating surface properties of plasmonic metal nanocrystals during growth has received considerable attention. However, the underlying mechanisms and the diverse functionalities of ligands are yet to be fully addressed. In this contribution,

we report a systematic study of ligand-mediated interface control in seeded growth of gold nanocrystals, leading to diverse and exotic nanostructures with an improved surface enhanced Raman scattering (SERS) activity. Three dimensional transmission electron microscopy (3D TEM) revealed an intriguing gold shell growth process mediated by the bifunctional ligand 1,4-benzenedithiol (BDT), which leads to a unique crystal growth mechanism as compared to other ligands, and subsequently to the concept of interfacial energy control mechanism. Volmer-Weber growth mode was proposed to be responsible for BDT-mediated seeded growth, favoring the strongest interfacial energy and generating an asymmetric island growth pathway with internal crevices/gaps. This additionally favors incorporation of BDT at the plasmonic nanogaps, thereby generating strong SERS activity with a maximum efficiency for a core-semishell configuration obtained along seeded growth. Numerical modeling was used to explain this observation. Interestingly, the same strategy can be used to engineer the structural diversity of this system, by using gold nanoparticle seeds with various sizes and shapes, and varying the [Au3+]/[Au0] ratio. This rendered a series of diverse and exotic plasmonic nanohybrids such as semishell-coated gold nanorods, with embedded Raman-active tags and Janus surface with distinct surface functionalities.

These would greatly enrich the plasmonic nanostructure toolbox for various studies and applications such as anisotropic nanocrystal engineering, SERS, and high-resolution Raman bioimaging or nanoantenna devices.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000366223200023 Publication Date 2015-10-09
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756;1520-5002; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.466 Times cited 18 Open Access OpenAccess
Notes The authors thank Bart Goris for his help with electron tomography. This work was funded by the European Commission (Grant #310445-2, SAVVY). The authors acknowledge financial support from European Research Council (ERC Advanced Grant # 267867- PLASMAQUO, ERC Starting Grant #335078-COLOURATOMS). The authors also appreciate financial support from the European Union under the Seventh Framework Program (Integrated Infrastructure Initiative N. 262348 European Soft Matter Infrastructure, ESMI). Wang Y. and Su X. would like to acknowledge the Agency for Science, Technology and Research (A*STAR), Singapore, for the financial support under the Grant JCO 14302FG096. M. C.-P. acknowledges an FPU scholarship from the Spanish Ministry of Education, Culture and Sports.; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); Approved (up) Most recent IF: 9.466; 2015 IF: 8.354
Call Number c:irua:129598 c:irua:129598 Serial 3972
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Author Batuk, M.; Batuk, D.; Tsirlin, A.A.; Filimonov, D.S.; Sheptyakov, D.V.; Frontzek, M.; Hadermann, J.; Abakumov, A.M.
Title Layered oxychlorides [PbBiO2]An+1BnO3n-1Cl2(A = Pb/Bi, B = Fe/Ti) : intergrowth of the hematophanite and sillen phases Type A1 Journal article
Year 2015 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 27 Issue 27 Pages 2946-2956
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract New layered structures corresponding to the general formula [PbBiO2]A(n+1)B(n)O(3n-1)Cl(2) Were prepared. Pb5BiFe3O10Cl2 (n = 3) and Pb5Bi2Fe4O13Cl2 (n = 4) are built as a stacking of truncated A(n+1)B(n)O(3n-1) perovskite blocks and alpha-PbO-type [A(2)O(2)](2+) (A = Pb, Bi) blocks combined with chlorine sheets. The alternation of these structural blocks can be represented as an intergrowth between the hematophanite and Sullen-type structural blocks. The crystal and-Magnetic structures of Pb5BiFe3O10Cl2 and Pb5Bi2Fe4O13Cl2 were investigated in the temperature range of 1.5-700 K using X-ray and neutron powder diffraction, transmission electron microscopy and Fe-57 Mossbauer spectroscopy. Both compounds crystallize in the I4/mmm space group with the unit cell parameters a approximate to a(p) approximate to 3.92 angstrom (a unit-cell parameter of the perovskite-structure), c approximate to 43.0 angstrom for the n = 3 member and c approximate to 53.5 angstrom for the n = 4 member. Despite the large separation between the slabs containing the Fe3+ ions (nearly 14 angstrom), long-range antiferromagnetic order sets in below similar to 600 K with the G-type arrangement of the Fe magnetic moments aligned along the c-axis. The possibility of mixing d(0) and d(n) cations at the B sublattice of these structures was also demonstrated by preparing the Ti-substituted n = 4 member Pb6BiFe3TiO13Cl2.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000353865800028 Publication Date 2015-03-26
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756;1520-5002; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.466 Times cited 11 Open Access
Notes Approved (up) Most recent IF: 9.466; 2015 IF: 8.354
Call Number c:irua:126060 Serial 1807
Permanent link to this record
 
 
Author van der Stam, W.; Berends, A.C.; Rabouw, F.T.; Willhammar, T.; Ke, X.; Meeldijk, J.D.; Bals, S.; de Donega, C.M.
Title Luminescent CuInS2 quantum dots by partial cation exchange in Cu2-xS nanocrystals Type A1 Journal article
Year 2015 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 27 Issue 27 Pages 621-628
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Here, we show successful partial cation exchange reactions in Cu2-xS nanocrystals (NCs) yielding luminescent CuInS2 (CIS) NCs. Our approach of mild reaction conditions ensures slow Cu extraction rates, which results in a balance with the slow In incorporation rate. With this method, we obtain CIS NCs with photoluminescence (PL) far in the near-infrared (NIR), which cannot be directly synthesized by currently available synthesis protocols. We discuss the factors that favor partial, self-limited cation exchange from Cu2-xS to CIS NCs, rather than complete cation exchange to In2S3. The product CIS NCs have the wurtzite crystal structure, which is understood in terms of conservation of the hexagonal close packing of the anionic sublattice of the parent NCs into the product NCs. These results are an important step toward the design of CIS NCs with sizes and shapes that are not attainable by direct synthesis protocols and may thus impact a number of potential applications.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000348618400028 Publication Date 2014-12-29
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756;1520-5002; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.466 Times cited 119 Open Access OpenAccess
Notes 335078 Colouratom; 262348 Esmi; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); Approved (up) Most recent IF: 9.466; 2015 IF: 8.354
Call Number c:irua:125291 Serial 1858
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Author McCalla, E.; Abakumov, A.; Rousse, G.; Reynaud, M.; Sougrati, M.T.; Budic, B.; Mahmoud, A.; Dominko, R.; Van Tendeloo, G.; Hermann, R.P.; Tarascon, J.M.;
Title Novel complex stacking of fully-ordered transition metal layers in Li4FeSbO6 materials Type A1 Journal article
Year 2015 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 27 Issue 27 Pages 1699-1708
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract As part of a broad project to explore Li4MM'O-6 materials (with M and M' being selected from a wide variety of metals) as positive electrode materials for Li-ion batteries, the structures of Li4FeSbO6 materials with both stoichiometric and slightly deficient lithium contents are studied here. For lithium content varying from 3.8 to 4.0, the color changes from yellow to black and extra superstructure peaks are seen in the XRD patterns. These extra peaks appear as satellites around the four superstructure peaks affected by the stacking of the transition metal atoms. Refinements of both XRD and neutron scattering patterns show a nearly perfect ordering of Li, Fe, and Sb in the transition metal layers of all samples, although these refinements must take the stacking faults into account in order to extract information about the structure of the TM layers. The structure of the most lithium rich sample, where the satellite superstructure peaks are seen, was determined with the help of HRTEM, XRD, and neutron scattering. The satellites arise due to a new stacking sequence where not all transition metal layers are identical but instead two slightly different compositions stack in an AABB sequence giving a unit cell that is four times larger than normal for such monoclinic layered materials. The more lithium deficient samples are found to contain metal site vacancies based on elemental analysis and Mossbauer spectroscopy results. The significant changes in physical properties are attributed to the presence of these vacancies. This study illustrates the great importance of carefully determining the final compositions in these materials, as very small differences in compositions may have large impacts on structures and properties.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000350919000032 Publication Date 2015-02-12
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756;1520-5002; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.466 Times cited 22 Open Access
Notes Approved (up) Most recent IF: 9.466; 2015 IF: 8.354
Call Number c:irua:125469 Serial 2373
Permanent link to this record
 
 
Author van der Stam, W.; Akkerman, Q.A.; Ke, X.; van Huis, M.A.; Bals, S.; de Donega, C.M.
Title Solution-processable ultrathin size- and shape-controlled colloidal Cu2-xS nanosheets Type A1 Journal article
Year 2015 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 27 Issue 27 Pages 283-291
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Ultrathin two-dimensional (2D) nanosheets (NSs) possess extraordinary properties that are attractive for both fundamental studies and technological devices. Solution-based bottom-up methods are emerging as promising routes to produce free-standing NSs, but the synthesis of colloidal NSs with well-defined size and shape has remained a major challenge. In this work, we report a novel method that yields 2 nm thick colloidal Cu2-xS NSs with well-defined shape (triangular or hexagonal) and size (100 nm to 3 mu m). The key feature of our approach is the use of a synergistic interaction between halides (Br or Cl) and copper-thiolate metal-organic frameworks to create a template that imposes 2D constraints on the Cu-catalyzed C-S thermolysis, resulting in nucleation and growth of colloidal 2D Cu2-xS NSs. Moreover, the NS composition can be postsynthetically tailored by exploiting topotactic cation exchange reactions. This is illustrated by converting the Cu2-xS NSs into ZnS and CdS NSs while preserving their size and shape. The method presented here thus holds great promise as a route to solution-processable compositionally diverse ultrathin colloidal NSs with well-defined shape and size.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000348085300036 Publication Date 2014-12-04
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756;1520-5002; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.466 Times cited 68 Open Access OpenAccess
Notes 335078 Colouratom; 246791 Countatoms; 312483 Esteem2; esteem2ta; ECASSara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); Approved (up) Most recent IF: 9.466; 2015 IF: 8.354
Call Number c:irua:123865 c:irua:123865 Serial 3052
Permanent link to this record
 
 
Author Wolf, D.; Rodriguez, L.A.; Béché, A.; Javon, E.; Serrano, L.; Magen, C.; Gatel, C.; Lubk, A.; Lichte, H.; Bals, S.; Van Tendeloo, G.; Fernández-Pacheco, A.; De Teresa, J.M.; Snoeck, E.
Title 3D Magnetic Induction Maps of Nanoscale Materials Revealed by Electron Holographic Tomography Type A1 Journal article
Year 2015 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 27 Issue 27 Pages 6771-6778
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The investigation of three-dimensional (3D) ferromagnetic nanoscale materials constitutes one of the key research areas of the current magnetism roadmap, and carries great potential to impact areas such as data storage, sensing and biomagnetism. The properties of such nanostructures are closely connected with their 3D magnetic nanostructure, making their determination highly valuable. Up to now, quantitative 3D maps providing both the internal magnetic and electric configuration of the same specimen with high spatial resolution are missing. Here, we demonstrate the quantitative 3D reconstruction of the dominant axial component of the magnetic induction and electrostatic potential within a cobalt nanowire (NW) of 100 nm in diameter with spatial resolution below 10 nanometers by applying electron holographic tomography. The tomogram was obtained using a dedicated TEM sample holder for acquisition, in combination with advanced alignment and tomographic reconstruction routines. The powerful approach presented here is widely applicable to a broad range of 3D magnetic nanostructures and may trigger the progress of novel spintronic non-planar nanodevices.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000362920700037 Publication Date 2015-09-08
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756;1520-5002; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.466 Times cited 50 Open Access OpenAccess
Notes This work was supported by the European Union under the Seventh Framework Program under a contract for an Inte-grated Infrastructure Initiative Reference 312483-ESTEEM2. S.B. and A.B. gratefully acknowledge funding by ERC Starting grants number 335078 COLOURATOMS and number 278510 VORTEX. AF-P acknowledges an EPSRC Early Career fellowship and support from the Winton Foundation. E.S., C.G. and L.A. R. acknowledge the French ANR program for support though the project EMMA.; esteem2jra4; ECASJO;; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); Approved (up) Most recent IF: 9.466; 2015 IF: 8.354
Call Number c:irua:129180 c:irua:129180 c:irua:129180 Serial 3950
Permanent link to this record
 
 
Author Morozov, V.A.; Arakcheeva, A.V.; Pattison, P.; Meert, K.W.; Smet, P.F.; Poelman, D.; Gauquelin, N.; Verbeeck, J.; Abakumov, A.M.; Hadermann, J.
Title KEu(MoO4)2 : polymorphism, structures, and luminescent properties Type A1 Journal article
Year 2015 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 27 Issue 27 Pages 5519-5530
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract In this paper, with the example of two different polymorphs of KEu(MoO4)2, the influence of the ordering of the A-cations on the luminescent properties in scheelite related compounds (A′,A″)n[(B′,B″)O4]m is investigated. The polymorphs were synthesized using a solid state method. The study confirmed the existence of only two polymorphic forms at annealing temperature range 9231203 K and ambient pressure: a low temperature anorthic α-phase and a monoclinic high temperature β-phase with an incommensurately modulated structure. The structures of both polymorphs were solved using transmission electron microscopy and refined from synchrotron powder X-ray diffraction data. The monoclinic β-KEu(MoO4)2 has a (3+1)-dimensional incommensurately modulated structure (superspace group I2/b(αβ0)00, a = 5.52645(4) Å, b = 5.28277(4) Å, c = 11.73797(8) Å, γ = 91.2189(4)o, q = 0.56821(2)a*0.12388(3)b*), whereas the anorthic α-phase is (3+1)-dimensional commensurately modulated (superspace group I1̅(αβγ)0, a = 5.58727(22) Å, b = 5.29188(18)Å, c = 11.7120(4) Å, α = 90.485(3)o, β = 88.074(3)o, γ = 91.0270(23)o, q = 1/2a* + 1/2c*). In both cases the modulation arises due to Eu/K cation ordering at the A site: the formation of a 2-dimensional Eu3+ network is characteristic for the α-phase, while a 3-dimensional Eu3+-framework is observed for the β-phase structure. The luminescent properties of KEu(MoO4)2 samples prepared under different annealing conditions were measured, and the relation between their optical properties and their structures is discussed.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000360323700011 Publication Date 2015-07-29
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756;1520-5002; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.466 Times cited 26 Open Access
Notes 278510 Vortex; Fwo G039211n; G004413n ECASJO_; Approved (up) Most recent IF: 9.466; 2015 IF: 8.354
Call Number c:irua:127244 Serial 3537
Permanent link to this record
 
 
Author Sun, M.; Rousse, G.; Abakumov, A.M.; Saubanere, M.; Doublet, M.-L.; Rodriguez-Carvajal, J.; Van Tendeloo, G.; Tarascon, J.-M.
Title Li2Cu2O(SO4)2: a possible electrode for sustainable Li-based batteries showing a 4.7 V redox activity vs Li+/Li0 Type A1 Journal article
Year 2015 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 27 Issue 27 Pages 3077-3087
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Li-ion batteries rely on the use of insertion positive electrodes with performances scaling with the redox potential of the 31) metals accompanying Liuptake/removal. Although not commonly studied, the Cu2+/Cu3+ redox potential has been predicted from theoretical calculations to possibly offer a high operating voltage redox couple. We herein report the synthesis and crystal structure of a hitherto-unknown oxysulfate phase, Li2Cu2O(SO4)(2), which contains infinite edgesharing CuO4 chains and presents attractive electrochemical redox activity with respect to Li+/Li, namely amphoteric characteristics. Li2Cu2O(SO4)(2) shows redox activity at 4.7 V vs Li+/Li corresponding to the oxidation of Cu2+ to Cu3+ enlisting ligand holes and associated with the reversible uptake-removal of 0.3 Li. Upon reduction, this compound reversibly uptakes similar to 2 Li at an average potential of about 2.5 V vs Li+/Li, associated with the Cu2+/Cu+ redox couple. The mechanism of the reactivity upon reduction is discussed in detail, with particular attention to the occasional appearance of an oscillation wave in the discharge profile. Our work demonstrates that Cu-based compounds can indeed be fertile scientific ground in the search for new high-energy-density electrodes.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000353865800043 Publication Date 2015-03-25
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756;1520-5002; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.466 Times cited 20 Open Access
Notes Approved (up) Most recent IF: 9.466; 2015 IF: 8.354
Call Number c:irua:126061 Serial 3541
Permanent link to this record
 
 
Author Cautaerts, N.; Delville, R.; Stergar, E.; Pakarinen, J.; Verwerft, M.; Yang, Y.; Hofer, C.; Schnitzer, R.; Lamm, S.; Felfer, P.; Schryvers, D.
Title The role of Ti and TiC nanoprecipitates in radiation resistant austenitic steel: A nanoscale study Type A1 Journal article
Year 2020 Publication Acta Materialia Abbreviated Journal Acta Mater
Volume 197 Issue Pages 184-197
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract This work encompasses an in-depth transmission electron microscopy and atom probe tomography study of Ti-stabilized austenitic steel irradiated with Fe-ions. The focus is on radiation induced segregation and precipitation, and in particular on how Ti and TiC affect these processes. A 15-15Ti steel (grade: DIN 1.4970) in two thermo-mechanical states (cold-worked and aged) was irradiated at different temperatures up to a dose of 40 dpa. At low irradiation temperatures, the cold-worked and aged materials evolved to a similar microstructure dominated by small Si and Ni clusters, corresponding to segregation to small point defect clusters. TiC precipitates, initially present in the aged material, were found to be unstable under these irradiation conditions. Elevated irradiation temperatures resulted in the nucleation of nanometer sized Cr enriched TiC precipitates surrounded by Si and Ni enriched shells. In addition, nanometer sized Ti- and Mn-enriched G-phase (M6Ni16Si7) precipitates formed, often attached to TiC precipitates. Post irradiation, larger number densities of TiC were observed in the cold-worked material compared to the aged material. This was correlated with a lower volume fraction of G-phase. The findings suggest that at elevated irradiation temperatures, the precipitate-matrix interface is an important point defect sink and contributes to the improved radiation resistance of this material. The study is a first of its kind on stabilized steel and demonstrates the significance of the small Ti addition to the evolution of the microstructure under irradiation. (C) 2020 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000564767000001 Publication Date 2020-07-10
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1359-6454 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.4 Times cited Open Access Not_Open_Access
Notes ; This work was supported by ENGIE [contract number 2015-AC-007 e BSUEZ6900]; the U.S. Department of Energy, Office of Nuclear Energy under DOE Idaho Operations Office Contract DE-AC07051D14517 as part of a Nuclear Science User Facilities experiment; and by the MYRRHA program at SCK-CEN, Belgium. Funding of the Austrian BMK (846933) in the framework of the program “Production of the future” and the “BMK Professorship for Industry” is gratefully acknowledged. We want to thank the staffat MIBL for assisting with the ion irradiations as well as the staffat CAES for assisting with FIB work and conducting APT measurements. ; Approved (up) Most recent IF: 9.4; 2020 IF: 5.301
Call Number UA @ admin @ c:irua:171956 Serial 6626
Permanent link to this record
 
 
Author Fang, C.; Verbrigghe, N.; Sigurdsson, B.D.D.; Ostonen, I.; Leblans, N.I.W.; Maranon-Jimenez, S.; Fuchslueger, L.; Sigurosson, P.; Meeran, K.; Portillo-Estrada, M.; Verbruggen, E.; Richter, A.; Sardans, J.; Penuelas, J.; Bahn, M.; Vicca, S.; Janssens, I.A.
Title Decadal soil warming decreased vascular plant above and belowground production in a subarctic grassland by inducing nitrogen limitation Type A1 Journal article
Year 2023 Publication New phytologist Abbreviated Journal
Volume 240 Issue 2 Pages 565-576
Keywords A1 Journal article; Plant and Ecosystems (PLECO) – Ecology in a time of change
Abstract Below and aboveground vegetation dynamics are crucial in understanding how climate warming may affect terrestrial ecosystem carbon cycling. In contrast to aboveground biomass, the response of belowground biomass to long-term warming has been poorly studied. Here, we characterized the impacts of decadal geothermal warming at two levels (on average +3.3 degrees C and +7.9 degrees C) on below and aboveground plant biomass stocks and production in a subarctic grassland. Soil warming did not change standing root biomass and even decreased fine root production and reduced aboveground biomass and production. Decadal soil warming also did not significantly alter the root-shoot ratio. The linear stepwise regression model suggested that following 10 yr of soil warming, temperature was no longer the direct driver of these responses, but losses of soil N were. Soil N losses, due to warming-induced decreases in organic matter and water retention capacity, were identified as key driver of the decreased above and belowground production. The reduction in fine root production was accompanied by thinner roots with increased specific root area. These results indicate that after a decade of soil warming, plant productivity in the studied subarctic grassland was affected by soil warming mainly by the reduction in soil N.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001043561400001 Publication Date 2023-08-07
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0028-646x ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.4 Times cited Open Access
Notes Approved (up) Most recent IF: 9.4; 2023 IF: 7.33
Call Number UA @ admin @ c:irua:198443 Serial 9199
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Author Mary Joy, R.; Pobedinskas, P.; Baule, N.; Bai, S.; Jannis, D.; Gauquelin, N.; Pinault-Thaury, M.-A.; Jomard, F.; Sankaran, K.J.; Rouzbahani, R.; Lloret, F.; Desta, D.; D’Haen, J.; Verbeeck, J.; Becker, M.F.; Haenen, K.
Title The effect of microstructure and film composition on the mechanical properties of linear antenna CVD diamond thin films Type A1 Journal article
Year 2024 Publication Acta materialia Abbreviated Journal Acta Materialia
Volume 264 Issue Pages 119548
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract This study reports the impact of film microstructure and composition on the Young’s modulus and residual stress in nanocrystalline diamond (NCD) thin films ( thick) grown on silicon substrates using a linear antenna microwave plasma-enhanced chemical vapor deposition (CVD) system. Combining laser acoustic wave spectroscopy to determine the elastic properties with simple wafer curvature measurements, a straightforward method to determine the intrinsic stress in NCD films is presented. Two deposition parameters are varied: (1) the substrate temperature from 400 °C to 900 °C, and (2) the [P]/[C] ratio from 0 ppm to 8090 ppm in the H2/CH4/CO2/PH3 diamond CVD plasma. The introduction of PH3 induces a transition in the morphology of the diamond film, shifting from NCD with larger grains to ultra-NCD with a smaller grain size, concurrently resulting in a decrease in Young’s modulus. Results show that the highest Young’s modulus of (113050) GPa for the undoped NCD deposited at 800 °C is comparable to single crystal diamond, indicating that NCD with excellent mechanical properties is achievable with our process for thin diamond films. Based on the film stress results, we propose the origins of tensile intrinsic stress in the diamond films. In NCD, the tensile intrinsic stress is attributed to larger grain size, while in ultra-NCD films the tensile intrinsic stress is due to grain boundaries and impurities.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001126632800001 Publication Date 2023-11-23
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1359-6454 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.4 Times cited Open Access Not_Open_Access
Notes This work was financially supported by the Special Research Fund (BOF) via Methusalem NANO network, the Research Foundation – Flanders (FWO) via Project G0D4920N, and the CORNET project nr 263-EN “ULTRAHARD: Ultrahard optical diamond coatings” (2020–2021). Approved (up) Most recent IF: 9.4; 2024 IF: 5.301
Call Number EMAT @ emat @c:irua:202169 Serial 8989
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Author Coulombier, M.; Baral, P.; Orekhov, A.; Dohmen, R.; Raskin, J.P.; Pardoen, T.; Cordier, P.; Idrissi, H.
Title On-chip very low strain rate rheology of amorphous olivine films Type A1 Journal article
Year 2024 Publication Acta materialia Abbreviated Journal
Volume 266 Issue Pages 119693-12
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Recent observations made by the authors revealed the activation of stress induced amorphization and sliding at grain boundary in olivine [1], a mechanism which is expected to play a pivotal role in the viscosity drop at the lithosphere-asthenosphere boundary and the brittle -ductile transition in the lithospheric mantle. However, there is a lack of information in the literature regarding the intrinsic mechanical properties and the elementary deformation mechanisms of this material, especially at time scales relevant for geodynamics. In the present work, amorphous olivine films were obtained by pulsed laser deposition (PLD). The mechanical response including the rate dependent behavior are investigated using a tension -on -chip (TOC) method developed at UCLouvain allowing to perform creep/relaxation tests on thin films at extremely low strain rates. In the present work, strain rate down to 10-12 s- 1 was reached which is unique. High strain rate sensitivity of 0.054 is observed together with the activation of relaxation at the very early stage of deformation. Furthermore, digital image correlation (DIC), used for the first time on films deformed by TOC, reveals local strain heterogeneities. The relationship between such heterogeneities, the high strain rate sensitivity and the effect of the electron beam in the scanning electron microscope is discussed and compared to the literature.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001170513400001 Publication Date 2024-01-17
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1359-6454 ISBN Additional Links UA library record; WoS full record
Impact Factor 9.4 Times cited Open Access
Notes Approved (up) Most recent IF: 9.4; 2024 IF: 5.301
Call Number UA @ admin @ c:irua:204864 Serial 9163
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Author Le Noir de Carlan, C.; Kaarlejarvi, E.; De Tender, C.; Heinecke, T.; Eskelinen, A.; Verbruggen, E.
Title Shifts in mycorrhizal types of fungi and plants in response to fertilisation, warming and herbivory in a tundra grassland Type A1 Journal article
Year 2024 Publication New phytologist Abbreviated Journal
Volume Issue Pages
Keywords A1 Journal article; Plant and Ecosystems (PLECO) – Ecology in a time of change
Abstract Climate warming is severely affecting high-latitude regions. In the Arctic tundra, it may lead to enhanced soil nutrient availability and interact with simultaneous changes in grazing pressure. It is presently unknown how these concurrently occurring global change drivers affect the root-associated fungal communities, particularly mycorrhizal fungi, and whether changes coincide with shifts in plant mycorrhizal types. We investigated changes in root-associated fungal communities and mycorrhizal types of the plant community in a 10-yr factorial experiment with warming, fertilisation and grazing exclusion in a Finnish tundra grassland. The strongest determinant of the root-associated fungal community was fertilisation, which consistently increased potential plant pathogen abundance and had contrasting effects on the different mycorrhizal fungal types, contingent on other treatments. Plant mycorrhizal types went through pronounced shifts, with warming favouring ecto- and ericoid mycorrhiza but not under fertilisation and grazing exclusion. Combination of all treatments resulted in dominance by arbuscular mycorrhizal plants. However, shifts in plant mycorrhizal types vs fungi were mostly but not always aligned in their magnitude and direction. Our results show that our ability to predict shifts in symbiotic and antagonistic fungal communities depend on simultaneous consideration of multiple global change factors that jointly alter plant and fungal communities.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001220955000001 Publication Date 2024-05-14
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0028-646x ISBN Additional Links UA library record; WoS full record
Impact Factor 9.4 Times cited Open Access
Notes Approved (up) Most recent IF: 9.4; 2024 IF: 7.33
Call Number UA @ admin @ c:irua:206016 Serial 9228
Permanent link to this record
 
 
Author Gogoi, A.; Neyts, E.C.; Milošević, M.V.; Peeters, F.M.
Title Arresting aqueous swelling of layered graphene-oxide membranes with H3O+ and OH- ions Type A1 Journal article
Year 2022 Publication ACS applied materials and interfaces Abbreviated Journal Acs Appl Mater Inter
Volume 14 Issue 30 Pages 34946-34954
Keywords A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract Over the past decade, graphene oxide (GO) has emerged as a promising membrane material with superior separation performance and intriguing mechanical/chemical stability. However, its practical implementation remains very challenging primarily because of its undesirable swelling in an aqueous environment. Here, we demonstrated that dissociation of water molecules into H3O+ and OH- ions inside the interlayer gallery of a layered GO membrane can strongly affect its stability and performance. We reveal that H3O+ and OH- ions form clusters inside the GO laminates that impede the permeance of water and salt ions through the membrane. Dynamics of those clusters is sensitive to an external ac electric field, which can be used to tailor the membrane performance. The presence of H3O+ and OH- ions also leads to increased stability of the hydrogen bond (H-bond) network among the water molecules and the GO layers, which further reduces water permeance through the membrane, while crucially imparting stability to the layered GO membrane against undesirable swelling. KEYWORDS: layered graphene-oxide membrane, aqueous stability, H3O+ and OH- ions, external electric field, molecular dynamics
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000835946500001 Publication Date 2022-07-25
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1944-8244 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.5 Times cited 9 Open Access OpenAccess
Notes Approved (up) Most recent IF: 9.5
Call Number UA @ admin @ c:irua:189467 Serial 7127
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Author Cunha, D.M.; Gauquelin, N.; Xia, R.; Verbeeck, J.; Huijben, M.
Title Self-assembled epitaxial cathode-electrolyte nanocomposites for 3D microbatteries Type A1 Journal article
Year 2022 Publication ACS applied materials and interfaces Abbreviated Journal Acs Appl Mater Inter
Volume 14 Issue 37 Pages 42208-42214
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract The downscaling of electronic devices requires rechargeable microbatteries with enhanced energy and power densities. Here, we evaluate self-assembled vertically aligned nano-composite (VAN) thin films as a platform to create high-performance three-dimensional (3D) microelectrodes. This study focuses on controlling the VAN formation to enable interface engineering between the LiMn2O4 cathode and the (Li,La)TiO3 solid electrolyte. Electrochemical analysis in a half cell against lithium metal showed the absence of sharp redox peaks due to the confinement in the electrode pillars at the nanoscale. The (100)-oriented VAN thin films showed better rate capability and stability during extensive cycling due to the better alignment to the Li-diffusion channels. However, an enhanced pseudocapacitive contribution was observed for the increased total surface area within the (110)-oriented VAN thin films. These results demonstrate for the first time the electrochemical behavior of cathode-electrolyte VANs for lithium-ion 3D microbatteries while pointing out the importance of control over the vertical interfaces.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000852647100001 Publication Date 2022-09-06
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1944-8244 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.5 Times cited 4 Open Access OpenAccess
Notes This research was carried out with the support from the Netherlands Organization for Scientific Research (NWO) under VIDI grant no. 13456. Approved (up) Most recent IF: 9.5
Call Number UA @ admin @ c:irua:190619 Serial 7206
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Author Agrawal, H.; Patra, B.K.; Altantzis, T.; De Backer, A.; Garnett, E.C.
Title Quantifying Strain and Dislocation Density at Nanocube Interfaces after Assembly and Epitaxy Type A1 Journal article
Year 2020 Publication Acs Applied Materials & Interfaces Abbreviated Journal Acs Appl Mater Inter
Volume 12 Issue 7 Pages 8788-8794
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Abstract Nanoparticle self-assembly and epitaxy are utilized extensively to make 1D and 2D structures with complex shapes. High-resolution transmission electron microscopy (HRTEM) has shown that single-crystalline interfaces can form, but little is known about the strain and dislocations at these interfaces. Such information is critically important for applications: drastically reducing

dislocation density was the key breakthrough enabling widespread implementation of light-emitting diodes, while strain engineering has been fundamental to modern high-performance transistors, solar cells, and thermoelectrics. In this work, the interfacial defect and strain formation after selfassembly and room temperature epitaxy of 7 nm Pd nanocubes capped with polyvinylpyrrolidone (PVP) is examined. It is observed that, during ligand removal, the cubes move over large distances on the substrate, leading to both spontaneous self-assembly and epitaxy to form single crystals. Subsequently, atomically resolved images are used to quantify the strain and dislocation density at the epitaxial interfaces between cubes with different lateral and angular misorientations. It is shown that dislocation- and strain-free interfaces form when the nanocubes align parallel to each other. Angular misalignment between adjacent cubes does not necessarily lead to grain boundaries but does cause dislocations, with higher densities associated with larger rotations.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000515214300101 Publication Date 2020-02-19
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1944-8244 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.5 Times cited Open Access OpenAccess
Notes Fonds Wetenschappelijk Onderzoek; H2020 Research Infrastructures, 731019 ; Nederlandse Organisatie voor Wetenschappelijk Onderzoek, 14846 ; The work at AMOLF is part of the research program of the “Nederlandse Organisatie voor Wetenschappelijk Onderzoek” (NWO). This work was supported by the NWO VIDI grant (project no. 14846). The authors would like to thank Reinout Jaarsma and Dr. Sven Askes for helping with the XPS measurements. A.D.B. 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. Approved (up) Most recent IF: 9.5; 2020 IF: 7.504
Call Number EMAT @ emat @c:irua:167770 Serial 6398
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Author Ben Dkhil, S.; Perkhun, P.; Luo, C.; Mueller, D.; Alkarsifi, R.; Barulina, E.; Quiroz, Y.A.A.; Margeat, O.; Dubas, S.T.; Koganezawa, T.; Kuzuhara, D.; Yoshimoto, N.; Caddeo, C.; Mattoni, A.; Zimmermann, B.; Wuerfel, U.; Pfannmöller, M.; Bals, S.; Ackermann, J.; Videlot-Ackermann, C.
Title Direct correlation of nanoscale morphology and device performance to study photocurrent generation in donor-enriched phases of polymer solar cells Type A1 Journal article
Year 2020 Publication Acs Applied Materials & Interfaces Abbreviated Journal Acs Appl Mater Inter
Volume 12 Issue 25 Pages 28404-28415
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract The nanoscale morphology of polymer blends is a key parameter to reach high efficiency in bulk heterojunction solar cells. Thereby, research typically focusing on optimal blend morphologies while studying nonoptimized blends may give insight into blend designs that can prove more robust against morphology defects. Here, we focus on the direct correlation of morphology and device performance of thieno[3,4-b]-thiophene-alt-benzodithiophene (PTB7):[6,6]phenyl C-71 butyric acid methyl ester (PC71BM) bulk heterojunction (BHJ) blends processed without additives in different donor/acceptor weight ratios. We show that while blends of a 1:1.5 ratio are composed of large donor-enriched and fullerene domains beyond the exciton diffusion length, reducing the ratio below 1:0.5 leads to blends composed purely of polymer-enriched domains. Importantly, the photocurrent density in such blends can reach values between 45 and 60% of those reached for fully optimized blends using additives. We provide here direct visual evidence that fullerenes in the donor-enriched domains are not distributed homogeneously but fluctuate locally. To this end, we performed compositional nanoscale morphology analysis of the blend using spectroscopic imaging of low-energy-loss electrons using a transmission electron microscope. Charge transport measurement in combination with molecular dynamics simulations shows that the fullerene substructures inside the polymer phase generate efficient electron transport in the polymer-enriched phase. Furthermore, we show that the formation of densely packed regions of fullerene inside the polymer phase is driven by the PTB7:PC71BM enthalpy of mixing. The occurrence of such a nanoscale network of fullerene clusters leads to a reduction of electron trap states and thus efficient extraction of photocurrent inside the polymer domain. Suitable tuning of the polymer-acceptor interaction can thus introduce acceptor subnetworks in polymer-enriched phases, improving the tolerance for high-efficiency BHJ toward morphological defects such as donor-enriched domains exceeding the exciton diffusion length.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000543780900058 Publication Date 2020-06-01
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1944-8244 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.5 Times cited 7 Open Access OpenAccess
Notes ; J.A., O.M., and C.V.-A. acknowledge financial support by the French Fond Unique Interministeriel (FUI) under the project “SFUMATO” (Grant Number: F1110019V/ 201308815) as well as by the European Commission under the Project “SUNFLOWER” (FP7-ICT-2011-7, Grant Number: 287594). J.A., C.V.-A., and E.B. acknowledge the Association Nationale de la Recherche et de la Technologie (ANRT) and the Ministere de l'Enseignement Superieur, de la Recherche et de l'Innovation, awarded through the company Dracula Technologies (Valence, France), for framework of a CIFRE Ph.D. grant 2017/0529. J.A. and P.P. received funding from the European Union's Horizon 2020 research and innovation program under the Marie Sklodowska-Curie Grant agreement no. 713750. They further acknowledge support of the Regional Council of Provence-Alpes-Cote d'Azur, A*MIDEX (no. ANR-11-IDEX-0001-02), and the Investissements d'Avenir project funded by the French Government, managed by the French National Research Agency (ANR). J.A. and Y.A.A.Q. acknowledge the French Research Agency for funding through the project NFA-15 (ANR-17-CE05-0020-01). N.Y. acknowledges that the synchrotron radiation experiments were performed at BL19B2 in SPring-8 with the approval of Japan Synchrotron Radiation Research Institute (JASRI) (proposal nos. 2017B1629 and 2018B1791). S.B. acknowledges financial support from the European Research Council (ERC Consolidator Grant 815128-REALNANO) and from FWO (G.0381.16N). M.P. gratefully acknowledges funding by the Ministerium fur Wissenschaft, Forschung und Kunst Baden-Wurttemberg through the HEiKA materials research centre FunTECH-3D (MWK, 33-753-30-20/3/3) and the Large-Scale-Data-Facility (LSDF) sds@hd through grant INST 35/1314-1 FUGG. A.M. acknowledges Italian MIUR for funding through the project PON04a2 00490 M2M Netergit, PRACE, for awarding access to Marconi KNL at CINECA, Italy, through projects DECONVOLVES (2018184466) and PROVING-IL (2019204911). C.C. acknowledges the CINECA award under the ISCRA initiative for the availability of high-performance computing resources and support (project MITOMASC). ; sygma Approved (up) Most recent IF: 9.5; 2020 IF: 7.504
Call Number UA @ admin @ c:irua:170703 Serial 6484
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Author Kertik, A.; Wee, L.H.; Şentosun, K.; Navarro, J.A.R.; Bals, S.; Martens, J.A.; Vankelecom, I.F.J.
Title High-performance CO2-selective hybrid membranes by exploiting MOF-breathing effects Type A1 Journal article
Year 2020 Publication Acs Applied Materials & Interfaces Abbreviated Journal Acs Appl Mater Inter
Volume 12 Issue 2 Pages 2952-2961
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Conventional CO2 separation in the petrochemical industry via cryogenic distillation or amine-based absorber-stripper units is energy-intensive and environmentally unfriendly. Membrane-based gas separation technology, in contrast, has contributed significantly to the development of energy-efficient systems for processes such as natural gas purification. The implementation of commercial polymeric membranes in gas separation processes is restricted by their permeability-selectivity trade-off and by their insufficient thermal and chemical stability. Herein, we present the fabrication of a Matrimid-based membrane loaded with a breathing metal-organic framework (MOF) (NH2-MIL-53(Al)) which is capable of separating binary CO2/CH4 gas mixtures with high selectivities without sacrificing much of its CO2 permeabilities. NH2-MIL-53(Al) crystals were embedded in a polyimide (PI) matrix, and the mixed-matrix membranes (MMMs) were treated at elevated temperatures (up to 350 degrees C) in air to trigger PI cross-linking and to create PI-MOF bonds at the interface to effectively seal the grain boundary. Most importantly, the MOF transitions from its narrow-pore form to its large-pore form during this treatment, which allows the PI chains to partly penetrate the pores and cross-link with the amino functions at the pore mouth of the NH2-MIL-53(Al) and stabilizes the open-pore form of NH2-MIL-53(Al). This cross-linked MMM, with MOF pore entrances was made more selective by the anchored PI-chains and achieves outstanding CO2/CH4 selectivities. This approach provides significant advancement toward the design of selective MMMs with enhanced thermal and chemical stabilities which could also be applicable for other potential applications, such as separation of hydrocarbons (olefin/paraffin or isomers), pervaporation, and solvent-resistant nanofiltration.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000508464500108 Publication Date 2019-12-20
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1944-8244 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.5 Times cited 26 Open Access OpenAccess
Notes ; A.K. is grateful to the Erasmus Mundus Doctorate in Membrane Engineering (EUDIME) programme. L.H.W. thanks the FWO-Vlaanderen for a postdoctoral research fellowships under contract number 12M1418N. We thank Methusalem and IAP-PAI for research funding. S.B. acknowledges financial support from European Research Council (ERC) (ERC Starting Grant No. 335078-COLOURATOM). We are also grateful to Frank Mathijs (KU Leuven) for the mechanical tests, Bart Goderis and Olivier Verkinderen for the DSC measurements, and Huntsman (Switzerland) for providing the Matrimid polymer. ; Approved (up) Most recent IF: 9.5; 2020 IF: 7.504
Call Number UA @ admin @ c:irua:166576 Serial 6534
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Author Bhatia, H.; Martin, C.; Keshavarz, M.; Dovgaliuk, I.; Schrenker, N.J.; Ottesen, M.; Qiu, W.; Fron, E.; Bremholm, M.; Van de Vondel, J.; Bals, S.; Roeffaers, M.B.J.; Hofkens, J.; Debroye, E.
Title Deciphering the role of water in promoting the optoelectronic performance of surface-engineered lead halide perovskite nanocrystals Type A1 Journal article
Year 2023 Publication ACS applied materials and interfaces Abbreviated Journal
Volume 15 Issue 5 Pages 7294-7307
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Lead halide perovskites are promising candidates for applicability is limited by their structural instability toward moisture. Although a deliberate addition of water to the precursor solution has recently been shown to improve the crystallinity and optical properties of perovskites, the corresponding thin films still do not exhibit a near-unity quantum yield. Herein, we report that the direct addition of a minute amount of water to post-treated substantially enhances the stability while achieving a 95% photoluminescence quantum yield in a NC thin film. We unveil the mechanism of how moisture assists in the formation of an additional NH4Br component. Alongside, we demonstrate the crucial role of moisture in assisting localized etching of the perovskite crystal, facilitating the partial incorporation of NH4+, which is key for improved performance under ambient conditions. Finally, as a proof-of-concept, the application of post-treated and watertreated perovskites is tested in LEDs, with the latter exhibiting a superior performance, offering opportunities toward commercial application in moisture-stable optoelectronics.
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Publisher Place of Publication Editor
Language Wos 000931729400001 Publication Date 2023-01-27
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1944-8244 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.5 Times cited 3 Open Access Not_Open_Access
Notes H.B. would like to express her sincere gratitude to Dr. Peter Erk (formerly BASF SE, Germany) for very insightful discussions. The authors acknowledge financial support from the Research Foundation-Flanders (FWO grant numbers S002019N, 1514220N, G.0B39.15, G.0B49.15, G098319N, and ZW15_09-GOH6316) , the KU Leuven Research Fund (C14/19/079, iBOF-21-085 PERSIST, and STG/21/010) , the Flemish government through long-term structural funding Methusalem (CASAS2, Meth/15/04) , the Hercules Founda-tion (HER/11/14) , and the ERC through the Marie Curie ITN iSwitch Ph.D. fellowship to H.B. (grant number 642196) . C.M. acknowledges the financial support from grants PID2021-128761OA-C22 funded by MCIN/AEI/10.13039/501100011033 by the ?European Union? and SBPLY/21/180501/000127 funded by JCCM and by the EU through Fondo Europeo de Desarollo Regional? (FEDER) . Martin Bremholm and Martin Ottesen acknowledge funding from the Danish Council for Independent Research, Natural Sciences, under the Sapere Aude program (grant no. 7027-00077B) and VILLUM FONDEN through the Centre of Excellence for Dirac Materials (grant no. 11744) . Affiliation with the Center for Integrated Materials Research (iMAT) at Aarhus University is gratefully acknowledged.-N.J.S. acknowledges financial support from the research foundation Flanders (FWO) through a postdoctoral fellowship (FWO grant no. 1238622N) . S.B. acknowledges financial support from the European Commission by the ERC Consolidator grant REALNANO (no. 815128) . Approved (up) Most recent IF: 9.5; 2023 IF: 7.504
Call Number UA @ admin @ c:irua:195375 Serial 7293
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Author Mulder, J.T.; Meijer, M.S.; van Blaaderen, J.J.; du Fosse, I.; Jenkinson, K.; Bals, S.; Manna, L.; Houtepen, A.J.
Title Understanding and preventing photoluminescence quenching to achieve unity photoluminescence quantum yield in Yb:YLF nanocrystals Type A1 Journal article
Year 2023 Publication ACS applied materials and interfaces Abbreviated Journal
Volume 15 Issue 2 Pages 3274-3286
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Ytterbium-doped LiYF4 (Yb:YLF) is a commonly used material for laser applications, as a photon upconversion medium, and for optical refrigeration. As nanocrystals (NCs), the material is also of interest for biological and physical applications. Unfortunately, as with most phosphors, with the reduction in size comes a large reduction of the photoluminescence quantum yield (PLQY), which is typically associated with an increase in surface-related PL quenching. Here, we report the synthesis of bipyramidal Yb:YLF NCs with a short axis of similar to 60 nm. We systematically study and remove all sources of PL quenching in these NCs. By chemically removing all traces of water from the reaction mixture, we obtain NCs that exhibit a near-unity PLQY for an Yb3+ concentration below 20%. At higher Yb3+ concentrations, efficient concentration quenching occurs. The surface PL quenching is mitigated by growing an undoped YLF shell around the NC core, resulting in near-unity PLQY values even for fully Yb3+-based LiYbF4 cores. This unambiguously shows that the only remaining quenching sites in core-only Yb:YLF NCs reside on the surface and that concentration quenching is due to energy transfer to the surface. Monte Carlo simulations can reproduce the concentration dependence of the PLQY. Surprisingly, Fo''rster resonance energy transfer does not give satisfactory agreement with the experimental data, whereas nearest-neighbor energy transfer does. This work demonstrates that Yb3+-based nanophosphors can be synthesized with a quality close to that of bulk single crystals. The high Yb3+ concentration in the LiYbF4/LiYF4 core/shell nanocrystals increases the weak Yb3+ absorption, making these materials highly promising for fundamental studies and increasing their effectiveness in bioapplications and optical refrigeration.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000912997300001 Publication Date 2023-01-06
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1944-8244 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.5 Times cited 3 Open Access OpenAccess
Notes This project has received funding from the European Union's Horizon 2020 research and innovation program under Grant Agreement No. 766900 (Testing the Large-Scale Limit of Quantum Mechanics). A.J.H. and I.d.F. further acknowledge the European Research Council Horizon 2020 ERC Grant Agreement No. 678004 (Doping on Demand) for financial support. The authors thank Freddy Rabouw and Andries Meijerink (Utrecht University) for very fruitful discussions and extremely useful advice. The author s thank Jos Thieme for his help with the laser setups used . The authors furthermore thank Niranjan Saikumar for proofreading the manuscript. Approved (up) Most recent IF: 9.5; 2023 IF: 7.504
Call Number UA @ admin @ c:irua:194317 Serial 7348
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Author Van den Hoek, J.; Daems, N.; Arnouts, S.; Hoekx, S.; Bals, S.; Breugelmans, T.
Title Improving stability of CO₂ electroreduction by incorporating Ag NPs in N-doped ordered mesoporous carbon structures Type A1 Journal article
Year 2024 Publication ACS applied materials and interfaces Abbreviated Journal
Volume 16 Issue 6 Pages 6931-6947
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Abstract The electroreduction of carbon dioxide (eCO2RR) to CO using Ag nanoparticles as an electrocatalyst is promising as an industrial carbon capture and utilization (CCU) technique to mitigate CO2 emissions. Nevertheless, the long-term stability of these Ag nanoparticles has been insufficient despite initial high Faradaic efficiencies and/or partial current densities. To improve the stability, we evaluated an up-scalable and easily tunable synthesis route to deposit low-weight percentages of Ag nanoparticles (NPs) on and into the framework of a nitrogen-doped ordered mesoporous carbon (NOMC) structure. By exploiting this so-called nanoparticle confinement strategy, the nanoparticle mobility under operation is strongly reduced. As a result, particle detachment and agglomeration, two of the most pronounced electrocatalytic degradation mechanisms, are (partially) blocked and catalyst durability is improved. Several synthesis parameters, such as the anchoring agent, the weight percentage of Ag NPs, and the type of carbonaceous support material, were modified in a controlled manner to evaluate their respective impact on the overall electrochemical performance, with a strong emphasis on operational stability. The resulting powders were evaluated through electrochemical and physicochemical characterization methods, including X-ray diffraction (XRD), N2-physisorption, Inductively coupled plasma mass spectrometry (ICP-MS), scanning electron microscopy (SEM), SEM-energy-dispersive X-ray spectroscopy (SEM-EDS), high-angle annular dark field scanning transmission electron microscopy (HAADF-STEM), STEM-EDS, electron tomography, and X-ray photoelectron spectroscopy (XPS). The optimized Ag/soft-NOMC catalysts showed both a promising selectivity (∼80%) and stability compared with commercial Ag NPs while decreasing the loading of the transition metal by more than 50%. The stability of both the 5 and 10 wt % Ag/soft-NOMC catalysts showed considerable improvements by anchoring the Ag NPs on and into a NOMC framework, resulting in a 267% improvement in CO selectivity after 72 h (despite initial losses) compared to commercial Ag NPs. These results demonstrate the promising strategy of anchoring Ag NPs to improve the CO selectivity during prolonged experiments due to the reduced mobility of the Ag NPs and thus enhanced stability.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001158812100001 Publication Date 2023-12-21
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1944-8244 ISBN Additional Links UA library record; WoS full record
Impact Factor 9.5 Times cited Open Access Not_Open_Access: Available from 21.06.2024
Notes Approved (up) Most recent IF: 9.5; 2024 IF: 7.504
Call Number UA @ admin @ c:irua:202309 Serial 9045
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Author Guerrero, R.M.; Lemir, I.D.; Carrasco, S.; Fernández-Ruiz, C.; Kavak, S.; Pizarro, P.; Serrano, D.P.; Bals, S.; Horcajada, P.; Pérez, Y.
Title Scaling-Up Microwave-Assisted Synthesis of Highly Defective Pd@UiO-66-NH2Catalysts for Selective Olefin Hydrogenation under Ambient Conditions Type A1 Journal Article
Year 2024 Publication ACS Applied Materials & Interfaces Abbreviated Journal ACS Appl. Mater. Interfaces
Volume Issue Pages
Keywords A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;
Abstract The need to develop green and cost-effective industrial catalytic processes has led to growing interest in preparing more robust, efficient, and selective heterogeneous catalysts at a large scale. In this regard, microwave-assisted synthesis is a fast method for fabricating heterogeneous catalysts (including metal oxides, zeolites, metal–organic frameworks, and supported metal nanoparticles) with enhanced catalytic properties, enabling synthesis scale-up. Herein, the synthesis of nanosized UiO-66-NH2 was optimized via a microwave-assisted hydrothermal method to obtain defective matrices essential for the stabilization of metal nanoparticles, promoting catalytically active sites for hydrogenation reactions (760 kg·m–3·day–1 space time yield, STY). Then, this protocol was scaled up in a multimodal microwave reactor, reaching 86% yield (ca. 1 g, 1450 kg·m–3·day–1 STY) in only 30 min. Afterward, Pd nanoparticles were formed in situ decorating the nanoMOF by an effective and fast microwave-assisted hydrothermal method, resulting in the formation of Pd@UiO-66-NH2 composites. Both the localization and oxidation states of Pd nanoparticles (NPs) in the MOF were achieved using high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and X-ray photoelectron spectroscopy (XPS), respectively. The optimal composite, loaded with 1.7 wt % Pd, exhibited an extraordinary catalytic activity (>95% yield, 100% selectivity) under mild conditions (1 bar H2, 25 °C, 1 h reaction time), not only in the selective hydrogenation of a variety of single alkenes (1-hexene, 1-octene, 1-tridecene, cyclohexene, and tetraphenyl ethylene) but also in the conversion of a complex mixture of alkenes (i.e., 1-hexene, 1-tridecene, and anethole). The results showed a powerful interaction and synergy between the active phase (Pd NPs) and the catalytic porous scaffold (UiO-66-NH2), which are essential for the selectivity and recyclability.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos Publication Date 2024-04-26
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1944-8244 ISBN Additional Links
Impact Factor 9.5 Times cited Open Access
Notes The authors gratefully acknowledge financial support from “Comunidad de Madrid” and European Regional Development Fund-FEDER through the project HUB MADRID+CIRCULAR; the State Research Agency (MCIN/AEI /10.13039/501100011033) through the grant with reference number CEX2019-000931-M received in the 2019 call for “Severo Ochoa Centres of Excellence” and “María de Maeztu Units of Excellence” of the State Programme for Knowledge Generation and Scientific and Technological Strengthening of the R&D&I System; and MICIU through the project “NAPOLION” (PID2022-139956OB-I00). S.K. acknowledges the Flemish Fund for Scientific Research (FWO Vlaanderen) through a PhD research grant (1181124N). Approved (up) Most recent IF: 9.5; 2024 IF: 7.504
Call Number EMAT @ emat @ Serial 9126
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Author Tiwari, S.; Van de Put, M.; Sorée, B.; Hinkle, C.; Vandenberghe, W.G.
Title Reduction of magnetic interaction due to clustering in doped transition-metal dichalcogenides : a case study of Mn-, V-, and Fe-doped WSe₂ Type A1 Journal article
Year 2024 Publication ACS applied materials and interfaces Abbreviated Journal
Volume 16 Issue 4 Pages 4991-4998
Keywords A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Abstract Using Hubbard-U-corrected density functional theory calculations, lattice Monte Carlo simulations, and spin Monte Carlo simulations, we investigate the impact of dopant clustering on the magnetic properties of WSe2 doped with period four transition metals. We use manganese (Mn) and iron (Fe) as candidate n-type dopants and vanadium (V) as the candidate p-type dopant, substituting the tungsten (W) atom in WSe2. Specifically, we determine the strength of the exchange interaction in Fe-, Mn-, and V-doped WSe2 in the presence of clustering. We show that the clusters of dopants are energetically more stable than discretely doped systems. Further, we show that in the presence of dopant clustering, the magnetic exchange interaction significantly reduces because the magnetic order in clustered WSe2 becomes more itinerant. Finally, we show that the clustering of the dopant atoms has a detrimental effect on the magnetic interaction, and to obtain an optimal Curie temperature, it is important to control the distribution of the dopant atoms.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001155511900001 Publication Date 2024-01-18
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1944-8244 ISBN Additional Links UA library record; WoS full record
Impact Factor 9.5 Times cited Open Access
Notes Approved (up) Most recent IF: 9.5; 2024 IF: 7.504
Call Number UA @ admin @ c:irua:203830 Serial 9169
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Author Ni, S.; Houwman, E.; Gauquelin, N.; Chezganov, D.; Van Aert, S.; Verbeeck, J.; Rijnders, G.; Koster, G.
Title Stabilizing perovskite Pb(Mg0.33Nb0.67)O3-PbTiO3 thin films by fast deposition and tensile mismatched growth template Type A1 Journal article
Year 2024 Publication ACS applied materials and interfaces Abbreviated Journal
Volume 16 Issue 10 Pages 12744-12753
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Because of its low hysteresis, high dielectric constant, and strong piezoelectric response, Pb(Mg1/3Nb2/3)O-3-PbTiO3 (PMN-PT) thin films have attracted considerable attention for the application in PiezoMEMS, field-effect transistors, and energy harvesting and storage devices. However, it remains a great challenge to fabricate phase-pure, pyrochlore-free PMN-PT thin films. In this study, we demonstrate that a high deposition rate, combined with a tensile mismatched template layer can stabilize the perovskite phase of PMN-PT films and prevent the nucleation of passive pyrochlore phases. We observed that an accelerated deposition rate promoted mixing of the B-site cation and facilitated relaxation of the compressively strained PMN-PT on the SrTiO3 (STO) substrate in the initial growth layer, which apparently suppressed the initial formation of pyrochlore phases. By employing La-doped-BaSnO3 (LBSO) as the tensile mismatched buffer layer, 750 nm thick phase-pure perovskite PMN-PT films were synthesized. The resulting PMN-PT films exhibited excellent crystalline quality close to that of the STO substrate.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001176343700001 Publication Date 2024-02-29
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1944-8244 ISBN Additional Links UA library record; WoS full record
Impact Factor 9.5 Times cited Open Access
Notes Approved (up) Most recent IF: 9.5; 2024 IF: 7.504
Call Number UA @ admin @ c:irua:204754 Serial 9174
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Author Wang, Y.-L.; Glatz, A.; Kimmel, G.J.; Aranson, I.S.; Thoutam, L.R.; Xiao, Z.-L.; Berdiyorov, G.R.; Peeters, F.M.; Crabtree, G.W.; Kwok, W.-K.
Title Parallel magnetic field suppresses dissipation in superconducting nanostrips Type A1 Journal article
Year 2017 Publication America Abbreviated Journal P Natl Acad Sci Usa
Volume 114 Issue 48 Pages E10274-E10280
Keywords A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Abstract <script type='text/javascript'>document.write(unpmarked('The motion of Abrikosov vortices in type-II superconductors results in a finite resistance in the presence of an applied electric current. Elimination or reduction of the resistance via immobilization of vortices is the \u0022holy grail\u0022 of superconductivity research. Common wisdom dictates that an increase in the magnetic field escalates the loss of energy since the number of vortices increases. Here we show that this is no longer true if the magnetic field and the current are applied parallel to each other. Our experimental studies on the resistive behavior of a superconducting Mo0.79Ge0.21 nanostrip reveal the emergence of a dissipative state with increasing magnetic field, followed by a pronounced resistance drop, signifying a reentrance to the superconducting state. Large-scale simulations of the 3D time-dependent Ginzburg-Landau model indicate that the intermediate resistive state is due to an unwinding of twisted vortices. When the magnetic field increases, this instability is suppressed due to a better accommodation of the vortex lattice to the pinning configuration. Our findings show that magnetic field and geometrical confinement can suppress the dissipation induced by vortex motion and thus radically improve the performance of superconducting materials.'));
Address
Corporate Author Thesis
Publisher Place of Publication Washington, D.C. Editor
Language Wos 000416891600007 Publication Date 2017-11-13
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0027-8424; 1091-6490 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.661 Times cited 18 Open Access
Notes ; This work was supported by the US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division. The simulation was supported by the Scientific Discovery through Advanced Computing program funded by US DOE, Office of Science, Advanced Scientific Computing Research and Basic Energy Science, Division of Materials Science and Engineering. L.R.T. and Z.-L.X. acknowledge support through National Science Foundation Grant DMR-1407175. Use of the Center for Nanoscale Materials, an Office of Science user facility, was supported by the DOE, Office of Science, Office of Basic Energy Sciences, under Contract DE-AC02-06CH11357. ; Approved (up) Most recent IF: 9.661
Call Number UA @ lucian @ c:irua:147697 Serial 4889
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Author Kumar, J.; Eraña, H.; López-Martínez, E.; Claes, N.; Martín, V.F.; Solís, D.M.; Bals, S.; Cortajarena, A.L.; Castilla, J.; Liz-Marzán, L.M.
Title Detection of amyloid fibrils in Parkinson’s disease using plasmonic chirality Type A1 Journal article
Year 2018 Publication Proceedings of the National Academy of Sciences of the United States of America Abbreviated Journal P Natl Acad Sci Usa
Volume 115 Issue 115 Pages 3225-3230
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Amyloid fibrils, which are closely associated with various neurodegenerative

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

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

wherein protein fibrils related to the disease were identified through chiral signals from Au nanorods in the visible and near IR, whereas healthy brain samples did not exhibit any meaningful optical activity. The technique was additionally extended to the specific detection of infectious amyloids formed by prion proteins, thereby confirming the wide potential of the technique. The intense chiral response driven by strong dipolar coupling in helical Au nanorod arrangements allowed us to detect amyloid fibrils down to nanomolar concentrations.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000428382400032 Publication Date 2018-03-12
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0027-8424 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.661 Times cited 187 Open Access OpenAccess
Notes We thank Prof. Dr. J.-P. Timmermans and the Antwerp Centre of Advanced Microscopy for providing access to the Tecnai G2 Spirit BioTWIN TEM. We also thank the Basque Biobank (Basque Foundation for Health Innovation and Research, BIOEF) for providing us with Parkinson’s disease-affected brain samples. J.K. acknowledges financial support from the European Commission under Marie Sklodowska-Curie Program H2020- MSCA-IF-2015708321. S.B. and A.L.C. acknowledge European Research Council Grants 335078 COLOURATOM and 648071 ProNANO. S.B. and L.M.L.-M. acknowledge funding from European Commission Grant EUSMI 731019. A.L.C., J.C., and L.M.L.-M. acknowledge funding from Spanish Ministry of Economy and Competitiveness (MINECO) Grants MAT2013-46101- R, AGL2015-65046-C2-1-R, and BIO2016-77367-C2-1-R. (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:restricted); saraecas; ECASSara; Approved (up) Most recent IF: 9.661
Call Number EMAT @ emat @c:irua:150355UA @ admin @ c:irua:150355 Serial 4918
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Author Liao, Z.; Gauquelin, N.; Green, R.J.; Müller-Caspary, K.; Lobato, I.; Li, L.; Van Aert, S.; Verbeeck, J.; Huijben, M.; Grisolia, M.N.; Rouco, V.; El Hage, R.; Villegas, J.E.; Mercy, A.; Bibes, M.; Ghosez, P.; Sawatzky, G.A.; Rijnders, G.; Koster, G.
Title Metal–insulator-transition engineering by modulation tilt-control in perovskite nickelates for room temperature optical switching Type A1 Journal article
Year 2018 Publication America Abbreviated Journal P Natl Acad Sci Usa
Volume 115 Issue 38 Pages 9515-9520
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract In transition metal perovskites ABO3 the physical properties are largely driven by the rotations of the BO6 octahedra, which can be tuned in thin films through strain and dimensionality control. However, both approaches have fundamental and practical limitations due to discrete and indirect variations in bond angles, bond lengths and film symmetry by using commercially available substrates. Here, we introduce modulation tilt control as a new approach to tune the ground state of perovskite oxide thin films by acting explicitly on the oxygen octahedra rotation modes, i.e. directly on the bond angles. By intercalating the prototype SmNiO3 target material with a tilt-control layer, we cause the system to change the natural amplitude of a given rotation mode without affecting the interactions. In contrast to strain and dimensionality engineering, our method enables a continuous fine-tuning of the materials properties. This is achieved through two independent adjustable parameters: the nature of the tilt-control material (through its symmetry, elastic constants and oxygen rotation angles) and the relative thicknesses of the target and tilt-control materials. As a result, a magnetic and electronic phase diagram can be obtained, normally only accessible by A-site element substitution, within the single SmNiO3 compound. With this unique approach, we successfully adjusted the metal-insulator transition (MIT) to room temperature to fulfill the desired conditions for optical switching applications.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000447224900057 Publication Date 2018-09-05
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0027-8424 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.661 Times cited 50 Open Access OpenAccess
Notes We would like to acknowledge Prof. Z. Zhong for stimulated discussion. M.H., G.K. and G.R. acknowledge funding from DESCO program of the Dutch Foundation for Fundamental Research on Matter (FOM) with financial support from the Netherlands Organization for Scientific Research (NWO). This work was funded by the European Union Council under the 7th Framework Program (FP7) grant nr NMP3-LA-2010-246102 IFOX. J.V., S.V.A, N.G. and K.M.C. acknowledge funding from FWO projects G.0044.13N, G.0374.13N, G. 0368.15N, and G.0369.15N. The Qu-Ant-EM microscope was partly funded by the Hercules fund from the Flemish Government. N.G. acknowledges funding from the European Research Council under the 7th Framework Program (FP7), ERC Starting Grant 278510 VORTEX. N.G. and J.V. acknowledge financial support from the European Union under the Seventh Framework Program under a contract for an Integrated Infrastructure Initiative (Reference No. 312483- ESTEEM2). The Canadian work was supported by NSERC and the Max Planck-UBC Centre for Quantum Materials. Some experiments for this work were performed at the Canadian Light Source, which is funded by the Canada Foundation for Innovation, NSERC, the National Research Council of Canada, the Canadian Institutes of Health Research, the Government of Saskatchewan, Western Economic Diversification Canada, and the University of Saskatchewan. MB acknowledges funding from the European Research Council under the 7th Framework Program (FP7), ERC CoG grant MINT #615759. A.M. and Ph.G. were supported by the ARC project AIMED and F.R.S-FNRS PDR project HiT4FiT and acknowledge access to Céci computing facilities funded by F.R.S-FNRS (Grant No 2.5020.1), Tier-1 supercomputer of the Fédération Wallonie-Bruxelles funded by the Walloon Region (Grant No 1117545) and HPC resources from the PRACE project Megapasta. Approved (up) Most recent IF: 9.661
Call Number EMAT @ emat @c:irua:154784UA @ admin @ c:irua:154784 Serial 5059
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