“Mn2FeWO6 : a new Ni3TeO6-type polar and magnetic oxide”. Li MR, Croft M, Stephens PW, Ye M, Vanderbilt D, Retuerto M, Deng Z, Grams CP, Hemberger J, Hadermann J, Li WM, Jin CQ, Saouma FO, Jang JI, Akamatsu H, Gopalan V, Walker D, Greenblatt M;, Advanced materials 27, 2177 (2015). http://doi.org/10.1002/adma.201405244
Abstract: Mn22+Fe2+W6+O6, a new polar magnetic phase, adopts the corundum-derived Ni3TeO6-type structure with large spontaneous polarization (P-S) of 67.8 mu C cm-2, complex antiferromagnetic order below approximate to 75 K, and field-induced first-order transition to a ferrimagnetic phase below approximate to 30 K. First-principles calculations predict a ferrimagnetic (udu) ground state, optimal switching path along the c-axis, and transition to a lower energy udu-udd magnetic double cell.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 19.791
Times cited: 32
DOI: 10.1002/adma.201405244
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“Pd5InSe and Pd8In2Se : new metal-rich homological selenides with 2D palladium-indium fragments : synthesis, structure and bonding”. Zakharova EY, Kazakov SM, Isaeva AA, Abakumov AM, Van Tendeloo G, Kuznetsov AN, Journal of alloys and compounds 589, 48 (2014). http://doi.org/10.1016/j.jallcom.2013.11.172
Abstract: Two new metal-rich palladium-indium selenides, Pd5InSe and Pd8In2Se, were synthesized using a high-temperature ampoule technique. Their crystal structures were determined from Rietveld analysis of powder diffraction data, supported by energy-dispersive X-ray spectroscopy and selected area electron diffraction. Both compounds crystallize in tetragonal system with P4/mmm space group (Pd5InSe: a = 4.0290(3) angstrom, c = 6.9858(5) angstrom, Z = 1; Pd8In2Se: a = 4.0045(4) angstrom, c = 10.952(1) angstrom, Z = 1). The first compound belongs to the Pd5TlAs structure type, while the second one – to a new structure type. Main structural units in both selenides are indium-centered [Pd12In] cuboctahedra of the tetragonally distorted Cu3Au type, single-and double-stacked along the c axis in Pd5InSe and Pd8In2Se, respectively, alternating with [Pd8Se] rectangular prisms. DFT electronic structure calculations predict both compounds to be 3D metallic conductors and Pauli-like paramagnets. According to the bonding analysis based on the electron localization function topology, both compounds feature multi-centered palladium-indium interactions in their heterometallic fragments. (C) 2013 Elsevier B. V. All rights reserved.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 3.133
Times cited: 12
DOI: 10.1016/j.jallcom.2013.11.172
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“Co-Rich ZnCoO Nanoparticles Embedded in Wurtzite Zn1-xCoxO Thin Films: Possible Origin of Superconductivity”. Zeng Y-J, Gauquelin N, Li D-Y, Ruan S-C, He H-P, Egoavil R, Ye Z-Z, Verbeeck J, Hadermann J, Van Bael MJ, Van Haesendonck C, ACS applied materials and interfaces 7, 22166 (2015). http://doi.org/10.1021/acsami.5b06363
Abstract: Co-rich ZnCoO nanoparticles embedded in wurtzite Zn0.7Co0.3O thin films are grown by pulsed laser deposition on a Si substrate. Local superconductivity with an onset Tc at 5.9 K is demonstrated in the hybrid system. The unexpected superconductivity probably results from Co(3+) in the Co-rich ZnCoO nanoparticles or from the interface between the Co-rich nanoparticles and the Zn0.7Co0.3O matrix.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 7.504
Times cited: 13
DOI: 10.1021/acsami.5b06363
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“Texture-dependent twin formation in nanocrystalline thin Pd films”. Wang B, Idrissi H, Shi H, Colla MS, Michotte S, Raskin JP, Pardoen T, Schryvers D, Scripta materialia 66, 866 (2012). http://doi.org/10.1016/j.scriptamat.2012.01.038
Abstract: Nanocrystalline Pd films were produced by electron-beam evaporation and sputter deposition. The electron-beam-evaporated films reveal randomly oriented nanograins with a relatively high density of growth twins, unexpected in view of the high stacking fault energy of Pd. In contrast, sputter-deposited films show a clear 〈1 1 1〉 crystallographic textured nanostructure without twins. These results provide insightful information to guide the generation of microstructures with enhanced strength/ductility balance in high stacking fault energy nanocrystalline metallic thin films.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 3.747
Times cited: 19
DOI: 10.1016/j.scriptamat.2012.01.038
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“The effect of microstructure on the hydrogenation of Mg/Fe thin film multilayers”. Mooij L, Perkisas T, Palsson G, Schreuders H, Wolff M, Hjorvarsson B, Bals S, Dam B, International journal of hydrogen energy 39, 17092 (2014). http://doi.org/10.1016/j.ijhydene.2014.08.035
Abstract: Nanoconfined magnesium hydride can be simultaneously protected and thermodynamically destabilized when interfaced with materials such as Ti and Fe. We study the hydrogenation of thin layers of Mg (<14 nm) nanoconfined in one dimension within thin film Fe/Mg/Fe/Pd multilayers by the optical technique Hydrogenography. The hydrogenation of nanosized magnesium layers in Fe/Mg/Fe multilayers surprisingly shows the presence of multiple plateau pressures, whose nature is thickness dependent. In contrast, hydrogen desorption occurs via a single plateau which does not depend on the Mg layer thickness. From structural and morphological analyses with X-ray diffraction/reflectometry and cross-section TEM, we find that the Mg layer roughness is large when deposited on Fe and furthermore contains high-angle grain boundaries (GB's). When grown on Ti, the Mg layer roughness is low and no high-angle GB's are detected. From a Ti/Mg/Fe multilayer, in which the Mg layer is flat and has little or no GB's, we conclude that MgH2 is indeed destabilized by the interface with Fe. In this case, both the ab- and desorption plateau pressures are increased by a factor two compared to the hydrogenation of Mg within Ti/Mg/Ti multilayers. We hypothesize that the GB's in the Fe/Mg/Fe multilayer act as diffusion pathways for Pd, which is known to greatly alter the hydrogenation behavior of Mg when the two materials share an interface. Copyright (C) 2014, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 3.582
Times cited: 15
DOI: 10.1016/j.ijhydene.2014.08.035
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“Thermally induced structural and morphological changes of CdSe/CdS octapods”. Goris B, van Huis MA, Bals S, Zandbergen HW, Manna L, Van Tendeloo G, Small 8, 937 (2012). http://doi.org/10.1002/smll.201101897
Abstract: Branched nanostructures are of great interest because of their promising optical and electronic properties. For successful and reliable integration in applications such as photovoltaic devices, the thermal stability of the nanostructures is of major importance. Here the different domains (CdSe cores, CdS pods) of the heterogeneous octapods are shown to have different thermal stabilities, and heating is shown to induce specific shape changes. The octapods are heated from room temperature to 700 °C, and investigated using (analytical and tomographic) transmission electron microscopy (TEM). At low annealing temperatures, pure Cd segregates in droplets at the outside of the octapods, indicating non-stochiometric composition of the octapods. Furthermore, the tips of the pods lose their faceting and become rounded. Further heating to temperatures just below the sublimation temperature induces growth of the zinc blende core at the expense of the wurtzite pods. At higher temperatures, (500700 °C), sublimation of the octapods is observed in real time in the TEM. Three-dimensional tomographic reconstructions reveal that the four pods pointing into the vacuum have a lower thermal stability than the four pods that are in contact with the support.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 8.643
Times cited: 20
DOI: 10.1002/smll.201101897
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“Thin films of the spin ice compound Ho2Ti2O7”. Leusink DP, Coneri F, Hoek M, Turner S, Idrissi H, Van Tendeloo G, Hilgenkamp H, APL materials 2, 032101 (2014). http://doi.org/10.1063/1.4867222
Abstract: The pyrochlore compounds Ho2Ti2O7 and Dy2Ti2O7 show an exotic form of magnetism called the spin ice state, resulting from the interplay between geometrical frustration and ferromagnetic coupling. A fascinating feature of this state is the appearance of magnetic monopoles as emergent excitations above the degenerate ground state. Over the past years, strong effort has been devoted to the investigation of these monopoles and other properties of the spin ice state in bulk crystals. Here, we report the fabrication of Ho2Ti2O7 thin films using pulsed laser deposition on yttria-stabilized ZrO2 substrates. We investigated the structural properties of these films by X-ray diffraction, scanning transmission electron microscopy, and atomic force microscopy, and the magnetic properties by vibrating sample magnetometry at 2 K. The films not only show a high crystalline quality, but also exhibit the hallmarks of a spin ice: a pronounced magnetic anisotropy and an intermediate plateau in the magnetization along the [111] crystal direction.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 4.335
Times cited: 18
DOI: 10.1063/1.4867222
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“Three-dimensional elemental mapping at the atomic scale in bimetallic nanocrystals”. Goris B, de Backer A, Van Aert S, Gómez-Graña S, Liz-Marzán LM, Van Tendeloo G, Bals S, Nano letters 13, 4236 (2013). http://doi.org/10.1021/nl401945b
Abstract: A thorough understanding of the three-dimensional (3D) atomic structure and composition of coreshell nanostructures is indispensable to obtain a deeper insight on their physical behavior. Such 3D information can be reconstructed from two-dimensional (2D) projection images using electron tomography. Recently, different electron tomography techniques have enabled the 3D characterization of a variety of nanostructures down to the atomic level. However, these methods have all focused on the investigation of nanomaterials containing only one type of chemical element. Here, we combine statistical parameter estimation theory with compressive sensing based tomography to determine the positions and atom type of each atom in heteronanostructures. The approach is applied here to investigate the interface in coreshell Au@Ag nanorods but it is of great interest in the investigation of a broad range of nanostructures.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 12.712
Times cited: 90
DOI: 10.1021/nl401945b
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“Multiscale investigation of quasi-brittle fracture characteristics in a 9Cr–1Mo ferritic–martensitic steel embrittled by liquid lead–bismuth under low cycle fatigue”. Gong X, Marmy P, Volodin A, Amin-Ahmadi B, Qin L, Schryvers D, Gavrilov S, Stergar E, Verlinden B, Wevers M, Seefeldt M, Corrosion science 102, 137 (2016). http://doi.org/10.1016/j.corsci.2015.10.003
Abstract: Liquid metal embrittlement (LME) induced quasi-brittle fracture characteristics of a 9Cr–1Mo ferritic–martensitic steel (T91) after fatigue cracking in lead–bismuth eutectic (LBE) have been investigated at various length scales. The results show that the LME fracture morphology is primarily characterized by quasi-brittle translath flat regions partially covered by nanodimples, shallow secondary cracks propagating along the martensitic lath boundaries as well as tear ridges covered by micro dimples. These diverse LME fracture features likely indicate a LME mechanism involving multiple physical processes, such as weakening induced interatomic decohesion at the crack tip and plastic shearing induced nano/micro voiding in the plastic zone.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Times cited: 16
DOI: 10.1016/j.corsci.2015.10.003
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“Topological surface state enhanced photothermoelectric effect in Bi2Se3 nanoribbons”. Yan Y, Liao ZM, Ke X, Van Tendeloo G, Wang Q, Sun D, Yao W, Zhou S, Zhang L, Wu HC, Yu DP;, Nano letters 14, 4389 (2014). http://doi.org/10.1021/nl501276e
Abstract: The photothermoelectric effect in topological insulator Bi2Se3 nanoribbons is studied. The topological surface states are excited to be spin-polarized by circularly polarized light. Because the direction of the electron spin is locked to its momentum for the spin-helical surface states, the photothermoelectric effect is significantly enhanced as the oriented motions of the polarized spins are accelerated by the temperature gradient. The results are explained based on the microscopic mechanisms of a photon induced spin transition from the surface Dirac cone to the bulk conduction band. The as-reported enhanced photothermoelectric effect is expected to have potential applications in a spin-polarized power source.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 12.712
Times cited: 51
DOI: 10.1021/nl501276e
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“Towards atomic resolution in sodium titanate nanotubes using near-edge X-ray-absorption fine-structure spectromicroscopy combined with multichannel multiple-scattering calculations”. Bittencourt C, Krüger P, Lagos MJ, Ke X, Van Tendeloo G, Ewels C, Umek P, Guttmann P, Beilstein journal of nanotechnology 3, 789 (2012). http://doi.org/10.3762/bjnano.3.88
Abstract: Recent advances in near-edge X-ray-absorption fine-structure spectroscopy coupled with transmission X-ray microscopy (NEXAFS-TXM) allow large-area mapping investigations of individual nano-objects with spectral resolution up to E/Delta E = 104 and spatial resolution approaching 10 nm. While the state-of-the-art spatial resolution of X-ray microscopy is limited by nanostructuring process constrains of the objective zone plate, we show here that it is possible to overcome this through close coupling with high-level theoretical modelling. Taking the example of isolated bundles of hydrothermally prepared sodium titanate nanotubes ((Na,H)TiNTs) we are able to unravel the complex nanoscale structure from the NEXAFS-TXM data using multichannel multiple-scattering calculations, to the extent of being able to associate specific spectral features in the O K-edge and Ti L-edge with oxygen atoms in distinct sites within the lattice. These can even be distinguished from the contribution of different hydroxyl groups to the electronic structure of the (Na,H)TiNTs.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 3.127
Times cited: 13
DOI: 10.3762/bjnano.3.88
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“Towards Novel Multifunctional Pillared Nanostructures: Effective Intercalation of Adamantylamine in Graphene Oxide and Smectite Clays”. Spyrou K, Potsi G, Diamanti EK, Ke X, Serestatidou E, Verginadis II, Velalopoulou AP, Evangelou AM, Deligiannakis Y, Van Tendeloo G, Gournis D, Rudolf P;, Advanced functional materials 24, 5841 (2014). http://doi.org/10.1002/adfm.201400975
Abstract: Multifunctional pillared materials are synthesized by the intercalation of cage-shaped adamantylamine (ADMA) molecules into the interlayer space of graphite oxide (GO) and aluminosilicate clays. The physicochemical and structural properties of these hybrids, determined by X-ray diffraction (XRD), Fourier transform infrared (FTIR), Raman and X-ray photoemission (XPS) spectroscopies and transmission electron microscopy (TEM) show that they can serve as tunable hydrophobic/hydrophilic and stereospecific nanotemplates. Thus, in ADMA-pillared clay hybrids, the phyllomorphous clay provides a hydrophilic nanoenvironment where the local hydrophobicity is modulated by the presence of ADMA moieties. On the other hand, in the ADMA-GO hybrid, both the aromatic rings of GO sheets and the ADMA molecules define a hydrophobic nanoenvironment where sp(3)-oxo moieties (epoxy, hydroxyl and carboxyl groups), present on GO, modulate hydrophilicity. As test applications, these pillared nanostructures are capable of selective/stereospecific trapping of small chlorophenols or can act as cytotoxic agents.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 12.124
Times cited: 19
DOI: 10.1002/adfm.201400975
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“Vapor phase processing of \alpha-Fe2O3 photoelectrodes for water splitting : an insight into the structure/property interplay”. Warwick MEA, Kaunisto K, Barreca D, Carraro G, Gasparotto A, Maccato C, Bontempi E, Sada C, Ruoko TP, Turner S, Van Tendeloo G;, ACS applied materials and interfaces 7, 8667 (2015). http://doi.org/10.1021/acsami.5b00919
Abstract: Harvesting radiant energy to trigger water photoelectrolysis and produce clean hydrogen is receiving increasing attention in the search of alternative energy resources. In this regard, hematite (alpha-Fe2O3) nanostructures with controlled nano-organization have been fabricated and investigated for use as anodes in photoelectrochemical (PEC) cells. The target systems have been grown on conductive substrates by plasma enhanced-chemical vapor deposition (PE-CVD) and subjected to eventual ex situ annealing in air to further tailor their structure and properties. A detailed multitechnique approach has enabled to elucidate between system characteristics and the generated photocurrent. The present alpha-Fe2O3 systems are characterized by a high purity and hierarchical morphologies consisting of nanopyramids/organized dendrites, offering a high contact area with the electrolyte. PEC data reveal a dramatic response enhancement upon thermal treatment, related to a more efficient electron transfer. The reasons underlying such a phenomenon are elucidated and discussed by transient absorption spectroscopy (TAS) studies of photogenerated charge carrier kinetics, investigated on different time scales for the first time on PE-CVD Fe2O3 nanostructures.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 7.504
Times cited: 51
DOI: 10.1021/acsami.5b00919
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“VEGF-targeted magnetic nanoparticles for MRI visualization of brain tumor”. Abakumov MA, Nukolova NV, Sokolsky-Papkov M, Shein SA, Sandalova TO, Vishwasrao HM, Grinenko NF, Gubsky IL, Abakumov AM, Kabanov AV, Chekhonin VP;, Nanomedicine: nanotechnology, biology and medicine 11, 825 (2015). http://doi.org/10.1016/j.nano.2014.12.011
Abstract: This work is focused on synthesis and characterization of targeted magnetic nanoparticles as magnetic resonance imaging (MRI) agents for in vivo visualization of gliomas. Ferric oxide (Fe3O4) cores were synthesized by thermal decomposition and coated with bovine serum albumin (BSA) to form nanoparticles with D-eff of 53 +/- 9 nm. The BSA was further cross-linked to improve colloidal stability. Monoclonal antibodies against vascular endothelial growth factor (mAbVEGF) were covalently conjugated to BSA through a polyethyleneglycol linker. Here we demonstrate that 1) BSA coated nanoparticles are stable and non-toxic to different cells at concentration up to 2.5 mg/mL; 2) conjugation of monoclonal antibodies to nanoparticles promotes their binding to VEGF-positive glioma C6 cells in vitro; 3) targeted nanoparticles are effective in MRI visualization of the intracranial glioma. Thus, mAbVEGF-targeted BSA-coated magnetic nanoparticles are promising MRI contrast agents for glioma visualization. (C) 2015 Elsevier Inc. All rights reserved.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 5.72
Times cited: 62
DOI: 10.1016/j.nano.2014.12.011
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“Femtosecond Laser-Controlled Tip-to-Tip Assembly and Welding of Gold Nanorods”. Gonzalez-Rubio G, Gonzalez-Izquierdo J, Banares L, Tardajos G, Rivera A, Altantzis T, Bals S, Pena-Rodriguez O, Guerrero-Martinez A, Liz-Marzan LM, Nano letters 15, 8282 (2015). http://doi.org/10.1021/acs.nanolett.5b03844
Abstract: Directed assembly of gold nanorods through the use of dithiolated molecular linkers is one of the most efficient methodologies for the morphologically controlled tip-to-tip assembly of this type of anisotropic nanocrystals. However, in a direct analogy to molecular polymerization synthesis, this process is characterized by difficulties in chain-growth control over nanoparticle oligomers. In particular, it is nearly impossible to favor the formation of one type of oligomer, making the methodology hard to use for actual applications in nanoplasmonics. We propose here a light-controlled synthetic procedure that allows obtaining selected plasmonic oligomers in high yield and with reaction times in the scale of minutes by irradiation with low fluence near-infrared (NIR) femtosecond laser pulses. Selective inhibition of the formation of gold nanorod n-mers (trimers) with a longitudinal localized surface plasmon in resonance with a 800 nm Ti:sapphire laser, allowed efficient trapping of the (n – 1)-mers (dimers) by hot spot mediated photothermal decomposition of the interparticle molecular linkers. Laser irradiation at higher energies produced near-field enhancement at the interparticle gaps, which is large enough to melt gold nanorod tips, offering a new pathway toward tip-to-tip welding of gold nanorod oligomers with a plasmonic response at the NIR. Thorough optical and electron microscopy characterization indicates that plasmonic oligomers can be selectively trapped and welded, which has been analyzed in terms of a model that predicts with reasonable accuracy the relative concentrations of the main plasmonic species.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 12.712
Times cited: 101
DOI: 10.1021/acs.nanolett.5b03844
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“Collective Plasmonic Properties in Few-Layer Gold Nanorod Supercrystals”. Hamon C, Novikov SM, Scarabelli L, Solís DM, Altantzis T, Bals S, Taboada JM, Obelleiro F, Liz-Marzán LM, ACS Photonics 2, 1482 (2015). http://doi.org/10.1021/acsphotonics.5b00369
Abstract: Gold nanorod supercrystals have been widely employed for the detection of relevant bioanalytes with detection limits ranging from nano- to picomolar levels,
confirming the promising nature of these structures for biosensing. Even though a relationship between the height of the supercrystal (i.e., the number of stacked nanorod layers)and the enhancement factor has been proposed, no systematic
study has been reported. In order to tackle this problem, we prepared gold nanorod supercrystals with varying numbers of stacked layers and analyzed them extensively by atomic force microscopy, electron microscopy and surface enhanced Raman scattering. The experimental results were compared to numerical
simulations performed on real-size supercrystals composed of thousands of nanorod building blocks. Analysis of the hot spot distribution in the simulated supercrystals showed the presence of standing waves that were distributed at different depths, depending on the number of layers in each supercrystal. On the basis of these theoretical results, we interpreted the experimental
data in terms of analyte penetration into the topmost layer only, which indicates that diffusion to the interior of the supercrystals would be crucial if the complete field enhancement produced by the stacked nanorods is to be exploited. We propose that our conclusions will be of high relevance in the design of next generation plasmonic devices.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 6.756
Times cited: 70
DOI: 10.1021/acsphotonics.5b00369
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“Nanoscale mapping of plasmon and exciton in ZnO tetrapods coupled with Au nanoparticles”. Bertoni G, Fabbri F, Villani M, Lazzarini L, Turner S, Van Tendeloo G, Calestani D, Gradečak S, Zappettini A, Salviati G, Scientific reports 6, 19168 (2016). http://doi.org/10.1038/srep19168
Abstract: Metallic nanoparticles can be used to enhance optical absorption or emission in semiconductors, thanks to a strong interaction of collective excitations of free charges (plasmons) with electromagnetic fields. Herein we present the direct imaging at the nanoscale of plasmon-exciton coupling in Au/ZnO nanostructures by combining scanning transmission electron energy loss and cathodoluminescence spectroscopy and mapping. The Au nanoparticles (~30 nm in diameter) are grown in-situ on ZnO nanotetrapods by means of a photochemical process without the need of binding agents or capping molecules. This results in clean interfaces, enabling to prove the occurrence of the plasmon-exciton coupling and the straightforward mapping of its spatial localization. Interestingly, the Au plasmon resonance is localized at the Au/vacuum interface, rather than presenting an isotropic distribution around the nanoparticle. On the contrary, a strong localization of the ZnO excitons, has been observed inside the Au nanoparticle, revealing the existence of the plasmon-exciton coupling, as also confirmed by numerical simulations.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 4.259
Times cited: 15
DOI: 10.1038/srep19168
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“Visualization of O-O peroxo-like dimers in high-capacity layered oxides for Li-ion batteries”. McCalla E, Abakumov AM, Saubanere M, Foix D, Berg EJ, Rousse G, Doublet M-L, Gonbeau D, Novak P, Van Tendeloo G, Dominko R, Tarascon J-M, Science 350, 1516 (2015). http://doi.org/10.1126/science.aac8260
Abstract: Lithium-ion (Li-ion) batteries that rely on cationic redox reactions are the primary energy source for portable electronics. One pathway toward greater energy density is through the use of Li-rich layered oxides. The capacity of this class of materials (>270 milliampere hours per gram) has been shown to be nested in anionic redox reactions, which are thought to form peroxo-like species. However, the oxygen-oxygen (O-O) bonding pattern has not been observed in previous studies, nor has there been a satisfactory explanation for the irreversible changes that occur during first delithiation. By using Li2IrO3 as a model compound, we visualize the O-O dimers via transmission electron microscopy and neutron diffraction. Our findings establish the fundamental relation between the anionic redox process and the evolution of the O-O bonding in layered oxides.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 37.205
Times cited: 281
DOI: 10.1126/science.aac8260
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“Atomic Layer Deposition of Pt Nanoparticles within the Cages of MIL-101: A Mild and Recyclable Hydrogenation Catalyst”. Leus K, Dendooven J, Tahir N, Ramachandran R, Meledina M, Turner S, Van Tendeloo G, Goeman J, Van der Eycken J, Detavernier C, Van Der Voort P, Nanomaterials 6, 45 (2016). http://doi.org/10.3390/nano6030045
Abstract: We present the in situ synthesis of Pt nanoparticles within MIL-101-Cr (MIL = Materials Institute Lavoisier) by means of atomic layer deposition (ALD). The obtained Pt@MIL-101 materials were characterized by means of N2 adsorption and X-ray powder diffraction (XRPD) measurements, showing that the structure of the metal organic framework was well preserved during the ALD deposition. X-ray fluorescence (XRF) and transmission electron microscopy (TEM) analysis confirmed the deposition of highly dispersed Pt nanoparticles with sizes determined by the MIL-101-Cr pore sizes and with an increased Pt loading for an increasing number of ALD cycles. The Pt@MIL-101 material was examined as catalyst in the hydrogenation of different linear and cyclic olefins at room temperature, showing full conversion for each substrate. Moreover, even under solvent free conditions, full conversion of the substrate was observed. A high concentration test has been performed showing that the Pt@MIL-101 is stable for a long reaction time without loss of activity, crystallinity and with very low Pt leaching.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 3.553
Times cited: 19
DOI: 10.3390/nano6030045
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“Single Particle Deformation and Analysis of Silica-Coated Gold Nanorods before and after Femtosecond Laser Pulse Excitation”. Albrecht W, Deng T-S, Goris B, van Huis MA, Bals S, van Blaaderen A, Nano letters 16, 1818 (2016). http://doi.org/10.1021/acs.nanolett.5b04851
Abstract: We performed single particle deformation experiments on silica-coated gold nanorods under femtosecond (fs) illumination. Changes in the particle shape were analyzed by electron microscopy and associated changes in the plasmon resonance by electron energy loss spectroscopy. Silica-coated rods were found to be more stable compared to uncoated rods but could still be deformed via an intermediate bullet-like shape for silica shell thicknesses of 14 nm. Changes in the size ratio of the rods after fs-illumination resulted in blue-shifting of the longitudinal plasmon resonances. Two-dimensional spatial mapping of the plasmon resonances revealed that the flat side of the bullet-like particles showed a less pronounced longitudinal plasmonic electric field enhancement. These findings were confirmed by finite-difference time-domain (FDTD) simulations. Furthermore, at higher laser fluences size reduction of the particles was found as well as for particles that were not completely deformed yet.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 12.712
Times cited: 55
DOI: 10.1021/acs.nanolett.5b04851
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“Large pinning forces and matching effects in YBa2Cu3O7-&delta, thin films with Ba2Y(Nb/Ta)O6 nano-precipitates”. Opherden L, Sieger M, Pahlke P, Hühne R, Schultz L, Meledin A, Van Tendeloo G, Nast R, Holzapfel B, Bianchetti M, MacManus-Driscoll JL, Hänisch J, Scientific reports 6, 21188 (2016). http://doi.org/10.1038/srep21188
Abstract: The addition of mixed double perovskite Ba2Y(Nb/Ta)O6 (BYNTO) to YBa2Cu3O7−δ (YBCO) thin films leads to a large improvement of the in-field current carrying capability. For low deposition rates, BYNTO grows as well-oriented, densely distributed nanocolumns. We achieved a pinning force density of 25 GN/m3 at 77 K at a matching field of 2.3 T, which is among the highest values reported for YBCO. The anisotropy of the critical current density shows a complex behavior whereby additional maxima are developed at field dependent angles. This is caused by a matching effect of the magnetic fields c-axis component. The exponent N of the current-voltage characteristics (inversely proportional to the creep rate S) allows the depinning mechanism to be determined. It changes from a double-kink excitation below the matching field to pinning-potential-determined creep above it.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 4.259
Times cited: 39
DOI: 10.1038/srep21188
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“Direct Imaging of ALD Deposited Pt Nanoclusters inside the Giant Pores of MIL-101”. Meledina M, Turner S, Filippousi M, Leus K, Lobato I, Ramachandran RK, Dendooven J, Detavernier C, Van Der Voort P, Van Tendeloo G, Particle and particle systems characterization 33, 382 (2016). http://doi.org/10.1002/ppsc.201500252
Abstract: MIL-101 giant-pore metal-organic framework (MOF) materials have been loaded with Pt nanoparticles using atomic layer deposition. The final structure has been investigated by aberration-corrected annular dark-field scanning transmission electron microscopy under strictly controlled low dose conditions. By combining the acquired experimental data with image simulations, the position of the small clusters within the individual pores of a metal-organic framework has been determined. The embedding of the Pt nanoparticles is confirmed by electron tomography, which shows a distinct ordering of the highly uniform Pt nanoparticles. The results show that atomic layer deposition is particularly well-suited for the deposition of individual nanoparticles inside MOF framework pores and that, upon proper regulation of the incident electron dose, annular dark-field scanning transmission electron microscopy is a powerful tool for the characterization of this type of materials at a local scale.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 4.474
Times cited: 11
DOI: 10.1002/ppsc.201500252
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“A New Method for Quantitative XEDS Tomography of Complex Heteronanostructures”. Zanaga D, Altantzis T, Polavarapu L, Liz-Marzán LM, Freitag B, Bals S, Particle and particle systems characterization 33, 396 (2016). http://doi.org/10.1002/ppsc.201600021
Abstract: Reliable quantification of 3D results obtained by X-ray Energy Dispersive Spectroscopy (XEDS) tomography is currently hampered by the presence of shadowing effects and poor spatial resolution. Here, we present a method that overcomes these problems by synergistically combining quantified XEDS data and High Angle Annular Dark Field – Scanning Transmission Electron Microscopy (HAADF-STEM) tomography. As a proof of principle, the approach is applied to characterize a complex Au/Ag nanorattle obtained through a galvanic replacement reaction. However, the technique we propose here is widely applicable to a broad range of nanostructures.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 4.474
Times cited: 29
DOI: 10.1002/ppsc.201600021
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“Domain Selectivity in BiFeO3Thin Films by Modified Substrate Termination”. Solmaz A, Huijben M, Koster G, Egoavil R, Gauquelin N, Van Tendeloo G, Verbeeck J, Noheda B, Rijnders G, Advanced functional materials 26, 2882 (2016). http://doi.org/10.1002/adfm.201505065
Abstract: Ferroelectric domain formation is an essential feature in ferroelectric thin films. These domains and domain walls can be manipulated depending on the growth conditions. In rhombohedral BiFeO3 thin films, the ordering of the domains and the presence of specific types of domain walls play a crucial role in attaining unique ferroelectric and magnetic properties. In this study, controlled ordering of domains in BiFeO3 film is presented, as well as a controlled selectivity between two types of domain walls is presented, i.e., 71° and 109°, by modifying the substrate termination. The experiments on two different substrates, namely SrTiO3 and TbScO3, strongly indicate that the domain selectivity is determined by the growth kinetics of the initial BiFeO3 layers.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 12.124
Times cited: 34
DOI: 10.1002/adfm.201505065
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“Dislocation/hydrogen interaction mechanisms in hydrided nanocrystalline palladium films”. Amin-Ahmadi B, Connétable D, Fivel M, Tanguy D, Delmelle R, Turner S, Malet L, Godet S, Pardoen T, Proost J, Schryvers D, Idrissi H, Acta materialia 111, 253 (2016). http://doi.org/10.1016/j.actamat.2016.03.054
Abstract: The nanoscale plasticity mechanisms activated during hydriding cycles in sputtered nanocrystalline Pd films have been investigated ex-situ using advanced transmission electron microscopy techniques. The internal stress developing within the films during hydriding has been monitored in-situ. Results showed that in Pd films hydrided to β-phase, local plasticity was mainly controlled by dislocation activity in spite of the small grain size. Changes of the grain size distribution and the crystallographic texture have not been observed. In contrast, significant microstructural changes were not observed in Pd films hydrided to α-phase. Moreover, the effect of hydrogen loading on the nature and density of dislocations has been investigated using aberration-corrected TEM. Surprisingly, a high density of shear type stacking faults has been observed after dehydriding, indicating a significant effect of hydrogen on the nucleation energy barriers of Shockley partial dislocations. Ab-initio calculations of the effect of hydrogen on the intrinsic stable and unstable stacking fault energies of palladium confirm the experimental observations.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 5.301
Times cited: 14
DOI: 10.1016/j.actamat.2016.03.054
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“Effect of cation dopant radius on the hydrothermal stability of tetragonal zirconia: Grain boundary segregation and oxygen vacancy annihilation”. Zhang F, Batuk M, Hadermann J, Manfredi G, Mariën A, Vanmeensel K, Inokoshi M, Van Meerbeek B, Naert I, Vleugels J, Acta materialia 106, 48 (2016). http://doi.org/10.1016/j.actamat.2015.12.051
Abstract: The hydrothermal aging stability of 3Y-TZP-xM2O3 (M = La, Nd, Sc) was investigated as a function of 0.02–5 mol% M2O3 dopant content and correlated to the overall phase content, t-ZrO2 lattice parameters, grain size distribution, grain boundary chemistry and ionic conductivity.
The increased aging stability with increasing Sc2O3 content and the optimum content of 0.4–0.6 mol% Nd2O3 or 0.2–0.4 mol% La2O3, resulting in the highest aging resistance, could be directly related to the constituent phases and the lattice parameters of the remaining tetragonal zirconia.
At low M2O3 dopant contents ≤0.4 mol%, the different aging behavior of tetragonal zirconia was attributed to the defect structure of the zirconia grain boundary which was influenced by the dopant cation radius. It was observed that the grain boundary ionic resistivity and the aging resistance followed the same trend: La3+ > Nd3+ > Al3+ > Sc3+, proving that hydrothermal aging is driven by the diffusion of water-derived mobile species through the oxygen vacancies. Accordingly, we elucidated the underlying mechanism by which a larger trivalent cation segregating at the zirconia grain boundary resulted in a higher aging resistance.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 5.301
Times cited: 37
DOI: 10.1016/j.actamat.2015.12.051
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“Enhanced 77K vortex-pinning in YBa2Cu3O7−x films with Ba2YTaO6 and mixed Ba2YTaO6 + Ba2YNbO6 nano-columnar inclusions with irreversibility field to 11T”. Rizzo F, Augieri A, Angrisani Armenio A, Galluzzi V, Mancini A, Pinto V, Rufoloni A, Vannozzi A, Bianchetti M, Kursumovic A, MacManus-Driscoll JL, Meledin A, Van Tendeloo G, Celentano G, APL materials 4, 061101 (2016). http://doi.org/10.1063/1.4953436
Abstract: Pulsed laser deposited thin YBa2Cu3O7−x (YBCO) films with pinning additions of 5at.% Ba2YTaO6 (BYTO) were compared to films with 2.5at.% Ba2YTaO6 + 2.5at.% Ba2YNbO6 (BYNTO) additions. Excellent magnetic flux-pinning at 77 K was obtained with remarkably high irreversibility fields greater than 10T (YBCO-BYTO) and 11T (YBCO-BYNTO), representing the highest ever achieved values in YBCO films.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 4.335
Times cited: 19
DOI: 10.1063/1.4953436
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“Gold Nanostar-Coated Polystyrene Beads as Multifunctional Nanoprobes for SERS Bioimaging”. Serrano-Montes AB, Langer J, Henriksen-Lacey M, Jimenez de Aberasturi D, Solís DM, Taboada JM, Obelleiro F, Sentosun K, Bals S, Bekdemir A, Stellacci F, Liz-Marzán LM, The journal of physical chemistry: C : nanomaterials and interfaces 120, 20860 (2016). http://doi.org/10.1021/acs.jpcc.6b02282
Abstract: Hybrid colloidal nanocomposites comprising polystyrene beads and plasmonic gold nanostars are reported as multifunctional optical nanoprobes. Such self-assembled structures are excellent Raman enhancers for bio-applications as they feature plasmon modes in the near infrared “first biological transparency window”. In this proof of concept study, we used 4- mercaptobenzoic acid as a Raman-active molecule to optimize the density of gold nanostars on polystyrene beads, improving SERS performance and thereby allowing in vitro cell culture imaging. Interestingly, intermediate gold nanostar loadings were found to yield higher SERS response, which was confirmed by electromagnetic modeling. These engineered hybrid nanostructures notably improve the possibilities of using gold nanostars as SERS tags. Additionally, when fluorescently labeled polystyrene bead are used as colloidal carriers, the composite particles can be applied as promising tools for multimodal bioimaging.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 4.536
Times cited: 64
DOI: 10.1021/acs.jpcc.6b02282
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“Encapsulation of Single Plasmonic Nanoparticles within ZIF-8 and SERS Analysis of the MOF Flexibility”. Zheng G, de Marchi S, Lopez-Puente V, Sentosun K, Polavarapu L, Perez-Juste I, Hill EH, Bals S, Liz-Marzan LM, Pastoriza-Santos I, Perez-Juste J, Small 12, 3935 (2016). http://doi.org/10.1002/smll.201600947
Abstract: Hybrid nanostructures composed of metal nanoparticles and metal-organic frameworks (MOFs) have recently received increasing attention toward various applications due to the combination of optical and catalytic properties of nanometals with the large internal surface area, tunable crystal porosity and unique chemical properties of MOFs. Encapsulation of metal nanoparticles of well-defined shapes into porous MOFs in a core-shell type configuration can thus lead to enhanced stability and selectivity in applications such as sensing or catalysis. In this study, the encapsulation of single noble metal nanoparticles with arbitrary shapes within zeolitic imidazolate-based metal organic frameworks (ZIF-8) is demonstrated. The synthetic strategy is based on the enhanced interaction between ZIF-8 nanocrystals and metal nanoparticle surfaces covered by quaternary ammonium surfactants. High resolution electron microscopy and tomography confirm a complete core-shell morphology. Such a well-defined morphology allowed us to study the transport of guest molecules through the ZIF-8 porous shell by means of surface-enhanced Raman scattering by the metal cores. The results demonstrate that even molecules larger than the ZIF-8 aperture and pore size may be able to diffuse through the framework and reach the metal core.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 8.643
Times cited: 140
DOI: 10.1002/smll.201600947
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“Quantifying a Heterogeneous Ru Catalyst on Carbon Black Using ADF STEM”. Varambhia AM, Jones L, De Backer A, Fauske VT, Van Aert S, Ozkaya D, Nellist PD, Particle and particle systems characterization 33, 438 (2016). http://doi.org/10.1002/ppsc.201600067
Abstract: Ru catalysts are part of a set of late transition metal nanocatalysts that have garnered much interest for catalytic applications such as ammonia synthesis and fuel cell production. Their performance varies greatly depending on their morphology and size, these catalysts are widely studied using electron microscopy. Using recent developments in Annular Dark Field (ADF) Scanning Transmission Electron Microscopy (STEM) quantification techniques, a rapid atom counting procedure was utilized to document the evolution of a heterogeneous Ru catalyst supported on carbon black. Areas of the catalyst were imaged for approximately 15 minutes using ADF STEM. When the Ru clusters were exposed to the electron beam, the clusters changed phase from amorphous to crystalline. To quantify the thickness of the crystalline clusters, two techniques were applied (simulation and statistical decomposition) and compared. These techniques show that stable face centredcubic crystal structures in the form of rafts, between 2 and 8 atoms thick, were formed after the initial wetting of the carbon support.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 4.474
Times cited: 4
DOI: 10.1002/ppsc.201600067
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