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“Thermal Stability of CoAu13Binary Nanoparticle Superlattices under the Electron Beam”. Altantzis T, Yang Z, Bals S, Van Tendeloo G, Pileni M-P, Chemistry of materials 28, 716 (2016). http://doi.org/10.1021/acs.chemmater.5b04898
Abstract: One primary goal of self-assembly in nanoscale regime is to implement multifunctional binary nanoparticle superlattices into practical use. In the last decade, considerable effort has been put into the fabrication of binary nanoparticle superlattices with controllable structure and stoichiometry. However, limited effort has been made in order to improve the stability of these binary nanoparticle superlattices, which is a prerequisite for their potential application. In this work, we demonstrate that the carbon deposition from specimen contamination can play an auxiliary role during the heat treatment of binary nanoparticle superlattices. With the in-situ carbon matrix formation, the thermal stability of CoAu 13 binary nanoparticle superlattices is unambiguously enhanced.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 9.466
Times cited: 10
DOI: 10.1021/acs.chemmater.5b04898
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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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“Easily doped p-type, low hole effective mass, transparent oxides”. Sarmadian N, Saniz R, Partoens B, Lamoen D, Scientific reports 6, 20446 (2016). http://doi.org/10.1038/srep20446
Abstract: Fulfillment of the promise of transparent electronics has been hindered until now largely by the lack of semiconductors that can be doped p-type in a stable way, and that at the same time present high hole mobility and are highly transparent in the visible spectrum. Here, a high-throughput study based on first-principles methods reveals four oxides, namely X2SeO2, with X = La, Pr, Nd, and Gd, which are unique in that they exhibit excellent characteristics for transparent electronic device applications – i.e., a direct band gap larger than 3.1 eV, an average hole effective mass below the electron rest mass, and good p-type dopability. Furthermore, for La2SeO2 it is explicitly shown that Na impurities substituting La are shallow acceptors in moderate to strong anion-rich growth conditions, with low formation energy, and that they will not be compensated by anion vacancies VO or VSe.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT)
Impact Factor: 4.259
Times cited: 55
DOI: 10.1038/srep20446
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“Direct imaging of boron segregation at dislocations in B:diamond heteroepitaxial films”. Turner S, Idrissi H, Sartori AF, Korneychuck S, Lu Y-G, Verbeeck J, Schreck M, Van Tendeloo G, Nanoscale 8, 2212 (2016). http://doi.org/10.1039/c5nr07535a
Abstract: A thin film of heavily B-doped diamond has been grown epitaxially by microwave plasma chemical vapor deposition on an undoped diamond layer, on top of a Ir/YSZ/Si(001) substrate stack, to study the boron segregation and boron environment at the dislocations present in the film. The density and nature of the dislocations were investigated by conventional and weak-beam dark-field transmission electron microscopy techniques, revealing the presence of two types of dislocations: edge and mixed-type 45 degrees dislocations. The presence and distribution of B in the sample was studied using annular dark-field scanning transmission electron microscopy and spatially resolved electron energy-loss spectroscopy. Using these techniques, a segregation of B at the dislocations in the film is evidenced, which is shown to be intermittent along the dislocation. A single edge-type dislocation was selected to study the distribution of the boron surrounding the dislocation core. By imaging this defect at atomic resolution, the boron is revealed to segregate towards the tensile strain field surrounding the edge-type dislocations. An investigation of the fine structure of the B-K edge at the dislocation core shows that the boron is partially substitutionally incorporated into the diamond lattice and partially present in a lower coordination (sp(2)-like hybridization).
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 7.367
Times cited: 15
DOI: 10.1039/c5nr07535a
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“AVPO4F (A = Li, K): A 4 V Cathode Material for High-Power Rechargeable Batteries”. Fedotov SS, Khasanova NR, Samarin AS, Drozhzhin OA, Batuk D, Karakulina OM, Hadermann J, Abakumov AM, Antipov EV, Chemistry of materials 28, 411 (2016). http://doi.org/10.1021/acs.chemmater.5b04065
Abstract: A novel potassium-based fluoride-phosphate, KVPO4F, with a KTiOPO4 (KTP) type structure is synthesized and characterized. About 85% of potassium has been electrochemically extracted on oxidation producing a cathode material with attractive performance for Li-ion batteries. The material operates at the electrode potential near 4V vs Li/Li+ exhibiting a sloping voltage profile, extremely low polarization, small volume change of about 2% and excellent rate capability, maintaining more than 75% of the initial capacity at 40C discharge rate without significant fading.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 9.466
Times cited: 46
DOI: 10.1021/acs.chemmater.5b04065
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“Trapping of Oxygen Vacancies at Crystallographic Shear Planes in Acceptor-Doped Pb-Based Ferroelectrics”. Batuk D, Batuk M, Tsirlin AA, Hadermann J, Abakumov AM, Angewandte Chemie: international edition in English 54, 14787 (2015). http://doi.org/10.1002/anie.201507729
Abstract: The defect chemistry of the ferroelectric material PbTiO3 after doping with Fe(III) acceptor ions is reported. Using advanced transmission electron microscopy and powder X-ray and neutron diffraction, we demonstrate that even at concentrations as low as circa 1.7% (material composition approximately ABO2.95), the oxygen vacancies are trapped into extended planar defects, specifically crystallographic shear planes. We investigate the evolution of these defects upon doping and unravel their detailed atomic structure using the formalism of superspace crystallography, thus unveiling their role in nonstoichiometry in the Pb-based perovskites.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 11.994
Times cited: 3
DOI: 10.1002/anie.201507729
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“Plasmonic ‘rainbow&rsquo, photocatalyst with broadband solar light response for environmental applications”. Verbruggen SW, Keulemans M, Goris B, Blommaerts N, Bals S, Martens JA, Lenaerts S, Applied catalysis : B : environmental 188, 147 (2016). http://doi.org/10.1016/j.apcatb.2016.02.002
Abstract: We propose the concept of a ‘rainbow’ photocatalyst that consists of TiO2 modified with gold-silver alloy nanoparticles of various sizes and compositions, resulting in a broad plasmon absorption band that covers the entire UV–vis range of the solar spectrum. It is demonstrated that this plasmonic ‘rainbow’ photocatalyst is 16% more effective than TiO2 P25 under both simulated and real solar light for pollutant degradation at the solid-gas interface. With this we provide a promising strategy to maximize the spectral response for solar to chemical energy conversion.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 9.446
Times cited: 47
DOI: 10.1016/j.apcatb.2016.02.002
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“Ferroelastic switching in a layered-perovskite thin film”. Wang C, Ke X, Wang J, Liang R, Luo Z, Tian Y, Yi D, Zhang Q, Wang J, Han X-F, Van Tendeloo G, Chen L-Q, Nan C-W, Ramesh R, Zhang J, Nature communications 7, 10636 (2016). http://doi.org/10.1038/ncomms10636
Abstract: A controllable ferroelastic switching in ferroelectric/multiferroic oxides is highly desirable due to the non-volatile strain and possible coupling between lattice and other order parameter in heterostructures. However, a substrate clamping usually inhibits their elastic deformation in thin films without micro/nano-patterned structure so that the integration of the non-volatile strain with thin film devices is challenging. Here, we report that reversible in-plane elastic switching with a non-volatile strain of approximately 0.4% can be achieved in layered-perovskite Bi2WO6 thin films, where the ferroelectric polarization rotates by 90 degrees within four in-plane preferred orientations. Phase-field simulation indicates that the energy barrier of ferroelastic switching in orthorhombic Bi2WO6 film is ten times lower than the one in PbTiO3 films, revealing the origin of the switching with negligible substrate constraint. The reversible control of the in-plane strain in this layered-perovskite thin film demonstrates a new pathway to integrate mechanical deformation with nanoscale electronic and/or magnetoelectronic applications.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 12.124
Times cited: 40
DOI: 10.1038/ncomms10636
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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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“Melting temperatures and possible precursor plastic phases of CCl4and GeI4as a function of pressure”. Matthai CC, Lamoen D, March NH, Physics and chemistry of liquids 54, 130 (2016). http://doi.org/10.1080/00319104.2015.1068666
Abstract: The motivation for the present study is to be found in the recent experiments of Fuchizaki and Hamaya on GeI4. They observed a rapid increase in the melting temperature Tm in going from atmospheric pressure to p ~ 2.6 GPa. Tm was found to be largely independent of pressure above this value. In this paper, heuristic arguments are presented to support the idea that until some critical pressure, a crystalline phase of SnI4, CCl4 and GeI4 molecular solids melts into a low density liquid. However, at this critical pressure, a phase boundary intersects Tm(p), separating a low density liquid phase from a high density liquid. The new phase boundary is between the crystal and an amorphous molecular solid with increasing polymerisation as the pressure is increased.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 1.145
DOI: 10.1080/00319104.2015.1068666
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“A La2−xGdxZr2O7layer deposited by chemical solution: a promising seed layer for the fabrication of high Jcand low cost coated conductors”. Muguerra H, Pescheux A-C, Meledin A, Van Tendeloo G, Soubeyroux J-L, Journal of materials chemistry C : materials for optical and electronic devices 3, 11766 (2015). http://doi.org/10.1039/C5TC03365A
Abstract: We deposited La2-xGdxZr2O7 seed layers by a chemical solution method on a Ni-5%W substrate to study the influence of these layers on the growth process of a 60 nm-thick La2Zr2O7 layer. We measured the performances of these new buffer layers integrated in a coated conductor with a 300 nm-thick Y0.5Gd0.5Ba2Cu3O7-x layer. For the seed layers{,} we considered two different gadolinium contents (x = 0.2 and x = 0.8) and three different thicknesses for these compositions (20 nm{,} 40 nm{,} and 60 nm). The most promising buffer layer stacks are those with 20 nm of the La1.8Gd0.2Zr2O7 layer or La1.2Gd0.8Zr2O7. Indeed the La2-xGdxZr2O7/La2Zr2O7 films are highly textured{,} similar to a 100 nm-thick La2Zr2O7 layer{,} but their roughness is four times lower. Moreover they contain less and smaller pores in the seed layer than a pure La2Zr2O7 layer. The surface of La2Zr2O7 is also homogenous and crystalline with an orientation deviation from the ideal ?011? (100) direction below 10[degree]. With the 20 nm La2-xGdxZr2O7 seed layers we obtain in the coated conductors an efficiently textured transfer with no gradual degradation from the substrate throughout the superconducting layer. The highest Tc and Jc values are achieved with the La1.8Gd0.2Zr2O7 layer and are{,} respectively{,} 91 K and 1.4 MA cm-2. This trend seems to be due to an improvement of the surface quality of the Ni5%W substrate by the addition of a thin seed layer. Our results offer the potential of the La2-xGdxZr2O7 seed layers as promising alternatives for the classic Ni-5%W/LZO/CeO2/YBCO architectures.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 5.256
Times cited: 4
DOI: 10.1039/C5TC03365A
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“Triple-Modal Imaging of Magnetically-Targeted Nanocapsules in Solid TumoursIn Vivo”. Bai J, Wang JT-W, Rubio N, Protti A, Heidari H, Elgogary R, Southern P, Al-Jamal W' T, Sosabowski J, Shah AM, Bals S, Pankhurst QA, Al-Jamal KT, Theranostics 6, 342 (2016). http://doi.org/10.7150/thno.11918
Abstract: Triple-modal imaging magnetic nanocapsules, encapsulating hydrophobic superparamagnetic iron oxide nanoparticles, are formulated and used to magnetically target solid tumours after intravenous administration in tumour-bearing mice. The engineered magnetic polymeric nanocapsules m-NCs are ~200 nm in size with negative Zeta potential and shown to be spherical in shape. The loading efficiency of superparamagnetic iron oxide nanoparticles in the m-NC was ~100%. Up to ~3- and ~2.2-fold increase in tumour uptake at 1 and 24 h was achieved, when a static magnetic field was applied to the tumour for 1 hour. m-NCs, with multiple imaging probes (e.g. indocyanine green, superparamagnetic iron oxide nanoparticles and indium-111), were capable of triple-modal imaging (fluorescence/magnetic resonance/nuclear imaging) in vivo. Using triple-modal imaging is to overcome the intrinsic limitations of single modality imaging and provides complementary information on the spatial distribution of the nanocarrier within the tumour. The significant findings of this study could open up new research perspectives in using novel magnetically-responsive nanomaterials in magnetic-drug targeting combined with multi-modal imaging.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 8.712
Times cited: 54
DOI: 10.7150/thno.11918
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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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“A versatile lab-on-chip test platform to characterize elementary deformation mechanisms and electromechanical couplings in nanoscopic objects”. Pardoen T, Colla M-S, Idrissi H, Amin-Ahmadi B, Wang B, Schryvers D, Bhaskar UK, Raskin J-P, Comptes rendus : physique 17, 485 (2016). http://doi.org/10.1016/j.crhy.2015.11.005
Abstract: A nanomechanical on-chip test platform has recently been developed to deform under a variety of loading conditions freestanding thin films, ribbons and nanowires involving submicron dimensions. The lab-on-chip involves thousands of elementary test structures from which the elastic modulus, strength, strain hardening, fracture, creep properties can be extracted. The technique is amenable to in situ transmission electron microscopy (TEM) investigations to unravel the fundamental underlying deformation and fracture mechanisms that often lead to size-dependent effects in small-scale samples. The method allows addressing electrical and magnetic couplings as well in order to evaluate the impact of large mechanical stress levels on different solid-state physics phenomena. We had the chance to present this technique in details to Jacques Friedel in 2012 who, unsurprisingly, made a series of critical and very relevant suggestions. In the spirit of his legacy, the paper will address both mechanics of materials related phenomena and couplings with solids state physics issues.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.048
Times cited: 7
DOI: 10.1016/j.crhy.2015.11.005
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“Microstructural Characterization and Transformation Behavior of Porous Ni50.8Ti49.2”. Yao X, Cao S, Zhang XP, Schryvers D, Materials Today: Proceedings 2, S833 (2015). http://doi.org/10.1016/j.matpr.2015.07.411
Abstract: Porous Ni50.8Ti49.2 bulk material was prepared by powder metallurgy sintering. Solid solution and aging treatments were applied to improve the phase homogeneity and phase transformation behavior. Scanning and transmission electron microscopy, aided by energy dispersive X-ray analysis, were used to study the microstructure and chemical phase content of the alloys. In-situ cooling was carried out to observe the phase transformation behavior. As-received material contains dispersed Ni2Ti4O particles while Ni4Ti3 precipitates appear after aging. Close to pore edges, the latter have a preferential orientation due to the induced stress fields in the matrix.
Keywords: P1 Proceeding; Electron microscopy for materials research (EMAT)
DOI: 10.1016/j.matpr.2015.07.411
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“Optimization of Automated Crystal Orientation and Phase Mapping in TEM Applied to Ni-Ti All Round Shape Memory Alloy”. Yao X, Li Y, Cao S, Ma X, Zhang X-ping, Schryvers D, MATEC web of conferences
T2 –, Proceedings of ESOMAT 2015 10th European Symposium on Martensitic Transformations, September 14-18, 2015, Antwerp, Belgium 33, 03022 (2015). http://doi.org/10.1051/matecconf/20153303022
Abstract: A new application which focuses on an artificial sphincter fabricated by Ni-Ti SMAs for human implantation is under investigation by applying the all-round shape memory effect with precise control of the phase transformation temperatures. In this study, a Ni51at.%-Ti alloy was fabricated by arc melting with fast solidification, followed by a proper strained aging which induces the two way shape memory effect needed for this particular application. Differential scanning calorimetry was used to investigate the thermal behavior and transmission electron microscopy was used for studying the microstructure of the alloys. With the latter the novel technique of automated crystal orientation microscopy is used and optimized to obtain phase and orientation mapping of the various structures.
Keywords: P1 Proceeding; Electron microscopy for materials research (EMAT)
Times cited: 1
DOI: 10.1051/matecconf/20153303022
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“Heterogeneous interfacial chemical nature and bonds in a W-coated diamond/Al composite”. Ji G, Tan Z, Lu Y, Schryvers D, Li Z, Zhang D, Materials characterization 112, 129 (2016). http://doi.org/10.1016/j.matchar.2015.12.013
Abstract: Heterogeneous Al/Al4C3/Al2O3/diamond{111}, Al/nanolayered Al4C3/diamond{111} and Al12W particle/Al4C3/Al2O3/diamond{111} multi-interfaces have been developed at the nanoscale in a W-coated diamond/Al composite produced by vacuum hot pressing. The formation of nanoscale Al4C3 crystals is strongly associated with local O enrichment and can be further promoted by Al12W interfacial particles. The latter effectively contributes to enhance interfacial chemical bonding reducing interfacial thermal resistance and, in turn, enhancing thermal conductivity.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 2.714
Times cited: 7
DOI: 10.1016/j.matchar.2015.12.013
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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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“Epitaxial YBa2Cu3O7−xnanocomposite thin films from colloidal solutions”. Cayado P, De Keukeleere K, Garzón A, Perez-Mirabet L, Meledin A, De Roo J, Vallés F, Mundet B, Rijckaert H, Pollefeyt G, Coll M, Ricart S, Palau A, Gázquez J, Ros J, Van Tendeloo G, Van Driessche I, Puig T, Obradors X, Superconductor science and technology 28, 124007 (2015). http://doi.org/10.1088/0953-2048/28/12/124007
Abstract: A methodology of general validity to prepare epitaxial nanocomposite films based on the use of colloidal solutions containing different crystalline preformed oxide nanoparticles ( ex situ nanocomposites) is reported. The trifluoroacetate (TFA) metal–organic chemical solution deposition route is used with alcoholic solvents to grow epitaxial YBa 2 Cu 3 O 7 (YBCO) films. For this reason stabilizing oxide nanoparticles in polar solvents is a challenging goal. We have used scalable nanoparticle synthetic methodologies such as thermal and microwave-assisted solvothermal techniques to prepare CeO 2 and ZrO 2 nanoparticles. We show that stable and homogeneous colloidal solutions with these nanoparticles can be reached using benzyl alcohol, triethyleneglycol, nonanoic acid, trifluoroacetic acid or decanoic acid as protecting ligands, thereby allowing subsequent mixing with alcoholic TFA solutions. An elaborate YBCO film growth analysis of these nanocomposites allows the identification of the different relevant growth phenomena, e.g. nanoparticles pushing towards the film surface, nanoparticle reactivity, coarsening and nanoparticle accumulation at the substrate interface. Upon mitigation of these effects, YBCO nanocomposite films with high self-field critical currents ( J c ∼ 3–4 MA cm −2 at 77 K) were reached, indicating no current limitation effects associated with epitaxy perturbation, while smoothed magnetic field dependences of the critical currents at high magnetic fields and decreased effective anisotropic pinning behavior confirm the effectiveness of the novel developed approach to enhance vortex pinning. In conclusion, a novel low cost solution-derived route to high current nanocomposite superconducting films and coated conductors has been developed with very promising features.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.878
Times cited: 32
DOI: 10.1088/0953-2048/28/12/124007
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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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“Surface-Facet-Dependent Phonon Deformation Potential in Individual Strained Topological Insulator Bi2Se3 Nanoribbons”. Yan Y, Zhou X, Jin H, Li C-Z, Ke X, Van Tendeloo G, Liu K, Yu D, Dressel M, Liao Z-M, ACS nano 9, 10244 (2015). http://doi.org/10.1021/acsnano.5b04057
Abstract: Strain is an important method to tune the properties of topological insulators. For example, compressive strain can induce superconductivity in Bi2Se3 bulk material. Topological insulator nanostructures are the superior candidates to utilize the unique surface states due to the large surface to volume ratio. Therefore, it is highly desirable to monitor the local strain effects in individual topological insulator nanostructures. Here, we report the systematical micro-Raman spectra of single strained Bi2Se3 nanoribbons with different thicknesses and different surface facets, where four optical modes are resolved in both Stokes and anti-Stokes Raman spectral lines. A striking anisotropy of the strain dependence is observed in the phonon frequency of strained Bi2Se3 nanoribbons grown along the ⟨112̅0⟩ direction. The frequencies of the in-plane Eg2 and out-of-plane A1g1 modes exhibit a nearly linear blue-shift against bending strain when the nanoribbon is bent along the ⟨112̅0⟩ direction with the curved {0001} surface. In this case, the phonon deformation potential of the Eg2 phonon for 100 nm-thick Bi2Se3 nanoribbon is up to 0.94 cm–1/%, which is twice of that in Bi2Se3 bulk material (0.52 cm–1/%). Our results may be valuable for the strain modulation of individual topological insulator nanostructures.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 13.942
Times cited: 14
DOI: 10.1021/acsnano.5b04057
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“Efficient Chemical Modification of Carbon Nanotubes with Metallacarboranes”. Cabana L, Gonzalez-Campo A, Ke X, Van Tendeloo G, Nunez R, Tobias G, Chemistry: a European journal 21, 16792 (2015). http://doi.org/10.1002/chem.201503096
Abstract: As-produced single-walled carbon nanotubes (SWCNTs) tend to aggregate in bundles due to pi-pi interactions. Several approaches are nowadays available to debundle, at least partially, the nanotubes through surface modification by both covalent and noncovalent approaches. Herein, we explore different strategies to afford an efficient covalent functionalization of SWCNTs with cobaltabisdicarbollide anions. Aberration-corrected HRTEM analysis reveals the presence of metallacarboranes along the walls of the SWCNTs. This new family of materials presents an outstanding water dispersibility that facilitates its processability for potential applications.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 5.317
Times cited: 5
DOI: 10.1002/chem.201503096
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“Fe2O3-TiO2Nano-heterostructure Photoanodes for Highly Efficient Solar Water Oxidation”. Barreca D, Carraro G, Gasparotto A, Maccato C, Warwick MEA, Kaunisto K, Sada C, Turner S, Gönüllü, Y, Ruoko T-P, Borgese L, Bontempi E, Van Tendeloo G, Lemmetyinen H, Mathur S, Advanced Materials Interfaces 2, 1500313 (2015). http://doi.org/10.1002/admi.201500313
Abstract: Harnessing solar energy for the production of clean hydrogen by photoelectrochemical water splitting represents a very attractive, but challenging approach for sustainable energy generation. In this regard, the fabrication of Fe2O3–TiO2 photoanodes is reported, showing attractive performances [≈2.0 mA cm−2 at 1.23 V vs. the reversible hydrogen electrode in 1 M NaOH] under simulated one-sun illumination. This goal, corresponding to a tenfold photoactivity enhancement with respect to bare Fe2O3, is achieved by atomic layer deposition of TiO2 over hematite (α-Fe2O3) nanostructures fabricated by plasma enhanced-chemical vapor deposition and final annealing at 650 °C. The adopted approach enables an intimate Fe2O3–TiO2 coupling, resulting in an electronic interplay at the Fe2O3/TiO2 interface. The reasons for the photocurrent enhancement determined by TiO2 overlayers with increasing thickness are unraveled by a detailed chemico-physical investigation, as well as by the study of photogenerated charge carrier dynamics. Transient absorption spectroscopy shows that the increased photoelectrochemical response of heterostructured photoanodes compared to bare hematite is due to an enhanced separation of photogenerated charge carriers and more favorable hole dynamics for water oxidation. The stable responses obtained even in simulated seawater provides a feasible route in view of the eventual large-scale generation of renewable energy.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.279
Times cited: 56
DOI: 10.1002/admi.201500313
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“BaHfO3artificial pinning centres in TFA-MOD-derived YBCO and GdBCO thin films”. Erbe M, Hänisch J, Hühne R, Freudenberg T, Kirchner A, Molina-Luna L, Damm C, Van Tendeloo G, Kaskel S, Schultz L, Holzapfel B, Superconductor science and technology 28, 114002 (2015). http://doi.org/10.1088/0953-2048/28/11/114002
Abstract: Chemical solution deposition (CSD) is a promising way to realize REBa2Cu3O7−x (REBCO;RE = rare earth (here Y, Gd))-coated conductors with high performance in applied magnetic fields. However, the preparation process contains numerous parameters which need to be tuned to achieve high-quality films. Therefore, we investigated the growth of REBCO thin films containing nanometre-scale BaHfO3 (BHO) particles as pinning centres for magnetic flux lines, with emphasis on the influence of crystallization temperature and substrate on the microstructure and superconductivity. Conductivity, microscopy and x-ray investigations show an enhanced performance of BHO nano-composites in comparison to pristine REBCO. Further, those measurements reveal the superiority of GdBCO to YBCO—e.g. by inductive critical current densities, Jc, at self-field and 77 K. YBCO is outperformed by more than 1 MA cm−2 with Jc values of up to 5.0 MA cm−2 for 265 nm thick layers of GdBCO(BHO) on lanthanum aluminate. Transport in-field Jc measurements demonstrate high pinning force maxima of around 4 GN m−3 for YBCO(BHO) and GdBCO(BHO). However, the irreversibility fields are appreciably higher for GdBCO. The critical temperature was not significantly reduced upon BHO addition to both YBCO and GdBCO, indicating a low tendency for Hf diffusion into the REBCO matrix. Angular-dependent Jc measurements show a reduction of the anisotropy in the same order of magnitude for both REBCO compounds. Theoretical models suggest that more than one sort of pinning centre is active in all CSD films.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.878
Times cited: 36
DOI: 10.1088/0953-2048/28/11/114002
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“Templated Growth of Surface Enhanced Raman Scattering -Active Branched Au Nanoparticles within Radial Mesoporous Silica Shells”. Sanz-Ortiz MN, Sentosun K, Bals S, Liz-Marzan LM, ACS nano 9, 10489 (2015). http://doi.org/10.1021/acsnano.5b04744
Abstract: Noble metal nanoparticles are widely used as probes or substrates for surface-enhanced Raman scattering (SERS), due to their characteristic plasmon resonances in the visible and NIR spectral ranges. Aiming at obtaining a versatile system with high SERS performance we developed the synthesis of quasi-monodisperse, non-aggregated gold nanoparticles protected by radial mesoporous silica shells. The radial channels of such shells were used as templates for the growth of gold tips branching from the cores, thereby improving the plasmonic performance of the particles while favoring the localization of analyte molecules at high electric field regions: close to the tips, inside the pores. The method, which allows control over tip length, was successfully applied to various gold nanoparticle shapes, leading to materials with highly efficient SERS performance. The obtained nanoparticles are stable in ethanol and water upon thermal consolidation and can be safely stored as a powder.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 13.942
Times cited: 110
DOI: 10.1021/acsnano.5b04744
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“Damage evaluation in graphene underlying atomic layer deposition dielectrics”. Tang X, Reckinger N, Poncelet O, Louette P, Urena F, Idrissi H, Turner S, Cabosart D, Colomer J-F, Raskin J-P, Hackens B, Francis LA, Scientific reports 5, 13523 (2015). http://doi.org/10.1038/srep13523
Abstract: Based on micro-Raman spectroscopy (muRS) and X-ray photoelectron spectroscopy (XPS), we study the structural damage incurred in monolayer (1L) and few-layer (FL) graphene subjected to atomic-layer deposition of HfO2 and Al2O3 upon different oxygen plasma power levels. We evaluate the damage level and the influence of the HfO2 thickness on graphene. The results indicate that in the case of Al2O3/graphene, whether 1L or FL graphene is strongly damaged under our process conditions. For the case of HfO2/graphene, muRS analysis clearly shows that FL graphene is less disordered than 1L graphene. In addition, the damage levels in FL graphene decrease with the number of layers. Moreover, the FL graphene damage is inversely proportional to the thickness of HfO2 film. Particularly, the bottom layer of twisted bilayer (t-2L) has the salient features of 1L graphene. Therefore, FL graphene allows for controlling/limiting the degree of defect during the PE-ALD HfO2 of dielectrics and could be a good starting material for building field effect transistors, sensors, touch screens and solar cells. Besides, the formation of Hf-C bonds may favor growing high-quality and uniform-coverage dielectric. HfO2 could be a suitable high-K gate dielectric with a scaling capability down to sub-5-nm for graphene-based transistors.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 4.259
Times cited: 18
DOI: 10.1038/srep13523
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“Near-Infrared Emitting CuInSe/CuInS Dot Core/Rod Shell Heteronanorods by Sequential Cation Exchange”. van der Stam W, Bladt E, Rabouw FT, Bals S, de Mello Donega C, ACS nano 9, 11430 (2015). http://doi.org/10.1021/acsnano.5b05496
Abstract: The direct synthesis of heteronanocrystals (HNCs) combining different ternary semiconductors is challenging and has not yet been successful. Here, we report a sequential topotactic cation exchange (CE) pathway that yields CuInSe2/CuInS2 dot core/rod shell nanorods with near-infrared luminescence. In our approach, the Cu+ extraction rate is coupled to the In3+ incorporation rate by the use of a stoichiometric trioctylphosphine-InCl3 complex, which fulfills the roles of both In-source and Cu-extracting agent. In this way, Cu+ ions can be extracted by trioctylphosphine ligands only when the In-P bond is broken. This results in readily available In3+ ions at the same surface site from which the Cu+ is extracted, making the process a direct place exchange reaction and shifting the overall energy balance in favor of the CE. Consequently, controlled cation exchange can occur even in large and anisotropic heterostructured nanocrystals with preservation of the size, shape, and heterostructuring of the template NCs into the product NCs. The cation exchange is self-limited, stopping when the ternary core/shell CuInSe2/CuInS2 composition is reached. The method is very versatile, successfully yielding a variety of luminescent CuInX2 (X = S, Se, and Te) quantum dots, nanorods, and HNCs, by using Cd-chalcogenide NCs and HNCs as templates. The approach reported here thus opens up routes toward materials with unprecedented properties, which would otherwise remain inaccessible.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 13.942
Times cited: 88
DOI: 10.1021/acsnano.5b05496
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“Chemical stability of YBiO3 buffer layers for implementation in YBa2Cu3O7-&delta, coated conductors”. Pollefeyt G, Meledin A, Pop C, Ricart S, Hühne R, Van Tendeloo G, Van Driessche I, Acta materialia 100, 224 (2015). http://doi.org/10.1016/j.actamat.2015.08.023
Abstract: In this work, the chemical and microstructural stability of YBiO3 buffer layers during the growth of YBa2Cu3O7-δ (YBCO) was studied. The superconducting YBCO films were deposited via both Pulsed Laser Deposition as well as Chemical Solution Deposition. Although excellent superconducting properties are obtained in both cases, self-field critical current densities of 3.6 and 1.2 MA/cm2 respectively, chemical instability of the YBiO3 buffer layer is observed. An elaborate transmission electron microscopy study showed that in the case of vacuum deposited YBCO, the YBiO3 becomes unstable and Bi2O3 sublimates out of the architecture. Due to this structural instability, an intermediate Y2O3 layer is obtained which maintains it microstructural orientation relation with the substrate and acts as growth template for YBCO. For chemical solution deposited YBCO, reaction of YBCO with the YBiO3 buffer layer is observed, leading to large grains of YBa2BiO6 which are pushed towards the surface of the films and strongly reduce the superconducting properties. Upon using high growth temperatures for the superconducting layer, these secondary phases decompose, which subsequently leads to Bi2O3 sublimation and a textured YBCO film which directly nucleated onto the LaAlO3 single crystal substrate. Hence, this electron microscopy study indicates that bismuth-based buffer layers systems are not suitable for implementation in coated conductors.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 5.301
DOI: 10.1016/j.actamat.2015.08.023
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“Influence of the support material and the resulting particle distribution on the deposition of Ag nanoparticles for the electrocatalytic activity of benzyl bromide reduction”. Vanrenterghem B, Geboes B, Bals S, Ustarroz J, Hubin A, Breugelmans T, Applied catalysis : B : environmental 181, 542 (2016). http://doi.org/10.1016/j.apcatb.2015.08.026
Abstract: tSilver nanoparticles (NPs) were deposited on nickel, titanium and gold substrates using a potentiostaticdouble-pulse method. The influence of the support material on both the morphology and the electro-catalytic activity of Ag NPs for the reduction reaction of benzyl bromide was investigated and comparedwith previous research regarding silver NPs on glassy carbon. Scanning electron microscopy (SEM) dataindicated that spherical monodispersed NPs were obtained on Ni, Au and GC substrate with an averageparticle size of respectively 216 nm, 413 nm and 116 nm. On a Ti substrate dendritic NPs were obtainedwith a larger average particle density of 480 nm. The influence of the support material on the electrocat-alytic activity was tested by means of cyclic voltammetry (CV) for the reduction reaction of benzylbromide(1 mM) in acetonitrile + 0.1 M tetrabutylammonium perchlorate (Bu4NClO4). When the nucleation poten-tial (En) was applied at high cathodic overpotential, a positive shift of the reduction potential was obtained.The nucleation (tn) and growth time (tg) mostly had an influence on the current density whereas longerdeposition times lead to larger current densities. For these three parameters an optimum was present.The best electrocatalytic activity was obtained with Ag NPs deposited on Ni were a shift of the reduc-tion peak potential of 145 mV for the reaction of benzyl bromide was measured in comparance to bulksilver. The deposition on Au substrate yielded a positive shift of 114 mV. There was no indication of analtered reaction mechanism as the reaction was characterized as diffusion controlled and the transfercoefficients were in accordance with bulk silver. There was a beneficial catalitic activity measured due tothe interplay between support and NPs. This resulted in a shift of the reduction peak potential of 34 mV(Ag NPs on Au) and 65 mV (Ag NPs on Ni) compared to Ag NPs on a GC substrate.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Impact Factor: 9.446
Times cited: 16
DOI: 10.1016/j.apcatb.2015.08.026
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“The ASTRA Toolbox: A platform for advanced algorithm development in electron tomography”. van Aarle W, Palenstijn WJ, De Beenhouwer J, Altantzis T, Bals S, Batenburg KJ, Sijbers J, Ultramicroscopy 157, 35 (2015). http://doi.org/10.1016/j.ultramic.2015.05.002
Abstract: We present the ASTRA Toolbox as an open platform for 3D image reconstruction in tomography. Most of the software tools that are currently used in electron tomography offer limited flexibility with respect to the geometrical parameters of the acquisition model and the algorithms used for reconstruction. The ASTRA Toolbox provides an extensive set of fast and flexible building blocks that can be used to develop advanced reconstruction algorithms, effectively removing these limitations. We demonstrate this flexibility, the resulting reconstruction quality, and the computational efficiency of this toolbox by a series of experiments, based on experimental dual-axis tilt series.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Vision lab
Impact Factor: 2.843
Times cited: 562
DOI: 10.1016/j.ultramic.2015.05.002
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