“Atomic scale electron vortices for nanoresearch”. Verbeeck J, Schattschneider P, Lazar S, Stöger-Pollach M, Löffler S, Steiger-Thirsfeld A, Van Tendeloo G, Applied physics letters 99, 203109 (2011). http://doi.org/10.1063/1.3662012
Abstract: Electron vortex beams were only recently discovered and their potential as a probe for magnetism in materials was shown. Here we demonstrate a method to produce electron vortex beams with a diameter of less than 1.2 Å. This unique way to prepare free electrons to a state resembling atomic orbitals is fascinating from a fundamental physics point of view and opens the road for magnetic mapping with atomic resolution in an electron microscope.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.411
Times cited: 90
DOI: 10.1063/1.3662012
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“Atomic scale investigation of a PbTiO3/SrRuO3/DyScO3 heterostructure”. Egoavil R, Tan H, Verbeeck J, Bals S, Smith B, Kuiper B, Rijnders G, Koster G, Van Tendeloo G, Applied physics letters 102, 223106 (2013). http://doi.org/10.1063/1.4809597
Abstract: An epitaxial PbTiO3 thin film grown on self-organized crystalline SrRuO3 nanowires deposited on a DyScO3 substrate with ordered DyO and ScO2 chemical terminations is investigated by transmission electron microscopy. In this PbTiO3/SrRuO3/DyScO3 heterostructure, the SrRuO3 nanowires are assumed to grow on only one type of substrate termination. Here, we report on the structure, morphology, and chemical composition analysis of this heterostructure. Electron energy loss spectroscopy reveals the exact termination sequence in this complex structure. The energy loss near-edge structure of the Ti-L-2,L-3, Sc-L-2,L-3, and O K edges shows intrinsic interfacial electronic reconstruction. Furthermore, PbTiO3 domain walls are observed to start at the end of the nanowires resulting in atomic steps on the film surface. (C) 2013 AIP Publishing LLC.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.411
Times cited: 12
DOI: 10.1063/1.4809597
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“Barrier efficiency of sponge-like La2Zr2O7 buffer layers for YBCO-coated conductors”. Molina L, Tan H, Biermans E, Batenburg KJ, Verbeeck J, Bals S, Van Tendeloo G, Superconductor science and technology 24, 065019 (2011). http://doi.org/10.1088/0953-2048/24/6/065019
Abstract: Solution derived La2Zr2O7 films have drawn much attention for potential applications as thermal barriers or low-cost buffer layers for coated conductor technology. Annealing and coating parameters strongly affect the microstructure of La2Zr2O7, but different film processing methods can yield similar microstructural features such as nanovoids and nanometer-sized La2Zr2O7 grains. Nanoporosity is a typical feature found in such films and the implications for the functionality of the films are investigated by a combination of scanning transmission electron microscopy (STEM), electron energy-loss spectroscopy (EELS) and quantitative electron tomography. Chemical solution based La2Zr2O7 films deposited on flexible Ni5 at.%W substrates with a {100}lang001rang biaxial texture were prepared for an in-depth characterization. A sponge-like structure composed of nanometer-sized voids is revealed by high-angle annular dark-field scanning transmission electron microscopy in combination with electron tomography. A three-dimensional quantification of nanovoids in the La2Zr2O7 film is obtained on a local scale. Mostly non-interconnected highly faceted nanovoids compromise more than one-fifth of the investigated sample volume. The diffusion barrier efficiency of a 170 nm thick La2Zr2O7 film is investigated by STEM-EELS, yielding a 1.8 ± 0.2 nm oxide layer beyond which no significant nickel diffusion can be detected and intermixing is observed. This is of particular significance for the functionality of YBa2Cu3O7 − δ coated conductor architectures based on solution derived La2Zr2O7 films as diffusion barriers.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Vision lab
Impact Factor: 2.878
Times cited: 31
DOI: 10.1088/0953-2048/24/6/065019
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“Boron-rich inclusions and boron distribution in HPHT polycrystalline superconducting diamond”. Lu Y-G, Turner S, Ekimov EA, Verbeeck J, Van Tendeloo G, Carbon 86, 156 (2015). http://doi.org/10.1016/j.carbon.2015.01.034
Abstract: Polycrystalline boron-doped superconducting diamond, synthesized at high pressure and high temperature (HPHT) via a reaction of a single piece of crystalline boron with monolithic graphite, has been investigated by analytical transmission electron microscopy. The local boron distribution and boron environment have been studied by a combination of (scanning) transmission electron microscopy ((S)TEM) and spatially resolved electron energy-loss spectroscopy (EELS). High resolution TEM imaging and EELS elemental mapping have established, for the first time, the presence of largely crystalline diamond-diamond grain boundaries within the material and have evidenced the presence of substitutional boron dopants within individual diamond grains. Confirmation of the presence of substitutional B dopants has been obtained through comparison of acquired boron K-edge EELS fine structures with known references. This confirmation is important to understand the origin of superconductivity in polycrystalline B-doped diamond. In addition to the substitutional boron doping, boron-rich inclusions and triple-points, both amorphous and crystalline, with chemical compositions close to boron carbide B4C, are evidenced. (C) 2015 Elsevier Ltd. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 6.337
Times cited: 20
DOI: 10.1016/j.carbon.2015.01.034
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“Casting light on the darkening of colors in historical paintings”. da Pieve F, Hogan C, Lamoen D, Verbeeck J, Vanmeert F, Radepont M, Cotte M, Janssens K, Gonze X, Van Tendeloo G, Physical review letters 111, 208302 (2013). http://doi.org/10.1103/PhysRevLett.111.208302
Abstract: The degradation of colors in historical paintings affects our cultural heritage in both museums and archeological sites. Despite intensive experimental studies, the origin of darkening of one of the most ancient pigments known to humankind, vermilion (α-HgS), remains unexplained. Here, by combining many-body theoretical spectroscopy and high-resolution microscopic x-ray diffraction, we clarify the composition of the damaged paint work and demonstrate possible physicochemical processes, induced by illumination and exposure to humidity and air, that cause photoactivation of the original pigment and the degradation of the secondary minerals. The results suggest a new path for the darkening process which was never considered by previous studies and prompt a critical examination of their findings.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 8.462
Times cited: 30
DOI: 10.1103/PhysRevLett.111.208302
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“Cation ordering and flexibility of the BO42- tetrahedra in incommensurately modulated CaEu2(BO4)4 (B = Mo, W) scheelites”. Abakumov AM, Morozov VA, Tsirlin AA, Verbeeck J, Hadermann J, Inorganic chemistry 53, 9407 (2014). http://doi.org/10.1021/ic5015412
Abstract: The factors mediating cation ordering in the scheelite-based molybdates and tungstates are discussed on the basis of the incommensurately modulated crystal structures of the CaEu2(BO4)(4) (B = Mo, W) red phosphors solved from high-resolution synchrotron powder X-ray diffraction data. Monoclinic CaEu2(WO4)(4) adopts a (3 + 1)-dimensionally modulated structure [superspace group I2/b(alpha beta 0)00, a = 5.238 73(1)A, b = 5.266 35(1) A, c = 11.463 19(9) A, gamma = 91.1511(2)degrees, q = 0.56153(6)a* + 0.7708(9)b*, R-F = 0.050, R-p = 0.069], whereas tetragonal CaEu2(MoO4)(4) is (3 + 2)-dimensionally modulated [superspace group I4(1)/ a(alpha beta 0)00(-beta alpha 0)00, a = 5.238 672(7) A, c = 11.548 43(2) A, q(1) = 035331(8)a* + 0.82068(9)b*, q(2) = -0.82068(9)a* + 0.55331(8)b*, R-F = 0.061, R-p = 0.082]. In both cases the modulation arises from the ordering of the Ca/Eu cations and the cation vacancies at the A-sublattice of the parent scheelite ABO(4) structure. The cation ordering is incomplete and better described with harmonic rather than with steplike occupational modulation functions. The structures respond to the variation of the effective charge and cation size at the A-position through the flexible geometry of the MoO42- and WO42- tetrahedra demonstrating an alternation of stretching the B-O bond lengths and bending the O-B-O bond angles. The tendency towards A-site cation ordering in scheelites is rationalized using the difference in ionic radii and concentration of the A-site vacancies as parameters and presented in the form of a structure map.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.857
Times cited: 48
DOI: 10.1021/ic5015412
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“Chemical insight into electroforming of resistive switching manganite heterostructures”. Borgatti F, Park C, Herpers A, Offi F, Egoavil R, Yamashita Y, Yang A, Kobata M, Kobayashi K, Verbeeck J, Panaccione G, Dittmann R;, Nanoscale 5, 3954 (2013). http://doi.org/10.1039/c3nr00106g
Abstract: We have investigated the role of the electroforming process in the establishment of resistive switching behaviour for Pt/Ti/Pr0.5Ca0.5MnO3/SrRuO3 layered heterostructures (Pt/Ti/PCMO/SRO) acting as non-volatile Resistance Random Access Memories (RRAMs). Electron spectroscopy measurements demonstrate that the higher resistance state resulting from electroforming of as-prepared devices is strictly correlated with the oxidation of the top electrode Ti layer through field-induced electromigration of oxygen ions. Conversely, PCMO exhibits oxygen depletion and downward change of the chemical potential for both resistive states. Impedance spectroscopy analysis, supported by the detailed knowledge of these effects, provides an accurate model description of the device resistive behaviour. The main contributions to the change of resistance from the as-prepared (low resistance) to the electroformed (high resistance) states are respectively due to reduced PCMO at the boundary with the Ti electrode and to the formation of an anisotropic np junction between the Ti and the PCMO layers.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 7.367
Times cited: 40
DOI: 10.1039/c3nr00106g
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“Circular dichroism in the electron microscope: progress and applications (invited)”. Schattschneider P, Ennen I, Stoger-Pollach M, Verbeeck J, Journal of applied physics 107, 09d311 (2010). http://doi.org/10.1063/1.3365517
Abstract: According to theory, x-ray magnetic circular dichroism in a synchrotron is equivalent to energy loss magnetic chiral dichroism (EMCD) in a transmission electron microscope (TEM). After a synopsis of the development of EMCD, the theoretical background is reviewed and recent results are presented, focusing on the study of magnetic nanoparticles for ferrofluids and Heusler alloys for spintronic devices. Simulated maps of the dichroic strength as a function of atom position in the crystal allow evaluating the influence of specimen thickness and sample tilt on the experimental EMCD signal. Finally, the possibility of direct observation of chiral electronic transitions with atomic resolution in a TEM is discussed.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.068
Times cited: 28
DOI: 10.1063/1.3365517
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“Computational aspects in quantitative EELS”. Verbeeck J, Van Aert S, Zhang L, Haiyan T, Schattschneider P, Rosenauer A, Microscopy and microanalysis 16, 240 (2010). http://doi.org/10.1017/S143192761005511X
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 1.891
DOI: 10.1017/S143192761005511X
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“Corrigendum: Structural phase transition at the percolation threshold in epitaxial (La0.7Ca0.3MnO3)1-x:(MgO)x nanocomposite films”. Moshnyaga V, Damaschke B, Shapoval O, Belenchuk A, Faupel J, Lebedev OI, Verbeeck J, Van Tendeloo G, Mücksch M, Tsurkan V, Tidecks R, Samwer K, Nature materials 4, 104 (2005)
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 39.737
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“Creating arrays of electron vortices”. Niermann T, Verbeeck J, Lehmann M, Ultramicroscopy 136, 165 (2014). http://doi.org/10.1016/j.ultramic.2013.10.002
Abstract: We demonstrate the production of an ordered array of electron vortices making use of an electron optical setup consisting of two electrostatic biprisms. The biprism filaments are oriented nearly orthogonal with respect to each other in a transmission electron microscope. Matching the position of the filaments, we can choose to form different topological features in the electron wave. We outline the working principle of the setup and demonstrate fist experimental results. This setup partially bridges the gap between angular momentum carried by electron spin, which is intrinsic and therefore present in any position of the wave, and angular momentum carried by the vortex character of the wave, which can be extrinsic depending on the axis around which it is measured. (C) 2013 Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.843
Times cited: 9
DOI: 10.1016/j.ultramic.2013.10.002
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“Crystal Structure and Luminescent Properties of R2-xEux(MoO4)(3) (R = Gd, Sm) Red Phosphors”. Morozov VA, Raskina MV, Lazoryak BI, Meert KW, Korthout K, Smet PF, Poelman D, Gauquelin N, Verbeeck J, Abakumov AM, Hadermann J;, Chemistry of materials 26, 7124 (2014). http://doi.org/10.1021/cm503720s
Abstract: The R-2(MoO4)(3) (R = rare earth elements) molybdates doped with Eu3+ cations are interesting red-emitting materials for display and solid-state lighting applications. The structure and luminescent properties of the R2-xEux(MoO4)(3) (R = Gd, Sm) solid solutions have been investigated as a function of chemical composition and preparation conditions. Monoclinic (alpha) and orthorhombic (beta') R2-xEux(MoO4)(3) (R = Gd, Sm; 0 <= x <= 2) modifications were prepared by solid-state reaction, and their structures were investigated using synchrotron powder X-ray diffraction and transmission electron microscopy. The pure orthorhombic beta'-phases could be synthesized only by quenching from high temperature to room temperature for Gd2-xEux(MoO4)(3) in the Eu3+-rich part (x > 1) and for all Sm2-xEux(MoO4)(3) solid solutions. The transformation from the alpha-phase to the beta'-phase results in a notable increase (similar to 24%) of the unit cell volume for all R2-xEux(MoO4)(3) (R = Sm, Gd) solid solutions. The luminescent properties of all R2-xEux(MoO4)(3) (R = Gd, Sm; 0 <= x <= 2) solid solutions were measured, and their optical properties were related to their structural properties. All R2-xEux(MoO4)(3) (R = Gd, Sm; 0 <= x <= 2) phosphors emit intense red light dominated by the D-5(0)-> F-7(2) transition at similar to 616 nm. However, a change in the multiplet splitting is observed when switching from the monoclinic to the orthorhombic structure, as a consequence of the change in coordination polyhedron of the luminescent ion from RO8 to RO7 for the alpha- and beta'-modification, respectively. The Gd2-xEux(MoO4)(3) solid solutions are the most efficient emitters in the range of 0 < x < 1.5, but their emission intensity is comparable to or even significantly lower than that of Sm2-xEux(MoO4)(3) for higher Eu3+ concentrations (1.5 <= x <= 1.75). Electron energy loss spectroscopy (EELS) measurements revealed the influence of the structure and element content on the number and positions of bands in the ultraviolet-visible-infrared regions of the EELS spectrum.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 9.466
Times cited: 24
DOI: 10.1021/cm503720s
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“Deconvolution of core electron energy loss spectra”. Verbeeck J, Bertoni G, Ultramicroscopy 109, 1343 (2009). http://doi.org/10.1016/j.ultramic.2009.06.010
Abstract: Different deconvolution methods for removing multiple scattering and instrumental broadening from core loss electron energy loss spectra are compared with special attention to the artefacts they introduce. The Gaussian modifier method, Wiener filter, maximum entropy, and model based methods are described. Their performance is compared on virtual spectra where the true single scattering distribution is known. A test on experimental spectra confirms the good performance of model based deconvolution in comparison to maximum entropy methods and shows the advantage of knowing the estimated error bars from a single spectrum acquisition.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.843
Times cited: 13
DOI: 10.1016/j.ultramic.2009.06.010
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“Defect engineering in oxide heterostructures by enhanced oxygen surface exchange”. Huijben M, Koster G, Kruize MK, Wenderich S, Verbeeck J, Bals S, Slooten E, Shi B, Molegraaf HJA, Kleibeuker JE, Van Aert S, Goedkoop JB, Brinkman A, Blank DHA, Golden MS, Van Tendeloo G, Hilgenkamp H, Rijnders G;, Advanced functional materials 23, 5240 (2013). http://doi.org/10.1002/adfm.201203355
Abstract: The synthesis of materials with well-controlled composition and structure improves our understanding of their intrinsic electrical transport properties. Recent developments in atomically controlled growth have been shown to be crucial in enabling the study of new physical phenomena in epitaxial oxide heterostructures. Nevertheless, these phenomena can be influenced by the presence of defects that act as extrinsic sources of both doping and impurity scattering. Control over the nature and density of such defects is therefore necessary to fully understand the intrinsic materials properties and exploit them in future device technologies. Here, it is shown that incorporation of a strontium copper oxide nano-layer strongly reduces the impurity scattering at conducting interfaces in oxide LaAlO3SrTiO3(001) heterostructures, opening the door to high carrier mobility materials. It is proposed that this remote cuprate layer facilitates enhanced suppression of oxygen defects by reducing the kinetic barrier for oxygen exchange in the hetero-interfacial film system. This design concept of controlled defect engineering can be of significant importance in applications in which enhanced oxygen surface exchange plays a crucial role.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 12.124
Times cited: 87
DOI: 10.1002/adfm.201203355
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“Degradation process of lead chromate in paintings by Vincent van Gogh studied by means of spectromicroscopic methods : 3 : synthesis, characterization, and detection of different crystal forms of the chrome yellow pigment”. Monico L, Janssens K, Miliani C, Brunetti BG, Vagnini M, Vanmeert F, Falkenberg G, Abakumov A, Lu Y, Tian H, Verbeeck J, Radepont M, Cotte M, Hendriks E, Geldof M, van der Loeff L, Salvant J, Menu M;, Analytical chemistry 85, 860 (2013). http://doi.org/10.1021/ac302158b
Abstract: The painter, Vincent van Gogh, and some of his contemporaries frequently made use of the pigment chrome yellow that is known to show a tendency toward darkening. This pigment may correspond to various chemical compounds such as PbCrO4 and PbCr1-xSxO4, that may each be present in various crystallographic forms with different tendencies toward degradation. Investigations by X-ray diffraction (XRD), mid-Fourier Transform infrared (FTIR), and Raman instruments (benchtop and portable) and synchrotron radiation-based micro-XRD and X-ray absorption near edge structure spectroscopy performed on oil-paint models, prepared with in-house synthesized PbCrO4 and PbCr1-xSxO4, permitted us to characterize the spectroscopic features of the various forms. On the basis of these results, an extended study has been carried out on historic paint tubes and on embedded paint microsamples taken from yellow-orange/pale yellow areas of 12 Van Gogh paintings, demonstrating that Van Gogh effectively made use of different chrome yellow types. This conclusion was also confirmed by in situ mid-FTIR investigations on Van Goghs Portrait of Gauguin (Van Gogh Museum, Amsterdam).
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 6.32
Times cited: 79
DOI: 10.1021/ac302158b
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“Degradation process of lead chromate in paintings by Vincent van Gogh studied by means of synchrotron X-ray spectromicroscopy and related methods : 1 : artificially aged model samples”. Monico L, van der Snickt G, Janssens K, de Nolf W, Miliani C, Verbeeck J, Tian H, Tan H, Dik J, Radepont M, Cotte M, Analytical chemistry 83, 1214 (2011). http://doi.org/10.1021/ac102424h
Abstract: On several paintings by artists of the end of the 19th century and the beginning of the 20th Century a darkening of the original yellow areas, painted with the chrome yellow pigment (PbCrO4, PbCrO4·xPbSO4, or PbCrO4·xPbO) is observed. The most famous of these are the various Sunflowers paintings Vincent van Gogh made during his career. In the first part of this work, we attempt to elucidate the degradation process of chrome yellow by studying artificially aged model samples. In view of the very thin (1−3 μm) alteration layers that are formed, high lateral resolution spectroscopic methods such as microscopic X-ray absorption near edge (μ-XANES), X-ray fluorescence spectrometry (μ-XRF), and electron energy loss spectrometry (EELS) were employed. Some of these use synchrotron radiation (SR). Additionally, microscopic SR X-ray diffraction (SR μ-XRD), μ-Raman, and mid-FTIR spectroscopy were employed to completely characterize the samples. The formation of Cr(III) compounds at the surface of the chrome yellow paint layers is particularly observed in one aged model sample taken from a historic paint tube (ca. 1914). About two-thirds of the chromium that is present at the surface has reduced from the hexavalent to the trivalent state. The EELS and μ-XANES spectra are consistent with the presence of Cr2O3·2H2O (viridian). Moreover, as demonstrated by μ-XANES, the presence of another Cr(III) compound, such as either Cr2(SO4)3·H2O or (CH3CO2)7Cr3(OH)2 [chromium(III) acetate hydroxide], is likely.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 6.32
Times cited: 113
DOI: 10.1021/ac102424h
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“Determination of size, morphology, and nitrogen impurity location in treated detonation nanodiamond by transmission electron microscopy”. Turner S, Lebedev OI, Shenderova O, Vlasov II, Verbeeck J, Van Tendeloo G, Advanced functional materials 19, 2116 (2009). http://doi.org/10.1002/adfm.200801872
Abstract: Size, morphology, and nitrogen impurity location, all of which are all thought to be related to the luminescent properties of detonation nanodiamonds, are determined in several detonation nanodiamond samples using a combination of transmission electron microscopy techniques. Results obtained from annealed and cleaned detonation nanodiamond samples are compared to results from conventionally purified detonation nanodiamond. Detailed electron energy loss spectroscopy combined with model-based quantification provides direct evidence for the sp3 like embedding of nitrogen impurities into the diamond cores of all the studied nanodiamond samples. Simultaneously, the structure and morphology of the cleaned detonation nanodiamond particles are studied using high resolution transmission electron microscopy. The results show that the size and morphology of detonation nanodiamonds can be modified by temperature treatment and that by applying a special cleaning procedure after temperature treatment, nanodiamond particles with clean facets almost free from sp2 carbon can be prepared. These clean facets are clear evidence that nanodiamond cores are not necessarily in coexistence with a graphitic shell of non-diamond carbon.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 12.124
Times cited: 100
DOI: 10.1002/adfm.200801872
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“Direct space structure solution from precession electron diffraction data: resolving heavy and light scatterers in Pb13Mn9O25”. Hadermann J, Abakumov AM, Tsirlin AA, Filonenko VP, Gonnissen J, Tan H, Verbeeck J, Gemmi M, Antipov EV, Rosner H, Ultramicroscopy 110, 881 (2010). http://doi.org/10.1016/j.ultramic.2010.03.012
Abstract: The crystal structure of a novel compound Pb13Mn9O25 has been determined through a direct space structure solution with a Monte-Carlo-based global optimization using precession electron diffraction data (a=14.177(3) Å, c=3.9320(7) Å, SG P4/m, RF=0.239) and compositional information obtained from energy dispersive X-ray analysis and electron energy loss spectroscopy. This allowed to obtain a reliable structural model even despite the simultaneous presence of both heavy (Pb) and light (O) scattering elements and to validate the accuracy of the electron diffraction-based structure refinement. This provides an important benchmark for further studies of complex structural problems with electron diffraction techniques. Pb13Mn9O25 has an anion- and cation-deficient perovskite-based structure with the A-positions filled by the Pb atoms and 9/13 of the B positions filled by the Mn atoms in an ordered manner. MnO6 octahedra and MnO5 tetragonal pyramids form a network by sharing common corners. Tunnels are formed in the network due to an ordered arrangement of vacancies at the B-sublattice. These tunnels provide sufficient space for localization of the lone 6s2 electron pairs of the Pb2+ cations, suggested as the driving force for the structural difference between Pb13Mn9O25 and the manganites of alkali-earth elements with similar compositions.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.843
Times cited: 24
DOI: 10.1016/j.ultramic.2010.03.012
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“Direct structural and spectroscopic investigation of ultrathin films of tetragonal CuO: Six-fold coordinated copper”. Samal D, Tan H, Takamura Y, Siemons W, Verbeeck J, Van Tendeloo G, Arenholz E, Jenkins CA, Rijnders G, Koster G, Europhysics letters 105, 17003 (2014). http://doi.org/10.1209/0295-5075/105/17003
Abstract: Unlike other 3d transition metal monoxides (MnO, FeO, CoO, and NiO), CuO is found in a low-symmetry distorted monoclinic structure rather than the rocksalt structure. We report here of the growth of ultrathin CuO films on SrTiO3 substrates; scanning transmission electron microscopy was used to show the stabilization of a tetragonal rocksalt structure with an elongated c-axis such that c/a similar to 1.34 and the Cu-O-Cu bond angle similar to 180 degrees, pointing to metastable six-fold coordinated Cu. X-ray absorption spectroscopy demonstrates that the hole at the Cu site for the CuO is localized in 3d(x2-y2) orbital unlike the well-studied monoclinic CuO phase. The experimental confirmation of the tetragonal structure of CuO opens up new avenues to explore electronic and magnetic properties of six-fold coordinated Cu. Copyright (C) EPLA, 2014
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 1.957
Times cited: 15
DOI: 10.1209/0295-5075/105/17003
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“Direct visualization of boron dopant distribution and coordination in individual chemical vapor deposition nanocrystalline B-doped diamond grains”. Lu Y-G, Turner S, Verbeeck J, Janssens SD, Wagner P, Haenen K, Van Tendeloo G, Applied physics letters 101, 041907 (2012). http://doi.org/10.1063/1.4738885
Abstract: The boron dopant distribution in individual heavily boron-doped nanocrystalline diamond film grains, with sizes ranging from 100 to 350nm in diameter, has been studied using a combination of high resolution annular dark field scanning transmission electron microscopy and spatially resolved electron energy-loss spectroscopy. Using these tools, the boron distribution and local boron coordination have been determined. Quantification results reveal embedding of B dopants in the diamond lattice, and a preferential enrichment of boron at defective areas and twin boundaries. Coordination mapping reveals a distinct difference in coordination of the B dopants in “pristine” diamond areas and in defective regions. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4738885]
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.411
Times cited: 59
DOI: 10.1063/1.4738885
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“EELS investigations of different niobium oxide phases”. Bach D, Störmer H, Schneider R, Gerthsen D, Verbeeck J, Microscopy and microanalysis 12, 416 (2006). http://doi.org/10.1017/S1431927606060521
Abstract: Electron energy loss spectra in conjunction with near-edge fine structures of purely stoichiometric niobium monoxide (NbO) and niobium pentoxide (Nb2O5) reference materials were recorded. The structures of the niobium oxide reference materials were checked by selected area electron diffraction to ensure a proper assignment of the fine structures. NbO and Nb2O5 show clearly different energy loss near-edge fine structures of the Nb-M-4,M-5 and -M-2,M-3 edges and of the O-K edge, reflecting the specific local environments of the ionized atoms. To distinguish the two oxides in a quantitative manner, the intensities under the Nb-M-4,M-5 as well as Nb-M-2,M-3 edges and the O-K edge were measured and their ratios calculated. k-factors were also derived from these measurements.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 1.891
Times cited: 50
DOI: 10.1017/S1431927606060521
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“EELS of niobium and stoichiometric niobium-oxide phases: part 1: plasmon and Near-edges fine structure”. Bach D, Schneider R, Gerthsen D, Verbeeck J, Sigle W, Microscopy and microanalysis 15, 505 (2009). http://doi.org/10.1017/S143192760999105X
Abstract: A comprehensive electron energy-loss spectroscopy study of niobium (Nb) and stable Nb-oxide phases (NbO, NbO2, Nb2O5) was carried out. In this work (Part I), the plasmons and energy-loss near-edge structures (ELNES) of all relevant Nb edges (Nb-N2,3, Nb-M4,5, Nb-M2,3, Nb-M1, and Nb-L2,3) up to energy losses of about 2600 eV and the O-K edge are analyzed with respect to achieving characteristic fingerprints of Nb in different formal oxidation states (0 for metallic Nb, +2 for NbO, +4 for NbO2, and +5 for Nb2O5). Chemical shifts of the Nb-N2,3, Nb-M4,5, Nb-M2,3, and Nb-L2,3 edges are extracted from the spectra that amount to about 4 eV as the oxidation state increases from 0 for Nb to +5 for Nb2O5. Four different microscopes, including a 200 keV ZEISS Libra with monochromator, were used. The corresponding wide range of experimental parameters with respect to the primary electron energy, convergence, and collection semi-angles as well as energy resolution allows an assessment of the influence of the experimental setup on the ELNES of the different edges. Finally, the intensity of the Nb-L2,3 white-line edges is correlated with niobium 4d-state occupancy in the different reference materials.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 1.891
Times cited: 55
DOI: 10.1017/S143192760999105X
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“The effect of probe inaccuracies on the quantitative model-based analysis of high angle annular dark field scanning transmission electron microscopy images”. Martinez GT, de Backer A, Rosenauer A, Verbeeck J, Van Aert S, Micron 63, 57 (2014). http://doi.org/10.1016/j.micron.2013.12.009
Abstract: Quantitative structural and chemical information can be obtained from high angle annular dark field scanning transmission electron microscopy (HAADF STEM) images when using statistical parameter estimation theory. In this approach, we assume an empirical parameterized imaging model for which the total scattered intensities of the atomic columns are estimated. These intensities can be related to the material structure or composition. Since the experimental probe profile is assumed to be known in the description of the imaging model, we will explore how the uncertainties in the probe profile affect the estimation of the total scattered intensities. Using multislice image simulations, we analyze this effect for Cs corrected and non-Cs corrected microscopes as a function of inaccuracies in cylindrically symmetric aberrations, such as defocus and spherical aberration of third and fifth order, and non-cylindrically symmetric aberrations, such as 2-fold and 3-fold astigmatism and coma.
Keywords: A1 Journal article; Engineering Management (ENM); Electron microscopy for materials research (EMAT)
Impact Factor: 1.98
Times cited: 25
DOI: 10.1016/j.micron.2013.12.009
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“An efficient way of including thermal diffuse scattering in simulation of scanning transmission electron microscopic images”. Croitoru MD, van Dyck D, Van Aert S, Bals S, Verbeeck J, Ultramicroscopy 106, 933 (2006). http://doi.org/10.1016/j.ultramic.2006.04.006
Abstract: We propose an improved image simulation procedure for atomic-resolution annular dark-field scanning transmission electron microscopy (STEM) based on the multislice formulation, which takes thermal diffuse scattering fully into account. The improvement with regard to the classical frozen phonon approach is realized by separating the lattice configuration statistics from the dynamical scattering so as to avoid repetitive calculations. As an example, the influence of phonon scattering on the image contrast is calculated and investigated. STEM image simulation of crystals can be applied with reasonable computing times to problems involving a large number of atoms and thick or large supercells.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT); Vision lab
Impact Factor: 2.843
Times cited: 18
DOI: 10.1016/j.ultramic.2006.04.006
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“Electrical nonlinearity in colossal magnetoresistance manganite films: relevance of correlated polarons”. Moshnyaga V, Gehrke K, Sudheendra L, Belenchuk A, Raabe S, Shapoval O, Verbeeck J, Van Tendeloo G, Samwer K, Physical review : B : solid state 79, 134413 (2009). http://doi.org/10.1103/PhysRevB.79.134413
Abstract: The metal-insulator (MI) transition in epitaxial thin films of La0.75Ca0.25MnO3 (LCMO) is accompanied by the appearance of an intrinsic electrical nonlinearity. The latter, probed by electrical third harmonic voltage, U3, or resistance, R3=dU3/dJ, is drastically enhanced in the vicinity of the MI transition, TMI=267 K. Applied magnetic field, B=5 T, suppresses the nonlinearity, resulting in a huge nonlinear CMR3(TMI)~105%. R3 shows a peculiar low-frequency (1 kHz) dependence, R3~(-0)n, with exponent, n, changing across the MI transition from n~1,52 for TTMI to n=1 (T<TMI). The observed electrical nonlinearity in LCMO reflects the behavior of correlated polarons, the number of which dramatically enhances in the vicinity of TMI. We argued that correlated polarons, considered as electric-elastic quadrupoles, provide a nonlinear (quadratic) coupling to the electric field, yielding a third harmonic electric nonlinearity in LCMO. The reference film of La0.7Sr0.3MnO3 (LSMO), a prototypic double exchange system with second-order phase transition, is characterized as a linear metallic material in the whole range of temperatures (T=10400 K), magnetic fields (B=05 T), and frequencies (=11000 Hz).
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.836
Times cited: 28
DOI: 10.1103/PhysRevB.79.134413
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“Electrical switching in Fe/Cr/MgO/Fe magnetic tunnel junctions”. Halley D, Majjad H, Bowen M, Najjari N, Henry Y, Ulhaq-Bouillet C, Weber W, Bertoni G, Verbeeck J, Van Tendeloo G, Applied physics letters 92, 212115 (2008). http://doi.org/10.1063/1.2938696
Abstract: Hysteretic resistance switching is observed in epitaxial Fe/Cr/MgO/Fe magnetic tunnel junctions under bias voltage cycling between negative and positive values of about 1 V. The junctions switch back and forth between high- and low-resistance states, both of which depend on the device bias history. A linear dependence is found between the magnitude of the tunnel magnetoresistance and the crafted resistance of the junctions. To explain these results, a model is proposed that considers electron transport both by elastic tunneling and by defect-assisted transmission. (c) 2008 American Institute of Physics.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.411
Times cited: 33
DOI: 10.1063/1.2938696
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“Electron energy-loss spectroscopy study of a (LaMnO3)8(SrMnO3)4 heterostructure”. Verbeeck J, Lebedev OI, Van Tendeloo G, Silcox J, Mercey B, Hervieu M, Haghiri-Gosnet AM, Applied physics letters 79, 2037 (2001). http://doi.org/10.1063/1.1403316
Abstract: An epitaxially grown heterostructure consisting of alternating layers of LaMnO3 (8 unit cells) and SrMnO3 (4 unit cells) on a SrTiO3 substrate has been studied by a combination of electron energy-loss spectroscopy (EELS) and high-resolution transmission electron microscopy (HRTEM) on an atomic scale. Excitation edges of all elements are captured with subnanometer spatial accuracy, and parametrized to obtain chemical profiles. The fine-edge structure of O K and Mn L-2,L-3 edges are interpreted as signatures of the local electronic structure and show a spatial modulation of the concentration of holes with O 2p character. The chemical concentration is found to be different for the bottom and top interface of a SrMnO3 layer. HRTEM complements the EELS results and confirms the asymmetry of the interfaces. (C) 2001 American Institute of Physics.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.411
Times cited: 19
DOI: 10.1063/1.1403316
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“Electron inelastic, scattering and anisotropy: the two-dimensional point of view”. Radtke G, Botton GA, Verbeeck J, Ultramicroscopy 106, 1082 (2006). http://doi.org/10.1016/j.ultramic.2006.04.023
Abstract: The measurement of the electronic structure of anisotropic materials using energy loss near edge structure (ELNES) spectroscopy is an important field of microanalysis in transmission electron microscopy. We present a novel method to study the angular dependence of electron inelastic scattering in anisotropic materials. This method has been applied to the study of 1s -> pi* and sigma* transitions on the carbon K edge in pyrolitic graphite. An excellent agreement between experimental and theoretical two-dimensional scattering patterns has been found. In particular, the need of a fully relativistic calculation of the inelastic scattering cross-section to explain the experimental results is demonstrated. (c) 2006 Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.843
Times cited: 5
DOI: 10.1016/j.ultramic.2006.04.023
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“Electron vortex beams in a magnetic field : a new twist on Landau levels and Aharonov-Bohm states”. Bliokh KY, Schattschneider P, Verbeeck J, Nori F, Physical review X 2, 041011 (2012). http://doi.org/10.1103/PhysRevX.2.041011
Abstract: We examine the propagation of the recently discovered electron vortex beams in a longitudinal magnetic field. We consider both the Aharonov-Bohm configuration with a single flux line and the Landau case of a uniform magnetic field. While stationary Aharonov-Bohm modes represent Bessel beams with flux- and vortex-dependent probability distributions, stationary Landau states manifest themselves as nondiffracting Laguerre-Gaussian beams. Furthermore, the Landau-state beams possess field- and vortex-dependent phases: (i) the Zeeman phase from coupling the quantized angular momentum to the magnetic field and (ii) the Gouy phase, known from optical Laguerre-Gaussian beams. Remarkably, together these phases determine the structure of Landau energy levels. This unified Zeeman-Landau-Gouy phase manifests itself in a nontrivial evolution of images formed by various superpositions of modes. We demonstrate that, depending on the chosen superposition, the image can rotate in a magnetic field with either (i) Larmor, (ii) cyclotron (double-Larmor), or (iii) zero frequency. At the same time, its centroid always follows the classical cyclotron trajectory, in agreement with the Ehrenfest theorem. Interestingly, the nonrotating superpositions reproduce stable multivortex configurations that appear in rotating superfluids. Our results open an avenue for the direct electron-microscopy observation of fundamental properties of free quantum-electron states in magnetic fields.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 12.789
Times cited: 130
DOI: 10.1103/PhysRevX.2.041011
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“Electronic reconstruction at n-type SrTiO3/LaAlO3 interfaces”. Verbeeck J, Bals S, Lamoen D, Luysberg M, Huijben M, Rijnders G, Brinkman A, Hilgenkamp H, Blank DHA, Van Tendeloo G, Physical review : B : condensed matter and materials physics 81, 085113 (2010). http://doi.org/10.1103/PhysRevB.81.085113
Abstract: Electron-energy-loss spectroscopy (EELS) is used to investigate single layers of LaAlO3 grown on SrTiO3 having an n-type interface as well as multilayers of LaAlO3 and SrTiO3 in which both n- and p-type interfaces occur. Only minor changes in Ti valence at the n-type interface are observed. This finding seems to contradict earlier experiments for other SrTiO3/LaAlO3 systems where large deviations in Ti valency were assumed to be responsible for the conductivity of these interfaces. Ab initio calculations have been carried out in order to interpret our EELS results. Using the concept of Bader charges, it is demonstrated that the so-called polar discontinuity is mainly resolved by lattice distortions and to a far lesser extent by changes in valency for both single layer and multilayer geometries.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.836
Times cited: 25
DOI: 10.1103/PhysRevB.81.085113
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