“Monitoring the impact of the indoor air quality on silver cultural heritage objects using passive and continuous corrosion rate assessments”. 't Hart L, Storme P, Anaf W, Nuyts G, Vanmeert F, Dorriné, W, Janssens K, De Wael K, Schalm O, Applied physics A : materials science &, processing 122, 923 (2016). http://doi.org/10.1007/S00339-016-0456-2
Abstract: There is a long tradition in evaluating industrial atmospheres by measuring the corrosion rate of exposed metal coupons. The heritage community also uses this method, but the interpretation of the corrosion rate often lacks clarity due to the low corrosivity in indoor museum environments. This investigation explores the possibilities and drawbacks of different silver corrosion rate assessments. The corrosion rate is determined by three approaches: (1) chemical characterization of metal coupons using analytical techniques such as electrochemical measurements, SEM-EDX, XRD, and µ-Raman spectroscopy, (2) continuous corrosion monitoring methods based on electrical resistivity loss of a corroding nm-sized metal wire and weight gain of a corroding silver coated quartz crystal, and (3) characterization of the visual degradation of the metal coupons. This study confirms that subtle differences in corrosivity between locations inside a museum can be determined on condition that the same corrosion rate assessment is used. However, the impact of the coupon orientation with respect to the prevailing direction of air circulation can be substantially larger than the impact of the coupon location.
Keywords: A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Antwerp Cultural Heritage Sciences (ARCHES)
Impact Factor: 1.455
Times cited: 3
DOI: 10.1007/S00339-016-0456-2
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“Neutron activation autoradiography and scanning macro-XRF of Rembrandt van Rijn's Susanna and the Elders (Gemaldegalerie Berlin) : a comparison of two methods for imaging of historical paintings with elemental contrast”. Alfeld M, Laurenze-Landsberg C, Denker A, Janssens K, Noble P, Applied physics A : materials science &, processing 119, 795 (2015). http://doi.org/10.1007/S00339-015-9081-8
Abstract: Imaging methods with elemental contrast are of great value for the investigation of historical paintings, as they allow for study of sub-surface layers that provide insight into a painting's creation process. Two of the most important methods are neutron activation autoradiography (NAAR) and scanning macro-XRF (MA-XRF). Given the differences between these methods in the fundamental physical phenomena exploited, a theoretical comparison of their capabilities is difficult and until now a critical comparison of their use on the same painting is missing. In this paper, we present a study of Rembrandt van Rijn's painting Susanna and the Elders from the Gemaldegalerie in Berlin employing both techniques. The painting features a considerable number of overpainted features and a wide range of pigments with different elemental tracers, including earth pigments (Mn/Fe), Azurite (Cu), lead white (Pb), vermilion (Hg) and smalt (Co, As). MA-XRF can detect all elements above Si (Z = 14), suffers from few spectral overlaps and can be performed in a few tens of hours in situ, i.e. in a museum. NAAR requires the stay of the painting at a research facility for several weeks, and inter-element interferences can be difficult to resolve. Also, only a limited number of elements contribute to the acquired autoradiographs, most notably Mn, Cu, As, Co, Hg and P. However, NAAR provides a higher lateral resolution and is less hindered by absorption in covering layers, which makes it the only method capable of visualizing P in lower paint layers.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 1.455
Times cited: 11
DOI: 10.1007/S00339-015-9081-8
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“Rembrandt's An Old Man in Military Costume: the underlying image re-examined”. Trentelman K, Janssens K, van der Snickt G, Szafran Y, Woollett AT, Dik J, Applied physics A : materials science &, processing 121, 801 (2015). http://doi.org/10.1007/S00339-015-9426-3
Abstract: The painting An Old Man in Military Costume in the J. Paul Getty Museum, by Rembrandt Harmensz van Rijn, was studied using two complementary, element-specific imaging techniques-neutron activation autoradiography (NAAR) and macro-X-ray fluorescence (MA-XRF) mapping-to reveal the second, hidden painting. NAAR provided a strong image of the face and cloak of the underlying figure, along with an indication of the chemical composition. The single-element distribution maps produced by MA-XRF mapping provided additional details into the shape of the underlying image and the composition of the pigments used. The underlying figure's face is richer in mercury, indicative of the pigment vermilion, than the face of the figure on the surface. Likewise, the cloak of the underlying figure is richer in copper than the surface figure though the identity of the copper-containing pigment cannot be determined from these data. The use of iron earth pigments, specifically Si-rich umbers, is indicated through the complementary information provided by the NAAR and MA-XRF maps. These data are used to create a false color digital reconstruction, yielding the most detailed representation of the underlying painting to date.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 1.455
Times cited: 22
DOI: 10.1007/S00339-015-9426-3
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“Resonant backward scattering of light by a subwavelength metallic slit with two open sides”. Kukhlevsky SV, Mechler M, Csapó, L, Janssens K, Samek O, Physical review : B : condensed matter and materials physics 72, 165421 (2005). http://doi.org/10.1103/PHYSREVB.72.165421
Abstract: The backward scattering of TM-polarized light by a two-side-open subwavelength slit in a metal film is analyzed. We show that the reflection coefficient versus wavelength possesses a Fabry-Perot-like dependence that is similar to the anomalous behavior of transmission reported in the study [Y. Takakura, Phys. Rev. Lett. 86, 5601 (2001)]. The open slit totally reflects the light at the near-to-resonance wavelengths. In addition, we show that the interference of incident and resonantly backward-scattered light produces in the near-field diffraction zone a spatially localized wave whose intensity is 10103 times greater than the incident wave, but one order of magnitude smaller than the intracavity intensity. The amplitude and phase of the resonant wave at the slit entrance and exit are different from that of a Fabry-Perot cavity.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 3.836
Times cited: 7
DOI: 10.1103/PHYSREVB.72.165421
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“Scanning XRF investigation of a Flower Still Life and its underlying composition from the collection of the Kröller-Muller Museum”. Alfeld M, van der Snickt G, Vanmeert F, Janssens K, Dik J, Appel K, van der Loeff L, Chavannes M, Meedendorp T, Hendriks E, Applied physics A : materials science &, processing 111, 165 (2013). http://doi.org/10.1007/S00339-012-7526-X
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 1.455
Times cited: 35
DOI: 10.1007/S00339-012-7526-X
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“Trace element fingerprinting of façon-de-Venise glass”. Šmit Ž, Bulska E, Janssens K, Bulska E, Wagner B, Kos M, Lazar I, Nuclear instruments and methods in physics research: B: beam interactions with materials and atoms 239, 94 (2005). http://doi.org/10.1016/J.NIMB.2005.06.182
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 1.109
Times cited: 27
DOI: 10.1016/J.NIMB.2005.06.182
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“Visualizing the 17th century underpainting in Portrait of an Old Man by Rembrandt van Rijn using synchrotron-based scanning macro-XRF”. Alfeld M, Siddons DP, Janssens K, Dik J, Woll A, Kirkham R, van de Wetering E, Applied physics A : materials science &, processing 111, 157 (2013). http://doi.org/10.1007/S00339-012-7490-5
Abstract: In 17th century Old Master Paintings, the underpainting generally refers to the first sketch of a composition. The underpainting is applied to a prepared ground using a monochrome, brown oil paint to roughly indicate light, shade and contours. So far, methods to visualize the underpainting-other than in localized cross-sections-have been very limited. Neither infrared reflectography nor neutron induced autoradiography have proven to be practical, adequate visualization tools. Thus, although of fundamental interest in the understanding of a painting's genesis, the underpainting has virtually escaped all imaging efforts. In this contribution we will show that 17th century underpainting may consist of a highly heterogeneous mixture of pigments, including copper pigments. We suggest that this brown pigment mixture is actually the recycled left-over of a palette scraping. With copper as the heaviest exclusive elemental component, we will hence show in a case study on a Portrait of an Old Man attributed to Rembrandt van Rijn how scanning macro-XRF can be used to efficiently visualize the underpainting below the surface painting and how this information can contribute to the discussion of the painting's authenticity.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 1.455
Times cited: 26
DOI: 10.1007/S00339-012-7490-5
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“2D X-ray and FTIR micro-analysis of the degradation of cadmium yellow pigment in paintings of Henri Matisse”. Pouyet E, Cotte M, Fayard B, Salome M, Meirer F, Mehta A, Uffelman ES, Hull A, Vanmeert F, Kieffer J, Burghammer M, Janssens K, Sette F, Mass J, Applied physics A : materials science &, processing 121, 967 (2015). http://doi.org/10.1007/S00339-015-9239-4
Abstract: The chemical and physical alterations of cadmium yellow (CdS) paints in Henri Matisse's The Joy of Life (1905-1906, The Barnes Foundation) have been recognized since 2006, when a survey by portable X-ray fluorescence identified this pigment in all altered regions of the monumental painting. This alteration is visible as fading, discoloration, chalking, flaking, and spalling of several regions of light to medium yellow paint. Since that time, synchrotron radiation-based techniques including elemental and spectroscopic imaging, as well as X-ray scattering have been employed to locate and identify the alteration products observed in this and related works by Henri Matisse. This information is necessary to formulate one or multiple mechanisms for degradation of Matisse's paints from this period, and thus ensure proper environmental conditions for the storage and the display of his works. This paper focuses on 2D full-field X-ray Near Edge Structure imaging, 2D micro-X-ray Diffraction, X-ray Fluorescence, and Fourier Transform Infra-red imaging of the altered paint layers to address one of the long-standing questions about cadmium yellow alteration-the roles of cadmium carbonates and cadmium sulphates found in the altered paint layers. These compounds have often been assumed to be photo-oxidation products, but could also be residual starting reagents from an indirect wet process synthesis of CdS. The data presented here allow identifying and mapping the location of cadmium carbonates, cadmium chlorides, cadmium oxalates, cadmium sulphates, and cadmium sulphides in thin sections of altered cadmium yellow paints from The Joy of Life and Matisse's Flower Piece (1906, The Barnes Foundation). Distribution of various cadmium compounds confirms that cadmium carbonates and sulphates are photo-degradation products in The Joy of Life, whereas in Flower Piece, cadmium carbonates appear to have been a [(partially) unreacted] starting reagent for the yellow paint, a role previously suggested in other altered yellow paints.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
DOI: 10.1007/S00339-015-9239-4
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“Coupled plasmon modes in 2D gold nanoparticle clusters and their effect on local temperature control”. Borah R, Verbruggen SW, The journal of physical chemistry: C : nanomaterials and interfaces 123, 30594 (2019). http://doi.org/10.1021/ACS.JPCC.9B09048
Abstract: Assemblies of closely separated gold nanoparticles exhibit a strong collective plasmonic response due to coupling of the plasmon modes of the individual nanostructures. In the context of self-assembly of nanoparticles, close-packed two-dimensional (2D) clusters of spherical nanoparticles present an important composite system that promises numerous applications. The present study probes the collective plasmonic characteristics and resulting photothermal behavior of close-packed 2D Au nanoparticle clusters to delineate the effects of the cluster size, interparticle distance, and particle size. Smaller nanoparticles (20 and 40 nm in diameter) that exhibit low individual scattering and high absorption were considered for their relevance to photothermal applications. In contrast to typical literature studies, the present study compares the optical response of clusters of different sizes ranging from a single nanoparticle up to large assemblies of 61 nanoparticles. Increasing the cluster size induces significant changes to the spectral position and optophysical characteristics. Based on the model outcome, an optimal cluster size for maximum absorption per nanoparticle is also determined for enhanced photothermal effects. The effect of the particle size and interparticle distance is investigated to elucidate the nature of interaction in terms of near-field and far-field coupling. The photothermal effect resulting from absorption is compared for different cluster sizes and interparticle distances considering a homogeneous water medium. A strong dependence of the steady-state temperature of the nanoparticles on the cluster size, particle position in the cluster, incident light polarization, and interparticle distance provides new physical insight into the local temperature control of plasmonic nanostructures.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 4.536
DOI: 10.1021/ACS.JPCC.9B09048
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“Impact of tank construction on corrosion of ship ballast tanks”. de Baere K, Verstraelen H, Dewil R, Lemmens L, Lenaerts S, Nkunzimana T, Potters G, Materials performance 49, 48 (2010)
Keywords: A1 Journal article; Theory of quantum systems and complex systems; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 0.149
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“In situ study of ballast tank corrosion on ships: part 1”. Verstraelen H, de Baere K, Schillemans W, Lemmens L, Dewil R, Lenaerts S, Potters G, Materials performance 48, 48 (2009)
Keywords: A1 Journal article; Engineering sciences. Technology; Theory of quantum systems and complex systems; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 0.149
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“In situ study of ballast tank corrosion on ships: part 2”. Verstraelen H, de Baere K, Schillemans W, Lemmens L, Dewil R, Lenaerts S, Potters G, Materials performance 48, 54 (2009)
Abstract: A study was undertaken to determine causes and effects of corrosion processes in ballast tanks. Part 1 of this article (October 2009 MP) described the data collection. Part 2 describes the development of a corrosion index (CI) derived from the general International Association of Classification Societies corrosion assessment methods. The CI can be used in situ to assess ballast tank corrosion. An average timeline for-corrosion of tanks is presented.
Keywords: A1 Journal article; Engineering sciences. Technology; Theory of quantum systems and complex systems; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 0.149
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“Mesoporous TiO2 from poly(N,N-dimethylacrylamide)-b-polystyrene block copolymers for long-term acetaldehyde photodegradation”. Billet J, Vandewalle S, Meire M, Blommaerts N, Lommens P, Verbruggen SW, De Buysser K, Du Prez F, Van Driesche I, Journal of materials science 55, 1933 (2019). http://doi.org/10.1007/S10853-019-04024-3
Abstract: Although already some mesoporous (2–50 nm) sol–gel TiO2 synthesis strategies exist, no pore size control beyond the 12 nm range is possible without using specialized organic structure-directing agents synthetized via controlled anionic/radical polymerizations. Here, we present the use of reversible addition–fragmentation chain transfer (RAFT) polymerization as a straightforward and industrial applicable alternative to the existing controlled polymerization methods for structure-directing agent synthesis. Poly(N,N-dimethylacrylamide)-block-polystyrene (PDMA-b-PS) block copolymer, synthesized via RAFT, was chosen as structure-directing agent for the formation of the mesoporous TiO2. Crack-free thin layers TiO2 with tunable pores from 8 to 45 nm could be acquired. For the first time, in a detailed and systematic approach, the influence of the block size and dispersity of the block copolymer is experimentally screened for their influence on the final meso-TiO2 layers. As expected, the mesoporous TiO2 pore sizes showed a clear correlation to the polystyrene block size and the dispersity of the PDMA-b-PS block copolymer. Surprisingly, the dispersity of the polymer was shown not to be affecting the standard deviation of the pores. As a consequence, RAFT could be seen as a viable alternative to the aforementioned controlled polymerization reactions for the synthesis of structure-directing agents enabling the formation of mesoporous pore size-controlled TiO2. To examine the photocatalytic activity of the mesoporous TiO2 thin layers, the degradation of acetaldehyde, a known indoor pollutant, was studied. Even after 3 years of aging, the TiO2 thin layer retained most of its activity.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 2.599
Times cited: 2
DOI: 10.1007/S10853-019-04024-3
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“Microwave-assisted synthesis of mesoporous titania with increased crystallinity, specific surface area, and photocatalytic activity”. Meire M, Verbruggen SW, Lenaerts S, Lommens P, Van Der Voort P, Van Driessche I, Journal of materials science 51, 9822 (2016). http://doi.org/10.1007/S10853-016-0215-Y
Abstract: Mesoporous titanium dioxide is a material finding its use in a wide range of applications. For many of these, it is important to achieve a high degree of crystallinity in the material. It is generally accepted that the use of the soft templating approach to synthesize mesoporous titania, results in a compromise between crystallinity and specific surface area due to thermal instability of the used templates. In this paper, we explore how the use of microwave irradiation can influence the crystallinity, specific surface area, and the electronic properties of mesoporous titania. Therefore, we combined microwave radiation with an evaporation-induced self-assembly (EISA) synthesis. We show that additional microwave treatment at carefully chosen synthesis steps can enhance the crystallinity with 20 % without causing significant loss of surface area (>360 m2/g). Surface photovoltage measurements were used to investigate the electronic properties. The photocatalytic activity of the samples was evaluated in aqueous media by following the degradation of an industrial dye, methylene blue, and the herbicide isoproturon under UV irradiation and in gaseous media looking at the degradation of acetaldehyde, a common indoor pollutant under UVA irradiation. In all cases, the microwave treatment results in more active materials.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 2.599
Times cited: 8
DOI: 10.1007/S10853-016-0215-Y
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“Plasma-enhanced atomic layer deposition of silver using Ag(fod)(PEt3) and NH3-plasma”. Minjauw MM, Solano E, Sree SP, Asapu R, Van Daele M, Ramachandran RK, Heremans G, Verbruggen SW, Lenaerts S, Martens JA, Detavernier C, Dendooven J, Chemistry of materials 29, 7114 (2017). http://doi.org/10.1021/ACS.CHEMMATER.7B00690
Abstract: A plasma-enhanced atomic layer deposition (ALD) process using the Ag(fod)(PEt3) precursor [(triethylphosphine)(6,6,7,7,8,8,8-heptafluoro-2,2-dimethy1-3,5-octanedionate)silver(I)] in combination with NH3-plasma is reported. The steady growth rate of the reported process (0.24 +/- 0.03 nm/cycle) was found to be 6 times larger than that of the previously reported Ag ALD process based on the same precursor in combination with H-2-plasma (0.04 +/- 0.02 nm/cycle). The ALD characteristics of the H-2-plasma and NH3-plasma processes were verified. The deposited Ag films were polycrystalline face-centered cubic Ag for both processes. The film morphology was investigated by ex situ scanning electron microscopy and grazing-incidence small-angle X-ray scattering, and it was found that films grown with the NH3-plasma process exhibit a much higher particle areal density and smaller particle sizes on oxide substrates compared to those deposited using the H-2-plasma process. This control over morphology of the deposited Ag is important for applications in catalysis and plasmonics. While films grown with the H-2-plasma process had oxygen impurities (similar to 9 atom %) in the bulk, the main impurity for the NH3-plasma process was nitrogen (similar to 7 atom %). In situ Fourier transform infrared spectroscopy experiments suggest that these nitrogen impurities are derived from NH surface groups generated during the NH3-plasma, which interact with the precursor molecules during the precursor pulse. We propose that the reaction of these surface groups with the precursor leads to additional deposition of Ag atoms during the precursor pulse compared to the H-2-plasma process, which explains the enhanced growth rate of the NH3-plasma process.
Keywords: A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 9.466
Times cited: 9
DOI: 10.1021/ACS.CHEMMATER.7B00690
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“Predicting the surface plasmon resonance wavelength of gold-silver alloy nanoparticles”. Verbruggen SW, Keulemans M, Martens JA, Lenaerts S, The journal of physical chemistry: C : nanomaterials and interfaces 117, 19142 (2013). http://doi.org/10.1021/JP4070856
Abstract: Gold-silver alloy nanoparticles display surface plasmon resonance (SPR) over a broad range of the UV-vis spectrum. We propose a model to predict the SPR wavelength of gold-silver alloy colloids based on the combined effect of alloy composition and particle size. The SPR wavelength is derived from extinction spectra simulated using available experimental dielectric constant data and accounts for particle size by applying Mie theory. Comparison of calculated values with experimental data evidences the accuracy of the model. The new SPR wavelength estimation tool will be of particular interest for developing dedicated bimetallic plasmonic nanostructures.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 4.536
Times cited: 51
DOI: 10.1021/JP4070856
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“The future of organic photovoltaic solar cells as a direct power source for consumer electronics”. Lizin S, Van Passel S, De Schepper E, Vranken L, Solar Energy Materials And Solar Cells 103, 1 (2012). http://doi.org/10.1016/J.SOLMAT.2012.04.001
Abstract: As the search for marketable photovoltaic solar cells continues, organic photovoltaic (OPV) solar cells have been identified as a technology with many attractive features for commercialization. Most photovoltaic technologies on the market today were improved in the consumer electronics market segment. A similar evolution has been envisioned for OPV. Hence this paper investigates consumer preferences for solar cells directly powering consumer electronics. Choice experiments were designed and responses were collected using a random sample of 300 individuals from the Flemish region (northern part of Belgium). Results allow for computation of attribute importance, willingness to pay (WTP), and simulation of theoretical market share. These measures point towards OPV being able to reach considerable market share in the long run, bearing in mind that efforts are first needed in elevating OPV's efficiency and lifetime as they most determine consumers' preferences. Price is found to be the least important product characteristic for OPV solar cells to be incorporated in consumer electronics devices. We therefore warn against generalizing attributes' importance across the boundaries of market segments. (C) 2012 Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; Engineering sciences. Technology; Engineering Management (ENM)
Impact Factor: 4.784
Times cited: 25
DOI: 10.1016/J.SOLMAT.2012.04.001
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“Heterogeneity in the solar-powered consumer electronics market : a discrete choice experiments study”. Lizin S, Van Passel S, Vranken L, Solar Energy Materials And Solar Cells 156, 140 (2016). http://doi.org/10.1016/J.SOLMAT.2016.04.060
Abstract: Solar-powered consumer electronics are a likely starting point for organic photovoltaic (OPV) market development. Therefore, a generic discrete choice experiments study can determine how Flemish consumers value solar-cell characteristics for solar-poweied consumer electronics. Such characteristics include efficiency, lifetime, aesthetics, integratability, and price. We contribute to the literature by investigating preference heterogeneity in a solar-power niche market with an experimental design with a fixed reference alternative. The error components random parameter logit (ECRPL) with interactions provides a better fit than the latent class (LC) model for our choice data. The main effects had the expected signs. Consequently, aesthetics and integratability are OPV's assets. Nevertheless, heterogeneity puts the results that are valid for the average consumer into perspective. Based on our findings, OPV commercialization efforts should target the experienced, impatient user who highly values design and functionality. (C) 2016 Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; Engineering sciences. Technology; Engineering Management (ENM)
Impact Factor: 4.784
Times cited: 2
DOI: 10.1016/J.SOLMAT.2016.04.060
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“Applications of plasma-liquid systems : a review”. Rezaei F, Vanraes P, Nikiforov A, Morent R, De Geyter N, Materials 12, 2751 (2019). http://doi.org/10.3390/MA12172751
Abstract: Plasma-liquid systems have attracted increasing attention in recent years, owing to their high potential in material processing and nanoscience, environmental remediation, sterilization, biomedicine, and food applications. Due to the multidisciplinary character of this scientific field and due to its broad range of established and promising applications, an updated overview is required, addressing the various applications of plasma-liquid systems till now. In the present review, after a brief historical introduction on this important research field, the authors aimed to bring together a wide range of applications of plasma-liquid systems, including nanomaterial processing, water analytical chemistry, water purification, plasma sterilization, plasma medicine, food preservation and agricultural processing, power transformers for high voltage switching, and polymer solution treatment. Although the general understanding of plasma-liquid interactions and their applications has grown significantly in recent decades, it is aimed here to give an updated overview on the possible applications of plasma-liquid systems. This review can be used as a guide for researchers from different fields to gain insight in the history and state-of-the-art of plasma-liquid interactions and to obtain an overview on the acquired knowledge in this field up to now.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 2.654
Times cited: 4
DOI: 10.3390/MA12172751
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“Growth mechanism of epitaxial SrTiO3 on a (1 x 2) + (2 x 1) reconstructed Sr(1/2 ML)/Si(001) surface”. Spreitzer M, Klement D, Egoavil R, Verbeeck J, Kovac J, Zaloznik A, Koster G, Van Tendeloo G, Suvorov D, Rijnders G, Journal Of Materials Chemistry C 8, 518 (2020). http://doi.org/10.1039/C9TC04092G
Abstract: Sub-monolayer control over the growth at silicon-oxide interfaces is a prerequisite for epitaxial integration of complex oxides with the Si platform, enriching it with a variety of functionalities. However, the control over this integration is hindered by the intense reaction of the constituents. The most suitable buffer material for Si passivation is metallic strontium. When it is overgrown with a layer of SrTiO3 (STO) it can serve as a pseudo-substrate for the integration with functional oxides. In our study we determined a mechanism for epitaxial integration of STO with a (1 x 2) + (2 x 1) reconstructed Sr(1/2 ML)/Si(001) surface using all-pulsed laser deposition (PLD) technology. A detailed analysis of the initial deposition parameters was performed, which enabled us to develop a complete protocol for integration, taking into account the peculiarities of the PLD growth, STO critical thickness, and process thermal budget, in order to kinetically trap the reaction between STO and Si and thus to minimize the thickness of the interface layer. The as-prepared oxide layer exhibits STO(001)8Si(001) out-of-plane and STO[110]8Si[100] in-plane orientation and together with recent advances in large-scale PLD tools these results represent a new technological solution for the implementation of oxide electronics on demand.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 6.4
Times cited: 12
DOI: 10.1039/C9TC04092G
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“Mechanistic studies of gas reactions with multicomponent solids : what can we learn by combining NAP XPS and atomic resolution STEM/EDX?”.Sirotina AP, Callaert C, Volykhov AA, Frolov AS, Sanchez-Barriga J, Knop-Gericke A, Hadermann J, Yashina LV, The journal of physical chemistry: C : nanomaterials and interfaces 123, 26201 (2019). http://doi.org/10.1021/ACS.JPCC.9B05052
Abstract: Rapid development of experimental techniques has enabled real time studies of solid gas reactions at the level reaching the atomic scale. In the present paper, we focus on a combination of atomic resolution STEM/EDX, which visualizes the reaction zone, and near ambient pressure (NAP) XPS, which collects information for a surface layer of variable thickness under reaction conditions. We compare the behavior of two affined topological insulators, Bi2Te3 and Sb2Te3. We used a simple reaction with molecular oxygen occurring at 298 K, which is of practical importance to avoid material degradation. Despite certain limitations, a combination of in situ XPS and ex situ cross-sectional STEM/EDX allowed us to obtain a self-consistent picture of the solid gas reaction mechanism for oxidation of Sb2Te3 and Bi2Te3 crystals, which includes component redistribution between the oxide and the subsurface layer and Te segregation with formation of a thin ordered layer at the interface. The process is multistep in case of both compounds. At the very beginning of the oxidation process the reactivity is determined by the energy benefit of the corresponding element oxygen bond formation. Further in the oxidation process, the behavior of these two compounds becomes similar and features component redistribution between the oxide and the subsurface layer.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 4.536
DOI: 10.1021/ACS.JPCC.9B05052
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“Nonlayered CdSe flakes homojunctions”. Jin B, Liang F, Hu Z-Y, Wei P, Liu K, Hu X, Van Tendeloo G, Lin Z, Li H, Zhou X, Xiong Q, Zhai T, Advanced Functional Materials 30, 1908902 (2020). http://doi.org/10.1002/ADFM.201908902
Abstract: 2D homojunctions have stimulated extensive attention because of their perfect thermal and lattice matches, as well as their tunable band structures in 2D morphology, which provide fascinating opportunities for novel electronics and optoelectronics. Recently, 2D nonlayered materials have attracted the attention of researchers owing to their superior functional applications and diverse portfolio of the 2D family. Therefore, 2D nonlayered homojunctions would open the door to a rich spectrum of exotic 2D materials. However, they are not investigated due to their extremely difficult synthesis methods. Herein, nonlayered CdSe flakes homojunctions are obtained via self-limited growth with InCl3 as a passivation agent. Interestingly, two pieces of vertical wurtzite-zinc blende (WZ-ZB) homojunctions epitaxially integrate into WZ/ZB lateral junctions. These homojunctions show a divergent second-harmonic generation intensity, strongly correlated to the multiple twinned ZB phase, as identified by aberration-corrected scanning transmission electron microscopy and theoretical calculations. Impressively, the photodetector based on this WZ/ZB CdSe homojunction shows excellent performances, integrating a high photoswitching ratio (3.4 x 10(5)) and photoresponsivity (3.7 x 10(3) A W-1), suggesting promising potential for applications in electronics and optoelectronics.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 19
Times cited: 8
DOI: 10.1002/ADFM.201908902
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“Structural, electronic and vibrational properties of ultra-thin octahedrally coordinated structure of EuO2”. Ozcan M, Ozen S, Yagmurcukardes M, Sahin H, Journal Of Magnetism And Magnetic Materials 493, 165668 (2020). http://doi.org/10.1016/J.JMMM.2019.165668
Abstract: Novel stable ultra-thin phases of europium oxide are investigated by means of state-of-the-art first principles calculations. Total energy calculations show that single layers of EuO2 and Eu(OH)(2) can be stabilized in an octahedrally coordinated (1T) atomic structure. However, phonon calculations reveal that although both structures are energetically feasible, only the 1T-EuO2 phase has dynamical stability. The phonon spectrum of 1T-EuO2 displays three Raman active modes; a non-degenerate out-of-plane A(1g) mode at 353.5 cm(-1) and two doubly-degenerate in-plane E-g modes at 304.3 cm(-1). Furthermore, magnetic ground state and electronic band dispersion calculations show that the single layer EuO2 is a metal with net magnetic moment of 5(mu B) per unitcell resulting in a half-metallic ferrimagnetic behavior. Moreover, robustness of the half-metallic ferrimagnetic characteristics of EuO2 is confirmed by the application of electric field and charging. Single layer 1T-EuO2, with its stable ultra-thin structure and half-metallic ferrimagnetic feature, is a promising novel material for nanoscale electronic and spintronic applications.
Keywords: A1 Journal article; Condensed Matter Theory (CMT)
Impact Factor: 2.7
Times cited: 1
DOI: 10.1016/J.JMMM.2019.165668
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“Tailoring vanadium dioxide film orientation using nanosheets : a combined microscopy, diffraction, transport, and soft X-ray in transmission study”. Tran Phong Le P, Hofhuis K, Rana A, Huijben M, Hilgenkamp H, Rijnders GAJHM, ten Elshof JE, Koster G, Gauquelin N, Lumbeeck G, Schuessler-Langeheine C, Popescu H, Fortuna F, Smit S, Verbeek XH, Araizi-Kanoutas G, Mishra S, Vaskivskyi I, Duerr HA, Golden MS, Advanced Functional Materials 30, 1900028 (2020). http://doi.org/10.1002/ADFM.201900028
Abstract: Vanadium dioxide (VO2) is a much-discussed material for oxide electronics and neuromorphic computing applications. Here, heteroepitaxy of VO2 is realized on top of oxide nanosheets that cover either the amorphous silicon dioxide surfaces of Si substrates or X-ray transparent silicon nitride membranes. The out-of-plane orientation of the VO2 thin films is controlled at will between (011)(M1)/(110)(R) and (-402)(M1)/(002)(R) by coating the bulk substrates with Ti0.87O2 and NbWO6 nanosheets, respectively, prior to VO2 growth. Temperature-dependent X-ray diffraction and automated crystal orientation mapping in microprobe transmission electron microscope mode (ACOM-TEM) characterize the high phase purity, the crystallographic and orientational properties of the VO2 films. Transport measurements and soft X-ray absorption in transmission are used to probe the VO2 metal-insulator transition, showing results of a quality equal to those from epitaxial films on bulk single-crystal substrates. Successful local manipulation of two different VO2 orientations on a single substrate is demonstrated using VO2 grown on lithographically patterned lines of Ti0.87O2 and NbWO6 nanosheets investigated by electron backscatter diffraction. Finally, the excellent suitability of these nanosheet-templated VO2 films for advanced lensless imaging of the metal-insulator transition using coherent soft X-rays is discussed.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 19
Times cited: 1
DOI: 10.1002/ADFM.201900028
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“Vertical van der Waals heterostructure of single layer InSe and SiGe”. Eren I, Ozen S, Sozen Y, Yagmurcukardes M, Sahin H, The journal of physical chemistry: C : nanomaterials and interfaces 123, 31232 (2019). http://doi.org/10.1021/ACS.JPCC.9B06404
Abstract: We present a first-principles investigation on the stability, electronic structure, and mechanical response of ultrathin heterostructures composed of single layers of InSe and SiGe. First, by performing total energy optimization and phonon calculations, we show that single layers of InSe and SiGe can form dynamically stable heterostructures in 12 different stacking types. Valence and conduction band edges of the heterobilayers form a type-I heterojunction having a tiny band gap ranging between 0.09 and 0.48 eV. Calculations on elastic-stiffness tensor reveal that two mechanically soft single layers form a heterostructure which is stiffer than the constituent layers because of relatively strong interlayer interaction. Moreover, phonon analysis shows that the bilayer heterostructure has highly Raman active modes at 205.3 and 43.7 cm(-1), stemming from the out-of-plane interlayer mode and layer breathing mode, respectively. Our results show that, as a stable type-I heterojunction, ultrathin heterobilayer of InSe/SiGe holds promise for nanoscale device applications.
Keywords: A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Impact Factor: 4.536
DOI: 10.1021/ACS.JPCC.9B06404
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“Accelerated molecular dynamics simulation of large systems with parallel collective variable-driven hyperdynamics”. Fukuhara S, Bal KM, Neyts EC, Shibuta Y, Computational Materials Science 177, 109581 (2020). http://doi.org/10.1016/j.commatsci.2020.109581
Abstract: The limitation in time and length scale is a major issue of molecular dynamics (MD) simulation. Although several methods have been developed to extend the MD time scale, their performance usually deteriorates with increasing system size. Therefore, an acceleration method which is applicable to large systems is required to bridge the gap between the MD simulations and target phenomena. In this study, an accelerated MD method for large system is developed based on the collective variable-driven hyperdynamics (CVHD) method [K.M. Bal and E.C. Neyts, 2015]. The key idea is to run CVHD in parallel with rate control and accelerate multiple possible events simultaneously. Using this novel method, carbon diffusion in bcc-iron bicrystal with grain boundary is examined as an application for practical materials. Carbon atoms reaching at the grain boundary are trapped whereas carbon atoms in the bulk region diffuse randomly, and both dynamic regimes can be simultaneously accelerated with the parallel CVHD technique.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 3.3
DOI: 10.1016/j.commatsci.2020.109581
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“Unraveling the Role of Lattice Substitutions on the Stabilization of the Intrinsically Unstable Pb2Sb2O7Pyrochlore: Explaining the Lightfastness of Lead Pyroantimonate Artists&rsquo, Pigments”. Marchetti A, Saniz R, Krishnan D, Rabbachin L, Nuyts G, De Meyer S, Verbeeck J, Janssens K, Pelosi C, Lamoen D, Partoens B, De Wael K, Chemistry Of Materials 32, 2863 (2020). http://doi.org/10.1021/acs.chemmater.9b04821
Abstract: The pyroantimonate pigments Naples yellow and lead tin antimonate yellow are recognized as some of the most stable synthetic yellow pigments in the history of art. However, this exceptional lightfastness is in contrast with experimental evidence suggesting that this class of mixed oxides is of semiconducting nature. In this study the electronic structure and light-induced behavior of the lead pyroantimonate pigments were determined by means of a combined multifaceted analytical and computational approach (photoelectrochemical measurements, UV-vis diffuse reflectance spectroscopy, STEM-EDS, STEM-HAADF, and density functional theory calculations). The results demonstrate both the semiconducting nature and the lightfastness of these pigments. Poor optical absorption and minority carrier mobility are the main properties responsible for the observed stability. In addition, novel fundamental insights into the role played by Na atoms in the stabilization of the otherwise intrinsically unstable Pb2Sb2O7 pyrochlore were obtained.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT)
Impact Factor: 8.6
Times cited: 8
DOI: 10.1021/acs.chemmater.9b04821
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“Thermal-strain-engineered ferromagnetism of LaMnO3/SrTiO3 heterostructures grown on silicon”. Chen B, Gauquelin N, Reith P, Halisdemir U, Jannis D, Spreitzer M, Huijben M, Abel S, Fompeyrine J, Verbeeck J, Hilgenkamp H, Rijnders G, Koster G, Physical review materials 4, 024406 (2020). http://doi.org/10.1103/PhysRevMaterials.4.024406
Abstract: The integration of oxides on Si remains challenging, which largely hampers the practical applications of oxide-based electronic devices with superior performance. Recently, LaMnO3/SrTiO3 (LMO/STO) heterostructures have gained renewed interest for the debating origin of the ferromagnetic-insulating ground state as well as for their spin-filter applications. Here we report on the structural and magnetic properties of high-quality LMO/STO heterostructures grown on silicon. The chemical abruptness across the interface was investigated by atomic-resolution scanning transmission electron microscopy. The difference in the thermal expansion coefficients between LMO and Si imposed a large biaxial tensile strain to the LMO film, resulting in a tetragonal structure with c/a∼ 0.983. Consequently, we observed a significantly suppressed ferromagnetism along with an enhanced coercive field, as compared to the less distorted LMO film (c/a∼1.004) grown on STO single crystal. The results are discussed in terms of tensile-strain enhanced antiferromagnetic instabilities. Moreover, the ferromagnetism of LMO on Si sharply disappeared below a thickness of 5 unit cells, in agreement with the LMO/STO case, pointing to a robust critical behavior irrespective of the strain state. Our results demonstrate that the growth of oxide films on Si can be a promising way to study the tensile-strain effects in correlated oxides, and also pave the way towards the integration of multifunctional oxides on Si with atomic-layer control.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.4
Times cited: 6
DOI: 10.1103/PhysRevMaterials.4.024406
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“Co valence transformation in isopolar LaCoO3/LaTiO3 perovskite heterostructures via interfacial engineering”. Araizi-Kanoutas G, Geessinck J, Gauquelin N, Smit S, Verbeek XH, Mishra SK, Bencok P, Schlueter C, Lee T-L, Krishnan D, Fatermans J, Verbeeck J, Rijnders G, Koster G, Golden MS, Physical review materials 4, 026001 (2020). http://doi.org/10.1103/PhysRevMaterials.4.026001
Abstract: We report charge transfer up to a single electron per interfacial unit cell across nonpolar heterointerfaces from the Mott insulator LaTiO3 to the charge transfer insulator LaCoO3. In high-quality bi- and trilayer systems grown using pulsed laser deposition, soft x-ray absorption, dichroism, and scanning transmission electron microscopy-electron energy loss spectroscopy are used to probe the cobalt-3d electron count and provide an element-specific investigation of the magnetic properties. The experiments show the cobalt valence conversion is active within 3 unit cells of the heterointerface, and able to generate full conversion to 3d7 divalent Co, which displays a paramagnetic ground state. The number of LaTiO3/LaCoO3 interfaces, the thickness of an additional, electronically insulating “break” layer between the LaTiO3 and LaCoO3, and the LaCoO3 film thickness itself in trilayers provide a trio of control knobs for average charge of the cobalt ions in LaCoO3, illustrating the efficacy of O−2p band alignment as a guiding principle for property design in complex oxide heterointerfaces.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.4
Times cited: 13
DOI: 10.1103/PhysRevMaterials.4.026001
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“Circumventing Wear and Tear of Adaptive Porous Materials”. Canossa S, Ji Z, Wuttke S, Advanced Functional Materials , 1908547 (2020). http://doi.org/10.1002/adfm.201908547
Abstract: The assessment of the architectural stability of molecular porous materials is not yet a common practice, but critical to their understanding and development. The conformational adaptation of porous materials to guest binding and other chemical dynamics poses a risk of architectural damage, leading to performance deterioration during their prolonged usage. The deformation of the framework backbone and the disconnection of building units are driven by chemical, mechanical, and thermal perturbations, and can be quantitatively described by the term connection completeness. Analytical means that can be used to measure this parameter are presented in order to provide a standard, practical protocol for evaluating architectural damage made to framework materials. Preventive and remedial strategies are proposed for enhancing the architectural integrity of frameworks without compromising their functional mechanisms, paving the way to the design of robust yet adaptive materials. In this way, the discussion on architectural stability is initiated, and readers are encouraged to carefully characterize molecular porous materials for a better understanding of their structure-property relationship.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 19
DOI: 10.1002/adfm.201908547
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