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“Structural characterization of Er-doped Li2O-Al2O3-SiO2 glass ceramics”. Krsmanovic R, Bals S, Bertoni G, Van Tendeloo G, Optical materials 30, 1183 (2008). http://doi.org/10.1016/j.optmat.2007.05.045
Abstract: Particularly favourable properties of glass ceramics are developed on the basis of two key advantages of these materials: the variation of chemical composition and of microstructure. Therefore, detailed structural and chemical information are necessary to get insight in novel glass ceramic materials. We present here two examples of Er-doped Li2O-Al2O3-SiO2, with different quantities of ZrO2, both obtained with sol-gel synthesis. Different transmission electron microscopy techniques: conventional TEM, HRTEM, and EELS are used and the results are compared with those previously obtained with XRD and Rietveld analysis. We also demonstrate the 3D reconstruction, obtained from HAADF-STEM imaging, to determine the morphology of nanosize precipitates in these composites. (c) 2007 Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.238
Times cited: 12
DOI: 10.1016/j.optmat.2007.05.045
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“Achieving High Moisture Tolerance in Pseudohalide Perovskite Nanocrystals for Light-Emitting Diode Application”. Bhatia H, Keshavarz M, Martin C, Van Gaal L, Zhang Y, de Coen B, Schrenker NJ, Valli D, Ottesen M, Bremholm M, Van de Vondel J, Bals S, Hofkens J, Debroye E, ACS Applied Optical Materials 1, 1184 (2023). http://doi.org/10.1021/acsaom.3c00096
Abstract: The addition of potassium thiocyanate (KSCN) to the FAPbBr3 structure and subsequent post-treatment of nanocrystals (NCs) lead to high quantum confinement, resulting in a photoluminescent quantum yield (PLQY) approaching unity and microsecond decay times. This synergistic approach demonstrated exceptional stability under humid conditions, retaining 70% of the PLQY for over a month, while the untreated NCs degrade within 24 h. Additionally, the devices incorporating the post-treated NCs displayed 1.5% external quantum efficiency (EQE), a 5-fold improvement over untreated devices. These results provide promising opportunities for the use of perovskites in moisture-stable optoelectronics.
Keywords: A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;
DOI: 10.1021/acsaom.3c00096
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“Three-Dimensional Nanoparticle Transformations Captured by an Electron Microscope”. Albrecht W, Van Aert S, Bals S, Accounts Of Chemical Research 54, 1189 (2021). http://doi.org/10.1021/acs.accounts.0c00711
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 20.268
Times cited: 12
DOI: 10.1021/acs.accounts.0c00711
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“Surfactant layers on gold nanorods”. Mosquera J, Wang D, Bals S, Liz-Marzan LM, Accounts of chemical research 56, 1204 (2023). http://doi.org/10.1021/ACS.ACCOUNTS.3C00101
Abstract: Gold nanorods (Au NRs) are an exceptionally promising tool in nanotechnology due to three key factors: (i) their strong interaction with electromagnetic radiation, stemming from their plasmonic nature, (ii) the ease with which the resonance frequency of their longitudinal plasmon mode can be tuned from the visible to the near-infrared region of the electromagnetic spect r u m based on their aspect ratio, and (iii) their simple and cost-effective preparation through seed-mediated chemical growth. In this synthetic method, surfactants play a critical role in controlling the size, shape, and colloidal stabi l i t y of Au NRs. For example, surfactants can stabilize specific crystallographic facets during the formation of Au NRs, leading to t h e formation of NRs with specific morphologies. The process of surfactant adsorption onto the NR surface may result in various assemblies of surfactant molecules, such as spherical micelles, elongated micelles, or bilayers. Again, the assembly mode is critical toward determining the further availabi l i t y of the Au NR surface to the surrounding medium. Despite its importance and a great deal of research effort, the interaction between Au NPs and surfactants remains insufficiently understood, because the assembly process is influenced by numerous factors, including the chemical nature of the surfactant, the surface morphology of Au NPs, and solution parameters. Therefore, gaining a more comprehensive understanding of these interactions is essential to unlock the full potential of the seed-mediated growth method and the applications of plasmonic NPs. A plethora of characterization techniques have been applied to reach such an understanding , but many open questions remain. In this Account, we review the current knowledge on the interactions between surfactants and Au NRs. We briefly introduce the state-of-the-art methods for synthesizing Au NRs and highlight the crucial role of cationic surfactants during this process. The self-assembly and organization of surfactants on the Au NR surface is then discussed to better understand their role in seed-mediated growth. Subsequently, we provide examples and elucidate how chemical additives can be used to modulate micellar assemblies, in turn allowing for a finer control over the growth of Au NRs, including chiral NRs. Next, we review the main experimental characterization and computational modeling techniques that have been applied to shed light on the arrangement of surfactants on Au NRs and summarize the advantages and disadvantages for each technique. The Account ends with a “Conclusions and Outlook” section, outlining promising future research directions and developments that we consider are sti l l required, mostly related to the application of electron microscopy in liquid and in 3D. Finally, we remark on the potential of exploiting machine learning techniques to predict synthetic routes for NPs with predefined structures and properties.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 18.3
Times cited: 8
DOI: 10.1021/ACS.ACCOUNTS.3C00101
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“Al2O3-Supported Transition Metals for Plasma-Catalytic NH3 Synthesis in a DBD Plasma: Metal Activity and Insights into Mechanisms”. Gorbanev Y, Engelmann Y, van’t Veer K, Vlasov E, Ndayirinde C, Yi Y, Bals S, Bogaerts A, Catalysts 11, 1230 (2021). http://doi.org/10.3390/catal11101230
Abstract: N2 fixation into NH3 is one of the main processes in the chemical industry. Plasma catalysis is among the environmentally friendly alternatives to the industrial energy-intensive Haber-Bosch process. However, many questions remain open, such as the applicability of the conventional catalytic knowledge to plasma. In this work, we studied the performance of Al2O3-supported Fe, Ru, Co and Cu catalysts in plasma-catalytic NH3 synthesis in a DBD reactor. We investigated the effects of different active metals, and different ratios of the feed gas components, on the concentration and production rate of NH3, and the energy consumption of the plasma system. The results show that the trend of the metal activity (common for thermal catalysis) does not appear in the case of plasma catalysis: here, all metals exhibited similar performance. These findings are in good agreement with our recently published microkinetic model. This highlights the virtual independence of NH3 production on the metal catalyst material, thus validating the model and indicating the potential contribution of radical adsorption and Eley-Rideal reactions to the plasma-catalytic mechanism of NH3 synthesis.
Keywords: A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Movement Antwerp (MOVANT)
Impact Factor: 3.082
Times cited: 19
DOI: 10.3390/catal11101230
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“Quantitative atomic resolution mapping using high-angle annular dark field scanning transmission electron microscopy”. Van Aert S, Verbeeck J, Erni R, Bals S, Luysberg M, van Dyck D, Van Tendeloo G, Ultramicroscopy 109, 1236 (2009). http://doi.org/10.1016/j.ultramic.2009.05.010
Abstract: A model-based method is proposed to relatively quantify the chemical composition of atomic columns using high angle annular dark field (HAADF) scanning transmission electron microscopy (STEM) images. The method is based on a quantification of the total intensity of the scattered electrons for the individual atomic columns using statistical parameter estimation theory. In order to apply this theory, a model is required describing the image contrast of the HAADF STEM images. Therefore, a simple, effective incoherent model has been assumed which takes the probe intensity profile into account. The scattered intensities can then be estimated by fitting this model to an experimental HAADF STEM image. These estimates are used as a performance measure to distinguish between different atomic column types and to identify the nature of unknown columns with good accuracy and precision using statistical hypothesis testing. The reliability of the method is supported by means of simulated HAADF STEM images as well as a combination of experimental images and electron energy-loss spectra. It is experimentally shown that statistically meaningful information on the composition of individual columns can be obtained even if the difference in averaged atomic number Z is only 3. Using this method, quantitative mapping at atomic resolution using HAADF STEM images only has become possible without the need of simultaneously recorded electron energy loss spectra.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Vision lab
Impact Factor: 2.843
Times cited: 166
DOI: 10.1016/j.ultramic.2009.05.010
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“Tuning Size and Seed Position in Small Silver Nanorods”. Sánchez-Iglesias A, Zhuo X, Albrecht W, Bals S, Liz-Marzán LM, ACS materials letters 2, 1246 (2020). http://doi.org/10.1021/acsmaterialslett.0c00388
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Times cited: 9
DOI: 10.1021/acsmaterialslett.0c00388
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“In situ study of the formation mechanism of two-dimensional superlattices from PbSe nanocrystals”. Geuchies JJ, van Overbeek C, Evers WH, Goris B, de Backer A, Gantapara AP, Rabouw FT, Hilhorst J, Peters JL, Konovalov O, Petukhov AV, Dijkstra M, Siebbeles LDA, van Aert S, Bals S, Vanmaekelbergh D, Nature materials 15, 1248 (2016). http://doi.org/10.1038/nmat4746
Abstract: Oriented attachment of PbSe nanocubes can result in the formation of two-dimensional (2D) superstructures with long-range nanoscale and atomic order. This questions the applicability of classic models in which the superlattice grows by first forming a nucleus, followed by sequential irreversible attachment of nanocrystals, as one misaligned attachment would disrupt the 2D order beyond repair. Here, we demonstrate the formation mechanism of 2D PbSe superstructures with square geometry by using in situ grazing-incidence X-ray scattering (small angle and wide angle), ex situ electron microscopy, and Monte Carlo simulations. We observed nanocrystal adsorption at the liquid/gas interface, followed by the formation of a hexagonal nanocrystal monolayer. The hexagonal geometry transforms gradually through a pseudo-hexagonal phase into a phase with square order, driven by attractive interactions between the {100} planes perpendicular to the liquid substrate, which maximize facet-to-facet overlap. The nanocrystals then attach atomically via a necking process, resulting in 2D square superlattices.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 39.737
Times cited: 182
DOI: 10.1038/nmat4746
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“Exploring different inelastic projection mechanisms for electron tomography”. Goris B, Bals S, van den Broek W, Verbeeck J, Van Tendeloo G, Ultramicroscopy 111, 1262 (2011). http://doi.org/10.1016/j.ultramic.2011.02.007
Abstract: Several different projection mechanisms that all make use of inelastically scattered electrons are used for electron tomography. The advantages and the disadvantages of these methods are compared to HAADFSTEM tomography, which is considered as the standard electron tomography technique in materials science. The different inelastic setups used are energy filtered transmission electron microscopy (EFTEM), thickness mapping based on the log-ratio method and bulk plasmon mapping. We present a comparison that can be used to select the best inelastic signal for tomography, depending on different parameters such as the beam stability and nature of the sample. The appropriate signal will obviously also depend on the exact information which is requested.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Vision lab
Impact Factor: 2.843
Times cited: 21
DOI: 10.1016/j.ultramic.2011.02.007
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“Nickel-containing N-doped carbon as effective electrocatalysts for the reduction of CO2 to CO in a continuous-flow electrolyzer”. Daems N, De Mot B, Choukroun D, Van Daele K, Li C, Hubin A, Bals S, Hereijgers J, Breugelmans T, Sustainable energy &, fuels 4, 1296 (2019). http://doi.org/10.1039/C9SE00814D
Abstract: Nickel-containing N-doped carbons were synthesized for the electrochemical reduction of CO2 to CO, which is a promising approach to reduce the atmospheric CO2 levels and its negative impact on the environment. Unfortunately, poor performance (activity, selectivity and/or stability) is still a major hurdle for the economical implementation of this type of materials. The electrocatalysts were prepared through an easily up-scalable and easily tunable method based on the pyrolysis of Ni-containing N-doped carbons. Ni–N–AC–B1 synthesized with a high relative amount of nitrogen and nickel with respect to carbon, was identified as the most promising candidate for this reaction based on its partial CO current density (4.2 mA cm−2), its overpotential (0.57 V) and its faradaic efficiency to CO (>99%). This results in unprecedented values for the current density per g active sites (690 A g−1 active sites). Combined with its decent stability and its high performance in an actual electrolyzer setup, this makes it a promising candidate for the electrochemical reduction of CO2 to CO on a larger scale. Finally, the evaluation of this kind of material in a flow-cell setup has been limited and to the best of our knowledge never included an evaluation of several crucial parameters (e.g. electrolyte type, anode composition and membrane type) and is an essential investigation in the move towards up-scaling and ultimately industrial application of this technique. This study resulted in an optimal cell configuration, consisting of Pt as an anode, Fumatech® as the membrane and 1 M KHCO3 and 2 M KOH as catholyte and anolyte, respectively. In conclusion, this research offers a unique combination of electrocatalyst development and reactor optimization.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Times cited: 14
DOI: 10.1039/C9SE00814D
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“Recent Advances in Transmission Electron Microscopy for Materials Science at the EMAT Lab of the University of Antwerp”. Guzzinati G, Altantzis T, Batuk M, De Backer A, Lumbeeck G, Samaee V, Batuk D, Idrissi H, Hadermann J, Van Aert S, Schryvers D, Verbeeck J, Bals S, Materials 11, 1304 (2018). http://doi.org/10.3390/ma11081304
Abstract: The rapid progress in materials science that enables the design of materials down to the nanoscale also demands characterization techniques able to analyze the materials down to the same scale, such as transmission electron microscopy. As Belgium’s foremost electron microscopy group, among the largest in the world, EMAT is continuously contributing to the development of TEM techniques, such as high-resolution imaging, diffraction, electron tomography, and spectroscopies, with an emphasis on quantification and reproducibility, as well as employing TEM methodology at the highest level to solve real-world materials science problems. The lab’s recent contributions are presented here together with specific case studies in order to highlight the usefulness of TEM to the advancement of materials science.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.654
Times cited: 15
DOI: 10.3390/ma11081304
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“TEM sample preparation by FIB for carbon nanotube interconnects”. Ke X, Bals S, Romo Negreira A, Hantschel T, Bender H, Van Tendeloo G, Ultramicroscopy 109, 1353 (2009). http://doi.org/10.1016/j.ultramic.2009.06.011
Abstract: A powerful method to study carbon nanotubes (CNTs) grown in patterned substrates for potential interconnects applications is transmission electron microscopy (TEM). However, high-quality TEM samples are necessary for such a study. Here, TEM specimen preparation by focused ion beam (FIB) has been used to obtain lamellae of patterned samples containing CNTs grown inside contact holes. A dual-cap Pt protection layer and an extensive 5 kV cleaning procedure are applied in order to preserve the CNTs and avoid deterioration during milling. TEM results show that the inner shell structure of the carbon nanotubes has been preserved, which proves that focused ion beam is a useful technique to prepare TEM samples of CNT interconnects.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.843
Times cited: 21
DOI: 10.1016/j.ultramic.2009.06.011
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“Bifunctional nickel-nitrogen-doped-carbon-supported copper electrocatalyst for CO2 reduction”. Choukroun D, Daems N, Kenis T, Van Everbroeck T, Hereijgers J, Altantzis T, Bals S, Cool P, Breugelmans T, Journal Of Physical Chemistry C 124, 1369 (2020). http://doi.org/10.1021/ACS.JPCC.9B08931
Abstract: Bifunctionality is a key feature of many industrial catalysts, supported metal clusters and particles in particular, and the development of such catalysts for the CO2 reduction reaction (CO2RR) to hydrocarbons and alcohols is gaining traction in light of recent advancements in the field. Carbon-supported Cu nanoparticles are suitable candidates for integration in the state-of-the-art reaction interfaces, and here, we propose, synthesize, and evaluate a bifunctional Ni–N-doped-C-supported Cu electrocatalyst, in which the support possesses active sites for selective CO2 conversion to CO and Cu nanoparticles catalyze either the direct CO2 or CO reduction to hydrocarbons. In this work, we introduce the scientific rationale behind the concept, its applicability, and the challenges with regard to the catalyst. From the practical aspect, the deposition of Cu nanoparticles onto carbon black and Ni–N–C supports via an ammonia-driven deposition precipitation method is reported and explored in more detail using X-ray diffraction, thermogravimetric analysis, and hydrogen temperature-programmed reduction. High-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and energy-dispersive X-ray spectroscopy (EDXS) give further evidence of the presence of Cu-containing nanoparticles on the Ni–N–C supports while revealing an additional relationship between the nanoparticle’s composition and the electrode’s electrocatalytic performance. Compared to the benchmark carbon black-supported Cu catalysts, Ni–N–C-supported Cu delivers up to a 2-fold increase in the partial C2H4 current density at −1.05 VRHE (C1/C2 = 0.67) and a concomitant 10-fold increase of the CO partial current density. The enhanced ethylene production metrics, obtained by virtue of the higher intrinsic activity of the Ni–N–C support, point out toward a synergistic action between the two catalytic functionalities.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Applied Electrochemistry & Catalysis (ELCAT)
Impact Factor: 3.7
Times cited: 24
DOI: 10.1021/ACS.JPCC.9B08931
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“Long-range orientation and atomic attachment of nanocrystals in 2D honeycomb superlattices”. Boneschanscher MP, Evers WH, Geuchies JJ, Altantzis T, Goris B, Rabouw FT, van Rossum SAP, van der Zant HSJ, Siebbeles LDA, Van Tendeloo G, Swart I, Hilhorst J, Petukhov AV, Bals S, Vanmaekelbergh D;, Science 344, 1377 (2014). http://doi.org/10.1126/science.1252642
Abstract: Oriented attachment of synthetic semiconductor nanocrystals is emerging as a route for obtaining new semiconductors that can have Dirac-type electronic bands like graphene, but also strong spin-orbit coupling. The two-dimensional assembly geometry will require both atomic coherence and long-range periodicity of the superlattices. We show how the interfacial self-assembly and oriented attachment of nanocrystals results in two-dimensional (2D) metal chalcogenide semiconductors with a honeycomb superlattice. We present an extensive atomic and nanoscale characterization of these systems using direct imaging and wave scattering methods. The honeycomb superlattices are atomically coherent, and have an octahedral symmetry that is buckled; the nanocrystals occupy two parallel planes. Considerable necking and large-scale atomic motion occurred during the attachment process.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 37.205
Times cited: 304
DOI: 10.1126/science.1252642
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“Polyethylene glycol conjugated polymeric nanocapsules for targeted delivery of quercetin to folate-expressing cancer cells in vitro and in vivo”. El-Gogary RI, Rubio N, Wang JTW, Al-Jamal WT, Bourgognon M, Kafa H, Naeem M, Klippstein R, Abbate V, Leroux F, Bals S, Van Tendeloo G, Kamel AO, Awad GAS, Mortada ND, Al-Jamal KT;, ACS nano 8, 1384 (2014). http://doi.org/10.1021/nn405155b
Abstract: In this work we describe the formulation and characterization of chemically modified polymeric nanocapsules incorporating the anticancer drug, quercetin, for the passive and active targeting to tumors. Folic acid was conjugated to poly(lactide-co-glycolide) (PLGA) polymer to facilitate active targeting to cancer cells. Two different methods for the conjugation of PLGA to folic acid were employed utilizing polyethylene glycol (PEG) as a spacer. Characterization of the conjugates was performed using FTIR and H-1 NMR studies. The PEG and folk acid content was independent of the conjugation methodology employed. PEGylation has shown to reduce the size of the nanocapsule; moreover, zeta-potential was shown to be polymer-type dependent. Comparative studies on the cytotoxicity and cellular uptake of the different formulations by He La cells, in the presence and absence of excess folic acid, were carried out using MTT assay and Confocal Laser Scanning Microscopy, respectively. Both results confirmed the selective uptake and cytotoxicity of the folic acid targeted nanocapsules to the folate enriched cancer cells in a folate-dependent manner. Finally, the passive tumor accumulation and the active targeting of the nanocapsules to folate-expressing cells were confirmed upon intravenous administration in He La or IGROV-1 tumor-bearing mice. The developed nanocapsules provide a system for targeted delivery of a range of hydrophobic anticancer drugs in vivo.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 13.942
Times cited: 144
DOI: 10.1021/nn405155b
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“Seedless synthesis of single crystalline Au nanoparticles with unusual shapes and tunable LSPR in the near-IR”. Angelomé, PC, Heidari Mezerji H, Goris B, Pastoriza-Santos I, Pérez-Juste J, Bals S, Liz-Marzán LM, Chemistry of materials 24, 1393 (2012). http://doi.org/10.1021/cm3004479
Abstract: The plasmonic properties of metal nanoparticles have acquired great importance because of their potential applications in very diverse fields. Metal nanoparticles with localized surface plasmon resonances (LSPR) in the near-infrared (NIR, 7501300 nm) are of particular interest because tissues, blood, and water display low absorption in this spectral range, thus facilitating biomedical applications. Cetyltrimethylammonium chloride (CTAC) was used to induce the seedless formation of highly anisotropic, twisted single crystalline Au nanoparticles in a single step. The LSPR of the obtained particles can be tuned from 600 nm up to 1400 nm by simply changing the reaction temperature or the reagents concentrations. The tunability of the LSPR is closely associated with significant changes in the final particle morphology, which was studied by advanced electron microscopy techniques (3D Tomography and HAADF-STEM). Kinetic experiments were carried out to establish the growth mechanism, suggesting that slow kinetics together with the complexation of the gold salt precursor to CTAC are key factors favoring the formation of these anisotropic particles.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 9.466
Times cited: 42
DOI: 10.1021/cm3004479
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“Halide perovskite-lead chalcohalide nanocrystal heterostructures”. Imran M, Peng L, Pianetti A, Pinchetti V, Ramade J, Zito J, Di Stasio F, Buha J, Toso S, Song J, Infante I, Bals S, Brovelli S, Manna L, Journal Of The American Chemical Society 143, 1435 (2021). http://doi.org/10.1021/JACS.0C10916
Abstract: We report the synthesis of colloidal CsPbX3-Pb4S3Br2 (X = Cl, Br, I) nanocrystal heterostructures, providing an example of a sharp and atomically resolved epitaxial interface between a metal halide perovskite and a non-perovskite lattice. The CsPbBr3-Pb4S3Br2 nanocrystals are prepared by a two-step direct synthesis using preformed subnanometer CsPbBr3 clusters. Density functional theory calculations indicate the creation of a quasi-type II alignment at the heterointerface as well as the formation of localized trap states, promoting ultrafast separation of photogenerated excitons and carrier trapping, as confirmed by spectroscopic experiments. Postsynthesis reaction with either Cl- or I- ions delivers the corresponding CsPbCI3-Pb4S3Br2 and CsPbI3-Pb4S3Br2 heterostructures, thus enabling anion exchange only in the perovskite domain. An increased structural rigidity is conferred to the perovskite lattice when it is interfaced with the chalcohalide lattice. This is attested by the improved stability of the metastable gamma phase (or “black” phase) of CsPbI3 in the CsPbI3-Pb4S3Br2 heterostructure.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 13.858
Times cited: 54
DOI: 10.1021/JACS.0C10916
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“Heterogeneity of silica and glycan-epitope distribution in epidermal idioblast cell walls in Adiantum raddianum laminae”. Van Hoorebeke L, Leroux O, Leroux F, Mastroberti AA, Santos-Silva F, Van Loo D, Bagniewska-Zadworna A, Bals S, Popper ZA, de Araujo Mariath JE, Planta 237, 1453 (2013). http://doi.org/10.1007/s00425-013-1856-6
Abstract: Laminae of Adiantum raddianum Presl., a fern belonging to the family Pteridaceae, are characterised by the presence of epidermal fibre-like cells under the vascular bundles. These cells were thought to contain silica bodies, but their thickened walls leave no space for intracellular silica suggesting it may actually be deposited within their walls. Using advanced electron microscopy in conjunction with energy dispersive X-ray microanalysis we showed the presence of silica in the cell walls of the fibre-like idioblasts. However, it was specifically localised to the outer layers of the periclinal wall facing the leaf surface, with the thick secondary wall being devoid of silica. Immunocytochemical experiments were performed to ascertain the respective localisation of silica deposition and glycan polymers. Epitopes characteristic for pectic homogalacturonan and the hemicelluloses xyloglucan and mannan were detected in most epidermal walls, including the silica-rich cell wall layers. The monoclonal antibody, LM6, raised against pectic arabinan, labelled the silica-rich primary wall of the epidermal fibre-like cells and the guard cell walls, which were also shown to contain silica. We hypothesise that the silicified outer wall layers of the epidermal fibre-like cells support the lamina during cell expansion prior to secondary wall formation. This implies that silicification does not impede cell elongation. Although our results suggest that pectic arabinan may be implicated in silica deposition, further detailed analyses are needed to confirm this. The combinatorial approach presented here, which allows correlative screening and in situ localisation of silicon and cell wall polysaccharide distribution, shows great potential for future studies.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.361
Times cited: 16
DOI: 10.1007/s00425-013-1856-6
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“Micelle-directed chiral seeded growth on anisotropic gold nanocrystals”. González-Rubio G, Mosquera J, Kumar V, Pedrazo-Tardajos A, Llombart P, Solís DM, Lobato I, Noya EG, Guerrero-Martínez A, Taboada JM, Obelleiro F, MacDowell LG, Bals S, Liz-Marzán LM, Science 368, 1472 (2020). http://doi.org/10.1126/science.aba0980
Abstract: Surfactant-assisted seeded growth of metal nanoparticles (NPs) can be engineered to produce anisotropic gold nanocrystals with high chiroptical activity through the templating effect of chiral micelles formed in the presence of dissymmetric cosurfactants. Mixed micelles adsorb on gold nanorods, forming quasihelical patterns that direct seeded growth into NPs with pronounced morphological and optical handedness. Sharp chiral wrinkles lead to chiral plasmon modes with high dissymmetry factors (~0.20). Through variation of the dimensions of chiral wrinkles, the chiroptical properties can be tuned within the visible and near-infrared electromagnetic spectrum. The micelle-directed mechanism allows extension to other systems, such as the seeded growth of chiral platinum shells on gold nanorods. This approach provides a reproducible, simple, and scalable method toward the fabrication of NPs with high chiral optical activity.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 56.9
Times cited: 187
DOI: 10.1126/science.aba0980
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“Collective Plasmonic Properties in Few-Layer Gold Nanorod Supercrystals”. Hamon C, Novikov SM, Scarabelli L, Solís DM, Altantzis T, Bals S, Taboada JM, Obelleiro F, Liz-Marzán LM, ACS Photonics 2, 1482 (2015). http://doi.org/10.1021/acsphotonics.5b00369
Abstract: Gold nanorod supercrystals have been widely employed for the detection of relevant bioanalytes with detection limits ranging from nano- to picomolar levels,
confirming the promising nature of these structures for biosensing. Even though a relationship between the height of the supercrystal (i.e., the number of stacked nanorod layers)and the enhancement factor has been proposed, no systematic
study has been reported. In order to tackle this problem, we prepared gold nanorod supercrystals with varying numbers of stacked layers and analyzed them extensively by atomic force microscopy, electron microscopy and surface enhanced Raman scattering. The experimental results were compared to numerical
simulations performed on real-size supercrystals composed of thousands of nanorod building blocks. Analysis of the hot spot distribution in the simulated supercrystals showed the presence of standing waves that were distributed at different depths, depending on the number of layers in each supercrystal. On the basis of these theoretical results, we interpreted the experimental
data in terms of analyte penetration into the topmost layer only, which indicates that diffusion to the interior of the supercrystals would be crucial if the complete field enhancement produced by the stacked nanorods is to be exploited. We propose that our conclusions will be of high relevance in the design of next generation plasmonic devices.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 6.756
Times cited: 70
DOI: 10.1021/acsphotonics.5b00369
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“Two-Dimensional CdSe-PbSe Heterostructures and PbSe Nanoplatelets: Formation, Atomic Structure, and Optical Properties”. Salzmann BBV, Wit J de, Li C, Arenas-Esteban D, Bals S, Meijerink A, Vanmaekelbergh D, The journal of physical chemistry: C : nanomaterials and interfaces 126, 1513 (2022). http://doi.org/10.1021/acs.jpcc.1c09412
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 3.7
Times cited: 12
DOI: 10.1021/acs.jpcc.1c09412
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“The influence of branched alkyl side chains in A-D-A oligothiophenes on the photovoltaic performance and morphology of solution-processed bulk-heterojunction solar cells”. Ata I, Ben Dkhil S, Pfannmoeller M, Bals S, Duche D, Simon J-J, Koganezawa T, Yoshimoto N, Videlot-Ackermann C, Margeat O, Ackermann J, Baeuerle P, Organic chemistry frontiers : an international journal of organic chemistry 4, 1561 (2017). http://doi.org/10.1039/C7QO00222J
Abstract: Besides providing sufficient solubility, branched alkyl chains also affect the film-forming and packing properties of organic semiconductors. In order to avoid steric hindrance as it is present in wide-spread alkyl chains comprising a branching point position at the C2-position, i.e., 2-ethylhexyl, the branching point can be moved away from the pi-conjugated backbone. In this report, we study the influence of the modification of the branching point position from the C2-position in 2-hexyldecylamine (1) to the C4-position in 4-hexyldecylamine (2) connected to the central dithieno[3,2-b: 2', 3'-d] pyrrole (DTP) moiety in a well-studied A-D-A oligothiophene on the optoelectronic properties and photovoltaic performance in solution- processed bulk heterojunction solar cells (BHJSCs) with [6,6]-phenyl-C71-butyric acid methyl ester (PC71BM) as the acceptor material. Post-treatment of the photoactive layers is performed via solvent vapor annealing (SVA) in order to improve the film microstructure of the bulk heterojunction. The time evolution of nanoscale morphological changes is followed by combining scanning transmission electron microscopy with low-energy-loss spectroscopic imaging (STEM-SI), solid-state absorption spectroscopy, and two-dimensional grazing incidence X-ray diffraction (2D-GIXRD). Our results show an improvement of the photovoltaic performance that is dependent on the branching point position in the donor oligomer. Optical spacers are utilized to increase light absorption inside the co-oligomer 2-based BHJSCs leading to increased power conversion efficiencies (PCEs) of 8.2% when compared to the corresponding co-oligomer 1-based devices. A STEM-SI analysis of the respective device cross-sections of active layers containing 1 and 2 as donor materials indeed reveals significant differences in their respective active layer morphologies.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.955
Times cited: 24
DOI: 10.1039/C7QO00222J
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“Comparison of As- and P-based metamorphic buffers for high performance InP heterojunction bipolar transistor and high electron mobility transistor applications”. Lubyshev D, Fastenau JM, Fang X-M, Wu Y, Doss C, Snyder A, Liu WK, Lamb MSM, Bals S, Song C, Journal of vacuum science &, technology. B. Microelectronics and nanometer structures. Processing, measurement and phenomena 22, 1565 (2004). http://doi.org/10.1116/1.1691412
Abstract: Metamorphic buffers (M-buffers) consisting of graded InAlAs or bulk InP were employed for the production of InP-based epiwafers on GaAs substrates by molecular-beam epitaxy. The graded InAlAs is the standard for production metamorphic high electron mobility transistors (M-HEMTs), while the bulk InP offers superior thermal properties for higher current density circuits. The surface morphology and crystal structure of the two M-buffers showed different relaxation mechanisms. The graded InAlAs gave a cross-hatched pattern with nearly full relaxation and very effective dislocation filtering, while the bulk InP had a uniform isotropic surface with dislocations propagating further up towards the active layers. Both types of M-buffers had atomic force microscopy root-mean-square roughness values around 2030 Å. The Hall transport properties of high electron mobility transistors (HEMTs) grown on the InAlAs M-buffer, and a baseline HEMT grown lattice matched on InP, both had room-temperature mobilities >10 000 cm2/V s, while the M-HEMT on the InP M-buffer showed a decrease to 9000 cm2/V s. Similarly, the dc parameters of a double heterojunction bipolar transistor (DHBT) grown on the InAlAs M-buffer were much closer to the baseline heterojunction bipolar transistor than a DHBT grown on the InP M-buffer. A high breakdown voltage of 11.3 V was achieved on an M-DHBT with the InAlAs M-buffer. We speculate that the degradation in device characteristics on the InP M-buffer was related to the incomplete dislocation filtering.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Times cited: 25
DOI: 10.1116/1.1691412
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“Gallium oxide nanorods : novel, template-free synthesis and high catalytic activity in epoxidation reactions”. Lueangchaichaweng W, Brooks NR, Fiorilli S, Gobechiya E, Lin K, Li L, Parres-Esclapez S, Javon E, Bals S, Van Tendeloo G, Martens JA, Kirschhock CEA, Jacobs PA, Pescarmona PP;, Angewandte Chemie: international edition in English 53, 1585 (2014). http://doi.org/10.1002/anie.201308384
Abstract: Gallium oxide nanorods with unprecedented small dimensions (20-80nm length and 3-5nm width) were prepared using a novel, template-free synthesis method. This nanomaterial is an excellent heterogeneous catalyst for the sustainable epoxidation of alkenes with H2O2, rivaling the industrial benchmark microporous titanosilicate TS-1 with linear alkenes and being much superior with bulkier substrates. A thorough characterization study elucidated the correlation between the physicochemical properties of the gallium oxide nanorods and their catalytic performance, and underlined the importance of the nanorod morphology for generating a material with high specific surface area and a high number of accessible acid sites.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 11.994
Times cited: 61
DOI: 10.1002/anie.201308384
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“Interfaceless exchange bias in CoFe₂O₄, nanocrystals”. Rivas-Murias B, Testa-Anta M, Skorikov AS, Comesana-Hermo M, Bals S, Salgueirino V, Nano letters 23, 1688 (2023). http://doi.org/10.1021/ACS.NANOLETT.2C04268
Abstract: Oxidized cobalt ferrite nanocrystals with a modified distribution of the magnetic cations in their spinel structure give place to an unusual exchange-coupled system with a double reversal of the magnetization, exchange bias, and increased coercivity, but without the presence of a clear physical interface that delimits two well-differentiated magnetic phases. More specifically, the partial oxidation of cobalt cations and the formation of Fe vacancies at the surface region entail the formation of a cobalt-rich mixed ferrite spinel, which is strongly pinned by the ferrimagnetic background from the cobalt ferrite lattice. This particular configuration of exchange-biased magnetic behavior, involving two different magnetic phases but without the occurrence of a crystallographically coherent interface, revolu-tionizes the established concept of exchange bias phenomenology.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 10.8
Times cited: 4
DOI: 10.1021/ACS.NANOLETT.2C04268
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“Small-angle X-ray scattering and light scattering study of hybrid nanoparticles composed of thermoresponsive triblock copolymer F127 and thermoresponsive statistical polyoxazolines with hydrophobic moieties”. Bogomolova A, Hruby M, Panek J, Rabyk M, Turner S, Bals S, Steinhart M, Zhigunov A, Sedlacek O, Stepanek P, Filippov SK;, Journal of applied crystallography 46, 1690 (2013). http://doi.org/10.1107/S0021889813027064
Abstract: A combination of new thermoresponsive statistical polyoxazolines, poly[(2-butyl-2-oxazoline)-stat-(2-isopropyl-2-oxazoline)] [pBuOx-co-piPrOx], with different hydrophobic moieties and F127 surfactant as a template system for the creation of thermosensitive nanoparticles for radionuclide delivery has recently been tested [Pánek, Filippov, Hrubý, Rabyk, Bogomolova, Kučka Stěpánek (2012). Macromol. Rapid Commun.33, 16831689]. It was shown that the presence of the thermosensitive F127 triblock copolymer in solution reduces nanoparticle size and polydispersity. This article focuses on a determination of the internal structure and solution properties of the nanoparticles in the temperature range from 288 to 312 K. Here, it is demonstrated that below the cloud point temperature (CPT) the polyoxazolines and F127 form complexes that co-exist in solution with single F127 molecules and large aggregates. When the temperature is raised above the CPT, nanoparticles composed of polyoxazolines and F127 are predominant in solution. These nanoparticles could be described by a spherical shell model. It was found that the molar weight and hydrophobicity of the polymer do not influence the size of the outer radius and only slightly change the inner radius of the nanoparticles. At the same time, molar weight and hydrophobicity did affect the process of nanoparticle formation. In conclusion, poly(2-oxazoline) molecules are fully incorporated inside of F127 micelles, and this result is very promising for the successful application of such systems in radionuclide delivery.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Times cited: 18
DOI: 10.1107/S0021889813027064
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“Electrodeposition of Ag nanoparticles onto carbon coated TEM grids : a direct approach to study early stages of nucleation”. Ustarroz J, Gupta U, Hubin A, Bals S, Terryn H, Electrochemistry communications 12, 1706 (2010). http://doi.org/10.1016/j.elecom.2010.10.002
Abstract: An innovative experimental approach to study the electrodeposition of small nanoparticles and the early stages of electrochemical nucleation and growth is presented. Carbon coated gold TEM grids are used as substrates for the electrodeposition of silver nanoparticles so that electrochemical data, FESEM, HAADFSTEM and HRTEM data can be acquired from the same sample without the need to remove the particles from the substrate. It is shown that the real distribution of nanoparticles cannot be resolved by FESEM whereas HAADFSTEM analysis confirms that a distribution of small nanoparticles (d ≈ 12 nm) coexist with large nanoparticles corresponding to a bimodal size distribution. Besides, particles grown under the same conditions have been found to present different structures such as monocrystals, polycrystals or aggregates of smaller particles.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.396
Times cited: 52
DOI: 10.1016/j.elecom.2010.10.002
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“Epitaxially grown silicon-based single-atom catalyst for visible-light-driven syngas production”. Chen H, Xiong Y, Li J, Abed J, Wang D, Pedrazo-Tardajos A, Cao Y, Zhang Y, Wang Y, Shakouri M, Xiao Q, Hu Y, Bals S, Sargent EHH, Su C-Y, Yang Z, Nature communications 14, 1719 (2023). http://doi.org/10.1038/S41467-023-37401-3
Abstract: Despite the natural abundance and promising properties of Si, there are few examples of crystalline Si-based catalysts. Here, the authors report an epitaxial growth method to construct Co single atoms on Si for light driven CO2 reduction to syngas. Improving the dispersion of active sites simultaneous with the efficient harvest of photons is a key priority for photocatalysis. Crystalline silicon is abundant on Earth and has a suitable bandgap. However, silicon-based photocatalysts combined with metal elements has proved challenging due to silicon's rigid crystal structure and high formation energy. Here we report a solid-state chemistry that produces crystalline silicon with well-dispersed Co atoms. Isolated Co sites in silicon are obtained through the in-situ formation of CoSi2 intermediate nanodomains that function as seeds, leading to the production of Co-incorporating silicon nanocrystals at the CoSi2/Si epitaxial interface. As a result, cobalt-on-silicon single-atom catalysts achieve an external quantum efficiency of 10% for CO2-to-syngas conversion, with CO and H-2 yields of 4.7 mol g((Co))(-1) and 4.4 mol g((Co))(-1), respectively. Moreover, the H-2/CO ratio is tunable between 0.8 and 2. This photocatalyst also achieves a corresponding turnover number of 2 x 10(4) for visible-light-driven CO2 reduction over 6 h, which is over ten times higher than previously reported single-atom photocatalysts.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 16.6
Times cited: 6
DOI: 10.1038/S41467-023-37401-3
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“Glycogen as a biodegradable construction nanomaterial for in vivo use”. Filippov SK, Sedlacek O, Bogomolova A, Vetrik M, Jirak D, Kovar J, Kucka J, Bals S, Turner S, Stepanek P, Hruby M;, Macromolecular bioscience 12, 1731 (2012). http://doi.org/10.1002/mabi.201200294
Abstract: It is demonstrated that glycogen as a biodegradable and inexpensive material coming from renewable resources can be used as a carrier for the construction of in vivo imaging nanoagents. The model system considered is composed of glycogen modified with gadolinium and fluorescent labels. Systematic studies of properties of these nanocarriers by a variety of physical methods and results of in vivo tests of biodegradability are reported. This represents, to the authors' best knowledge, the first such use of glycogen.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.238
Times cited: 22
DOI: 10.1002/mabi.201200294
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“Three-dimensional atomic structure of supported Au nanoparticles at high temperature”. Liu P, Arslan Irmak E, De Backer A, De wael A, Lobato I, Béché, A, Van Aert S, Bals S, Nanoscale 13 (2021). http://doi.org/10.1039/D0NR08664A
Abstract: Au nanoparticles (NPs) deposited on CeO2 are extensively used as thermal catalysts since the morphology of the NPs is expected to be stable at elevated temperatures. Although it is well known that the activity of Au NPs depends on their size and surface structure, their three-dimensional (3D) structure at the atomic scale has not been completely characterized as a function of temperature. In this paper, we overcome the limitations of conventional electron tomography by combining atom counting applied to aberration-corrected scanning transmission electron microscopy images and molecular dynamics relaxation. In this manner, we are able to perform an atomic resolution 3D investigation of supported Au NPs. Our results enable us to characterize the 3D equilibrium structure of single NPs as a function of temperature. Moreover, the dynamic 3D structural evolution of the NPs at high temperatures, including surface layer jumping and crystalline transformations, has been studied.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 7.367
Times cited: 13
DOI: 10.1039/D0NR08664A
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