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“Self-assembled ligand-capped plasmonic Au nanoparticle films in the Kretschmann configuration for sensing of volatile organic compounds”. Borah R, Smets J, Ninakanti R, Tietze ML, Ameloot R, Chigrin DN, Bals S, Lenaerts S, Verbruggen SW, ACS applied nano materials 5, acsanm.2c02524 (2022). http://doi.org/10.1021/ACSANM.2C02524
Abstract: Films of close-packed Au nanoparticles are coupled electrodynamically through their collective plasmon resonances. This collective optical response results in enhanced light–matter interactions, which can be exploited in various applications. Here, we demonstrate their application in sensing volatile organic compounds, using methanol as a test case. Ordered films over several cm2 were obtained by interfacial self-assembly of colloidal Au nanoparticles (∼10 nm diameter) through controlled evaporation of the solvent. Even though isolated nanoparticles of this size are inherently nonscattering, when arranged in a close-packed film the plasmonic coupling results in a strong reflectance and absorbance. The in situ tracking of vapor phase methanol concentration through UV–vis transmission measurements of the nanoparticle film is first demonstrated. Next, in situ ellipsometry of the self-assembled films in the Kretschmann (also known as ATR) configuration is shown to yield enhanced sensitivity, especially with phase difference measurements, Δ. Our study shows the excellent agreement between theoretical models of the spectral response of self-assembled films with experimental in situ sensing experiments. At the same time, the theoretical framework provides the basis for the interpretation of the various observed experimental trends. Combining periodic nanoparticle films with ellipsometry in the Kretschmann configuration is a promising strategy toward highly sensitive and selective plasmonic thin-film devices based on colloidal fabrication methods for volatile organic compound (VOC) sensing applications.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 5.9
Times cited: 11
DOI: 10.1021/ACSANM.2C02524
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“Use of nanoscale carbon layers on Ag-based gas diffusion electrodes to promote CO production”. Pacquets L, Van den Hoek J, Arenas Esteban D, Ciocarlan R-G, Cool P, Baert K, Hauffman T, Daems N, Bals S, Breugelmans T, ACS applied nano materials 5, 7723 (2022). http://doi.org/10.1021/ACSANM.2C00473
Abstract: A promising strategy for the inhibition of the hydrogen evolution reaction along with the stabilization of the electrocatalyst in electrochemical CO2 reduction cells involves the application of a nanoscale amorphous carbon layer on top of the active catalyst layer in a gas diffusion electrode. Without modifying the chemical nature of the electrocatalyst itself, these amorphous carbon layers lead to the stabilization of the electrocatalyst, and a significant improvement with respect to the inhibition of the hydrogen evolution reaction was also obtained. The faradaic efficiencies of hydrogen could be reduced from 31.4 to 2.1% after 1 h of electrolysis with a 5 nm thick carbon layer. Furthermore, the impact of the carbon layer thickness (5–30 nm) on this inhibiting effect was investigated. We determined an optimal thickness of 15 nm where the hydrogen evolution reaction was inhibited and a decent stability was obtained. Next, a thickness of 15 nm was selected for durability measurements. Interestingly, these durability measurements revealed the beneficial impact of the carbon layer already after 6 h by suppressing the hydrogen evolution such that an increase of only 37.9% exists compared to 56.9% without the use of an additional carbon layer, which is an improvement of 150%. Since carbon is only applied afterward, it reveals its great potential in terms of electrocatalysis in general.
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: 5.9
Times cited: 3
DOI: 10.1021/ACSANM.2C00473
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“Possible Synergies of Nanomaterial-Assisted Tissue Regeneration in Plasma Medicine: Mechanisms and Safety Concerns”. Shaw P, Vanraes P, Kumar N, Bogaerts A, Nanomaterials 12, 3397 (2022). http://doi.org/10.3390/nano12193397
Abstract: Cold atmospheric plasma and nanomedicine originally emerged as individual domains, but are increasingly applied in combination with each other. Most research is performed in the context of cancer treatment, with only little focus yet on the possible synergies. Many questions remain on the potential of this promising hybrid technology, particularly regarding regenerative medicine and tissue engineering. In this perspective article, we therefore start from the fundamental mechanisms in the individual technologies, in order to envision possible synergies for wound healing and tissue recovery, as well as research strategies to discover and optimize them. Among these strategies, we demonstrate how cold plasmas and nanomaterials can enhance each other’s strengths and overcome each other’s limitations. The parallels with cancer research, biotechnology and plasma surface modification further serve as inspiration for the envisioned synergies in tissue regeneration. The discovery and optimization of synergies may also be realized based on a profound understanding of the underlying redox- and field-related biological processes. Finally, we emphasize the toxicity concerns in plasma and nanomedicine, which may be partly remediated by their combination, but also partly amplified. A widespread use of standardized protocols and materials is therefore strongly recommended, to ensure both a fast and safe clinical implementation.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 5.3
DOI: 10.3390/nano12193397
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“Experimental reconstructions of 3D atomic structures from electron microscopy images using a Bayesian genetic algorithm”. De Backer A, Van Aert S, Faes C, Arslan Irmak E, Nellist PD, Jones L, N P J Computational Materials 8, 216 (2022). http://doi.org/10.1038/s41524-022-00900-w
Abstract: We introduce a Bayesian genetic algorithm for reconstructing atomic models of monotype crystalline nanoparticles from a single projection using Z-contrast imaging. The number of atoms in a projected atomic column obtained from annular dark field scanning transmission electron microscopy images serves as an input for the initial three-dimensional model. The algorithm minimizes the energy of the structure while utilizing a priori information about the finite precision of the atom-counting results and neighbor-mass relations. The results show promising prospects for obtaining reliable reconstructions of beam-sensitive nanoparticles during dynamical processes from images acquired with sufficiently low incident electron doses.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
DOI: 10.1038/s41524-022-00900-w
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“Chiral Seeded Growth of Gold Nanorods Into 4‐Fold Twisted Nanoparticles with Plasmonic Optical Activity”. Ni B, Mychinko M, Gómez‐Graña S, Morales‐Vidal J, Obelleiro‐Liz M, Heyvaert W, Vila‐Liarte D, Zhuo X, Albrecht W, Zheng G, González‐Rubio G, Taboada JM, Obelleiro F, López N, Pérez‐Juste J, Pastoriza‐Santos I, Cölfen H, Bals S, Liz‐Marzán LM, Advanced materials , 2208299 (2022). http://doi.org/10.1002/adma.202208299
Abstract: A robust and reproducible methodology to prepare stable inorganic nanoparticles with chiral morphology might hold the key to the practical utilization of these materials. We describe herein an optimized chiral growth method to prepare 4-fold twisted gold nanorods, where the amino acid cysteine is used as a dissymmetry inducer. Four tilted ridges were found to develop on the surface of single-crystal nanorods upon repeated reduction of HAuCl4, in the presence of cysteine as the chiral inducer and ascorbic acid as a reducing agent. From detailed electron microscopy analysis of the crystallographic structures, we propose that dissymmetry results from the development of chiral facets in the form of protrusions (tilted ridges) on the initial nanorods, eventually leading to a twisted shape. The role of cysteine is attributed to assisting enantioselective facet evolution, which is supported by density functional theory simulations of the surface energies, modified upon adsorption of the chiral molecule. The development of R-type and S-type chiral structures (small facets, terraces, or kinks) would thus be non-equal, removing the mirror symmetry of the Au NR and in turn resulting in a markedly chiral morphology with high plasmonic optical activity.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 29.4
Times cited: 35
DOI: 10.1002/adma.202208299
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“Arresting aqueous swelling of layered graphene-oxide membranes with H3O+ and OH- ions”. Gogoi A, Neyts EC, Milošević, MV, Peeters FM, ACS applied materials and interfaces 14, 34946 (2022). http://doi.org/10.1021/ACSAMI.2C05926
Abstract: Over the past decade, graphene oxide (GO) has emerged as a promising membrane material with superior separation performance and intriguing mechanical/chemical stability. However, its practical implementation remains very challenging primarily because of its undesirable swelling in an aqueous environment. Here, we demonstrated that dissociation of water molecules into H3O+ and OH- ions inside the interlayer gallery of a layered GO membrane can strongly affect its stability and performance. We reveal that H3O+ and OH- ions form clusters inside the GO laminates that impede the permeance of water and salt ions through the membrane. Dynamics of those clusters is sensitive to an external ac electric field, which can be used to tailor the membrane performance. The presence of H3O+ and OH- ions also leads to increased stability of the hydrogen bond (H-bond) network among the water molecules and the GO layers, which further reduces water permeance through the membrane, while crucially imparting stability to the layered GO membrane against undesirable swelling. KEYWORDS: layered graphene-oxide membrane, aqueous stability, H3O+ and OH- ions, external electric field, molecular dynamics
Keywords: A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 9.5
Times cited: 9
DOI: 10.1021/ACSAMI.2C05926
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“Assessing the potential of application of titanium dioxide for photocatalytic degradation of deposited soot on asphalt pavement surfaces”. Omranian SR, Geluykens M, Van Hal M, Hasheminejad N, Rocha Segundo I, Pipintakos G, Denys S, Tytgat T, Fraga Freitas E, Carneiro J, Verbruggen S, Vuye C, Construction and building materials 350, 128859 (2022). http://doi.org/10.1016/J.CONBUILDMAT.2022.128859
Abstract: It is known that pollutants and their irreparable influence can considerably jeopardize the environment and human health. Such disastrous, growing, hazardous particles urged researchers to find effective ways and diminish their destructive impacts and preserve our planet. This study evaluates the potential of incorporating Titanium Dioxide (TiO2) semiconductor nanoparticles on asphalt pavements to degrade pollutants without compromising bitumen performance. Accordingly, the Response Surface Method (RSM) was employed to develop an experimental matrix based on the central composite design. Image Analysis (IA) was used to determine the rate of soot degradation (as pollutant representative) using MATLAB and ImageJ software. Confocal Laser Scanning Microscopy (CLSM), Fourier Transform Infrared spectroscopy (FTIR), and Dynamic Shear Rheometer (DSR) were finally carried out to estimate the effects of adding different percentages of TiO2 on the micro -structural features and dispersion of the TiO2, chemical fingerprinting, and rheological performance of the bituminous binder. The results showed a promising potential of TiO2 to degrade soot (over 50%) during the conducted experiments. In addition, the RSM outcomes showed that applying a higher amount of TiO2 is more efficient for pollutant degradation. Finally, no negative impact was observed, neither on the rheological behavior nor on the aging susceptibility of the bitumen, even though the homogenous dispersion of the TiO2 was clearly captured via CLSM.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 7.4
DOI: 10.1016/J.CONBUILDMAT.2022.128859
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“Axion insulator states in a topological insulator proximitized to magnetic insulators : a tight-binding characterization”. Shafiei M, Fazileh F, Peeters FM, Milošević, MV, Physical review materials 6, 074205 (2022). http://doi.org/10.1103/PHYSREVMATERIALS.6.074205
Abstract: The recent discovery of axion states in materials such as antiferromagnetic topological insulators has boosted investigations of the magnetoelectric response in topological insulators and their promise towards realizing dissipationless topological electronics. In this paper, we develop a tight-binding methodology to explore the emergence of axion states in Bi2Se3 in proximity to magnetic insulators on the top and bottom surfaces. The topological protection of the surface states is lifted by a time-reversal-breaking perturbation due to the proximity of a magnetic insulator, and a gap is opened on the surfaces, giving rise to half-quantized Hall conductance and a zero Hall plateau-evidencing an axion insulator state. We developed a real-space tight-binding Hamiltonian for Bi2Se3 using first-principles data. Transport properties of the system were obtained within the Landauer-Buttiker formalism, and we discuss the creation of axion states through Hall conductance and a zero Hall plateau at the surfaces, as a function of proximitized magnetization and corresponding potentials at the surfaces, as well as the thickness of the topological insulator.
Keywords: A1 Journal article; Condensed Matter Theory (CMT)
Impact Factor: 3.4
Times cited: 4
DOI: 10.1103/PHYSREVMATERIALS.6.074205
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“Characterization of IASCC crack tips extracted from neutron-irradiated flux thimble tube specimens in view of a probabilistic fracture model”. Penders AG, Konstantinović, MJ, Van Renterghem W, Bosch R-W, Schryvers D, Somville F, Journal of nuclear materials 571, 154015 (2022). http://doi.org/10.1016/J.JNUCMAT.2022.154015
Abstract: This study reports the properties of irradiation assisted stress corrosion crack tips extracted by means of focused-ion beam from 60 to 80 dpa neutron-irradiated O-ring specimens tested under straining conditions under a pressurized-water reactor environment. Various crack tip morphologies and surrounding deformation features were analyzed as a function of applied stress, surface oxidation state and loading form – constant versus cyclic. All investigated cracks exhibit grain boundary oxidation in front of the crack tip, with the extent of oxidation being proportional to applied stress. These findings clearly demonstrate that, under the subcritical crack propagation regime, the grain boundary oxide grows faster than the crack. On the other hand, crack tips appertaining to specimens with removed oxide layer at the outer surface show comparatively less oxidation at the crack tip, which could indicate towards crack initiation from regions that exemplify lower stress, such as the O-ring inner surface. Cyclic loading is found to have a more pronounced effect on the crack tip microstructure, demonstrating increased deformation twinning and -martensitic transformation, which signifies towards an increased susceptibility to intergranular failure. Still, the extent of crack tip grain boundary oxidation in this case agrees well with expected values for maximum stress applied during cyclic loading. All results are interpreted based on the probabilistic subcritical crack propagation mechanism and provide strong support to a stress-driven internal oxidation model.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 3.1
DOI: 10.1016/J.JNUCMAT.2022.154015
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“Self-assembled epitaxial cathode-electrolyte nanocomposites for 3D microbatteries”. Cunha DM, Gauquelin N, Xia R, Verbeeck J, Huijben M, ACS applied materials and interfaces 14, 42208 (2022). http://doi.org/10.1021/ACSAMI.2C09474
Abstract: The downscaling of electronic devices requires rechargeable microbatteries with enhanced energy and power densities. Here, we evaluate self-assembled vertically aligned nano-composite (VAN) thin films as a platform to create high-performance three-dimensional (3D) microelectrodes. This study focuses on controlling the VAN formation to enable interface engineering between the LiMn2O4 cathode and the (Li,La)TiO3 solid electrolyte. Electrochemical analysis in a half cell against lithium metal showed the absence of sharp redox peaks due to the confinement in the electrode pillars at the nanoscale. The (100)-oriented VAN thin films showed better rate capability and stability during extensive cycling due to the better alignment to the Li-diffusion channels. However, an enhanced pseudocapacitive contribution was observed for the increased total surface area within the (110)-oriented VAN thin films. These results demonstrate for the first time the electrochemical behavior of cathode-electrolyte VANs for lithium-ion 3D microbatteries while pointing out the importance of control over the vertical interfaces.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 9.5
Times cited: 4
DOI: 10.1021/ACSAMI.2C09474
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“Topotactic redox cycling in SrFeO2.5+&delta, explored by 3D electron diffraction in different gas atmospheres”. Batuk M, Vandemeulebroucke D, Ceretti M, Paulus W, Hadermann J, Journal of materials chemistry A : materials for energy and sustainability (2022). http://doi.org/10.1039/D2TA03247C
Abstract: For oxygen conducting materials applied in solid oxide fuel cells and chemical-looping processes, the understanding of the oxygen diffusion mechanism and the materials’ crystal structure at different stages of the redox reactions is a key parameter to control their performance. In this paper we report the first ever in situ 3D ED experiment in a gas environment and with it uncover the structure evolution of SrFeO2.5 as notably different from that reported from in situ X-ray and in situ neutron powder diffraction studies in gas environments. Using in situ 3D ED on submicron sized single crystals obtained from a high quality monodomain SrFeO2.5 single crystal , we observe the transformation under O2 flow of SrFeO2.5 with an intra- and interlayer ordering of the left and right twisted (FeO4) tetrahedral chains (space group Pcmb) into consecutively SrFeO2.75 with space group Cmmm (at 350°C, 33% O2) and SrFeO3-δ with space group Pm3 ̅m (at 400°C, 100% O2). Upon reduction in H2 flow, the crystals return to the brownmillerite structure with intralayer order, but without regaining the interlayer order of the pristine crystals. Therefore, redox cycling of SrFeO2.5 crystals in O2 and H2 introduces stacking faults into the structure, resulting in an I2/m(0βγ)0s symmetry with variable β.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 11.9
DOI: 10.1039/D2TA03247C
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“Bioactive Nonthermal Biocompatible Plasma Enhances Migration on Human Gingival Fibroblasts”. Han I, Song IS, Choi SA, Lee T, Yusupov M, Shaw P, Bogaerts A, Choi EH, Ryu JJ, Advanced healthcare materials 12, 2200527 (2023). http://doi.org/10.1002/adhm.202200527
Abstract: This study hypothesizes that the application of low-dose nonthermal biocompatible dielectric barrier discharge plasma (DBD-NBP) to human gingival fibroblasts (HGFs) will inhibit colony formation but not cell death and induce matrix metalloproteinase (MMP) expression, extracellular matrix (ECM) degradation, and subsequent cell migration, which can result in enhanced wound healing. HGFs treated with plasma for 3 min migrate to each other across the gap faster than those in the control and 5-min treatment groups on days 1 and 3. The plasma-treated HGFs show significantly high expression levels of the cell cycle arrest-related p21 gene and enhanced MMP activity. Focal adhesion kinase (FAK) mediated attenuation of wound healing or actin cytoskeleton rearrangement, and plasma-mediated reversal of this attenuation support the migratory effect of DBD-NBP. Further, this work performs computer simulations to investigate the effect of oxidation on the stability and conformation of the catalytic kinase domain (KD) of FAK. It is found that the oxidation of highly reactive amino acids (AAs) Cys427, Met442, Cys559, Met571, Met617, and Met643 changes the conformation and increases the structural flexibility of the FAK protein and thus modulates its function and activity. Low-dose DBD-NBP-induces host cell cycle arrest, ECM breakdown, and subsequent migration, thus contributing to the enhanced wound healing process.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 10
DOI: 10.1002/adhm.202200527
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“Study of the Mechanism and Increasing Crystallinity in the Self-Templated Growth of Ultrathin PbS Nanosheets”. van der Sluijs MM, Salzmann BBV, Arenas Esteban D, Li C, Jannis D, Brafine LC, Laning TD, Reinders JWC, Hijmans NSA, Moes JR, Verbeeck J, Bals S, Vanmaekelbergh D, Chemistry of materials (2023). http://doi.org/10.1021/acs.chemmater.3c00300
Abstract: Colloidal 2D semiconductor nanocrystals, the analogue of solid-state quantum wells, have attracted strong interest in material science and physics. Molar quantities of suspended quantum objects with spectrally pure absorption and emission can be synthesized. For the visible region, CdSe nanoplatelets with atomically precise thickness and tailorable emission have been (almost) perfected. For the near-infrared region, PbS nanosheets (NSs) hold strong promise, but the photoluminescence quantum yield is low and many questions on the crystallinity, atomic structure, intriguing rectangular shape, and formation mechanism remain to be answered. Here, we report on a detailed investigation of the PbS NSs prepared with a lead thiocyanate single source precursor. Atomically resolved HAADF-STEM imaging reveals the presence of defects and small cubic domains in the deformed orthorhombic PbS crystal lattice. Moreover, variations in thickness are observed in the NSs, but only in steps of 2 PbS monolayers. To study the reaction mechanism, a synthesis at a lower temperature allowed for the study of reaction intermediates. Specifically, we studied the evolution of pseudo-crystalline templates towards mature, crystalline PbS NSs. We propose a self-induced templating mechanism based on an oleylamine-lead-thiocyanate (OLAM-Pb-SCN) complex with two Pb-SCN units as a building block; the interactions between the long-chain ligands regulate the crystal structure and possibly the lateral dimensions.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 8.6
Times cited: 2
DOI: 10.1021/acs.chemmater.3c00300
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“Hybrid core–shell nanoparticles for cell-specific magnetic separation and photothermal heating”. de la Encarnación C, Jungwirth F, Vila-Liarte D, Renero-Lecuna C, Kavak S, Orue I, Wilhelm C, Bals S, Henriksen-Lacey M, Jimenez de Aberasturi D, Liz-Marzán LM, Journal of materials chemistry B : materials for biology and medicine (2023). http://doi.org/10.1039/D3TB00397C
Abstract: Hyperthermia, as the process of heating a malignant site above 42 °C to trigger cell death, has emerged as an effective and selective cancer therapy strategy. Various modalities of hyperthermia have been proposed, among which magnetic and photothermal hyperthermia are known to benefit from the use of nanomaterials. In this context, we introduce herein a hybrid colloidal nanostructure comprising plasmonic gold nanorods (AuNRs) covered by a silica shell, onto which iron oxide nanoparticles (IONPs) are subsequently grown. The resulting hybrid nanostructures are responsive to both external magnetic fields and near-infrared irradiation. As a result, they can be applied for the targeted magnetic separation of selected cell populations – upon targeting by antibody functionalization – as well as for photothermal heating. Through this combined functionality, the therapeutic effect of photothermal heating can be enhanced. We demonstrate both the fabrication of the hybrid system and its application for targeted photothermal hyperthermia of human glioblastoma cells.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 7
Times cited: 1
DOI: 10.1039/D3TB00397C
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“Benchmarking the photocatalytic self-cleaning activity of industrial and experimental materials with ISO 27448:2009”. Peeters H, Lenaerts S, Verbruggen SW, Materials 16, 1119 (2023). http://doi.org/10.3390/MA16031119
Abstract: Various industrial surface materials are tested for their photocatalytic self-cleaning activity by performing the ISO 27448:2009 method. The samples are pre-activated by UV irradiation, fouled with oleic acid and irradiated by UV light. The degradation of oleic acid over time is monitored by taking water contact angle measurements using a contact angle goniometer. The foulant, oleic acid, is an organic acid that makes the surface more hydrophobic. The water contact angle will thus decrease over time as the photocatalytic material degrades the oleic acid. In this study, we argue that the use of this method is strongly limited to specific types of surface materials, i.e., only those that are hydrophilic and smooth in nature. For more hydrophobic materials, the difference in the water contact angles of a clean surface and a fouled surface is not measurable. Therefore, the photocatalytic self-cleaning activity cannot be established experimentally. Another type of material that cannot be tested by this standard are rough surfaces. For rough surfaces, the water contact angle cannot be measured accurately using a contact angle goniometer as prescribed by the standard. Because of these limitations, many potentially interesting industrial substrates cannot be evaluated. Smooth samples that were treated with an in-house developed hydrophilic titania thin film (PCT/EP2018/079983) showed a great photocatalytic self-cleaning performance according to the ISO standard. Apart from discussing the pros and cons of the current ISO standard, we also stress how to carefully interpret the results and suggest alternative testing solutions.
Keywords: A1 Journal article; Engineering sciences. Technology
Impact Factor: 3.4
DOI: 10.3390/MA16031119
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“Causes and consequences of ordering and dynamic phases of confined vortex rows in superconducting nanostripes”. McNaughton B, Pinto N, Perali A, Milošević, MV, Nanomaterials 12, 4043 (2022). http://doi.org/10.3390/NANO12224043
Abstract: Understanding the behaviour of vortices under nanoscale confinement in superconducting circuits is important for the development of superconducting electronics and quantum technologies. Using numerical simulations based on the Ginzburg-Landau theory for non-homogeneous superconductivity in the presence of magnetic fields, we detail how lateral confinement organises vortices in a long superconducting nanostripe, presenting a phase diagram of vortex configurations as a function of the stripe width and magnetic field. We discuss why the average vortex density is reduced and reveal that confinement influences vortex dynamics in the dissipative regime under sourced electrical current, mapping out transitions between asynchronous and synchronous vortex rows crossing the nanostripe as the current is varied. Synchronous crossings are of particular interest, since they cause single-mode modulations in the voltage drop along the stripe in a high (typically GHz to THz) frequency range.
Keywords: A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Impact Factor: 5.3
Times cited: 2
DOI: 10.3390/NANO12224043
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“Controlled precipitation in a new Al-Mg-Sc alloy for enhanced corrosion behavior while maintaining the mechanical performance”. Krishnamurthy SC, Arseenko M, Kashiwar A, Dufour P, Marchal Y, Delahaye J, Idrissi H, Pardoen T, Mertens A, Simar A, Materials characterization 200, 112886 (2023). http://doi.org/10.1016/J.MATCHAR.2023.112886
Abstract: The hot working of 5xxx series alloys with Mg ≥3.5 wt% is a concern due to the precipitation of β (Al3Mg2) phase at grain boundaries favoring Inter Granular Corrosion (IGC). The mechanical and corrosion properties of a new 5028-H116 Al-Mg-Sc alloy under various β precipitates distribution is analyzed by imposing different cooling rates from the hot forming temperature (i.e. 325 °C). The mechanical properties are maintained regardless of the heat treatment. However, the different nucleation sites and volume fractions of β precipitates for different cooling rates critically affect IGC. Controlled furnace cooling after the 325 °C heat treatment is ideal in 5028-H116 alloy to reduce susceptibility to IGC after sensitization.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 4.7
DOI: 10.1016/J.MATCHAR.2023.112886
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“Effect of annealing on mechanical properties and thermal stability of ZrCu/O nanocomposite amorphous films synthetized by pulsed laser deposition”. Bignoli F, Rashid S, Rossi E, Jaddi S, Djemia P, Terraneo G, Li Bassi A, Idrissi H, Pardoen T, Sebastiani M, Ghidelli M, Materials &, design 221, 110972 (2022). http://doi.org/10.1016/J.MATDES.2022.110972
Abstract: Binary ZrCu nanocomposite amorphous films are synthetized by pulsed laser deposition (PLD) under vac-uum (2 x 10-3 Pa) and 10 Pa He pressure, leading to fully amorphous compact and nanogranular mor-phologies, respectively. Then, post-thermal annealing treatments are carried out to explore thermal stability and crystallization phenomena together with the evolution of mechanical properties. Compact films exhibit larger thermal stability with partial crystallization phenomena starting at 420 degrees C, still to be completed at 550 degrees C, while nanogranular films exhibit early-stage crystallization at 300 degrees C and com-pleted at 485 degrees C. The microstructural differences are related to a distinct evolution of mechanical
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 8.4
DOI: 10.1016/J.MATDES.2022.110972
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“High-strain-induced local modification of the electronic properties of VO₂, thin films”. Birkholzer YA, Sotthewes K, Gauquelin N, Riekehr L, Jannis D, van der Minne E, Bu Y, Verbeeck J, Zandvliet HJW, Koster G, Rijnders G, ACS applied electronic materials 4, 6020 (2022). http://doi.org/10.1021/ACSAELM.2C01176
Abstract: Vanadium dioxide (VO2) is a popular candidate for electronic and optical switching applications due to its well-known semiconductor-metal transition. Its study is notoriously challenging due to the interplay of long- and short-range elastic distortions, as well as the symmetry change and the electronic structure changes. The inherent coupling of lattice and electronic degrees of freedom opens the avenue toward mechanical actuation of single domains. In this work, we show that we can manipulate and monitor the reversible semiconductor-to-metal transition of VO2 while applying a controlled amount of mechanical pressure by a nanosized metallic probe using an atomic force microscope. At a critical pressure, we can reversibly actuate the phase transition with a large modulation of the conductivity. Direct tunneling through the VO2-metal contact is observed as the main charge carrier injection mechanism before and after the phase transition of VO2. The tunneling barrier is formed by a very thin but persistently insulating surface layer of the VO2. The necessary pressure to induce the transition decreases with temperature. In addition, we measured the phase coexistence line in a hitherto unexplored regime. Our study provides valuable information on pressure-induced electronic modifications of the VO2 properties, as well as on nanoscale metal-oxide contacts, which can help in the future design of oxide electronics.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Times cited: 2
DOI: 10.1021/ACSAELM.2C01176
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“Orbital-hybridization-driven charge density wave transition in CsV₃Sb₅, kagome superconductor”. Han S, Tang CS, Li L, Liu Y, Liu H, Gou J, Wu J, Zhou D, Yang P, Diao C, Ji J, Bao J, Zhang L, Zhao M, Milošević, MV, Guo Y, Tian L, Breese MBH, Cao G, Cai C, Wee ATS, Yin X, Advanced materials , 1 (2022). http://doi.org/10.1002/ADMA.202209010
Abstract: Owing to its inherent non-trivial geometry, the unique structural motif of the recently discovered kagome topological superconductor AV(3)Sb(5) (A = K, Rb, Cs) is an ideal host of diverse topologically non-trivial phenomena, including giant anomalous Hall conductivity, topological charge order, charge density wave (CDW), and unconventional superconductivity. Despite possessing a normal-state CDW order in the form of topological chiral charge order and diverse superconducting gaps structures, it remains unclear how fundamental atomic-level properties and many-body effects including Fermi surface nesting, electron-phonon coupling, and orbital hybridization contribute to these symmetry-breaking phenomena. Here, the direct participation of the V3d-Sb5p orbital hybridization in mediating the CDW phase transition in CsV3Sb5 is reported. The combination of temperature-dependent X-ray absorption and first-principles studies clearly indicates the inverse Star-of-David structure as the preferred reconstruction in the low-temperature CDW phase. The results highlight the critical role that Sb orbitals play and establish orbital hybridization as the direct mediator of the CDW states and structural transition dynamics in kagome unconventional superconductors. This is a significant step toward the fundamental understanding and control of the emerging correlated phases from the kagome lattice through the orbital interactions and provides promising approaches to novel regimes in unconventional orders and topology.
Keywords: A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Impact Factor: 29.4
Times cited: 1
DOI: 10.1002/ADMA.202209010
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“Stacking-dependent topological magnons in bilayer CrI₃”. Soenen M, Bacaksiz C, Menezes RM, Milošević, MV, Physical review materials 7, 024421 (2023). http://doi.org/10.1103/PHYSREVMATERIALS.7.024421
Abstract: Motivated by the potential of atomically thin magnets towards achieving tunable high-frequency magnonics, we detail the spin-wave dispersion of bilayer CrI3. We demonstrate that the magnonic behavior of the bilayer strongly depends on its stacking configuration and the interlayer magnetic ordering, where a topological band gap opens in the dispersion caused by the Dzyaloshinskii-Moriya and Kitaev interactions, classifying bilayer CrI3 as a topological magnon insulator. We further reveal that both the size and the topology of the band gap in a CrI3 bilayer with an antiferromagnetic interlayer ordering are tunable by an external magnetic field.
Keywords: A1 Journal article; Condensed Matter Theory (CMT)
Impact Factor: 3.4
DOI: 10.1103/PHYSREVMATERIALS.7.024421
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“Sunlight-powered reverse water gas shift reaction catalysed by plasmonic Au/TiO₂, nanocatalysts : effects of Au particle size on the activity and selectivity”. Volders J, Elen K, Raes A, Ninakanti R, Kelchtermans A-S, Sastre F, Hardy A, Cool P, Verbruggen SW, Buskens P, Van Bael MK, Nanomaterials 12, 4153 (2022). http://doi.org/10.3390/NANO12234153
Abstract: This study reports the low temperature and low pressure conversion (up to 160 °C, p = 3.5 bar) of CO2 and H2 to CO using plasmonic Au/TiO2 nanocatalysts and mildly concentrated artificial sunlight as the sole energy source (up to 13.9 kW·m-2 = 13.9 suns). To distinguish between photothermal and non-thermal contributors, we investigated the impact of the Au nanoparticle size and light intensity on the activity and selectivity of the catalyst. A comparative study between P25 TiO2-supported Au nanocatalysts of a size of 6 nm and 16 nm displayed a 15 times higher activity for the smaller particles, which can only partially be attributed to the higher Au surface area. Other factors that may play a role are e.g., the electronic contact between Au and TiO2 and the ratio between plasmonic absorption and scattering. Both catalysts displayed ≥84% selectivity for CO (side product is CH4). Furthermore, we demonstrated that the catalytic activity of Au/TiO2 increases exponentially with increasing light intensity, which indicated the presence of a photothermal contributor. In dark, however, both Au/TiO2 catalysts solely produced CH4 at the same catalyst bed temperature (160 °C). We propose that the difference in selectivity is caused by the promotion of CO desorption through charge transfer of plasmon generated charges (as a non-thermal contributor).
Keywords: A1 Journal article; Engineering sciences. Technology; Laboratory of adsorption and catalysis (LADCA); Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 5.3
DOI: 10.3390/NANO12234153
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“Two-dimensional heterostructures formed by graphenelike ZnO and MgO monolayers for optoelectronic applications”. Seyedmohammadzadeh M, Sevik C, Guelseren O, Physical review materials 6, 104004 (2022). http://doi.org/10.1103/PHYSREVMATERIALS.6.104004
Abstract: Two-dimensional heterostructures are an emerging class of materials for novel applications because of extensive engineering potential by tailoring intriguing properties of different layers as well as the ones arising from their interface. A systematic investigation of mechanical, electronic, and optical properties of possible heterostructures formed by bilayer structures graphenelike ZnO and MgO monolayers is presented. Different functionality of each layer makes these heterostructures very appealing for device applications. ZnO layer is convenient for electron transport in these structures, while MgO layer improves electron collection. At the outset, all of the four possible stacking configurations across the heterostructure are mechanically stable. In addition, stability analysis using phonon dispersion reveals that the AB stacking formed by placing the Mg atom on top of the O atom of the ZnO layer is also dynamically stable at zero temperature. Henceforth, we have investigated the optical properties of these stable heterostructures by applying many-body perturbation theory within the framework of GW approximation and solving the Bethe-Salpeter equation. It is demonstrated that strong excitonic effects reduce the optical band gap to the visible light spectrum range. These results show that this new two-dimensional form of ZnO/MgO heterostructures open an avenue for novel optoelectronic device applications.
Keywords: A1 Journal article; Condensed Matter Theory (CMT)
Impact Factor: 3.4
DOI: 10.1103/PHYSREVMATERIALS.6.104004
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“Understanding and preventing photoluminescence quenching to achieve unity photoluminescence quantum yield in Yb:YLF nanocrystals”. Mulder JT, Meijer MS, van Blaaderen JJ, du Fosse I, Jenkinson K, Bals S, Manna L, Houtepen AJ, ACS applied materials and interfaces 15, 3274 (2023). http://doi.org/10.1021/ACSAMI.2C17888
Abstract: Ytterbium-doped LiYF4 (Yb:YLF) is a commonly used material for laser applications, as a photon upconversion medium, and for optical refrigeration. As nanocrystals (NCs), the material is also of interest for biological and physical applications. Unfortunately, as with most phosphors, with the reduction in size comes a large reduction of the photoluminescence quantum yield (PLQY), which is typically associated with an increase in surface-related PL quenching. Here, we report the synthesis of bipyramidal Yb:YLF NCs with a short axis of similar to 60 nm. We systematically study and remove all sources of PL quenching in these NCs. By chemically removing all traces of water from the reaction mixture, we obtain NCs that exhibit a near-unity PLQY for an Yb3+ concentration below 20%. At higher Yb3+ concentrations, efficient concentration quenching occurs. The surface PL quenching is mitigated by growing an undoped YLF shell around the NC core, resulting in near-unity PLQY values even for fully Yb3+-based LiYbF4 cores. This unambiguously shows that the only remaining quenching sites in core-only Yb:YLF NCs reside on the surface and that concentration quenching is due to energy transfer to the surface. Monte Carlo simulations can reproduce the concentration dependence of the PLQY. Surprisingly, Fo''rster resonance energy transfer does not give satisfactory agreement with the experimental data, whereas nearest-neighbor energy transfer does. This work demonstrates that Yb3+-based nanophosphors can be synthesized with a quality close to that of bulk single crystals. The high Yb3+ concentration in the LiYbF4/LiYF4 core/shell nanocrystals increases the weak Yb3+ absorption, making these materials highly promising for fundamental studies and increasing their effectiveness in bioapplications and optical refrigeration.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 9.5
Times cited: 3
DOI: 10.1021/ACSAMI.2C17888
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“Epitaxial growth of the candidate ferroelectric Rashba material SrBiO3by pulsed laser deposition”. Verdierre G, Gauquelin N, Jannis D, Birkhölzer YA, Mallik S, Verbeeck J, Bibes M, Koster G, APL materials 11, 031109 (2023). http://doi.org/10.1063/5.0138222
Abstract: Among oxides, bismuthates have been gaining much interest due to their unique features. In addition to their superconducting properties, they show potential for applications as topological insulators and as possible spin-to-charge converters. After being first investigated in their bulk form in the 1980s, bismuthates have been successfully grown as thin films. However, most efforts have focused on BaBiO<sub>3</sub>, with SrBiO<sub>3</sub>receiving only little attention. Here, we report the growth of epitaxial films of SrBiO<sub>3</sub>on both TiO<sub>2</sub>-terminated SrTiO<sub>3</sub>and NdO-terminated NdScO<sub>3</sub>substrates by pulsed laser deposition. SrBiO<sub>3</sub>has a pseudocubic lattice constant of ∼4.25 Å and grows relaxed on NdScO<sub>3</sub>. Counter-intuitively, it grows with a slight tensile strain on SrTiO<sub>3</sub>despite a large lattice mismatch, which should induce compressive strain. High-resolution transmission electron microscopy reveals that this occurs as a consequence of structural domain matching, with blocks of 10 SrBiO<sub>3</sub>unit planes matching blocks of 11 SrTiO<sub>3</sub>unit planes. This work provides a framework for the synthesis of high quality perovskite bismuthates films and for the understanding of their interface interactions with homostructural substrates.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 6.1
DOI: 10.1063/5.0138222
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“Insights into the Photoelectrocatalytic Behavior of gCN-Based Anode Materials Supported on Ni Foams”. Benedoue S, Benedet M, Gasparotto A, Gauquelin N, Orekhov A, Verbeeck J, Seraglia R, Pagot G, Rizzi GA, Balzano V, Gavioli L, Noto VD, Barreca D, Maccato C, Nanomaterials 13, 1035 (2023). http://doi.org/10.3390/nano13061035
Abstract: Graphitic carbon nitride (gCN) is a promising n-type semiconductor widely investigated for photo-assisted water splitting, but less studied for the (photo)electrochemical degradation of aqueous organic pollutants. In these fields, attractive perspectives for advancements are offered by a proper engineering of the material properties, e.g., by depositing gCN onto conductive and porous scaffolds, tailoring its nanoscale morphology, and functionalizing it with suitable cocatalysts. The present study reports on a simple and easily controllable synthesis of gCN flakes on Ni foam substrates by electrophoretic deposition (EPD), and on their eventual decoration with Co-based cocatalysts [CoO, CoFe2O4, cobalt phosphate (CoPi)] via radio frequency (RF)-sputtering or electrodeposition. After examining the influence of processing conditions on the material characteristics, the developed systems are comparatively investigated as (photo)anodes for water splitting and photoelectrocatalysts for the degradation of a recalcitrant water pollutant [potassium hydrogen phthalate (KHP)]. The obtained results highlight that while gCN decoration with Co-based cocatalysts boosts water splitting performances, bare gCN as such is more efficient in KHP abatement, due to the occurrence of a different reaction mechanism. The related insights, provided by a multi-technique characterization, may provide valuable guidelines for the implementation of active nanomaterials in environmental remediation and sustainable solar-to-chemical energy conversion.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 5.3
Times cited: 3
DOI: 10.3390/nano13061035
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“Efficient iron phosphide catalyst as a counter electrode in dye-sensitized solar cells”. Yildiz A, Chouki T, Atli A, Harb M, Verbruggen SW, Ninakanti R, Emin S, ACS applied energy materials 4, 10618 (2021). http://doi.org/10.1021/ACSAEM.1C01628
Abstract: Developing an efficient material as a counter electrode (CE) with excellent catalytic activity, intrinsic stability, and low cost is essential for the commercial application of dye-sensitized solar cells (DSSCs). Transition metal phosphides have been demonstrated as outstanding multifunctional catalysts in a broad range of energy conversion technologies. Here, we exploited different phases of iron phosphide as CEs in DSSCs with an I–/I3–-based electrolyte. Solvothermal synthesis using a triphenylphosphine precursor as a phosphorus source allows to grow a Fe2P phase at 300 °C and a FeP phase at 350 °C. The obtained iron phosphide catalysts were coated on fluorine-doped tin oxide substrates and heat-treated at 450 °C under an inert gas atmosphere. The solar-to-current conversion efficiency of the solar cells assembled with the Fe2P material reached 3.96 ± 0.06%, which is comparable to the device assembled with a platinum (Pt) CE. DFT calculations support the experimental observations and explain the fundamental origin behind the improved performance of Fe2P compared to FeP. These results indicate that the Fe2P catalyst exhibits excellent performance along with desired stability to be deployed as an efficient Pt-free alternative in DSSCs.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
DOI: 10.1021/ACSAEM.1C01628
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“Hydrogen clathrates : next generation hydrogen storage materials”. Gupta A, Baron GV, Perreault P, Lenaerts S, Ciocarlan R-G, Cool P, Mileo PGM, Rogge S, Van Speybroeck V, Watson G, Van Der Voort P, Houlleberghs M, Breynaert E, Martens J, Denayer JFM, Energy Storage Materials 41, 69 (2021). http://doi.org/10.1016/J.ENSM.2021.05.044
Abstract: Extensive research has been carried on the molecular adsorption in high surface area materials such as carbonaceous materials and MOFs as well as atomic bonded hydrogen in metals and alloys. Clathrates stand among the ones to be recently suggested for hydrogen storage. Although, the simulations predict lower capacity than the expected by the DOE norms, the additional benefits of clathrates such as low production and operational cost, fully reversible reaction, environmentally benign nature, low risk of flammability make them one of the most promising materials to be explored in the next decade. The inherent ability to tailor the properties of clathrates using techniques such as addition of promoter molecules, use of porous supports and formation of novel reverse micelles morphology provide immense scope customisation and growth. As rapidly evolving materials, clathrates promise to get as close as possible in the search of “holy grail” of hydrogen storage. This review aims to provide the audience with the background of the current developments in the solid-state hydrogen storage materials, with a special focus on the hydrogen clathrates. The in-depth analysis of the hydrogen clathrates will be provided beginning from their discovery, various additives utilised to enhance their thermodynamic and kinetic properties, challenges in the characterisation of hydrogen in clathrates, theoretical developments to justify the experimental findings and the upscaling opportunities presented by this system. The review will present state of the art in the field and also provide a global picture for the path forward.
Keywords: A1 Journal article; Engineering sciences. Technology; Laboratory of adsorption and catalysis (LADCA); Sustainable Energy, Air and Water Technology (DuEL)
DOI: 10.1016/J.ENSM.2021.05.044
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“Linking bi-metal distribution patterns in porous carbon nitride fullerene to its catalytic activity toward gas adsorption”. Nematollahi P, Neyts EC, Nanomaterials 11, 1794 (2021). http://doi.org/10.3390/NANO11071794
Abstract: Immobilization of two single transition metal (TM) atoms on a substrate host opens numerous possibilities for catalyst design. If the substrate contains more than one vacancy site, the combination of TMs along with their distribution patterns becomes a design parameter potentially complementary to the substrate itself and the bi-metal composition. By means of DFT calculations, we modeled three dissimilar bi-metal atoms (Ti, Mn, and Cu) doped into the six porphyrin-like cavities of porous C24N24 fullerene, considering different bi-metal distribution patterns for each binary complex, viz. TixCuz@C24N24, TixMny@C24N24, and MnyCuz@C24N24 (with x, y, z = 0-6). We elucidate whether controlling the distribution of bi-metal atoms into the C24N24 cavities can alter their catalytic activity toward CO2, NO2, H-2, and N-2 gas capture. Interestingly, Ti2Mn4@C24N24 and Ti2Cu4@C24N24 complexes showed the highest activity and selectively toward gas capture. Our findings provide useful information for further design of novel few-atom carbon-nitride-based catalysts.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 3.553
DOI: 10.3390/NANO11071794
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“Simulating highly activated sticking of H₂, on Al(110) : quantum versus quasi-classical dynamics”. Tchakoua T, Powell AD, Gerrits N, Somers MF, Doblhoff-Dier K, Busnengo HF, Kroes G-J, The journal of physical chemistry: C : nanomaterials and interfaces 127, 5395 (2023). http://doi.org/10.1021/ACS.JPCC.3C00426
Abstract: We evaluate the importance of quantum effects on the sticking of H2 on Al(110) for conditions that are close to those of molecular beam experiments that have been done on this system. Calculations with the quasi-classical trajectory (QCT) method and with quantum dynamics (QD) are performed using a model in which only motion in the six molecular degrees of freedom is allowed. The potential energy surface used has a minimum barrier height close to the value recently obtained with the quantum Monte Carlo method. Monte Carlo averaging over the initial rovibrational states allowed the QD calculations to be done with an order of magnitude smaller computational expense. The sticking probability curve computed with QD is shifted to lower energies relative to the QCT curve by 0.21 to 0.05 kcal/mol, with the highest shift obtained for the lowest incidence energy. Quantum effects are therefore expected to play a small role in calculations that would evaluate the accuracy of electronic structure methods for determining the minimum barrier height to dissociative chemisorption for H2 + Al(110) on the basis of the standard procedure for comparing results of theory with molecular beam experiments.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 3.7
DOI: 10.1021/ACS.JPCC.3C00426
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