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Author | Chen, B.; Gauquelin, N.; Reith, P.; Halisdemir, U.; Jannis, D.; Spreitzer, M.; Huijben, M.; Abel, S.; Fompeyrine, J.; Verbeeck, J.; Hilgenkamp, H.; Rijnders, G.; Koster, G. | ||||
Title | Thermal-strain-engineered ferromagnetism of LaMnO3/SrTiO3 heterostructures grown on silicon | Type | A1 Journal article | ||
Year | 2020 | Publication | Physical review materials | Abbreviated Journal | Phys. Rev. Materials |
Volume | 4 | Issue | 2 | Pages | 024406 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | The integration of oxides on Si remains challenging, which largely hampers the practical applications of oxide-based electronic devices with superior performance. Recently, LaMnO3/SrTiO3 (LMO/STO) heterostructures have gained renewed interest for the debating origin of the ferromagnetic-insulating ground state as well as for their spin-filter applications. Here we report on the structural and magnetic properties of high-quality LMO/STO heterostructures grown on silicon. The chemical abruptness across the interface was investigated by atomic-resolution scanning transmission electron microscopy. The difference in the thermal expansion coefficients between LMO and Si imposed a large biaxial tensile strain to the LMO film, resulting in a tetragonal structure with c/a∼ 0.983. Consequently, we observed a significantly suppressed ferromagnetism along with an enhanced coercive field, as compared to the less distorted LMO film (c/a∼1.004) grown on STO single crystal. The results are discussed in terms of tensile-strain enhanced antiferromagnetic instabilities. Moreover, the ferromagnetism of LMO on Si sharply disappeared below a thickness of 5 unit cells, in agreement with the LMO/STO case, pointing to a robust critical behavior irrespective of the strain state. Our results demonstrate that the growth of oxide films on Si can be a promising way to study the tensile-strain effects in correlated oxides, and also pave the way towards the integration of multifunctional oxides on Si with atomic-layer control. | ||||
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Language | Wos | 000513552900003 | Publication Date | 2020-02-12 | |
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ISSN | 2475-9953 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 3.4 | Times cited | 6 | Open Access | Not_Open_Access |
Notes | Nederlandse Organisatie voor Wetenschappelijk Onderzoek; Universiteit Antwerpen; Vlaamse regering; Fonds Wetenschappelijk Onderzoek, G093417N ; Javna Agencija za Raziskovalno Dejavnost RS, J2-9237 P2-0091 ; European Commission, H2020-ICT-2016-1-732642 ; | Approved | Most recent IF: 3.4; 2020 IF: NA | ||
Call Number | EMAT @ emat @c:irua:167782 | Serial | 6375 | ||
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Author | Araizi-Kanoutas, G.; Geessinck, J.; Gauquelin, N.; Smit, S.; Verbeek, X.H.; Mishra, S.K.; Bencok, P.; Schlueter, C.; Lee, T.-L.; Krishnan, D.; Fatermans, J.; Verbeeck, J.; Rijnders, G.; Koster, G.; Golden, M.S. | ||||
Title | Co valence transformation in isopolar LaCoO3/LaTiO3 perovskite heterostructures via interfacial engineering | Type | A1 Journal article | ||
Year | 2020 | Publication | Physical review materials | Abbreviated Journal | Phys. Rev. Materials |
Volume | 4 | Issue | 2 | Pages | 026001 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | We report charge transfer up to a single electron per interfacial unit cell across nonpolar heterointerfaces from the Mott insulator LaTiO3 to the charge transfer insulator LaCoO3. In high-quality bi- and trilayer systems grown using pulsed laser deposition, soft x-ray absorption, dichroism, and scanning transmission electron microscopy-electron energy loss spectroscopy are used to probe the cobalt-3d electron count and provide an element-specific investigation of the magnetic properties. The experiments show the cobalt valence conversion is active within 3 unit cells of the heterointerface, and able to generate full conversion to 3d7 divalent Co, which displays a paramagnetic ground state. The number of LaTiO3/LaCoO3 interfaces, the thickness of an additional, electronically insulating “break” layer between the LaTiO3 and LaCoO3, and the LaCoO3 film thickness itself in trilayers provide a trio of control knobs for average charge of the cobalt ions in LaCoO3, illustrating the efficacy of O−2p band alignment as a guiding principle for property design in complex oxide heterointerfaces. | ||||
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Language | Wos | 000513551200007 | Publication Date | 2020-02-10 | |
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ISSN | 2475-9953 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 3.4 | Times cited | 13 | Open Access | OpenAccess |
Notes | Nederlandse Organisatie voor Wetenschappelijk Onderzoek; Universiteit Antwerpen; Horizon 2020, 730872 ; Department of Science and Technology, Ministry of Science and Technology, SR/NM/Z-07/2015 ; Jawaharlal Nehru Centre for Advanced Scientific Research; | Approved | Most recent IF: 3.4; 2020 IF: NA | ||
Call Number | EMAT @ emat @c:irua:167787 | Serial | 6376 | ||
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Author | Das, P.P.; Guzzinati, G.; Coll, C.; Gomez Perez, A.; Nicolopoulos, S.; Estrade, S.; Peiro, F.; Verbeeck, J.; Zompra, A.A.; Galanis, A.S. | ||||
Title | Reliable Characterization of Organic & Pharmaceutical Compounds with High Resolution Monochromated EEL Spectroscopy | Type | A1 Journal article | ||
Year | 2020 | Publication | Polymers | Abbreviated Journal | Polymers-Basel |
Volume | 12 | Issue | 7 | Pages | 1434 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Organic and biological compounds (especially those related to the pharmaceutical industry) have always been of great interest for researchers due to their importance for the development of new drugs to diagnose, cure, treat or prevent disease. As many new API (active pharmaceutical ingredients) and their polymorphs are in nanocrystalline or in amorphous form blended with amorphous polymeric matrix (known as amorphous solid dispersion—ASD), their structural identification and characterization at nm scale with conventional X-Ray/Raman/IR techniques becomes difficult. During any API synthesis/production or in the formulated drug product, impurities must be identified and characterized. Electron energy loss spectroscopy (EELS) at high energy resolution by transmission electron microscope (TEM) is expected to be a promising technique to screen and identify the different (organic) compounds used in a typical pharmaceutical or biological system and to detect any impurities present, if any, during the synthesis or formulation process. In this work, we propose the use of monochromated TEM-EELS, to analyze selected peptides and organic compounds and their polymorphs. In order to validate EELS for fingerprinting (in low loss/optical region) and by further correlation with advanced DFT, simulations were utilized. | ||||
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Language | Wos | 000556786700001 | Publication Date | 2020-06-27 | |
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Series Volume | Series Issue | Edition | |||
ISSN | 2073-4360 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 3.364 | Times cited | 6 | Open Access | OpenAccess |
Notes | C.C., F.P., S.E. acknowledges the Spanish government for projects MAT2016-79455-P, Research Network RED2018-102609-T and the FPI (BES-2017-080045) grant of Ministerio de Ciència, Innovación y Universidades. G.G. acknowledges support from a postdoctoral fellowship grant from the Fonds Wetenschappelijk Onderzoek—Vlaanderen (FWO). P.P.D., A.G.P., S.N. gratefully acknowledge much helpful discussion on EELS study for organic compounds with Dr. Andrey Chuvilin (CIC NANOGUNE, Donostia—San Sebastian, Spain). The authors also acknowledge Raúl Arenal (University de Zaragoza, Spain) for useful discussion on EELS. The authors acknowledge also Ulises Julio Amador Elizondo (Universidad CEU San Pablo, Spain) for kindly provide the aripiprazole and piroxicam samples for EELS study.; EUSMI_TA; | Approved | Most recent IF: NA | ||
Call Number | EMAT @ emat @c:irua:170603 | Serial | 6400 | ||
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Author | Groenendijk, D.J.; Autieri, C.; van Thiel, T.C.; Brzezicki, W.; Hortensius, J.R.; Afanasiev, D.; Gauquelin, N.; Barone, P.; van den Bos, K.H.W.; van Aert, S.; Verbeeck, J.; Filippetti, A.; Picozzi, S.; Cuoco, M.; Caviglia, A.D. | ||||
Title | Berry phase engineering at oxide interfaces | Type | A1 Journal article | ||
Year | 2020 | Publication | Abbreviated Journal | Phys. Rev. Research | |
Volume | 2 | Issue | 2 | Pages | 023404 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Three-dimensional strontium ruthenate (SrRuO3) is an itinerant ferromagnet that features Weyl points acting as sources of emergent magnetic fields, anomalous Hall conductivity, and unconventional spin dynamics. Integrating SrRuO3 in oxide heterostructures is potentially a novel route to engineer emergent electrodynamics, but its electronic band topology in the two-dimensional limit remains unknown. Here we show that ultrathin SrRuO3 exhibits spin-polarized topologically nontrivial bands at the Fermi energy. Their band anticrossings show an enhanced Berry curvature and act as competing sources of emergent magnetic fields. We control their balance by designing heterostructures with symmetric (SrTiO3/SrRuO3/SrTiO3 and SrIrO3/SrRuO3/SrIrO3) and asymmetric interfaces (SrTiO3/SrRuO3/SrIrO3). Symmetric structures exhibit an interface-tunable single-channel anomalous Hall effect, while ultrathin SrRuO3 embedded in asymmetric structures shows humplike features consistent with multiple Hall contributions. The band topology of two-dimensional SrRuO3 proposed here naturally accounts for these observations and harmonizes a large body of experimental results. | ||||
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Language | Wos | 000603642700008 | Publication Date | 2020-06-25 | |
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ISSN | 2643-1564 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | Times cited | 58 | Open Access | OpenAccess | |
Notes | Nederlandse Organisatie voor Wetenschappelijk Onderzoek; Fonds Wetenschappelijk Onderzoek; European Research Council; Horizon 2020, 677458 770887 731473 ; Fondazione Cariplo, 2013-0726 ; Narodowe Centrum Nauki, 2016/23/B/ST3/00839 ; Fundacja na rzecz Nauki Polskiej; Universiteit Antwerpen; Vlaamse regering; | Approved | Most recent IF: NA | ||
Call Number | EMAT @ emat @c:irua:172462 | Serial | 6401 | ||
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Author | Prabhakara, V.; Jannis, D.; Guzzinati, G.; Béché, A.; Bender, H.; Verbeeck, J. | ||||
Title | HAADF-STEM block-scanning strategy for local measurement of strain at the nanoscale | Type | A1 Journal article | ||
Year | 2020 | Publication | Ultramicroscopy | Abbreviated Journal | Ultramicroscopy |
Volume | 219 | Issue | Pages | 113099 | |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Lattice strain measurement of nanoscale semiconductor devices is crucial for the semiconductor industry as strain substantially improves the electrical performance of transistors. High resolution scanning transmission electron microscopy (HR-STEM) imaging is an excellent tool that provides spatial resolution at the atomic scale and strain information by applying Geometric Phase Analysis or image fitting procedures. However, HR-STEM images regularly suffer from scanning distortions and sample drift during image acquisition. In this paper, we propose a new scanning strategy that drastically reduces artefacts due to drift and scanning distortion, along with extending the field of view. It consists of the acquisition of a series of independent small subimages containing an atomic resolution image of the local lattice. All subimages are then analysed individually for strain by fitting a nonlinear model to the lattice images. The method allows flexible tuning of spatial resolution and the field of view within the limits of the dynamic range of the scan engine while maintaining atomic resolution sampling within the subimages. The obtained experimental strain maps are quantitatively benchmarked against the Bessel diffraction technique. We demonstrate that the proposed scanning strategy approaches the performance of the diffraction technique while having the advantage that it does not require specialized diffraction cameras. | ||||
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Language | Wos | 000594768500006 | Publication Date | 2020-09-01 | |
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ISSN | 0304-3991 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 2.2 | Times cited | 4 | Open Access | OpenAccess |
Notes | A.B. D.J. and J.V. acknowledge funding through FWO project G093417N ('Compressed sensing enabling low dose imaging in transmission electron microscopy') from the Flanders Research Fund. J.V acknowledges funding from the European Union's Horizon 2020 research and innovation programme under grant agreement No 823717 – ESTEEM3. The Qu-Ant-EM microscope and the direct electron detector used in the diffraction experiments was partly funded by the Hercules fund from the Flemish Government. This project has received funding from the GOA project “Solarpaint” of the University of Antwerp. GG acknowledges support from a postdoctoral fellowship grant from the Fonds Wetenschappelijk Onderzoek – Vlaanderen (FWO). Special thanks to Dr. Thomas Nuytten, Prof. Dr. Wilfried Vandervorst, Dr. Paola Favia, Dr. Olivier Richard from IMEC, Leuven and Prof. Dr. Sara Bals from EMAT, Antwerp for their continuous support and collaboration with the project and to the IMEC processing group for the device fabrication. | Approved | Most recent IF: 2.2; 2020 IF: 2.843 | ||
Call Number | EMAT @ emat @c:irua:172485 | Serial | 6404 | ||
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Author | Vanrompay, H.; Skorikov, A.; Bladt, E.; Béché, A.; Freitag, B.; Verbeeck, J.; Bals, S. | ||||
Title | Fast versus conventional HAADF-STEM tomography of nanoparticles: advantages and challenges | Type | A1 Journal article | ||
Year | 2021 | Publication | Ultramicroscopy | Abbreviated Journal | Ultramicroscopy |
Volume | 221 | Issue | Pages | 113191 | |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | HAADF-STEM tomography is a widely used experimental technique for analyzing nanometer-scale crystalline structures of a large variety of materials in three dimensions. Unfortunately, the acquisition of conventional HAADF-STEM tilt series can easily take up one hour or more, depending on the complexity of the experiment. It is therefore far from straightforward to investigate samples that do not withstand long acquisition or to acquire large amounts of tilt series during a single TEM experiment. The latter would lead to the ability to obtain statistically meaningful 3D data, or to perform in situ 3D characterizations with a much shorter time resolution. Various HAADF-STEM acquisition strategies have been proposed to accelerate the tomographic acquisition and reduce the required electron dose. These methods include tilting the holder continuously while acquiring a projection “movie” and a hybrid, incremental, methodology which combines the benefits of the conventional and continuous technique. However, until now an experimental evaluation has been lacking. In this paper, the different acquisition strategies will be experimentally compared in terms of speed, resolution and electron dose. This evaluation will be performed based on experimental tilt series acquired for various metallic nanoparticles with different shapes and sizes. We discuss the data processing involved with the fast HAADF-STEM tilt series and provide a general guideline when which acquisition strategy should be preferentially used. | ||||
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Language | Wos | 000612539600003 | Publication Date | 2020-12-08 | |
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ISSN | 0304-3991 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 2.843 | Times cited | 15 | Open Access | OpenAccess |
Notes | We acknowledge Prof. Luis M. Liz-Marzán and co-workers of the Bionanoplasmonics Laboratory, CIC biomaGUNE, Spain for providing the Au@Ag nanoparticles, Prof. Sara. E. Skrabalak and co-workers of Indiana University, United States for the provision of the Au octopods and Prof. Teri W. Odom of Northwestern University, United States for the provision of the Au nanostars. H.V. acknowledges financial support by the Research Foundation Flanders (FWO grant 1S32617N). S.B acknowledges financial support by the Research Foundation Flanders (FWO grant G.0381.16N). This project received funding as well from the European Union’s Horizon 2020 research and innovation program under grant agreement No 731019 (EUSMI) and No 815128 (REALNANO). The authors acknowledge the entire EMAT technical staff for their support.; sygma | Approved | Most recent IF: 2.843 | ||
Call Number | EMAT @ emat @c:irua:174551 | Serial | 6660 | ||
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Author | Wang, J.; Gauquelin, N.; Huijben, M.; Verbeeck, J.; Rijnders, G.; Koster, G. | ||||
Title | Metal-insulator transition of SrVO 3 ultrathin films embedded in SrVO 3 / SrTiO 3 superlattices | Type | A1 Journal article | ||
Year | 2020 | Publication | Applied Physics Letters | Abbreviated Journal | Appl Phys Lett |
Volume | 117 | Issue | 13 | Pages | 133105 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | The metal-insulator transition (MIT) in strongly correlated oxides is a topic of great interest for its potential applications, such as Mott field effect transistors and sensors. We report that the MIT in high quality epitaxial SrVO3 (SVO) thin films is present as the film thickness is reduced, lowering the dimensionality of the system, and electron-electron correlations start to become the dominant interactions. The critical thickness of 3 u.c is achieved by avoiding effects due to off-stoichiometry using optimal growth conditions and excluding any surface effects by a STO capping layer. Compared to the single SVO thin films, conductivity enhancement in SVO/STO superlattices is observed. This can be explained by the interlayer coupling effect between SVO sublayers in the superlattices. Magnetoresistance and Hall measurements indicate that the dominant driving force of MIT is the electron–electron interaction. | ||||
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Language | Wos | 000577126100001 | Publication Date | 2020-09-28 | |
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ISSN | 0003-6951 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 4 | Times cited | 8 | Open Access | OpenAccess |
Notes | Nederlandse Organisatie voor Wetenschappelijk Onderzoek, 13HTSM01 ; | Approved | Most recent IF: 4; 2020 IF: 3.411 | ||
Call Number | EMAT @ emat @c:irua:172461 | Serial | 6415 | ||
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Author | Jovanović, Z.; Gauquelin, N.; Koster, G.; Rubio-Zuazo, J.; Ghosez, P.; Verbeeck, J.; Suvorov, D.; Spreitzer, M. | ||||
Title | Simultaneous heteroepitaxial growth of SrO (001) and SrO (111) during strontium-assisted deoxidation of the Si (001) surface | Type | A1 Journal article | ||
Year | 2020 | Publication | Rsc Advances | Abbreviated Journal | Rsc Adv |
Volume | 10 | Issue | 52 | Pages | 31261-31270 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Epitaxial integration of transition-metal oxides with silicon brings a variety of functional properties to the well-established platform of electronic components. In this process, deoxidation and passivation of the silicon surface are one of the most important steps, which in our study were controlled by an ultra-thin layer of SrO and monitored by using transmission electron microscopy (TEM), electron energy-loss spectroscopy (EELS), synchrotron X-ray diffraction (XRD) and reflection high energy electron diffraction (RHEED) methods. Results revealed that an insufficient amount of SrO leads to uneven deoxidation of the silicon surface<italic>i.e.</italic>formation of pits and islands, whereas the composition of the as-formed heterostructure gradually changes from strontium silicide at the interface with silicon, to strontium silicate and SrO in the topmost layer. Epitaxial ordering of SrO, occurring simultaneously with silicon deoxidation, was observed. RHEED analysis has identified that SrO is epitaxially aligned with the (001) Si substrate both with SrO (001) and SrO (111) out-of-plane directions. This observation was discussed from the point of view of SrO desorption, SrO-induced deoxidation of the Si (001) surface and other interfacial reactions as well as structural ordering of deposited SrO. Results of the study present an important milestone in understanding subsequent epitaxial integration of functional oxides with silicon using SrO. | ||||
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Language | Wos | 000566579400025 | Publication Date | 2020-08-24 | |
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ISSN | 2046-2069 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 3.9 | Times cited | 1 | Open Access | OpenAccess |
Notes | Vlaamse regering, Hercules Fund ; Ministarstvo Prosvete, Nauke i Tehnološkog Razvoja, III 45006 ; Javna Agencija za Raziskovalno Dejavnost RS, J2-9237 P2-0091 ; Fonds Wetenschappelijk Onderzoek, G.0044.13N ; Ministerio de Ciencia, Innovación y Universidades; Universiteit Antwerpen, GOA project Solarpaint ; F.R.S.-FNRS, PDR project PROMOSPAN ; Consejo Superior de Investigaciones Cientificas; University of Liège, ARC project AIMED ; Ministry of Education, Science and Sport, M.ERA-NET project SIOX ; | Approved | Most recent IF: 3.9; 2020 IF: 3.108 | ||
Call Number | EMAT @ emat @c:irua:172059 | Serial | 6416 | ||
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Author | Bigiani, L.; Gasparotto, A.; Andreu, T.; Verbeeck, J.; Sada, C.; Modin, E.; Lebedev, O.I.; Morante, J.R.; Barreca, D.; Maccato, C. | ||||
Title | Au-manganese oxide nanostructures by a plasma-assisted process as electrocatalysts for oxygen evolution : a chemico-physical investigation | Type | A1 Journal article | ||
Year | 2020 | Publication | Advanced sustainable systems | Abbreviated Journal | |
Volume | Issue | Pages | 2000177-11 | ||
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | Earth-abundant and eco-friendly manganese oxides are promising platforms for the oxygen evolution reaction (OER) in water electrolysis. Herein, a versatile and potentially scalable route to gold-decorated manganese oxide-based OER electrocatalysts is reported. In particular, MnxOy(MnO2, Mn2O3) host matrices are grown on conductive glasses by plasma assisted-chemical vapor deposition (PA-CVD), and subsequently functionalized with gold nanoparticles (guest) as OER activators by radio frequency (RF)-sputtering. The final selective obtainment of MnO2- or Mn2O3-based systems is then enabled by annealing under oxidizing or inert atmosphere, respectively. A detailed material characterization evidences the formation of high-purity Mn(x)O(y)dendritic nanostructures with an open morphology and an efficient guest dispersion into the host matrices. The tailoring of Mn(x)O(y)phase composition and host-guest interactions has a remarkable influence on OER activity yielding, for the best performing Au/Mn(2)O(3)system, a current density of approximate to 5 mA cm(-2)at 1.65 V versus the reversible hydrogen electrode (RHE) and an overpotential close to 300 mV at 1 mA cm(-2). Such results, comparing favorably with literature data on manganese oxide-based materials, highlight the importance of compositional control, as well as of surface and interface engineering, to develop low-cost and efficient anode nanocatalysts for water splitting applications. | ||||
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Language | Wos | 000572376000001 | Publication Date | 2020-09-25 | |
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ISSN | 2366-7486 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 7.1 | Times cited | 4 | Open Access | Not_Open_Access |
Notes | ; Padova University (DOR 2017-2019 and P-DiSC #03BIRD2018-UNIPD OXYGENA projects), as well as the INSTM Consortium (INSTMPD004 – NETTUNO project) and AMGA Foundation (Mn4Energy project), are gratefully acknowledged for financial support. The Qu-Ant-EM microscope was partially funded by the Hercules fund from the Flemish Government. J.V. acknowledges funding from a GOA project “Solarpaint” from the University of Antwerp and from EU H2020 823717 ESTEEM3 project. The authors thank Dr. Daniele Valbusa, Dr. Gianluca Corr, Dr. Andrea Gallo, and Dr. Dileep Khrishnan for helpful experimental assistance. ; esteem3TA; esteem3reported | Approved | Most recent IF: 7.1; 2020 IF: NA | ||
Call Number | UA @ admin @ c:irua:171937 | Serial | 6457 | ||
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Author | Bigiani, L.; Gasparotto, A.; Maccato, C.; Sada, C.; Verbeeck, J.; Andreu, T.; Morante, J.R.; Barreca, D. | ||||
Title | Dual improvement of beta-MnO₂ oxygen evolution electrocatalysts via combined substrate control and surface engineering | Type | A1 Journal article | ||
Year | 2020 | Publication | Chemcatchem | Abbreviated Journal | Chemcatchem |
Volume | Issue | Pages | 1-10 | ||
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | The development of catalysts with high intrinsic activity towards the oxygen evolution reaction (OER) plays a critical role in sustainable energy conversion and storage. Herein, we report on the development of efficient (photo)electrocatalysts based on functionalized MnO(2)systems. Specifically,beta-MnO(2)nanostructures grown by plasma enhanced-chemical vapor deposition on fluorine-doped tin oxide (FTO) or Ni foams were decorated with Co(3)O(4)or Fe(2)O(3)nanoparticles by radio frequency sputtering. Upon functionalization, FTO-supported materials yielded a performance increase with respect to bare MnO2, with current densities at 1.65 Vvs. the reversible hydrogen electrode (RHE) up to 3.0 and 3.5 mA/cm(2)in the dark and under simulated sunlight, respectively. On the other hand, the use of highly porous and conductive Ni foam substrates enabled to maximize cooperative interfacial effects between catalyst components. The best performing Fe2O3/MnO(2)system provided a current density of 17.9 mA/cm(2)at 1.65 Vvs. RHE, an overpotential as low as 390 mV, and a Tafel slope of 69 mV/decade under dark conditions, comparing favorably with IrO(2)and RuO(2)benchmarks. Overall, the control of beta-MnO2/substrate interactions and the simultaneous surface property engineering pave the way to an efficient energy generation from abundant natural resources. | ||||
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Language | Wos | 000571229000001 | Publication Date | 2020-09-18 | |
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ISSN | 1867-3880; 1867-3899 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 4.5 | Times cited | 5 | Open Access | Not_Open_Access |
Notes | ; This work has been financially supported by Padova University DOR 2017-2019, P-DiSC #03BIRD2016-UNIPD and #03BIRD2018-UNIPD projects. A.G. acknowledges AMGA Foundation and INSTM Consortium. J.V. gratefully acknowledges funding from the GOA project “Solarpaint” of the University of Antwerp and the European Union's Horizon 2020 research and innovation programme under grant agreement No 823717-ESTEEM3. ; esteem3TA; esteem3reported | Approved | Most recent IF: 4.5; 2020 IF: 4.803 | ||
Call Number | UA @ admin @ c:irua:171949 | Serial | 6493 | ||
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Author | Bigiani, L.; Andreu, T.; Maccato, C.; Fois, E.; Gasparotto, A.; Sada, C.; Tabacchi, G.; Krishnan, D.; Verbeeck, J.; Ramon Morante, J.; Barreca, D. | ||||
Title | Engineering Au/MnO₂ hierarchical nanoarchitectures for ethanol electrochemical valorization | Type | A1 Journal article | ||
Year | 2020 | Publication | Journal Of Materials Chemistry A | Abbreviated Journal | J Mater Chem A |
Volume | 8 | Issue | 33 | Pages | 16902-16907 |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | The design of eco-friendly electrocatalysts for ethanol valorization is an open challenge towards sustainable hydrogen production. Herein we present an original fabrication route to effective electrocatalysts for the ethanol oxidation reaction (EOR). In particular, hierarchical MnO(2)nanostructures are grown on high-area nickel foam scaffolds by a plasma-assisted strategy and functionalized with low amounts of optimally dispersed Au nanoparticles. This strategy leads to catalysts with a unique morphology, designed to enhance reactant-surface contacts and maximize active site utilization. The developed nanoarchitectures show superior performances for ethanol oxidation in alkaline media. We reveal that Au decoration boosts MnO(2)catalytic activity by inducing pre-dissociation and pre-oxidation of the adsorbed ethanol molecules. This evidence validates our strategy as an effective route for the development of green electrocatalysts for efficient electrical-to-chemical energy conversion. | ||||
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Language | Wos | 000562931300008 | Publication Date | 2020-07-21 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2050-7488; 2050-7496 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 11.9 | Times cited | 16 | Open Access | OpenAccess |
Notes | ; This work was financially supported by Padova University DOR 2016-2019 and P-DiSC #03BIRD2018-UNIPD OXYGENA projects, as well as by the INSTM Consortium (INSTMPD004 – NETTUNO), AMGA Foundation Mn4Energy project and Insubria University FAR2018. J. V. and D. K. acknowledge funding from the Flemish Government (Hercules), GOA project “Solarpaint” (Antwerp University) and European Union's H2020 programme under grant agreement no. 823717 ESTEEM3. The authors are grateful to Dr Gianluca Corr for skillful technical support. ; esteem3TA; esteem3reported | Approved | Most recent IF: 11.9; 2020 IF: 8.867 | ||
Call Number | UA @ admin @ c:irua:171989 | Serial | 6506 | ||
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Author | Chen, B.; Gauquelin, N.; Jannis, D.; Cunha, D.M.; Halisdemir, U.; Piamonteze, C.; Lee, J.H.; Belhadi, J.; Eltes, F.; Abel, S.; Jovanovic, Z.; Spreitzer, M.; Fompeyrine, J.; Verbeeck, J.; Bibes, M.; Huijben, M.; Rijnders, G.; Koster, G. | ||||
Title | Strain-engineered metal-to-insulator transition and orbital polarization in nickelate superlattices integrated on silicon | Type | A1 Journal article | ||
Year | 2020 | Publication | Advanced Materials | Abbreviated Journal | Adv Mater |
Volume | Issue | Pages | 2004995 | ||
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | Epitaxial growth of SrTiO3 (STO) on silicon greatly accelerates the monolithic integration of multifunctional oxides into the mainstream semiconductor electronics. However, oxide superlattices (SLs), the birthplace of many exciting discoveries, remain largely unexplored on silicon. In this work, LaNiO3/LaFeO3 SLs are synthesized on STO-buffered silicon (Si/STO) and STO single-crystal substrates, and their electronic properties are compared using dc transport and X-ray absorption spectroscopy. Both sets of SLs show a similar thickness-driven metal-to-insulator transition, albeit with resistivity and transition temperature modified by the different amounts of strain. In particular, the large tensile strain promotes a pronounced Ni 3dx2-y2 orbital polarization for the SL grown on Si/STO, comparable to that reported for LaNiO3 SL epitaxially strained to DyScO3 substrate. Those results illustrate the ability to integrate oxide SLs on silicon with structure and property approaching their counterparts grown on STO single crystal, and also open up new prospects of strain engineering in functional oxides based on the Si platform. | ||||
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Language | Wos | 000588146500001 | Publication Date | 2020-11-11 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0935-9648 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 29.4 | Times cited | 18 | Open Access | OpenAccess |
Notes | ; This work is supported by the international M-ERA.NET project SIOX (project 4288) and H2020 project ULPEC (project 732642). M.S. acknowledges funding from Slovenian Research Agency (Grants No. J2-9237 and No. P2-0091). This work received support from the ERC CoG MINT (#615759) and from a PHC Van Gogh grant. M.B. thanks the French Academy of Science and the Royal Netherlands Academy of Arts and Sciences for supporting his stays in the Netherlands. This project has received funding as a transnational access project from the European Union's Horizon 2020 research and innovation programme under grant agreement No 823717 – ESTEEM3. N.G. and J.V. acknowledge GOA project “Solarpaint” of the University of Antwerp. ; esteem3TA; esteem3reported | Approved | Most recent IF: 29.4; 2020 IF: 19.791 | ||
Call Number | UA @ admin @ c:irua:173516 | Serial | 6617 | ||
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Author | Savchenko, T.M.; Buzzi, M.; Howald, L.; Ruta, S.; Vijayakumar, J.; Timm, M.; Bracher, D.; Saha, S.; Derlet, P.M.; Béché, A.; Verbeeck, J.; Chantrell, R.W.; Vaz, C.A.F.; Nolting, F.; Kleibert, A. | ||||
Title | Single femtosecond laser pulse excitation of individual cobalt nanoparticles | Type | A1 Journal article | ||
Year | 2020 | Publication | Physical Review B | Abbreviated Journal | Phys Rev B |
Volume | 102 | Issue | 20 | Pages | 205418 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Laser-induced manipulation of magnetism at the nanoscale is a rapidly growing research topic with potential for applications in spintronics. In this work, we address the role of the scattering cross section, thermal effects, and laser fluence on the magnetic, structural, and chemical stability of individual magnetic nanoparticles excited by single femtosecond laser pulses. We find that the energy transfer from the fs laser pulse to the nanoparticles is limited by the Rayleigh scattering cross section, which in combination with the light absorption of the supporting substrate and protective layers determines the increase in the nanoparticle temperature. We investigate individual Co nanoparticles (8 to 20 nm in size) as a prototypical model system, using x-ray photoemission electron microscopy and scanning electron microscopy upon excitation with single femtosecond laser pulses of varying intensity and polarization. In agreement with calculations, we find no deterministic or stochastic reversal of the magnetization in the nanoparticles up to intensities where ultrafast demagnetization or all-optical switching is typically reported in thin films. Instead, at higher fluences, the laser pulse excitation leads to photo-chemical reactions of the nanoparticles with the protective layer, which results in an irreversible change in the magnetic properties. Based on our findings, we discuss the conditions required for achieving laser-induced switching in isolated nanomagnets. | ||||
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Language | Wos | 000589602000005 | Publication Date | 2020-11-16 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2469-9950 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 3.7 | Times cited | 1 | Open Access | OpenAccess |
Notes | This work received funding by the Swiss National Foundation (SNF) (Grants No. 200021160186 and No. 2002153540), the Swiss Nanoscience Institute (SNI) (Grant No. SNI P1502), the European Union’s Horizon 2020 research and innovation programme under Grant Agreement No. 737093 (FEMTOTERABYTE), and the COST Action CA17123 (MAGNETOFON). Part of this work was performed at the SIM beamline of the Swiss Light Source (SLS), Paul Scherrer Institut, Villigen, Switzerland. Part of the simulations were undertaken on the VIKING cluster, which is a high-performance compute facility provided by the University of York. We kindly acknowledge Anja Weber from PSI for preparation of substrates with marker structures. A.B. and Jo Verbeeck acknowledge funding through FWO Project No. G093417N (“Compressed sensing enabling low dose imaging in transmission electron microscopy”) from the Flanders Research Fund. Jo Verbeeck acknowledges funding from the European Union’s Horizon 2020 research and innovation program under Grant Agreement No. 823717 – ESTEEM3. S.S. acknowledges ETH Zurich Post-Doctoral fellowship and Marie Curie actions for people COFUND program.; esteem3JRA; esteem3reported | Approved | Most recent IF: 3.7; 2020 IF: 3.836 | ||
Call Number | EMAT @ emat @c:irua:174273 | Serial | 6669 | ||
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Author | Lin, S.-C.; Kuo, C.-T.; Shao, Y.-C.; Chuang, Y.-D.; Geessinck, J.; Huijben, M.; Rueff, J.-P.; Graff, I.L.; Conti, G.; Peng, Y.; Bostwick, A.; Gullikson, E.; Nemsak, S.; Vailionis, A.; Gauquelin, N.; Verbeeck, J.; Ghiringhelli, G.; Schneider, C.M.; Fadley, C.S. | ||||
Title | Two-dimensional electron systems in perovskite oxide heterostructures : role of the polarity-induced substitutional defects | Type | A1 Journal article | ||
Year | 2020 | Publication | Physical review materials | Abbreviated Journal | |
Volume | 4 | Issue | 11 | Pages | 115002 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | The discovery of a two-dimensional electron system (2DES) at the interfaces of perovskite oxides such as LaAlO3 and SrTiO3 has motivated enormous efforts in engineering interfacial functionalities with this type of oxide heterostructures. However, the fundamental origins of the 2DES are still not understood, e.g., the microscopic mechanisms of coexisting interface conductivity and magnetism. Here we report a comprehensive spectroscopic investigation on the depth profile of 2DES-relevant Ti 3d interface carriers using depthand element-specific techniques like standing-wave excited photoemission and resonant inelastic scattering. We found that one type of Ti 3d interface carriers, which give rise to the 2DES are located within three unit cells from the n-type interface in the SrTiO3 layer. Unexpectedly, another type of interface carriers, which are polarity-induced Ti-on-Al antisite defects, reside in the first three unit cells of the opposing LaAlO3 layer (similar to 10 angstrom). Our findings provide a microscopic picture of how the localized and mobile Ti 3d interface carriers distribute across the interface and suggest that the 2DES and 2D magnetism at the LaAlO3/SrTiO3 interface have disparate explanations as originating from different types of interface carriers. | ||||
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Language | Wos | 000592432200004 | Publication Date | 2020-11-20 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2475-9953 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 3.4 | Times cited | 7 | Open Access | OpenAccess |
Notes | ; We thank G. M. De Luca and L. Braicovich for discussions. Charles S. Fadley was deceased on August 1, 2019. We are grateful for his significant contributions to this work. We thank Advanced Light Source for the access to Beamline 8.0.3 (qRIXS) via Proposal No. 09892 and beamline 7.0.2 (MAESTRO) via Proposal No. RA-00291 that contributed to the results presented here. We thank synchrotron SOLEIL (via Proposal No. 99180118) for the access to Beamline GALAXIES. This work was supported by the U.S. Department of Energy (DOE) under Contract No. DE-AC02-05CH11231 (Advanced Light Source), and by DOE Contract No. DE-SC0014697 through the University of California, Davis (S.-C.L., C.-T.K, and C.S.F.), and from the Julich Research Center, Peter Grunberg Institute, PGI-6. I. L. G. wishes to thank Brazilian scientific agencies CNPQ (Project No. 200789/2017-1) and CAPES (CAPES-PrInt-UFPR) for their financial support. J.V. and N.G. acknowledge funding from the Geconcentreerde Onderzoekacties (GOA) project “Solarpaint” of the University of Antwerp and the European Union's horizon 2020 research and innovation program ES-TEEM3 under grant agreement no 823717. The Qu-Ant-EM microscope used in this study was partly funded by the Hercules fund from the Flemish Government. ; esteem3TA; esteem3reported | Approved | Most recent IF: 3.4; 2020 IF: NA | ||
Call Number | UA @ admin @ c:irua:174316 | Serial | 6713 | ||
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Author | Bigiani, L.; Barreca, D.; Gasparotto, A.; Andreu, T.; Verbeeck, J.; Sada, C.; Modin, E.; Lebedev, O.I.; Morante, J.R.; Maccato, C. | ||||
Title | Selective anodes for seawater splitting via functionalization of manganese oxides by a plasma-assisted process | Type | A1 Journal article | ||
Year | 2021 | Publication | Applied Catalysis B-Environmental | Abbreviated Journal | Appl Catal B-Environ |
Volume | 284 | Issue | Pages | 119684 | |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | The electrolysis of seawater, a significantly more abundant natural reservoir than freshwater, stands as a promising alternative for sustainable hydrogen production, provided that the competitive chloride electro-oxidation is minimized. Herein, we propose an original material combination to selectively trigger oxygen evolution from seawater at expenses of chlorine generation. The target systems, based on MnO2 or Mn2O3 decorated with Fe2O3 or Co3O4, are fabricated by plasma enhanced-chemical vapor deposition of manganese oxides, functionalization with Fe2O3 and Co3O4 by sputtering, and annealing in air/Ar to obtain Mn(IV)/Mn(III) oxides. Among the various options, MnO2 decorated with Co3O4 yields the best performances in alkaline seawater splitting, with an outstanding Tafel slope of approximate to 40 mV x dec(-1) and an overpotential of 450 mV, enabling to rule out chlorine evolution. These attractive performances, resulting from the synergistic contribution of catalytic and electronic effects, open the door to low-cost hydrogen generation from seawater under real-world conditions, paving the way to eventual large-scale applications. | ||||
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Language | Wos | 000623591500008 | Publication Date | 2020-11-20 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0926-3373 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 9.446 | Times cited | 67 | Open Access | OpenAccess |
Notes | The authors thank Padova University (DOR 2017–2020 and P-DiSC #03BIRD2018-UNIPD OXYGENA projects), as well as the INSTM Consortium (INSTMPD004 – NETTUNO project) and AMGA Foundation (Mn4Energy project), for financial support. The Qu-Ant-EM microscope was partly funded by the Hercules fund from the Flemish Government. J.V. acknowledges funding from a GOA project 'Solarpaint' (University of Antwerp) and from the EU-H2020 programme (grant agreement No. 823717 – ESTEEM3). J.R.M. and T.A. acknowledge Generalitat de Catalunya for financial support through the CERCA Programme, 27 M2E (2017SGR1246) and by ERDEF-MINECO coordinated projects ENE2017-85087-C3 and ENE2016-80788-C5-5-R. Thanks are also due to Proff. Gloria Tabacchi and Ettore Fois (Department of Science and High Technology, Insubria University, Como, Italy) for valuable discussions and support. Dr. Daniele Valbusa, Dr. Gianluca Corrò, Dr. Andrea Gallo and Dr. Dileep Khrishnan are gratefully acknowledged for helpful technical assistance. | Approved | Most recent IF: 9.446 | ||
Call Number | UA @ admin @ c:irua:176718 | Serial | 6733 | ||
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Author | Ghidelli, M.; Orekhov, A.; Bassi, A.L.; Terraneo, G.; Djemia, P.; Abadias, G.; Nord, M.; Béché, A.; Gauquelin, N.; Verbeeck, J.; Raskin, J.-p.; Schryvers, D.; Pardoen, T.; Idrissi, H. | ||||
Title | Novel class of nanostructured metallic glass films with superior and tunable mechanical properties | Type | A1 Journal article | ||
Year | 2021 | Publication | Acta Materialia | Abbreviated Journal | Acta Mater |
Volume | Issue | Pages | 116955 | ||
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | A novel class of nanostructured Zr50Cu50 (%at.) metallic glass films with superior and tunable mechanical properties is produced by pulsed laser deposition. The process can be controlled to synthetize a wide range of film microstructures including dense fully amorphous, amorphous embedded with nanocrystals and amorphous nano-granular. A unique dense self-assembled nano-laminated atomic arrangement characterized by alternating Cu-rich and Zr/O-rich nanolayers with different local chemical enrichment and amorphous or amorphous-crystalline composite nanostructure has been discovered, while significant in-plane clustering is reported for films synthetized at high deposition pressures. This unique nanoarchitecture is at the basis of superior mechanical properties including large hardness and elastic modulus up to 10 and 140 GPa, respectively and outstanding total elongation to failure (>9%), leading to excellent strength/ductility balance, which can be tuned by playing with the film architecture. These results pave the way to the synthesis of novel class of engineered nanostructured metallic glass films with high structural performances attractive for a number of applications in microelectronics and coating industry. |
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Language | Wos | 000670077800004 | Publication Date | 2021-05-12 | |
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Series Volume | Series Issue | Edition | |||
ISSN | 1359-6454 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 5.301 | Times cited | 27 | Open Access | OpenAccess |
Notes | H.I. is mandated by the Belgian National Fund for Scientific Research (FSR-FNRS). This work was supported by the Fonds de la Recherche Scientifique – FNRS under Grant T.0178.19 and Grant CDR– J011320F. We acknowledge funding for the direct electron detector used in the 4D stem studies from the Hercules fund 'Direct electron detector for soft matter TEM' from the Flemish Government J.V acknowledges funding from the European Union's Horizon 2020 research and innovation program under grant agreement No 823717 – ESTEEM3. A.O. has received partial funding from the GOA project “Solarpaint” of the University of Antwerp. A.B. and J.V. acknowledge funding through FWO project G093417N ('Compressed sensing enabling low dose imaging in transmission electron microscopy') from the Flanders Research Fund. M.G. and A.L.B acknowledge Chantelle Ekanem for support in PLD depositions. | Approved | Most recent IF: 5.301 | ||
Call Number | EMAT @ emat @c:irua:178142 | Serial | 6761 | ||
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Author | Esteban, D.A.; Vanrompay, H.; Skorikov, A.; Béché, A.; Verbeeck, J.; Freitag, B.; Bals, S. | ||||
Title | Fast electron low dose tomography for beam sensitive materials | Type | A1 Journal article | ||
Year | 2021 | Publication | Microscopy And Microanalysis | Abbreviated Journal | Microsc Microanal |
Volume | 27 | Issue | S1 | Pages | 2116-2118 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
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Language | Wos | Publication Date | 2021-07-30 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1431-9276 | ISBN | Additional Links | UA library record | |
Impact Factor | 1.891 | Times cited | Open Access | OpenAccess | |
Notes | Approved | Most recent IF: 1.891 | |||
Call Number | EMAT @ emat @c:irua:183278 | Serial | 6813 | ||
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Author | Prabhakara, V.; Nuytten, T.; Bender, H.; Vandervorst, W.; Bals, S.; Verbeeck, J. | ||||
Title | Linearized radially polarized light for improved precision in strain measurements using micro-Raman spectroscopy | Type | A1 Journal article | ||
Year | 2021 | Publication | Optics Express | Abbreviated Journal | Opt Express |
Volume | 29 | Issue | 21 | Pages | 34531 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Strain engineering in semiconductor transistor devices has become vital in the semiconductor industry due to the ever-increasing need for performance enhancement at the nanoscale. Raman spectroscopy is a non-invasive measurement technique with high sensitivity to mechanical stress that does not require any special sample preparation procedures in comparison to characterization involving transmission electron microscopy (TEM), making it suitable for inline strain measurement in the semiconductor industry. Indeed, at present, strain measurements using Raman spectroscopy are already routinely carried out in semiconductor devices as it is cost effective, fast and non-destructive. In this paper we explore the usage of linearized radially polarized light as an excitation source, which does provide significantly enhanced accuracy and precision as compared to linearly polarized light for this application. Numerical simulations are done to quantitatively evaluate the electric field intensities that contribute to this enhanced sensitivity. We benchmark the experimental results against TEM diffraction-based techniques like nano-beam diffraction and Bessel diffraction. Differences between both approaches are assigned to strain relaxation due to sample thinning required in TEM setups, demonstrating the benefit of Raman for nondestructive inline testing. | ||||
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Language | Wos | 000708940500144 | Publication Date | 2021-10-11 | |
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Series Volume | Series Issue | Edition | |||
ISSN | 1094-4087 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 3.307 | Times cited | 2 | Open Access | OpenAccess |
Notes | Horizon 2020 Framework Programme, 823717 – ESTEEM3 ; GOA project, “Solarpaint” ; Herculesstichting;; esteem3jra; esteem3reported; | Approved | Most recent IF: 3.307 | ||
Call Number | EMAT @ emat @c:irua:182472 | Serial | 6816 | ||
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Author | Velazco, A.; Béché, A.; Jannis, D.; Verbeeck, J. | ||||
Title | Reducing electron beam damage through alternative STEM scanning strategies, Part I: Experimental findings | Type | A1 Journal article | ||
Year | 2022 | Publication | Ultramicroscopy | Abbreviated Journal | Ultramicroscopy |
Volume | 232 | Issue | Pages | 113398 | |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | The highly energetic electrons in a transmission electron microscope (TEM) can alter or even completely destroy the structure of samples before sufficient information can be obtained. This is especially problematic in the case of zeolites, organic and biological materials. As this effect depends on both the electron beam and the sample and can involve multiple damage pathways, its study remained difficult and is plagued with irreproducibility issues, circumstantial evidence, rumors, and a general lack of solid data. Here we take on the experimental challenge to investigate the role of the STEM scan pattern on the damage behavior of a commercially available zeolite sample with the clear aim to make our observations as reproducible as possible. We make use of a freely programmable scan engine that gives full control over the tempospatial distribution of the electron probe on the sample and we use its flexibility to obtain multiple repeated experiments under identical conditions comparing the difference in beam damage between a conventional raster scan pattern and a newly proposed interleaved scan pattern that provides exactly the same dose and dose rate and visits exactly the same scan points. We observe a significant difference in beam damage for both patterns with up to 11 % reduction in damage (measured from mass loss). These observations demonstrate without doubt that electron dose, dose rate and acceleration voltage are not the only parameters affecting beam damage in (S)TEM experiments and invite the community to rethink beam damage as an unavoidable consequence of applied electron dose. | ||||
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Language | Wos | 000714819200002 | Publication Date | 2021-10-02 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0304-3991 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 2.2 | Times cited | 18 | Open Access | OpenAccess |
Notes | A.V., D.J., A.B. and J.V. acknowledge funding from FWO project G093417N (’Compressed sensing enabling low dose imaging in transmission electron microscopy’) and G042920N (’Coincident event detection for advanced spectroscopy in transmission electron microscopy’). This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 823717 ESTEEM3. The Qu-Ant-EM microscope was partly funded by the Hercules fund from the Flemish Government. J.V. acknowledges funding from GOA project “Solarpaint” of the University of Antwerp.; JRA; reported | Approved | Most recent IF: 2.2 | ||
Call Number | EMAT @ emat @c:irua:183282 | Serial | 6818 | ||
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Author | Jannis, D.; Müller-Caspary, K.; Béché, A.; Verbeeck, J. | ||||
Title | Coincidence Detection of EELS and EDX Spectral Events in the Electron Microscope | Type | A1 Journal article | ||
Year | 2021 | Publication | Applied Sciences-Basel | Abbreviated Journal | Appl Sci-Basel |
Volume | 11 | Issue | 19 | Pages | 9058 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Recent advances in the development of electron and X-ray detectors have opened up the possibility to detect single events from which its time of arrival can be determined with nanosecond resolution. This allows observing time correlations between electrons and X-rays in the transmission electron microscope. In this work, a novel setup is described which measures individual events using a silicon drift detector and digital pulse processor for the X-rays and a Timepix3 detector for the electrons. This setup enables recording time correlation between both event streams while at the same time preserving the complete conventional electron energy loss (EELS) and energy dispersive X-ray (EDX) signal. We show that the added coincidence information improves the sensitivity for detecting trace elements in a matrix as compared to conventional EELS and EDX. Furthermore, the method allows the determination of the collection efficiencies without the use of a reference sample and can subtract the background signal for EELS and EDX without any prior knowledge of the background shape and without pre-edge fitting region. We discuss limitations in time resolution arising due to specificities of the silicon drift detector and discuss ways to further improve this aspect. | ||||
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Language | Wos | 000710160300001 | Publication Date | 2021-09-28 | |
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Series Volume | Series Issue | Edition | |||
ISSN | 2076-3417 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 1.679 | Times cited | 9 | Open Access | OpenAccess |
Notes | Fonds Wetenschappelijk Onderzoek, G042920 ; Horizon 2020 Framework Programme, 101017720 ; Helmholtz-Fonds, VH-NG-1317 ; | Approved | Most recent IF: 1.679 | ||
Call Number | EMAT @ emat @c:irua:183336 | Serial | 6821 | ||
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Author | Lebedev, N.; Stehno, M.; Rana, A.; Reith, P.; Gauquelin, N.; Verbeeck, J.; Hilgenkamp, H.; Brinkman, A.; Aarts, J. | ||||
Title | Gate-tuned anomalous Hall effect driven by Rashba splitting in intermixed LaAlO3/GdTiO3/SrTiO3 | Type | A1 Journal article | ||
Year | 2021 | Publication | Scientific Reports | Abbreviated Journal | Sci Rep-Uk |
Volume | 11 | Issue | 1 | Pages | 10726 |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | The Anomalous Hall Effect (AHE) is an important quantity in determining the properties and understanding the behaviour of the two-dimensional electron system forming at the interface of SrTiO<sub>3</sub>-based oxide heterostructures. The occurrence of AHE is often interpreted as a signature of ferromagnetism, but it is becoming more and more clear that also paramagnets may contribute to AHE. We studied the influence of magnetic ions by measuring intermixed LaAlO<sub>3</sub>/GdTiO<sub>3</sub>/SrTiO<sub>3</sub>at temperatures below 10 K. We find that, as function of gate voltage, the system undergoes a Lifshitz transition while at the same time an onset of AHE is observed. However, we do not observe clear signs of ferromagnetism. We argue the AHE to be due to the change in Rashba spin-orbit coupling at the Lifshitz transition and conclude that also paramagnetic moments which are easily polarizable at low temperatures and high magnetic fields lead to the presence of AHE, which needs to be taken into account when extracting carrier densities and mobilities. | ||||
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Language | Wos | 000658820100014 | Publication Date | 2021-05-21 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2045-2322 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 4.259 | Times cited | 5 | Open Access | OpenAccess |
Notes | J.V. and N.G. acknowledge funding from the Geconcentreerde Onderzoekacties (GOA) project “Solarpaint” of the University of Antwerp and the European Union’s horizon 2020 research and innovation programme ESTEEM3 under grant agreement 823717. The Qu-Ant-EM microscope used in this study was partly funded by the Hercules fund from the Flemish Government.; esteem3TA; esteem3reported | Approved | Most recent IF: 4.259 | ||
Call Number | EMAT @ emat @c:irua:179608 | Serial | 6822 | ||
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Author | Herzog, M.J.; Gauquelin, N.; Esken, D.; Verbeeck, J.; Janek, J. | ||||
Title | Increased Performance Improvement of Lithium-Ion Batteries by Dry Powder Coating of High-Nickel NMC with Nanostructured Fumed Ternary Lithium Metal Oxides | Type | A1 Journal article | ||
Year | 2021 | Publication | ACS applied energy materials | Abbreviated Journal | ACS Appl. Energy Mater. |
Volume | 4 | Issue | 9 | Pages | 8832-8848 |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | Dry powder coating is an effective approach to protect the surfaces of layered cathode active materials (CAMs) in lithium-ion batteries. Previous investigations indicate an incorporation of lithium ions in fumed Al2O3, ZrO2, and TiO2 coatings on LiNi0.7Mn0.15Co0.15O2 during cycling, improving the cycling performance. Here, this coating approach is transferred for the first time to fumed ternary LiAlO2, Li4Zr3O8, and Li4Ti5O12 and directly compared with their lithium-free equivalents. All materials could be processed equally and their nanostructured small aggregates accumulate on the CAM surfaces to quite homogeneous coating layers with a certain porosity. The LiNixMnyCozO2 (NMC) coated with lithium-containing materials shows an enhanced improvement in overall capacity, capacity retention, rate performance, and polarization behavior during cycling, compared to their lithium-free analogues. The highest rate performance was achieved with the fumed ZrO2 coating, while the best long-term cycling stability with the highest absolute capacity was obtained for the fumed LiAlO2-coated NMC. The optimal coating agent for NMC to achieve a balanced system is fumed Li4Ti5O12, providing a good compromise between high rate capability and good capacity retention. The coating agents prevent CAM particle cracking and degradation in the order LiAlO2 ≈ Al2O3 > Li4Ti5O12 > Li4Zr3O8 > ZrO2 > TiO2. A schematic model for the protection and electrochemical performance enhancement of high-nickel NMC with fumed metal oxide coatings is sketched. It becomes apparent that physical and chemical characteristics of the coating significantly influence the performance of NMC. A high degree of coating-layer porosity is favorable for the rate capability, while a high coverage of the surface, especially in vulnerable grain boundaries, enhances the long-term cycling stability and improves the cracking behavior of NMCs. While zirconium-containing coatings possess the best chemical properties for high rate performances, aluminum-containing coatings feature a superior chemical nature to protect high-nickel NMCs. | ||||
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Language | Wos | 000703338600018 | Publication Date | 2021-09-27 | |
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Series Volume | Series Issue | Edition | |||
ISSN | 2574-0962 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | Times cited | 15 | Open Access | OpenAccess | |
Notes | For his support in scanning electron microscopy analysis, the authors thank Erik Peldszus. N. G. and J. V. acknowledge funding from GOA project “Solarpaint” of the University of Antwerp and from the Flemish Research Fund (FWO) project G0F1320N. The Qu-Ant-EM microscope and the direct electron detector were partly funded by the Hercules fund from the Flemish Government | Approved | Most recent IF: NA | ||
Call Number | EMAT @ emat @c:irua:183949 | Serial | 6823 | ||
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Author | van Thiel, T. c.; Brzezicki, W.; Autieri, C.; Hortensius, J. r.; Afanasiev, D.; Gauquelin, N.; Jannis, D.; Janssen, N.; Groenendijk, D. j.; Fatermans, J.; Van Aert, S.; Verbeeck, J.; Cuoco, M.; Caviglia, A. d. | ||||
Title | Coupling Charge and Topological Reconstructions at Polar Oxide Interfaces | Type | A1 Journal article | ||
Year | 2021 | Publication | Physical Review Letters | Abbreviated Journal | Phys Rev Lett |
Volume | 127 | Issue | 12 | Pages | 127202 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | In oxide heterostructures, different materials are integrated into a single artificial crystal, resulting in a breaking of inversion symmetry across the heterointerfaces. A notable example is the interface between polar and nonpolar materials, where valence discontinuities lead to otherwise inaccessible charge and spin states. This approach paved the way for the discovery of numerous unconventional properties absent in the bulk constituents. However, control of the geometric structure of the electronic wave functions in correlated oxides remains an open challenge. Here, we create heterostructures consisting of ultrathin SrRuO3, an itinerant ferromagnet hosting momentum-space sources of Berry curvature, and LaAlO3, a polar wide-band-gap insulator. Transmission electron microscopy reveals an atomically sharp LaO/RuO2/SrO interface configuration, leading to excess charge being pinned near the LaAlO3/SrRuO3 interface. We demonstrate through magneto-optical characterization, theoretical calculations and transport measurements that the real-space charge reconstruction drives a reorganization of the topological charges in the band structure, thereby modifying the momentum-space Berry curvature in SrRuO3. Our results illustrate how the topological and magnetic features of oxides can be manipulated by engineering charge discontinuities at oxide interfaces. |
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Language | Wos | 000704665000010 | Publication Date | 2021-09-16 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0031-9007 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.462 | Times cited | 17 | Open Access | OpenAccess |
Notes | The authors thank E. Lesne, M. Lee, H. Barakov, M. Matthiesen and U. Filippozzi for discussions. The authors are grateful to E.J.S. van Thiel for producing the illustration in Fig. 4a. This work was supported by the European Research Council under the European Unions Horizon 2020 programme/ERC Grant agreements No. [677458], [770887] and No. [731473] (Quantox of QuantERA ERA-NET Cofund in Quantum Technologies) and by the Netherlands Organisation for Scientific Research (NWO/OCW) as part of the Frontiers of Nanoscience (NanoFront) and VIDI program. The authors acknowledge funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No. [823717] – ESTEEM3. N. G., J. V., and S. V. A. acknowledge funding from the University of Antwerp through the Concerted Research Actions (GOA) project Solarpaint and the TOP project. C. A. and W. B. are supported by the Foundation for Polish Science through the International Research Agendas program co-financed by the European Union within the Smart Growth Operational Programme. C. A. acknowledges access to the computing facilities of the Interdisciplinary Center of Modeling at the University of Warsaw, Grant No. G73-23 and G75-10. W.B. acknowledges support from the Narodowe Centrum Nauk (NCN, National Science Centre, Poland) Project No. 2019/34/E/ST3/00404'; esteem3TA; esteem3reported | Approved | Most recent IF: 8.462 | ||
Call Number | EMAT @ emat @c:irua:182595 | Serial | 6824 | ||
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Author | Jannis, D.; Hofer, C.; Gao, C.; Xie, X.; Béché, A.; Pennycook, Tj.; Verbeeck, J. | ||||
Title | Event driven 4D STEM acquisition with a Timepix3 detector: Microsecond dwell time and faster scans for high precision and low dose applications | Type | A1 Journal article | ||
Year | 2022 | Publication | Ultramicroscopy | Abbreviated Journal | Ultramicroscopy |
Volume | 233 | Issue | Pages | 113423 | |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | Four dimensional scanning transmission electron microscopy (4D STEM) records the scattering of electrons in a material in great detail. The benefits offered by 4D STEM are substantial, with the wealth of data it provides facilitating for instance high precision, high electron dose efficiency phase imaging via centre of mass or ptychography based analysis. However the requirement for a 2D image of the scattering to be recorded at each probe position has long placed a severe bottleneck on the speed at which 4D STEM can be performed. Recent advances in camera technology have greatly reduced this bottleneck, with the detection efficiency of direct electron detectors being especially well suited to the technique. However even the fastest frame driven pixelated detectors still significantly limit the scan speed which can be used in 4D STEM, making the resulting data susceptible to drift and hampering its use for low dose beam sensitive applications. Here we report the development of the use of an event driven Timepix3 direct electron camera that allows us to overcome this bottleneck and achieve 4D STEM dwell times down to 100 ns; orders of magnitude faster than what has been possible with frame based readout. We characterize the detector for different acceleration voltages and show that the method is especially well suited for low dose imaging and promises rich datasets without compromising dwell time when compared to conventional STEM imaging. | ||||
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Language | Wos | 000734396800003 | Publication Date | 2021-11-13 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0304-3991 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 2.2 | Times cited | 31 | Open Access | OpenAccess |
Notes | This project has received funding from the Euro- pean Union’s Horizon 2020 Research Infrastructure – Integrating Activities for Advanced Communities under grant agreement No 823717 – ESTEEM3. J.V. and A.B. acknowledge funding from FWO project G093417N (‘Compressed sensing enabling low dose imaging in transmission electron microscopy’). J.V. and D.J. ac- knowledge funding from FWO project G042920N ‘Co- incident event detection for advanced spectroscopy in transmission electron microscopy’. We acknowledge funding under the European Union’s Horizon 2020 re- search and innovation programme (J.V. and D.J un- der grant agreement No 101017720, FET-Proactive EBEAM, and C.H., C.G., X.X. and T.J.P. from the Eu- ropean Research Council (ERC) Grant agreement No. 802123-HDEM).; esteem3JRA; esteem3reported | Approved | Most recent IF: 2.2 | ||
Call Number | EMAT @ emat @c:irua:183948 | Serial | 6828 | ||
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Author | Chen, B.; Gauquelin, N.; Green, R.J.; Verbeeck, J.; Rijnders, G.; Koster, G. | ||||
Title | Asymmetric Interfacial Intermixing Associated Magnetic Coupling in LaMnO3/LaFeO3 Heterostructures | Type | A1 Journal article | ||
Year | 2021 | Publication | Frontiers in physics | Abbreviated Journal | Front. Phys. |
Volume | 9 | Issue | Pages | ||
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | The structural and magnetic properties of LaMnO<sub>3</sub>/LaFeO<sub>3</sub>(LMO/LFO) heterostructures are characterized using a combination of scanning transmission electron microscopy, electron energy-loss spectroscopy, bulk magnetometry, and resonant x-ray reflectivity. Unlike the relatively abrupt interface when LMO is deposited on top of LFO, the interface with reversed growth order shows significant cation intermixing of Mn<sup>3+</sup>and Fe<sup>3+</sup>, spreading ∼8 unit cells across the interface. The asymmetric interfacial chemical profiles result in distinct magnetic properties. The bilayer with abrupt interface shows a single magnetic hysteresis loop with strongly enhanced coercivity, as compared to the LMO plain film. However, the bilayer with intermixed interface shows a step-like hysteresis loop, associated with the separate switching of the “clean” and intermixed LMO sublayers. Our study illustrates the key role of interfacial chemical profile in determining the functional properties of oxide heterostructures. | ||||
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Language | Wos | 000745284500001 | Publication Date | 2021-12-14 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2296-424X | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | Times cited | 1 | Open Access | OpenAccess | |
Notes | This work is supported by the international M-ERA.NET project SIOX (project 4288) and H2020 project ULPEC (project 732642). The X-Ant-EM microscope and the direct electron detector were partly funded by the Hercules fund from the Flemish Government. NG and JV acknowledge funding from GOA project “Solarpaint” of the University of Antwerp. RG was supported by the Natural Sciences and Engineering Research Council of Canada (NSERC). Part of the research described in this paper was performed at the Canadian Light Source, a national research facility of the University of Saskatchewan, which is supported by the Canada Foundation for Innovation (CFI), NSERC, the National Research Council (NRC), the Canadian Institutes of Health Research (CIHR), the Government of Saskatchewan, and the University of Saskatchewan. | Approved | Most recent IF: NA | ||
Call Number | EMAT @ emat @c:irua:185176 | Serial | 6901 | ||
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Author | Chen, B.; Gauquelin, N.; Strkalj, N.; Huang, S.; Halisdemir, U.; Nguyen, M.D.; Jannis, D.; Sarott, M.F.; Eltes, F.; Abel, S.; Spreitzer, M.; Fiebig, M.; Trassin, M.; Fompeyrine, J.; Verbeeck, J.; Huijben, M.; Rijnders, G.; Koster, G. | ||||
Title | Signatures of enhanced out-of-plane polarization in asymmetric BaTiO3 superlattices integrated on silicon | Type | A1 Journal article | ||
Year | 2022 | Publication | Nature communications | Abbreviated Journal | Nat Commun |
Volume | 13 | Issue | 1 | Pages | 265 |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | In order to bring the diverse functionalities of transition metal oxides into modern electronics, it is imperative to integrate oxide films with controllable properties onto the silicon platform. Here, we present asymmetric LaMnO<sub>3</sub>/BaTiO<sub>3</sub>/SrTiO<sub>3</sub>superlattices fabricated on silicon with layer thickness control at the unit-cell level. By harnessing the coherent strain between the constituent layers, we overcome the biaxial thermal tension from silicon and stabilize<italic>c</italic>-axis oriented BaTiO<sub>3</sub>layers with substantially enhanced tetragonality, as revealed by atomically resolved scanning transmission electron microscopy. Optical second harmonic generation measurements signify a predominant out-of-plane polarized state with strongly enhanced net polarization in the tricolor superlattices, as compared to the BaTiO<sub>3</sub>single film and conventional BaTiO<sub>3</sub>/SrTiO<sub>3</sub>superlattice grown on silicon. Meanwhile, this coherent strain in turn suppresses the magnetism of LaMnO<sub>3</sub>as the thickness of BaTiO<sub>3</sub>increases. Our study raises the prospect of designing artificial oxide superlattices on silicon with tailored functionalities. | ||||
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Language | Wos | 000741852200073 | Publication Date | 2022-01-11 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2041-1723 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 16.6 | Times cited | 11 | Open Access | OpenAccess |
Notes | This project has received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement No 823717—ESTEEM3. B.C. is sponsored by Shanghai Sailing Program 21YF1410700. J.V. and N.G. acknowledge funding through the GOA project “Solarpaint” of the University of Antwerp. The microscope used in this work was partly funded by the Hercules Fund from the Flemish Government. D.J. acknowledges funding from FWO Project G093417N from the Flemish fund for scientific research. M.T., N.S., M.F.S. and M.F. acknowledge the financial support by the EU European Research Council (Advanced Grant 694955—INSEETO). M.T. acknowledges the Swiss National Science Foundation under Project No. 200021-188414. N.S. acknowledges support under the Swiss National Science Foundation under Project No. P2EZP2-199913. M.S. acknowledges funding from Slovenian Research Agency (Grants No. J2-2510, N2-0149 and P2-0091). B.C. acknowledges Prof. C.D.; Prof. F.Y.; Prof. B.T. and Dr. K.J. for valuable discussions.; esteem3reported; esteem3TA | Approved | Most recent IF: 16.6 | ||
Call Number | EMAT @ emat @c:irua:185179 | Serial | 6902 | ||
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Author | Park, D.-s.; Hadad, M.; Riemer, L.M.; Ignatans, R.; Spirito, D.; Esposito, V.; Tileli, V.; Gauquelin, N.; Chezganov, D.; Jannis, D.; Verbeeck, J.; Gorfman, S.; Pryds, N.; Muralt, P.; Damjanovic, D. | ||||
Title | Induced giant piezoelectricity in centrosymmetric oxides | Type | A1 Journal article | ||
Year | 2022 | Publication | Science | Abbreviated Journal | Science |
Volume | 375 | Issue | 6581 | Pages | 653-657 |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | Giant piezoelectricity can be induced in centrosymmetric oxides by controlling the long-range motion of oxygen vacancies. | ||||
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Language | Wos | 000753975300036 | Publication Date | 2022-02-11 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0036-8075 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 56.9 | Times cited | 51 | Open Access | OpenAccess |
Notes | D.-S.P., V.E., N.P., P.M., and D.D. acknowledge the European Commission for project Biowings H2020 Fetopen 2018-2022 (grant no. 80127). N.P. acknowledges funding from the Villum Fonden for the NEED project (grant no. 00027993) and the Danish Council for Independent Research Technology and Production Sciences for the DFF-Research Project 3 (grant no. 00069B). S.G. acknowledges funding from the Israel Science Foundation (research grant 1561/18 and equipment grant 2247/18). This project has received funding from the European Union’s Horizon 2020 research and innovation program under grant no. 823717 – ESTEEM3. D.C. acknowledges TOP/BOF funding of the University of Antwerp. M.H. and P.M. acknowledge funding from the Swiss National Science Foundation (grant nos. 200020-162664/1 and 200021-143424/1); esteem3reported; esteem3TA | Approved | Most recent IF: 56.9 | ||
Call Number | EMAT @ emat @c:irua:185876 | Serial | 6909 | ||
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Author | Monico, L.; Rosi, F.; Vivani, R.; Cartechini, L.; Janssens, K.; Gauquelin, N.; Chezganov, D.; Verbeeck, J.; Cotte, M.; D'Acapito, F.; Barni, L.; Grazia, C.; Buemi, L.P.; Andral, J.-L.; Miliani, C.; Romani, A. | ||||
Title | Deeper insights into the photoluminescence properties and (photo)chemical reactivity of cadmium red (CdS1-xSex) paints in renowned twentieth century paintings by state-of-the-art investigations at multiple length scales | Type | A1 Journal article | ||
Year | 2022 | Publication | The European Physical Journal Plus | Abbreviated Journal | Eur Phys J Plus |
Volume | 137 | Issue | 3 | Pages | 311 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT); Antwerp X-ray Imaging and Spectroscopy (AXIS) | ||||
Abstract | Cadmium red is the name used for denoting a class of twentieth century artists' pigments described by the general formula CdS1-xSex. For their vibrant hues and excellent covering power, a number of renowned modern and contemporary painters, including Jackson Pollock, often used cadmium reds. As direct band gap semiconductors, CdS1-xSex compounds undergo direct radiative recombination (with emissions from the green to orange region) and radiative deactivation from intragap trapping states due to crystal defects, which give rise to two peculiar red-NIR emissions, known as deep level emissions (DLEs). The positions of the DLEs mainly depend on the Se content of CdS1-xSex; thus, photoluminescence and diffuse reflectance vis-NIR spectroscopy have been profitably used for the non-invasive identification of different cadmium red varieties in artworks over the last decade. Systematic knowledge is however currently lacking on what are the parameters related to intrinsic crystal defects of CdS1-xSex and environmental factors influencing the spectral properties of DLEs as well as on the overall (photo)chemical reactivity of cadmium reds in paint matrixes. Here, we present the application of a novel multi-length scale and multi-method approach to deepen insights into the photoluminescence properties and (photo)chemical reactivity of cadmium reds in oil paintings by combining both well established and new non-invasive/non-destructive analytical techniques, including macro-scale vis-NIR and vibrational spectroscopies and micro-/nano-scale advanced electron microscopy mapping and X-ray methods employing synchrotron radiation and conventional sources. Macro-scale vis-NIR spectroscopy data obtained from the in situ non-invasive analysis of nine masterpieces by Gerardo Dottori, Jackson Pollock and Nicolas de Stael allowed classifying the CdS1-xSex-paints in three groups, according to the relative intensity of the two DLE bands. These outcomes, combined with results from micro-/nano-scale electron microscopy mapping and X-ray analysis of a set of CdS1-xSex powders and artificially aged paint mock-ups, indicated that the relative intensity of DLEs is not affected by the morphology, microstructure and local atomic environment of the pigment particles but it is influenced by the presence of moisture. Furthermore, the extensive study of artificially aged oil paint mock-ups permitted us to provide first evidence of the tendency of cadmium reds toward photo-degradation and to establish that the conversion of CdS1-xSex to CdSO4 and/or oxalates is triggered by the oil binding medium and moisture level and depends on the Se content. Based on these findings, we could interpret the localized presence of CdSO4 and cadmium oxalate as alteration products of the original cadmium red paints in two paintings by Pollock. | ||||
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Language | Wos | 000765807600002 | Publication Date | 0000-00-00 | |
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Series Volume | Series Issue | Edition | |||
ISSN | 2190-5444 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 3.4 | Times cited | 3 | Open Access | OpenAccess |
Notes | g The research was financially supported by the EU FP7 and Horizon 2020 Projects CHARISMA (FP7-INFRASTRUCTURES, GA No. 228330), IPERION-CH (H2020-INFRAIA-2014-2015, GA No. 654028), IPERION-HS (H2020-INFRAIA-2019-1, GA No. 871034) and ESTEEM3 (Research and innovation programme, GA No. 823717) and the Italian project AMIS (Dipartimenti di Eccellenza 2018–2022, funded by MIUR and Perugia University). For the beamtime grants received, we thank ESRF-ID21 (Experiment No. HG156 and in-house beamtimes) and the CERIC-ERIC Research Infrastructure for the investigations at ESRF-BM08 (LISA) beamline (Proposal Id: 20207042). D.C. acknowledges TOP/BOF funding of the University of Antwerp.; esteem3reported; esteem3TA | Approved | Most recent IF: 3.4 | ||
Call Number | UA @ admin @ c:irua:187375 | Serial | 7060 | ||
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Author | Zillner, J.; Boyen, H.-G.; Schulz, P.; Hanisch, J.; Gauquelin, N.; Verbeeck, J.; Kueffner, J.; Desta, D.; Eisele, L.; Ahlswede, E.; Powalla, M. | ||||
Title | The role of SnF₂ additive on interface formation in all lead-free FASnI₃ perovskite solar cells | Type | A1 Journal article | ||
Year | 2022 | Publication | Advanced functional materials | Abbreviated Journal | Adv Funct Mater |
Volume | Issue | Pages | 2109649-9 | ||
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | Tin-based perovskites are promising alternative absorber materials for leadfree perovskite solar cells but need strategies to avoid fast tin (Sn) oxidation. Generally, this reaction can be slowed down by the addition of tin fluoride (SnF2) to the perovskite precursor solution, which also improves the perovskite layer morphology. Here, this work analyzes the spatial distribution of the additive within formamidinium tin triiodide (FASnI(3)) films deposited on top of poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) hole transporting layers. Employing time-of-flight secondary ion mass spectrometry and a combination of hard and soft X-ray photoelectron spectroscopy, it is found that Sn F2 preferably accumulates at the PEDOT:PSS/perovskite interface, accompanied by the formation of an ultrathin SnS interlayer with an effective thickness of approximate to 1.2 nm. | ||||
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Language | Wos | 000779891000001 | Publication Date | 0000-00-00 | |
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ISSN | 1616-301x | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 19 | Times cited | 22 | Open Access | OpenAccess |
Notes | J.Z. and H.-G.B. contributed equally to this work. This project received funding from the European Union's Horizon 2020 research and innovation programme under grant agreement No. 850937 (PERCISTAND). H.-G.B. and D.D. are very grateful to the Research Foundation Flanders (FWO) for funding the HAXPES-lab instrument within the HERCULES program for Large Research Infrastructure of the Flemish government. P.S. thanks the French Agence Nationale de la Recherche for funding under the contract number ANR-17-MPGA-0012. This work was supported by the Federal Ministry for Economic Affairs and Energy (BMWi) Germany under the contract number 03EE1038A (CAPITANO) and financed by the Ministry of Science, Research and the Arts of Baden-Württemberg as part of the sustainability financing of the projects of the Excellence Initiative II (KSOP). | Approved | Most recent IF: 19 | ||
Call Number | UA @ admin @ c:irua:187969 | Serial | 7067 | ||
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Author | Yu, C.-P.; Friedrich, T.; Jannis, D.; Van Aert, S.; Verbeeck, J. | ||||
Title | Real-Time Integration Center of Mass (riCOM) Reconstruction for 4D STEM | Type | A1 Journal article | ||
Year | 2022 | Publication | Microscopy and microanalysis | Abbreviated Journal | Microsc Microanal |
Volume | Issue | Pages | 1-12 | ||
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | A real-time image reconstruction method for scanning transmission electron microscopy (STEM) is proposed. With an algorithm requiring only the center of mass of the diffraction pattern at one probe position at a time, it is able to update the resulting image each time a new probe position is visited without storing any intermediate diffraction patterns. The results show clear features at high spatial frequency, such as atomic column positions. It is also demonstrated that some common post-processing methods, such as band-pass filtering, can be directly integrated in the real-time processing flow. Compared with other reconstruction methods, the proposed method produces high-quality reconstructions with good noise robustness at extremely low memory and computational requirements. An efficient, interactive open source implementation of the concept is further presented, which is compatible with frame-based, as well as event-based camera/file types. This method provides the attractive feature of immediate feedback that microscope operators have become used to, for example, conventional high-angle annular dark field STEM imaging, allowing for rapid decision-making and fine-tuning to obtain the best possible images for beam-sensitive samples at the lowest possible dose. | ||||
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Language | Wos | 000792176100001 | Publication Date | 2022-04-25 | |
Series Editor | Series Title | Abbreviated Series Title | |||
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ISSN | 1431-9276 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 2.8 | Times cited | 7 | Open Access | OpenAccess |
Notes | Bijzonder Onderzoeksfonds UGent; H2020 European Research Council, 770887 ; H2020 European Research Council, 823717 ; H2020 European Research Council, ESTEEM3 / 823717 ; H2020 European Research Council, PICOMETRICS / 770887 ; Fonds Wetenschappelijk Onderzoek, 30489208 ; Herculesstichting; esteem3reported; esteem3jra | Approved | Most recent IF: 2.8 | ||
Call Number | EMAT @ emat @c:irua:188538 | Serial | 7068 | ||
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