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Author Jenkinson, K.; Spadaro, M.C.; Golovanova, V.; Andreu, T.; Morante, J.R.; Arbiol, J.; Bals, S.
  Title Direct operando visualization of metal support interactions induced by hydrogen spillover during CO₂ hydrogenation Type A1 Journal article
  Year (down) 2023 Publication Advanced materials Abbreviated Journal
  Volume 35 Issue 51 Pages 2306447-10
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
  Abstract The understanding of catalyst active sites is a fundamental challenge for the future rational design of optimized and bespoke catalysts. For instance, the partial reduction of Ce4+ surface sites to Ce3+ and the formation of oxygen vacancies are critical for CO2 hydrogenation, CO oxidation, and the water gas shift reaction. Furthermore, metal nanoparticles, the reducible support, and metal support interactions are prone to evolve under reaction conditions; therefore a catalyst structure must be characterized under operando conditions to identify active states and deduce structure-activity relationships. In the present work, temperature-induced morphological and chemical changes in Ni nanoparticle-decorated mesoporous CeO2 by means of in situ quantitative multimode electron tomography and in situ heating electron energy loss spectroscopy, respectively, are investigated. Moreover, operando electron energy loss spectroscopy is employed using a windowed gas cell and reveals the role of Ni-induced hydrogen spillover on active Ce3+ site formation and enhancement of the overall catalytic performance.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 001106139400001 Publication Date 2023-10-22
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN 0935-9648 ISBN Additional Links UA library record; WoS full record
  Impact Factor 29.4 Times cited Open Access OpenAccess
  Notes Approved Most recent IF: 29.4; 2023 IF: 19.791
  Call Number UA @ admin @ c:irua:201143 Serial 9022
Permanent link to this record
 

 
Author Rakesh Roshan, S.C.; Yedukondalu, N.; Pandey, T.; Kunduru, L.; Muthaiah, R.; Rajaboina, R.K.; Ehm, L.; Parise, J.B.
  Title Effect of atomic mass contrast on lattice thermal conductivity : a case study for alkali halides and alkaline-earth chalcogenides Type A1 Journal article
  Year (down) 2023 Publication ACS applied electronic materials Abbreviated Journal
  Volume 5 Issue 11 Pages 5852-5863
  Keywords A1 Journal article; Condensed Matter Theory (CMT)
  Abstract Lattice thermal conductivity (kappa(L)) is of great scientific interest for the development of efficient energy conversion technologies. Therefore, microscopic understanding of phonon transport is critically important for designing functional materials. In our previous study (Roshan et al., ACS Applied Energy Mater. 2021, 5, 882-896), anomalous kappa(L) trends were predicted for rocksalt alkaline-earth chalcogenides (AECs). In the present work, we extended it to alkali halides (AHs) and conducted a thorough investigation to explore the role of atomic mass contrast on lattice dynamics and phonon transport properties of 36 binary compounds (20 AHs + 16 AECs). The calculated spectral and cumulative kappa(L) reveal that low-lying optical phonon modes significantly boost kappa(L) alongside acoustic phonons in materials where the atomic mass ratio approaches unity and cophonocity nears zero. Phonon scattering rates are relatively low for materials with a mass ratio close to one, and the corresponding phonon lifetimes are higher, which enhances kappa(L). Phonon lifetimes play a critical role, outweighing phonon group velocities, in determining the anomalous trends in kappa(L) for both AHs and AECs. To further explore the role of atomic mass contrast in kappa(L), the effect of tensile lattice strain on phonon transport has also been investigated. Under tensile strain, both group velocities and phonon lifetimes decrease in the low frequency range, leading to a decrease in kappa(L). This work provides insights on how atomic mass contrast can tune the contribution of optical phonons to kappa(L) and its implications on scattering rates by either enhancing or suppressing kappa(L). These insights would aid in the selection of elements for designing new functional materials with and without atomic mass contrast to achieve relatively high and low kappa(L) values, respectively.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 001096792500001 Publication Date 2023-10-26
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN 2637-6113 ISBN Additional Links UA library record; WoS full record
  Impact Factor Times cited Open Access
  Notes Approved Most recent IF: NA
  Call Number UA @ admin @ c:irua:201198 Serial 9026
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Author Watson, G.; Kummamuru, N.B.; Verbruggen, S.W.; Perreault, P.; Houlleberghs, M.; Martens, J.; Breynaert, E.; Van Der Voort, P.
  Title Engineering of hollow periodic mesoporous organosilica nanorods for augmented hydrogen clathrate formation Type A1 Journal article
  Year (down) 2023 Publication Journal of materials chemistry A : materials for energy and sustainability Abbreviated Journal
  Volume 11 Issue 47 Pages 26265-26276
  Keywords A1 Journal article; Engineering sciences. Technology
  Abstract Hydrogen (H2) storage, in the form of clathrate hydrates, has emerged as an attractive alternative to classical storage methods like compression or liquefaction. Nevertheless, the sluggish enclathration kinetics along with low gas storage capacities in bulk systems is currently impeding the progress of this technology. To this end, unstirred systems coupled with porous materials have been shown to tackle the aforementioned drawbacks. In line with this approach, the present study explores the use of hydrophobic periodic organosilica nanoparticles, later denoted as hollow ring-PMO (HRPMO), for H2 storage as clathrate hydrates under mild operating conditions (5.56 mol% THF, 7 MPa, and 265–273 K). The surface of the HRPMO nanoparticles was carefully decorated/functionalized with THF-like moieties, which are well-known promoter agents in clathrate formation when applied in classical, homogeneous systems. The study showed that, while the non-functionalized HRPMO can facilitate the formation of binary H2-THF clathrates, the incorporation of surface-bound promotor structures enhances this process. More intriguingly, tuning the concentration of these surface-bound promotor agents on the HRPMO led to a notable effect on solid-state H2 storage capacities. An increase of 3% in H2 storage capacity, equivalent to 0.26 wt%, along with a substantial increase of up to 28% in clathrate growth kinetics, was observed when an optimal loading of 0.14 mmol g−1 of promoter agent was integrated into the HRPMO framework. Overall, the findings from this study highlight that such tuning effects in the solid-state have the potential to significantly boost hydrate formation/growth kinetics and H2 storage capacities, thereby opening new avenues for the ongoing development of H2 clathrates in industrial applications.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 001108752600001 Publication Date 2023-11-24
  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 Open Access
  Notes Approved Most recent IF: 11.9; 2023 IF: 8.867
  Call Number UA @ admin @ c:irua:201007 Serial 9031
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Author Manzaneda-Gonzalez, V.; Jenkinson, K.; Pena-Rodriguez, O.; Borrell-Grueiro, O.; Trivino-Sanchez, S.; Banares, L.; Junquera, E.; Espinosa, A.; Gonzalez-Rubio, G.; Bals, S.; Guerrero-Martinez, A.
  Title From multi- to single-hollow trimetallic nanocrystals by ultrafast heating Type A1 Journal article
  Year (down) 2023 Publication Chemistry of materials Abbreviated Journal
  Volume 35 Issue 22 Pages 9603-9612
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract Metal nanocrystals (NCs) display unique physicochemical features that are highly dependent on nanoparticle dimensions, anisotropy, structure, and composition. The development of synthesis methodologies that allow us to tune such parameters finely emerges as crucial for the application of metal NCs in catalysis, optical materials, or biomedicine. Here, we describe a synthetic methodology to fabricate hollow multimetallic heterostructures using a combination of seed-mediated growth routes and femtosecond-pulsed laser irradiation. The envisaged methodology relies on the coreduction of Ag and Pd ions on gold nanorods (Au NRs) to form Au@PdAg core-shell nanostructures containing small cavities at the Au-PdAg interface. The excitation of Au@PdAg NRs with low fluence femtosecond pulses was employed to induce the coalescence and growth of large cavities, forming multihollow anisotropic Au@PdAg nanostructures. Moreover, single-hollow alloy AuPdAg could be achieved in high yield by increasing the irradiation energy. Advanced electron microscopy techniques, energy-dispersive X-ray spectroscopy (EDX) tomography, X-ray absorption near-edge structure (XANES) spectroscopy, and finite differences in the time domain (FDTD) simulations allowed us to characterize the morphology, structure, and elemental distribution of the irradiated NCs in detail. The ability of the reported synthesis route to fabricate multimetallic NCs with unprecedented hollow nanostructures offers attractive prospects for the fabrication of tailored high-entropy alloy nanoparticles.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 001110623500001 Publication Date 2023-11-06
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN 0897-4756; 1520-5002 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 8.6 Times cited 2 Open Access OpenAccess
  Notes Approved Most recent IF: 8.6; 2023 IF: 9.466
  Call Number UA @ admin @ c:irua:202144 Serial 9040
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Author Hugenschmidt, M.; Jannis, D.; Kadu, A.A.; Grünewald, L.; De Marchi, S.; Perez-Juste, J.; Verbeeck, J.; Van Aert, S.; Bals, S.
  Title Low-dose 4D-STEM tomography for beam-sensitive nanocomposites Type A1 Journal article
  Year (down) 2023 Publication ACS materials letters Abbreviated Journal
  Volume 6 Issue 1 Pages 165-173
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract Electron tomography is essential for investigating the three-dimensional (3D) structure of nanomaterials. However, many of these materials, such as metal-organic frameworks (MOFs), are extremely sensitive to electron radiation, making it difficult to acquire a series of projection images for electron tomography without inducing electron-beam damage. Another significant challenge is the high contrast in high-angle annular dark field scanning transmission electron microscopy that can be expected for nanocomposites composed of a metal nanoparticle and an MOF. This strong contrast leads to so-called metal artifacts in the 3D reconstruction. To overcome these limitations, we here present low-dose electron tomography based on four-dimensional scanning transmission electron microscopy (4D-STEM) data sets, collected using an ultrafast and highly sensitive direct electron detector. As a proof of concept, we demonstrate the applicability of the method for an Au nanostar embedded in a ZIF-8 MOF, which is of great interest for applications in various fields, including drug delivery.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 001141178500001 Publication Date 2023-12-11
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN 2639-4979 ISBN Additional Links UA library record; WoS full record
  Impact Factor Times cited Open Access Not_Open_Access
  Notes This work was supported by the European Research Council (Grant 815128 REALNANO to S.B., Grant 770887 PICOMETRICS to S.V.A.). J.P.-J. and S.M. acknowledge financial support from the MCIN/AEI/10.13039/501100011033 (Grants No. PID2019-108954RB-I00) and EU Horizon 2020 research and innovation program under grant agreement no. 883390 (SERSing). J.V., S.B., S.V.A., and L.G. acknowledge funding from the Flemish government (iBOF-21-085 PERsist). Approved Most recent IF: NA
  Call Number UA @ admin @ c:irua:202771 Serial 9053
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Author Kumar, M.; Sengupta, A.; Kummamuru, N.B.
  Title Molecular simulations for carbon dioxide capture in silica slit pores Type A3 Journal article
  Year (down) 2023 Publication Materials Today: Proceedings Abbreviated Journal
  Volume Issue Pages 1-9
  Keywords A3 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
  Abstract In present work, we have performed the Grand Canonical Monte Carlo (GCMC) simulations to quantify CO2 capture inside porous silica at high operating temperatures of 673.15 K and 873.15 K; and over a operating pressure range of 500 kPa – 4000 kPa that are methane steam reforming process parameters. Related chemical potential values at these thermodynamic conditions are obtained from the bulk phase simulations in the Canonical ensemble in conjunction with Widom’s insertion technique, where the CO2 has been accurately represented by TraPPE force field. Present structure of the porous silica is a single slit pore geometry of various heights (H = 20 Å, 31.6 Å, 63.2 Å and 126.5 Å), dimensions in which possible vapour-liquid equilibria for generic square well fluids has been reported in literature. Estimation of the pore-fluid interactions show a higher interaction between silica pore and adsorbed CO2 compared to the reported pore-fluid interactions between homogeneous carbon slit pore and adsorbed CO2; thus resulting in an enhancement of adsorption inside silica pores of H = 20 Å and H = 126.5 Å, which are respectively 3.5 times and 1.5 times higher than that in homogeneous carbon slit pores of same dimensions and at 673.15 K and 500 kPa. Estimated local density plots indicate the presence of structured layers due to more molecular packing, which confirms possible liquid-like and vapour-like phase coexistence of the supercritical bulk phase CO2 under confinement.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos Publication Date 2023-05-06
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN 2214-7853 ISBN Additional Links UA library record
  Impact Factor Times cited Open Access
  Notes Approved Most recent IF: NA
  Call Number UA @ admin @ c:irua:200944 Serial 9058
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Author Li, H.; Pandey, T.; Jiang, Y.; Gu, X.; Lindsay, L.; Koh, Y.K.
  Title Origins of heat transport anisotropy in MoTe₂ and other bulk van der Waals materials Type A1 Journal article
  Year (down) 2023 Publication Materials Today Physics Abbreviated Journal
  Volume 37 Issue Pages 101196-101198
  Keywords A1 Journal article; Condensed Matter Theory (CMT)
  Abstract Knowledge of how heat flows anisotropically in van der Waals (vdW) materials is crucial for thermal management of emerging 2D materials devices and design of novel anisotropic thermoelectric materials. Despite the importance, anisotropic heat transport in vdW materials is yet to be systematically studied and is often presumably attributed to anisotropic speeds of sound in vdW materials due to soft interlayer bonding relative to covalent in-plane networks of atoms. In this work, we investigate the origins of the anisotropic heat transport in vdW materials, through time-domain thermoreflectance (TDTR) measurements and first-principles calculations of anisotropic thermal conductivity of three different phases of MoTe2. MoTe2 is ideal for the study due to its weak anisotropy in the speeds of sound. We find that even when the speeds of sound are roughly isotropic, the measured thermal conductivity of MoTe2 along the c-axis is 5-8 times lower than that along the in-plane axes. We derive meaningful characteristic heat capacity, phonon group velocity, and relaxation times from our first principles calculations for selected vdW materials (MoTe2, BP, h-BN, and MoS2), to assess the contributions of these factors to the anisotropic heat transport. Interestingly, we find that the main contributor to the heat transport anisotropy in vdW materials is anisotropy in heat capacity of the dominant heat-carrying phonon modes in different directions, which originates from anisotropic optical phonon dispersion and disparity in the frequency of heat-carrying phonons in different directions. The discrepancy in frequency of the heat-carrying phonons also leads to similar to 2 times larger average relaxation times in the cross-plane direction, and partially explains the apparent dependence of the anisotropic heat transport on the anisotropic speeds of sound. This work provides insight into understanding of the anisotropic heat transport in vdW materials.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 001093005700001 Publication Date 2023-08-09
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN 2542-5293 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 11.5 Times cited Open Access
  Notes Approved Most recent IF: 11.5; 2023 IF: NA
  Call Number UA @ admin @ c:irua:201295 Serial 9070
Permanent link to this record
 

 
Author Souza, J.C.B.; Vizarim, N.P.; Reichhardt, C.J.O.; Reichhardt, C.; Venegas, P.A.
  Title Soliton motion induced along ferromagnetic skyrmion chains in chiral thin nanotracks Type A1 Journal article
  Year (down) 2023 Publication Journal of magnetism and magnetic materials Abbreviated Journal
  Volume 587 Issue Pages 171280-171289
  Keywords A1 Journal article; Condensed Matter Theory (CMT)
  Abstract Using atomistic magnetic simulations we investigate the soliton motion along a pinned skyrmion chain containing an interstitial skyrmion. We find that the soliton can exhibit stable motion along the chain without a skyrmion Hall effect for an extended range of drives. Under a constant drive the solitons have a constant velocity. We also measure the skyrmion velocity-current curves and identify the signatures of different phases including a pinned phase, stable soliton motion, and quasi-free motion at higher drives where all of the skyrmions depin from the pinning centers and move along the rigid wall. In the quasi-free motion regime, the velocity is oscillatory due to the motion of the skyrmions over the pinning sites. For increasing pinning strength, the onset of soliton motion shifts to higher values of current density. We also find that for stronger pinning, the characteristic velocity-current shape is affected by the annihilation of single or multiple skyrmions in the drive interval over which the soliton motion occurs. Our results indicate that stable skyrmion soliton motion is possible and that the solitons could be used as information carriers instead of the skyrmions themselves for technological applications.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 001086712600001 Publication Date 2023-09-21
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN 0304-8853 ISBN Additional Links UA library record; WoS full record
  Impact Factor 2.7 Times cited Open Access
  Notes Approved Most recent IF: 2.7; 2023 IF: 2.63
  Call Number UA @ admin @ c:irua:201139 Serial 9095
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Author Xiao, H.; Zhang, Z.; Xu, W.; Wang, Q.; Xiao, Y.; Ding, L.; Huang, J.; Li, H.; He, B.; Peeters, F.M.
  Title Terahertz optoelectronic properties of synthetic single crystal diamond Type A1 Journal article
  Year (down) 2023 Publication Diamond and related materials Abbreviated Journal
  Volume 139 Issue Pages 110266-110268
  Keywords A1 Journal article; Condensed Matter Theory (CMT)
  Abstract A systematic investigation is undertaken for studying the optoelectronic properties of single crystal diamond (SCD) grown by microwave plasma chemical vapor deposition (MPCVD). It is indicated that, without intentional doping and surface treatment during the sample growth, the terahertz (THz) optical conduction in SCD is mainly affected by surface H-terminations, -OH-, O- and N-based functional groups. By using THz time-domain spectroscopy (TDS), we measure the transmittance, the complex dielectric constant and optical conductivity σ(ω) of SCD. We find that SCD does not show typical semiconductor characteristics in THz regime, where σ(ω) cannot be described rightly by the conventional Drude formula. Via fitting the real and imaginary parts of σ(ω) to the Drude-Smith formula, the ratio of the average carrier density to the effective electron mass γ = ne/m*, the electronic relaxation time τ and the electronic backscattering or localization factor can be determined optically. The temperature dependence of these parameters is examined. From the temperature dependence of γ, a metallic to semiconductor transition is observed at about T = 10 K. The temperature dependence of τ is mainly induced by electron coupling with acoustic-phonons and there is a significant effect of photon-induced electron backscattering or localization in SCD. This work demonstrates that THz TDS is a powerful technique in studying SCD which contains H-, N- and O-based bonds and has low electron density and high dc resistivity. The results obtained from this study can benefit us to gain an in-depth understanding of SCD and may provide new guidance for the application of SCD as electronic, optical and optoelectronic materials.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos Publication Date 2023-08-02
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN 0925-9635 ISBN Additional Links UA library record
  Impact Factor 4.1 Times cited Open Access
  Notes Approved Most recent IF: 4.1; 2023 IF: 2.561
  Call Number UA @ admin @ c:irua:200920 Serial 9103
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Author Salzmann, B.B.V.; Wit, J. de; Li, C.; Arenas-Esteban, D.; Bals, S.; Meijerink, A.; Vanmaekelbergh, D.
  Title Two-Dimensional CdSe-PbSe Heterostructures and PbSe Nanoplatelets: Formation, Atomic Structure, and Optical Properties Type A1 Journal article
  Year (down) 2022 Publication The journal of physical chemistry: C : nanomaterials and interfaces Abbreviated Journal J Phys Chem C
  Volume 126 Issue 3 Pages 1513-1522
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
  Abstract
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000744909200001 Publication Date 2022-01-27
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN 1932-7447 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 3.7 Times cited 12 Open Access OpenAccess
  Notes H. Meeldijk is kindly acknowledged for helping with electron microscopy at Utrecht University. T. Prins is kindly acknowledged for useful discussions. B.B.V.S. and D.V. acknowledge the Dutch NWO for financial support via the TOP-ECHO Grant No. 715.016.002. D.V. acknowledges financial support from the European ERC Council, ERC Advanced Grant 692691 “First Step”. J.W. and A.M. acknowledge financial support from the project CHEMIE.PGT.2019.004 of TKI/ Topsector Chemie, which is partly financed by the Dutch NWO. S.B, C.L., and D.A.E. acknowledge financial support from the European ERC Council, ERC Consolidator Grant realnano No. 815128. This project has received funding from the European Union’s Horizon 2020 research and innovation program under Grant No. 731019 (EUSMI). sygmaSB Approved Most recent IF: 3.7
  Call Number EMAT @ emat @c:irua:185454 Serial 6953
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Author Heyvaert, W.; Pedrazo-Tardajos, A.; Kadu, A.; Claes, N.; González-Rubio, G.; Liz-Marzán, L.M.; Albrecht, W.; Bals, S.
  Title Quantification of the Helical Morphology of Chiral Gold Nanorods Type A1 Journal article
  Year (down) 2022 Publication ACS materials letters Abbreviated Journal ACS Materials Lett.
  Volume 4 Issue Pages 642-649
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract Chirality in inorganic nanoparticles and nanostructures has gained increasing scientific interest, because of the possibility to tune their ability to interact differently with left- and right-handed circularly polarized light. In some cases, the optical activity is hypothesized to originate from a chiral morphology of the nanomaterial. However, quantifying the degree of chirality in objects with sizes of tens of nanometers is far from straightforward. Electron tomography offers the possibility to faithfully retrieve the three-dimensional morphology of nanomaterials, but only a qualitative interpretation of the morphology of chiral nanoparticles has been possible so far. We introduce herein a methodology that enables us to quantify the helicity of complex chiral nanomaterials, based on the geometrical properties of a helix. We demonstrate that an analysis at the single particle level can provide significant insights into the origin of chiroptical properties.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000784490000013 Publication Date 2022-03-08
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN 2639-4979 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor Times cited 11 Open Access OpenAccess
  Notes S.B. and A.P.-T. gratefully acknowledge funding by the European Research Council (ERC Consolidator Grant #815128-REALNANO) the European Union’s Horizon 2020 research and innovation program under grant agreement #823717ESTEEM3. L.M.L.-M. acknowledges funding from MCIN/ AEI /10.13039/501100011033, grant # PID2020- 117779RB-I00 and the Maria de Maeztu Units of Excellence Program from the Spanish State Research Agency (Grant No. MDM-2017-0720). G.G.-R. thanks the Spanish Spanish Ministerio de Ciencia e Innovación for an FPI (BES-2014- 068972) fellowship.; SygmaSB; esteem3reported; esteem3jra Approved Most recent IF: NA
  Call Number EMAT @ emat @c:irua:186959 Serial 6956
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Author Meng, X.; Chen, S.; Peng, H.; Bai, H.; Zhang, S.; Su, X.; Tan, G.; Van Tendeloo, G.; Sun, Z.; Zhang, Q.; Tang, X.; Wu, J.
  Title Ferroelectric engineering : enhanced thermoelectric performance by local structural heterogeneity Type A1 Journal article
  Year (down) 2022 Publication Science China : materials Abbreviated Journal Sci China Mater
  Volume Issue Pages
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract Although traditional ferroelectric materials are usually dielectric and nonconductive, GeTe is a typical ferroelectric semiconductor, possessing both ferroelectric and semiconducting properties. GeTe is also a widely studied thermoelectric material, whose performance has been optimized by doping with various elements. However, the impact of the ferroelectric domains on the thermoelectric properties remains unclear due to the difficulty to directly observe the ferroelectric domains and their evolutions under actual working conditions where the material is exposed to high temperatures and electric currents. Herein, based on in-situ investigations of the ferroelectric domains and domain walls in both pure and Sb-doped GeTe crystals, we have been able to analyze the dynamic evolution of the ferroelectric domains and domain walls, exposed to an electric field and temperature. Local structural heterogeneities and nano-sized ferroelectric domains are generated due to the interplay of the Sb3+ dopant and the Ge-vacancies, leading to the increased number of charged domain walls and a much improved thermoelectric performance. This work reveals the fundamental mechanism of ferroelectric thermoelectrics and provides insights into the decoupling of previously interdependent properties such as thermo-power and electrical conductivity.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000749973500001 Publication Date 2022-02-02
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN 2095-8226; 2199-4501 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 8.1 Times cited Open Access Not_Open_Access
  Notes Approved Most recent IF: 8.1
  Call Number UA @ admin @ c:irua:186429 Serial 6959
Permanent link to this record
 

 
Author Lu, W.; Cui, W.; Zhao, W.; Lin, W.; Liu, C.; Van Tendeloo, G.; Sang, X.; Zhao, W.; Zhang, Q.
  Title In situ atomistic insight into magnetic metal diffusion across Bi0.5Sb1.5Te3 quintuple layers Type A1 Journal article
  Year (down) 2022 Publication Advanced Materials Interfaces Abbreviated Journal Adv Mater Interfaces
  Volume Issue Pages 2102161
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract Diffusion and occupancy of magnetic atoms in van der Waals (VDW) layered materials have significant impact on applications such as energy storage, thermoelectrics, catalysis, and topological phenomena. However, due to the weak VDW bonding, most research focus on in-plane diffusion within the VDW gap, while out-of-plane diffusion has rarely been reported. Here, to investigate out-of-plane diffusion in VDW-layered Bi2Te3-based alloys, a Ni/Bi0.5Sb1.5Te3 heterointerface is synthesized by depositing magnetic Ni metal on a mechanically exfoliated Bi0.5Sb1.5Te3 (0001) substrate. Diffusion of Ni atoms across the Bi0.5Sb1.5Te3 quintuple layers is directly observed at elevated temperatures using spherical-aberration-corrected scanning transmission electron microscopy (STEM). Density functional theory calculations demonstrate that the diffusion energy barrier of Ni atoms is only 0.31-0.45 eV when they diffuse through Te-3(Bi, Sb)(3) octahedron chains. Atomic-resolution in situ STEM reveals that the distortion of the Te-3(Bi, Sb)(3) octahedron, induced by the Ni occupancy, drives the formation of coherent NiM (M = Bi, Sb, Te) at the heterointerfaces. This work can lead to new strategies to design novel thermoelectric and topological materials by introducing magnetic dopants to VDW-layered materials.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000751742300001 Publication Date 2022-02-07
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN 2196-7350 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 5.4 Times cited Open Access Not_Open_Access
  Notes Approved Most recent IF: 5.4
  Call Number UA @ admin @ c:irua:186421 Serial 6960
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Author Missen, O.P.; Mills, S.J.; Canossa, S.; Hadermann, J.; Nenert, G.; Weil, M.; Libowitzky, E.; Housley, R.M.; Artner, W.; Kampf, A.R.; Rumsey, M.S.; Spratt, J.; Momma, K.; Dunstan, M.A.
  Title Polytypism in mcalpineite : a study of natural and synthetic Cu₃TeO₆ Type A1 Journal article
  Year (down) 2022 Publication Acta Crystallographica. Section B: Structural Science, Crystal Engineering and Materials (Online) Abbreviated Journal Acta Crystallogr B
  Volume 78 Issue 1 Pages
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract Synthetic and naturally occurring forms of tricopper orthotellurate, (Cu3TeO6)-Te-II-O-IV (the mineral mcalpineite) have been investigated by 3D electron diffraction (3D ED), X-ray powder diffraction (XRPD), Raman and infrared (IR) spectroscopic measurements. As a result of the diffraction analyses, (Cu3TeO6)-Te-II-O-IV is shown to occur in two polytypes. The higher-symmetric (Cu3TeO6)-Te-II-O-IV-1C polytype is cubic, space group 1a (3) over bar, with a = 9.537 (1) angstrom and V = 867.4 (3) angstrom(3) as reported in previous studies. The 1C polytype is a well characterized structure consisting of alternating layers of (CuO6)-O-II octahedra and both (CuO6)-O-II and (TeO6)-O-VI octahedra in a patchwork arrangement. The structure of the lower-symmetric orthorhombic (Cu3TeO6)-Te-II-O-IV-2O polytype was determined for the first time in this study by 3D ED and verified by Rietveld refinement. The 2O polytype crystallizes in space group Pcca, with a = 9.745 (3) angstrom, b = 9.749 (2) angstrom, c = 9.771 (2) angstrom and V = 928.3 (4) angstrom(3) . High-precision XRPD data were also collected on (Cu3TeO6)-Te-II-O-IV-2O to verify the lower-symmetric structure by performing a Rietveld refinement. The resultant structure is identical to that determined by 3D ED, with unit-cell parameters a = 9.56157 (19) angstrom, b = 9.55853 (11) angstrom, c = 9.62891 (15) angstrom and V = 880.03 (2) angstrom(3) . The lower symmetry of the 2O polytype is a consequence of a different cation ordering arrangement, which involves the movement of every second (CuO6)-O-II and (TeO6)-O-VI octahedral layer by (1/4, 1/4, 0), leading to an offset of (TeO6)-O-VI and (CuO6)-O-II octahedra in every second layer giving an ABAB* stacking arrangement. Syntheses of (Cu3TeO6)-Te-II-O-IV showed that low-temperature (473 K) hydrothermal conditions generally produce the 2O polytype. XRPD measurements in combination with Raman spectroscopic analysis showed that most natural mcalpineite is the orthorhombic 2O polytype. Both XRPD and Raman spectroscopy measurements may be used to differentiate between the two polytypes of (Cu3TeO6)-Te-II-O-IV. In Raman spectroscopy, (Cu3TeO6)-Te-II-O-IV-1C has a single strong band around 730 cm(-1), whereas (Cu3TeO6)-Te-II-O-IV-2O shows a broad double maximum with bands centred around 692 and 742 cm(-1).
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000752899700003 Publication Date 2022-01-18
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN 2052-5206 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 1.9 Times cited Open Access OpenAccess
  Notes Approved Most recent IF: 1.9
  Call Number UA @ admin @ c:irua:186529 Serial 6962
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Author Pandey, T.; Peeters, F.M.; Milošević, M.V.
  Title Pivotal role of magnetic ordering and strain in lattice thermal conductivity of chromium-trihalide monolayers Type A1 Journal article
  Year (down) 2022 Publication 2D materials Abbreviated Journal 2D Mater
  Volume 9 Issue 1 Pages 015034
  Keywords A1 Journal article; Condensed Matter Theory (CMT)
  Abstract Understanding the coupling between spin and phonons is critical for controlling the lattice thermal conductivity (kappa ( l )) in magnetic materials, as we demonstrate here for CrX3 (X = Br and I) monolayers. We show that these compounds exhibit large spin-phonon coupling (SPC), dominated by out-of-plane vibrations of Cr atoms, resulting in significantly different phonon dispersions in ferromagnetic (FM) and paramagnetic (PM) phases. Lattice thermal conductivity calculations provide additional evidence for strong SPC, where particularly large kappa ( l ) is found for the FM phase. Most strikingly, PM and FM phases exhibit radically different behavior with tensile strain, where kappa ( l ) increases with strain for the PM phase, and strongly decreases for the FM phase-as we explain through analysis of phonon lifetimes and scattering rates. Taken all together, we uncover the high significance of SPC on the phonon transport in CrX3 monolayers, a result extendable to other 2D magnetic materials, that will be useful in further design of thermal spin devices.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000735170300001 Publication Date 2021-12-13
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN 2053-1583 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 5.5 Times cited 2 Open Access Not_Open_Access
  Notes Approved Most recent IF: 5.5
  Call Number UA @ admin @ c:irua:184642 Serial 7010
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Author Chaves, A.; Covaci, L.; Peeters, F.M.; Milošević, M.V.
  Title Topologically protected moiré exciton at a twist-boundary in a van der Waals heterostructure Type A1 Journal article
  Year (down) 2022 Publication 2D materials Abbreviated Journal 2D Mater
  Volume 9 Issue 2 Pages 025012
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT)
  Abstract A twin boundary in one of the layers of a twisted van der Waals heterostructure separates regions with near opposite inter-layer twist angles. In a MoS<sub>2</sub>/WSe<sub>2</sub>bilayer, the regions with<inline-formula><tex-math><?CDATA $Rh^h$?></tex-math><math overflow=“scroll”><msubsup><mi>R</mi><mi>h</mi><mi>h</mi></msubsup></math><inline-graphic href=“tdmac529dieqn1.gif” type=“simple” /></inline-formula>and<inline-formula><tex-math><?CDATA $Rh^X$?></tex-math><math overflow=“scroll”><msubsup><mi>R</mi><mi>h</mi><mi>X</mi></msubsup></math><inline-graphic href=“tdmac529dieqn2.gif” type=“simple” /></inline-formula>stacking registry that defined the sub-lattices of the moiré honeycomb pattern would be mirror-reflected across such a twist boundary. In that case, we demonstrate that topologically protected chiral moiré exciton states are confined at the twist boundary. These are one-dimensional and uni-directional excitons with opposite velocities for excitons composed by electronic states with opposite valley/spin character, enabling intrinsic, guided, and far reaching valley-polarized exciton currents.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000760518100001 Publication Date 2022-04-01
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN 2053-1583 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 5.5 Times cited 3 Open Access OpenAccess
  Notes Fonds Wetenschappelijk Onderzoek; Conselho Nacional de Desenvolvimento Científico e Tecnológico, PQ ; Approved Most recent IF: 5.5
  Call Number CMT @ cmt @c:irua:187124 Serial 7046
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Author Sevik, C.; Bekaert, J.; Petrov, M.; Milošević, M.V.
  Title High-temperature multigap superconductivity in two-dimensional metal borides Type A1 Journal article
  Year (down) 2022 Publication Physical review materials Abbreviated Journal Phys. Rev. Materials
  Volume 6 Issue 2 Pages 024803
  Keywords A1 Journal article; Condensed Matter Theory (CMT)
  Abstract
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000766666300003 Publication Date 2022-02-28
  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 4 Open Access Not_Open_Access
  Notes Universiteit Antwerpen; Türkiye Bilimsel ve Teknolojik Araştirma Kurumu, COST-118F187 ; Air Force Office of Scientific Research, FA9550-19-1-7048 ; Fonds Wetenschappelijk Onderzoek; Approved Most recent IF: 3.4
  Call Number CMT @ cmt @c:irua:187126 Serial 7047
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Author Menezes, R.M.; Šabani, D.; Bacaksiz, C.; de Souza Silva, C.C.; Milošević, M.V.
  Title Tailoring high-frequency magnonics in monolayer chromium trihalides Type A1 Journal article
  Year (down) 2022 Publication 2D materials Abbreviated Journal 2D Mater
  Volume 9 Issue 2 Pages 025021
  Keywords A1 Journal article; Condensed Matter Theory (CMT)
  Abstract Monolayer chromium-trihalides, the archetypal two-dimensional (2D) magnetic materials, are readily suggested as a promising platform for high-frequency magnonics. Here we detail the spin-wave properties of monolayer CrBr<sub>3</sub>and CrI<sub>3</sub>, using spin-dynamics simulations parametrized from the first principles. We reveal that spin-wave dispersion can be tuned in a broad range of frequencies by strain, paving the way towards flexo-magnonic applications. We further show that ever-present halide vacancies in these monolayers host sufficiently strong Dzyaloshinskii-Moriya interaction to scatter spin-waves, which promotes design of spin-wave guides by defect engineering. Finally we discuss the spectra of spin-waves propagating across a moiré-periodic modulation of magnetic parameters in a van der Waals heterobilayer, and show that the nanoscale moiré periodicities in such samples are ideal for realization of a magnonic crystal in the terahertz frequency range. Recalling the additional tunability of magnetic 2D materials by electronic gating, our results situate these systems among the front-runners for prospective high-frequency magnonic applications.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000771735500001 Publication Date 2022-04-01
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN 2053-1583 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 5.5 Times cited Open Access OpenAccess
  Notes Fundação de Amparo à Ciência e Tecnologia do Estado de Pernambuco; Special Research Funds of the University of Antwerp; Conselho Nacional de Desenvolvimento Científico e Tecnológico; Fonds Wetenschappelijk Onderzoek; Coordenação de Aperfeiçoamento de Pessoal de Nível Superior; Approved Most recent IF: 5.5
  Call Number CMT @ cmt @c:irua:187125 Serial 7048
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Author Idrissi, H.; Carrez, P.; Cordier, P.
  Title On amorphization as a deformation mechanism under high stresses Type A1 Journal article
  Year (down) 2022 Publication Current opinion in solid state and materials science Abbreviated Journal Curr Opin Solid St M
  Volume 26 Issue 1 Pages 100976-17
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract In this paper we review the work related to amorphization under mechanical stress. Beyond pressure, we highlight the role of deviatoric or shear stresses. We show that the most recent works make amorphization appear as a deformation mechanism in its own right, in particular under extreme conditions (shocks, deformations under high stresses, high strain-rates).
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000779433300002 Publication Date 2022-01-13
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN 1359-0286 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 11 Times cited Open Access OpenAccess
  Notes Approved Most recent IF: 11
  Call Number UA @ admin @ c:irua:188014 Serial 7064
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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 (down) 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.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000779891000001 Publication Date 0000-00-00
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  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 Sun, C.; Street, M.; Zhang, C.; Van Tendeloo, G.; Zhao, W.; Zhang, Q.
  Title Boron structure evolution in magnetic Cr₂O₃ thin films Type A1 Journal article
  Year (down) 2022 Publication Materials Today Physics Abbreviated Journal
  Volume 27 Issue Pages 100753-100757
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract B substituting O in antiferromagnetic Cr2O3 is known to increase the Ne ' el temperature, whereas the actual B dopant site and the corresponding functionality remains unclear due to the complicated local structure. Herein, A combination of electron energy loss spectroscopy and first-principles calculations were used to unveil B local structures in B doped Cr2O3 thin films. B was found to form either magnetic active BCr4 tetrahedra or various inactive BO3 triangles in the Cr2O3 lattice, with a* and z* bonds exhibiting unique spectral features. Identification of BO3 triangles was achieved by changing the electron momentum transfer to manipulate the differential cross section for the 1s-z* and 1s-a* transitions. Modeling the experimental spectra as a linear combination of simulated B K edges reproduces the experimental z* / a* ratios for 15-42% of the B occupying the active BCr4 structure. This result is further supported by first-principles based thermodynamic calculations.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000827323200003 Publication Date 2022-06-09
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN 2542-5293 ISBN Additional Links UA library record; WoS full record
  Impact Factor 11.5 Times cited Open Access OpenAccess
  Notes Approved Most recent IF: 11.5
  Call Number UA @ admin @ c:irua:189660 Serial 7078
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Author Poulain, R.; Lumbeeck, G.; Hunka, J.; Proost, J.; Savolainen, H.; Idrissi, H.; Schryvers, D.; Gauquelin, N.; Klein, A.
  Title Electronic and chemical properties of nickel oxide thin films and the intrinsic defects compensation mechanism Type A1 Journal article
  Year (down) 2022 Publication ACS applied electronic materials Abbreviated Journal
  Volume 4 Issue 6 Pages 2718-2728
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract Although largely studied, contradictory results on nickel oxide (NiO) properties can be found in the literature. We herein propose a comprehensive study that aims at leveling contradictions related to NiO materials with a focus on its conductivity, surface properties, and the intrinsic charge defects compensation mechanism with regards to the conditions preparation. The experiments were performed by in situ photo-electron spectroscopy, electron energy loss spectroscopy, and optical as well as electrical measurements on polycrystalline NiO thin films prepared under various preparation conditions by reactive sputtering. The results show that surface and bulk properties were strongly related to the deposition temperature with in particular the observation of Fermi level pinning, high work function, and unstable oxygen-rich grain boundaries for the thin films produced at room temperature but not at high temperature (>200 degrees C). Finally, this study provides substantial information about surface and bulk NiO properties enabling to unveil the origin of the high electrical conductivity of room temperature NiO thin films and also for supporting a general electronic charge compensation mechanism of intrinsic defects according to the deposition temperature.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000819431200001 Publication Date 2022-06-07
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN 2637-6113 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor Times cited Open Access Not_Open_Access
  Notes Approved Most recent IF: NA
  Call Number UA @ admin @ c:irua:189555 Serial 7081
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Author Vishwakarma, M.; Batra, Y.; Hadermann, J.; Singh, A.; Ghosh, A.; Mehta, B.R.
  Title Exploring the role of graphene oxide as a co-catalyst in the CZTS photocathodes for improved photoelectrochemical properties Type A1 Journal article
  Year (down) 2022 Publication ACS applied energy materials Abbreviated Journal
  Volume 5 Issue 6 Pages 7538-7549
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
  Abstract The hydrogen evolution properties of CZTS heterostructure photocathodes are reported with graphene oxide (GO) as a co-catalyst layer coated by a drop-cast method and an Al2O3 protection layer fabricated using atomic layer deposition. In the CZTS absorber, a minor deviation from stoichiometry across the cross section of the thin film results in nanoscale growth of spurious phases, but the kesterite phase remains the dominant phase. We have investigated the band alignment parameters such as the band gap, work function, and Fermi level position that are crucial for making kesterite-based heterostructure devices. The photocurrent density in the photocathode CZTS/CdS/ZnO is found to be improved to -4.71 mAmiddotcm(-2) at -0.40 V-RHE, which is 3 times that of the pure CZTS. This enhanced photoresponse can be attributed to faster carrier separation at p-n junction regions driven by upward band bending at CZTS grain boundaries and the ZnO layer. GO as a co-catalyst over the heterostructure photocathode significantly improves the photocurrent density to -6.14 mAmiddotcm(-2) at -0.40 V-RHE by effective charge migration in the CZTS/CdS/ZnO/GO configuration, but the onset potential shifts only after application of the Al2O3 protection layer. Significant photocurrents of -29 mAmiddotcm(-2) at -0.40 V-RHE and -8 mAmiddotcm(-2) at 0 V-RHE are observed, with an onset potential of 0.7 V-RHE in CZTS/CdS/ZnO/GO/Al2O3. The heterostructure configuration and the GO co-catalyst reduce the charge-transfer resistance, while the Al2O3 top layer provides a stable photocurrent for a prolonged time (similar to 16 h). The GO co-catalyst increases the flat band potential from 0.26 to 0.46 V-RHE in CZTS/CdS/ZnO/GO, which supports the bias-induced band bending at the electrolyte-electrode interface.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000820418400001 Publication Date 2022-05-24
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN 2574-0962 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 6.4 Times cited Open Access Not_Open_Access
  Notes Approved Most recent IF: 6.4
  Call Number UA @ admin @ c:irua:189666 Serial 7082
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Author Hao, Y.; Velpula, G.; Kaltenegger, M.; Bodlos, W.R.; Vibert, F.; Mali, K.S.; De Feyter, S.; Resel, R.; Geerts, Y.H.; Van Aert, S.; Beljonne, D.; Lazzaroni, R.
  Title From 2D to 3D : bridging self-assembled monolayers to a substrate-induced polymorph in a molecular semiconductor Type A1 Journal article
  Year (down) 2022 Publication Chemistry of materials Abbreviated Journal Chem Mater
  Volume 34 Issue 5 Pages 2238-2248
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract In this study, a new bottom-up approach is proposed to predict the crystal structure of the substrate-induced polymorph (SIP) of an archetypal molecular semiconductor. In spite of intense efforts, the formation mechanism of SIPs is still not fully understood, and predicting their crystal structure is a very delicate task. Here, we selected lead phthalocyanine (PbPc) as a prototypical molecular material because it is a highly symmetrical yet nonplanar molecule and we demonstrate that the growth and crystal structure of the PbPc SIPs can be templated by the corresponding physisorbed self-assembled molecular networks (SAMNs). Starting from SAMNs of PbPc formed at the solution/graphite interface, the structural and energetic aspects of the assembly were studied by a combination of in situ scanning tunneling microscopy and multiscale computational chemistry approach. Then, the growth of a PbPc SIP on top of the physisorbed monolayer was modeled without prior experimental knowledge, from which the crystal structure of the SIP was predicted. The theoretical prediction of the SIP was verified by determining the crystal structure of PbPc thin films using X-ray diffraction techniques, revealing the formation of a new polymorph of PbPc on the graphite substrate. This study clearly illustrates the correlation between the SAMNs and SIPs, which are traditionally considered as two separate but conceptually connected research areas. This approach is applicable to molecular materials in general to predict the crystal structure of their SIPs.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000812125800001 Publication Date 2022-02-17
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN 0897-4756; 1520-5002 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 8.6 Times cited Open Access Not_Open_Access
  Notes Approved Most recent IF: 8.6
  Call Number UA @ admin @ c:irua:189086 Serial 7084
Permanent link to this record
 

 
Author Penders, A.G.; Konstantinovic, M.J.; Yang, T.; Bosch, R.-w.; Schryvers, D.; Somville, F.
  Title Microstructural investigation of IASCC crack tips extracted from thimble tube O-ring specimens Type A1 Journal article
  Year (down) 2022 Publication Journal of nuclear materials Abbreviated Journal J Nucl Mater
  Volume 565 Issue Pages 153727-16
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
  Abstract The microstructural features of intergranular irradiation-assisted stress corrosion crack tips from a redeemed neutron-irradiated flux thimble tube (60 dpa) have been investigated using focused-ion beam analysis and (scanning) transmission electron microscopy. The current work presents a close examination of the deformation field and oxide assembly associated with intergranular cracking, in addition to the analysis of radiation-induced segregation at leading grain boundaries. Evidence of stress induced martensitic transformation extending from the crack tips is presented. Intergranular crack arrest is demonstrated on the account of the external tensile stress orientation, and as a consequence of MnS inclusion particles segregating close to the fractured grain boundary. Exclusive observations of grain boundary oxidation prior to the cracking are presented, which is in full-agreement with the internal oxidation model.(c) 2022 Elsevier B.V. All rights reserved.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000799256300004 Publication Date 2022-04-11
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN 0022-3115 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 3.1 Times cited Open Access OpenAccess
  Notes Approved Most recent IF: 3.1
  Call Number UA @ admin @ c:irua:188609 Serial 7086
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Author Jenkinson, K.; Liz-Marzan, L.M.; Bals, S.
  Title Multimode electron tomography sheds light on synthesis, structure, and properties of complex metal-based nanoparticles Type A1 Journal article
  Year (down) 2022 Publication Advanced materials Abbreviated Journal Adv Mater
  Volume 34 Issue 36 Pages 2110394-19
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
  Abstract Electron tomography has become a cornerstone technique for the visualization of nanoparticle morphology in three dimensions. However, to obtain in-depth information about a nanoparticle beyond surface faceting and morphology, different electron microscopy signals must be combined. The most notable examples of these combined signals include annular dark-field scanning transmission electron microscopy (ADF-STEM) with different collection angles and the combination of ADF-STEM with energy-dispersive X-ray or electron energy loss spectroscopies. Here, the experimental and computational development of various multimode tomography techniques in connection to the fundamental materials science challenges that multimode tomography has been instrumental to overcoming are summarized. Although the techniques can be applied to a wide variety of compositions, the study is restricted to metal and metal oxide nanoparticles for the sake of simplicity. Current challenges and future directions of multimode tomography are additionally discussed.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000831332200001 Publication Date 2022-04-19
  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 10 Open Access OpenAccess
  Notes The authors thank the financial support of the European Research Council (ERC-AdG-2017 787510, ERC-CoG-2019 815128) and of the European Commission (EUSMI, Grant 731019 and ESTEEM3, Grant 823717). Approved Most recent IF: 29.4
  Call Number UA @ admin @ c:irua:189616 Serial 7087
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Author Lebedev, N.; Huang, Y.; Rana, A.; Jannis, D.; Gauquelin, N.; Verbeeck, J.; Aarts, J.
  Title Resistance minimum in LaAlO3/Eu1-xLaxTiO3/SrTiO3 heterostructures Type A1 Journal article
  Year (down) 2022 Publication Physical review materials Abbreviated Journal
  Volume 6 Issue 7 Pages 075003-75010
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
  Abstract In this paper we study LaAlO3/Eu1-xLaxTiO3/SrTiO3 structures with nominally x = 0, 0.1 and different thicknesses of the Eu1-xLaxTiO3 layer. We observe that both systems have many properties similar to previously studied LaAlO3/EuTiO3/SrTiO3 and other oxide interfaces, such as the formation of a two-dimensional electron liquid for two unit cells of Eu1-xLaxTiO3; a metal-insulator transition driven by the increase in thickness of the Eu1-xLaxTiO3 layer; the presence of an anomalous Hall effect when driving the systems above the Lifshitz point with a back-gate voltage; and a minimum in the temperature dependence of the sheet resistance below the Lifshitz point in the one-band regime, which becomes more pronounced with increasing negative gate voltage. However, and notwithstanding the likely presence of magnetism in the system, we do not attribute that minimum to the Kondo effect, but rather to the properties of the SrTiO3 crystal and the inevitable effects of charge trapping when using back gates.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000834035300001 Publication Date 2022-07-12
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN 2475-9953 ISBN Additional Links UA library record; WoS full record
  Impact Factor 3.4 Times cited Open Access OpenAccess
  Notes N.L. and J.A. gratefully acknowledge the financial support of the research program DESCO, which is financed by the Netherlands Organisation for Scientific Research (NWO). 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 under grant agreement №823717 – ESTEEM3. The QuAnt-EM microscope used in this study was partly funded by the Hercules fund from the Flemish Government. The authors want to thank M. Stehno, G. Koster, and F.J.G. Roesthuis for useful discussions.; esteem3reported; esteem3TA Approved Most recent IF: 3.4
  Call Number UA @ admin @ c:irua:189674 Serial 7094
Permanent link to this record
 

 
Author Borah, R.; Smets, J.; Ninakanti, R.; Tietze, M.L.; Ameloot, R.; Chigrin, D.N.; Bals, S.; Lenaerts, S.; Verbruggen, S.W.
  Title Self-assembled ligand-capped plasmonic Au nanoparticle films in the Kretschmann configuration for sensing of volatile organic compounds Type A1 Journal article
  Year (down) 2022 Publication ACS applied nano materials Abbreviated Journal
  Volume 5 Issue 8 Pages acsanm.2c02524-12
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Sustainable Energy, Air and Water Technology (DuEL)
  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.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000834348300001 Publication Date 2022-07-27
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN 2574-0970 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 5.9 Times cited 11 Open Access OpenAccess
  Notes R.B. acknowledges financial support from the University of Antwerp Special Research Fund (BOF) for a DOCPRO4 doctoral scholarship. J.S. acknowledges financial support from the Research Foundation Flanders (FWO) by a Ph.D. fellowship (11H8121N) . M.L.T. acknowledges financial support from the Research Foundation Flanders (FWO) by a senior postdoctoral fellowship (12ZK720N) . Approved Most recent IF: 5.9
  Call Number UA @ admin @ c:irua:189295 Serial 7095
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Author Hendrickx, M.; Paulus, A.; Kirsanova, M.A.; Van Bael, M.K.; Abakumov, A.M.; Hardy, A.; Hadermann, J.
  Title The influence of synthesis method on the local structure and electrochemical properties of Li-rich/Mn-rich NMC cathode materials for Li-Ion batteries Type A1 Journal article
  Year (down) 2022 Publication Nanomaterials Abbreviated Journal Nanomaterials-Basel
  Volume 12 Issue 13 Pages 2269-18
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
  Abstract Electrochemical energy storage plays a vital role in combating global climate change. Nowadays lithium-ion battery technology remains the most prominent technology for rechargeable batteries. A key performance-limiting factor of lithium-ion batteries is the active material of the positive electrode (cathode). Lithium- and manganese-rich nickel manganese cobalt oxide (LMR-NMC) cathode materials for Li-ion batteries are extensively investigated due to their high specific discharge capacities (>280 mAh/g). However, these materials are prone to severe capacity and voltage fade, which deteriorates the electrochemical performance. Capacity and voltage fade are strongly correlated with the particle morphology and nano- and microstructure of LMR-NMCs. By selecting an adequate synthesis strategy, the particle morphology and structure can be controlled, as such steering the electrochemical properties. In this manuscript we comparatively assessed the morphology and nanostructure of LMR-NMC (Li1.2Ni0.13Mn0.54Co0.13O2) prepared via an environmentally friendly aqueous solution-gel and co-precipitation route, respectively. The solution-gel (SG) synthesized material shows a Ni-enriched spinel-type surface layer at the {200} facets, which, based on our post-mortem high-angle annual dark-field scanning transmission electron microscopy and selected-area electron diffraction analysis, could partly explain the retarded voltage fade compared to the co-precipitation (CP) synthesized material. In addition, deviations in voltage fade and capacity fade (the latter being larger for the SG material) could also be correlated with the different particle morphology obtained for both materials.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000824547500001 Publication Date 2022-07-01
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN 2079-4991 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 5.3 Times cited Open Access Not_Open_Access
  Notes Approved Most recent IF: 5.3
  Call Number UA @ admin @ c:irua:189591 Serial 7098
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Author Pacquets, L.; Van den Hoek, J.; Arenas Esteban, D.; Ciocarlan, R.-G.; Cool, P.; Baert, K.; Hauffman, T.; Daems, N.; Bals, S.; Breugelmans, T.
  Title Use of nanoscale carbon layers on Ag-based gas diffusion electrodes to promote CO production Type A1 Journal article
  Year (down) 2022 Publication ACS applied nano materials Abbreviated Journal
  Volume 5 Issue 6 Pages 7723-7732
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Applied Electrochemistry & Catalysis (ELCAT)
  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.
  Address
  Corporate Author Thesis
  Publisher Place of Publication Editor
  Language Wos 000818507900001 Publication Date 2022-05-19
  Series Editor Series Title Abbreviated Series Title
  Series Volume Series Issue Edition
  ISSN 2574-0970 ISBN Additional Links UA library record; WoS full record; WoS citing articles
  Impact Factor 5.9 Times cited 3 Open Access OpenAccess
  Notes L.P. was supported through a Ph.D. fellowship strategic basic research (1S56920N) of the Research Foundation-Flanders (FWO). S.B. acknowledges financial support from ERC Consolidator Grant Number 815128 REALNANO. This research was financed by the Research Council of the University of Antwerp (BOF-GOA 33928). P.C. and R.-G.C. acknowledge financial support by FWO Flanders (project no. G038215N). The authors recognize the contribution of S. Pourbabak and T. Derez for the assistance with the Ag and carbon coating, Indah Prihatiningtyas and Bart Van der Bruggen for the assistance with the contact angle measurements, Daniel Choukroun for the use of the in-house-made hybrid flow cell, and Stijn Van den Broeck for his assistance with the FIB measurements. Approved Most recent IF: 5.9
  Call Number UA @ admin @ c:irua:188887 Serial 7099
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