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Author Chen, H.; Xu, J.; Wang, Y.; Wang, D.; Ferrer-Espada, R.; Wang, Y.; Zhou, J.; Pedrazo-Tardajos, A.; Yang, M.; Tan, J.-H.; Yang, X.; Zhang, L.; Sychugov, I.; Chen, S.; Bals, S.; Paulsson, J.; Yang, Z.
Title Color-switchable nanosilicon fluorescent probes Type A1 Journal article
Year 2022 Publication ACS nano Abbreviated Journal Acs Nano
Volume 16 Issue 9 Pages 15450-15459
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Fluorescent probes are vital to cell imaging by allowing specific parts of cells to be visualized and quantified. Color-switchable probes (CSPs), with tunable emission wavelength upon contact with specific targets, are particularly powerful because they not only eliminate the need to wash away all unbound probe but also allow for internal controls of probe concentrations, thereby facilitating quantification. Several such CSPs exist and have proven very useful, but not for all key cellular targets. Here we report a pioneering CSP for in situ cell imaging using aldehydefunctionalized silicon nanocrystals (SiNCs) that switch their intrinsic photoluminescence from red to blue quickly when interacting with amino acids in live cells. Though conventional probes often work better in cell-free extracts than in live cells, the SiNCs display the opposite behavior and function well and fast in universal cell lines at 37 ? while requiring much higher temperature in extracts. Furthermore, the SiNCs only disperse in cytoplasm not nucleus, and their fluorescence intensity correlated linearly with the concentration of fed amino acids. We believe these nanosilicon probes will be promising tools to visualize distribution of amino acids and potentially quantify amino acid related processes in live cells.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000861080700001 Publication Date 2022-09-15
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 17.1 Times cited 1 Open Access Not_Open_Access
Notes Z.Y. and H.C. acknowledge the funding support from the National Natural Science Foundation of China (21905316, 22175201) , the Science and Technology Planning Project of Guangdong Province (2019A050510018) , the Pearl River Recruitment Program of Talent (2019QN01C108) , the EU Infrastructure Project EUSMI (Grant No. E190700310) , and Sun Yat-sen University. S.C. acknowledge the funding support from the National Natural Science Foundation of China (32171192) . D.W. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020 program (Grant No. 894254 SuprAtom) . S.B. and A.P.-T. acknowledge financial support from the European Commission under the Horizon 2020 Programme by means of the grant agreement No. 731019 (EUSMI) and the ERC Consolidator Grant No. 815128 (REALNANO) . J.Z. acknowledged the funding support from the China Scholarship Council (CSC) . L.Z and J.X. thank Huzhou Li-in Biotechnology Co., Ltd. for the instrumentational and financial support. J.X. and R.F.-E. appreciate fruitful discussion with Dr. Emanuele Leoncini and Dr. Noah Olsman. J.X. and R.F.-E. also thank Mr. Daniel Eaton and Mr. Carlos Sanchez for their help with microscope setups. Approved Most recent IF: 17.1
Call Number UA @ admin @ c:irua:191574 Serial 7288
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Author Yao, Y.; Ugras, T.J.; Meyer, T.; Dykes, M.; Wang, D.; Arbe, A.; Bals, S.; Kahr, B.; Robinson, R.D.
Title Extracting pure circular dichroism from hierarchically structured CdS magic cluster films Type A1 Journal article
Year 2022 Publication ACS nano Abbreviated Journal Acs Nano
Volume 16 Issue 12 Pages 20457-20469
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Chiroptically active, hierarchically structured materials are difficult to accurately characterize due to linear anisotropic contributions (i.e., linear dichroism (LD) and linear birefringence (LB)) and parasitic ellipticities that produce artifactual circular dichroism (CD) signals, in addition to chiral analyte contributions ranging from molecular-scale clusters to micron-sized assemblies. Recently, we have shown that CdS magic-sized clusters (MSC) can self-assemble into ordered films that have a hierarchical structure spanning seven orders of length-scale. These films have a strong CD response, but the chiral origins are obfuscated by the hierarchical architecture and LDLB contributions. Here, we derive and demonstrate a method for extracting the “pure” CD signal (CD generated by structural dissymmetry) from hierarchical MSC films and identified the chiral origin. The theory behind the method is derived using Mueller matrix and Stokes vector conventions and verified experimentally before being applied to hierarchical MSC and nanoparticle films with varying macroscopic orderings. Each film's extracted “true CD” shares a bisignate profile aligned with the exciton peak, indicating the assemblies adopt a chiral arrangement and form an exciton coupled system. Interestingly, the linearly aligned MSC film possesses one of the highest g-factors (0.05) among semiconducting nanostructures reported. Additionally, we find that films with similar electronic transition dipole alignment can possess greatly different g-factors, indicating chirality change rather than anisotropy is the cause of the difference in the CD signal. The difference in g-factor is controllable via film evaporation geometry. This study provides a simple means to measure “true” CD and presents an example of experimentally understanding chiroptic interactions in hierarchical nanostructures.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000888219600001 Publication Date 2022-11-17
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 17.1 Times cited 8 Open Access Not_Open_Access
Notes This work was supported in part by the National Science Foundation (NSF) under Award Nos. DMR-2003431 and CHE-2003586. This work made use of the Cornell Center for Materials Research Shared Facilities, which are supported through the NSF MRSEC program (DMR-1719875). This work is partly supported by Grant PID2021-123438NB-I00 (MCIN/AEI/10.13039/501100011033 and “ERDF vA way of making Europe”) and Grant IT1566-22 (Eusko Jaurlaritza). D.W. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in the Horizon 2020 program (Grant 894254 SuprAtom). S.B. acknowledges financial support from ERC Consolidator Grant No. 815128 REALNANO. B.K. acknowledges NSF award DMR-2003968. We would like to thank Dr. Mark August Pfeifer for help with circular dichroism measurements. Additionally, we would like to thank Professor Luis M. Liz-Marzan for invaluable discussions on chirality. Approved Most recent IF: 17.1
Call Number UA @ admin @ c:irua:192070 Serial 7305
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Author Parzyszek, S.; Tessarolo, J.; Pedrazo-Tardajos, A.; Ortuno, A.M.; Baginski, M.; Bals, S.; Clever, G.H.; Lewandowski, W.
Title Tunable circularly polarized luminescence via chirality induction and energy transfer from organic films to semiconductor nanocrystals Type A1 Journal article
Year 2022 Publication ACS nano Abbreviated Journal Acs Nano
Volume 16 Issue 11 Pages 18472-18482
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Circularly polarized luminescent (CPL) films with high dissymmetry factors hold great potential for optoelectronic applications. Herei n , we propose a strategy for achieving strongly dissymetric CPL in nanocomposite films based on chira l i t y induction and energy transfer to semiconductor nanocrystals. First, focusing on a purely organic system, aggregation-induced emission (AIE) and CPL activity of organic liquid crystals (LCs) forming helical nanofilaments was detected, featuring green emission with high dissymmetry factors g(lum) similar to 10(-2). The handedness of helical filaments, and thus the sign of CPL, was controlled via minute amounts of a small chiral organic dopant. Second, nanocomposite films were fabricated by incorporating InP/ZnS semi-conductor quantum dots (QDs) into the LC matri x , which induced the chiral assembly of QDs and endowed them with chiroptical properties. Due to the spectral matching of the components, energy transfer (ET) from LC to QDs was possible enabling a convenient way of tuning CPL wavelengths by varying the LC/QD ratio. As obtained, composite films exhibited absolute glum values up to similar to 10(-2) and thermally on/off switchable luminescence. Overall, we demonstrate the induction of chiroptical properties by the assembly of nonchiral building QDs on the chiral organic template and energy transfer from organic films to QDs, representing a simple and versatile approach to tune the CPL activity of organic materials.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000883943600001 Publication Date 2022-11-07
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 17.1 Times cited 10 Open Access OpenAccess
Notes W.L., S.P., and M.B. acknowledge support from the National Science Center Poland under the OPUS Grant UMO-2019/35/B/ST5/04488. J.T. and G.H.C. acknowledge the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany's Excellence Strategy, Grant EXC 2033-390677874-RESOLV. W.L. acknowledges financial support from the European Commission under the Horizon 2020 Programme by Grant E210400529. S.B. and A.P.-T. acknowledge financial support from the European Commission under the Horizon 2020 Programme by Grant 731019 (EUSMI) and ERC Consolidator Grant 815128 (REALNANO). We thank Elie Benchimol for his help with the CPL measurements. We thank Damian Pociecha for his help in the determination of phase sequences of organic compounds. Approved Most recent IF: 17.1
Call Number UA @ admin @ c:irua:192101 Serial 7345
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Author Kante, M.V.; Weber, M.L.; Ni, S.; van den Bosch, I.C.G.; van der Minne, E.; Heymann, L.; Falling, L.J.; Gauquelin, N.; Tsvetanova, M.; Cunha, D.M.; Koster, G.; Gunkel, F.; Nemsak, S.; Hahn, H.; Estrada, L.V.; Baeumer, C.
Title A high-entropy oxide as high-activity electrocatalyst for water oxidation Type A1 Journal article
Year 2023 Publication ACS nano Abbreviated Journal
Volume 17 Issue 6 Pages 5329-5339
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract High-entropy materials are an emerging pathway in the development of high-activity (electro)catalysts because of the inherent tunability and coexistence of multiple potential active sites, which may lead to earth-abundant catalyst materials for energy-efficient electrochemical energy storage. In this report, we identify how the multication composition in high-entropy perovskite oxides (HEO) contributes to high catalytic activity for the oxygen evolution reaction (OER), i.e., the key kinetically limiting half-reaction in several electrochemical energy conversion technologies, including green hydrogen generation. We compare the activity of the (001) facet of LaCr0.2Mn0.2Fe0.2Co0.2Ni0.2O3-delta with the parent compounds (single B-site in the ABO3 perovskite). While the single B-site perovskites roughly follow the expected volcano-type activity trends, the HEO clearly outperforms all of its parent compounds with 17 to 680 times higher currents at a fixed overpotential. As all samples were grown as an epitaxial layer, our results indicate an intrinsic composition-function relationship, avoiding the effects of complex geometries or unknown surface composition. In-depth X-ray photoemission studies reveal a synergistic effect of simultaneous oxidation and reduction of different transition metal cations during the adsorption of reaction intermediates. The surprisingly high OER activity demonstrates that HEOs are a highly attractive, earth-abundant material class for high-activity OER electrocatalysts, possibly allowing the activity to be fine-tuned beyond the scaling limits of mono-or bimetallic oxides.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000953440900001 Publication Date 2023-03-13
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 17.1 Times cited Open Access OpenAccess
Notes Approved Most recent IF: 17.1; 2023 IF: 13.942
Call Number UA @ admin @ c:irua:196097 Serial 7390
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Author Scolfaro, D.; Finamor, M.; Trinchao, L.O.; Rosa, B.L.T.; Chaves, A.; Santos, P., V.; Iikawa, F.; Couto, O.D.D., Jr.
Title Acoustically driven stark effect in transition metal dichalcogenide monolayers Type A1 Journal article
Year 2021 Publication Acs Nano Abbreviated Journal Acs Nano
Volume 15 Issue 9 Pages 15371-15380
Keywords A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Abstract The Stark effect is one of the most efficient mechanisms to manipulate many-body states in nanostructured systems. In mono- and few-layer transition metal dichalcogenides, it has been successfully induced by optical and electric field means. Here, we tune the optical emission energies and dissociate excitonic states in MoSe2 monolayers employing the 220 MHz in-plane piezoelectric field carried by surface acoustic waves. We transfer the monolayers to high dielectric constant piezoelectric substrates, where the neutral exciton binding energy is reduced, allowing us to efficiently quench (above 90%) and red-shift the excitonic optical emissions. A model for the acoustically induced Stark effect yields neutral exciton and trion in-plane polarizabilities of 530 and 630 x 10(-5) meV/(kV/cm)(2), respectively, which are considerably larger than those reported for monolayers encapsulated in hexagonal boron nitride. Large in-plane polarizabilities are an attractive ingredient to manipulate and modulate multiexciton interactions in two-dimensional semiconductor nanostructures for optoelectronic applications.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000703553600129 Publication Date 2021-08-27
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.942 Times cited Open Access OpenAccess
Notes Approved Most recent IF: 13.942
Call Number UA @ admin @ c:irua:182545 Serial 7415
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Author Zhang, G.; Huang, S.; Chaves, A.; Yan, H.
Title Black phosphorus as tunable Van der Waals quantum wells with high optical quality Type A1 Journal article
Year 2023 Publication ACS nano Abbreviated Journal
Volume 17 Issue 6 Pages 6073-6080
Keywords A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Abstract Van der Waals quantum wells, naturally formed in two-dimensional layered materials with nanoscale thickness, possess many inherent advantages over conventional molecular beam epitaxy grown counterparts, and could bring up intriguing physics and applications. However, optical transitions originated from the series of quantized states in these emerging quantum wells are still elusive. Here, we show that multilayer black phosphorus appears to be an excellent candidate for van der Waals quantum wells with well-defined subbands and high optical quality. Using infrared absorption spectroscopy, we probe subband structures of multilayer black phosphorus with tens of atomic layers, revealing clear signatures for optical transitions with subband index as high as 10, far from what was attainable previously. Surprisingly, in addition to allowed transitions, an unexpected series of “forbidden” transitions is also evidently observed, which enables us to determine energy spacings separately for conduction and valence subbands. Furthermore, the linear tunability of subband spacings by temperature and strain is demonstrated. Our results are expected to facilitate potential applications for infrared optoelectronics based on tunable van der Waals quantum wells.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000953463300001 Publication Date 2023-03-13
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 17.1 Times cited Open Access Not_Open_Access
Notes Approved Most recent IF: 17.1; 2023 IF: 13.942
Call Number UA @ admin @ c:irua:196100 Serial 7565
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Author Byrnes, I.; Rossbach, L.M.; Brede, D.A.; Grolimund, D.; Sanchez, D.F.; Nuyts, G.; Cuba, V.; Reinoso-Maset, E.; Salbu, B.; Janssens, K.; Oughton, D.; Scheibener, S.; Teien, H.-C.; Lind, O.C.
Title Synchrotron-based X-ray fluorescence imaging elucidates uranium toxicokinetics in Daphnia magna Type A1 Journal article
Year 2023 Publication ACS nano Abbreviated Journal
Volume 17 Issue 6 Pages 5296-5305
Keywords A1 Journal article; Engineering sciences. Technology; Antwerp X-ray Imaging and Spectroscopy (AXIS)
Abstract A combination of synchrotron-based elemental anal-ysis and acute toxicity tests was used to investigate the biodistribution and adverse effects in Daphnia magna exposed to uranium nanoparticle (UNP, 3-5 nm) suspensions or to uranium reference (Uref) solutions. Speciation analysis revealed similar size distributions between exposures, and toxicity tests showed com-parable acute effects (UNP LC50: 402 mu g L-1 [336-484], Uref LC50: 268 mu g L-1 [229-315]). However, the uranium body burden was 3 -to 5-fold greater in UNP-exposed daphnids, and analysis of survival as a function of body burden revealed a similar to 5-fold higher specific toxicity from the Uref exposure. High-resolution X-ray fluorescence elemental maps of intact, whole daphnids from sublethal, acute exposures of both treatments revealed high uranium accumulation onto the gills (epipodites) as well as within the hepatic ceca and the intestinal lumen. Uranium uptake into the hemolymph circulatory system was inferred from signals observed in organs such as the heart and the maxillary gland. The substantial uptake in the maxillary gland and the associated nephridium suggests that these organs play a role in uranium removal from the hemolymph and subsequent excretion. Uranium was also observed associated with the embryos and the remnants of the chorion, suggesting uptake in the offspring. The identification of target organs and tissues is of major importance to the understanding of uranium and UNP toxicity and exposure characterization that should ultimately contribute to reducing uncertainties in related environmental impact and risk assessments.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000960129800001 Publication Date 2023-03-15
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 17.1 Times cited Open Access OpenAccess
Notes Approved Most recent IF: 17.1; 2023 IF: 13.942
Call Number UA @ admin @ c:irua:196061 Serial 8631
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Author Zhang, Y.; van Schayck, J.P.; Pedrazo-Tardajos, A.; Claes, N.; Noteborn, W.E.M.; Lu, P.-H.; Duimel, H.; Dunin-Borkowski, R.E.; Bals, S.; Peters, P.J.; Ravelli, R.B.G.
Title Charging of vitreous samples in cryogenic electron microscopy mitigated by graphene Type A1 Journal article
Year 2023 Publication ACS nano Abbreviated Journal
Volume 17 Issue 16 Pages 15836-15846
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Cryogenic electronmicroscopy can provide high-resolution reconstructionsof macromolecules embedded in a thin layer of ice from which atomicmodels can be built de novo. However, the interactionbetween the ionizing electron beam and the sample results in beam-inducedmotion and image distortion, which limit the attainable resolutions.Sample charging is one contributing factor of beam-induced motionsand image distortions, which is normally alleviated by including partof the supporting conducting film within the beam-exposed region.However, routine data collection schemes avoid strategies wherebythe beam is not in contact with the supporting film, whose rationaleis not fully understood. Here we characterize electrostatic chargingof vitreous samples, both in imaging and in diffraction mode. We mitigatesample charging by depositing a single layer of conductive grapheneon top of regular EM grids. We obtained high-resolution single-particleanalysis (SPA) reconstructions at 2 & ANGS; when the electron beamonly irradiates the middle of the hole on graphene-coated grids, usingdata collection schemes that previously failed to produce sub 3 & ANGS;reconstructions without the graphene layer. We also observe that theSPA data obtained with the graphene-coated grids exhibit a higher b factor and reduced particle movement compared to dataobtained without the graphene layer. This mitigation of charging couldhave broad implications for various EM techniques, including SPA andcryotomography, and for the study of radiation damage and the developmentof future sample carriers. Furthermore, it may facilitate the explorationof more dose-efficient, scanning transmission EM based SPA techniques.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001041649900001 Publication Date 2023-08-02
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851 ISBN Additional Links UA library record; WoS full record
Impact Factor 17.1 Times cited Open Access OpenAccess
Notes We thank H. Nguyen for editing the manuscript. We warmly thank the M4i Microscopy CORE Lab team of FHML Maastricht University (MU) for their support and collaboration and Eve Timlin and Ye Gao (MU) for providing protein samples. Members of the Amsterdam Scientific Instruments team are acknowledged for their Timepix detector support. This work benefited from access to The Netherlands Centre for Electron Nanoscopy (NeCEN) with assistance from Ludovic Renault and Meindert Lamers. The authors acknowledge financial support of the Netherlands Electron Microscopy Infrastructure (NEMI), project number 184.034.014 of the National Roadmap for Large-Scale Research Infrastructure of the Dutch Research Council (NWO), the PPP Allowance made available by Health-Holland, Top Sector Life Sciences & Health, to stimulate public-private partnerships, project 4DEM, number LSHM21029, and the LINK program from the Province of Limburg, The Netherlands, as well as financial support from the European Commission under the Horizon 2020 Programme by grant no. 815128 (REALNANO). Approved Most recent IF: 17.1; 2023 IF: 13.942
Call Number UA @ admin @ c:irua:198376 Serial 8840
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Author Vega-Paredes, M.; Aymerich-Armengol, R.; Arenas Esteban, D.; Marti-Sanchez, S.; Bals, S.; Scheu, C.; Manjon, A.G.
Title Electrochemical stability of rhodium-platinum core-shell nanoparticles : an identical location scanning transmission electron microscopy study Type A1 Journal article
Year 2023 Publication ACS nano Abbreviated Journal
Volume 17 Issue 17 Pages 16943-16951
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Rhodium-platinum core-shell nanoparticleson a carbonsupport (Rh@Pt/C NPs) are promising candidates as anode catalystsfor polymer electrolyte membrane fuel cells. However, their electrochemicalstability needs to be further explored for successful applicationin commercial fuel cells. Here we employ identical location scanningtransmission electron microscopy to track the morphological and compositionalchanges of Rh@Pt/C NPs during potential cycling (10 000 cycles,0.06-0.8 V-RHE, 0.5 H2SO4)down to the atomic level, which are then used for understanding thecurrent evolution occurring during the potential cycles. Our resultsreveal a high stability of the Rh@Pt/C system and point toward particledetachment from the carbon support as the main degradation mechanism.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001051495900001 Publication Date 2023-08-21
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 17.1 Times cited 2 Open Access OpenAccess
Notes The authors would like to thank C. Bodirsky for providing the samples, N. Rivas Rivas for his corrections on the manuscript, and D. Chatain for providing her expertise on the equilibrium shape of nanoparticles. Special thanks to B. Breitbach for performing the XRD experiments. A.G.M. acknowledges the Grant RYC2021-033479- I funded by MCIN/AEI/10.13039/501100011033 and, as appropriate, by European Union NextGenerationEU/PRTR. Approved Most recent IF: 17.1; 2023 IF: 13.942
Call Number UA @ admin @ c:irua:199253 Serial 8859
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Author Tran, T.T.; Lee, Y.; Roy, S.; Tran, T.U.; Kim, Y.; Taniguchi, T.; Watanabe, K.; Milošević, M.V.; Lim, S.C.; Chaves, A.; Jang, J.I.; Kim, J.
Title Synergetic enhancement of quantum yield and exciton lifetime of monolayer WS₂ by proximal metal plate and negative electric bias Type A1 Journal article
Year 2023 Publication ACS nano Abbreviated Journal
Volume 18 Issue 1 Pages 220-228
Keywords A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Abstract The efficiency of light emission is a critical performance factor for monolayer transition metal dichalcogenides (1L-TMDs) for photonic applications. While various methods have been studied to compensate for lattice defects to improve the quantum yield (QY) of 1L-TMDs, exciton-exciton annihilation (EEA) is still a major nonradiative decay channel for excitons at high exciton densities. Here, we demonstrate that the combined use of a proximal Au plate and a negative electric gate bias (NEGB) for 1L-WS2 provides a dramatic enhancement of the exciton lifetime at high exciton densities with the corresponding QY enhanced by 30 times and the EEA rate constant decreased by 80 times. The suppression of EEA by NEGB is attributed to the reduction of the defect-assisted EEA process, which we also explain with our theoretical model. Our results provide a synergetic solution to cope with EEA to realize high-intensity 2D light emitters using TMDs.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001139516800001 Publication Date 2023-12-21
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851 ISBN Additional Links UA library record; WoS full record
Impact Factor 17.1 Times cited Open Access
Notes Approved Most recent IF: 17.1; 2023 IF: 13.942
Call Number UA @ admin @ c:irua:202811 Serial 9101
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Author Vlasov, E.; Heyvaert, W.; Ni, B.; Van Gordon, K.; Girod, R.; Verbeeck, J.; Liz-Marzán, L.M.; Bals, S.
Title High-Throughput Morphological Chirality Quantification of Twisted and Wrinkled Gold Nanorods Type A1 Journal Article
Year 2024 Publication ACS Nano Abbreviated Journal ACS Nano
Volume Issue Pages
Keywords A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;
Abstract Chirality in gold nanostructures offers an exciting opportunity to tune their differential optical response to left- and right-handed circularly polarized light, as well as their interactions with biomolecules and living matter. However, tuning and understanding such interactions demands quantification of the structural features that are responsible for the chiral behavior. Electron tomography (ET) enables structural characterization at the single-particle level and has been used to quantify the helicity of complex chiral nanorods. However, the technique is time-consuming and consequently lacks statistical value. To address this issue, we introduce herein a high-throughput methodology that combines images acquired by secondary electron-based electron beam-induced current (SEEBIC) with quantitative image analysis. As a result, the geometric chirality of hundreds of nanoparticles can be quantified in less than 1 h. When combining the drastic gain in data collection efficiency of SEEBIC with a limited number of ET data sets, a better understanding of how the chiral structure of individual chiral nanoparticles translates into the ensemble chiroptical response can be reached.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos Publication Date 2024-04-26
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851 ISBN Additional Links
Impact Factor 17.1 Times cited Open Access
Notes The authors acknowledge financial support by the European Research Council (ERC CoG No. 815128 REALNANO to S.B.) and from MCIN/AEI/10.13039/501100011033 (Grant PID2020-117779RB-I00 to L.M.L.-M and FPI Fellowship PRE2021-097588 to K.V.G.). Funded by the European Union under Project 101131111 − DELIGHT, JV acknowledges the eBEAM project supported by the European Union’s Horizon 2020 research and innovation program FETPROACT-EIC-07- 2020: emerging paradigms and communities. Approved Most recent IF: 17.1; 2024 IF: 13.942
Call Number EMAT @ emat @ Serial 9121
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Author Sethu, K.K.V.; Yasin, F.; Swerts, J.; Sorée, B.; De Boeck, J.; Kar, G.S.; Garello, K.; Couet, S.
Title Spin-orbit torque vector quantification in nanoscale magnetic tunnel junctions Type A1 Journal article
Year 2024 Publication ACS nano Abbreviated Journal
Volume 18 Issue 21 Pages 13506-13516
Keywords A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Abstract Spin-orbit torques (SOT) allow ultrafast, energy-efficient toggling of magnetization state by an in-plane charge current for applications such as magnetic random-access memory (SOT-MRAM). Tailoring the SOT vector comprising of antidamping (T-AD) and fieldlike (T-FL) torques could lead to faster, more reliable, and low-power SOT-MRAM. Here, we establish a method to quantify the longitudinal (T-AD) and transverse (T-FL) components of the SOT vector and its efficiency chi(AD) and chi(FL), respectively, in nanoscale three-terminal SOT magnetic tunnel junctions (SOT-MTJ). Modulation of nucleation or switching field (B-SF) for magnetization reversal by SOT effective fields (B-SOT) leads to the modification of SOT-MTJ hysteresis loop behavior from which chi(AD) and chi(FL) are quantified. Surprisingly, in nanoscale W/CoFeB SOT-MTJ, we find chi(FL) to be (i) twice as large as chi(AD) and (ii) 6 times as large as chi(FL) in micrometer-sized W/CoFeB Hall-bar devices. Our quantification is supported by micromagnetic and macrospin simulations which reproduce experimental SOT-MTJ Stoner-Wohlfarth astroid behavior only for chi(FL) > chi(AD). Additionally, from the threshold current for current-induced magnetization switching with a transverse magnetic field, we show that in SOT-MTJ, T-FL plays a more prominent role in magnetization dynamics than T-AD. Due to SOT-MRAM geometry and nanodimensionality, the potential role of nonlocal spin Hall spin current accumulated adjacent to the SOT-MTJ in the mediation of T-FL and chi(FL) amplification merits to be explored.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001226121700001 Publication Date 2024-05-15
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851 ISBN Additional Links UA library record; WoS full record
Impact Factor Times cited Open Access
Notes Approved no
Call Number UA @ admin @ c:irua:205980 Serial 9173
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Author Lentijo-Mozo, S.; Tan, R.P.; Garcia-Marcelot, C.; Altantzis, T.; Fazzini, P.F.; Hungria, T.; Cormary, B.; Gallagher, J.R.; Miller, J.T.; Martinez, H.; Schrittwieser, S.; Schotter, J.; Respaud, M.; Bals, S.; Van Tendeloo, G.; Gatel, C.; Soulantica, K.
Title Air- and water-resistant noble metal coated ferromagnetic cobalt nanorods Type A1 Journal article
Year 2015 Publication ACS nano Abbreviated Journal Acs Nano
Volume 9 Issue 9 Pages 2792-2804
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Cobalt nanorods possess ideal magnetic properties for applications requiring magnetically hard nanoparticles. However, their exploitation is undermined by their sensitivity toward oxygen and water, which deteriorates their magnetic properties. The development of a continuous metal shell inert to oxidation could render them stable, opening perspectives not only for already identified applications but also for uses in which contact with air and/or aqueous media is inevitable. However, the direct growth of a conformal noble metal shell on magnetic metals is a challenge. Here, we show that prior treatment of Co nanorods with a tin coordination compound is the crucial step that enables the subsequent growth of a continuous noble metal shell on their surface, rendering them air- and water-resistant, while conserving the monocrystallity, metallicity and the magnetic properties of the Co core. Thus, the as-synthesized coreshell ferromagnetic nanorods combine high magnetization and strong uniaxial magnetic anisotropy, even after exposure to air and water, and hold promise for successful implementation in in vitro biodiagnostics requiring probes of high magnetization and anisotropic shape.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000351791800055 Publication Date 2015-03-03
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.942 Times cited 25 Open Access OpenAccess
Notes 312483 Esteem2; 246791 Countatoms; 335078 Colouratom; esteem2ta; ECASSara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); Approved Most recent IF: 13.942; 2015 IF: 12.881
Call Number c:irua:125380 c:irua:125380 Serial 87
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Author Kundu, P.; Turner, S.; Van Aert, S.; Ravishankar, N.; Van Tendeloo, G.
Title Atomic structure of quantum gold nanowires : quantification of the lattice strain Type A1 Journal article
Year 2014 Publication ACS nano Abbreviated Journal Acs Nano
Volume 8 Issue 1 Pages 599-606
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Theoretical studies exist to compute the atomic arrangement in gold nanowires and the influence on their electronic behavior with decreasing diameter. Experimental studies, e.g., by transmission electron microscopy, on chemically synthesized ultrafine wires are however lacking owing to the unavailability of suitable protocols for sample preparation and the stability of the wires under electron beam irradiation. In this work, we present an atomic scale structural investigation on quantum single crystalline gold nanowires of 2 nm diameter, chemically prepared on a carbon film grid. Using low dose aberration-corrected high resolution (S)TEM, we observe an inhomogeneous strain distribution in the crystal, largely concentrated at the twin boundaries and the surface along with the presence of facets and surface steps leading to a noncircular cross section of the wires. These structural aspects are critical inputs needed to determine their unique electronic character and their potential as a suitable catalyst material. Furthermore, electron-beam-induced structural changes at the atomic scale, having implications on their mechanical behavior and their suitability as interconnects, are discussed.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000330542900061 Publication Date 2013-11-29
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.942 Times cited 20 Open Access
Notes FWO; Countatoms; Hercules Approved Most recent IF: 13.942; 2014 IF: 12.881
Call Number UA @ lucian @ c:irua:113856 Serial 199
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Author Xu, X.; Vereecke, G.; Chen, C.; Pourtois, G.; Armini, S.; Verellen, N.; Tsai, W.K.; Kim, D.W.; Lee, E.; Lin, C.Y.; Van Dorpe, P.; Struyf, H.; Holsteyns, F.; Moshchalkov, V.; Indekeu, J.; De Gendt, S.;
Title Capturing wetting states in nanopatterned silicon Type A1 Journal article
Year 2014 Publication ACS nano Abbreviated Journal Acs Nano
Volume 8 Issue 1 Pages 885-893
Keywords A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract Spectacular progress in developing advanced Si circuits with reduced size, along the track of Moore's law, has been relying on necessary developments in wet cleaning of nanopatterned Si wafers to provide contaminant free surfaces. The most efficient cleaning is achieved when complete wetting can be realized. In this work, ordered arrays of silicon nanopillars on a hitherto unexplored small scale have been used to study the wetting behavior on nanomodulated surfaces in a substantial range of surface treatments and geometrical parameters. With the use of optical reflectance measurements, the nanoscale water imbibition depths have been measured and the transition to the superhydrophobic Cassie-Baxter state has been accurately determined. For pillars of high aspect ratio (about 15), the transition occurs even when the surface is grafted with a hydrophilic functional group. We have found a striking consistent deviation between the contact angle measurements and the straightforward application of the classical wetting models. Molecular dynamics simulations show that these deviations can be attributed to the long overlooked atomic-scale surface perturbations that are introduced during the nanofabrication process. When the transition condition is approached, transient states of partial imbibition that characterize intermediate states between the Wenzel and Cassie-Baxter states are revealed in our experiments.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000330542900092 Publication Date 2013-12-31
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.942 Times cited 39 Open Access
Notes Approved Most recent IF: 13.942; 2014 IF: 12.881
Call Number UA @ lucian @ c:irua:114871 Serial 276
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Author Neyts, E.C.; Shibuta, Y.; van Duin, A.C.T.; Bogaerts, A.
Title Catalyzed growth of carbon nanotube with definable chirality by hybrid molecular dynamics-force biased Monte Carlo simulations Type A1 Journal article
Year 2010 Publication ACS nano Abbreviated Journal Acs Nano
Volume 4 Issue 11 Pages 6665-6672
Keywords A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract Metal-catalyzed growth mechanisms of carbon nanotubes (CNTs) were studied by hybrid molecular dynamics−Monte Carlo simulations using a recently developed ReaxFF reactive force field. Using this novel approach, including relaxation effects, a CNT with definable chirality is obtained, and a step-by-step atomistic description of the nucleation process is presented. Both root and tip growth mechanisms are observed. The importance of the relaxation of the network is highlighted by the observed healing of defects.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000284438000043 Publication Date 2010-10-12
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.942 Times cited 129 Open Access
Notes Approved Most recent IF: 13.942; 2010 IF: 9.865
Call Number UA @ lucian @ c:irua:84759 Serial 294
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Author Javon, E.; Gaceur, M.; Dachraoui, W.; Margeat, O.; Ackermann, J.; Ilenia Saba, M.; Delugas, P.; Mattoni, A.; Bals, S.; Van Tendeloo, G.
Title Competing forces in the self-assembly of coupled ZnO nanopyramids Type A1 Journal article
Year 2015 Publication ACS nano Abbreviated Journal Acs Nano
Volume 9 Issue 9 Pages 3685-3694
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Self-assembly (SA) of nanostructures has recently gained increasing interest. A clear understanding of the process is not straightforward since SA of nanoparticles is a complex multiscale phenomenon including different driving forces. Here, we study the SA between aluminum doped ZnO nanopyramids into couples by combining inorganic chemistry and advanced electron microscopy techniques with atomistic simulations. Our results show that the SA of the coupled nanopyramids is controlled first by morphology, as coupling only occurs in the case of pyramids with well-developed facets of the basal planes. The combination of electron microscopy and atomistic modeling reveals that the coupling is further driven by strong ligandligand interaction between the bases of the pyramids as dominant force, while screening effects due to Al doping or solvent as well as corecore interaction are only minor contributions. Our combined approach provides a deeper understanding of the complex interplay between the interactions at work in the coupled SA of ZnO nanopyramids.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000353867000030 Publication Date 2015-03-12
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.942 Times cited 21 Open Access OpenAccess
Notes Esmi; 335078 Colouratom; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); Approved Most recent IF: 13.942; 2015 IF: 12.881
Call Number c:irua:125978 Serial 434
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Author Bertoni, G.; Grillo, V.; Brescia, R.; Ke, X.; Bals, S.; Catellani, A.; Li, H.; Manna, L.
Title Direct determination of polarity, faceting, and core location in colloidal core/shell wurtzite semiconductor nanocrystals Type A1 Journal article
Year 2012 Publication ACS nano Abbreviated Journal Acs Nano
Volume 6 Issue 7 Pages 6453-6461
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract The ability to determine the atomic arrangement and termination of various facets of surfactant-coated nanocrystals is of great importance for understanding their growth mechanism and their surface properties and represents a critical piece of information that can be coupled to other experimental techniques and to calculations. This is especially appealing in the study of nanocrystals that can be grown in strongly anisotropic shapes, for which the relative growth rates of various facets can be influenced under varying reaction conditions. Here we show that in two representative cases of rod-shaped nanocrystals in the wurtzite phase (CdSe(core)/CdS(shell) and ZnSe(core)/ZnS(shell) nanorods) the terminations of the polar facets can be resolved unambiguously by combining advanced electron microscopy techniques, such as aberration-corrected HRTEM with exit wave reconstruction or aberration-corrected HAADF-STEM. The [0001] and [000-1] polar directions of these rods, which grow preferentially along their c-axis, are revealed clearly, with one side consisting of the Cd (or Zn)-terminated (0001) facet and the other side with a pronounced faceting due to Cd (or Zn)-terminated {10-1-1} facets. The lateral faceting of the rods is instead dominated by three nonpolar {10-10} facets. The core buried in the nanostructure can be localized in both the exit wave phase and HAADF-STEM images.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000306673800079 Publication Date 2012-06-18
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.942 Times cited 63 Open Access
Notes The authors gratefully acknowledge funding from the European Research Council under grant number 240111 (NANO-ARCH) and the financial support from the Flemish Hercules 3 Programme for large infrastructures. G.B. and V.G. thank E. Rotunno for his help with STEM_CELL and IWFR. Approved Most recent IF: 13.942; 2012 IF: 12.062
Call Number UA @ lucian @ c:irua:101138 Serial 710
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Author Rossell, M.D.; Abakumov, A.M.; Ramasse, Q.M.; Erni, R.
Title Direct evidence of stacking disorder in the mixed ionic-electronic conductor Sr4Fe6O12+\delta Type A1 Journal article
Year 2013 Publication ACS nano Abbreviated Journal Acs Nano
Volume 7 Issue 4 Pages 3078-3085
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Determining the structure-to-property relationship of materials becomes particularly challenging when the material under investigation is dominated by defects and structural disorder. Knowledge on the exact atomic arrangement at the defective structure is required to understand its influence on the functional properties. However, standard diffraction techniques deliver structural information that is averaged over many unit cells. In particular, information about defects and order-disorder phenomena is contained in the coherent diffuse scattering intensity which often is difficult to uniquely interpret. Thus, the examination of the local disorder in materials requires a direct method to study their structure on the atomic level with chemical sensitivity. Using aberration-corrected scanning transmission electron microscopy in combination with atomic-resolution electron energy-loss spectroscopy, we show that the controversial structural arrangement of the Fe2O2+delta layers in the mixed ionic-electronic conducting Sr4Fe6O12+delta perovskite can be unambiguously resolved. Our results provide direct experimental evidence for the presence of a nanomixture of “ordered” and “disordered” domains in an epitaxial Sr4Fe6O12+delta thin film. The most favorable arrangement is the disordered structure and is interpreted as a randomly occurring but well-defined local shift of the Fe-O chains in the Fe2O2+delta layers. By analyzing the electron energy-loss near-edge structure of the different building blocks in the Sr4Fe6O12+delta unit cell we find that the mobile holes in this mixed ionic-electronic conducting oxide are highly localized in the Fe2O2+delta layers, which are responsible for the oxide-ion conductivity. A possible link between disorder and oxygen-ion transport along the Fe2O2+delta layers is proposed by arguing that the disorder can effectively break the oxygen diffusion pathways.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000318143300021 Publication Date 2013-03-04
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.942 Times cited 4 Open Access
Notes Approved Most recent IF: 13.942; 2013 IF: 12.033
Call Number UA @ lucian @ c:irua:108476 Serial 713
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Author Chen, B.; Sahin, H.; Suslu, A.; Ding, L.; Bertoni, M.I.; Peeters, F.M.; Tongay, S.
Title Environmental changes in MoTe2 excitonic dynamics by defects-activated molecular interaction Type A1 Journal article
Year 2015 Publication ACS nano Abbreviated Journal Acs Nano
Volume 9 Issue 9 Pages 5326-5332
Keywords A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Abstract Monolayers of group VI transition metal dichalcogenides possess direct gaps in the visible spectrum with the exception of MoTe2, where its gap is suitably located in the infrared region but its stability is of particular interest, as tellurium compounds are acutely sensitive to oxygen exposure. Here, our environmental (time-dependent) measurements reveal two distinct effects on MoTe2 monolayers: For weakly luminescent monolayers, photoluminescence signal and optical contrast disappear, as if they are decomposed, but yet remain intact as evidenced by AFM and Raman measurements. In contrast, strongly luminescent monolayers retain their optical contrast for a prolonged amount of time, while their PL peak blue-shifts and PL intensity saturates to slightly lower values. Our X-ray photoelectron spectroscopy measurements and DFT calculations suggest that the presence of defects and functionalization of these defect sites with O-2 molecules strongly dictate their material properties and aging response by changing the excitonic dynamics due to deep or shallow states that are created within the optical band gap. Presented results not only shed light on environmental effects on fundamental material properties and excitonic dynamics of MoTe2 monolayers but also highlight striking material transformation for metastable 20 systems such as WTe2, silicone, and phosphorene.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000355383000068 Publication Date 2015-04-14
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.942 Times cited 150 Open Access
Notes ; This work was supported by the Arizona State University seeding program. The authors thank Hui Cai and Kedi Wu for useful discussions. We gratefully acknowledge the use of facilities at the LeRoy Eyring Center for Solid State Science at Arizona State University. This work was supported by the Flemish Science Foundation (FWO-VI) and the Methusalem Foundation of the Flemish government. H.S. is supported by a FWO Pegasus Long Marie Curie Fellowship. ; Approved Most recent IF: 13.942; 2015 IF: 12.881
Call Number c:irua:126441 Serial 1068
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Author Sanz-Ortiz, M.N.; Sentosun, K.; Bals, S.; Liz-Marzan, L.M.
Title Templated Growth of Surface Enhanced Raman Scattering -Active Branched Au Nanoparticles within Radial Mesoporous Silica Shells Type A1 Journal article
Year 2015 Publication ACS nano Abbreviated Journal Acs Nano
Volume 9 Issue 9 Pages 10489-10497
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Noble metal nanoparticles are widely used as probes or substrates for surface-enhanced Raman scattering (SERS), due to their characteristic plasmon resonances in the visible and NIR spectral ranges. Aiming at obtaining a versatile system with high SERS performance we developed the synthesis of quasi-monodisperse, non-aggregated gold nanoparticles protected by radial mesoporous silica shells. The radial channels of such shells were used as templates for the growth of gold tips branching from the cores, thereby improving the plasmonic performance of the particles while favoring the localization of analyte molecules at high electric field regions: close to the tips, inside the pores. The method, which allows control over tip length, was successfully applied to various gold nanoparticle shapes, leading to materials with highly efficient SERS performance. The obtained nanoparticles are stable in ethanol and water upon thermal consolidation and can be safely stored as a powder.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language English Wos 000363915300105 Publication Date 2015-09-15
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.942 Times cited 110 Open Access OpenAccess
Notes This work has been funded by the European Research Council (ERC Advanced Grant 267867 Plasmaquo and Starting Grant Colouratom). The research leading to these results has received funding from the European Union's Seventh Framework Programme (FP7/2007-2013 under grant agreement no. 312184, SACS). Help from Mert Kurttepeli is acknowledged. Pentatwinned nanorods and nanotriangles were synthesized by L. Scarabelli.; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); Approved Most recent IF: 13.942; 2015 IF: 12.881
Call Number c:irua:129194 Serial 3947
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Author Tognalii, N.G.; Cortés, E.; Hernández-Nieves, A.D.; Carro, P.; Usaj, G.; Balseiro, C.A.; Vela, M.E.; Salvarezza, R.C.; Fainstein, A.
Title From single to multiple Ag-layer modification of Au nanocavity substrates : a tunable probe of the chemical surface-enhanced Raman scattering mechanism Type A1 Journal article
Year 2011 Publication ACS nano Abbreviated Journal Acs Nano
Volume 5 Issue 7 Pages 5433-5443
Keywords A1 Journal article; Condensed Matter Theory (CMT)
Abstract We present experimental and computational results that enlighten the mechanisms underlying the chemical contribution to surface-enhanced Raman scattering (SERS). Gold void metallic arrays electrochemically covered either by a Ag monolayer or 10100 Ag layers were modified with a self-assembled monolayer of 4-mercaptopyridine as a molecular Raman probe displaying a rich and unexpected Raman response. A resonant increase of the Raman intensity in the red part of the spectrum is observed that cannot be related to plasmon excitations of the cavity-array. Notably, we find an additional 1020 time increase of the SERS amplification upon deposition of a single Ag layer on the Au substrate, which is, however, almost quenched upon deposition of 10 atomic layers. Further deposition of 100 atomic Ag layers results in a new increase of the SERS signal, consistent with the improved plasmonic efficiency of Ag bulk-like structures. The SERS response as a function of the Ag layer thickness is analyzed in terms of ab initio calculations and a microscopic model for the SERS chemical mechanism based on a resonant charge transfer process between the molecular HOMO state and the Fermi level in the metal surface. We find that a rearrangement of the electronic charge density related to the presence of the Ag monolayer in the Au/Ag/molecule complex causes an increase in the distance between the HOMO center of charge and the metallic image plane that is responsible for the variation of Raman enhancement between the studied substrates. Our results provide a general platform for studying the chemical contribution to SERS, and for enhancing the Raman efficiency of tailored Au-SERS templates through electrochemical modification with Ag films.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000293035200019 Publication Date 2011-06-15
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.942 Times cited 26 Open Access
Notes ; We acknowledge financial support from ANPCyT (Argentina, PICT08-1617, PICT08-2236, PICT06-621, PICT-CNPQ-08-0019, PAE 22711, PICT06-01061, PICT06-483) and Project CTQ2008-06017/BQU, Spain. N.G.T, E.C., A.D.H.N., R.C.S, G.U., C.A.B., and A.F. are also at CONICET. M.E.V. is a member of the research career of CIC BsAs. R.C.S., C.A.B., and A.F. are Guggenheim Foundation Fellows. We would like to thank Dr. M. H. Fonticelli for fruitful discussions on the electrochemical measurements and Dr. H. Pastoriza for the help with the SEM measurements. ; Approved Most recent IF: 13.942; 2011 IF: 11.421
Call Number UA @ lucian @ c:irua:91775 Serial 1285
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Author Sánchez-Iglesias, A.; Grzelczak, M.; Altantzis, T.; Goris, B.; Pérez-Juste, J.; Bals, S.; Van Tendeloo, G.; Donaldson, S.H.; Chmelka, B.F.; Israelachvili, J.N.; Liz-Marzán, L.M.;
Title Hydrophobic interactions modulate self-assembly of nanoparticles Type A1 Journal article
Year 2012 Publication ACS nano Abbreviated Journal Acs Nano
Volume 6 Issue 12 Pages 11059-11065
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Hydrophobic interactions constitute one of the most important types of nonspecific interactions in biological systems, which emerge when water molecules rearrange as two hydrophobic species come close to each other. The prediction of hydrophobic interactions at the level of nanoparticles (Brownian objects) remains challenging because of uncontrolled diffusive motion of the particles. We describe here a general methodology for solvent-induced, reversible self-assembly of gold nanoparticles into 3D clusters with well-controlled sizes. A theoretical description of the process confirmed that hydrophobic interactions are the main driving force behind nanoparticle aggregation.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000312563600070 Publication Date 2012-11-28
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.942 Times cited 311 Open Access
Notes 267867 Plasma Quo; 246791 Countatoms; 262348 Esmi Approved Most recent IF: 13.942; 2012 IF: 12.062
Call Number UA @ lucian @ c:irua:105292 Serial 1538
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Author Quintana, M.; López, A.M.; Rapino, S.; Toma, F.M.; Iurlo, M.; Carraro, M.; Sartorel, A.; Maccato, C.; Ke, X.; Bittencourt, C.; Da Ros, T.; Van Tendeloo, G.; Marcaccio, M.; Paolucci, F.; Prato, M.; Bonchio, M.;
Title Knitting the catalytic pattern of artificial photosynthesis to a hybrid graphene nanotexture Type A1 Journal article
Year 2013 Publication ACS nano Abbreviated Journal Acs Nano
Volume 7 Issue 1 Pages 811-817
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract The artificial leaf project calls for new materials enabling multielectron catalysis with minimal overpotential, high turnover frequency, and long-term stability. Is graphene a better material than carbon nanotubes to enhance water oxidation catalysis for energy applications? Here we show that functionalized graphene with a tailored distribution of polycationic, quaternized, ammonium pendants provides an sp(2) carbon nanoplatform to anchor a totally inorganic tetraruthenate catalyst, mimicking the oxygen evolving center of natural PSII. The resulting hybrid material displays oxygen evolution at overpotential as low as 300 mV at neutral pH with negligible loss of performance after 4 h testing. This multilayer electroactive asset enhances the turnover frequency by 1 order of magnitude with respect to the isolated catalyst, and provides a definite up-grade of the carbon nanotube material, with a similar surface functionalization. Our innovation is based on a noninvasive, synthetic protocol for graphene functionalization that goes beyond the ill-defined oxidation-reduction methods, allowing a definite control of the surface properties.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000314082800088 Publication Date 2012-12-17
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.942 Times cited 69 Open Access
Notes 246791 COUNTATOMS; 262348 ESMI; ESF Cost Action NanoTP MP0901 Approved Most recent IF: 13.942; 2013 IF: 12.033
Call Number UA @ lucian @ c:irua:107707 Serial 1766
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Author Quintana, M.; Ke, X.; Van Tendeloo, G.; Meneghetti, M.; Bittencourt, C.; Prato, M.
Title Light-induced selective deposition of Au nanoparticles on single-wall carbon nanotubes Type A1 Journal article
Year 2010 Publication ACS nano Abbreviated Journal Acs Nano
Volume 4 Issue 10 Pages 6105-6113
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Novel applications of single-walled carbon nanotubes (SWNT) rely on the development of new strategies to make them easier to handle without affecting their structural properties. In this work, we have selectively deposited Au nanoparticles (Au NP) on SWNT assisted by UV light irradiation. XPS analysis and UV-vis spectroscopy indicate that the deposition occurs at the defects generated after oxidation of the SWNT. By addition of n-dodecylthiol, the separation of oxidized tubes with Au NP (Au-ox-SWNT) from tubes devoid of Au NP (bare tubes, b-SWNT) was achieved. Raman and UV-vis-NIR spectra indicate that UV irradiation induces a faster nucleation of Au NP on metallic SWNT. This new technique can be useful for the preparation of nanohybrid composites with enhanced properties, as increased thermal stability, and to obtain purified SWNT.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000283453700081 Publication Date 2010-09-24
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.942 Times cited 26 Open Access
Notes Approved Most recent IF: 13.942; 2010 IF: 9.865
Call Number UA @ lucian @ c:irua:99202 Serial 1819
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Author Walter, A.L.; Sahin, H.; Jeon, K.J.; Bostwick, A.; Horzum, S.; Koch, R.; Speck, F.; Ostler, M.; Nagel, P.; Merz, M.; Schupler, S.; Moreschini, L.; Chang, Y.J.; Seyller, T.; Peeters, F.M.; Horn, K.; Rotenberg, E.;
Title Luminescence, patterned metallic regions, and photon-mediated electronic changes in single-sided fluorinated graphene sheets Type A1 Journal article
Year 2014 Publication ACS nano Abbreviated Journal Acs Nano
Volume 8 Issue 8 Pages 7801-7808
Keywords A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Abstract Single-sided fluorination has been predicted to open an electronic band gap in graphene and to exhibit unique electronic and magnetic properties; however, this has not been substantiated by experimental reports. Our comprehensive experimental and theoretical study of this material on a SiC(0001) substrate shows that single-sided fluorographene exhibits two phases, a stable one with a band gap of similar to 6 eV and a metastable one, induced by UV irradiation, with a band gap of similar to 2.5 eV. The metastable structure, which reverts to the stable “ground-state” phase upon annealing under emission of blue light, in our view is induced by defect states, based on the observation of a nondispersive electronic state at the top of the valence band, not unlike that found in organic molecular layers. Our structural data show that the stable C2F ground state has a “boat” structure, in agreement with our X-ray magnetic circular dichroism data, which show the absence of an ordered magnetic phase. A high flux of UV or X-ray photons removes the fluorine atoms, demonstrating the possibility of lithographically patterning conducting regions into an otherwise semiconducting 2D material.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000340992300025 Publication Date 2014-08-09
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.942 Times cited 23 Open Access
Notes Approved Most recent IF: 13.942; 2014 IF: 12.881
Call Number UA @ lucian @ c:irua:119263 Serial 1857
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Author Felten, A.; Gillon, X.; Gulas, M.; Pireaux, J.-J.; Ke, X.; Van Tendeloo, G.; Bittencourt, C.; Najafi, E.; Hitchcock, A.P.
Title Measuring point defect density in individual carbon nanotubes using polarization-dependent X-ray microscopy Type A1 Journal article
Year 2010 Publication ACS nano Abbreviated Journal Acs Nano
Volume 4 Issue 8 Pages 4431-4436
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The presence of defects in carbon nanotubes strongly modifies their electrical, mechanical, and chemical properties. It was long thought undesirable, but recent experiments have shown that introduction of structural defects using ion or electron irradiation can lead to novel nanodevices. We demonstrate a method for detecting and quantifying point defect density in individual carbon nanotubes (CNTs) based on measuring the polarization dependence (linear dichroism) of the C 1s → π* transition at specific locations along individual CNTs with a scanning transmission X-ray microscope (STXM). We show that STXM can be used to probe defect density in individual CNTs with high spatial resolution. The quantitative relationship between ion dose, nanotube diameter, and defect density was explored by purposely irradiating selected sections of nanotubes with kiloelectronvolt (keV) Ga+ ions. Our results establish polarization-dependent X-ray microscopy as a new and very powerful characterization technique for carbon nanotubes and other anisotropic nanostructures.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000281052700014 Publication Date 2010-07-07
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.942 Times cited 26 Open Access
Notes Approved Most recent IF: 13.942; 2010 IF: 9.865
Call Number UA @ lucian @ c:irua:84734 Serial 1966
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Author Yan, Y.; Zhou, X.; Jin, H.; Li, C.-Z.; Ke, X.; Van Tendeloo, G.; Liu, K.; Yu, D.; Dressel, M.; Liao, Z.-M.
Title Surface-Facet-Dependent Phonon Deformation Potential in Individual Strained Topological Insulator Bi2Se3 Nanoribbons Type A1 Journal article
Year 2015 Publication ACS nano Abbreviated Journal Acs Nano
Volume 9 Issue 9 Pages 10244-10251
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Strain is an important method to tune the properties of topological insulators. For example, compressive strain can induce superconductivity in Bi2Se3 bulk material. Topological insulator nanostructures are the superior candidates to utilize the unique surface states due to the large surface to volume ratio. Therefore, it is highly desirable to monitor the local strain effects in individual topological insulator nanostructures. Here, we report the systematical micro-Raman spectra of single strained Bi2Se3 nanoribbons with different thicknesses and different surface facets, where four optical modes are resolved in both Stokes and anti-Stokes Raman spectral lines. A striking anisotropy of the strain dependence is observed in the phonon frequency of strained Bi2Se3 nanoribbons grown along the ⟨112̅0⟩ direction. The frequencies of the in-plane Eg2 and out-of-plane A1g1 modes exhibit a nearly linear blue-shift against bending strain when the nanoribbon is bent along the ⟨112̅0⟩ direction with the curved {0001} surface. In this case, the phonon deformation potential of the Eg2 phonon for 100 nm-thick Bi2Se3 nanoribbon is up to 0.94 cm–1/%, which is twice of that in Bi2Se3 bulk material (0.52 cm–1/%). Our results may be valuable for the strain modulation of individual topological insulator nanostructures.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language English Wos 000363915300079 Publication Date 2015-09-12
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.942 Times cited 14 Open Access
Notes Y.Y. would like to thank Xuewen Fu for helpful discussions. This work was supported by MOST (Nos. 2013CB934600, 2013CB932602) and NSFC (Nos. 11274014, 11234001). Approved Most recent IF: 13.942; 2015 IF: 12.881
Call Number c:irua:129216 Serial 3963
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Author Chen, J.J.; Wang, Q.; Meng, J.; Ke, X.; Van Tendeloo, G.; Bie, Y.Q.; Liu, J.; Liu, K.; Liao, Z.M.; Sun, D.; Yu, D.;
Title Photovoltaic effect and evidence of carrier multiplication in graphene vertical homojunctions with asymmetrical metal contacts Type A1 Journal article
Year 2015 Publication ACS nano Abbreviated Journal Acs Nano
Volume 9 Issue 9 Pages 8851-8858
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Graphene exhibits exciting potentials for high-speed wideband photodetection and high quantum efficiency solar energy harvest because of its broad spectral absorption, fast photoelectric response, and potential carrier multiplication. Although photocurrent can be generated near a metalgraphene interface in lateral devices, the photoactive area is usually limited to a tiny one-dimensional line-like interface region. Here, we report photoelectric devices based on vertical graphene two-dimensional homojunction, which is fabricated via vertically stacking four graphene monolayers with asymmetric metal contacts. The devices show excellent photovoltaic output with excitation wavelength ranging from visible light to mid-infrared. The wavelength dependence of the internal quantum efficiency gives direct evidence of the carrier multiplication effect in graphene. The simple fabrication process, easy scale-up, large photoresponsive active area, and broadband response of the vertical graphene device are very promising for practical applications in optoelectronics and photovoltaics.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000361935800023 Publication Date 2015-08-15
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.942 Times cited 11 Open Access
Notes 246791 Countatoms Approved Most recent IF: 13.942; 2015 IF: 12.881
Call Number c:irua:127689 Serial 2615
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Author El-Gogary, R.I.; Rubio, N.; Wang, J.T.W.; Al-Jamal, W.T.; Bourgognon, M.; Kafa, H.; Naeem, M.; Klippstein, R.; Abbate, V.; Leroux, F.; Bals, S.; Van Tendeloo, G.; Kamel, A.O.; Awad, G.A.S.; Mortada, N.D.; Al-Jamal, K.T.;
Title Polyethylene glycol conjugated polymeric nanocapsules for targeted delivery of quercetin to folate-expressing cancer cells in vitro and in vivo Type A1 Journal article
Year 2014 Publication ACS nano Abbreviated Journal Acs Nano
Volume 8 Issue 2 Pages 1384-1401
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract In this work we describe the formulation and characterization of chemically modified polymeric nanocapsules incorporating the anticancer drug, quercetin, for the passive and active targeting to tumors. Folic acid was conjugated to poly(lactide-co-glycolide) (PLGA) polymer to facilitate active targeting to cancer cells. Two different methods for the conjugation of PLGA to folic acid were employed utilizing polyethylene glycol (PEG) as a spacer. Characterization of the conjugates was performed using FTIR and H-1 NMR studies. The PEG and folk acid content was independent of the conjugation methodology employed. PEGylation has shown to reduce the size of the nanocapsule; moreover, zeta-potential was shown to be polymer-type dependent. Comparative studies on the cytotoxicity and cellular uptake of the different formulations by He La cells, in the presence and absence of excess folic acid, were carried out using MTT assay and Confocal Laser Scanning Microscopy, respectively. Both results confirmed the selective uptake and cytotoxicity of the folic acid targeted nanocapsules to the folate enriched cancer cells in a folate-dependent manner. Finally, the passive tumor accumulation and the active targeting of the nanocapsules to folate-expressing cells were confirmed upon intravenous administration in He La or IGROV-1 tumor-bearing mice. The developed nanocapsules provide a system for targeted delivery of a range of hydrophobic anticancer drugs in vivo.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000332059200032 Publication Date 2014-01-07
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.942 Times cited 144 Open Access Not_Open_Access
Notes 290023 Raddel; 262348 Esmi; Iap-Pai Approved Most recent IF: 13.942; 2014 IF: 12.881
Call Number UA @ lucian @ c:irua:115862 Serial 2670
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