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Author |
Zhuo, X.; Mychinko, M.; Heyvaert, W.; Larios, D.; Obelleiro-Liz, M.; Taboada, J.M.; Bals, S.; Liz-Marzán, L.M. |
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Title |
Morphological and Optical Transitions during Micelle-Seeded Chiral Growth on Gold Nanorods |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
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Issue |
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Pages |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Chiral plasmonics is a rapidly developing field where breakthroughs and unsolved problems coexist. We have recently reported binary surfactant-assisted seeded growth of chiral gold nanorods (Au NRs) with high chiroptical activity. Such a seeded-growth process involves the use of a chiral cosurfactant that induces micellar helicity, in turn driving the transition from achiral to chiral Au NRs, from both the morphological and the optical points of view. We report herein a detailed study on both transitions, which reveals intermediate states that were hidden so far. The correlation between structure and optical response is carefully analyzed, including the (linear and CD) spectral evolution over time, electron tomography, the impact of NR dimensions on their optical response, the variation of the absorption-to-scattering ratio during the evolution from achiral to chiral Au NRs, and the near-field enhancement related to chiral plasmon modes. Our findings provide further understanding of the growth process of chiral Au NRs and the associated optical changes, which will facilitate further study and applications of chiral nanomaterials. |
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Wos |
000878324400001 |
Publication Date |
2022-10-26 |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN  |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
17.1 |
Times cited |
17 |
Open Access |
OpenAccess |
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Notes |
This work was supported by the European Research Council (ERC-AdG-4DbioSERS-787510 to L.M.L.-M. and ERC-CoG-REALNANO-815128 to S.B.) and the MCIN/AEI/10.13039/501100011033 (Grant PID2020-117779RB-I00). X.Z. acknowledges funding from the Juan de la Cierva fellowship (FJC2018-036104-I) and the University Development Fund (UDF01002665, CUHK-Shenzhen). D.L., M.O.-L., and J.M.T. acknowledge funding from the European Regional Development Fund (ERDF) and the Spanish Ministerio de Ciencia, Innovación y Universidades, under Projects PID2020-116627RB-C21 and PID2020-116627RB-C22, as well as from the ERDF/Galician Regional Government as part of the agreement for funding the Atlantic Research Center for Information and Communication Technologies (atlanTTic) and ERDF/Extremadura Regional Government under Projects IB18073 and GR18055. This work was performed in the framework of the Maria de Maeztu Units of Excellence Program from the Spanish State Research Agency (Grant No. MDM-2017-0720). The authors acknowledge Dr. Guillermo González-Rubio for providing suggestions for synthesis and Dr. Irantzu Llarena for assisting with the CD measurements. |
Approved |
Most recent IF: 17.1 |
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Call Number |
EMAT @ emat @c:irua:191815 |
Serial |
7116 |
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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. |
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Title |
Color-switchable nanosilicon fluorescent probes |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
16 |
Issue |
9 |
Pages |
15450-15459 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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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. |
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Wos |
000861080700001 |
Publication Date |
2022-09-15 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
17.1 |
Times cited |
1 |
Open Access |
Not_Open_Access |
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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 |
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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. |
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Title |
Extracting pure circular dichroism from hierarchically structured CdS magic cluster films |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
16 |
Issue |
12 |
Pages |
20457-20469 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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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. |
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Wos |
000888219600001 |
Publication Date |
2022-11-17 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
17.1 |
Times cited |
8 |
Open Access |
Not_Open_Access |
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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 |
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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. |
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Title |
Tunable circularly polarized luminescence via chirality induction and energy transfer from organic films to semiconductor nanocrystals |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
16 |
Issue |
11 |
Pages |
18472-18482 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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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. |
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Wos |
000883943600001 |
Publication Date |
2022-11-07 |
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Series Editor |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
17.1 |
Times cited |
10 |
Open Access |
OpenAccess |
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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 |
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Call Number |
UA @ admin @ c:irua:192101 |
Serial |
7345 |
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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. |
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Title |
Charging of vitreous samples in cryogenic electron microscopy mitigated by graphene |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
ACS nano |
Abbreviated Journal |
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Volume |
17 |
Issue |
16 |
Pages |
15836-15846 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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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. |
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Wos |
001041649900001 |
Publication Date |
2023-08-02 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
17.1 |
Times cited |
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Open Access |
OpenAccess |
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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 |
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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. |
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Title |
Electrochemical stability of rhodium-platinum core-shell nanoparticles : an identical location scanning transmission electron microscopy study |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
ACS nano |
Abbreviated Journal |
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Volume |
17 |
Issue |
17 |
Pages |
16943-16951 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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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. |
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Wos |
001051495900001 |
Publication Date |
2023-08-21 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
17.1 |
Times cited |
2 |
Open Access |
OpenAccess |
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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 |
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Call Number |
UA @ admin @ c:irua:199253 |
Serial |
8859 |
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Author |
Vlasov, E.; Heyvaert, W.; Ni, B.; Van Gordon, K.; Girod, R.; Verbeeck, J.; Liz-Marzán, L.M.; Bals, S. |
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Title |
High-Throughput Morphological Chirality Quantification of Twisted and Wrinkled Gold Nanorods |
Type |
A1 Journal Article |
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Year |
2024 |
Publication |
ACS Nano |
Abbreviated Journal |
ACS Nano |
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Volume |
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Issue |
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Pages |
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Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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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. |
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Wos |
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Publication Date |
2024-04-26 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
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Impact Factor |
17.1 |
Times cited |
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Open Access |
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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 |
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Call Number |
EMAT @ emat @ |
Serial |
9121 |
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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. |
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Title |
Air- and water-resistant noble metal coated ferromagnetic cobalt nanorods |
Type |
A1 Journal article |
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Year |
2015 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
9 |
Issue |
9 |
Pages |
2792-2804 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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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. |
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Wos |
000351791800055 |
Publication Date |
2015-03-03 |
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Abbreviated Series Title |
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ISSN |
1936-0851;1936-086X; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
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 |
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| |
Call Number |
c:irua:125380 c:irua:125380 |
Serial |
87 |
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| Permanent link to this record |
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| |
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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. |
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| |
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 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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| |
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. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000353867000030 |
Publication Date |
2015-03-12 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
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 |
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| |
Call Number |
c:irua:125978 |
Serial |
434 |
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| Permanent link to this record |
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Author |
Bertoni, G.; Grillo, V.; Brescia, R.; Ke, X.; Bals, S.; Catellani, A.; Li, H.; Manna, L. |
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| |
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 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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| |
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. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000306673800079 |
Publication Date |
2012-06-18 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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| |
ISSN |
1936-0851;1936-086X; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
13.942 |
Times cited |
63 |
Open Access |
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| |
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 |
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| |
Call Number |
UA @ lucian @ c:irua:101138 |
Serial |
710 |
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| Permanent link to this record |
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Author |
Sanz-Ortiz, M.N.; Sentosun, K.; Bals, S.; Liz-Marzan, L.M. |
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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 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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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. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
English |
Wos |
000363915300105 |
Publication Date |
2015-09-15 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
|
Edition |
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| |
ISSN |
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 |
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| |
Call Number |
c:irua:129194 |
Serial |
3947 |
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| Permanent link to this record |
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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.; |
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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 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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| |
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. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000312563600070 |
Publication Date |
2012-11-28 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
|
Edition |
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| |
ISSN |
1936-0851;1936-086X; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
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 |
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| |
Call Number |
UA @ lucian @ c:irua:105292 |
Serial |
1538 |
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| Permanent link to this record |
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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.; |
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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 |
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| |
Volume |
8 |
Issue |
2 |
Pages |
1384-1401 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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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. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000332059200032 |
Publication Date |
2014-01-07 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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| |
ISSN |
1936-0851;1936-086X; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
13.942 |
Times cited |
144 |
Open Access |
Not_Open_Access |
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| |
Notes |
290023 Raddel; 262348 Esmi; Iap-Pai |
Approved |
Most recent IF: 13.942; 2014 IF: 12.881 |
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| |
Call Number |
UA @ lucian @ c:irua:115862 |
Serial |
2670 |
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| Permanent link to this record |
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Author |
Galván-Moya, J.E.; Altantzis, T.; Nelissen, K.; Peeters, F.M.; Grzelczak, M.; Liz-Marán, L.M.; Bals, S.; Van Tendeloo, G. |
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Title |
Self-organization of highly symmetric nanoassemblies : a matter of competition |
Type |
A1 Journal article |
| |
Year |
2014 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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| |
Volume |
8 |
Issue |
4 |
Pages |
3869-3875 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT) |
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Abstract |
The properties and applications of metallic nanoparticles are inseparably connected not only to their detailed morphology and composition but also to their structural configuration and mutual interactions. As a result, the assemblies often have superior properties as compared to individual nanoparticles. Although it has been reported that nanoparticles can form highly symmetric clusters, if the configuration can be predicted as a function of the synthesis parameters, more targeted and accurate synthesis will be possible. We present here a theoretical model that accurately predicts the structure and configuration of self-assembled gold nanoclusters. The validity of the model is verified using quantitative experimental data extracted from electron tomography 3D reconstructions of different assemblies. The present theoretical model is generic and can in principle be used for different types of nanoparticles, providing a very wide window of potential applications. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000334990600084 |
Publication Date |
2014-03-13 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
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| |
ISSN |
1936-0851;1936-086X; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
13.942 |
Times cited |
34 |
Open Access |
OpenAccess |
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| |
Notes |
FWO; Methusalem; 246791 COUNTATOMS; 335078 COLOURATOM; 262348 ESMI; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 13.942; 2014 IF: 12.881 |
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Call Number |
UA @ lucian @ c:irua:116955 |
Serial |
2977 |
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| Permanent link to this record |
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Author |
Groeneveld, E.; Witteman, L.; Lefferts, M.; Ke, X.; Bals, S.; Van Tendeloo, G.; de Mello Donega, C. |
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Title |
Tailoring ZnSe-CdSe colloidal quantum dots via cation exchange : from core/shell to alloy nanocrystals |
Type |
A1 Journal article |
| |
Year |
2013 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
|
| |
Volume |
7 |
Issue |
9 |
Pages |
7913-7930 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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| |
Abstract |
We report a study of Zn2+ by Cd2+ cation exchange (CE) in colloidal ZnSe nanocrystals (NCs). Our results reveal that CE in ZnSe NCs is a thermally activated isotropic process. The CE efficiency (i.e., fraction of Cd2+ ions originally in solution, Cdsol, that is incorporated in the ZnSe NC) increases with temperature and depends also on the Cdsol/ZnSe ratio. Interestingly, the reaction temperature can be used as a sensitive parameter to tailor both the composition and the elemental distribution profile of the product (Zn,Cd)Se NCs. At 150 °C ZnSe/CdSe core/shell hetero-NCs (HNCs) are obtained, while higher temperatures (200 and 220 °C) produce (Zn1xCdx)Se gradient alloy NCs, with increasingly smoother gradients as the temperature increases, until homogeneous alloy NCs are obtained at T ≥ 240 °C. Remarkably, sequential heating (150 °C followed by 220 °C) leads to ZnSe/CdSe core/shell HNCs with thicker shells, rather than (Zn1xCdx)Se gradient alloy NCs. Thermal treatment at 250 °C converts the ZnSe/CdSe core/shell HNCs into (Zn1xCdx)Se homogeneous alloy NCs, while preserving the NC shape. A mechanism for the cation exchange in ZnSe NCs is proposed, in which fast CE takes place at the NC surface, and is followed by relatively slower thermally activated solid-state cation diffusion, which is mediated by Frenkel defects. The findings presented here demonstrate that cation exchange in colloidal ZnSe NCs provides a very sensitive tool to tailor the nature and localization regime of the electron and hole wave functions and the optoelectronic properties of colloidal ZnSeCdSe NCs. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000330016900051 |
Publication Date |
2013-08-13 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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| |
ISSN |
1936-0851;1936-086X; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
13.942 |
Times cited |
153 |
Open Access |
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| |
Notes |
262348 Esmi; 246791 Countatoms |
Approved |
Most recent IF: 13.942; 2013 IF: 12.033 |
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Call Number |
UA @ lucian @ c:irua:110038 |
Serial |
3469 |
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| Permanent link to this record |
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Author |
Goris, B.; Turner, S.; Bals, S.; Van Tendeloo, G. |
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Title |
Three-dimensional valency mapping in ceria nanocrystals |
Type |
A1 Journal article |
| |
Year |
2014 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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| |
Volume |
8 |
Issue |
10 |
Pages |
10878-10884 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Using electron tomography combined with electron energy loss spectroscopy (EELS), we are able to map the valency of the Ce ions in CeO2-x nanocrystals in three dimensions. Our results show a clear facet-dependent reduction shell at the surface of ceria nanoparticles; {111} surface facets show a low surface reduction, whereas at {001} surface facets, the cerium ions are more likely to be reduced over a larger surface shell. Our generic tomographic technique allows a full 3D data cube to be reconstructed, containing an EELS spectrum in each voxel. This possibility enables a three-dimensional investigation of a plethora of material-specific physical properties such as valency, chemical composition, oxygen coordination, or bond lengths, triggering the synthesis of nanomaterials with improved properties. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000343952600126 |
Publication Date |
2014-10-06 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
|
Edition |
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| |
ISSN |
1936-0851;1936-086X; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
13.942 |
Times cited |
85 |
Open Access |
OpenAccess |
|
| |
Notes |
335078 Colouratom; 246791 Countatoms; Fwo; 312483 Esteem2; esteem2jra4; ECASSara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 13.942; 2014 IF: 12.881 |
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| |
Call Number |
UA @ lucian @ c:irua:121219 |
Serial |
3656 |
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| Permanent link to this record |
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Author |
van der Stam, W.; Bladt, E.; Rabouw, F.T.; Bals, S.; de Mello Donega, C. |
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Title |
Near-Infrared Emitting CuInSe/CuInS Dot Core/Rod Shell Heteronanorods by Sequential Cation Exchange |
Type |
A1 Journal article |
| |
Year |
2015 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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| |
Volume |
9 |
Issue |
9 |
Pages |
11430-11438 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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| |
Abstract |
The direct synthesis of heteronanocrystals (HNCs) combining different ternary semiconductors is challenging and has not yet been successful. Here, we report a sequential topotactic cation exchange (CE) pathway that yields CuInSe2/CuInS2 dot core/rod shell nanorods with near-infrared luminescence. In our approach, the Cu+ extraction rate is coupled to the In3+ incorporation rate by the use of a stoichiometric trioctylphosphine-InCl3 complex, which fulfills the roles of both In-source and Cu-extracting agent. In this way, Cu+ ions can be extracted by trioctylphosphine ligands only when the In-P bond is broken. This results in readily available In3+ ions at the same surface site from which the Cu+ is extracted, making the process a direct place exchange reaction and shifting the overall energy balance in favor of the CE. Consequently, controlled cation exchange can occur even in large and anisotropic heterostructured nanocrystals with preservation of the size, shape, and heterostructuring of the template NCs into the product NCs. The cation exchange is self-limited, stopping when the ternary core/shell CuInSe2/CuInS2 composition is reached. The method is very versatile, successfully yielding a variety of luminescent CuInX2 (X = S, Se, and Te) quantum dots, nanorods, and HNCs, by using Cd-chalcogenide NCs and HNCs as templates. The approach reported here thus opens up routes toward materials with unprecedented properties, which would otherwise remain inaccessible. |
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| |
Address |
Debye Institute for Nanomaterials Science, Utrecht University , P.O. Box 80000, 3508 TA Utrecht, The Netherlands |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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| |
Language |
English |
Wos |
000365464800094 |
Publication Date |
2015-10-09 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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| |
Series Volume |
|
Series Issue |
|
Edition |
|
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| |
ISSN |
1936-0851;1936-086X; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
13.942 |
Times cited |
88 |
Open Access |
OpenAccess |
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| |
Notes |
The authors thank Gang Wang for XRD measurements and Eline Hutter for providing CdSe/CdS NRs. W.v.d.S. and C.d.M.D. acknowledge financial support from the division of Chemical Sciences (CW) of The Netherlands Organization for Scientific Research (NWO) under grant number ECHO.712.012.001. This work was supported by the European Research Council (ERC Starting Grant #335078 Colouratom). E.B. gratefully acknowledges financial support by the Flemish Fund for Scientific Research (FWO Vlaanderen).; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 13.942; 2015 IF: 12.881 |
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| |
Call Number |
c:irua:129184 |
Serial |
3948 |
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Author |
Schrittwieser, S.; Pelaz, B.; Parak, W.J.; Lentijo-Mozo, S.; Soulantica, K.; Dieckhoff, J.; Ludwig, F.; Altantzis, T.; Bals, S.; Schotter, J. |
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Title |
Homogeneous Protein Analysis by Magnetic Core-Shell Nanorod Probes |
Type |
A1 Journal article |
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Year |
2016 |
Publication |
ACS applied materials and interfaces |
Abbreviated Journal |
Acs Appl Mater Inter |
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Volume |
8 |
Issue |
8 |
Pages |
8893-8899 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Studying protein interactions is of vital importance both to fundamental biology research and to medical applications. Here, we report on the experimental proof of a universally applicable label-free homogeneous platform for rapid protein analysis. It is based on optically detecting changes in the rotational dynamics of magnetically agitated core-shell nanorods upon their specific interaction with proteins. By adjusting the excitation frequency, we are able to optimize the measurement signal for each analyte protein size. In addition, due to the locking of the optical signal to the magnetic excitation frequency, background signals are suppressed, thus allowing exclusive studies of processes at the nanoprobe surface only. We study target proteins (soluble domain of the human epidermal growth factor receptor 2 – sHER2) specifically binding to antibodies (trastuzumab) immobilized on the surface of our nanoprobes and demonstrate direct deduction of their respective sizes. Additionally, we examine the dependence of our measurement signal on the concentration of the analyte protein, and deduce a minimally detectable sHER2 concentration of 440 pM. For our homogeneous measurement platform, good dispersion stability of the applied nanoprobes under physiological conditions is of vital importance. To that end, we support our measurement data by theoretical modeling of the total particle-particle interaction energies. The successful implementation of our platform offers scope for applications in biomarker-based diagnostics as well as for answering basic biology questions. |
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Address |
Molecular Diagnostics, AIT Austrian Institute of Technology , Vienna, Austria |
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Language |
English |
Wos |
000374274900007 |
Publication Date |
2016-03-29 |
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Series Issue |
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Edition |
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ISSN |
1944-8244 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7.504 |
Times cited |
16 |
Open Access |
OpenAccess |
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Notes |
The authors thank Frauke Alves, Julia Bode and Fernanda Ramos Gomes from the Max-Planck-Institute of Experimental Medicine in Göttingen for providing the trastuzumab antibody in form of the Herceptin therapeutic drug. The figure showing the measurement principle has been created by Darragh Crotty (www.darraghcrotty.com). Parts of this research were supported by the European Commission FP7 NAMDIATREAM project (EU NMP4-LA-2010−246479), by the German research foundation (DFG grant GRK 1782 to W.J.P.), and by the European Research Council (ERC Starting Grant #335078 Colouratom). B.P. acknowledges a PostDoctoral fellowship from the Alexander von Humboldt foundation. (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); ; ECAS_Sara; |
Approved |
Most recent IF: 7.504 |
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Call Number |
c:irua:132889 |
Serial |
4059 |
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Author |
Ustarroz, J.; Geboes, B.; Vanrompay, H.; Sentosun, K.; Bals, S.; Breugelmans, T.; Hubin, A. |
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Title |
Electrodeposition of Highly Porous Pt Nanoparticles Studied by Quantitative 3D Electron Tomography: Influence of Growth Mechanisms and Potential Cycling on the Active Surface Area |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
ACS applied materials and interfaces |
Abbreviated Journal |
Acs Appl Mater Inter |
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Volume |
9 |
Issue |
9 |
Pages |
16168-16177 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
Nanoporous Pt nanoparticles (NPs) are promising fuel cell catalysts due to their large surface area and increased electrocatalytic activity towards the oxygen reduction reaction (ORR). Herein, we report on the infuence of the growth mechanisms on the surface properties of electrodeposited Pt dendritic NPs with large surface areas. The electrochemically active surface was studied by hydrogen underpotential deposition (HUPD) and compared for the rst time to high angle annular dark eld scanning transmission electron microscopy (HAADF-STEM) quantitative 3D electron tomography of individual nanoparticles. Large nucleation overpotential leads to a large surface coverage of Pt roughened spheroids, which provide large roughness factor (Rf ) but low mass-speci c electrochemically active surface area (EASA). Lowering the nucleation overpotential leads to highly porous Pt NPs with pores protruding to the center of the structure. At the expense of smaller Rf , the obtained EASA values of these structures are in the range of these of large surface area supported fuel cell catalysts. The active surface area of the Pt dendritic NPs was measured by electron tomography and it was found that the potential cycling in the H adsorption/desorption and Pt oxidation/reduction region, which is generally performed to determine the EASA, leads to a signi cant reduction of that surface area due to a partial collapse of their dendritic and porous morphology. Interestingly, the extrapolation of the microscopic tomography results to macroscopic electrochemical parameters indicated that the surface properties measured by H UPD are comparable to the values measured on individual NPs by electron tomography after the degradation caused by the H UPD measurement. These results highlight that the combination of electrochemical and quantitative 3D surface analysis techniques is essential to provide insights into the surface properties, the electrochemical stability and, hence, the applicability of these materials. Moreover, it indicates that care must be taken with widely used electrochemical methods of surface area determination, especially in the case of large surface area and possibly unstable nanostructures, since the measured surface can be strongly a ected by the measurement itself. |
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Wos |
000401782500028 |
Publication Date |
2017-04-18 |
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Series Editor |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1944-8244 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7.504 |
Times cited |
24 |
Open Access |
OpenAccess |
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Notes |
Jon Ustarroz acknowledges funding from the Fonds Wetenschappelijk Onderzoek in Flanders (FWO, postdoctoral grant 12I7816N). S. Bals acknowledges funding from the European Research Council (Starting Grant No. COLOURATOMS 335078). S.B. and T.B. acknowledge the University of Antwerp for nancial support in the frame of a GOA project. H.V. gratefully acknowledges nancial support by the Flemish Fund for Scienti c Research (FWO Vlaanderen). All the authors acknowledge Laurens Stevaert for his contribution to the work presented in this manuscript. (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); ECAS_Sara |
Approved |
Most recent IF: 7.504 |
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Call Number |
EMAT @ emat @ c:irua:142345UA @ admin @ c:irua:142345 |
Serial |
4552 |
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Author |
Kurttepeli, M.; Deng, S.; Mattelaer, F.; Cott, D.J.; Vereecken, P.; Dendooven, J.; Detavernier, C.; Bals, S. |
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Title |
Heterogeneous TiO2/V2O5/Carbon Nanotube Electrodes for Lithium-Ion Batteries |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
ACS applied materials and interfaces |
Abbreviated Journal |
Acs Appl Mater Inter |
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Volume |
9 |
Issue |
9 |
Pages |
8055-8064 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Vanadium pentoxide (V2O5) is proposed and investigated as a cathode material for lithium-ion (Li-ion) batteries. However, the dissolution of V2O5 during the charge/discharge remains as an issue at the V2O5–electrolyte interface. In this work, we present a heterogeneous nanostructure with carbon nanotubes supported V2O5/titanium dioxide (TiO2) multilayers as electrodes for thin-film Li-ion batteries. Atomic layer deposition of V2O5 on carbon nanotubes provides enhanced Li storage capacity and high rate performance. An additional TiO2 layer leads to increased morphological stability and in return higher electrochemical cycling performance of V2O5/carbon nanotubes. The physical and chemical properties of TiO2/V2O5/carbon nanotubes are characterized by cyclic voltammetry and charge/discharge measurements as well as electron microscopy. The detailed mechanism of the protective TiO2 layer to improve the electrochemical cycling stability of the V2O5 is unveiled. |
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Wos |
000396186000021 |
Publication Date |
2017-03-08 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1944-8244 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7.504 |
Times cited |
28 |
Open Access |
OpenAccess |
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Notes |
European Research Council, 239865 335078 ; Fonds Wetenschappelijk Onderzoek; Agentschap voor Innovatie door Wetenschap en Technologie, 18142 ; Bijzonder Onderzoeksfonds, GOA – 01G01513 ; This research was funded by the Flemish research foundation FWO-Vlaanderen, by the European Research Council (Starting Grant No. 239865 and No. 335078), by IWT-Flanders (SBO project IWT 18142 “SoS-Lion”) and by the Special Research Fund BOF of Ghent University (GOA – 01G01513); colouratoms (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); ECAS_Sara |
Approved |
Most recent IF: 7.504 |
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Call Number |
EMAT @ emat @ c:irua:142446UA @ admin @ c:irua:142446 |
Serial |
4572 |
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Author |
Asapu, R.; Ciocarlan, R.-G.; Claes, N.; Blommaerts, N.; Minjauw, M.; Ahmad, T.; Dendooven, J.; Cool, P.; Bals, S.; Denys, S.; Detavernier, C.; Lenaerts, S.; Verbruggen, S.W. |
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Title |
Plasmonic Near-Field Localization of Silver Core–Shell Nanoparticle Assemblies via Wet Chemistry Nanogap Engineering |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
ACS applied materials and interfaces |
Abbreviated Journal |
Acs Appl Mater Inter |
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Volume |
9 |
Issue |
9 |
Pages |
41577-41585 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL) |
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Abstract |
Silver nanoparticles are widely used in the field of plasmonics because of their unique optical properties. The wavelength-dependent surface plasmon resonance gives rise to a strongly enhanced electromagnetic field, especially at so-called hot spots located in the nanogap in-between metal nanoparticle assemblies. Therefore, the interparticle distance is a decisive factor in plasmonic applications, such as surface-enhanced Raman spectroscopy (SERS). In this study, the aim is to engineer this interparticle distance for silver nanospheres using a convenient wet-chemical approach and to predict and quantify the corresponding enhancement factor using both theoretical and experimental tools. This was done by building a tunable ultrathin polymer shell around the nanoparticles using the layer-by-layer method, in which the polymer shell acts as the separating interparticle spacer layer. Comparison of different theoretical approaches and corroborating the results with SERS analytical experiments using silver and silver−polymer core−shell nanoparticle clusters as SERS substrates was also done. Herewith, an approach is provided to estimate the extent of plasmonic near-field enhancement both theoretically as well as experimentally. |
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Wos |
000417005900057 |
Publication Date |
2017-11-29 |
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Series Editor |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1944-8244 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7.504 |
Times cited |
29 |
Open Access |
OpenAccess |
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Notes |
financial support through a research fellowship. C.D. wishes to thank the Hercules foundation for the financial support (SPINAL). P.C. and R.-G.C. acknowledge financial support by FWO Vlaanderen (project no. G038215N). N.C. and S.B. acknowledge the financial support from the European Research Council (ERC starting grant #335078-COLOURATOM). (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); saraecas; ECAS_Sara; |
Approved |
Most recent IF: 7.504 |
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Call Number |
EMAT @ emat @c:irua:147243 |
Serial |
4804 |
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Author |
Ben Dkhil, S.; Pfannmöller, M.; Schroeder, R.R.; Alkarsifi, R.; Gaceur, M.; Koentges, W.; Heidari, H.; Bals, S.; Margeat, O.; Ackermann, J.; Videlot-Ackermann, C. |
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Title |
Interplay of interfacial layers and blend composition to reduce thermal degradation of polymer solar cells at high temperature |
Type |
A1 Journal article |
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Year |
2018 |
Publication |
ACS applied materials and interfaces |
Abbreviated Journal |
Acs Appl Mater Inter |
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Volume |
10 |
Issue |
10 |
Pages |
3874-3884 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
The thermal stability of printed polymer solar cells at elevated temperatures needs to be improved to achieve high-throughput fabrication including annealing steps as well as long-term stability. During device processing, thermal annealing impacts both the organic photoactive layer, and the two interfacial layers make detailed studies of degradation mechanism delicate. A recently identified thermally stable poly[[4,8-bis[(2-ethylhexyl)oxy]benzo[1,2-b:4,5-b'-dithiopherie-2,6-diyl] [3-fluoro-2-[(2-ethylhexyl) carbonyl] thieno [3,4-b]thiophenediyl]] : [6,6]-phenyl- C-71-butyric acid methyl ester (PTB7:PC70BM) blend as photoactive layer in combination with poly(3,4-ethylenedioxythiophene) polystyrene sulfonate as hole extraction layer is used here to focus on the impact of electron extraction layer (EEL) on the thermal stability of solar cells. Solar cells processed with densely packed ZnO nanoparticle layers still show 92% of the initial efficiency after constant annealing during 1 day at 140 degrees C, whereas partially covering ZnO layers as well as an evaporated calcium layer leads to performance losses of up to 30%. This demonstrates that the nature and morphology of EELs highly influence the thermal stability of the device. We extend our study to thermally unstable PTB7:[6,6]-phenyl-C-61-butyric acid methyl ester (PC60BM) blends to highlight the impact of ZnO on the device degradation during annealing. Importantly, only 12% loss in photocurrent density is observed after annealing at 140 degrees C during 1 day when using closely packed ZnO. This is in stark contrast to literature and addressed here to the use of a stable double-sided confinement during thermal annealing. The underlying mechanism of the inhibition of photocurrent losses is revealed by electron microscopy imaging and spatially resolved spectroscopy. We found that the double-sided confinement suppresses extensive fullerene diffusion during the annealing step, but with still an increase in size and distance of the enriched donor and acceptor domains inside the photoactive layer by an average factor of 5. The later result in combination with comparably small photocurrent density losses indicates the existence of an efficient transport of minority charge carriers inside the donor and acceptor enriched phases in PTB7:PC60BM blends. |
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Wos |
000424728800082 |
Publication Date |
2018-01-12 |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1944-8244 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7.504 |
Times cited |
9 |
Open Access |
OpenAccess |
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Notes |
; We acknowledge the financial support by the French Fond Unique Interministeriel (FUI) under the project “SFUMATO” (grant number: F1110019V/201308815) as well as by the European Commission under the Project “SUNFLOWER” (FP7-ICT-2011-7-contract number: 287594). M.P. and R.R.S. acknowledge support by the HeiKA (Heidelberg Karlsruhe Research Partnership) FunTech-3D materials science program. ; |
Approved |
Most recent IF: 7.504 |
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Call Number |
UA @ lucian @ c:irua:149309UA @ admin @ c:irua:149309 |
Serial |
4939 |
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Author |
Ben Dkhil, S.; Perkhun, P.; Luo, C.; Mueller, D.; Alkarsifi, R.; Barulina, E.; Quiroz, Y.A.A.; Margeat, O.; Dubas, S.T.; Koganezawa, T.; Kuzuhara, D.; Yoshimoto, N.; Caddeo, C.; Mattoni, A.; Zimmermann, B.; Wuerfel, U.; Pfannmöller, M.; Bals, S.; Ackermann, J.; Videlot-Ackermann, C. |
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Title |
Direct correlation of nanoscale morphology and device performance to study photocurrent generation in donor-enriched phases of polymer solar cells |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Acs Applied Materials & Interfaces |
Abbreviated Journal |
Acs Appl Mater Inter |
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Volume |
12 |
Issue |
25 |
Pages |
28404-28415 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
The nanoscale morphology of polymer blends is a key parameter to reach high efficiency in bulk heterojunction solar cells. Thereby, research typically focusing on optimal blend morphologies while studying nonoptimized blends may give insight into blend designs that can prove more robust against morphology defects. Here, we focus on the direct correlation of morphology and device performance of thieno[3,4-b]-thiophene-alt-benzodithiophene (PTB7):[6,6]phenyl C-71 butyric acid methyl ester (PC71BM) bulk heterojunction (BHJ) blends processed without additives in different donor/acceptor weight ratios. We show that while blends of a 1:1.5 ratio are composed of large donor-enriched and fullerene domains beyond the exciton diffusion length, reducing the ratio below 1:0.5 leads to blends composed purely of polymer-enriched domains. Importantly, the photocurrent density in such blends can reach values between 45 and 60% of those reached for fully optimized blends using additives. We provide here direct visual evidence that fullerenes in the donor-enriched domains are not distributed homogeneously but fluctuate locally. To this end, we performed compositional nanoscale morphology analysis of the blend using spectroscopic imaging of low-energy-loss electrons using a transmission electron microscope. Charge transport measurement in combination with molecular dynamics simulations shows that the fullerene substructures inside the polymer phase generate efficient electron transport in the polymer-enriched phase. Furthermore, we show that the formation of densely packed regions of fullerene inside the polymer phase is driven by the PTB7:PC71BM enthalpy of mixing. The occurrence of such a nanoscale network of fullerene clusters leads to a reduction of electron trap states and thus efficient extraction of photocurrent inside the polymer domain. Suitable tuning of the polymer-acceptor interaction can thus introduce acceptor subnetworks in polymer-enriched phases, improving the tolerance for high-efficiency BHJ toward morphological defects such as donor-enriched domains exceeding the exciton diffusion length. |
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Wos |
000543780900058 |
Publication Date |
2020-06-01 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1944-8244 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.5 |
Times cited |
7 |
Open Access |
OpenAccess |
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Notes |
; J.A., O.M., and C.V.-A. acknowledge financial support by the French Fond Unique Interministeriel (FUI) under the project “SFUMATO” (Grant Number: F1110019V/ 201308815) as well as by the European Commission under the Project “SUNFLOWER” (FP7-ICT-2011-7, Grant Number: 287594). J.A., C.V.-A., and E.B. acknowledge the Association Nationale de la Recherche et de la Technologie (ANRT) and the Ministere de l'Enseignement Superieur, de la Recherche et de l'Innovation, awarded through the company Dracula Technologies (Valence, France), for framework of a CIFRE Ph.D. grant 2017/0529. J.A. and P.P. received funding from the European Union's Horizon 2020 research and innovation program under the Marie Sklodowska-Curie Grant agreement no. 713750. They further acknowledge support of the Regional Council of Provence-Alpes-Cote d'Azur, A*MIDEX (no. ANR-11-IDEX-0001-02), and the Investissements d'Avenir project funded by the French Government, managed by the French National Research Agency (ANR). J.A. and Y.A.A.Q. acknowledge the French Research Agency for funding through the project NFA-15 (ANR-17-CE05-0020-01). N.Y. acknowledges that the synchrotron radiation experiments were performed at BL19B2 in SPring-8 with the approval of Japan Synchrotron Radiation Research Institute (JASRI) (proposal nos. 2017B1629 and 2018B1791). S.B. acknowledges financial support from the European Research Council (ERC Consolidator Grant 815128-REALNANO) and from FWO (G.0381.16N). M.P. gratefully acknowledges funding by the Ministerium fur Wissenschaft, Forschung und Kunst Baden-Wurttemberg through the HEiKA materials research centre FunTECH-3D (MWK, 33-753-30-20/3/3) and the Large-Scale-Data-Facility (LSDF) sds@hd through grant INST 35/1314-1 FUGG. A.M. acknowledges Italian MIUR for funding through the project PON04a2 00490 M2M Netergit, PRACE, for awarding access to Marconi KNL at CINECA, Italy, through projects DECONVOLVES (2018184466) and PROVING-IL (2019204911). C.C. acknowledges the CINECA award under the ISCRA initiative for the availability of high-performance computing resources and support (project MITOMASC). ; sygma |
Approved |
Most recent IF: 9.5; 2020 IF: 7.504 |
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Call Number |
UA @ admin @ c:irua:170703 |
Serial |
6484 |
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Author |
Kertik, A.; Wee, L.H.; Şentosun, K.; Navarro, J.A.R.; Bals, S.; Martens, J.A.; Vankelecom, I.F.J. |
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Title |
High-performance CO2-selective hybrid membranes by exploiting MOF-breathing effects |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Acs Applied Materials & Interfaces |
Abbreviated Journal |
Acs Appl Mater Inter |
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Volume |
12 |
Issue |
2 |
Pages |
2952-2961 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Conventional CO2 separation in the petrochemical industry via cryogenic distillation or amine-based absorber-stripper units is energy-intensive and environmentally unfriendly. Membrane-based gas separation technology, in contrast, has contributed significantly to the development of energy-efficient systems for processes such as natural gas purification. The implementation of commercial polymeric membranes in gas separation processes is restricted by their permeability-selectivity trade-off and by their insufficient thermal and chemical stability. Herein, we present the fabrication of a Matrimid-based membrane loaded with a breathing metal-organic framework (MOF) (NH2-MIL-53(Al)) which is capable of separating binary CO2/CH4 gas mixtures with high selectivities without sacrificing much of its CO2 permeabilities. NH2-MIL-53(Al) crystals were embedded in a polyimide (PI) matrix, and the mixed-matrix membranes (MMMs) were treated at elevated temperatures (up to 350 degrees C) in air to trigger PI cross-linking and to create PI-MOF bonds at the interface to effectively seal the grain boundary. Most importantly, the MOF transitions from its narrow-pore form to its large-pore form during this treatment, which allows the PI chains to partly penetrate the pores and cross-link with the amino functions at the pore mouth of the NH2-MIL-53(Al) and stabilizes the open-pore form of NH2-MIL-53(Al). This cross-linked MMM, with MOF pore entrances was made more selective by the anchored PI-chains and achieves outstanding CO2/CH4 selectivities. This approach provides significant advancement toward the design of selective MMMs with enhanced thermal and chemical stabilities which could also be applicable for other potential applications, such as separation of hydrocarbons (olefin/paraffin or isomers), pervaporation, and solvent-resistant nanofiltration. |
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Wos |
000508464500108 |
Publication Date |
2019-12-20 |
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Series Issue |
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Edition |
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ISSN |
1944-8244 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.5 |
Times cited |
26 |
Open Access |
OpenAccess |
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Notes |
; A.K. is grateful to the Erasmus Mundus Doctorate in Membrane Engineering (EUDIME) programme. L.H.W. thanks the FWO-Vlaanderen for a postdoctoral research fellowships under contract number 12M1418N. We thank Methusalem and IAP-PAI for research funding. S.B. acknowledges financial support from European Research Council (ERC) (ERC Starting Grant No. 335078-COLOURATOM). We are also grateful to Frank Mathijs (KU Leuven) for the mechanical tests, Bart Goderis and Olivier Verkinderen for the DSC measurements, and Huntsman (Switzerland) for providing the Matrimid polymer. ; |
Approved |
Most recent IF: 9.5; 2020 IF: 7.504 |
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| |
Call Number |
UA @ admin @ c:irua:166576 |
Serial |
6534 |
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| Permanent link to this record |
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Author |
Bhatia, H.; Martin, C.; Keshavarz, M.; Dovgaliuk, I.; Schrenker, N.J.; Ottesen, M.; Qiu, W.; Fron, E.; Bremholm, M.; Van de Vondel, J.; Bals, S.; Roeffaers, M.B.J.; Hofkens, J.; Debroye, E. |
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Title |
Deciphering the role of water in promoting the optoelectronic performance of surface-engineered lead halide perovskite nanocrystals |
Type |
A1 Journal article |
| |
Year |
2023 |
Publication |
ACS applied materials and interfaces |
Abbreviated Journal |
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| |
Volume |
15 |
Issue |
5 |
Pages |
7294-7307 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Lead halide perovskites are promising candidates for applicability is limited by their structural instability toward moisture. Although a deliberate addition of water to the precursor solution has recently been shown to improve the crystallinity and optical properties of perovskites, the corresponding thin films still do not exhibit a near-unity quantum yield. Herein, we report that the direct addition of a minute amount of water to post-treated substantially enhances the stability while achieving a 95% photoluminescence quantum yield in a NC thin film. We unveil the mechanism of how moisture assists in the formation of an additional NH4Br component. Alongside, we demonstrate the crucial role of moisture in assisting localized etching of the perovskite crystal, facilitating the partial incorporation of NH4+, which is key for improved performance under ambient conditions. Finally, as a proof-of-concept, the application of post-treated and watertreated perovskites is tested in LEDs, with the latter exhibiting a superior performance, offering opportunities toward commercial application in moisture-stable optoelectronics. |
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Place of Publication |
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Editor |
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Wos |
000931729400001 |
Publication Date |
2023-01-27 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1944-8244 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.5 |
Times cited |
3 |
Open Access |
Not_Open_Access |
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Notes |
H.B. would like to express her sincere gratitude to Dr. Peter Erk (formerly BASF SE, Germany) for very insightful discussions. The authors acknowledge financial support from the Research Foundation-Flanders (FWO grant numbers S002019N, 1514220N, G.0B39.15, G.0B49.15, G098319N, and ZW15_09-GOH6316) , the KU Leuven Research Fund (C14/19/079, iBOF-21-085 PERSIST, and STG/21/010) , the Flemish government through long-term structural funding Methusalem (CASAS2, Meth/15/04) , the Hercules Founda-tion (HER/11/14) , and the ERC through the Marie Curie ITN iSwitch Ph.D. fellowship to H.B. (grant number 642196) . C.M. acknowledges the financial support from grants PID2021-128761OA-C22 funded by MCIN/AEI/10.13039/501100011033 by the ?European Union? and SBPLY/21/180501/000127 funded by JCCM and by the EU through Fondo Europeo de Desarollo Regional? (FEDER) . Martin Bremholm and Martin Ottesen acknowledge funding from the Danish Council for Independent Research, Natural Sciences, under the Sapere Aude program (grant no. 7027-00077B) and VILLUM FONDEN through the Centre of Excellence for Dirac Materials (grant no. 11744) . Affiliation with the Center for Integrated Materials Research (iMAT) at Aarhus University is gratefully acknowledged.-N.J.S. acknowledges financial support from the research foundation Flanders (FWO) through a postdoctoral fellowship (FWO grant no. 1238622N) . S.B. acknowledges financial support from the European Commission by the ERC Consolidator grant REALNANO (no. 815128) . |
Approved |
Most recent IF: 9.5; 2023 IF: 7.504 |
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| |
Call Number |
UA @ admin @ c:irua:195375 |
Serial |
7293 |
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| Permanent link to this record |
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Author |
Mulder, J.T.; Meijer, M.S.; van Blaaderen, J.J.; du Fosse, I.; Jenkinson, K.; Bals, S.; Manna, L.; Houtepen, A.J. |
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Title |
Understanding and preventing photoluminescence quenching to achieve unity photoluminescence quantum yield in Yb:YLF nanocrystals |
Type |
A1 Journal article |
| |
Year |
2023 |
Publication |
ACS applied materials and interfaces |
Abbreviated Journal |
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| |
Volume |
15 |
Issue |
2 |
Pages |
3274-3286 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Ytterbium-doped LiYF4 (Yb:YLF) is a commonly used material for laser applications, as a photon upconversion medium, and for optical refrigeration. As nanocrystals (NCs), the material is also of interest for biological and physical applications. Unfortunately, as with most phosphors, with the reduction in size comes a large reduction of the photoluminescence quantum yield (PLQY), which is typically associated with an increase in surface-related PL quenching. Here, we report the synthesis of bipyramidal Yb:YLF NCs with a short axis of similar to 60 nm. We systematically study and remove all sources of PL quenching in these NCs. By chemically removing all traces of water from the reaction mixture, we obtain NCs that exhibit a near-unity PLQY for an Yb3+ concentration below 20%. At higher Yb3+ concentrations, efficient concentration quenching occurs. The surface PL quenching is mitigated by growing an undoped YLF shell around the NC core, resulting in near-unity PLQY values even for fully Yb3+-based LiYbF4 cores. This unambiguously shows that the only remaining quenching sites in core-only Yb:YLF NCs reside on the surface and that concentration quenching is due to energy transfer to the surface. Monte Carlo simulations can reproduce the concentration dependence of the PLQY. Surprisingly, Fo''rster resonance energy transfer does not give satisfactory agreement with the experimental data, whereas nearest-neighbor energy transfer does. This work demonstrates that Yb3+-based nanophosphors can be synthesized with a quality close to that of bulk single crystals. The high Yb3+ concentration in the LiYbF4/LiYF4 core/shell nanocrystals increases the weak Yb3+ absorption, making these materials highly promising for fundamental studies and increasing their effectiveness in bioapplications and optical refrigeration. |
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Place of Publication |
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Editor |
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Language |
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Wos |
000912997300001 |
Publication Date |
2023-01-06 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1944-8244 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.5 |
Times cited |
3 |
Open Access |
OpenAccess |
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Notes |
This project has received funding from the European Union's Horizon 2020 research and innovation program under Grant Agreement No. 766900 (Testing the Large-Scale Limit of Quantum Mechanics). A.J.H. and I.d.F. further acknowledge the European Research Council Horizon 2020 ERC Grant Agreement No. 678004 (Doping on Demand) for financial support. The authors thank Freddy Rabouw and Andries Meijerink (Utrecht University) for very fruitful discussions and extremely useful advice. The author s thank Jos Thieme for his help with the laser setups used . The authors furthermore thank Niranjan Saikumar for proofreading the manuscript. |
Approved |
Most recent IF: 9.5; 2023 IF: 7.504 |
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Call Number |
UA @ admin @ c:irua:194317 |
Serial |
7348 |
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| Permanent link to this record |
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Author |
Van den Hoek, J.; Daems, N.; Arnouts, S.; Hoekx, S.; Bals, S.; Breugelmans, T. |
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Title |
Improving stability of CO₂ electroreduction by incorporating Ag NPs in N-doped ordered mesoporous carbon structures |
Type |
A1 Journal article |
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Year |
2024 |
Publication |
ACS applied materials and interfaces |
Abbreviated Journal |
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Volume |
16 |
Issue |
6 |
Pages |
6931-6947 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
The electroreduction of carbon dioxide (eCO2RR) to CO using Ag nanoparticles as an electrocatalyst is promising as an industrial carbon capture and utilization (CCU) technique to mitigate CO2 emissions. Nevertheless, the long-term stability of these Ag nanoparticles has been insufficient despite initial high Faradaic efficiencies and/or partial current densities. To improve the stability, we evaluated an up-scalable and easily tunable synthesis route to deposit low-weight percentages of Ag nanoparticles (NPs) on and into the framework of a nitrogen-doped ordered mesoporous carbon (NOMC) structure. By exploiting this so-called nanoparticle confinement strategy, the nanoparticle mobility under operation is strongly reduced. As a result, particle detachment and agglomeration, two of the most pronounced electrocatalytic degradation mechanisms, are (partially) blocked and catalyst durability is improved. Several synthesis parameters, such as the anchoring agent, the weight percentage of Ag NPs, and the type of carbonaceous support material, were modified in a controlled manner to evaluate their respective impact on the overall electrochemical performance, with a strong emphasis on operational stability. The resulting powders were evaluated through electrochemical and physicochemical characterization methods, including X-ray diffraction (XRD), N2-physisorption, Inductively coupled plasma mass spectrometry (ICP-MS), scanning electron microscopy (SEM), SEM-energy-dispersive X-ray spectroscopy (SEM-EDS), high-angle annular dark field scanning transmission electron microscopy (HAADF-STEM), STEM-EDS, electron tomography, and X-ray photoelectron spectroscopy (XPS). The optimized Ag/soft-NOMC catalysts showed both a promising selectivity (∼80%) and stability compared with commercial Ag NPs while decreasing the loading of the transition metal by more than 50%. The stability of both the 5 and 10 wt % Ag/soft-NOMC catalysts showed considerable improvements by anchoring the Ag NPs on and into a NOMC framework, resulting in a 267% improvement in CO selectivity after 72 h (despite initial losses) compared to commercial Ag NPs. These results demonstrate the promising strategy of anchoring Ag NPs to improve the CO selectivity during prolonged experiments due to the reduced mobility of the Ag NPs and thus enhanced stability. |
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Place of Publication |
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Wos |
001158812100001 |
Publication Date |
2023-12-21 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1944-8244 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
9.5 |
Times cited |
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Open Access |
Not_Open_Access: Available from 21.06.2024 |
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Notes |
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Approved |
Most recent IF: 9.5; 2024 IF: 7.504 |
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Call Number |
UA @ admin @ c:irua:202309 |
Serial |
9045 |
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Author |
Guerrero, R.M.; Lemir, I.D.; Carrasco, S.; Fernández-Ruiz, C.; Kavak, S.; Pizarro, P.; Serrano, D.P.; Bals, S.; Horcajada, P.; Pérez, Y. |
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Title |
Scaling-Up Microwave-Assisted Synthesis of Highly Defective Pd@UiO-66-NH2Catalysts for Selective Olefin Hydrogenation under Ambient Conditions |
Type |
A1 Journal Article |
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Year |
2024 |
Publication |
ACS Applied Materials & Interfaces |
Abbreviated Journal |
ACS Appl. Mater. Interfaces |
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Volume |
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Issue |
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Pages |
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Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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Abstract |
The need to develop green and cost-effective industrial catalytic processes has led to growing interest in preparing more robust, efficient, and selective heterogeneous catalysts at a large scale. In this regard, microwave-assisted synthesis is a fast method for fabricating heterogeneous catalysts (including metal oxides, zeolites, metal–organic frameworks, and supported metal nanoparticles) with enhanced catalytic properties, enabling synthesis scale-up. Herein, the synthesis of nanosized UiO-66-NH2 was optimized via a microwave-assisted hydrothermal method to obtain defective matrices essential for the stabilization of metal nanoparticles, promoting catalytically active sites for hydrogenation reactions (760 kg·m–3·day–1 space time yield, STY). Then, this protocol was scaled up in a multimodal microwave reactor, reaching 86% yield (ca. 1 g, 1450 kg·m–3·day–1 STY) in only 30 min. Afterward, Pd nanoparticles were formed in situ decorating the nanoMOF by an effective and fast microwave-assisted hydrothermal method, resulting in the formation of Pd@UiO-66-NH2 composites. Both the localization and oxidation states of Pd nanoparticles (NPs) in the MOF were achieved using high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and X-ray photoelectron spectroscopy (XPS), respectively. The optimal composite, loaded with 1.7 wt % Pd, exhibited an extraordinary catalytic activity (>95% yield, 100% selectivity) under mild conditions (1 bar H2, 25 °C, 1 h reaction time), not only in the selective hydrogenation of a variety of single alkenes (1-hexene, 1-octene, 1-tridecene, cyclohexene, and tetraphenyl ethylene) but also in the conversion of a complex mixture of alkenes (i.e., 1-hexene, 1-tridecene, and anethole). The results showed a powerful interaction and synergy between the active phase (Pd NPs) and the catalytic porous scaffold (UiO-66-NH2), which are essential for the selectivity and recyclability. |
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Wos |
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Publication Date |
2024-04-26 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1944-8244 |
ISBN |
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Additional Links |
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Impact Factor |
9.5 |
Times cited |
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Open Access |
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Notes |
The authors gratefully acknowledge financial support from “Comunidad de Madrid” and European Regional Development Fund-FEDER through the project HUB MADRID+CIRCULAR; the State Research Agency (MCIN/AEI /10.13039/501100011033) through the grant with reference number CEX2019-000931-M received in the 2019 call for “Severo Ochoa Centres of Excellence” and “María de Maeztu Units of Excellence” of the State Programme for Knowledge Generation and Scientific and Technological Strengthening of the R&D&I System; and MICIU through the project “NAPOLION” (PID2022-139956OB-I00). S.K. acknowledges the Flemish Fund for Scientific Research (FWO Vlaanderen) through a PhD research grant (1181124N). |
Approved |
Most recent IF: 9.5; 2024 IF: 7.504 |
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Call Number |
EMAT @ emat @ |
Serial |
9126 |
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Author |
González-Rubio, G.; Milagres de Oliveira, T.; Albrecht, W.; Díaz-Núñez, P.; Castro-Palacio, J.C.; Prada, A.; González, R.I.; Scarabelli, L.; Bañares, L.; Rivera, A.; Liz-Marzán, L.M.; Peña-Rodríguez, O.; Bals, S.; Guerrero-Martínez, A. |
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Title |
Formation of Hollow Gold Nanocrystals by Nanosecond Laser Irradiation |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Journal Of Physical Chemistry Letters |
Abbreviated Journal |
J Phys Chem Lett |
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Volume |
11 |
Issue |
11 |
Pages |
670-677 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
The irradiation of spherical gold nanoparticles (AuNPs) with nanosecond laser pulses induces shape transformations yielding nanocrystals with an inner cavity. The concentration of the stabilizing surfactant, the use of moderate pulse fluences, and the size of the irradiated AuNPs determine the efficiency of the process and the nature of the void. Hollow nanocrystals are obtained when molecules from the surrounding medium (e.g., water and organic matter derived from the surfactant) are trapped during laser pulse irradiation. These experimental observations suggest the existence of a subtle balance between the heating and cooling processes experienced by the nanocrystals, which induce their expansion and subsequent recrystallization keeping exogenous matter inside. The described approach provides valuable insight into the mechanism of interaction of pulsed nanosecond laser with AuNPs, along with interesting prospects for the development of hollow plasmonic nanoparticles with potential applications related to gas and liquid storage at the nanoscale. |
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Place of Publication |
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Wos |
000512223400012 |
Publication Date |
2020-02-06 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1948-7185 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
5.7 |
Times cited |
15 |
Open Access |
OpenAccess |
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Notes |
This work has been funded by the Spanish Ministry of Science, Innovation and Universities (MICIU) (Grants RTI2018-095844-B-I00, PGC2018-096444-B-I00, ENE2015-70300-C3-3, and MAT2017-86659-R), the EUROfusion Consortium (Grant ENR-IFE19.CCFE-01) and the Madrid Regional Government (Grants P2018/NMT-4389 and P2018/EMT-4437). This project has received funding from the European Commission (grant 731019, EUSMI & grant 823717, ESTEEM3). The publication is based also upon work from COST Action TUMIEE (CA17126). The facilities provided by the Center for Ultrafast Lasers at Complutense University of Madrid are gratefully acknowledged. The authors also acknowledge the computer resources and technical assistance provided by the Centro de Supercomputacion y Visualizacion de Madrid (CeSViMa). L.M.L.-M. acknowledges the Maria de Maeztu Units of Excellence Program from the Spanish State Research Agency (Grant MDM-2017-0720). This project has also received funding from the European Research Council (ERC Consolidator Grant 815128, REALNANO). W.A. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020 program (Grant 797153, SOPMEN). A.P. and R.I.G. acknowledge the support of FONDECYT under Grants 3190123 and 11180557 and Financiamiento Basal para Centros Cientificos y Tecnologicos de Excelencia FB-0807. This research was partially supported by the supercomputing infrastructure of the NLHPC (ECM-02).; sygma; esteem3JRA; esteem3reported |
Approved |
Most recent IF: 5.7; 2020 IF: 9.353 |
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Call Number |
EMAT @ emat @c:irua:166504 |
Serial |
6334 |
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Author |
Leemans, J.; Singh, S.; Li, C.; Ten Brinck, S.; Bals, S.; Infante, I.; Moreels, I.; Hens, Z. |
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Title |
Near-Edge Ligand Stripping and Robust Radiative Exciton Recombination in CdSe/CdS Core/Crown Nanoplatelets |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Journal Of Physical Chemistry Letters |
Abbreviated Journal |
J Phys Chem Lett |
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Volume |
11 |
Issue |
9 |
Pages |
3339-3344 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
We address the relation between surface chemistry and optoelectronic properties in semiconductor nanocrystals using core/crown CdSe/CdS nanoplatelets passivated by cadmium oleate (Cd(Ol)2) as model systems. We show that addition of butylamine to a nanoplatelet (NPL) dispersion maximally displaces ∼40% of the original Cd(Ol)2 capping. On the basis of density functional theory simulations, we argue that this behavior reflects the preferential displacement of Cd(Ol)2 from (near)-edge surface sites. Opposite from CdSe core NPLs, core/crown NPL dispersions can retain 45% of their initial photoluminescence efficiency after ligand displacement, while radiative exciton recombination keeps dominating the luminescent decay. Using electron microscopy observations, we assign this robust photoluminescence to NPLs with a complete CdS crown, which prevents charge carrier trapping in the near-edge surface sites created by ligand displacement. We conclude that Z-type ligands such as cadmium carboxylates can provide full electronic passivation of (100) facets yet are prone to displacement from (near)-edge surface sites. |
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Place of Publication |
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Language |
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Wos |
000535177500024 |
Publication Date |
2020-05-07 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1948-7185 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
5.7 |
Times cited |
24 |
Open Access |
OpenAccess |
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Notes |
Universiteit Gent, GOA 01G01019 ; Fonds Wetenschappelijk Onderzoek, 17006602 FWO17/PDO/184 ; H2020 European Research Council, 714876 Phocona 815128 Realnano ; SIM-Flanders, SBO-QDOCCO ; Z.H. and S.B. acknowledge support by SIM-Flanders (SBO-QDOCCO). Z.H. acknowledges support by FWO-Vlaanderen (research project 17006602). Z.H. and I.M. acknowledge support by Ghent University (GOA n◦ 01G01019). J.L. acknowledges FWO-vlaanderen for a fellowship (SB PhD fellow at FWO). Sh.S acknowledges FWO postdoctoral funding (FWO17/PDO/184). This project has further received funding from the European Research Counsil under the European Union’s Horizon 2020 research and innovation programme (ERC Consolidator grant no. 815128 REALNANO and starting grant no. 714876 PHOCONA).; sygma |
Approved |
Most recent IF: 5.7; 2020 IF: 9.353 |
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Call Number |
EMAT @ emat @c:irua:173994 |
Serial |
6657 |
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| Permanent link to this record |
