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Author |
Xu, P.; Dong, L.; Neek-Amal, M.; Ackerman, M.L.; Yu, J.; Barber, S.D.; Schoelz, J.K.; Qi, D.; Xu, F.; Thibado, P.M.; Peeters, F.M.; |
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Title |
Self-organized platinum nanoparticles on freestanding graphene |
Type |
A1 Journal article |
| |
Year |
2014 |
Publication |
ACS nano |
Abbreviated Journal  |
Acs Nano |
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| |
Volume |
8 |
Issue |
3 |
Pages |
2697-2703 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT) |
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Abstract |
Freestanding graphene membranes were successfully functionalized with platinum nanoparticles (Pt NPs). High-resolution transmission electron microscopy revealed a homogeneous distribution of single-crystal Pt NPs that tend to exhibit a preferred orientation. Unexpectedly, the NPs were also found to be partially exposed to the vacuum with the top Pt surface raised above the graphene substrate, as deduced from atomic-scale scanning tunneling microscopy images and detailed molecular dynamics simulations. Local strain accumulation during the growth process is thought to be the origin of the NP self-organization. These findings are expected to shape future approaches in developing Pt NP catalysts for fuel cells as well as NP-functionalized graphene-based high-performance electronics. |
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Wos |
000333539400085 |
Publication Date |
2014-02-05 |
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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 |
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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 |
38 |
Open Access |
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Notes |
; M.N.A. acknowledges financial support by the EU-Marie Curie IIF postdoc Fellowship/299855. F.M.P. acknowledges financial support by the ESF-EuroGRAPHENE project CONGRAN, the Flemish Science Foundation (FWO-VI), and the Methusalem Foundation of the Flemish Government. L.D. acknowledges financial support by the Taishan Overseas Scholar program (tshw20091005), the International Science & Technology Cooperation Program of China (2014DFA60150), the National Natural Science Foundation of China (51172113), the Shandong Natural Science Foundation (JQ201118), the Qingdao Municipal Science and Technology Commission (12-1-4-136-hz), and the National Science Foundation (DMR-0821159). P.M.T. is thankful for the financial support of the Office of Naval Research under Grant No. N00014-10-1-0181 and the National Science Foundation under Grant No. DMR-0855358. ; |
Approved |
Most recent IF: 13.942; 2014 IF: 12.881 |
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| |
Call Number |
UA @ lucian @ c:irua:116881 |
Serial |
2978 |
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| Permanent link to this record |
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Author |
Ghosh, S.; Gaspari, R.; Bertoni, G.; Spadaro, M.C.; Prato, M.; Turner, S.; Cavalli, A.; Manna, L.; Brescia, R. |
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Title |
Pyramid-Shaped Wurtzite CdSe Nanocrystals with Inverted Polarity |
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 |
8537-8546 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
We report on pyramid-shaped wurtzite cadmium selenide (CdSe) nanocrystals (NCs), synthesized by hot injection in the presence of chloride ions as shape-directing agents, exhibiting reversed crystal polarity compared to former reports. Advanced transmission electron microscopy (TEM) techniques (image-corrected high-resolution TEM with exit wave reconstruction and probe-corrected high-angle annular dark field-scanning TEM) unequivocally indicate that the triangular base of the pyramids is the polar (0001) facet and their apex points toward the [0001] direction. Density functional theory calculations, based on a simple model of binding of Cl(-) ions to surface Cd atoms, support the experimentally evident higher thermodynamic stability of the (0001) facet over the (0001) one conferred by Cl(-) ions. The relative stability of the two polar facets of wurtzite CdSe is reversed compared to previous experimental and computational studies on Cd chalcogenide NCs, in which no Cl-based chemicals were deliberately used in the synthesis or no Cl(-) ions were considered in the binding models. Self-assembly of these pyramids in a peculiar clover-like geometry, triggered by the addition of oleic acid, suggests that the basal (polar) facet has a density and perhaps type of ligands significantly different from the other three facets, since the pyramids interact with each other exclusively via their lateral facets. A superstructure, however with no long-range order, is observed for clovers with their (0001) facets roughly facing each other. The CdSe pyramids were also exploited as seeds for CdS pods growth, and the peculiar shape of the derived branched nanostructures clearly arises from the inverted polarity of the seeds. |
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Address |
Department of Nanochemistry, Istituto Italiano di Tecnologia (IIT) , via Morego 30, I-16163 Genova, Italy |
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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 |
000360323300085 |
Publication Date |
2015-07-23 |
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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 |
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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 |
16 |
Open Access |
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Notes |
PMID:26203791 |
Approved |
Most recent IF: 13.942; 2015 IF: 12.881 |
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Call Number |
c:irua:127807 |
Serial |
3956 |
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Author |
De Trizio, L.; Figuerola, A.; Manna, L.; Genovese, A.; George, C.; Brescia, R.; Saghi, Z.; Simonutti, R.; van Huis, M.; Falqui, A. |
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Title |
Size-tunable, hexagonal plate-like Cu3P and Janus-like Cu-Cu3P nanocrystals |
Type |
A1 Journal article |
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Year |
2012 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
6 |
Issue |
1 |
Pages |
32-41 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
We describe two synthesis approaches to colloidal Cu3P nanocrystals using trioctylphosphine (TOP) as phosphorus precursor. One approach is based on the homogeneous nucleation of small Cu3P nanocrystals with hexagonal plate-like morphology and with sizes that can be tuned from 5 to 50 nm depending on the reaction time. In the other approach, metallic Cu nanocrystals are nucleated first and then they are progressively phosphorized to Cu3P. In this case, intermediate Janus-like dimeric nanoparticles can be isolated, which are made of two domains of different materials, Cu and Cu3P, sharing a flat epitaxial interface. The Janus-like nanoparticles can be transformed back to single-crystalline copper particles if they are annealed at high temperature under high vacuum conditions, which makes them an interesting source of phosphorus. The features of the Cu Cu3P Janus-like nanoparticles are compared with those of the Wiped microstructure discovered more than two decades ago in the rapidly quenched Cu Cu3P eutectic of the Cu P alloy, suggesting that other alloy/eutectic systems that display similar behavior might give origin to nanostructures with flat, epitaxial Interface between domains of two diverse materials. Finally, the electrochemical properties of the copper phosphide plates are studied, and they are found to be capable of undergoing lithiation/delithiation through a displacement reaction, while the Janus-like Cu Cu3P particles do not display an electrochemical behavior that would make them suitable for applications in batteries. |
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Wos |
000299368300006 |
Publication Date |
2011-12-03 |
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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 |
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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 |
60 |
Open Access |
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Notes |
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Approved |
Most recent IF: 13.942; 2012 IF: 12.062 |
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Call Number |
UA @ lucian @ c:irua:99172 |
Serial |
3039 |
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Author |
Suarez-Martinez, I.; Ewels, C.P.; Ke, X.; Van Tendeloo, G.; Thiess, S.; Drube, W.; Felten, A.; Pireaux, J.-J.; Ghijsen, J.; Bittencourt, C. |
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Title |
Study of the interface between rhodium and carbon nanotubes |
Type |
A1 Journal article |
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Year |
2010 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
4 |
Issue |
3 |
Pages |
1680-1686 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
X-ray photoelectron spectroscopy at 3.5 keV photon energy, in combination with high-resolution transmission electron microscopy, is used to follow the formation of the interface between rhodium and carbon nanotubes. Rh nucleates at defect sites, whether initially present or induced by oxygen-plasma treatment. More uniform Rh cluster dispersion is observed on plasma-treated CNTs. Experimental results are compared to DFT calculations of small Rh clusters on pristine and defective graphene. While Rh interacts as strongly with the carbon as Ti, it is less sensitive to the presence of oxygen, suggesting it as a good candidate for nanotube contacts. |
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Wos |
000275858200053 |
Publication Date |
2010-02-18 |
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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 |
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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 |
26 |
Open Access |
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Notes |
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Approved |
Most recent IF: 13.942; 2010 IF: 9.865 |
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Call Number |
UA @ lucian @ c:irua:82440 |
Serial |
3337 |
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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 |
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Year |
2013 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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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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Corporate Author |
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Place of Publication |
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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 |
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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 |
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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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 |
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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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Corporate Author |
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Place of Publication |
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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 |
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Edition |
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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 |
85 |
Open Access |
OpenAccess |
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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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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 |
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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 |
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Series Issue |
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Edition |
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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 |
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 |
Heyer, S.; Janssen, W.; Turner, S.; Lu, Y.-G.; Yeap, W.S.; Verbeeck, J.; Haenen, K.; Krueger, A. |
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Title |
Toward deep blue nano hope diamonds : heavily boron-doped diamond nanoparticles |
Type |
A1 Journal article |
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Year |
2014 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
8 |
Issue |
6 |
Pages |
5757-5764 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
The production of boron-doped diamond nanoparticles enables the application of this material for a broad range of fields, such as electrochemistry, thermal management, and fundamental superconductivity research. Here we present the production of highly boron-doped diamond nanoparticles using boron-doped CVD diamond films as a starting material. In a multistep milling process followed by purification and surface oxidation we obtained diamond nanoparticles of 1060 nm with a boron content of approximately 2.3 × 1021 cm3. Aberration-corrected HRTEM reveals the presence of defects within individual diamond grains, as well as a very thin nondiamond carbon layer at the particle surface. The boron K-edge electron energy-loss near-edge fine structure demonstrates that the B atoms are tetrahedrally embedded into the diamond lattice. The boron-doped diamond nanoparticles have been used to nucleate growth of a boron-doped diamond film by CVD that does not contain an insulating seeding layer. |
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Wos |
000338089200039 |
Publication Date |
2014-04-09 |
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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 |
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Series Issue |
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Edition |
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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 |
71 |
Open Access |
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Notes |
the Research Foundation Flanders (FWO-Vlaanderen) (G.0555.10N;G.0568.10N; G.0456.12; G0044.13N and a postdoctoral scholarship for S.T.); EU FP7 through Marie Curie ITN “MATCON” (PITNGA-127 2009-238201)the Collaborative Project “DINAMO” (No. 245122) Integrated Infrastructure Initiative, Reference No. 312483-ESTEEM2.; esteem2_jra3 |
Approved |
Most recent IF: 13.942; 2014 IF: 12.881 |
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Call Number |
UA @ lucian @ c:irua:117599 |
Serial |
3683 |
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Author |
Altantzis, T.; Coutino-Gonzalez, E.; Baekelant, W.; Martinez, G.T.; Abakumov, A.M.; Van Tendeloo, G.; Roeffaers, M.B.J.; Bals, S.; Hofkens, J. |
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Title |
Direct Observation of Luminescent Silver Clusters Confined in Faujasite Zeolites |
Type |
A1 Journal article |
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Year |
2016 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
10 |
Issue |
10 |
Pages |
7604-7611 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
One of the ultimate goals in the study of metal clusters is the correlation between the atomic-scale organization and their physicochemical properties. However, direct observation of the atomic organization of such minuscule metal clusters is heavily hindered by radiation damage imposed by the different characterization techniques. We present direct evidence of the structural arrangement, at an atomic level, of luminescent silver species stabilized in faujasite (FAU) zeolites using aberration-corrected scanning transmission electron microscopy. Two different silver clusters were identified in Ag-FAU zeolites, a trinuclear silver species associated with green emission and a tetranuclear silver species related to yellow emission. By combining direct imaging with complementary information obtained from X-ray powder diffraction and Rietveld analysis, we were able to elucidate the main differences at an atomic scale between luminescent (heat-treated) and nonluminescent (cation-exchanged) Ag-FAU zeolites. It is expected that such insights will trigger the directed synthesis of functional metal nanocluster-zeolite composites with tailored luminescent properties. |
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Address |
RIES, Hokkaido University , N20W10, Kita-Ward Sapporo 001-0020, Japan |
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Place of Publication |
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Editor |
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Language |
English |
Wos |
000381959100043 |
Publication Date |
2016-07-08 |
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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 |
13.942 |
Times cited |
57 |
Open Access |
OpenAccess |
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Notes |
The authors gratefully acknowledge financial support from the Belgian Federal government (Belspo through the IAP-VI/27 and IAP-VII/05 programs), the European Union’s Seventh Framework Programme (FP7/2007-2013 under grant agreement no. 310651 SACS and no. 312483-ESTEEM2), the Flemish government in the form of long-term structural funding “Methusalem” grant METH/15/04 CASAS2, the Hercules foundation (HER/11/14), the “Strategisch Initiatief Materialen” SoPPoM program, and the Fund for Scientific Research Flanders (FWO) grants G.0349.12 and G.0B39.15. S.B. acknowledges funding from ERC Starting Grant COLOURATOMS (335078). The authors thank Prof. S. Van Aert for helpful discussions, Dr. T. De Baerdemaeker for XRD measurements, Mr. B. Dieu for the preparation of graphical material, and UOP Antwerp for the kind donation of zeolite samples.; esteem2jra4; ECASSara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 13.942 |
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| |
Call Number |
c:irua:134576 c:irua:134576 |
Serial |
4102 |
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| Permanent link to this record |
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Author |
Schouteden, K.; Govaerts, K.; Debehets, J.; Thupakula, U.; Chen, T.; Li, Z.; Netsou, A.; Song, F.; Lamoen, D.; Van Haesendonck, C.; Partoens, B.; Park, K. |
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Title |
Annealing-Induced Bi Bilayer on Bi2Te3 Investigated via Quasi-Particle-Interference Mapping |
Type |
A1 Journal article |
| |
Year |
2016 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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| |
Volume |
10 |
Issue |
10 |
Pages |
8778-8787 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT) |
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Abstract |
Topological insulators (TIs) are renowned for their exotic topological surface states (TSSs) that reside in the top atomic layers, and hence, detailed knowledge of the surface top atomic layers is of utmost importance. Here we present the remarkable morphology changes of Bi2Te3 surfaces, which have been freshly cleaved in air, upon subsequent systematic annealing in ultrahigh vacuum and the resulting effects on the local and area-averaging electronic properties of the surface states, which are investigated by combining scanning tunneling microscopy (STM), scanning tunneling spectroscopy (STS), and Auger electron spectroscopy (AES) experiments with density functional theory (DFT) calculations. Our findings demonstrate that the annealing induces the formation of a Bi bilayer atop the Bi2Te3 surface. The adlayer results in n-type doping, and the atomic defects act as scattering centers of the TSS electrons. We also investigated the annealing-induced Bi bilayer surface on Bi2Te3 via voltage-dependent quasi-particle-interference (QPI) mapping of the surface local density of states and via comparison with the calculated constant-energy contours and QPI patterns. We observed closed hexagonal patterns in the Fourier transform of real-space QPI maps with secondary outer spikes. DFT calculations attribute these complex QPI patterns to the appearance of a “second” cone due to the surface charge transfer between the Bi bilayer and the Bi2Te3. Annealing in ultrahigh vacuum offers a facile route for tuning of the topological properties and may yield similar results for other topological materials. |
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Address |
Department of Physics, Virginia Tech , Blacksburg, Virginia 24061, United States |
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Corporate Author |
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Thesis |
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Place of Publication |
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Editor |
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Language |
English |
Wos |
000384399300073 |
Publication Date |
2016-09-02 |
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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; WoS citing articles |
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Impact Factor |
13.942 |
Times cited |
15 |
Open Access |
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Notes |
The research in Leuven and Antwerp was supported by the Research FoundationFlanders (FWO, Belgium). The research in Leuven received additional support from the Flemish Concerted Research Action Program (BOF KULeuven, Project GOA/14/007) and the KULeuven Project GOA “Fundamental Challenges in Semiconductor Research”. Z.L. acknowledges the support from the China Scholarship Council (2011624021) and from KU Leuven Internal Funds (PDM). K.S. and J.D. acknowledge additional support from the FWO. T.C. and F.S. acknowledge the financial support of the National Key Projects for Basic Research of China (Grants 2013CB922103 and 2011CB922103), the National NaturalScience Foundation of China (Grant s 91421109, 11134005,11522432, and 11274003), the Natural Science Foundation ofJiangsu Province (Grant BK20130054), and the FundamentalResearch Funds for the Central Universities. K.P. wassupported by the U.S. National Science Foundation (DMR-1206354) and San Diego Supercomputer Center (SDSC)Comet and Gordon (DMR060009N). |
Approved |
Most recent IF: 13.942 |
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| |
Call Number |
EMAT @ emat @ c:irua:136269 |
Serial |
4294 |
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| Permanent link to this record |
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Author |
Zhang, L.; Lin, B.-C.; Wu, Y.-F.; Wu, H.; Huang, T.-W.; Chang, C.-R.; Ke, X.; Kurttepeli, M.; Tendeloo, G.V.; Xu, J.; Yu, D.; Liao, Z.-M. |
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Title |
Electronic Coupling between Graphene and Topological Insulator Induced Anomalous Magnetotransport Properties |
Type |
A1 Journal article |
| |
Year |
2017 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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| |
Volume |
11 |
Issue |
11 |
Pages |
6277-6285 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
It has been theoretically proposed that the spin textures of surface states in a topological insulator can be directly transferred to graphene by means of the proximity effect, which is very important for realizing the two-dimensional topological insulator based on graphene. Here we report the anomalous magnetotransport properties of graphene-topological insulator Bi2Se3 heterojunctions, which are sensitive to the electronic coupling between graphene and the topological surface state. The coupling between the p_z orbitals of graphene and the p orbitals of the surface states on the Bi2Se3 bottom surface can be enhanced by applying a perpendicular negative magnetic field, resulting in a giant negative magnetoresistance at the Dirac point up to about -91%. Obvious resistances dip in the transfer curve at the Dirac point is also observed in the hybrid devices, which is consistent with theoretical predictions of the distorted Dirac bands with nontrivial spin textures inherited from the Bi2Se3 surface states. |
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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 |
000404808000110 |
Publication Date |
2017-05-10 |
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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 |
13.942 |
Times cited |
12 |
Open Access |
OpenAccess |
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Notes |
; This work was supported by National Key Research and Development Program of China (Nos. 2016YFA0300802, 2013CB934600) and NSFC (No. 11234001). ; |
Approved |
Most recent IF: 13.942 |
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Call Number |
EMAT @ emat @ c:irua:143192 |
Serial |
4569 |
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| Permanent link to this record |
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Author |
Montanarella, F.; Altantzis, T.; Zanaga, D.; Rabouw, F.T.; Bals, S.; Baesjou, P.; Vanmaekelbergh, D.; van Blaaderen, A. |
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Title |
Composite Supraparticles with Tunable Light Emission |
Type |
A1 Journal article |
| |
Year |
2017 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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| |
Volume |
11 |
Issue |
11 |
Pages |
9136-9142 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Robust luminophores emitting light with broadly tunable colors are desirable in many applications such as light-emitting diode (LED)-based lighting, displays, integrated optoelectronics and biology. Nanocrystalline quantum dots with multicolor emission, from core- and shell-localized excitons, as well as solid layers of mixed quantum dots that emit different colors have been proposed. Here, we report on colloidal supraparticles that are composed of three types of Cd(Se,ZnS) core/(Cd,Zn)S shell nanocrystals with emission in the red, green, and blue. The emission of the supraparticles can be varied from pure to composite colors over the entire visible region and finetuned into variable shades of white light by mixing the nanocrystals in controlled proportions. Our approach results in supraparticles with sizes spanning the colloidal domain and beyond that combine versatility and processability with a broad, stable, and tunable emission, promising applications in lighting devices and biological research. |
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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 |
000411918200062 |
Publication Date |
2017-09-26 |
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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 |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.942 |
Times cited |
36 |
Open Access |
OpenAccess |
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Notes |
We thank J. J. Geuchies for help with the optical analysis, W. Vlug for providing silica particles filled with RITC, J. D. Meeldijk for his assistance with SE-STEM measurements, E. B. van der Wee for help with the calculation of the radial distribution functions, and M. van Huis and S. Dussi for very fruitful discussions. This work was supported by the European Comission via the Marie-Sklodowska Curie action Phonsi (H2020-MSCA-ITN-642656). D.V. wishes to thank the Dutch FOM (program DDC13), NWO−CW (Toppunt 718.015.002), and the European Research Council under HORIZON 2020 (grant 692691 FIRSTSTEP) for financial support. A.v.B. and F.M. acknowledge partial funding from the European Research Council under the European Union’s Seventh Framework Programme (FP-2007-2013)/ERC advanced grant agreement 291667: HierarSACol. S.B. and D.Z. acknowledge financial support from the European Research Council (starting grant no. COLOURATOM 335078), and T.A. acknowledges funding from the Research Foundation Flanders (FWO, Belgium) through a postdoctoral grant. ECAS_Sara (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 13.942 |
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Call Number |
EMAT @ emat @c:irua:146095UA @ admin @ c:irua:146095 |
Serial |
4732 |
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Author |
Fedoseeva, Y.V.; Orekhov, A.S.; Chekhova, G.N.; Koroteev, V.O.; Kanygin, M.A.; Seovskiy, B.V.; Chuvilin, A.; Pontiroli, D.; Ricco, M.; Bulusheva, L.G.; Okotrub, A.V. |
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Title |
Single-walled carbon nanotube reactor for redox transformation of mercury dichloride |
Type |
A1 Journal article |
| |
Year |
2017 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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| |
Volume |
11 |
Issue |
9 |
Pages |
8643-8649 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
<script type='text/javascript'>document.write(unpmarked('Single-walled carbon nanotubes (SWCNTs) possessing a confined inner space protected by chemically resistant shells are promising for delivery, storage, and desorption of various compounds, as well as carrying out specific reactions. Here, we show that SWCNTs interact with molten mercury dichloride (HgCl2) and guide its transformation into dimercury dichloride (Hg2Cl2) in the cavity. The chemical state of host SWCNTs remains almost unchanged except for a small p-doping from the guest Hg2Cl2 nanocrystals. The density functional theory calculations reveal that the encapsulated HgCl2 molecules become negatively charged and start interacting via chlorine bridges when local concentration increases. This reduces the bonding strength in HgCl2, which facilitates removal of chlorine, finally leading to formation of Hg2Cl2 species. The present work demonstrates that SWCNTs not only serve as a template for growing nanocrystals but also behave as an electron-transfer catalyst in the spatially confined redox reaction by donation of electron density for temporary use by the guests.')); |
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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 |
000411918200012 |
Publication Date |
2017-08-07 |
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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 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.942 |
Times cited |
11 |
Open Access |
Not_Open_Access |
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Notes |
; Collaboration between partner institutions was partially supported by European FP7 IRSES project 295180. We are grateful to the bilateral Program “Russian-German Laboratory at BESSY II” for the assistance in XPS and NEXAFS measurements. We acknowledge C. Tollan for proofreading the manuscript. We are grateful to Dr. Y.V. Shubin for XRD measurements of graphite with HgCl<INF>2</ INF>. ; |
Approved |
Most recent IF: 13.942 |
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Call Number |
UA @ lucian @ c:irua:146770 |
Serial |
4895 |
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Author |
Sandoval, S.; Kepic, D.; Perez del Pino, A.; Gyorgy, E.; Gomez, A.; Pfannmöller, M.; Van Tendeloo, G.; Ballesteros, B.; Tobias, G. |
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Title |
Selective laser-assisted synthesis of tubular van der Waals heterostructures of single-layered PbI2 within carbon nanotubes exhibiting carrier photogeneration |
Type |
A1 Journal article |
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Year |
2018 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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| |
Volume |
12 |
Issue |
7 |
Pages |
6648-6656 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
The electronic and optical properties of two-dimensional layered materials allow the miniaturization of nanoelectronic and optoelectronic devices in a competitive manner. Even larger opportunities arise when two or more layers of different materials are combined. Here, we report on an ultrafast energy efficient strategy, using laser irradiation, which allows bulk synthesis of crystalline single-layered lead iodide in the cavities of carbon nanotubes by forming cylindrical van der Waals heterostructures. In contrast to the filling of van der Waals solids into carbon nanotubes by conventional thermal annealing, which favors the formation of inorganic nanowires, the present strategy is highly selective toward the growth of monolayers forming lead iodide nanotubes. The irradiated bulk material bearing the nanotubes reveals a decrease of the resistivity as well as a significant increase in the current flow upon illumination. Both effects are attributed to the presence of single-walled lead iodide nanotubes in the cavities of carbon nanotubes, which dominate the properties of the whole matrix. The present study brings in a simple, ultrafast and energy efficient strategy for the tailored synthesis of rolled-up single-layers of lead iodide (i.e., single-walled PbI2 nanotubes), which we believe could be expanded to other two-dimensional (2D) van der Waals solids. In fact, initial tests with ZnI2 already reveal the formation of single-walled ZnI2 nanotubes, thus proving the versatility of the approach. |
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Address |
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Corporate Author |
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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 |
000440505000029 |
Publication Date |
2018-07-05 |
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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 |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.942 |
Times cited |
8 |
Open Access |
OpenAccess |
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Notes |
; We acknowledge funding from MINECO (Spain), through MAT2017-86616-R, ENE2017-89210-C2-1-R, and “Severo Ochoa” Programme for Centres of Excellence in R&D (SEV-2015-0496, SEV-2013-0295), CERCA programme for funding ICN2 and support from AGAUR of Generalitat de Catalunya through the projects 2017 SGR 1086, 2017 SGR 581 and 2017 SGR 327. We thank Thomas Swan Co., Ltd., for supplying MWCNT Elicarb samples. D.K. acknowledges financial support from the Ministry of Education, Science, and Technological Development of the Republic of Serbia for postdoctoral research. We are grateful to R Rurali (ICMAB-CSIC) for providing the structural model of the PbI<INF>2</INF> nanotube employed for the schematic representation of PbI<INF>2</INF>@MVWCNT. ; |
Approved |
Most recent IF: 13.942 |
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| |
Call Number |
UA @ lucian @ c:irua:153169 |
Serial |
5127 |
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Author |
Feld, A.; Weimer, A.; Kornowski, A.; Winckelmans, N.; Merkl, J.-P.; Kloust, H.; Zierold, R.; Schmidtke, C.; Schotten, T.; Riedner, M.; Bals, S.; Weller, P.D., Horst |
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Title |
Chemistry of Shape-Controlled Iron Oxide Nanocrystal Formation |
Type |
A1 Journal article |
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Year |
2018 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
13 |
Issue |
13 |
Pages |
152-162 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Herein we demonstrate that meticulous and in-depth analysis of the reaction mechanisms of nanoparticle formation is rewarded by full control of size, shape and crystal structure of superparamagnetic iron oxide nanocrystals during synthesis. Starting from two iron sources – iron(II)- and iron(III) carbonate -a strict separation of oleate formation from the generation of reactive pyrolysis products and concomitant nucleation of iron oxide nanoparticles was achieved. This protocol enabled us to analyze each step of nanoparticle formation independently in depth. Progress of the entire reaction was monitored via matrix-assisted laser desorption ionization time-of-flight mass spectrometry (MALDI-TOF MS) and gas chromatography (GC) gaining insight into the formation of various iron oleate species prior to nucleation. Interestingly, due to the intrinsic strongly reductive pyrolysis conditions of the oleate intermediates and redox process in early stages of the synthesis, pristine iron oxide nuclei were composed exclusively from wustite, irrespective of the oxidation state of the iron source. Controlling the reaction conditions provided a very broad range of size- and shape defined monodisperse iron oxide nanoparticles. Curiously, after nucleation star shaped nanocrystals were obtained, which underwent metamorphism towards cubic shaped particles. EELS tomography revealed ex post oxidation of the primary wustite nanocrystal providing a full 3D image of Fe2+ and Fe3+ distribution within. Overall, we developed a highly flexible synthesis, yielding multigram amounts of well-defined iron oxide nanocrystals of different sizes and morphologies. |
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Corporate Author |
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Publisher |
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Place of Publication |
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Language |
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Wos |
000456749900017 |
Publication Date |
2018-12-12 |
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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 |
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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 |
13.942 |
Times cited |
54 |
Open Access |
OpenAccess |
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Notes |
The authors gratefully acknowledge financial support from the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) – Projektnummer 192346071 – SFB 986 and the excellence cluster ‘The Hamburg Centre for Ultrafast Imaging – Structure, Dynamics and Control of Matter at the Atomic Scale’ (by grant EXC 1074) S.B. and N.W. acknowledge financial support from European Research Council (ERC Starting Grant #335078-COLOURATOMS) and from the Research Foundation Flanders (FWO, Belgium) through Project fundings G038116N. Dr. Volker Sauerland for his support in calibrating the MALDI-TOF spectra. Almut Bark for measuring XRD (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); ecas_sara |
Approved |
Most recent IF: 13.942 |
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Call Number |
EMAT @ emat @c:irua:155716UA @ admin @ c:irua:155716 |
Serial |
5073 |
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Author |
Gonzalez-Rubio, G.; Kumar, V.; Llombart, P.; Diaz-Nunez, P.; Bladt, E.; Altantzis, T.; Bals, S.; Pena-Rodriguez, O.; Noya, E.G.; MacDowell, L.G.; Guerrero-Martinez, A.; Liz-Marzan, L.M. |
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Title |
Disconnecting Symmetry Breaking from Seeded Growth for the Reproducible Synthesis of High Quality Gold Nanorods |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
13 |
Issue |
13 |
Pages |
4424-4435 |
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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 |
One of the major difficulties hindering the widespread application of colloidal anisotropic plasmonic nanoparticles is the limited robustness and reproducibility of multistep synthetic methods. We demonstrate herein that the reproducibility and reliability of colloidal gold nanorod (AuNR) synthesis can be greatly improved by disconnecting the symmetry-breaking event from the seeded growth process. We have used a modified silver-assisted seeded growth method in the presence of the surfactant hexadecyltrimethylammonium bromide and n-decanol as a co-surfactant to prepare small AuNRs in high yield, which were then used as seeds for the growth of high quality AuNR colloids. Whereas the use of n-decanol provides a more-rigid micellar system, the growth on anisotropic seeds avoids sources of irreproducibility during the symmetry breaking step, yielding uniform AuNR colloids with narrow plasmon bands, ranging from 600 to 1270 nm, and allowing the fine-tuning of the final dimensions. This method provides a robust route for the preparation of high quality AuNR colloids with tunable morphology, size, and optical response in a reproducible and scalable manner. |
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Place of Publication |
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Wos |
000466052900067 |
Publication Date |
2019-04-02 |
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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; WoS citing articles |
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Impact Factor |
13.942 |
Times cited |
100 |
Open Access |
OpenAccess |
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Notes |
; This work has been funded by the Spanish MINECO (grant nos. FIS2017-89361-C3-2-P and MAT2017-86659-R), the Madrid Regional Government (grant no. P2018/NMT-4389) and the Complutense University of Madrid (grant no. PR75/18-21616). Funding is acknowledged from the European Commission (grant no. EUSMI 731019). G.G.-R. acknowledges receipt of FPI Fellowship from the Spanish MINECO. E.B. and T.A. acknowledge postdoctoral grants from the Research Foundation Flanders (FWO). The authors are indebted to Profs. Justin Gooding, Watson Loh, Nicholas Kotov, Deqing Zhang, Mihaela Delcea, Maurizio Prato, and Krishna Ganesh, for providing milli-Q water samples. ; |
Approved |
Most recent IF: 13.942 |
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| |
Call Number |
UA @ admin @ c:irua:160417 |
Serial |
5246 |
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Author |
Jishkariani, D.; Elbert, K.C.; Wu, Y.; Lee, J.D.; Hermes, M.; Wang, D.; van Blaaderen, A.; Murray, C.B. |
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Title |
Nanocrystal Core Size and Shape Substitutional Doping and Underlying Crystalline Order in Nanocrystal Superlattices |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
13 |
Issue |
5 |
Pages |
5712-5719 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Substitutional doping is a potentially powerful technique to control the properties of nanocrystal (NC) superlattices (SLs). However, not every NC can be substituted into any lattice, as the NCs have to be close in size and shape, limiting the application of substitutional doping. Here we show that this limitation can be overcome by employing ligands of various size. We show that small NCs with long ligands can be substituted into SLs of big NCs with short ligands. Furthermore, we show that shape differences can also be overcome and that cubes can substitute spheres when both are coated with long ligands. Finally, we use the NC effective ligand size, softness, and effective overall size ratio to explain observed doping behaviors. |
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Wos |
000469886300078 |
Publication Date |
2019-05-03 |
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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 |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
13.942 |
Times cited |
6 |
Open Access |
Not_Open_Access |
|
| |
Notes |
; This work was supported by the University of Pennsylvania's NSF MRSEC under award no. DMR-112090 and the CNRS-UPENN-SOLVAY through the Complex Assemblies of Soft Matter Laboratory (COMPASS). K.C.E. acknowledges support from the NSF Graduate Research Fellowship Program under grant no. DGE-1321851. C.B.M. acknowledges the Richard Perry University Professorship at the University of Pennsylvania. D.W. and A.v.B. acknowledge partial funding from the European Research Council under the European Union's Seventh Framework Programme (FP -2007-2013)/ERC Advanced Grant Agreement 291667 HierarSACol. M.H. was supported by The Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), an NWO Gravitation programme funded by the Ministry of Education, Culture and Science of the government of The Netherlands. The authors thank EM square in Utrecht University for the access to the microscopes. ; |
Approved |
Most recent IF: 13.942 |
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| |
Call Number |
UA @ admin @ c:irua:160344 |
Serial |
5256 |
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| Permanent link to this record |
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| |
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Author |
Albrecht, W.; Bladt, E.; Vanrompay, H.; Smith, J.D.; Skrabalak, S.E.; Bals, S. |
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| |
Title |
Thermal Stability of Gold/Palladium Octopods Studied in Situ in 3D: Understanding Design Rules for Thermally Stable Metal Nanoparticles |
Type |
A1 Journal article |
| |
Year |
2019 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
|
| |
Volume |
13 |
Issue |
13 |
Pages |
6522-6530 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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| |
Abstract |
Multifunctional metal nanoparticles (NPs) such as anisotropic multimetallic NPs are crucial for boosting nanomaterial based applications. Advanced synthetic protocols exist to make a large variety of such nanostructures. However, a major limiting factor for the usability of them in real life applications is their stability. Here, we show that Au/Pd octopods, 8-branched nanocrystals with Oh symmetry, with only a low amount of Pd exhibited a high thermal stability and maintained strong plasmon resonances up to 600 ◦C. Furthermore, we study the influence of the composition, morphology and environment on the thermal stability and define key parameters for the design of thermally stable multifunctional NPs. |
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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 |
000473248300038 |
Publication Date |
2019-06-25 |
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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 |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
13.942 |
Times cited |
46 |
Open Access |
OpenAccess |
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| |
Notes |
W. A. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020. H. V. acknowledges financial support by the Research Foundation Flanders (FWO grant 1S32617N). E. B. acknowledges a post-doctoral grant from the Research Foundation Flanders (FWO, Belgium). J. D. S. and S.E.S acknowledge funding from the US National Science Foundation (award number: CHE-1602476). The authors acknowledge funding from the European Commission Grant (EUSMI E180600101 to S. B. and S. E. S.) and European Research Council (ERC Starting Grant #335078-COLOURATOMS). Realnano 815128; sygma |
Approved |
Most recent IF: 13.942 |
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| |
Call Number |
EMAT @ emat @c:irua:161356 |
Serial |
5285 |
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| Permanent link to this record |
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| |
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Author |
Skorikov, A.; Albrecht, W.; Bladt, E.; Xie, X.; van der Hoeven, J.E.S.; van Blaaderen, A.; Van Aert, S.; Bals, S. |
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| |
Title |
Quantitative 3D Characterization of Elemental Diffusion Dynamics in Individual Ag@Au Nanoparticles with Different Shapes |
Type |
A1 Journal article |
| |
Year |
2019 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
|
| |
Volume |
13 |
Issue |
13 |
Pages |
13421-13429 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Anisotropic bimetallic nanoparticles are promising candidates for plasmonic and catalytic applications. Their catalytic performance and plasmonic properties are closely linked to the distribution of the two metals, which can change during applications in which the particles are exposed to heat. Due to this fact, correlating the thermal stability of complex heterogeneous nanoparticles to their microstructural properties is of high interest for the practical applications of such materials. Here, we employ quantitative electron tomography in high-angle annular dark-field scanning transmission electron microscopy (HAADFSTEM) mode to measure the 3D elemental diffusion dynamics in individual anisotropic Au−Ag nanoparticles upon heating in situ. This approach allows us to study the elemental redistribution in complex, asymmetric nanoparticles on a single particle level, which has been inaccessible to other techniques so far. In this work, we apply the proposed method to compare the alloying dynamics of Au−Ag nanoparticles with different shapes and compositions and find that the shape of the nanoparticle does not exhibit a significant effect on the alloying speed whereas the composition does. Finally, comparing the experimental results to diffusion simulations allows us to estimate the diffusion coefficients of the metals for individual nanoparticles. |
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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 |
000500650000115 |
Publication Date |
2019-10-25 |
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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 |
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Edition |
|
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| |
ISSN |
1936-0851 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
13.942 |
Times cited |
29 |
Open Access |
OpenAccess |
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| |
Notes |
This project has received funding from the European Commission (grant 731019, EUSMI) and European Research Council (ERC Consolidator Grants 815128, REALNANO; 770887, PICOMETRICS; 648991, 3MC; and ERC Advanced Grant 291667, HierarSACol). This project has also received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement 823717, ESTEEM3. W.A. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020 program (grant 797153, SOPMEN). E.B. acknowledges a postdoctoral grant 12T2719N from the Research Foundation Flanders (FWO, Belgium). X.X. acknowledges financial support from the EU H2020-MSCAITN-2015 project 676045, MULTIMAT. The authors also acknowledge financial support by the Research Foundation Flanders (FWO grants G038116N, G026718N, and G036915N).; sygma; esteem3JRA; esteem3reported |
Approved |
Most recent IF: 13.942 |
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| |
Call Number |
EMAT @ emat @c:irua:164061 |
Serial |
5379 |
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| Permanent link to this record |
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Author |
Hinterding, S.O.M.; Berends, A.C.; Kurttepeli, M.; Moret, M.-E.; Meeldijk, J.D.; Bals, S.; van der Stam, W.; de Donega, C.M. |
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| |
Title |
Tailoring Cu+ for Ga3+ cation exchange in Cu2-xS and CuInS2 nanocrystals by controlling the Ga precursor chemistry |
Type |
A1 Journal article |
| |
Year |
2019 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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| |
Volume |
13 |
Issue |
13 |
Pages |
12880-12893 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Nanoscale cation exchange (CE) has resulted in colloidal nanomaterials that are unattainable by direct synthesis methods. Aliovalent CE is complex and synthetically challenging because the exchange of an unequal number of host and guest cations is required to maintain charge balance. An approach to control aliovalent CE reactions is the use of a single reactant to both supply the guest cation and extract the host cation. Here, we study the application of GaCl3-L complexes [L = trioctylphosphine (TOP), triphenylphosphite (TPP), diphenylphosphine (DPP)] as reactants in the exchange of Cu+ for Ga3+ in Cu2-xS nanocrystals. We find that noncomplexed GaCl3 etches the nanocrystals by S2- extraction, whereas GaCl3-TOP is unreactive. Successful exchange of Cu+ for Ga3+ is only possible when GaCl3 is complexed with either TPP or DPP. This is attributed to the pivotal role of the Cu2-xS-GaCl3-L activated complex that forms at the surface of the nanocrystal at the onset of the CE reaction, which must be such that simultaneous Ga3+ insertion and Cu+ extraction can occur. This requisite is only met if GaCl3 is bound to a phosphine ligand, with a moderate bond strength, to allow facile dissociation of the complex at the nanocrystal surface. The general validity of this mechanism is demonstrated by using GaCl3-DPP to convert CuInS2 into (Cu,Ga,In)S-2 nanocrystals, which increases the photoluminescence quantum yield 10 -fold, while blue -shifting the photoluminescence into the NIR biological window. This highlights the general applicability of the mechanistic insights provided by our work. |
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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 |
000500650000061 |
Publication Date |
2019-10-16 |
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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 |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
13.942 |
Times cited |
27 |
Open Access |
OpenAccess |
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| |
Notes |
; S.O.M.H., W.v.d.S., A.C.B., 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 Nos. ECHO.712.012.0001 and ECHO.712.014.001. S.B. acknowledges financial support from the European Research Council (ERC Consolidator Grant No. 815128-REALNANO). S.O.M.H. is supported by The Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), an NWO Gravitation Programme funded by the Ministry of Education, Culture and Science of the government of The Netherlands. DFT calculations were carried out on the Dutch national e-infrastructure with the support of SURF Cooperative. This work was sponsored by NWO Physical Sciences for the use of supercomputer facilities. The authors thank Jessi van der Hoeven for EDS and TEM measurements. ; sygma |
Approved |
Most recent IF: 13.942 |
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| |
Call Number |
UA @ admin @ c:irua:165149 |
Serial |
6324 |
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| Permanent link to this record |
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Author |
Rodal-Cedeira, S.; Vázquez-Arias, A.; Bodelon, G.; Skorikov, A.; Núñez-Sanchez, S.; La Porta, A.; Polavarapu, L.; Bals, S.; Liz-Marzán, L.M.; Perez-Juste, J.; Pastoriza-Santos, I. |
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Title |
An Expanded Surface-Enhanced Raman Scattering Tags Library by Combinatorial Encapsulation of Reporter Molecules in Metal Nanoshells |
Type |
A1 Journal article |
| |
Year |
2020 |
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 |
Raman-encoded gold nanoparticles have been widely employed as photostable multifunctional probes for sensing, bioimaging, multiplex diagnostics, and surface-enhanced Raman scattering (SERS)-guided tumor therapy. We report a strategy toward obtaining a particularly large library of Au nanocapsules encoded with Raman codes defined by the combination of different thiol-free Raman reporters, encapsulated at defined molar ratios. The fabrication of SERS tags with tailored size and pre-defined codes is based on the in situ incorporation of Raman reporter molecules inside Au nanocapsules during their formation via Galvanic replacement coupled to seeded growth on Ag NPs. The hole-free closed shell structure of the nanocapsules is confirmed by electron tomography. The unusually wide encoding possibilities of the obtained SERS tags are investigated by means of either wavenumber-based encoding or Raman frequency combined with signal intensity, leading to an outstanding performance as exemplified by 26 and 54 different codes, respectively. We additionally demonstrate that encoded nanocapsules can be readily bioconjugated with antibodies for applications such as SERS-based targeted cell imaging and phenotyping. |
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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 |
000595533800019 |
Publication Date |
2020-09-01 |
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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 |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
17.1 |
Times cited |
14 |
Open Access |
OpenAccess |
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| |
Notes |
L.M.L.-M. acknowledges financial support from the European Research Council (ERC-AdG-4DbioSERS-787510) and the Spanish State Research Agency (Grant No. MDM-2017-0720 and PID2019-108954RB-I00). I.P.-S. and J.P.-J. acknowledge financial support from the Spanish State Research Agency (Grant No. MAT2016-77809-R)) and Ramon Areces Foundation (Grant No. SERSforSAFETY). G.B. acknowledges financial support from CINBIO (Grant number ED431G 2019/07 Xunta de Galicia). S.B. and A.S. acknowledge financial support by the Research Foundation Flanders (FWO grant G038116N). This project received funding as well from the European Union’s Horizon 2020 research and innovation program under grant agreement No 731019 (EUSMI). S.B. acknowledges support from the European Research Council (ERC Consolidator Grant #815128 REALNANO). We thank Carlos Fernández-Lodeiro and Daniel García-Lojo for their helpful contribution to the SEM characterization and SERS analysis and Veronica Montes-García for her fruitful contribution in the PCA analysis.; sygma |
Approved |
Most recent IF: 17.1; 2020 IF: 13.942 |
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Call Number |
EMAT @ emat @c:irua:172492 |
Serial |
6403 |
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| Permanent link to this record |
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Author |
Milagres de Oliveira, T.; Albrecht, W.; González-Rubio, G.; Altantzis, T.; Lobato Hoyos, I.P.; Béché, A.; Van Aert, S.; Guerrero-Martínez, A.; Liz-Marzán, L.M.; Bals, S. |
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| |
Title |
3D Characterization and Plasmon Mapping of Gold Nanorods Welded by Femtosecond Laser Irradiation |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Acs Nano |
Abbreviated Journal |
Acs Nano |
|
| |
Volume |
14 |
Issue |
|
Pages |
acsnano.0c02610 |
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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 |
Ultrafast laser irradiation can induce morphological and structural changes in plasmonic nanoparticles. Gold nanorods (Au NRs), in particular, can be welded together upon irradiation with femtosecond laser pulses, leading to dimers and trimers through the formation of necks between individual nanorods. We used electron tomography to determine the 3D (atomic) structure at such necks for representative welding geometries and to characterize the induced defects. The spatial distribution of localized surface plasmon modes for different welding configurations was assessed by electron energy loss spectroscopy. Additionally, we were able to directly compare the plasmon line width of single-crystalline and welded Au NRs with single defects at the same resonance energy, thus making a direct link between the structural and plasmonic properties. In this manner, we show that the occurrence of (single) defects results in significant plasmon broadening. |
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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 |
000586793400016 |
Publication Date |
2020-08-19 |
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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 |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
17.1 |
Times cited |
25 |
Open Access |
OpenAccess |
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| |
Notes |
This project has received funding from the European Research Council under the European Union's Horizon 2020 research and innovation program (ERC Consolidator Grants #815128 – REALNANO and #770887 – PICOMETRICS). The authors gratefully acknowledge funding from the Research Foundation Flanders (FWO, Belgium) through project funding G.0381.16N and G.0267.18N. W.A. acknowledges an Individual Fellowship funded by the Marie 27 Sklodowska-Curie Actions (MSCA) in Horizon 2020 program (grant 797153, SOPMEN). G.G.-R. acknowledge receipt of FPI Fellowship from the Spanish MINECO. This work has been funded by the Spanish Ministry of Science, Innovation and Universities (MICIU) (Grants RTI2018-095844-B-I00 and MAT2017-86659-R) and the Madrid Regional Government (Grant P2018/NMT-4389). A.B. acknowledges funding from FWO project G093417N and from the European Union's Horizon 2020 research and innovation programme under grant agreement No 823717 – ESTEEM3. L.M.L.-M. acknowledges the Maria de Maeztu Units of Excellence Program from the Spanish State Research Agency (Grant No. MDM-2017-0720); Comunidad de Madrid, P2018/NMT-4389 ; Ministerio de Ciencia, Innovación y Universidades, MAT2017-86659-R RTI2018-095844-B-I00 ; Ministerio de Economía y Competitividad; H2020 Marie Sklodowska-Curie Actions, 797153 ; Fonds Wetenschappelijk Onderzoek, G.0267.18N G.0381.16N G093417N ; H2020 Research Infrastructures, 823717 ; H2020 European Research Council, 770887 815128 ; Agencia Estatal de Investigación, Ministerio de Ciencia, Innovación y Universidades, MDM-2017-0720 ; sygma |
Approved |
Most recent IF: 17.1; 2020 IF: 13.942 |
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| |
Call Number |
EMAT @ emat @c:irua:172440 |
Serial |
6426 |
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| Permanent link to this record |
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Author |
Busatto, S.; Ruiter, M. de; Jastrzebski, J.T.B.H.; Albrecht, W.; Pinchetti, V.; Brovelli, S.; Bals, S.; Moret, M.-E.; de Mello Donega, C. |
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Title |
Luminescent Colloidal InSb Quantum Dots from In Situ Generated Single-Source Precursor |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Acs Nano |
Abbreviated Journal |
Acs Nano |
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| |
Volume |
14 |
Issue |
10 |
Pages |
13146-13160 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Despite recent advances, the synthesis of colloidal InSb quantum dots (QDs) remains underdeveloped, mostly due to the lack of suitable precursors. In this work, we use Lewis acid–base interactions between Sb(III) and In(III) species formed at room temperature in situ from commercially available compounds (viz., InCl3, Sb[NMe2]3 and a primary alkylamine) to obtain InSb adduct complexes. These complexes are successfully used as precursors for the synthesis of colloidal InSb QDs ranging from 2.8 to 18.2 nm in diameter by fast coreduction at sufficiently high temperatures (≥230 °C). Our findings allow us to propose a formation mechanism for the QDs synthesized in our work, which is based on a nonclassical nucleation event, followed by aggregative growth. This yields ensembles with multimodal size distributions, which can be fractionated in subensembles with relatively narrow polydispersity by postsynthetic size fractionation. InSb QDs with diameters below 7.0 nm have the zinc blende crystal structure, while ensembles of larger QDs (≥10 nm) consist of a mixture of wurtzite and zinc blende QDs. The QDs exhibit photoluminescence with small Stokes shifts and short radiative lifetimes, implying that the emission is due to band-edge recombination and that the direct nature of the bandgap of bulk InSb is preserved in InSb QDs. Finally, we constructed a sizing curve correlating the peak position of the lowest energy absorption transition with the QD diameters, which shows that the band gap of colloidal InSb QDs increases with size reduction following a 1/d dependence. |
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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 |
000586793400068 |
Publication Date |
2020-10-27 |
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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 |
1936-0851 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
17.1 |
Times cited |
21 |
Open Access |
OpenAccess |
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Notes |
S.B. 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 No. TOP.715.016.001. W.A. acknowledges an Individual Fellowship from the Marie Sklodowska-Curie actions (MSCA) under the EU?s Horizon 2020 program (Grant No. 797153, SOPMEN). This project has received funding from the European Commission Grant (EUSMI E180900184) and European Research Council (ERC Consolidator Grant No. 815128 REALNANO).; sygma |
Approved |
Most recent IF: 17.1; 2020 IF: 13.942 |
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Call Number |
EMAT @ emat @c:irua:173862 |
Serial |
6438 |
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| Permanent link to this record |
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Author |
Sun, C.; Liao, X.; Xia, F.; Zhao, Y.; Zhang, L.; Mu, S.; Shi, S.; Li, Y.; Peng, H.; Van Tendeloo, G.; Zhao, K.; Wu, J. |
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Title |
High-voltage cycling induced thermal vulnerability in LiCoO₂ cathode : cation loss and oxygen release driven by oxygen vacancy migration |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Acs Nano |
Abbreviated Journal |
Acs Nano |
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| |
Volume |
14 |
Issue |
5 |
Pages |
6181-6190 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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| |
Abstract |
The release of the lattice oxygen due to the thermal degradation of layered lithium transition metal oxides is one of the major safety concerns in Li-ion batteries. The oxygen release is generally attributed to the phase transitions from the layered structure to spinel and rocksalt structures that contain less lattice oxygen. Here, a different degradation pathway in LiCoO2 is found, through oxygen vacancy facilitated cation migration and reduction. This process leaves undercoordinated oxygen that gives rise to oxygen release while the structure integrity of the defect-free region is mostly preserved. This oxygen release mechanism can be called surface degradation due to the kinetic control of the cation migration but has a slow surface to bulk propagation with continuous loss of the surface cation ions. It is also strongly correlated with the high-voltage cycling defects that end up with a significant local oxygen release at low temperatures. This work unveils the thermal vulnerability of high-voltage Li-ion batteries and the critical role of the surface fraction as a general mitigating approach. |
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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 |
000537682300101 |
Publication Date |
2020-04-17 |
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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 |
|
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 |
; C.S., X.L., and F.X. contributed equally to this work. This work was supported by the National Natural Science Foundation of China (21905169). The S/TEM work was performed at the Nanostructure Research Center (NRC), which is supported by the Fundamental Research Funds for the Central Universities (WUT: 2019III012GX), the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, and the State Key Laboratory of Silicate Materials for Architectures (all of the laboratories are at Wuhan University of Technology). ; |
Approved |
Most recent IF: 17.1; 2020 IF: 13.942 |
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Call Number |
UA @ admin @ c:irua:170246 |
Serial |
6537 |
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Author |
Griffin, E.; Mogg, L.; Hao, G.-P.; Kalon, G.; Bacaksiz, C.; Lopez-Polin, G.; Zhou, T.Y.; Guarochico, V.; Cai, J.; Neumann, C.; Winter, A.; Mohn, M.; Lee, J.H.; Lin, J.; Kaiser, U.; Grigorieva, I., V; Suenaga, K.; Ozyilmaz, B.; Cheng, H.-M.; Ren, W.; Turchanin, A.; Peeters, F.M.; Geim, A.K.; Lozada-Hidalgo, M. |
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Title |
Proton and Li-Ion permeation through graphene with eight-atom-ring defects |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Acs Nano |
Abbreviated Journal |
Acs Nano |
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| |
Volume |
14 |
Issue |
6 |
Pages |
7280-7286 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT) |
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Abstract |
Defect-free graphene is impermeable to gases and liquids but highly permeable to thermal protons. Atomic-scale defects such as vacancies, grain boundaries, and Stone-Wales defects are predicted to enhance graphene's proton permeability and may even allow small ions through, whereas larger species such as gas molecules should remain blocked. These expectations have so far remained untested in experiment. Here, we show that atomically thin carbon films with a high density of atomic-scale defects continue blocking all molecular transport, but their proton permeability becomes similar to 1000 times higher than that of defect-free graphene. Lithium ions can also permeate through such disordered graphene. The enhanced proton and ion permeability is attributed to a high density of eight-carbon-atom rings. The latter pose approximately twice lower energy barriers for incoming protons compared to that of the six-atom rings of graphene and a relatively low barrier of similar to 0.6 eV for Li ions. Our findings suggest that disordered graphene could be of interest as membranes and protective barriers in various Li-ion and hydrogen technologies. |
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Wos |
000543744100086 |
Publication Date |
2020-05-19 |
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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 |
34 |
Open Access |
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Notes |
; The work was supported by the Lloyd's Register Foundation, EPSRC-EP/N010345/1, the European Research Council, the Graphene Flagship, the Deutsche Forschungsgemeinschaft project TRR 234 “CataLight” (Project B7, Grant No. 364549901), and the research infrastructure Grant No. INST 275/25 7-1 FUGG. E.G. and L.M. acknowledge the EPSRC NowNANO programme for funding. ; |
Approved |
Most recent IF: 17.1; 2020 IF: 13.942 |
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Call Number |
UA @ admin @ c:irua:170708 |
Serial |
6586 |
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Author |
Bagiński, M.; Pedrazo-Tardajos, A.; Altantzis, T.; Tupikowska, M.; Vetter, A.; Tomczyk, E.; Suryadharma, R.N.S.; Pawlak, M.; Andruszkiewicz, A.; Górecka, E.; Pociecha, D.; Rockstuhl, C.; Bals, S.; Lewandowski, W. |
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Title |
Understanding and Controlling the Crystallization Process in Reconfigurable Plasmonic Superlattices |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Acs Nano |
Abbreviated Journal |
Acs Nano |
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Volume |
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Issue |
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Pages |
acsnano.0c09746 |
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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 crystallization of nanomaterials is a primary source of solid-state, photonic structures. Thus, a detailed understanding of this process is of paramount importance for the successful application of photonic nanomaterials in emerging optoelectronic technologies. While colloidal crystallization has been thoroughly studied, for example, with advanced in situ electron microscopy methods, the noncolloidal crystallization (freezing) of nanoparticles (NPs) remains so far unexplored. To fill this gap, in this work, we present proof-of principle experiments decoding a crystallization of reconfigurable assemblies of NPs at a solid state. The chosen material corresponds to an excellent testing bed, as it enables both in situ and ex situ investigation using X-ray diffraction (XRD), transmission electron microscopy (TEM), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), atomic force microscopy (AFM), and optical spectroscopy in visible and ultraviolet range (UV−vis) techniques. In particular, ensemble measurements with small-angle XRD highlighted the dependence of the correlation length in the NPs assemblies on the number of heating/cooling cycles and the rate of cooling. Ex situ TEM imaging further supported these results by revealing a dependence of domain size and structure on the sample preparation route and by showing we can control the domain size over 2 orders of magnitude. The application of HAADF-STEM tomography, combined with in situ thermal control, provided three-dimensional single-particle level information on the positional order evolution within assemblies. This combination of real and reciprocal space provides insightful information on the anisotropic, reversibly reconfigurable assemblies of NPs. TEM measurements also highlighted the importance of interfaces in the polydomain structure of nanoparticle solids, allowing us to understand experimentally observed differences in UV−vis extinction spectra of the differently prepared crystallites. Overall, the obtained results show that the combination of in situ heating HAADF-STEM tomography with XRD and ex situ TEM techniques is a powerful approach to study nanoparticle freezing processes and to reveal the crucial impact of disorder in the solid-state aggregates of NPs on their plasmonic properties. |
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Wos |
000634569100101 |
Publication Date |
2021-02-23 |
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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 |
13.942 |
Times cited |
10 |
Open Access |
OpenAccess |
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Notes |
Ministerstwo Nauki i Szkolnictwa Wyzszego, 0112/DIA/2019/48 ; European Commission, 731019 E171000009 (EUSMI) ; Narodowe Centrum Nauki, 2016/21/N/ST5/03356 ; Deutsche Forschungsgemeinschaft, RO 3640/12-1 ; Fundacja na rzecz Nauki Polskiej, First TEAM2016–2/15 ; European Research Council, 815128 (REALNANO) ; sygma; |
Approved |
Most recent IF: 13.942 |
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Call Number |
EMAT @ emat @c:irua:175872 |
Serial |
6673 |
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Author |
Frolov, A.S.; Sanchez-Barriga, J.; Callaert, C.; Hadermann, J.; Fedorov, A., V; Usachov, D.Y.; Chaika, A.N.; Walls, B.C.; Zhussupbekov, K.; Shvets, I., V.; Muntwiler, M.; Amati, M.; Gregoratti, L.; Varykhalov, A.Y.; Rader, O.; Yashina, L., V. |
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Title |
Atomic and electronic structure of a multidomain GeTe crystal |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Acs Nano |
Abbreviated Journal |
Acs Nano |
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Volume |
14 |
Issue |
12 |
Pages |
16576-16589 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Renewed interest in the ferroelectric semi-conductor germanium telluride was recently triggered by the direct observation of a giant Rashba effect and a 30-year-old dream about a functional spin field-effect transistor. In this respect, all-electrical control of the spin texture in this material in combination with ferroelectric properties at the nanoscale would create advanced functionalities in spintronics and data information processing. Here, we investigate the atomic and electronic properties of GeTe bulk single crystals and their (111) surfaces. We succeeded in growing crystals possessing solely inversion domains of similar to 10 nm thickness parallel to each other. Using HAADF-TEM we observe two types of domain boundaries, one of them being similar in structure to the van der Waals gap in layered materials. This structure is responsible for the formation of surface domains with preferential Te-termination (similar to 68%) as we determined using photoelectron diffraction and XPS. The lateral dimensions of the surface domains are in the range of similar to 10-100 nm, and both Ge- and Te-terminations reveal no reconstruction. Using spin-ARPES we establish an intrinsic quantitative relationship between the spin polarization of pure bulk states and the relative contribution of different terminations, a result that is consistent with a reversal of the spin texture of the bulk Rashba bands for opposite configurations of the ferroelectric polarization within individual nanodomains. Our findings are important for potential applications of ferroelectric Rashba semiconductors in nonvolatile spintronic devices with advanced memory and computing capabilities at the nanoscale. |
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Wos |
000603308800022 |
Publication Date |
2020-11-02 |
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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 |
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Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 17.1; 2020 IF: 13.942 |
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Call Number |
UA @ admin @ c:irua:175027 |
Serial |
6716 |
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Author |
Walters, A.A.; Santacana-Font, G.; Li, J.; Routabi, N.; Qin, Y.; Claes, N.; Bals, S.; Tzu-Wen Wang, J.; Al-Jamal, K.T. |
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Title |
Nanoparticle-MediatedIn SituMolecular Reprogramming of Immune Checkpoint Interactions for Cancer Immunotherapy |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Acs Nano |
Abbreviated Journal |
Acs Nano |
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Volume |
15 |
Issue |
11 |
Pages |
17549-17564 |
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Keywords |
A1 Journal article; Pharmacology. Therapy; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Immune checkpoint blockade involves targeting immune
regulatory molecules with antibodies. Preclinically, complex multiantibody
regimes of both inhibitory and stimulatory targets are a promising
candidate for the next generation of immunotherapy. However, in this
setting, the antibody platform may be limited due to excessive toxicity
caused by off target effects as a result of systemic administration. RNA
can be used as an alternate to antibodies as it can both downregulate
immunosuppressive checkpoints (siRNA) or induce expression of
immunostimulatory checkpoints (mRNA). In this study, we demonstrate
that the combination of both siRNA and mRNA in a single
formulation can simultaneously knockdown and induce expression of
immune checkpoint targets, thereby reprogramming the tumor
microenvironment from immunosuppressive to immunostimulatory
phenotype. To achieve this, RNA constructs were synthesized and
formulated into stable nucleic acid lipid nanoparticles (SNALPs); the SNALPs produced were 140−150 nm in size with >80%
loading efficiency. SNALPs could transfect macrophages and B16F10 cells in vitro resulting in 75% knockdown of inhibitory
checkpoint (PDL1) expression and simultaneously express high levels of stimulatory checkpoint (OX40L) with minimal
toxicity. Intratumoral treatment with the proposed formulation resulted in statistically reduced tumor growth, a greater
density of CD4+ and CD8+ infiltrates in the tumor, and immune activation within tumor-draining lymph nodes. These data
suggest that a single RNA-based formulation can successfully reprogram multiple immune checkpoint interactions on a
cellular level. Such a candidate may be able to replace future immune checkpoint therapeutic regimes composed of both
stimulatory- and inhibitory-receptor-targeting antibodies. |
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Wos |
000747115200039 |
Publication Date |
2021-11-23 |
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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 |
13.942 |
Times cited |
11 |
Open Access |
OpenAccess |
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Notes |
A.A.W. is the grateful recipient of a Maplethorpe Fellowship. K.A.J. acknowledges funding from the British Council (Newton Fund, 337313), Wellcome Trust (WT103913), and the Cancer Research UK King’s Health Partners Centre at King’s College London. Financial support is acknowledged from the European Commission under the Horizon 2020 Programme, by means of Grant Agreement No. 731019 (EUSMI). Images were drawn on BioRender.com. |
Approved |
Most recent IF: 13.942 |
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Call Number |
EMAT @ emat @c:irua:183950 |
Serial |
6829 |
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Author |
Choukroun, D.; Pacquets, L.; Li, C.; Hoekx, S.; Arnouts, S.; Baert, K.; Hauffman, T.; Bals, S.; Breugelmans, T. |
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Title |
Mapping composition–selectivity relationships of supported sub-10 nm Cu–Ag nanocrystals for high-rate CO₂ electroreduction |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Acs Nano |
Abbreviated Journal |
Acs Nano |
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Volume |
15 |
Issue |
9 |
Pages |
14858-14872 |
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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 |
Colloidal Cu–Ag nanocrystals measuring less than 10 nm across are promising candidates for integration in hybrid CO2 reduction reaction (CO2RR) interfaces, especially in the context of tandem catalysis and selective multicarbon (C2–C3) product formation. In this work, we vary the synthetic-ligand/copper molar ratio from 0.1 to 1.0 and the silver/copper atomic ratio from 0 to 0.7 and study the variations in the nanocrystals’ size distribution, morphology and reactivity at rates of ≥100 mA cm–2 in a gas-fed recycle electrolyzer operating under neutral to mildly basic conditions (0.1–1.0 M KHCO3). High-resolution electron microscopy and spectroscopy are used in order to characterize the morphology of sub-10 nm Cu–Ag nanodimers and core–shells and to elucidate trends in Ag coverage and surface composition. It is shown that Cu–Ag nanocrystals can be densely dispersed onto a carbon black support without the need for immediate ligand removal or binder addition, which considerably facilitates their application. Although CO2RR product distribution remains an intricate function of time, (kinetic) overpotential and processing conditions, we nevertheless conclude that the ratio of oxygenates to hydrocarbons (which depends primarily on the initial dispersion of the nanocrystals and their composition) rises 3-fold at moderate Ag atom % relative to Cu NCs-based electrodes. Finally, the merits of this particular Cu–Ag/C system and the recycling reactor employed are utilized to obtain maximum C2–C3 partial current densities of 92–140 mA cm–2 at −1.15 VRHE and liquid product concentrations in excess of 0.05 wt % in 1 M KHCO3 after short electrolysis periods. |
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Wos |
000703553600082 |
Publication Date |
2021-08-24 |
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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 |
13.942 |
Times cited |
25 |
Open Access |
OpenAccess |
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Notes |
D.C. acknowledges Thomas Kenis for configuring the analytical instrumentation (HPLC/GC-FID/ICP-MS), Hannelore Andries for assistance with ICP-MS measurements, and Dr. Saeid Pourbabak and Dr. Tine Derez for assistance with Cu sputtering. L.P. was supported by Research Foundation of Flanders (FWO 1S56920N). S.B. acknowledges financial support from ERC Consolidator grant number 815128 REALNANO. S.B. and T.B. acknowledge financial support from the university research fund (BOF-GOA-PS ID no. 33928).; sygmaSB |
Approved |
Most recent IF: 13.942 |
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Call Number |
UA @ admin @ c:irua:180305 |
Serial |
6844 |
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Author |
Dey, A.; Ye, J.; De, A.; Debroye, E.; Ha, S.K.; Bladt, E.; Kshirsagar, A.S.; Wang, Z.; Yin, J.; Wang, Y.; Quan, L.N.; Yan, F.; Gao, M.; Li, X.; Shamsi, J.; Debnath, T.; Cao, M.; Scheel, M.A.; Kumar, S.; Steele, J.A.; Gerhard, M.; Chouhan, L.; Xu, K.; Wu, X.-gang; Li, Y.; Zhang, Y.; Dutta, A.; Han, C.; Vincon, I.; Rogach, A.L.; Nag, A.; Samanta, A.; Korgel, B.A.; Shih, C.-J.; Gamelin, D.R.; Son, D.H.; Zeng, H.; Zhong, H.; Sun, H.; Demir, H.V.; Scheblykin, I.G.; Mora-Sero, I.; Stolarczyk, J.K.; Zhang, J.Z.; Feldmann, J.; Hofkens, J.; Luther, J.M.; Perez-Prieto, J.; Li, L.; Manna, L.; Bodnarchuk, M., I; Kovalenko, M., V; Roeffaers, M.B.J.; Pradhan, N.; Mohammed, O.F.; Bakr, O.M.; Yang, P.; Muller-Buschbaum, P.; Kamat, P., V; Bao, Q.; Zhang, Q.; Krahne, R.; Galian, R.E.; Stranks, S.D.; Bals, S.; Biju, V.; Tisdale, W.A.; Yan, Y.; Hoye, R.L.Z.; Polavarapu, L. |
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Title |
State of the art and prospects for Halide Perovskite Nanocrystals |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Acs Nano |
Abbreviated Journal |
Acs Nano |
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Volume |
15 |
Issue |
7 |
Pages |
10775-10981 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Metal-halide perovskites have rapidly emerged as one of the most promising materials of the 21st century, with many exciting properties and great potential for a broad range of applications, from photovoltaics to optoelectronics and photocatalysis. The ease with which metal-halide perovskites can be synthesized in the form of brightly luminescent colloidal nanocrystals, as well as their tunable and intriguing optical and electronic properties, has attracted researchers from different disciplines of science and technology. In the last few years, there has been a significant progress in the shape-controlled synthesis of perovskite nanocrystals and understanding of their properties and applications. In this comprehensive review, researchers having expertise in different fields (chemistry, physics, and device engineering) of metal-halide perovskite nanocrystals have joined together to provide a state of the art overview and future prospects of metal-halide perovskite nanocrystal research. |
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Wos |
000679406500006 |
Publication Date |
2021-06-17 |
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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 |
13.942 |
Times cited |
538 |
Open Access |
OpenAccess |
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Notes |
E.D. and J.H. acknowledge financial support from the Research FoundationFlanders (FWO Grant Nos. S002019N, G.0B39.15, G.0B49.15, G.0962.13, G098319N, and ZW15_09-GOH6316), the Research Foundation Flanders postdoctoral fellowships to J.A.S. and E.D. (FWO Grant Nos. 12Y7218N and 12O3719N, respectively), |
Approved |
Most recent IF: 13.942 |
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Call Number |
UA @ admin @ c:irua:180553 |
Serial |
6846 |
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| Permanent link to this record |
