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Author Javon, E.; Gaceur, M.; Dachraoui, W.; Margeat, O.; Ackermann, J.; Ilenia Saba, M.; Delugas, P.; Mattoni, A.; Bals, S.; Van Tendeloo, G. pdf  url
doi  openurl
  Title Competing forces in the self-assembly of coupled ZnO nanopyramids Type A1 Journal article
  Year 2015 Publication ACS nano Abbreviated Journal Acs Nano  
  Volume 9 Issue 9 Pages 3685-3694  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Self-assembly (SA) of nanostructures has recently gained increasing interest. A clear understanding of the process is not straightforward since SA of nanoparticles is a complex multiscale phenomenon including different driving forces. Here, we study the SA between aluminum doped ZnO nanopyramids into couples by combining inorganic chemistry and advanced electron microscopy techniques with atomistic simulations. Our results show that the SA of the coupled nanopyramids is controlled first by morphology, as coupling only occurs in the case of pyramids with well-developed facets of the basal planes. The combination of electron microscopy and atomistic modeling reveals that the coupling is further driven by strong ligandligand interaction between the bases of the pyramids as dominant force, while screening effects due to Al doping or solvent as well as corecore interaction are only minor contributions. Our combined approach provides a deeper understanding of the complex interplay between the interactions at work in the coupled SA of ZnO nanopyramids.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000353867000030 Publication Date 2015-03-12  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 13.942 Times cited 21 Open Access OpenAccess  
  Notes Esmi; 335078 Colouratom; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); Approved Most recent IF: 13.942; 2015 IF: 12.881  
  Call Number (up) c:irua:125978 Serial 434  
Permanent link to this record
 

 
Author Chen, B.; Sahin, H.; Suslu, A.; Ding, L.; Bertoni, M.I.; Peeters, F.M.; Tongay, S. doi  openurl
  Title Environmental changes in MoTe2 excitonic dynamics by defects-activated molecular interaction Type A1 Journal article
  Year 2015 Publication ACS nano Abbreviated Journal Acs Nano  
  Volume 9 Issue 9 Pages 5326-5332  
  Keywords A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)  
  Abstract Monolayers of group VI transition metal dichalcogenides possess direct gaps in the visible spectrum with the exception of MoTe2, where its gap is suitably located in the infrared region but its stability is of particular interest, as tellurium compounds are acutely sensitive to oxygen exposure. Here, our environmental (time-dependent) measurements reveal two distinct effects on MoTe2 monolayers: For weakly luminescent monolayers, photoluminescence signal and optical contrast disappear, as if they are decomposed, but yet remain intact as evidenced by AFM and Raman measurements. In contrast, strongly luminescent monolayers retain their optical contrast for a prolonged amount of time, while their PL peak blue-shifts and PL intensity saturates to slightly lower values. Our X-ray photoelectron spectroscopy measurements and DFT calculations suggest that the presence of defects and functionalization of these defect sites with O-2 molecules strongly dictate their material properties and aging response by changing the excitonic dynamics due to deep or shallow states that are created within the optical band gap. Presented results not only shed light on environmental effects on fundamental material properties and excitonic dynamics of MoTe2 monolayers but also highlight striking material transformation for metastable 20 systems such as WTe2, silicone, and phosphorene.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000355383000068 Publication Date 2015-04-14  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 13.942 Times cited 150 Open Access  
  Notes ; This work was supported by the Arizona State University seeding program. The authors thank Hui Cai and Kedi Wu for useful discussions. We gratefully acknowledge the use of facilities at the LeRoy Eyring Center for Solid State Science at Arizona State University. This work was supported by the Flemish Science Foundation (FWO-VI) and the Methusalem Foundation of the Flemish government. H.S. is supported by a FWO Pegasus Long Marie Curie Fellowship. ; Approved Most recent IF: 13.942; 2015 IF: 12.881  
  Call Number (up) c:irua:126441 Serial 1068  
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Author Chen, J.J.; Wang, Q.; Meng, J.; Ke, X.; Van Tendeloo, G.; Bie, Y.Q.; Liu, J.; Liu, K.; Liao, Z.M.; Sun, D.; Yu, D.; pdf  url
doi  openurl
  Title Photovoltaic effect and evidence of carrier multiplication in graphene vertical homojunctions with asymmetrical metal contacts Type A1 Journal article
  Year 2015 Publication ACS nano Abbreviated Journal Acs Nano  
  Volume 9 Issue 9 Pages 8851-8858  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Graphene exhibits exciting potentials for high-speed wideband photodetection and high quantum efficiency solar energy harvest because of its broad spectral absorption, fast photoelectric response, and potential carrier multiplication. Although photocurrent can be generated near a metalgraphene interface in lateral devices, the photoactive area is usually limited to a tiny one-dimensional line-like interface region. Here, we report photoelectric devices based on vertical graphene two-dimensional homojunction, which is fabricated via vertically stacking four graphene monolayers with asymmetric metal contacts. The devices show excellent photovoltaic output with excitation wavelength ranging from visible light to mid-infrared. The wavelength dependence of the internal quantum efficiency gives direct evidence of the carrier multiplication effect in graphene. The simple fabrication process, easy scale-up, large photoresponsive active area, and broadband response of the vertical graphene device are very promising for practical applications in optoelectronics and photovoltaics.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000361935800023 Publication Date 2015-08-15  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 13.942 Times cited 11 Open Access  
  Notes 246791 Countatoms Approved Most recent IF: 13.942; 2015 IF: 12.881  
  Call Number (up) c:irua:127689 Serial 2615  
Permanent link to this record
 

 
Author Ghosh, S.; Gaspari, R.; Bertoni, G.; Spadaro, M.C.; Prato, M.; Turner, S.; Cavalli, A.; Manna, L.; Brescia, R. pdf  url
doi  openurl
  Title Pyramid-Shaped Wurtzite CdSe Nanocrystals with Inverted Polarity Type A1 Journal article
  Year 2015 Publication ACS nano Abbreviated Journal Acs Nano  
  Volume 9 Issue 9 Pages 8537-8546  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  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.  
  Address Department of Nanochemistry, Istituto Italiano di Tecnologia (IIT) , via Morego 30, I-16163 Genova, Italy  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language English Wos 000360323300085 Publication Date 2015-07-23  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 13.942 Times cited 16 Open Access  
  Notes PMID:26203791 Approved Most recent IF: 13.942; 2015 IF: 12.881  
  Call Number (up) c:irua:127807 Serial 3956  
Permanent link to this record
 

 
Author van der Stam, W.; Bladt, E.; Rabouw, F.T.; Bals, S.; de Mello Donega, C. pdf  url
doi  openurl
  Title Near-Infrared Emitting CuInSe/CuInS Dot Core/Rod Shell Heteronanorods by Sequential Cation Exchange Type A1 Journal article
  Year 2015 Publication ACS nano Abbreviated Journal Acs Nano  
  Volume 9 Issue 9 Pages 11430-11438  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  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.  
  Address Debye Institute for Nanomaterials Science, Utrecht University , P.O. Box 80000, 3508 TA Utrecht, The Netherlands  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language English Wos 000365464800094 Publication Date 2015-10-09  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 13.942 Times cited 88 Open Access OpenAccess  
  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  
  Call Number (up) c:irua:129184 Serial 3948  
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Author Sanz-Ortiz, M.N.; Sentosun, K.; Bals, S.; Liz-Marzan, L.M. pdf  url
doi  openurl
  Title Templated Growth of Surface Enhanced Raman Scattering -Active Branched Au Nanoparticles within Radial Mesoporous Silica Shells Type A1 Journal article
  Year 2015 Publication ACS nano Abbreviated Journal Acs Nano  
  Volume 9 Issue 9 Pages 10489-10497  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Noble metal nanoparticles are widely used as probes or substrates for surface-enhanced Raman scattering (SERS), due to their characteristic plasmon resonances in the visible and NIR spectral ranges. Aiming at obtaining a versatile system with high SERS performance we developed the synthesis of quasi-monodisperse, non-aggregated gold nanoparticles protected by radial mesoporous silica shells. The radial channels of such shells were used as templates for the growth of gold tips branching from the cores, thereby improving the plasmonic performance of the particles while favoring the localization of analyte molecules at high electric field regions: close to the tips, inside the pores. The method, which allows control over tip length, was successfully applied to various gold nanoparticle shapes, leading to materials with highly efficient SERS performance. The obtained nanoparticles are stable in ethanol and water upon thermal consolidation and can be safely stored as a powder.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language English Wos 000363915300105 Publication Date 2015-09-15  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 13.942 Times cited 110 Open Access OpenAccess  
  Notes This work has been funded by the European Research Council (ERC Advanced Grant 267867 Plasmaquo and Starting Grant Colouratom). The research leading to these results has received funding from the European Union's Seventh Framework Programme (FP7/2007-2013 under grant agreement no. 312184, SACS). Help from Mert Kurttepeli is acknowledged. Pentatwinned nanorods and nanotriangles were synthesized by L. Scarabelli.; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); Approved Most recent IF: 13.942; 2015 IF: 12.881  
  Call Number (up) c:irua:129194 Serial 3947  
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Author Yan, Y.; Zhou, X.; Jin, H.; Li, C.-Z.; Ke, X.; Van Tendeloo, G.; Liu, K.; Yu, D.; Dressel, M.; Liao, Z.-M. url  doi
openurl 
  Title Surface-Facet-Dependent Phonon Deformation Potential in Individual Strained Topological Insulator Bi2Se3 Nanoribbons Type A1 Journal article
  Year 2015 Publication ACS nano Abbreviated Journal Acs Nano  
  Volume 9 Issue 9 Pages 10244-10251  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Strain is an important method to tune the properties of topological insulators. For example, compressive strain can induce superconductivity in Bi2Se3 bulk material. Topological insulator nanostructures are the superior candidates to utilize the unique surface states due to the large surface to volume ratio. Therefore, it is highly desirable to monitor the local strain effects in individual topological insulator nanostructures. Here, we report the systematical micro-Raman spectra of single strained Bi2Se3 nanoribbons with different thicknesses and different surface facets, where four optical modes are resolved in both Stokes and anti-Stokes Raman spectral lines. A striking anisotropy of the strain dependence is observed in the phonon frequency of strained Bi2Se3 nanoribbons grown along the ⟨112̅0⟩ direction. The frequencies of the in-plane Eg2 and out-of-plane A1g1 modes exhibit a nearly linear blue-shift against bending strain when the nanoribbon is bent along the ⟨112̅0⟩ direction with the curved {0001} surface. In this case, the phonon deformation potential of the Eg2 phonon for 100 nm-thick Bi2Se3 nanoribbon is up to 0.94 cm–1/%, which is twice of that in Bi2Se3 bulk material (0.52 cm–1/%). Our results may be valuable for the strain modulation of individual topological insulator nanostructures.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language English Wos 000363915300079 Publication Date 2015-09-12  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 13.942 Times cited 14 Open Access  
  Notes Y.Y. would like to thank Xuewen Fu for helpful discussions. This work was supported by MOST (Nos. 2013CB934600, 2013CB932602) and NSFC (Nos. 11274014, 11234001). Approved Most recent IF: 13.942; 2015 IF: 12.881  
  Call Number (up) c:irua:129216 Serial 3963  
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Author Neek-Amal, M.; Peeters, F.M.; Grigorieva, I.V.; Geim, A.K. url  doi
openurl 
  Title Commensurability Effects in Viscosity of Nanoconfined Water Type A1 Journal article
  Year 2016 Publication ACS nano Abbreviated Journal Acs Nano  
  Volume 10 Issue 10 Pages 3685-3692  
  Keywords A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)  
  Abstract The rate of water flow through hydrophobic nanocapillaries is greatly enhanced as compared to that expected from macroscopic hydrodynamics. This phenomenon is usually described in terms of a relatively large slip length, which is in turn defined by such microscopic properties as the friction between water and capillary surfaces and the viscosity of water. We show that the viscosity of water and, therefore, its flow rate are profoundly affected by the layered structure of confined water if the capillary size becomes less than 2 nm. To this end, we study the structure and dynamics of water confined between two parallel graphene layers using equilibrium molecular dynamics simulations. We find that the shear viscosity is not only greatly enhanced for subnanometer capillaries, but also exhibits large oscillations that originate from commensurability between the capillary size and the size of water molecules. Such oscillating behavior of viscosity and, consequently, the slip length should be taken into account in designing and studying graphene-based and similar membranes for desalination and filtration.  
  Address School of Physics and Astronomy, University of Manchester , Manchester M13 9PL, United Kingdom  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language English Wos 000372855400073 Publication Date 2016-02-16  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 13.942 Times cited 160 Open Access  
  Notes ; M.N.A. was support by Shahid Rajaee Teacher Training University under contract number 29605. ; Approved Most recent IF: 13.942  
  Call Number (up) c:irua:133237 Serial 4012  
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Author Lentijo-Mozo, S.; Tan, R.P.; Garcia-Marcelot, C.; Altantzis, T.; Fazzini, P.F.; Hungria, T.; Cormary, B.; Gallagher, J.R.; Miller, J.T.; Martinez, H.; Schrittwieser, S.; Schotter, J.; Respaud, M.; Bals, S.; Van Tendeloo, G.; Gatel, C.; Soulantica, K. pdf  url
doi  openurl
  Title Air- and water-resistant noble metal coated ferromagnetic cobalt nanorods Type A1 Journal article
  Year 2015 Publication ACS nano Abbreviated Journal Acs Nano  
  Volume 9 Issue 9 Pages 2792-2804  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Cobalt nanorods possess ideal magnetic properties for applications requiring magnetically hard nanoparticles. However, their exploitation is undermined by their sensitivity toward oxygen and water, which deteriorates their magnetic properties. The development of a continuous metal shell inert to oxidation could render them stable, opening perspectives not only for already identified applications but also for uses in which contact with air and/or aqueous media is inevitable. However, the direct growth of a conformal noble metal shell on magnetic metals is a challenge. Here, we show that prior treatment of Co nanorods with a tin coordination compound is the crucial step that enables the subsequent growth of a continuous noble metal shell on their surface, rendering them air- and water-resistant, while conserving the monocrystallity, metallicity and the magnetic properties of the Co core. Thus, the as-synthesized coreshell ferromagnetic nanorods combine high magnetization and strong uniaxial magnetic anisotropy, even after exposure to air and water, and hold promise for successful implementation in in vitro biodiagnostics requiring probes of high magnetization and anisotropic shape.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000351791800055 Publication Date 2015-03-03  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851;1936-086X; ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 13.942 Times cited 25 Open Access OpenAccess  
  Notes 312483 Esteem2; 246791 Countatoms; 335078 Colouratom; esteem2ta; ECASSara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); Approved Most recent IF: 13.942; 2015 IF: 12.881  
  Call Number (up) c:irua:125380 c:irua:125380 Serial 87  
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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. pdf  url
doi  openurl
  Title Direct Observation of Luminescent Silver Clusters Confined in Faujasite Zeolites Type A1 Journal article
  Year 2016 Publication ACS nano Abbreviated Journal Acs Nano  
  Volume 10 Issue 10 Pages 7604-7611  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  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.  
  Address RIES, Hokkaido University , N20W10, Kita-Ward Sapporo 001-0020, Japan  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language English Wos 000381959100043 Publication Date 2016-07-08  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 13.942 Times cited 57 Open Access OpenAccess  
  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  
  Call Number (up) c:irua:134576 c:irua:134576 Serial 4102  
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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. pdf  url
doi  openurl
  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  
  Volume 10 Issue 10 Pages 8778-8787  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT)  
  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.  
  Address Department of Physics, Virginia Tech , Blacksburg, Virginia 24061, United States  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language English Wos 000384399300073 Publication Date 2016-09-02  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 13.942 Times cited 15 Open Access  
  Notes The research in Leuven and Antwerp was supported by the Research FoundationFlanders (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  
  Call Number (up) EMAT @ emat @ c:irua:136269 Serial 4294  
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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. url  doi
openurl 
  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  
  Volume 11 Issue 11 Pages 6277-6285  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  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.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000404808000110 Publication Date 2017-05-10  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 13.942 Times cited 12 Open Access OpenAccess  
  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  
  Call Number (up) EMAT @ emat @ c:irua:143192 Serial 4569  
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Author Montanarella, F.; Altantzis, T.; Zanaga, D.; Rabouw, F.T.; Bals, S.; Baesjou, P.; Vanmaekelbergh, D.; van Blaaderen, A. pdf  url
doi  openurl
  Title Composite Supraparticles with Tunable Light Emission Type A1 Journal article
  Year 2017 Publication ACS nano Abbreviated Journal Acs Nano  
  Volume 11 Issue 11 Pages 9136-9142  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  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.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000411918200062 Publication Date 2017-09-26  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 13.942 Times cited 36 Open Access OpenAccess  
  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  
  Call Number (up) EMAT @ emat @c:irua:146095UA @ admin @ c:irua:146095 Serial 4732  
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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 url  doi
openurl 
  Title Chemistry of Shape-Controlled Iron Oxide Nanocrystal Formation Type A1 Journal article
  Year 2018 Publication ACS nano Abbreviated Journal Acs Nano  
  Volume 13 Issue 13 Pages 152-162  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  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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  Language Wos 000456749900017 Publication Date 2018-12-12  
  Series Editor Series Title Abbreviated Series Title  
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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 54 Open Access OpenAccess  
  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  
  Call Number (up) EMAT @ emat @c:irua:155716UA @ admin @ c:irua:155716 Serial 5073  
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Author Albrecht, W.; Bladt, E.; Vanrompay, H.; Smith, J.D.; Skrabalak, S.E.; Bals, S. url  doi
openurl 
  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  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  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.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000473248300038 Publication Date 2019-06-25  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 13.942 Times cited 46 Open Access OpenAccess  
  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  
  Call Number (up) EMAT @ emat @c:irua:161356 Serial 5285  
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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. pdf  url
doi  openurl
  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  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  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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  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000500650000115 Publication Date 2019-10-25  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 13.942 Times cited 29 Open Access OpenAccess  
  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  
  Call Number (up) EMAT @ emat @c:irua:164061 Serial 5379  
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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. url  doi
openurl 
  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  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)  
  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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  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000586793400016 Publication Date 2020-08-19  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 17.1 Times cited 25 Open Access OpenAccess  
  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  
  Call Number (up) EMAT @ emat @c:irua:172440 Serial 6426  
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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. url  doi
openurl 
  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  
  Volume Issue Pages  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  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.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000595533800019 Publication Date 2020-09-01  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 17.1 Times cited 14 Open Access OpenAccess  
  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  
  Call Number (up) EMAT @ emat @c:irua:172492 Serial 6403  
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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. url  doi
openurl 
  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  
  Volume 14 Issue 10 Pages 13146-13160  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  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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  Language Wos 000586793400068 Publication Date 2020-10-27  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 17.1 Times cited 21 Open Access OpenAccess  
  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  
  Call Number (up) EMAT @ emat @c:irua:173862 Serial 6438  
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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. url  doi
openurl 
  Title Understanding and Controlling the Crystallization Process in Reconfigurable Plasmonic Superlattices Type A1 Journal article
  Year 2021 Publication Acs Nano Abbreviated Journal Acs Nano  
  Volume Issue Pages acsnano.0c09746  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)  
  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.  
  Address  
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  Publisher Place of Publication Editor  
  Language Wos 000634569100101 Publication Date 2021-02-23  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 13.942 Times cited 10 Open Access OpenAccess  
  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  
  Call Number (up) EMAT @ emat @c:irua:175872 Serial 6673  
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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. pdf  url
doi  openurl
  Title Nanoparticle-MediatedIn SituMolecular Reprogramming of Immune Checkpoint Interactions for Cancer Immunotherapy Type A1 Journal article
  Year 2021 Publication Acs Nano Abbreviated Journal Acs Nano  
  Volume 15 Issue 11 Pages 17549-17564  
  Keywords A1 Journal article; Pharmacology. Therapy; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  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.
 
  Address  
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  Language Wos 000747115200039 Publication Date 2021-11-23  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 13.942 Times cited 11 Open Access OpenAccess  
  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  
  Call Number (up) EMAT @ emat @c:irua:183950 Serial 6829  
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Author Choo, P.; Arenas-Esteban, D.; Jung, I.; Chang, W.J.; Weiss, E.A.; Bals, S.; Odom, T.W. pdf  url
doi  openurl
  Title Investigating Reaction Intermediates during the Seedless Growth of Gold Nanostars Using Electron Tomography Type A1 Journal article
  Year 2022 Publication ACS nano Abbreviated Journal Acs Nano  
  Volume 16 Issue 3 Pages 4408-4414  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Good’s buffers can act both as nucleating and shape- directing agents during the synthesis of anisotropic gold nanostars (AuNS). Although different Good’s buffers can produce AuNS shapes with branches that are oriented along specific crystallographic directions, the mechanism is not fully understood. This paper reports how an analysis of the intermediate structures during AuNS synthesis from HEPES, EPPS, and MOPS Good’s buffers can provide insight into the formation of seedless AuNS. Electron tomography of AuNS structures quenched at early times (minutes) was used to characterize the morphology of the incipient seeds, and later times were used to construct the growth maps. Through this approach, we identified how the crystallinity and shape of the first structures synthesized with different Good’s buffers determine the final AuNS morphologies.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000780214300084 Publication Date 2022-03-22  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 17.1 Times cited 12 Open Access OpenAccess  
  Notes This work was supported by the National Science Foundation (NSF) under award NSF CHE-1808502 (P.C. and I.J.). This work made use of the EPIC facility of Northwestern University’s NUANCE Center, which has received support from the SHyNE Resource (NSF ECCS-2025633), the IIN, and Northwestern’s MRSEC program (NSF DMR-1720139). D.A E. and S.B. acknowledge funding from the European Research Council under the European Union’s Horizon 2020 research and innovation program (ERC Consolidator Grants No. 815128 REALNANO and Grant Agreement No. 731019 EUSMI).; sygmaSB Approved Most recent IF: 17.1  
  Call Number (up) EMAT @ emat @c:irua:187930 Serial 7055  
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Author Pedrazo-Tardajos, A.; Arslan Irmak, E.; Kumar, V.; Sánchez-Iglesias, A.; Chen, Q.; Wirix, M.; Freitag, B.; Albrecht, W.; Van Aert, S.; Liz-Marzán, L.M.; Bals, S. pdf  url
doi  openurl
  Title Thermal Activation of Gold Atom Diffusion in Au@Pt Nanorods Type A1 Journal article
  Year 2022 Publication ACS nano Abbreviated Journal Acs Nano  
  Volume Issue Pages  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Understanding the thermal stability of bimetallic nanoparticles is of vital importance to preserve their functionalities during their use in a variety of applications. In contrast to well-studied bimetallic systems such as Au@Ag, heat-induced morphological and compositional changes in Au@Pt nanoparticles are insufficiently understood, even though Au@Pt is an important material for catalysis. To investigate the thermal instability of Au@Pt nanorods at temperatures below their bulk melting point, we combined in situ heating with two- and three-dimensional electron microscopy techniques, including three-dimensional energy-dispersive X-ray spectroscopy. The experimental results were used as input for molecular dynamics simulations, to unravel the mechanisms behind the morphological transformation of Au@Pt core–shell nanorods. We conclude that thermal stability is influenced not only by the degree of coverage of Pt on Au but also by structural details of the Pt shell.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000819246800001 Publication Date 2022-06-10  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 17.1 Times cited 8 Open Access OpenAccess  
  Notes S.B., S.V.A., L.M.L.-M. and A.P.-T. acknowledge financial support from the European Commission under the Horizon 2020 Programme by grant nos. 731019 (EUSMI) and 823717 (ESTEEM3) and ERC Consolidator grant nos. 815128 (REALNANO) and 770887 (PICOMETRICS). L.M.L.-M. acknowledges funding from MCIN/AEI/10.13039/501100011033 through grants no. PID2020-117779RB-I00 and Maria de Maeztu Unit of Excellence no. MDM-2017-0720. The authors acknowledge the resources and services used for the simulations in this work were provided by the VSC (Flemish Supercomputer Center), funded by the Research Foundation – Flanders (FWO) and the Flemish Government.; esteem3reported; esteem3JRA Approved Most recent IF: 17.1  
  Call Number (up) EMAT @ emat @c:irua:188540 Serial 7072  
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Author Zhuo, X.; Mychinko, M.; Heyvaert, W.; Larios, D.; Obelleiro-Liz, M.; Taboada, J.M.; Bals, S.; Liz-Marzán, L.M. url  doi
openurl 
  Title Morphological and Optical Transitions during Micelle-Seeded Chiral Growth on Gold Nanorods Type A1 Journal article
  Year 2022 Publication ACS nano Abbreviated Journal Acs Nano  
  Volume Issue Pages  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Chiral plasmonics is a rapidly developing field where breakthroughs and unsolved problems coexist. We have recently reported binary surfactant-assisted seeded growth of chiral gold nanorods (Au NRs) with high chiroptical activity. Such a seeded-growth process involves the use of a chiral cosurfactant that induces micellar helicity, in turn driving the transition from achiral to chiral Au NRs, from both the morphological and the optical points of view. We report herein a detailed study on both transitions, which reveals intermediate states that were hidden so far. The correlation between structure and optical response is carefully analyzed, including the (linear and CD) spectral evolution over time, electron tomography, the impact of NR dimensions on their optical response, the variation of the absorption-to-scattering ratio during the evolution from achiral to chiral Au NRs, and the near-field enhancement related to chiral plasmon modes. Our findings provide further understanding of the growth process of chiral Au NRs and the associated optical changes, which will facilitate further study and applications of chiral nanomaterials.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000878324400001 Publication Date 2022-10-26  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 17.1 Times cited 17 Open Access OpenAccess  
  Notes This work was supported by the European Research Council (ERC-AdG-4DbioSERS-787510 to L.M.L.-M. and ERC-CoG-REALNANO-815128 to S.B.) and the MCIN/AEI/10.13039/501100011033 (Grant PID2020-117779RB-I00). X.Z. acknowledges funding from the Juan de la Cierva fellowship (FJC2018-036104-I) and the University Development Fund (UDF01002665, CUHK-Shenzhen). D.L., M.O.-L., and J.M.T. acknowledge funding from the European Regional Development Fund (ERDF) and the Spanish Ministerio de Ciencia, Innovación y Universidades, under Projects PID2020-116627RB-C21 and PID2020-116627RB-C22, as well as from the ERDF/Galician Regional Government as part of the agreement for funding the Atlantic Research Center for Information and Communication Technologies (atlanTTic) and ERDF/Extremadura Regional Government under Projects IB18073 and GR18055. This work was performed in the framework of the Maria de Maeztu Units of Excellence Program from the Spanish State Research Agency (Grant No. MDM-2017-0720). The authors acknowledge Dr. Guillermo González-Rubio for providing suggestions for synthesis and Dr. Irantzu Llarena for assisting with the CD measurements. Approved Most recent IF: 17.1  
  Call Number (up) EMAT @ emat @c:irua:191815 Serial 7116  
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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. pdf  doi
openurl 
  Title Nanocrystal Core Size and Shape Substitutional Doping and Underlying Crystalline Order in Nanocrystal Superlattices Type A1 Journal article
  Year 2019 Publication ACS nano Abbreviated Journal Acs Nano  
  Volume 13 Issue 5 Pages 5712-5719  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  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.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000469886300078 Publication Date 2019-05-03  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  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  
  Call Number (up) UA @ admin @ c:irua:160344 Serial 5256  
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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. pdf  url
doi  openurl
  Title Disconnecting Symmetry Breaking from Seeded Growth for the Reproducible Synthesis of High Quality Gold Nanorods Type A1 Journal article
  Year 2019 Publication ACS nano Abbreviated Journal Acs Nano  
  Volume 13 Issue 13 Pages 4424-4435  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)  
  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.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000466052900067 Publication Date 2019-04-02  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 13.942 Times cited 100 Open Access OpenAccess  
  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  
  Call Number (up) UA @ admin @ c:irua:160417 Serial 5246  
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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. url  doi
openurl 
  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  
  Volume 13 Issue 13 Pages 12880-12893  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  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.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000500650000061 Publication Date 2019-10-16  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  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  
  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  
  Call Number (up) UA @ admin @ c:irua:165149 Serial 6324  
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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. pdf  doi
openurl 
  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  
  Volume 14 Issue 5 Pages 6181-6190  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  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.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000537682300101 Publication Date 2020-04-17  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 17.1 Times cited 8 Open Access Not_Open_Access  
  Notes ; 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  
  Call Number (up) 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. pdf  url
doi  openurl
  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  
  Volume 14 Issue 6 Pages 7280-7286  
  Keywords A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)  
  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.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000543744100086 Publication Date 2020-05-19  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 17.1 Times cited 34 Open Access  
  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  
  Call Number (up) UA @ admin @ c:irua:170708 Serial 6586  
Permanent link to this record
 

 
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. pdf  url
doi  openurl
  Title Atomic and electronic structure of a multidomain GeTe crystal Type A1 Journal article
  Year 2020 Publication Acs Nano Abbreviated Journal Acs Nano  
  Volume 14 Issue 12 Pages 16576-16589  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  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.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000603308800022 Publication Date 2020-11-02  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 17.1 Times cited Open Access OpenAccess  
  Notes Approved Most recent IF: 17.1; 2020 IF: 13.942  
  Call Number (up) UA @ admin @ c:irua:175027 Serial 6716  
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