| Records |
| Author |
Marchetti, A.; Saniz, R.; Krishnan, D.; Rabbachin, L.; Nuyts, G.; De Meyer, S.; Verbeeck, J.; Janssens, K.; Pelosi, C.; Lamoen, D.; Partoens, B.; De Wael, K. |
| Title |
Unraveling the Role of Lattice Substitutions on the Stabilization of the Intrinsically Unstable Pb2Sb2O7Pyrochlore: Explaining the Lightfastness of Lead Pyroantimonate Artists’ Pigments |
Type |
A1 Journal article |
| Year |
2020 |
Publication |
Chemistry Of Materials |
Abbreviated Journal |
Chem Mater |
| Volume |
32 |
Issue |
7 |
Pages |
2863-2873 |
| Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT) |
| Abstract |
The pyroantimonate pigments Naples yellow and lead tin antimonate yellow are recognized as some of the most stable synthetic yellow pigments in the history of art. However, this exceptional lightfastness is in contrast with experimental evidence suggesting that this class of mixed oxides is of semiconducting nature. In this study the electronic structure and light-induced behavior of the lead pyroantimonate pigments were determined by means of a combined multifaceted analytical and computational approach (photoelectrochemical measurements, UV-vis diffuse reflectance spectroscopy, STEM-EDS, STEM-HAADF, and density functional theory calculations). The results demonstrate both the semiconducting nature and the lightfastness of these pigments. Poor optical absorption and minority carrier mobility are the main properties responsible for the observed stability. In addition, novel fundamental insights into the role played by Na atoms in the stabilization of the otherwise intrinsically unstable Pb2Sb2O7 pyrochlore were obtained. |
| 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 |
000526394000016 |
Publication Date |
2020-04-14 |
| 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 |
0897-4756 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
| Impact Factor |
8.6 |
Times cited |
8 |
Open Access |
OpenAccess |
| Notes |
Universiteit Antwerpen; Belgian Federal Science Policy Office; |
Approved  |
Most recent IF: 8.6; 2020 IF: 9.466 |
| Call Number |
EMAT @ emat @c:irua:168819 |
Serial |
6363 |
| Permanent link to this record |
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| Author |
Imran, M.; Ramade, J.; Di Stasio, F.; De Franco, M.; Buha, J.; Van Aert, S.; Goldoni, L.; Lauciello, S.; Prato, M.; Infante, I.; Bals, S.; Manna, L. |
| Title |
Alloy CsCdxPb1–xBr3Perovskite Nanocrystals: The Role of Surface Passivation in Preserving Composition and Blue Emission |
Type |
A1 Journal article |
| Year |
2020 |
Publication |
Chemistry Of Materials |
Abbreviated Journal |
Chem Mater |
| Volume |
32 |
Issue |
|
Pages |
acs.chemmater.0c03825 |
| Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
| Abstract |
Various strategies have been proposed to engineer the band gap of metal halide perovskite nanocrystals (NCs) while preserving their structure and composition and thus ensuring spectral stability of the emission color. An aspect that has only been marginally investigated is how the type of surface passivation influences the structural/color stability of AMX3 perovskite NCs composed of two different M2+ cations. Here, we report the synthesis of blue-emitting Cs-oleate capped CsCdxPb1–xBr3 NCs, which exhibit a cubic perovskite phase containing Cd-rich domains of Ruddlesden–Popper phases (RP phases). The RP domains spontaneously transform into pure orthorhombic perovskite ones upon NC aging, and the emission color of the NCs shifts from blue to green over days. On the other hand, postsynthesis ligand exchange with various Cs-carboxylate or ammonium bromide salts, right after NC synthesis, provides monocrystalline NCs with cubic phase, highlighting the metastability of RP domains. When NCs are treated with Cs-carboxylates (including Cs-oleate), most of the Cd2+ ions are expelled from NCs upon aging, and the NCs phase evolves from cubic to orthorhombic and their emission color changes from blue to green. Instead, when NCs are coated with ammonium bromides, the loss of Cd2+ ions is suppressed and the NCs tend to retain their blue emission (both in colloidal dispersions and in electroluminescent devices), as well as their cubic phase, over time. The improved compositional and structural stability in the latter cases is ascribed to the saturation of surface vacancies, which may act as channels for the expulsion of Cd2+ ions from NCs. |
| 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 |
000603288800034 |
Publication Date |
2020-12-04 |
| 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 |
0897-4756 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
| Impact Factor |
8.6 |
Times cited |
44 |
Open Access |
OpenAccess |
| Notes |
European Commission; Fonds Wetenschappelijk Onderzoek, G.0267.18N ; H2020 European Research Council, 770887 815128 851794 ; We acknowledge funding from the FLAG-ERA JTC2019 project PeroGas. S.B., and S.V.A. acknowledges funding from the European Research Council under the European Union’s Horizon 2020 research and innovation program (ERC Consolidator Grants #815128REALNANO and #770887PICOMETRICS) and from the Research Foundation Flanders (FWO, Belgium) through project funding G.0267.18N. F.D.S. acknowledges the funding from ERC starting grant NANOLED (851794). The computational work was carried out on the Dutch National e-infrastructure with the support of the SURF Cooperative; sygma |
Approved |
Most recent IF: 8.6; 2020 IF: 9.466 |
| Call Number |
EMAT @ emat @c:irua:174004 |
Serial |
6659 |
| Permanent link to this record |
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| Author |
Hao, Y.; Velpula, G.; Kaltenegger, M.; Bodlos, W.R.; Vibert, F.; Mali, K.S.; De Feyter, S.; Resel, R.; Geerts, Y.H.; Van Aert, S.; Beljonne, D.; Lazzaroni, R. |
| Title |
From 2D to 3D : bridging self-assembled monolayers to a substrate-induced polymorph in a molecular semiconductor |
Type |
A1 Journal article |
| Year |
2022 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
| Volume |
34 |
Issue |
5 |
Pages |
2238-2248 |
| Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
| Abstract |
In this study, a new bottom-up approach is proposed to predict the crystal structure of the substrate-induced polymorph (SIP) of an archetypal molecular semiconductor. In spite of intense efforts, the formation mechanism of SIPs is still not fully understood, and predicting their crystal structure is a very delicate task. Here, we selected lead phthalocyanine (PbPc) as a prototypical molecular material because it is a highly symmetrical yet nonplanar molecule and we demonstrate that the growth and crystal structure of the PbPc SIPs can be templated by the corresponding physisorbed self-assembled molecular networks (SAMNs). Starting from SAMNs of PbPc formed at the solution/graphite interface, the structural and energetic aspects of the assembly were studied by a combination of in situ scanning tunneling microscopy and multiscale computational chemistry approach. Then, the growth of a PbPc SIP on top of the physisorbed monolayer was modeled without prior experimental knowledge, from which the crystal structure of the SIP was predicted. The theoretical prediction of the SIP was verified by determining the crystal structure of PbPc thin films using X-ray diffraction techniques, revealing the formation of a new polymorph of PbPc on the graphite substrate. This study clearly illustrates the correlation between the SAMNs and SIPs, which are traditionally considered as two separate but conceptually connected research areas. This approach is applicable to molecular materials in general to predict the crystal structure of their SIPs. |
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Thesis |
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Place of Publication |
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Editor |
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Wos |
000812125800001 |
Publication Date |
2022-02-17 |
| 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 |
0897-4756; 1520-5002 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
| Impact Factor |
8.6 |
Times cited |
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Open Access |
Not_Open_Access |
| Notes |
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Approved |
Most recent IF: 8.6 |
| Call Number |
UA @ admin @ c:irua:189086 |
Serial |
7084 |
| Permanent link to this record |
